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Sample records for 4d ultrafast electron

  1. Perspective: 4D ultrafast electron microscopy—Evolutions and revolutions

    Shorokhov, Dmitry; Zewail, Ahmed H.

    2016-02-01

    In this Perspective, the evolutionary and revolutionary developments of ultrafast electron imaging are overviewed with focus on the "single-electron concept" for probing methodology. From the first electron microscope of Knoll and Ruska [Z. Phys. 78, 318 (1932)], constructed in the 1930s, to aberration-corrected instruments and on, to four-dimensional ultrafast electron microscopy (4D UEM), the developments over eight decades have transformed humans' scope of visualization. The changes in the length and time scales involved are unimaginable, beginning with the micrometer and second domains, and now reaching the space and time dimensions of atoms in matter. With these advances, it has become possible to follow the elementary structural dynamics as it unfolds in real time and to provide the means for visualizing materials behavior and biological functions. The aim is to understand emergent phenomena in complex systems, and 4D UEM is now central for the visualization of elementary processes involved, as illustrated here with examples from past achievements and future outlook.

  2. Ultrafast electron diffraction: Visualization of atomic motion in 4D

    The pathways of transitions in materials and molecules are determined by the motions of atoms and electron densities, on Angstrom scales and in femtosecond or attosecond times. We provide here an account of how ultrashort electron pulses can be used to obtain a four-dimensional visualization in space and time. At two examples, the insulator-metal phase transformation in VO2 and the interlayer dynamics of graphite, we demonstrate the resolution of coherent and incoherent atomic displacements with picometer and femtosecond resolution, indicating the sequential nature of atomic motion in condensed matter transitions. Electron densities can move in times as short as attoseconds. Single-electron pulses afford some promise to reach into this novel regime; we discuss our approaches and what discoveries we may expect to see.

  3. 4D Nanoscale Diffraction Observed by Convergent-Beam Ultrafast Electron Microscopy

    Yurtsever, Aycan; Zewail, Ahmed H.

    2009-01-01

    Diffraction with focused electron probes is among the most powerful tools for the study of time-averaged nanoscale structures in condensed matter. Here, we report four-dimensional (4D) nanoscale diffraction, probing specific site dynamics with 10 orders of magnitude improvement in time resolution, in convergent-beam ultrafast electron microscopy (CB-UEM). As an application, we measured the change of diffraction intensities in laser-heated crystalline silicon as a function of time and fluence....

  4. 4D scanning transmission ultrafast electron microscopy: Single-particle imaging and spectroscopy.

    Ortalan, Volkan; Zewail, Ahmed H

    2011-07-20

    We report the development of 4D scanning transmission ultrafast electron microscopy (ST-UEM). The method was demonstrated in the imaging of silver nanowires and gold nanoparticles. For the wire, the mechanical motion and shape morphological dynamics were imaged, and from the images we obtained the resonance frequency and the dephasing time of the motion. Moreover, we demonstrate here the simultaneous acquisition of dark-field images and electron energy loss spectra from a single gold nanoparticle, which is not possible with conventional methods. The local probing capabilities of ST-UEM open new avenues for probing dynamic processes, from single isolated to embedded nanostructures, without being affected by the heterogeneous processes of ensemble-averaged dynamics. Such methodology promises to have wide-ranging applications in materials science and in single-particle biological imaging. PMID:21615171

  5. 4D nanoscale diffraction observed by convergent-beam ultrafast electron microscopy.

    Yurtsever, Aycan; Zewail, Ahmed H

    2009-10-30

    Diffraction with focused electron probes is among the most powerful tools for the study of time-averaged nanoscale structures in condensed matter. Here, we report four-dimensional (4D) nanoscale diffraction, probing specific site dynamics with 10 orders of magnitude improvement in time resolution, in convergent-beam ultrafast electron microscopy (CB-UEM). As an application, we measured the change of diffraction intensities in laser-heated crystalline silicon as a function of time and fluence. The structural dynamics (change in 7.3 +/- 3.5 picoseconds), the temperatures (up to 366 kelvin), and the amplitudes of atomic vibrations (up to 0.084 angstroms) are determined for atoms strictly localized within the confined probe area (10 to 300 nanometers in diameter). We anticipate a broad range of applications for CB-UEM and its variants, especially in the studies of single particles and heterogeneous structures. PMID:19900928

  6. Scanning ultrafast electron microscopy

    Yang, Ding-Shyue; Mohammed, Omar F.; Zewail, Ahmed H.

    2010-01-01

    Progress has been made in the development of four-dimensional ultrafast electron microscopy, which enables space-time imaging of structural dynamics in the condensed phase. In ultrafast electron microscopy, the electrons are accelerated, typically to 200 keV, and the microscope operates in the transmission mode. Here, we report the development of scanning ultrafast electron microscopy using a field-emission-source configuration. Scanning of pulses is made in the single-electron mode, for whic...

  7. Ultrafast Science Opportunities with Electron Microscopy

    DURR, HERMANN; Wang, X.J., ed.

    2016-04-28

    X-rays and electrons are two of the most fundamental probes of matter. When the Linac Coherent Light Source (LCLS), the world’s first x-ray free electron laser, began operation in 2009, it transformed ultrafast science with the ability to generate laser-like x-ray pulses from the manipulation of relativistic electron beams. This document describes a similar future transformation. In Transmission Electron Microscopy, ultrafast relativistic (MeV energy) electron pulses can achieve unsurpassed spatial and temporal resolution. Ultrafast temporal resolution will be the next frontier in electron microscopy and can ideally complement ultrafast x-ray science done with free electron lasers. This document describes the Grand Challenge science opportunities in chemistry, material science, physics and biology that arise from an MeV ultrafast electron diffraction & microscopy facility, especially when coupled with linac-based intense THz and X-ray pump capabilities.

  8. 4D electron microscopy visualization of anisotropic atomic motions in carbon nanotubes.

    Park, Sang Tae; Flannigan, David J; Zewail, Ahmed H

    2012-06-01

    We report the anisotropic atomic expansion dynamics of multi-walled carbon nanotubes, using 4D electron microscopy. From time-resolved diffraction on the picosecond to millisecond scale, following ultrafast heating at the rate of 10(13) K/s, it is shown that nanotubes expand only in the radial (intertubule) direction, whereas no significant change is observed in the intratubular axial or equatorial dimensions. The non-equilibrium heating occurs on an ultrafast time scale, indicating that the anisotropy is the result of an efficient electron-lattice coupling and is maintained up to equilibration. The recovery time, which measures the heat dissipation rate for equilibration, was found to be on the order of ∼100 μs. This recovery is reproduced theoretically by considering the composite specimen-substrate heat exchange. PMID:22591381

  9. Real-Space Visualization of Energy Loss and Carrier Diffusion in a Semiconductor Nanowire Array Using 4D Electron Microscopy.

    Bose, Riya; Sun, Jingya; Khan, Jafar I; Shaheen, Basamat S; Adhikari, Aniruddha; Ng, Tien Khee; Burlakov, Victor M; Parida, Manas R; Priante, Davide; Goriely, Alain; Ooi, Boon S; Bakr, Osman M; Mohammed, Omar F

    2016-07-01

    A breakthrough in the development of 4D scanning ultrafast electron microscopy is described for real-time and space imaging of secondary electron energy loss and carrier diffusion on the surface of an array of nanowires as a model system, providing access to a territory that is beyond the reach of either static electron imaging or any time-resolved laser spectroscopy. PMID:27111855

  10. Inelastic electron scattering investigation of the complete 4d shell

    In order to test for collective behavior in the filled 4d shell of single atoms with Z approx. = 54, inelastic electron scattering experiments were performed on thin films of antimony, tellurium and barium fluoride using 300 keV electrons. The Te measurements at low momentum transfers are in absolute agreement with photoabsorption results. For Te, a high concentration of oscillator strength is found in the broad maximum which dominates the 4d excitation spectrum. With the aid of a background subtraction, the energy centroid of this feature is located. In a comparison with simple models, the measured energy shift in the 4d continuum as a function of momentum transfer favors a single particle rather than collective description

  11. Biomechanics of DNA structures visualized by 4D electron microscopy

    Lorenz, Ulrich J.; Zewail, Ahmed H.

    2013-01-01

    We present a technique for in situ visualization of the biomechanics of DNA structural networks using 4D electron microscopy. Vibrational oscillations of the DNA structure are excited mechanically through a short burst of substrate vibrations triggered by a laser pulse. Subsequently, the motion is probed with electron pulses to observe the impulse response of the specimen in space and time. From the frequency and amplitude of the observed oscillations, we determine the normal modes and eig...

  12. Optomechanical and crystallization phenomena visualized with 4D electron microscopy: interfacial carbon nanotubes on silicon nitride.

    Flannigan, David J; Zewail, Ahmed H

    2010-05-12

    With ultrafast electron microscopy (UEM), we report observation of the nanoscopic crystallization of amorphous silicon nitride, and the ultrashort optomechanical motion of the crystalline silicon nitride at the interface of an adhering carbon nanotube network. The in situ static crystallization of the silicon nitride occurs only in the presence of an adhering nanotube network, thus indicating their mediating role in reaching temperatures close to 1000 degrees C when exposed to a train of laser pulses. Under such condition, 4D visualization of the optomechanical motion of the specimen was followed by quantifying the change in diffraction contrast of crystalline silicon nitride, to which the nanotube network is bonded. The direction of the motion was established from a tilt series correlating the change in displacement with both the tilt angle and the response time. Correlation of nanoscopic motion with the picosecond atomic-scale dynamics suggests that electronic processes initiated in the nanotubes are responsible for the initial ultrafast optomechanical motion. The time scales accessible to UEM are 12 orders of magnitude shorter than those traditionally used to study the optomechanical motion of carbon nanotube networks, thus allowing for distinctions between the different electronic and thermal mechanisms to be made. PMID:20377202

  13. Biomechanics of DNA structures visualized by 4D electron microscopy.

    Lorenz, Ulrich J; Zewail, Ahmed H

    2013-02-19

    We present a technique for in situ visualization of the biomechanics of DNA structural networks using 4D electron microscopy. Vibrational oscillations of the DNA structure are excited mechanically through a short burst of substrate vibrations triggered by a laser pulse. Subsequently, the motion is probed with electron pulses to observe the impulse response of the specimen in space and time. From the frequency and amplitude of the observed oscillations, we determine the normal modes and eigenfrequencies of the structures involved. Moreover, by selective "nano-cutting" at a given point in the network, it was possible to obtain Young's modulus, and hence the stiffness, of the DNA filament at that position. This experimental approach enables nanoscale mechanics studies of macromolecules and should find applications in other domains of biological networks such as origamis. PMID:23382239

  14. Ultrafast electron diffraction using an ultracold source

    van Mourik, M W; Vredenbregt, E J D; Luiten, O J

    2014-01-01

    We present diffraction patterns from micron-sized areas of mono-crystalline graphite obtained with an ultracold and ultrafast electron source. We show that high spatial coherence is manifest in the visibility of the patterns even for picosecond bunches of appreciable charge, enabled by the extremely low source temperature (~ 10 K). For a larger, ~ 100 um spot size on the sample, spatial coherence lengths > 10 nm result, sufficient to resolve diffraction patterns of complex protein crystals. This makes the source ideal for ultrafast electron diffraction of complex macromolecular structures such as membrane proteins, in a regime unattainable by conventional photocathode sources. By further reducing the source size, sub-um spot sizes on the sample become possible with spatial coherence lengths exceeding 1 nm, enabling ultrafast nano-diffraction for material science.

  15. Ultrafast dynamics of electrons in ammonia.

    Vöhringer, Peter

    2015-04-01

    Solvated electrons were first discovered in solutions of metals in liquid ammonia. The physical and chemical properties of these species have been studied extensively for many decades using an arsenal of electrochemical, spectroscopic, and theoretical techniques. Yet, in contrast to their hydrated counterpart, the ultrafast dynamics of ammoniated electrons remained completely unexplored until quite recently. Femtosecond pump-probe spectroscopy on metal-ammonia solutions and femtosecond multiphoton ionization spectroscopy on the neat ammonia solvent have provided new insights into the optical properties and the reactivities of this fascinating species. This article reviews the nature of the optical transition, which gives the metal-ammonia solutions their characteristic blue appearance, in terms of ultrafast relaxation processes involving bound and continuum excited states. The recombination processes following the injection of an electron via photoionization of the solvent are discussed in the context of the electronic structure of the liquid and the anionic defect associated with the solvated electron. PMID:25493716

  16. Real-space Mapping of Surface Trap States in CIGSe Nanocrystals using 4D Electron Microscopy

    Bose, Riya

    2016-05-26

    Surface trap states in semiconductor copper indium gallium selenide nanocrystals (NCs) which serve as undesirable channels for non-radiative carrier recombination, remain a great challenge impeding the development of solar and optoelectronics devices based on these NCs. In order to design efficient passivation techniques to minimize these trap states, a precise knowledge about the charge carrier dynamics on the NCs surface is essential. However, selective mapping of surface traps requires capabilities beyond the reach of conventional laser spectroscopy and static electron microscopy; it can only be accessed by using a one-of-a-kind, second-generation four-dimensional scanning ultrafast electron microscope (4D S-UEM) with sub-picosecond temporal and nanometer spatial resolutions. Here, we precisely map the surface charge carrier dynamics of copper indium gallium selenide NCs before and after surface passivation in real space and time using S-UEM. The time-resolved snapshots clearly demonstrate that the density of the trap states is significantly reduced after zinc sulfide (ZnS) shelling. Furthermore, removal of trap states and elongation of carrier lifetime are confirmed by the increased photocurrent of the self-biased photodetector fabricated using the shelled NCs.

  17. Real-Space Mapping of Surface Trap States in CIGSe Nanocrystals Using 4D Electron Microscopy.

    Bose, Riya; Bera, Ashok; Parida, Manas R; Adhikari, Aniruddha; Shaheen, Basamat S; Alarousu, Erkki; Sun, Jingya; Wu, Tom; Bakr, Osman M; Mohammed, Omar F

    2016-07-13

    Surface trap states in copper indium gallium selenide semiconductor nanocrystals (NCs), which serve as undesirable channels for nonradiative carrier recombination, remain a great challenge impeding the development of solar and optoelectronics devices based on these NCs. In order to design efficient passivation techniques to minimize these trap states, a precise knowledge about the charge carrier dynamics on the NCs surface is essential. However, selective mapping of surface traps requires capabilities beyond the reach of conventional laser spectroscopy and static electron microscopy; it can only be accessed by using a one-of-a-kind, second-generation four-dimensional scanning ultrafast electron microscope (4D S-UEM) with subpicosecond temporal and nanometer spatial resolutions. Here, we precisely map the collective surface charge carrier dynamics of copper indium gallium selenide NCs as a function of the surface trap states before and after surface passivation in real space and time using S-UEM. The time-resolved snapshots clearly demonstrate that the density of the trap states is significantly reduced after zinc sulfide (ZnS) shelling. Furthermore, the removal of trap states and elongation of carrier lifetime are confirmed by the increased photocurrent of the self-biased photodetector fabricated using the shelled NCs. PMID:27228321

  18. Coherent Electron Source for Ultrafast Electron Diffraction and Imaging

    Xu C.

    2013-03-01

    Full Text Available We numerically investigate the suitability of photoexcited nanotips as a source of coherent femtosecond single electron pulses for ultrafast surface-sensitive electron diffraction and non-destructive imaging with low-energy electrons. The experimental parameters for realizing hundred femtosecond time resolution are identified by evaluating the effects of vacuum dispersion and beam divergence on the temporal broadening of the electron wave packet during its propagation to the sample.

  19. Ultrafast electronic dynamics driven by nuclear motion

    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.

  20. Ultrafast electron diffraction studies of optically excited thin bismuth films

    This thesis contains work on the design and the realization of an experimental setup capable of providing sub-picosecond electron pulses for ultrafast electron diffraction experiments, and performing the study of ultrafast dynamics in bismuth after optical excitation using this setup. (orig.)

  1. Ultrafast electron diffraction studies of optically excited thin bismuth films

    Rajkovic, Ivan

    2008-10-21

    This thesis contains work on the design and the realization of an experimental setup capable of providing sub-picosecond electron pulses for ultrafast electron diffraction experiments, and performing the study of ultrafast dynamics in bismuth after optical excitation using this setup. (orig.)

  2. Ultrafast non-thermal electron dynamics in single layer graphene

    Novoselov K.S.; Geim A.K.; Nair R.R.; Polini M.; Tomadin A.; Cerullo G.; Manzoni C.; Brida D.; Milana S.; Lombardo A.; Ferrari A.C.

    2012-01-01

    We study the ultrafast dynamics of non-thermal electron relaxation in graphene upon impulsive excitation. The 10-fs resolution two color pump-probe allows us to unveil the non-equilibrium electron gas decay at early times.

  3. Challenges of 4D(ata Model for Electronic Government

    Bogdan GHILIC-MICU

    2015-01-01

    Full Text Available Social evolution pyramid, built on the foundation of the ‘90s capitalist society, lead to the emergence of the informational society – years 1990 to 2005 – and knowledge society – years 2005 to 2020. The literature starts using a new concept, a new form of association – artificial intelligence society – foreseen to be established in the next time frame. All these developments of human society and translations or leaps (most of the times apparently timeless were, are and will be possible only due to the advancing information and communications technologies. The leap to Democracy 3.0, based on information and communication technologies prompts to a radical change in the majority of the classical concepts targeting society structure and the way it is guided and controlled. Thus, concepts become electronic concepts (or e-concepts through the use of new technologies. E-concepts keep the essence of the classical principles of liberty and democracy, adding a major aspect of the new way of communication and spreading ideas between people. The main problem is to quantify, analyze and foresee the way technological changes will influence not only the economic system, but also the daily life of the individual and the society. Unfortunately (or maybe fortunately, depending on the point of view, all these evolutions and technological and social developments are as many challenges for the governments of the world. In this paper we will highlight only four of the challenges facing the governments, grouped in a structured model with the following specific concepts: Big Data, Social Data, Linked Data and Mobile Data. This is an emerging paradigm of the information and communication technology supporting national and global eGovernment projects.

  4. Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses

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

    2014-01-01

    In the last 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-fs temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules repr...

  5. Ultrafast proton coupled electron transfer (PCET) dynamics in 9-anthranol-aliphatic amine system

    Nibbering Erik T.J.; Dreyer Jens; Verma Sandeep; Ghosh Hirendra N.; Adamczyk Katrin

    2013-01-01

    Femtosecond infrared absorption studies strongly suggest that photoexcited 9-anthranol takes part in an ultrafast electron transfer (ET) reaction in electron-donating triethylamine solvent, but that ultrafast proton coupled electron transfer (PCET) occurs in diethylamine solvent.

  6. Ultrafast proton coupled electron transfer (PCET dynamics in 9-anthranol-aliphatic amine system

    Nibbering Erik T. J.

    2013-03-01

    Full Text Available Femtosecond infrared absorption studies strongly suggest that photoexcited 9-anthranol takes part in an ultrafast electron transfer (ET reaction in electron-donating triethylamine solvent, but that ultrafast proton coupled electron transfer (PCET occurs in diethylamine solvent.

  7. Optomechanical and Crystallization Phenomena Visualized with 4D Electron Microscopy: Interfacial Carbon Nanotubes on Silicon Nitride

    Flannigan, David J.; Zewail, Ahmed H.

    2010-01-01

    With ultrafast electron microscopy (UEM), we report observation of the nanoscopic crystallization of amorphous silicon nitride, and the ultrashort optomechanical motion of the crystalline silicon nitride at the interface of an adhering carbon nanotube network. The in situ static crystallization of the silicon nitride occurs only in the presence of an adhering nanotube network, thus indicating their mediating role in reaching temperatures close to 1000 °C when exposed to a train of laser pulse...

  8. Ultrafast Non-Thermal Electron Dynamics in Single Layer Graphene

    Novoselov K.S.

    2013-03-01

    Full Text Available We study the ultrafast dynamics of non-thermal electron relaxation in graphene upon impulsive excitation. The 10-fs resolution two color pump-probe allows us to unveil the non-equilibrium electron gas decay at early times.

  9. Enhanced Optoelectronic Performance of a Passivated Nanowire-Based Device: Key Information from Real-Space Imaging Using 4D Electron Microscopy.

    Khan, Jafar I; Adhikari, Aniruddha; Sun, Jingya; Priante, Davide; Bose, Riya; Shaheen, Basamat S; Ng, Tien Khee; Zhao, Chao; Bakr, Osman M; Ooi, Boon S; Mohammed, Omar F

    2016-05-01

    Managing trap states and understanding their role in ultrafast charge-carrier dynamics, particularly at surface and interfaces, remains a major bottleneck preventing further advancements and commercial exploitation of nanowire (NW)-based devices. A key challenge is to selectively map such ultrafast dynamical processes on the surfaces of NWs, a capability so far out of reach of time-resolved laser techniques. Selective mapping of surface dynamics in real space and time can only be achieved by applying four-dimensional scanning ultrafast electron microscopy (4D S-UEM). Charge carrier dynamics are spatially and temporally visualized on the surface of InGaN NW arrays before and after surface passivation with octadecylthiol (ODT). The time-resolved secondary electron images clearly demonstrate that carrier recombination on the NW surface is significantly slowed down after ODT treatment. This observation is fully supported by enhancement of the performance of the light emitting device. Direct observation of surface dynamics provides a profound understanding of the photophysical mechanisms on materials' surfaces and enables the formulation of effective surface trap state management strategies for the next generation of high-performance NW-based optoelectronic devices. PMID:26938476

  10. Ultrafast Charge Transfer Visualized by Two-Dimensional Electronic Spectroscopy

    Mančal T.; Milota F.; Hauer J; Christensson N.; Bixner O.; Lukeš V.; Kauffmann H. F.

    2013-01-01

    Two-dimensional electronic spectroscopy (2D-ES) is used to investigate ultrafast excited-state dynamics in a lutetium bisphthalocyanine dimer. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra. The combination of density matrix propagation and quantum chemical calculations results in a molecular view of the charge transfer dynamics and highlights the role of the counter-ion in providing an en...

  11. Investigations of ultrafast dynamics in electronically excited alkylbenzenes

    Maksyutenko P.

    2013-03-01

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

  12. Calculated electronic properties of ordered alloys a handbook : the element and their 3d/3d and 4d/4d alloys

    Moruzzi, VL

    1995-01-01

    This is a handbook of calculated electronic properties of elements and of 3d/3d and 4d/4d ordered alloys. The book derives the ground-state or equilibrium properties of the metallic elements in both bcc and fcc structures, and of existing and nonexisting ordered binary transition-metal alloys in CsCl, CuAu, and Cu 3 Au structures by the analysis of binding curves, or total energy vs. volume curves, calculated from first-principles augmented-spherical-wave methods. The calculated properties, energy bands along symmetry lines in the respective Brillouin zones, and the total and I-decomposed dens

  13. 4D attosecond imaging with free electrons: Diffraction methods and potential applications

    Baum, Peter, E-mail: peter.baum@lmu.de [Max-Planck-Institute of Quantum Optics, and Ludwig-Maximilians-Universitaet Muenchen, Am Coulombwall 1, 85748 Garching (Germany); Zewail, Ahmed H., E-mail: zewail@caltech.edu [Physical Biology Center for Ultrafast Science and Technology, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology, Pasadena, CA 91125 (United States)

    2009-12-10

    We consider here the extension of four-dimensional (4D) electron imaging methodology to the attosecond time domain. Specifically, we discuss the generation of attosecond electron pulses and the in situ probing with electron diffraction. The free electron pulses have a de Broglie wavelength on the order of picometers and a high degree of monochromaticity ({Delta}E/E{sub 0} {approx} 10{sup -4}); attosecond optical pulses have typically a wavelength of 20 nm and {Delta}E/E{sub 0} {approx} 0.5, where E{sub 0} is the central energy and {Delta}E is the energy bandwidth. Diffraction, and tilting of the electron pulses/specimen, permit the direct investigation of electron density changes in molecules and condensed matter. We predict the relevant changes in diffraction caused by electron density motion and give two examples as prototype applications, one that involves matter-field interaction, and the other is that of change in bonding order. This 4D imaging on the attosecond time scale is a pump-probe approach in free space and with free electrons.

  14. Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

    Weathersby, S. P. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Brown, G. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Centurion, M. [University of Nebraska-Lincoln, 855 N 16th Street, Lincoln, Nebraska 68588, USA; Chase, T. F. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Coffee, R. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Corbett, J. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Eichner, J. P. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Frisch, J. C. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Fry, A. R. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Gühr, M. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Hartmann, N. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Hast, C. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Hettel, R. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Jobe, R. K. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Jongewaard, E. N. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Lewandowski, J. R. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Li, R. K. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Lindenberg, A. M. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Makasyuk, I. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; May, J. E. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; McCormick, D. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Nguyen, M. N. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Reid, A. H. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Shen, X. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Sokolowski-Tinten, K. [University of Duisburg-Essen, Lotharstrasse 1, 47048 Duisburg, Germany; Vecchione, T. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Vetter, S. L. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Wu, J. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Yang, J. [University of Nebraska-Lincoln, 855 N 16th Street, Lincoln, Nebraska 68588, USA; Dürr, H. A. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA; Wang, X. J. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA

    2015-07-01

    Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

  15. Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

    Weathersby, S. P.; Brown, G.; Chase, T. F.; Coffee, R.; Corbett, J.; Eichner, J. P.; Frisch, J. C.; Fry, A. R.; Gühr, M.; Hartmann, N.; Hast, C.; Hettel, R.; Jobe, R. K.; Jongewaard, E. N.; Lewandowski, J. R.; Li, R. K., E-mail: lrk@slac.stanford.edu; Lindenberg, A. M.; Makasyuk, I.; May, J. E.; McCormick, D. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); and others

    2015-07-15

    Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

  16. Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory.

    Weathersby, S P; Brown, G; Centurion, M; Chase, T F; Coffee, R; Corbett, J; Eichner, J P; Frisch, J C; Fry, A R; Gühr, M; Hartmann, N; Hast, C; Hettel, R; Jobe, R K; Jongewaard, E N; Lewandowski, J R; Li, R K; Lindenberg, A M; Makasyuk, I; May, J E; McCormick, D; Nguyen, M N; Reid, A H; Shen, X; Sokolowski-Tinten, K; Vecchione, T; Vetter, S L; Wu, J; Yang, J; Dürr, H A; Wang, X J

    2015-07-01

    Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability. PMID:26233391

  17. Ultrafast electron transport across nano gaps in nanowire circuits

    Potma, Eric O. [Univ. of California, Irvine, CA (United States)

    2015-07-31

    In this Program we aim for a closer look at electron transfer through single molecules. To achieve this, we use ultrafast laser pulses to time stamp an electron tunneling event in a molecule that is connected between two metallic electrodes, while reading out the electron current. A key aspect of this project is the use of metallic substrates with plasmonic activity to efficiently manipulate the tunneling probability. The first Phase of this program is concerned with developing highly sensitive tools for the ultrafast optical manipulation of tethered molecules through the evanescent surface field of plasmonic substrates. The second Phase of the program aims to use these tools for exercising control over the electron tunneling probability.

  18. High-brightness electron beams for ultrafast electron microdiffraction and imaging

    Sun, Tianyin; Zhou, Faran; Chang, Kiseok; Tao, Zhensheng; Williams, Joe; Ruan, Chong-Yu; MSU UEM Collaboration

    Currently the ultrafast electron diffraction has achieved sub-picosecond temporal resolution and atomic resolution. However, direct ultrafast imaging of a nanometer scale specimen through coherent single-particle diffraction has not been achieved largely due to insufficient intensity when tuned to a coherence length that matches the size of the specimen under the projected phase space density. Utilizing a recently implemented high-brightness electron source with flexible optical design, we test the performance of ultrafast electron microdiffraction and coherence imaging. We demonstrate the feasibilities of single-shot microdiffraction on a single micrometer-sized domain in Highly Ordered Pyrolytic Graphite (HOPG) and coherent diffractive imaging of 10 nm scale charge-ordered domain structures in single-crystal complex materials, as validated by the measured brightness at the sample plane. These initial results show that source-limited performance even from a sub-relativistic electron beamline can drastically improve the current performance of ultrafast electron imaging and diffraction.

  19. Ultrafast electron microscopy in materials science, biology, and chemistry

    The use of pump-probe experiments to study complex transient events has been an area of significant interest in materials science, biology, and chemistry. While the emphasis has been on laser pump with laser probe and laser pump with x-ray probe experiments, there is a significant and growing interest in using electrons as probes. Early experiments used electrons for gas-phase diffraction of photostimulated chemical reactions. More recently, scientists are beginning to explore phenomena in the solid state such as phase transformations, twinning, solid-state chemical reactions, radiation damage, and shock propagation. This review focuses on the emerging area of ultrafast electron microscopy (UEM), which comprises ultrafast electron diffraction (UED) and dynamic transmission electron microscopy (DTEM). The topics that are treated include the following: (1) The physics of electrons as an ultrafast probe. This encompasses the propagation dynamics of the electrons (space-charge effect, Child's law, Boersch effect) and extends to relativistic effects. (2) The anatomy of UED and DTEM instruments. This includes discussions of the photoactivated electron gun (also known as photogun or photoelectron gun) at conventional energies (60-200 keV) and extends to MeV beams generated by rf guns. Another critical aspect of the systems is the electron detector. Charge-coupled device cameras and microchannel-plate-based cameras are compared and contrasted. The effect of various physical phenomena on detective quantum efficiency is discussed. (3) Practical aspects of operation. This includes determination of time zero, measurement of pulse-length, and strategies for pulse compression. (4) Current and potential applications in materials science, biology, and chemistry. UEM has the potential to make a significant impact in future science and technology. Understanding of reaction pathways of complex transient phenomena in materials science, biology, and chemistry will provide fundamental

  20. Ultrafast Charge Transfer Visualized by Two-Dimensional Electronic Spectroscopy

    Mančal T.

    2013-03-01

    Full Text Available Two-dimensional electronic spectroscopy (2D-ES is used to investigate ultrafast excited-state dynamics in a lutetium bisphthalocyanine dimer. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra. The combination of density matrix propagation and quantum chemical calculations results in a molecular view of the charge transfer dynamics and highlights the role of the counter-ion in providing an energetic perturbation which promotes charge transfer across the complex.

  1. Ultrafast electron diffraction with megahertz MeV electron pulses from a superconducting radio-frequency photoinjector

    Feng, L. W.; Lin, L.; Huang, S. L.; Quan, S. W.; Hao, J. K.; Zhu, F.; Wang, F.; Liu, K. X., E-mail: kxliu@pku.edu.cn [Institute of Heavy Ion Physics and State Key Laboratory of Nuclear Physics and Technology, Peking University, Beijing 100871 (China); Jiang, T.; Zhu, P. F.; Fu, F.; Wang, R.; Zhao, L.; Xiang, D., E-mail: dxiang@sjtu.edu.cn [Key Laboratory for Laser Plasmas (Ministry of Education), Department of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240 (China); IFSA Collaborative Innovation Center, Shanghai Jiao Tong University, Shanghai 200240 (China)

    2015-11-30

    We report ultrafast relativistic electron diffraction operating at the megahertz repetition rate where the electron beam is produced in a superconducting radio-frequency (rf) photoinjector. We show that the beam quality is sufficiently high to provide clear diffraction patterns from gold and aluminium samples. With the number of electrons, several orders of magnitude higher than that from a normal conducting photocathode rf gun, such high repetition rate ultrafast MeV electron diffraction may open up many new opportunities in ultrafast science.

  2. Ultrafast electron diffraction from aligned molecules

    Centurion, Martin [Univ. of Nebraska, Lincoln, NE (United States)

    2015-08-17

    The aim of this project was to record time-resolved electron diffraction patterns of aligned molecules and to reconstruct the 3D molecular structure. The molecules are aligned non-adiabatically using a femtosecond laser pulse. A femtosecond electron pulse then records a diffraction pattern while the molecules are aligned. The diffraction patterns are then be processed to obtain the molecular structure.

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

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

    2016-03-17

    Selectively capturing the ultrafast dynamics of charge carriers on materials surfaces and at interfaces is crucial to the design of solar cells and optoelectronic devices. Despite extensive research efforts over the past few decades, information and understanding about surface-dynamical processes, including carrier trapping and recombination remains extremely limited. A key challenge is to selectively map such dynamic processes, a capability that is hitherto impractical by time-resolved laser techniques, which are limited by the laser's relatively large penetration depth and consequently these techniques record mainly bulk information. Such surface dynamics can only be mapped in real space and time by applying four-dimensional (4D) scanning ultrafast electron microscopy (S-UEM), which records snapshots of materials surfaces with nanometer spatial and subpicosecond temporal resolutions. In this method, the secondary electron (SE) signal emitted from the sample's surface is extremely sensitive to the surface dynamics and is detected in real time. In several unique applications, we spatially and temporally visualize the SE energy gain and loss, the charge carrier dynamics on the surface of InGaN nanowires and CdSe single crystal and its powder film. We also discuss the mechanisms for the observed dynamics, which will be the foundation for future potential applications of S-UEM to a wide range of studies on material surfaces and device interfaces. PMID:26911313

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

    Sun, Jingya

    2016-02-25

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

  5. Ultrafast electron diffraction using an ultracold source

    M. W. van Mourik

    2014-05-01

    Full Text Available The study of structural dynamics of complex macromolecular crystals using electrons requires bunches of sufficient coherence and charge. We present diffraction patterns from graphite, obtained with bunches from an ultracold electron source, based on femtosecond near-threshold photoionization of a laser-cooled atomic gas. By varying the photoionization wavelength, we change the effective source temperature from 300 K to 10 K, resulting in a concomitant change in the width of the diffraction peaks, which is consistent with independently measured source parameters. This constitutes a direct measurement of the beam coherence of this ultracold source and confirms its suitability for protein crystal diffraction.

  6. Ultrafast dynamics of electrons at interfaces

    McNeill, Jason D.

    1999-05-03

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

  7. Adapting High Brightness Relativistic Electron Beams for Ultrafast Science

    Scoby, Cheyne Matthew

    This thesis explores the use of ultrashort bunches generated by a radiofrequency electron photoinjector driven by a femtosecond laser. Rf photoinjector technology has been developed to generate ultra high brightness beams for advanced accelerators and to drive advanced light source applications. The extremely good quality of the beams generated by this source has played a key role in the development of 4th generation light sources such as the Linac Coherent Light Source, thus opening the way to studies of materials science and biological systems with high temporal and spatial resolution. At the Pegasus Photoinjector Lab, we have developed the application of a BNL/SLAC/UCLA 1.6-cell rf photoinjector as a tool for ultrafast science in its own right. It is the aim of this work to explore the generation of ultrashort electron bunches, give descriptions of the novel ultrafast diagnostics developed to be able to characterize the electron bunch and synchronize it with a pump laser, and share some of the scientific results that were obtained with this technology at the UCLA Pegasus laboratory. This dissertation explains the requirements of the drive laser source and describes the principles of rf photoinjector design and operation necessary to produce electron bunches with an rms longitudinal length < 100 femtoseconds containing 107 - 108 electrons per bunch. In this condition, when the laser intensity is sufficiently high, multiphoton photoemission is demonstrated to be more efficient in terms of charge yield than single photon photoemission. When a short laser pulse hits the cathode the resulting beam dynamics are dominated by a strong space charge driven longitudinal expansion which leads to the creation of a nearly ideal uniformly filled ellipsoidal distribution. These beam distributions are characterized by linear space charge forces and hence by high peak brightness and small transverse emittances. This regime of operation of the RF photoinjector is also termed the

  8. Ultra-fast electron diffraction using electrons accelerated by intense femtosecond laser pulses

    We have demonstrated to use electron pulses accelerated by intense femtosecond laser pulses and self-compressed for ultrafast electron diffraction (UED). The electron pulses are generated by irradiating tightly focused terawatt femtosecond laser pulses on a polyethylene foil target, then, the pulses are compressed by using an achromatic bending magnet system. These femtosecond electron pulses have an intensity to demonstrate a single-shot diffraction pattern. (author)

  9. Probing Transient Electron Dynamics Using Ultrafast X Rays

    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.

  10. Ultrafast Electron-Ion Dynamics Near Aluminum Surfaces

    Schleife, Andre; Wells, Kai; Knewstub, Sam

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

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

    L. Piazza

    2014-01-01

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

  12. Ultrafast Spectroscopy of Delocalized Excited States of the Hydrated Electron

    Research under support of this grant has been focused on the understanding of highly delocalized ''conduction-band-like'' excited states of solvated electrons in bulk water, in water trapped in the core of reverse micelles, and in alkane solvents. We have strived in this work to probe conduction-band-like states by a variety of ultrafast spectroscopy techniques. (Most of which were developed under DOE support in a previous funding cycle.) We have recorded the optical spectrum of the hydrated electron for the first time. This was accomplished by applying a photo-detrapping technique that we had developed in a previous funding cycle, but had not yet been applied to characterize the actual spectrum. In the cases of reverse micelles, we have been investigating the potential role of conduction bands in the electron attachment process and the photoinduced detrapping, and have published two papers on this topic. Finally, we have been exploring solvated electrons in isooctane from various perspectives. All of these results strongly support the conclusion that optically accessible, highly delocalized electronic states exist in these various media

  13. Electron Pulse Compression with a Practical Reflectron Design for Ultrafast Electron Diffraction

    Wang, Yihua; Gedik, Nuh

    2013-01-01

    Ultrafast electron diffraction (UED) is a powerful method for studying time-resolved structural changes. Currently, space charge induced temporal broadening prevents obtaining high brightness electron pulses with sub-100 fs durations limiting the range of phenomena that can be studied with this technique. We review the state of the the art of UED in this respect and propose a practical design for reflectron based pulse compression which utilizes only electro-static optics and has a tunable te...

  14. Electron Pulse Compression with a Practical Reflectron Design for Ultrafast Electron Diffraction

    Wang, Yihua; Gedik, Nuh

    2011-01-01

    Ultrafast electron diffraction (UED) is a powerful method for studying time-resolved structural changes. Currently, space-charge-induced temporal broadening prevents obtaining high-brightness electron pulses with sub-100 fs durations limiting the range of phenomena that can be studied with this technique. We review the state of the art of UED in this respect and propose a practical design for reflectron-based pulse compression that utilizes only electrostatic optics and has a tunable temporal...

  15. Term structure of 4d-electron configurations and calculated spectrum in Sn-isonuclear sequence

    Theoretical calculations of term structure are carried out for the ground configurations 4dw, of atomic ions in the Sn isonuclear sequence. Atomic computations are performed to give a detailed account of the transitions in Sn+6 to Sn+13 ions. The spectrum is calculated for the most important excited configurations 4p5 4dn+1, 4dn-1 4f1, and 4dn-1 5p1 with respect to the ground configuration 4dn, with n=8-1, respectively. The importance of 4p-4d, 4d-4f, and 4d-5p transitions is stressed, as well as the need for the configuration-interaction CI treatment of the Δn=0 transitions. In the region of importance for extreme ultraviolet (EUV) lithography around 13.4nm, the strongest lines were expected to be 4dn-4p5 4dn+1 and 4dn-4dn-1 4f1

  16. Ultrafast Structural Dynamics of Tertiary Amines upon Electronic Excitation

    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.

  17. Role of electron-electron interference in ultrafast time-resolved imaging of electronic wavepackets

    Dixit, Gopal

    2013-01-01

    Ultrafast time-resolved x-ray scattering is an emerging approach to image the dynamical evolution of the electronic charge distribution during complex chemical and biological processes in real-space and real-time. Recently, the differences between semiclassical and quantum-electrodynamical (QED) theory of light-matter interaction for scattering of ultrashort x-ray pulses from the electronic wavepacket were formally demonstrated and visually illustrated by scattering patterns calculated for an electronic wavepacket in atomic hydrogen [Proc. Natl. Acad. Sci. U.S.A., {\\bf 109}, 11636 (2012)]. In this work, we present a detailed analysis of time-resolved x-ray scattering from a sample containing a mixture of non-stationary and stationary electrons within both the theories. In a many-electron system, the role of scattering interference between a non-stationary and several stationary electrons to the total scattering signal is investigated. In general, QED and semiclassical theory provide different results for the ...

  18. Ultrafast electron diffraction and direct observation of transient structures in a chemical reaction

    Cao, Jianming; Ihee, Hyotcherl; Zewail, Ahmed H.

    1999-01-01

    Ultrafast electron diffraction is a unique method for the studies of structural changes of complex molecular systems. In this contribution, we report direct ultrafast electron diffraction study of the evolution of short-lived intermediates in the course of a chemical change. Specifically, we observe the transient intermediate in the elimination reaction of 1,2-diiodotetrafluoroethane (C2F4I2) to produce the corresponding ethylene derivative by the breakage of two carbon-iodine, C---I, bonds. ...

  19. Ultrafast electron injection into photo-excited organic molecules.

    Cvetko, Dean; Fratesi, Guido; Kladnik, Gregor; Cossaro, Albano; Brivio, Gian Paolo; Venkataraman, Latha; Morgante, Alberto

    2016-08-10

    Charge transfer rates at metal/organic interfaces affect the efficiencies of devices for organic based electronics and photovoltaics. A quantitative study of electron transfer rates, which take place on the femtosecond timescale, is often difficult, especially since in most systems the molecular adsorption geometry is unknown. Here, we use X-ray resonant photoemission spectroscopy to measure ultrafast charge transfer rates across pyridine/Au(111) interfaces while also controlling the molecular orientation on the metal. We demonstrate that a bi-directional charge transfer across the molecule/metal interface is enabled upon creation of a core-exciton on the molecule with a rate that has a strong dependence on the molecular adsorption angle. Through density functional theory calculations, we show that the alignment of molecular levels relative to the metal Fermi level is dramatically altered when a core-hole is created on the molecule, allowing the lowest unoccupied molecular orbital to fall partially below the metal Fermi level. We also calculate charge transfer rates as a function of molecular adsorption geometry and find a trend that agrees with the experiment. These findings thus give insight into the charge transfer dynamics of a photo-excited molecule on a metal surface. PMID:27444572

  20. Design of a high-flux instrument for ultrafast electron diffraction and microscopy

    Filippetto, D.; Qian, H.

    2016-05-01

    We present the design and optimization of a new instrument for ultrafast electron diffraction and imaging. The proposed instrument merges the high peak current and relativistic electron energies of radio-frequency guns, with the high average electron flux of static electron microscopes, extending the beam parameter space achievable with relativistic electrons by many orders of magnitude. An immediate consequence of this work is a broader range of accessible science by using electron probes, enabling techniques as femtosecond nano-diffraction and coherent diffraction imaging, and paving the way to direct observation of ultrafast dynamics in complex and isolated samples, from nanocrystals, to nano/micro droplets and organic molecules.

  1. Ultrafast science: A multiscale modeling approach to femtosecond electron diffraction and its applications

    Portman, Jenni Minttu Eleonora

    The focus of this work is the study of processes at the edge of the current space and time resolutions. This includes both efforts in the development of an ultrafast electron microscope (UEM) and in the study of correlated electron systems that reflect measurements taken with this instrument. The development of a reliable ultrafast electron diffraction and imaging system requires a low emittance source of photoemitted electrons and an understanding of how the properties of the generated bunch depend on the photocathode properties. In order to gain more understanding of this process, we combine the so-called three-step photoemission model with N-particle electron simulations. By using the Fast Multipole Method to treat space charge effects, we are able to follow the time evolution of pulses containing over 106 electrons and investigate the role of laser fluence and extraction field on the total number of electrons that escape the surface as well as virtual cathode physics and the limits to spatio-temporal and spectroscopic resolution originating from the image charge on the surface and from the profile of the exciting laser pulse. The results of these simulations are compared to experimental images of the photoemission process collected using the shadow imaging technique. By contrasting the effect of varying surface properties (leading to expanding or pinned image charge) and laser profiles (Gaussian, uniform and elliptical) under different extraction field strengths and numbers of generated electrons, we quantify the effect of these experimental parameters on macroscopic pulse properties such as emittance, brightness (4D and 6D), coherence length and energy spread. Based on our results, we outline optimal conditions of pulse generation for UEM systems. With our knowledge of the photoemitted pulse properties, we also present our development of a design for the whole UEM column using the Analytic Gaussian model. We summarize the derivation of the equations governing

  2. Role of electron-electron interference in ultrafast time-resolved imaging of electronic wavepackets

    Ultrafast time-resolved x-ray scattering is an emerging approach to image the dynamical evolution of the electronic charge distribution during complex chemical and biological processes in real-space and real-time. Recently, the differences between semiclassical and quantum-electrodynamical (QED) theory of light-matter interaction for scattering of ultrashort x-ray pulses from the electronic wavepacket were formally demonstrated and visually illustrated by scattering patterns calculated for an electronic wavepacket in atomic hydrogen [G. Dixit, O. Vendrell, and R. Santra, Proc. Natl. Acad. Sci. U.S.A. 109, 11636 (2012)]. In this work, we present a detailed analysis of time-resolved x-ray scattering from a sample containing a mixture of non-stationary and stationary electrons within both the theories. In a many-electron system, the role of scattering interference between a non-stationary and several stationary electrons to the total scattering signal is investigated. In general, QED and semiclassical theory provide different results for the contribution from the scattering interference, which depends on the energy resolution of the detector and the x-ray pulse duration. The present findings are demonstrated by means of a numerical example of x-ray time-resolved imaging for an electronic wavepacket in helium. It is shown that the time-dependent scattering interference vanishes within semiclassical theory and the corresponding patterns are dominated by the scattering contribution from the time-independent interference, whereas the time-dependent scattering interference contribution do not vanish in the QED theory and the patterns are dominated by the scattering contribution from the non-stationary electron scattering.

  3. A brief review: Ultrafast electron diffractive voltammetry: General formalism and applications

    Chang, Kiseok; Murdick, Ryan A.; Tao, Zhensheng; Han, Tzong-Ru T.; Ruan, Chong-Yu

    2013-01-01

    We present a general formalism of ultrafast diffractive voltammetry approach as a contact-free tool to investigate the ultrafast surface charge dynamics in nanostructured interfaces. As case studies, the photoinduced surface charging processes in oxidized silicon surface and the hot electron dynamics in nanoparticle-decorated interface are examined based on the diffractive voltammetry framework. We identify that the charge redistribution processes appear on the surface, sub-surface, and vacuu...

  4. Bunch evolution study in optimization of MeV ultrafast electron diffraction

    Lu, Xianhai; Du, Yingchao; Huang, Wenhui; Tang, Chuanxiang

    2014-01-01

    Megaelectronvolt ultrafast electron diffraction (UED) is a promising detection tool for ultrafast processes. The quality of diffraction image is determined by the transverse evolution of the probe bunch. In this paper, we study the contributing terms of the emittance and space charge effects to the bunch evolution in MeV UED scheme, employing a mean-field model with an ellipsoidal distribution as well as particle tracking simulation. Small transverse dimension of the drive laser is found crit...

  5. Quantum effects in ultrafast electron transfers within cryptochromes.

    Firmino, Thiago; Mangaud, Etienne; Cailliez, Fabien; Devolder, Adrien; Mendive-Tapia, David; Gatti, Fabien; Meier, Christoph; Desouter-Lecomte, Michèle; de la Lande, Aurélien

    2016-08-21

    Cryptochromes and photolyases are flavoproteins that may undergo ultrafast charge separation upon electronic excitation of their flavin cofactors. Charge separation involves chains of three or four tryptophan residues depending on the protein of interest. The molecular mechanisms of these processes are not completely clear. In the present work we investigate the relevance of quantum effects like the occurrence of nuclear tunneling and of coherences upon charge transfer in Arabidopsis thaliana cryptochromes. The possible breakdown of the Condon approximation is also investigated. We have devised a simulation protocol based on the realization of molecular dynamics simulations on diabatic potential energy surfaces defined at the hybrid constrained density functional theory/molecular mechanics level. The outcomes of the simulations are analyzed through various dedicated kinetics schemes related to the Marcus theory that account for the aforementioned quantum effects. MD simulations also provide a basic material to define realistic model Hamiltonians for subsequent quantum dissipative dynamics. To carry out quantum simulations, we have implemented an algorithm based on the Hierarchical Equations of Motion. With this new tool in hand we have been able to model the electron transfer chain considering either two- or three-state models. Kinetic models and quantum simulations converge to the conclusion that quantum effects have a significant impact on the rate of charge separation. Nuclear tunneling involving atoms of the tryptophan redox cofactors as well as of the environment (protein atoms and water molecules) is significant. On the other hand non-Condon effects are negligible in most simulations. Taken together, the results of the present work provide new insights into the molecular mechanisms controlling charge separation in this family of flavoproteins. PMID:27427185

  6. An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

    Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha, E-mail: schaefer@ph4.physik.uni-goettingen.de; Ropers, Claus, E-mail: cropers@gwdg.de [4th Physical Institute, Solids and Nanostructures, University of Göttingen, Göttingen 37077 (Germany)

    2015-11-07

    We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy.

  7. An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

    We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy

  8. Ultrafast electron field emission from gold resonant antennas studied by two terahertz pulse experiments

    Iwaszczuk, Krzysztof; Zalkovskij, Maksim; Strikwerda, Andrew C.;

    2015-01-01

    Summary form only given. Ultrafast electron field emission from gold resonant antennas induced by strong terahertz (THz) transient is investigated using two THz pulse experiments. It is shown that UV emission from nitrogen plasma generated by liberated electrons is a good indication of the local...

  9. Observation of O+ (4P-4D0 lines in electron aurora over Svalbard

    K. Throp

    2004-09-01

    Full Text Available This work reports on observations of O+ lines in aurora over Svalbard, Norway. The Spectrographic Imaging Facility measures auroral spectra in three wavelength intervals (Hβ, N+2 1N(0,2 and N+2 1N(1,3. The oxygen ion multiplet (4639-4696Å is blended with the band. It is found that in electron aurora, the brightness of this multiplet, is on average, about 0.1 of the total brightness. A joint optical and incoherent scatter radar study of an electron aurora event shows that the ratio is enhanced when the ionisation in the upper E-layer (140-190km is significant with respect to the E-layer peak below 130km. Rayed arcs were observed on one such occasion, whereas on other occasions the auroral intensity was below the threshold of the imager. A one-dimensional electron transport model is used to estimate the cross section for production of the multiplet in electron collisions, yielding 0.18x10-18cm2.

  10. An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

    Schröder, Benjamin; Sivis, Murat; Bormann, Reiner; Schäfer, Sascha; Ropers, Claus

    2015-12-01

    We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction.

  11. An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

    Schröder, Benjamin; Sivis, Murat; Bormann, Reiner; Schäfer, Sascha; Ropers, Claus, E-mail: cropers@gwdg.de [4th Physical Institute - Solids and Nanostructures, University of Göttingen, Friedrich-Hund-Platz 1, 37077 Göttingen (Germany)

    2015-12-07

    We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction.

  12. Communication: Effects of thermionic-gun parameters on operating modes in ultrafast electron microscopy

    Erik Kieft; Karl B. Schliep; Pranav K. Suri; David J. Flannigan

    2015-01-01

    Ultrafast electron microscopes with thermionic guns and LaB6 sources can be operated in both the nanosecond, single-shot and femtosecond, single-electron modes. This has been demonstrated with conventional Wehnelt electrodes and absent any applied bias. Here, by conducting simulations using the General Particle Tracer code, we define the electron-gun parameter space within which various modes may be optimized. The properties of interest include electron collection efficiency, temporal and ene...

  13. An ultrafast nanotip electron gun triggered by grating-coupled surface plasmons

    We demonstrate multiphoton photoelectron emission from gold nanotips induced by nanofocusing surface plasmons, resonantly excited on the tip shaft by a grating coupler. The tip is integrated into an electron gun assembly, which facilitates control over the spatial emission sites and allows us to disentangle direct grating emission from plasmon-triggered apex emission. The nanoscale source size of this electron gun concept enables highly coherent electron pulses with applications in ultrafast electron imaging and diffraction

  14. The Electronic and Magnetic Properties of FCC Iron Clusters in FCC 4D Metals

    The electronic and magnetic structures of small FCC iron clusters in FCC Rh, Pd and Ag were calculated using the discrete variational method as a function of cluster size and lattice relaxation. It was found that unrelaxed iron clusters, remain ferromagnetic as the cluster sizes increase, while for relaxed clusters antiferromagnetism develops as the size increases depending on the host metal. For iron in Rh the magnetic structure changes from ferromagnetic to antiferromagnetic for clusters as small as 13 Fe atoms, whereas for Fe in Ag antiferromagnetism is exhibited for clusters of 24 Fe atoms. On the hand, for Fe in Pd the transition from ferromagnetism to antiferromagnetism occurs for clusters as large as 42 Fe atoms. The difference in the magnetic trends of these Fe clusters is related to the electronic properties of the underlying metallic matrix. The local d densities of states, the magnetic moments and hyperfine parameters are calculated in the ferromagnetic and the antiferromagnetic regions. In addition, the average local moment in iron-palladium alloys is calculated and compared to experimental results.

  15. The Electronic and Magnetic Properties of FCC Iron Clusters in FCC 4D Metals

    Elzain, M. E., E-mail: elzain@squ.edu.om; Yousif, A. A.; Rawas, A. D. Al; Gismelseed, A. M.; Widatallah, H.; Bouziani, K.; Al-Omari, I. [Sultan Qaboos University, Department of Physics, College of Science (Oman)

    2005-07-15

    The electronic and magnetic structures of small FCC iron clusters in FCC Rh, Pd and Ag were calculated using the discrete variational method as a function of cluster size and lattice relaxation. It was found that unrelaxed iron clusters, remain ferromagnetic as the cluster sizes increase, while for relaxed clusters antiferromagnetism develops as the size increases depending on the host metal. For iron in Rh the magnetic structure changes from ferromagnetic to antiferromagnetic for clusters as small as 13 Fe atoms, whereas for Fe in Ag antiferromagnetism is exhibited for clusters of 24 Fe atoms. On the hand, for Fe in Pd the transition from ferromagnetism to antiferromagnetism occurs for clusters as large as 42 Fe atoms. The difference in the magnetic trends of these Fe clusters is related to the electronic properties of the underlying metallic matrix. The local d densities of states, the magnetic moments and hyperfine parameters are calculated in the ferromagnetic and the antiferromagnetic regions. In addition, the average local moment in iron-palladium alloys is calculated and compared to experimental results.

  16. The APSEL4D Monolithic Active Pixel Sensor and its Usage in a Single Electron Interference Experiment

    Alberghi, Gian Luigi

    We have realized a Data Acquisition chain for the use and characterization of APSEL4D, a 32 x 128 Monolithic Active Pixel Sensor, developed as a prototype for frontier experiments in high energy particle physics. In particular a transition board was realized for the conversion between the chip and the FPGA voltage levels and for the signal quality enhancing. A Xilinx Spartan-3 FPGA was used for real time data processing, for the chip control and the communication with a Personal Computer through a 2.0 USB port. For this purpose a firmware code, developed in VHDL language, was written. Finally a Graphical User Interface for the online system monitoring, hit display and chip control, based on windows and widgets, was realized developing a C++ code and using Qt and Qwt dedicated libraries. APSEL4D and the full acquisition chain were characterized for the first time with the electron beam of the transmission electron microscope and with 55Fe and 90Sr radioactive sources. In addition, a beam test was performed at ...

  17. Ultrafast electronic relaxation of excited state vitamin B12 in the gas phase

    The time evolution of electronically excited vitamin B12 (cyanocobalamin) has been observed for the first time in the gas phase. It reveals an ultrafast decay to a state corresponding to metal excitation. This decay is interpreted as resulting from a ring to metal electron transfer. This opens the observation of the excited state of other complex biomimetic systems in the gas phase, the key to the characterisation of their complex evolution through excited electronic states

  18. Impact of ultrafast electronic damage in single particle x-ray imaging experiments

    Lorenz, U.; Kabachnik, Nikolay; Weckert, E.; Vartanyants, I. A.

    2012-01-01

    In single particle coherent x-ray diffraction imaging experiments, performed at x-ray free-electron lasers (XFELs), samples are exposed to intense x-ray pulses to obtain single-shot diffraction patterns. The high intensity induces electronic dynamics on the femtosecond time scale in the system, which can reduce the contrast of the obtained diffraction patterns and adds an isotropic background. We quantify the degradation of the diffraction pattern from ultrafast electronic damage by performin...

  19. Ultrafast electron injection at the cationic porphyrin-graphene interface assisted by molecular flattening

    Aly, Shawkat Mohammede

    2014-01-01

    The steady-state and femtosecond (fs) time-resolved data clearly demonstrate that the charge transfer (CT) process at the porphyrin-graphene carboxylate (GC) interfaces can be tuned from zero to very sufficient and ultrafast by changing the electronic structure of the meso unit and the redox properties of the porphyrin cavity. This journal is © the Partner Organisations 2014.

  20. Mechanical and Electronic Properties of Ferromagnetic GaMnAs Using Ultrafast Coherent Acoustic Phonons

    Qi, J; Yan, J. A.; Park, H.; Steigerwald, A.; Xu, Y; Gilbert, S. N.; Liu, X.; J. K. Furdyna; Pantelides, S.T.; Tolk, N.

    2008-01-01

    Ultrafast two-color pump-probe measurements, involving coherent acoustic phonon (CAP) waves, have provided information simultaneously on the mechanical properties and on the electronic structure of ferromagnetic GaMnAs. The elastic constant C11 of Ga1-xMnxAs (0.03

  1. Bunch evolution study in optimization of MeV ultrafast electron diffraction

    Lu, Xianhai; Huang, Wenhui; Tang, Chuanxiang

    2014-01-01

    Megaelectronvolt ultrafast electron diffraction (UED) is a promising detection tool for ultrafast processes. The quality of diffraction image is determined by the transverse evolution of the probe bunch. In this paper, we study the contributing terms of the emittance and space charge effects to the bunch evolution in MeV UED scheme, employing a mean-field model with an ellipsoidal distribution as well as particle tracking simulation. Small transverse dimension of the drive laser is found critical to improve the reciprocal resolution, exploiting both smaller emittance and larger transverse bunch size before the solenoid. The degradation of reciprocal spatial resolution caused by the space charge effects should be carefully controlled.

  2. A brief review: Ultrafast electron diffractive voltammetry: General formalism and applications

    Chang, Kiseok; Tao, Zhensheng; Han, Tzong-Ru T; Ruan, Chong-Yu

    2013-01-01

    We present a general formalism of ultrafast diffractive voltammetry approach as a contact-free tool to investigate the ultrafast surface charge dynamics in nanostructured interfaces. As case studies, the photoinduced surface charging processes in oxidized silicon surface and the hot electron dynamics in nanoparticle-decorated interface are examined based on the diffractive voltammetry framework. We identify that the charge redistribution processes appear on the surface, sub-surface, and vacuum levels when driven by intense femtosecond laser pulses. To elucidate the voltammetry contribution from different sources, we perform controlled experiments using shadow imaging techniques and N-particle simulations to aid the investigation of the photovoltage dynamics in the presence of pho- toemission. We show that voltammetry contribution associated with photoemission has a long decay tail and plays a more visible role in the nanosecond timescale, whereas the ultrafast voltammetry are dominated by local charge transfe...

  3. Beyond Vibrationally Mediated Electron Transfer: Coherent Phenomena Induced by Ultrafast Charge Separation

    Huber, Robert; Moser, Jacques E; Grätzel, Michael; Wachtveitl, Josef

    2016-01-01

    Wave packet propagation succeeding electron transfer (ET) from alizarin dye molecules into the nanocrystalline TiO2 semiconductor has been studied by ultrafast transient absorption spectroscopy. Due to the ultrafast time scale of the ET reaction of about 6 fs the system shows substantial differences to molecular ET systems. We show that the ET process is not mediated by molecular vibrations and therefore classical ET theories lose their applicability. Here the ET reaction itself prepares a vibrational wave packet and not the electromagnetic excitation by the laser pulse. Furthermore, the generation of phonons during polaron formation in the TiO2 lattice is observed in real time for this system. The presented investigations enable an unambiguous assignment of the involved photoinduced mechanisms and can contribute to a corresponding extension of molecular ET theories to ultrafast ET systems like alizarin/TiO2.

  4. Real-time observation of ultrafast electron injection at graphene–Zn porphyrin interfaces

    Masih, Dilshad

    2015-02-25

    We report on the ultrafast interfacial electron transfer ( ET) between zinc( II) porphyrin ( ZnTMPyP) and negatively charged graphene carboxylate ( GC) using state- of- the- art femtosecond laser spectroscopy with broadband capabilities. The steady- state interaction between GC and ZnTMPyP results in a red- shifted absorption spectrum, providing a clear indication for the binding affinity between ZnTMPyP and GC via electrostatic and p- p stacking interactions. Ultrafast transient absorption ( TA) spectra in the absence and presence of three different GC concentrations reveal ( i) the ultrafast formation of singlet excited ZnTMPyP*, which partially relaxes into a long- lived triplet state, and ( ii) ET from the singlet excited ZnTMPyP* to GC, forming ZnTMPyP + and GC , as indicated by a spectral feature at 650- 750 nm, which is attributed to a ZnTMPyP radical cation resulting from the ET process.

  5. Structural, elastic, magnetic and electronic properties of 4d perovskite CaTcO3: a DFT+U investigation

    Zhang, Wei; Tong, Peiqing

    2012-05-01

    The structural, elastic, magnetic and electronic properties of 4d high Neél temperature perovskite (Pv) CaTcO3 have been studied using density functional theory plus the Hubbard U (DFT+U) method. The degree of correlations of CaTcO3 is determined with a reasonable value of U. The compound is found to be an indirect band gap semiconductor with G-type antiferromagnetic ordering and large superexchange interactions. Large anisotropic compression behavior is found that is much alike the case of Pv CaIrO3 reported by recent high pressure experiment. The b and c axes decrease linearly with pressure whereas the a axis nearly keeps constant and even slightly expands after ˜23 GPa. Finally, we predict the single crystal elastic constants and investigate the polycrystalline elastic properties.

  6. 4d electronic structure analysis of ruthenium in the perovskite oxides by Ru Κ- and L-edge XAS

    The 4d electronic structure of ruthenium in the perovskite oxides, La2MRuIVO6) (M = Zn, Mg, and Li) and (Ba2YRuVO6), has been investigated by the Ru Κ-and L-edge XANES and EXAFS analyses. Such X-ray absorption spectroscopic results clarify that the Ru-IV (d4) and RuV (d3) ions are stabilized in nearly regular Oh site. Comparing the Ru L-edge XANES spectra of perovskites containing isovalent ruthenium, it has been found that the t2g state is mainly influenced by A site cation, whereas the eg is mainly affected by neighboring B site cation. The experimental EXAFS spectra in the range of R ≤ ∼ to 4.5 Angstrom are well reproduced by abinitio calculation based on crystallographic data, which supports the long-range structure presented by Rietveld refinement. (au)

  7. Ultrafast carrier dynamics in tetrahedral amorphous carbon: carrier trapping versus electron-hole recombination

    We report the investigation of the ultrafast carrier dynamics in thin tetrahedral amorphous carbon films by means of femtosecond time-resolved reflectivity. We estimated the electron-phonon relaxation time of a few hundred femtoseconds and we observed that under low optical excitation photo-generated carriers decay according to two distinct mechanisms attributed to trapping by defect states and direct electron-hole recombination. With high excitation, when photo-carrier and trap densities are comparable, a unique temporal evolution develops, as the time dependence of the trapping process becomes degenerate with the electron-hole recombination. This experimental evidence highlights the role of defects in the ultrafast electronic dynamics and is not specific to this particular form of carbon, but has general validity for amorphous and disordered semiconductors

  8. Phonon-phonon interactions in photoexcited graphite studied by ultrafast electron diffraction

    Harb, M.; Enquist, H.; Jurgilaitis, A.; Tuyakova, F. T.; Obraztsov, A. N.; Larsson, J.

    2016-03-01

    We investigated phonon-phonon interactions in photoexcited single-crystalline graphite by ultrafast electron diffraction. Transient electron diffraction profiles from a 35 nm graphite film were observed following laser excitation. Changes in intensities of diffraction spots revealed a two-exponential relaxation process with decay of strongly coupled optical phonons, and the slow relaxation process to redistribution of phonon energy to the equilibrium thermal distribution.

  9. The electronic structure of lanthanide doped compounds with 3d, 4d, 5d, or 6d conduction band states

    Dorenbos, Pieter, E-mail: p.dorenbos@tudelft.nl

    2014-07-01

    The chemical shift model of electronic binding energies will be applied to the lanthanides in T O{sub 2} and MT O{sub 3} compounds where T is the cation Ti{sup 4+}, Zr{sup 4+}, Ce{sup 4+}, Hf{sup 4+}, or Th{sup 4+} and M is the alkaline earth cation Ba{sup 2+}, Sr{sup 2+}, or Ca{sup 2+}. As input, data from lanthanide spectroscopy will be used to generate the binding energies of electrons in all lanthanide impurity states and in the valence band and conduction band states of the host compound. In these compounds the bottom of the conduction band has a strong nd-orbital character (n=3, 4, 5, and 6 for titanates, zirconates, hafnates, and thorates, respectively). Electronic structure diagrams are determined that show the valence band and conduction band energy together with all lanthanide impurity level energies relative to the vacuum level. They reveal clear trends when n increases that has profound consequences for the lanthanide luminescence properties. - Highlights: • Electronic level schemes with all divalent and all trivalent lanthanide impurity states in titanate, zirconate, hafnate, and thorate compounds are presented. • Level schemes can be compared with each other with respect to a common energy reference, i.e., the energy of an electron at rest in vacuum. • It is found that the conduction band energy systematically increases when its character changes from 3d, to 4d, to 5d, to 6d-orbital type.

  10. Ultrafast Photoinduced Electron Transfer in a π-Conjugated Oligomer/Porphyrin Complex

    Aly, Shawkat Mohammede

    2014-10-02

    Controlling charge transfer (CT), charge separation (CS), and charge recombination (CR) at the donor-acceptor interface is extremely important to optimize the conversion efficiency in solar cell devices. In general, ultrafast CT and slow CR are desirable for optimal device performance. In this Letter, the ultrafast excited-state CT between platinum oligomer (DPP-Pt(acac)) as a new electron donor and porphyrin as an electron acceptor is monitored for the first time using femtosecond (fs) transient absorption (TA) spectroscopy with broad-band capability and 120 fs temporal resolution. Turning the CT on/off has been shown to be possible either by switching from an organometallic oligomer to a metal-free oligomer or by controlling the charge density on the nitrogen atom of the porphyrin meso unit. Our time-resolved data show that the CT and CS between DPP-Pt(acac) and cationic porphyrin are ultrafast (approximately 1.5 ps), and the CR is slow (ns time scale), as inferred from the formation and the decay of the cationic and anionic species. We also found that the metallic center in the DPP-Pt(acac) oligomer and the positive charge on the porphyrin are the keys to switching on/off the ultrafast CT process.

  11. Ultrafast quenching of tryptophan fluorescence in proteins: Interresidue and intrahelical electron transfer

    Quenching of tryptophan fluorescence in proteins has been critical to the understanding of protein dynamics and enzyme reactions using tryptophan as a molecular optical probe. We report here our systematic examinations of potential quenching residues with more than 40 proteins. With site-directed mutation, we placed tryptophan to desired positions or altered its neighboring residues to screen quenching groups among 20 amino acid residues and of peptide backbones. With femtosecond resolution, we observed the ultrafast quenching dynamics within 100 ps and identified two ultrafast quenching groups, the carbonyl- and sulfur-containing residues. The former is glutamine and glutamate residues and the later is disulfide bond and cysteine residue. The quenching by the peptide-bond carbonyl group as well as other potential residues mostly occurs in longer than 100 ps. These ultrafast quenching dynamics occur at van der Waals distances through intraprotein electron transfer with high directionality. Following optimal molecular orbital overlap, electron jumps from the benzene ring of the indole moiety in a vertical orientation to the LUMO of acceptor quenching residues. Molecular dynamics simulations were invoked to elucidate various correlations of quenching dynamics with separation distances, relative orientations, local fluctuations and reaction heterogeneity. These unique ultrafast quenching pairs, as recently found to extensively occur in high-resolution protein structures, may have significant biological implications

  12. Forward acceleration and generation of femtosecond, megaelectronvolt electron beams by an ultrafast intense laser pulse

    Xiaofang wang(王晓方); Quandong Wang(汪权东); Baifei Shen(沈百飞)

    2003-01-01

    We present a new mechanism of energy gain of electrons accelerated by a laser pulse. It is shown that when the intensity of an ultrafast intense laser pulse decreases rapidly along the direction of propagation, electrons leaving the pulse experience an action of ponderomotive deceleration at the descending part of a lower-intensity laser field than acceleration at the ascending part of a high-intensity field, thus gain net energy from the pulse and move directly forward. By means of such a mechanism, a megaelectronvolt electron beam with a bunch length shorter than 100 fs could be realized with an ultrafast (≤30 fs),intense (>1019 W/cm2) laser pulse.

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

    Sun, Jingya

    2015-09-14

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

  14. Absolute measurement of the ultrafast nonlinear electronic and rovibrational response in H$_2$ and D$_2$

    Wahlstrand, J K; Cheng, Y -H; Palastro, J P; Milchberg, H M

    2015-01-01

    The electronic, rotational, and vibrational components of the ultrafast optical nonlinearity in H$_2$ and D$_2$ are measured directly and absolutely at intensities up to the ionization threshold of $\\sim$10$^{14}$ W/cm$^2$. As the most basic nonlinear interactions of the simplest molecules exposed to high fields, these results constitute a benchmark for high field laser-matter theory and simulation.

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

    L. Piazza; Ma, C.; H. X. Yang; 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, ...

  16. Realizing Ultrafast Electron Pulse Self-Compression by Femtosecond Pulse Shaping Technique.

    Qi, Yingpeng; Pei, Minjie; Qi, Dalong; Yang, Yan; Jia, Tianqing; Zhang, Shian; Sun, Zhenrong

    2015-10-01

    Uncorrelated position and velocity distribution of the electron bunch at the photocathode from the residual energy greatly limit the transverse coherent length and the recompression ability. Here we first propose a femtosecond pulse-shaping method to realize the electron pulse self-compression in ultrafast electron diffraction system based on a point-to-point space-charge model. The positively chirped femtosecond laser pulse can correspondingly create the positively chirped electron bunch at the photocathode (such as metal-insulator heterojunction), and such a shaped electron pulse can realize the self-compression in the subsequent propagation process. The greatest advantage for our proposed scheme is that no additional components are introduced into the ultrafast electron diffraction system, which therefore does not affect the electron bunch shape. More importantly, this scheme can break the limitation that the electron pulse via postphotocathode static compression schemes is not shorter than the excitation laser pulse due to the uncorrelated position and velocity distribution of the initial electron bunch. PMID:26722884

  17. Nanowires: Enhanced Optoelectronic Performance of a Passivated Nanowire-Based Device: Key Information from Real-Space Imaging Using 4D Electron Microscopy (Small 17/2016).

    Khan, Jafar I; Adhikari, Aniruddha; Sun, Jingya; Priante, Davide; Bose, Riya; Shaheen, Basamat S; Ng, Tien Khee; Zhao, Chao; Bakr, Osman M; Ooi, Boon S; Mohammed, Omar F

    2016-05-01

    Selective mapping of surface charge carrier dynamics of InGaN nanowires before and after surface passivation with octadecylthiol (ODT) is reported by O. F. Mohammed and co-workers on page 2313, using scanning ultrafast electron microscopy. In a typical experiment, the 343 nm output of the laser beam is used to excite the microscope tip to generate pulsed electrons for probing, and the 515 nm output is used as a clocking excitation pulse to initiate dynamics. Time-resolved images demonstrate clearly that carrier recombination is significantly slowed after ODT treatment, which supports the efficient removal of surface trap states. PMID:27124006

  18. Ultrafast electronic dynamics in laser-excited crystalline bismuth

    Chekalin S.

    2013-03-01

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

  19. Electron diffraction using ultrafast electron bunches from a laser-wakefield accelerator at kHz repetition rate

    He, Z.-H.; Thomas, A. G. R.; Beaurepaire, B.; Nees, J. A.; Hou, B.; Malka, V.; Krushelnick, K.; Faure, J.

    2013-02-01

    We show that electron bunches in the 50-100 keV range can be produced from a laser wakefield accelerator using 10 mJ, 35 fs laser pulses operating at 0.5 kHz. It is shown that using a solenoid magnetic lens, the electron bunch distribution can be shaped. The resulting transverse and longitudinal coherence is suitable for producing diffraction images from a polycrystalline 10 nm aluminum foil. The high repetition rate, the stability of the electron source, and the fact that its uncorrelated bunch duration is below 100 fs make this approach promising for the development of sub-100 fs ultrafast electron diffraction experiments.

  20. Electron diffraction using ultrafast electron bunches from a laser-wakefield accelerator at kHz repetition rate

    We show that electron bunches in the 50–100 keV range can be produced from a laser wakefield accelerator using 10 mJ, 35 fs laser pulses operating at 0.5 kHz. It is shown that using a solenoid magnetic lens, the electron bunch distribution can be shaped. The resulting transverse and longitudinal coherence is suitable for producing diffraction images from a polycrystalline 10 nm aluminum foil. The high repetition rate, the stability of the electron source, and the fact that its uncorrelated bunch duration is below 100 fs make this approach promising for the development of sub-100 fs ultrafast electron diffraction experiments.

  1. Ultrafast nanoelectronics: steering electrons in infrared near-fields (Presentation Recording)

    Herink, Georg; Ropers, Claus

    2015-09-01

    Plasmonic nanostructures can break the diffraction limit and confine optical fields on the nanoscale. The coupling of intense femtosecond transients to the apex of metallic nanotips enables ultrafast electron point sources which find applications in ultrafast electron microscopy and time-resolved diffraction instruments. In this contribution, we demonstrate the impact of near-field localization onto strong-field photoemission and present the control of electron trajectories via the momentary electric near-field. The photoemission dynamics at single gold and tungsten nanotips are experimentally studied over a broad range of excitation frequencies, spanning from 1 - 400 Terahertz (THz). The transition from oscillatory electron acceleration to a field-driven interaction is presented as a result of intense, long-wavelength and localized excitation. The high field enhancement at lower frequencies is demonstrated to induce localized field emission from a nanotip with moderate incident fields as provided by table-top THz sources. Such THz-induced cold field emission can be used, e.g., for the temporal tracking of optically excited hot-electron dynamics in nanostructures. Moreover, the field-driven electron acceleration in the enhanced THz near-field is employed in a pump-probe scheme to temporally map the local THz-response of the nanostructure by projecting the momentary apex near-field onto the kinetic energy of femtosecond electron pulses. Besides the electrical characterization of nanostructures at THz-frequencies, the temporally and spatially confined interaction of free electrons with ultrashort near-fields is expected to enable a novel class of ultrafast vacuum micro- and nanoelectronic devices, and first applications are presented in this talk.

  2. Bunch evolution study in optimization of MeV ultrafast electron diffraction

    Lu, Xian-Hai; Du, Ying-Chao; Huang, Wen-Hui; Tang, Chuan-Xiang

    2014-12-01

    Megaelectronvolt ultrafast electron diffraction (UED) is a promising detection tool for ultrafast processes. The quality of diffraction image is determined by the transverse evolution of the probe bunch. In this paper, we study the contributing terms of the emittance and space charge effects to the bunch evolution in the MeV UED scheme, employing a mean-field model with an ellipsoidal distribution as well as particle tracking simulation. The small transverse dimension of the drive laser is found to be critical to improve the reciprocal resolution, exploiting both smaller emittance and larger transverse bunch size before the solenoid. The degradation of the reciprocal spatial resolution caused by the space charge effects should be carefully controlled.

  3. 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

  4. Ultrafast Electron Transfer in Solutions Studied by Picosecond Pulse Radiolysis

    Ma, Jun

    2015-01-01

    The interaction of energetic particles with water results in the excitation and ionization of water molecules. The ionization process refers to the generation of the excess electrons detached from their parent molecules and leaving behind the positive hole (denoted as H₂O•⁺). This occurs on the timescale of an electronic transition ~10⁻¹⁵ s. The earliest chemical processes of H₂O•⁺ and excess electron towards other matter followed water ionizing in bulk still remain relative little known and ...

  5. Ultrafast electron diffraction from non-equilibrium phonons in femtosecond laser heated Au films

    Chase, T. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Department of Applied Physics, Stanford University, Stanford, California 94305 (United States); Trigo, M.; Reid, A. H.; Dürr, H. A. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Li, R.; Vecchione, T.; Shen, X.; Weathersby, S.; Coffee, R.; Hartmann, N.; Wang, X. J. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Reis, D. A. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Department of Applied Physics, Stanford University, Stanford, California 94305 (United States); PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States)

    2016-01-25

    We use ultrafast electron diffraction to detect the temporal evolution of non-equilibrium phonons in femtosecond laser-excited ultrathin single-crystalline gold films. From the time-dependence of the Debye-Waller factor, we extract a 4.7 ps time-constant for the increase in mean-square atomic displacements. The observed increase in the diffuse scattering intensity demonstrates that the energy transfer from laser-heated electrons to phonon modes near the X and K points in the Au fcc Brillouin zone proceeds with timescales of 2.3 and 2.9 ps, respectively, faster than the Debye-Waller average mean-square displacement.

  6. Ultrafast electron diffraction from non-equilibrium phonons in femtosecond laser heated Au films

    We use ultrafast electron diffraction to detect the temporal evolution of non-equilibrium phonons in femtosecond laser-excited ultrathin single-crystalline gold films. From the time-dependence of the Debye-Waller factor, we extract a 4.7 ps time-constant for the increase in mean-square atomic displacements. The observed increase in the diffuse scattering intensity demonstrates that the energy transfer from laser-heated electrons to phonon modes near the X and K points in the Au fcc Brillouin zone proceeds with timescales of 2.3 and 2.9 ps, respectively, faster than the Debye-Waller average mean-square displacement

  7. Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators

    Matlis, N. H.; Bakeman, M.; Geddes, C. G. R.; Gonsalves, T.; Lin, C.; Nakamura, K.; Osterhoff, J.; Plateau, G. R.; Schroeder, C. B.; Shiraishi, S.; Sokollik, T.; van Tilborg, J.; Toth, Cs.; Leemans, W. P.

    2010-06-01

    We present an overview of diagnostic techniques for measuring key parameters of electron bunches from Laser Plasma Accelerators (LPAs). The diagnostics presented here were chosen because they highlight the unique advantages (e.g., diverse forms of electromagnetic emission) and difficulties (e.g., shot-to-shot variability) associated with LPAs. Non destructiveness and high resolution (in space and time and energy) are key attributes that enable the formation of a comprehensive suite of simultaneous diagnostics which are necessary for the full characterization of the ultrashort, but highly-variable electron bunches from LPAs.

  8. Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators

    We present an overview of diagnostic techniques for measuring key parameters of electron bunches from Laser Plasma Accelerators (LPAs). The diagnostics presented here were chosen because they highlight the unique advantages (e.g., diverse forms of electromagnetic emission) and difficulties (e.g., shot-to-shot variability) associated with LPAs. Non destructiveness and high resolution (in space and time and energy) are key attributes that enable the formation of a comprehensive suite of simultaneous diagnostics which are necessary for the full characterization of the ultrashort, but highly-variable electron bunches from LPAs.

  9. Ultrafast Hot Electron Induced Phase Transitions in Vanadium Dioxide

    Haglund R. F.

    2013-03-01

    Full Text Available The Au/Cr/VO2/Si system was investigated in pump–probe experiments. Hot-electrons generated in the Au were found to penetrate into the underlying VO2 and couple with its lattice inducing a semiconductor-to-metal phase transition in ~2 picoseconds.

  10. Imaging interatomic electron current in crystals with ultrafast resonant x-ray scattering

    Popova-Gorelova, Daria

    2015-01-01

    We demonstrate how the technique of ultrafast resonant x-ray scattering can be applied to imaging dynamics of electronic wave packets in crystals. We study scattering patterns from crystals with electron dynamics in valence bands taking into account that inelastic and elastic scattering events induced by a broad-band probe pulse cannot be separated through the spectroscopy of the scattered photon. As a result, scattering patterns are not determined by the structure factor at the time of measurement, but can encode the instantaneous electron current between scattering atoms. We provide examples of how the interatomic electron current in a periodic structure can be extracted from a single scattering pattern by considering valence electron hole motion in (KBr)$_{108}$ and Ge$_{83}$ clusters.

  11. Imaging instantaneous electron flow with ultrafast resonant x-ray scattering

    Popova-Gorelova, Daria

    2015-01-01

    We propose a novel way to image dynamical properties of nonstationary electron systems using ultrafast resonant x-ray scattering. Employing a rigorous theoretical analysis within the framework of quantum electrodynamics, we demonstrate that a single scattering pattern from a nonstationary electron system encodes the instantaneous interatomic electron current in addition to the structural information usually obtained by resonant x-ray scattering from stationary systems. Thus, inelastic contributions that are indistinguishable from elastic processes induced by a broadband probe pulse, instead of being a concern, serve as an advantage for time-resolved resonant x-ray scattering. Thereby, we propose an approach combining elastic and inelastic resonant x-ray scattering for imaging dynamics of nonstationary electron systems in both real space and real time. In order to illustrate its power, we show how it can be applied to image the electron hole current in an ionized diatomic molecule.

  12. Electron-phonon scattering dynamics in ferromagnetic metals and their influence on ultrafast demagnetization processes

    Essert, Sven; Schneider, Hans Christian

    2011-12-01

    We theoretically investigate spin-dependent carrier dynamics due to the electron-phonon interaction after ultrafast optical excitation in ferromagnetic metals. We calculate the electron-phonon matrix elements including the spin-orbit interaction in the electronic wave functions and the interaction potential. Using the matrix elements in Boltzmann scattering integrals, the momentum-resolved carrier distributions are obtained by solving their equation of motion numerically. We find that the optical excitation with realistic laser intensities alone leads to a negligible magnetization change, and that the demagnetization due to electron-phonon interaction is mostly due to hole scattering. Importantly, the calculated demagnetization quenching due to this Elliot-Yafet-type depolarization mechanism is not large enough to explain the experimentally observed result. We argue that the ultrafast demagnetization of ferromagnets does not occur exclusively via an Elliott-Yafet type process, i.e., scattering in the presence of the spin-orbit interaction, but is influenced to a large degree by a dynamical change of the band structure, i.e., the exchange splitting.

  13. On the ultrafast kinetics of the energy and electron transfer reactions in photosystem I

    Slavov, Chavdar Lyubomirov

    2009-07-09

    The subject of the current work is one of the main participants in the light-dependent phase of oxygenic photosynthesis, Photosystem I (PS I). This complex carries an immense number of cofactors: chlorophylls (Chl), carotenoids, quinones, etc, which together with the protein entity exhibit several exceptional properties. First, PS I has an ultrafast light energy trapping kinetics with a nearly 100% quantum efficiency. Secondly, both of the electron transfer branches in the reaction center are suggested to be active. Thirdly, there are some so called 'red' Chls in the antenna system of PS I, absorbing light with longer wavelengths than the reaction center. These 'red' Chls significantly modify the trapping kinetics of PS I. The purpose of this thesis is to obtain better understanding of the above-mentioned, specific features of PS I. This will not merely cast more light on the mechanisms of energy and electron transfer in the complex, but also will contribute to the future developments of optimized artificial light-harvesting systems. In the current work, a number of PS I complexes isolated from different organisms (Thermosynechococcus elongatus, Chlamydomonas reinhardtii, Arabidopsis thaliana) and possessing distinctive features (different macroorganisation, monomers, trimers, monomers with a semibelt of peripheral antenna attached; presence of 'red' Chls) is investigated. The studies are primarily focused on the electron transfer kinetics in each of the cofactor branches in the PS I reaction center, as well as on the effect of the antenna size and the presence of 'red' Chls on the trapping kinetics of PS I. These aspects are explored with the help of several ultrafast optical spectroscopy methods: (i) time-resolved fluorescence ? single photon counting and synchroscan streak camera; and (ii) ultrafast transient absorption. Physically meaningful information about the molecular mechanisms of the energy trapping in PS I is

  14. Ultrafast Electron Trapping in Ligand-Exchanged Quantum Dot Assemblies

    Kikkawa, J. M.; Turk, M. E.; Vora, P. M.; Fafarman, A. T.; Diroll, B. T.; Murray, C. B.; Kagan, C. R.

    2015-03-01

    We use time-integrated and time-resolved photoluminescence and absorption to characterize the low-temperature (10 K) optical properties of CdSe quantum dot (QD) solids with different ligand and annealing preparation. Close-packed CdSe quantum dot solids are prepared with native aliphatic ligands and with thiocyanate with and without thermal annealing. Using sub-picosecond, broadband time-resolved photoluminescence and absorption, we find that ligand exchange increases the rate of carrier surface trapping. We further determine that holes within the QD core, rather than electrons, can bleach the band-edge transition in these samples at low temperature, a finding that comes as a surprise given what is known about the surface treatment in these QDs. We find that our ligand treatments lead to faster electron trapping to the quantum dot surface, a greater proportion of surface photoluminescence, and an increased rate of nonradiative decay due to enhanced interparticle coupling upon exchange and annealing. All aspects of this work supported by the U.S. Department of Energy Office of Basic Energy Sciences, Division of Materials Science and Engineering, under Award No. DE-SC0002158.

  15. Communication: Effects of thermionic-gun parameters on operating modes in ultrafast electron microscopy.

    Kieft, Erik; Schliep, Karl B; Suri, Pranav K; Flannigan, David J

    2015-09-01

    Ultrafast electron microscopes with thermionic guns and LaB6 sources can be operated in both the nanosecond, single-shot and femtosecond, single-electron modes. This has been demonstrated with conventional Wehnelt electrodes and absent any applied bias. Here, by conducting simulations using the General Particle Tracer code, we define the electron-gun parameter space within which various modes may be optimized. The properties of interest include electron collection efficiency, temporal and energy spreads, and effects of laser-pulse duration incident on the LaB6 source. We find that collection efficiencies can reach 100% for all modes, despite there being no bias applied to the electrode. PMID:26798820

  16. Communication: Effects of thermionic-gun parameters on operating modes in ultrafast electron microscopy

    Erik Kieft

    2015-09-01

    Full Text Available Ultrafast electron microscopes with thermionic guns and LaB6 sources can be operated in both the nanosecond, single-shot and femtosecond, single-electron modes. This has been demonstrated with conventional Wehnelt electrodes and absent any applied bias. Here, by conducting simulations using the General Particle Tracer code, we define the electron-gun parameter space within which various modes may be optimized. The properties of interest include electron collection efficiency, temporal and energy spreads, and effects of laser-pulse duration incident on the LaB6 source. We find that collection efficiencies can reach 100% for all modes, despite there being no bias applied to the electrode.

  17. Impact of ultrafast electronic damage in single particle x-ray imaging experiments

    Lorenz, U; Weckert, E; Vartanyants, I A

    2012-01-01

    In single particle coherent x-ray diffraction imaging experiments, performed at x-ray free-electron lasers (XFELs), samples are exposed to intense x-ray pulses to obtain single-shot diffraction patterns. The high intensity induces electronic dynamics on the femtosecond time scale in the system, which can reduce the contrast of the obtained diffraction patterns and adds an isotropic background. We quantify the degradation of the diffraction pattern from ultrafast electronic damage by performing simulations on a biological sample exposed to x-ray pulses with different parameters. We find that the contrast is substantially reduced and the background is considerably strong only if almost all electrons are removed from their parent atoms. This happens at fluences of at least one order of magnitude larger than provided at currently available XFEL sources.

  18. Ultrafast Coherent Diffraction Imaging with X-ray Free-Electron Lasers

    The ultrafast pulses from X-ray free-electron lasers will enable imaging of non-periodic objects at near-atomic resolution [1, Neutze]. These objects could include single molecules, protein complexes, or virus particles. The specimen would be completely destroyed by the pulse in a Coulomb explosion, but that destruction will only happen after the pulse. The scattering from the sample will give structural information about the undamaged object. There are many technical challenges that must be addressed before carrying out such experiments at an XFEL, which we are doing so with experiments at FLASH, the soft-X-ray FEL at DESY

  19. Approaches for ultrafast imaging of transient materials processes in the transmission electron microscope.

    LaGrange, Thomas; Reed, Bryan W; Santala, Melissa K; McKeown, Joseph T; Kulovits, Andreas; Wiezorek, Jörg M K; Nikolova, Liliya; Rosei, Federico; Siwick, Bradely J; Campbell, Geoffrey H

    2012-11-01

    The growing field of ultrafast materials science, aimed at exploring short-lived transient processes in materials on the microsecond to femtosecond timescales, has spawned the development of time-resolved, in situ techniques in electron microscopy capable of capturing these events. This article gives a brief overview of two principal approaches that have emerged in the past decade: the stroboscopic ultrafast electron microscope and the nanosecond-time-resolved single-shot instrument. The high time resolution is garnered through the use of advanced pulsed laser systems and a pump-probe experimental platforms using laser-driven photoemission processes to generate time-correlated electron probe pulses synchronized with laser-driven events in the specimen. Each technique has its advantages and limitations and thus is complementary in terms of the materials systems and processes that they can investigate. The stroboscopic approach can achieve atomic resolution and sub-picosecond time resolution for capturing transient events, though it is limited to highly repeatable (>10(6) cycles) materials processes, e.g., optically driven electronic phase transitions that must reset to the material's ground state within the repetition rate of the femtosecond laser. The single-shot approach can explore irreversible events in materials, but the spatial resolution is limited by electron source brightness and electron-electron interactions at nanosecond temporal resolutions and higher. The first part of the article will explain basic operating principles of the stroboscopic approach and briefly review recent applications of this technique. As the authors have pursued the development of the single-shot approach, the latter part of the review discusses its instrumentation design in detail and presents examples of materials science studies and the near-term instrumentation developments of this technique. PMID:22595460

  20. Electronic structure of positive and negative polarons in functionalized dithienylthiazolo-[5,4-d]thiazoles: a combined EPR and DFT study

    Ling, Yun; Van Mierloo, Sarah; Schnegg, Alexander; Fehr, Matthias; Adriaensens, Peter; Lutsen, Laurence; Vanderzande, Dirk; Maes, Wouter; Goovaerts, Etienne; Van Doorslaer, Sabine

    2014-01-01

    2,5-Dithienylthiazolo[5,4-d]thiazole (DTTzTz) derivatives have high potential for solution-processed organic field-effect transistors and solar cells, both as electron acceptors and donors. Here, the electronic structure of positive and negative radicals (polarons) of two functionalized DTTzTz materials is studied using multi-frequency and multi-resonance electron paramagnetic resonance (EPR) in combination with density functional theory (DFT). It is shown that the negative and positive DTTzT...

  1. Accelerator-based single-shot ultrafast transmission electron microscope with picosecond temporal resolution and nanometer spatial resolution

    We present feasibility study of an accelerator-based ultrafast transmission electron microscope (u-TEM) capable of producing a full field image in a single-shot with simultaneous picosecond temporal resolution and nanometer spatial resolution. We study key physics related to performance of u-TEMs and discuss major challenges as well as possible solutions for practical realization of u-TEMs. The feasibility of u-TEMs is confirmed through simulations using realistic electron beam parameters. We anticipate that u-TEMs with a product of temporal and spatial resolution beyond 10−19 ms will open up new opportunities in probing matter at ultrafast temporal and ultrasmall spatial scales

  2. Ultrafast geminate electron-radical recombination dynamics in photoactive yellow protein

    van Stokkum Ivo H.M.

    2013-03-01

    Full Text Available Photoinduced ionization of the chromophore inside photoactive yellow protein (PYP was investigated by ultrafast spectroscopy in the visible-near infrared spectral region. A solvated electron absorption-like band was observed that extended from around 550nm to 850nm, centred at 700nm. Simulation of the decay traces of the band with a classic diffusion model indicated that ejected electrons were located an average distance of ~3Å away from the radical centre, and around 40% the solvated electrons were annihilated by geminate recombination. The remaining 60% escaped out of the protein pocket to be annihilated by bulk recombination. This result indicates that the chromophore is in a local environment inside PYP that is only slightly different from the bath solvent.

  3. Advances in Ultrafast Control and Probing of Correlated-Electron Materials

    Wall, Simon; Rini, Matteo; Dhesi, Sarnjeet S.; Schoenlein, Robert W.; Cavalleri, Andrea

    2011-02-01

    In this paper, we present recent results on ultrafast control and probing of strongly correlated-electron materials. We focus on magnetoresistive manganites, applying excitation and probing wavelengths that cover the mid-IR to the soft X-rays. In analogy with near-equilibrium filling and bandwidth control of phase transitions, our approach uses both visible and mid-IR pulses to stimulate the dynamics by exciting either charges across electronic bandgaps or specific vibrational resonances. X-rays are used to unambiguously measure the microscopic electronic, orbital, and structural dynamics. Our experiments dissect and separate the nonequilibrium physics of these compounds, revealing the complex interplay and evolution of spin, lattice, charge, and orbital degrees of freedoms in the time domain.

  4. Ultrafast Spectroscopic Signatures of Coherent Electron-Transfer Mechanisms in a Transition Metal Complex.

    Guo, Zhenkun; Giokas, Paul G; Cheshire, Thomas P; Williams, Olivia F; Dirkes, David J; You, Wei; Moran, Andrew M

    2016-07-28

    The prevalence of ultrafast electron-transfer processes in light-harvesting materials has motivated a deeper understanding of coherent reaction mechanisms. Kinetic models based on the traditional (equilibrium) form of Fermi's Golden Rule are commonly employed to understand photoinduced electron-transfer dynamics. These models fail in two ways when the electron-transfer process is fast compared to solvation dynamics and vibrational dephasing. First, electron-transfer dynamics may be accelerated if the photoexcited wavepacket traverses the point of degeneracy between donor and acceptor states in the solvent coordinate. Second, traditional kinetic models fail to describe electron-transfer transitions that yield products which undergo coherent nuclear motions. We address the second point in this work. Transient absorption spectroscopy and a numerical model are used to investigate coherent back-electron-transfer mechanisms in a transition metal complex composed of titanium and catechol, [Ti(cat)3](2-). The transient absorption experiments reveal coherent wavepacket motions initiated by the back-electron-transfer process. Model calculations suggest that the vibrationally coherent product states may originate in either vibrational populations or coherences of the reactant. That is, vibrational coherence may be produced even if the reactant does not undergo coherent nuclear motions. The analysis raises a question of broader significance: can a vibrational population-to-coherence transition (i.e., a nonsecular transition) accelerate electron-transfer reactions even when the rate is slower than vibrational dephasing? PMID:27362388

  5. Understanding the Electronic Structure of 4d Metal Complexes: From Molecular Spinors to L-Edge Spectra of a di-Ru Catalyst

    Alperovich, Igor; Smolentsev, Grigory; Moonshiram, Dooshaye; Jurss, Jonah W.; Concepcion, Javier J.; Meyer, Thomas J.; Soldatov, Alexander; Pushkar, Yulia (UNC); (Purdue); (SFU-Russia); (Lund)

    2015-09-17

    L{sub 2,3}-edge X-ray absorption spectroscopy (XAS) has demonstrated unique capabilities for the analysis of the electronic structure of di-Ru complexes such as the blue dimer cis,cis-[Ru{sub 2}{sup III}O(H{sub 2}O){sub 2}(bpy){sub 4}]{sup 4+} water oxidation catalyst. Spectra of the blue dimer and the monomeric [Ru(NH{sub 3}){sub 6}]{sup 3+} model complex show considerably different splitting of the Ru L{sub 2,3} absorption edge, which reflects changes in the relative energies of the Ru 4d orbitals caused by hybridization with a bridging ligand and spin-orbit coupling effects. To aid the interpretation of spectroscopic data, we developed a new approach, which computes L{sub 2,3}-edges XAS spectra as dipole transitions between molecular spinors of 4d transition metal complexes. This allows for careful inclusion of the spin-orbit coupling effects and the hybridization of the Ru 4d and ligand orbitals. The obtained theoretical Ru L{sub 2,3}-edge spectra are in close agreement with experiment. Critically, existing single-electron methods (FEFF, FDMNES) broadly used to simulate XAS could not reproduce the experimental Ru L-edge spectra for the [Ru(NH{sub 3}){sub 6}]{sup 3+} model complex nor for the blue dimer, while charge transfer multiplet (CTM) calculations were not applicable due to the complexity and low symmetry of the blue dimer water oxidation catalyst. We demonstrated that L-edge spectroscopy is informative for analysis of bridging metal complexes. The developed computational approach enhances L-edge spectroscopy as a tool for analysis of the electronic structures of complexes, materials, catalysts, and reactive intermediates with 4d transition metals.

  6. Ultrafast core-loss spectroscopy in four-dimensional electron microscopy

    Renske M. van der Veen

    2015-03-01

    Full Text Available We demonstrate ultrafast core-electron energy-loss spectroscopy in four-dimensional electron microscopy as an element-specific probe of nanoscale dynamics. We apply it to the study of photoexcited graphite with femtosecond and nanosecond resolutions. The transient core-loss spectra, in combination with ab initio molecular dynamics simulations, reveal the elongation of the carbon-carbon bonds, even though the overall behavior is a contraction of the crystal lattice. A prompt energy-gap shrinkage is observed on the picosecond time scale, which is caused by local bond length elongation and the direct renormalization of band energies due to temperature-dependent electron–phonon interactions.

  7. Ultrafast electron kinetics in SiO2 under X-ray femtosecond irradiation

    When a dielectric is irradiated with an ultrashort laser pulse at X-ray photon energy, various physical processes take place. The photons are absorbed mostly by the deep-shell electrons, which are then excited to the high energy states of the conduction band and/or to the continuum. These electron propagate further and perform secondary scatterings via elastic and inelastic channels. All these processes occur on femtosecond timescales. Material properties are then defined by the transient state of the electronic distribution within the solid. In this contribution we present a theoretical study of the ultrafast electron kinetics in solid SiO2, irradiated with the femtosecond X-ray laser pulse (40 fs duration). A Monte-Carlo code is applied to model the electron kinetics, which includes the primary ionization, secondary scattering of electrons, and Auger-decays of deep-shell holes. With the calculated transient electron density, the transient change of the optical properties (reflection, transmittance of visible light) of the material is estimated. The analysis of the results allows us to conclude that in the X-ray excited dielectric, the holes in the valence band give the dominant contribution to the the optical properties of the material on femtosecond scales.

  8. Using Betatron Emissions from Laser Wakefield Accelerated Electrons to Probe Ultra-fast Warm Dense Matter

    Kotick, Jordan; Schumaker, Will; Condamine, Florian; Albert, Felicie; Barbrel, Benjamin; Galtier, Eric; Granados, Eduardo; Ravasio, Alessandra; Glenzer, Siegfried

    2015-11-01

    Laser wakefield acceleration (LWFA) has been shown to produce short X-ray pulses from betatron oscillations of electrons within the plasma wake. These betatron X-rays pulses have a broad, synchrotron-like energy spectrum and a duration on the order of the driving laser pulse, thereby enabling probing of ultrafast interactions. Using the 1 J, 40fs short-pulse laser at the Matter in Extreme Conditions experimental station at LCLS, we have implemented LWFA to generate and subsequently characterized betatron X-rays. Notch filtering and single photon counting techniques were used to measure the betatron X-ray spectrum while the spatial profile was measured using X-ray CCDs and image plates. We used an ellipsoidal mirror to focus the soft betatron X-rays for pump-probe studies on various targets in conjunction with LCLS X-ray and optical laser pulses. This experimental platform provides the conditions necessary to do a detailed study of warm-dense matter dynamics on the ultrafast time-scale.

  9. Ultrafast Science: Using Lasers and X-rays to Reveal the Motion of Atoms and Electrons (LBNL Summer Lecture Series)

    Summer Lecture Series 2009: The ultrafast motion of atoms and electrons lies at the heart of chemical reactions, advanced materials with exotic properties, and biological processes such as the first event in vision. Bob Schoenlein, Deputy Director for Science at the Advanced Light Source, will discuss how such processes are revealed by using laser pulses spanning a millionth of a billionth of a second, and how a new generation of light sources will bring the penetrating power of x-rays to the world of ultrafast science.

  10. Transition from ultrafast laser photo-electron emission to space charge limited current in a 1D gap

    Liu, Yangjie; Ang, L. K.

    2013-01-01

    A one-dimensional (1D) model has been constructed to study the transition of the time-dependent ultrafast laser photo-electron emission from a flat metallic surface to the space charge limited (SCL) current, including the effect of non-equilibrium laser heating on metals at the ultrafast time scale. At a high laser field, it is found that the space charge effect cannot be ignored and the SCL current emission is reached at a lower value predicted by a short pulse SCL current model that assumed...

  11. Design, construction and characterization of the compact ultrafast terahertz free-electron laser undulator

    B Biswas; V Kumar; S Chouksey; S Krishnagopal

    2008-12-01

    A compact ultrafast terahertz (CUTE) free-electron laser (FEL) is being developed at the Raja Ramanna Centre for Advanced Technology (RRCAT), Indore. The undulator required for the CUTE-FEL has recently been developed. We have designed, built and characterized a variable gap, 5 cm period, 2.5 m long pure permanent magnet undulator in two identical segments. The tolerable error in the magnetic field was 1% in rms, and we have measured it to be 0.7%. The obtained rms phase shake is around 2°. To ensure that the trajectories do not have an exit error in position or angle, corrector coils have been designed. Shimming coils have been applied for both the undulator segments to reduce the amplitude of the betatron oscillations in the vertical trajectory. Details of novel corrector coils and soft iron shims are given and their performance is discussed.

  12. Ultrafast Relaxation Dynamics of Photoexcited Zinc-Porphyrin: Electronic-Vibrational Coupling.

    Abraham, Baxter; Nieto-Pescador, Jesus; Gundlach, Lars

    2016-08-18

    Cyclic tetrapyrroles are the active core of compounds with crucial roles in living systems, such as hemoglobin and chlorophyll, and in technology as photocatalysts and light absorbers for solar energy conversion. Zinc-tetraphenylporphyrin (Zn-TPP) is a prototypical cyclic tetrapyrrole that has been intensely studied in past decades. Because of its importance for photochemical processes the optical properties are of particular interest, and, accordingly, numerous studies have focused on light absorption and excited-state dynamics of Zn-TPP. Relaxation after photoexcitation in the Soret band involves internal conversion that is preceded by an ultrafast process. This relaxation process has been observed by several groups. Hitherto, it has not been established if it involves a higher lying "dark" state or vibrational relaxation in the excited S2 state. Here we combine high time resolution electronic and vibrational spectroscopy to show that this process constitutes vibrational relaxation in the anharmonic S2 potential. PMID:27482847

  13. Ultrafast photoinduced energy and electron transfer in multi-modular donor-acceptor conjugates.

    El-Khouly, Mohamed E; Wijesinghe, Channa A; Nesterov, Vladimir N; Zandler, Melvin E; Fukuzumi, Shunichi; D'Souza, Francis

    2012-10-22

    New multi-modular donor-acceptor conjugates featuring zinc porphyrin (ZnP), catechol-chelated boron dipyrrin (BDP), triphenylamine (TPA) and fullerene (C(60)), or naphthalenediimide (NDI) have been newly designed and synthesized as photosynthetic antenna and reaction-center mimics. The X-ray structure of triphenylamine-BDP is also reported. The wide-band capturing polyad revealed ultrafast energy-transfer (k(ENT) =1.0 × 10(12) s(-1)) from the singlet excited BDP to the covalently linked ZnP owing to close proximity and favorable orientation of the entities. Introducing either fullerene or naphthalenediimide electron acceptors to the TPA-BDP-ZnP triad through metal-ligand axial coordination resulted in electron donor-acceptor polyads whose structures were revealed by spectroscopic, electrochemical and computational studies. Excitation of the electron donor, zinc porphyrin resulted in rapid electron-transfer to coordinated fullerene or naphthalenediimide yielding charge separated ion-pair species. The measured electron transfer rate constants from femtosecond transient spectral technique in non-polar toluene were in the range of 5.0 × 10(9)-3.5 × 10(10) s(-1). Stabilization of the charge-separated state in these multi-modular donor-acceptor polyads is also observed to certain level. PMID:22996909

  14. Ultrafast Photo-Induced Charge Transfer Unveiled by Two-Dimensional Electronic Spectroscopy

    Bixner, Oliver; Mancal, Tomas; Hauer, Juergen; Milota, Franz; Fischer, Michael; Pugliesi, Igor; Bradler, Maximilian; Schmid, Walther; Riedle, Eberhard; Kauffmann, Harald F; Christensson, Niklas

    2012-01-01

    The interaction of exciton and charge transfer (CT) states plays a central role in photo-induced CT processes in chemistry, biology and physics. In this work, we use a combination of two-dimensional electronic spectroscopy (2D-ES), pump-probe measurements and quantum chemistry to investigate the ultrafast CT dynamics in a lutetium bisphthalocyanine dimer in different oxidation states. It is found that in the anionic form, the combination of strong CT-exciton interaction and electronic asymmetry induced by a counter-ion enables CT between the two macrocycles of the complex on a 30 fs timescale. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra, and we monitor how the excited state charge density ultimately localizes on the macrocycle closest to the counter-ion within 100 fs. A comparison with the dynamics in the radical species further elucidates how CT states modulate the electronic structure and tune fs-reac...

  15. Vacuum Referred Binding Energy of the Single 3d, 4d, or 5d Electron in Transition Metal and Lanthanide Impurities in Compounds

    Rogers, E.G.; Dorenbos, P.

    2014-01-01

    The vacuum referred binding energy (VRBE) of the single electron in the lowest energy 3d level of Sc2 +, V4 +, Cr5 +, the lowest 4d level of Y2 +, Zr3 +, Nb4 +, Mo5 + and the lowest 5d level of Ta4 +, and W5 + in various compounds are determined by means of the chemical shift model. They will be compared with the VRBE in the already established lowest 3d level of Ti3 + and the lowest 5d level of Eu2 + and Ce3 +. Clear trends with changing charge of the transition metal (TM) cation and with ch...

  16. Direct observation of ultrafast-electron-transfer reactions unravels high effectiveness of reductive DNA damage.

    Nguyen, Jenny; Ma, Yuhan; Luo, Ting; Bristow, Robert G; Jaffray, David A; Lu, Qing-Bin

    2011-07-19

    Both water and electron-transfer reactions play important roles in chemistry, physics, biology, and the environment. Oxidative DNA damage is a well-known mechanism, whereas the relative role of reductive DNA damage is unknown. The prehydrated electron (e(pre)-), a novel species of electrons in water, is a fascinating species due to its fundamental importance in chemistry, biology, and the environment. e(pre)- is an ideal agent to observe reductive DNA damage. Here, we report both the first in situ femtosecond time-resolved laser spectroscopy measurements of ultrafast-electron-transfer (UET) reactions of e(pre)- with various scavengers (KNO(3), isopropanol, and dimethyl sulfoxide) and the first gel electrophoresis measurements of DNA strand breaks induced by e(pre)- and OH(•) radicals co-produced by two-UV-photon photolysis of water. We strikingly found that the yield of reductive DNA strand breaks induced by each e(pre)- is twice the yield of oxidative DNA strand breaks induced by each OH(•) radical. Our results not only unravel the long-standing mystery about the relative role of radicals in inducing DNA damage under ionizing radiation, but also challenge the conventional notion that oxidative damage is the main pathway for DNA damage. The results also show the potential of femtomedicine as a new transdisciplinary frontier and the broad significance of UET reactions of e(pre)- in many processes in chemistry, physics, biology, and the environment. PMID:21730183

  17. Tilted femtosecond pulses for velocity matching in gas-phase ultrafast electron diffraction

    Recent advances in pulsed electron gun technology have resulted in femtosecond electron pulses becoming available for ultrafast electron diffraction experiments. For experiments investigating chemical dynamics in the gas phase, the resolution is still limited to picosecond time scales due to the velocity mismatch between laser and electron pulses. Tilted laser pulses can be used for velocity matching, but thus far this has not been demonstrated over an extended target in a diffraction setting. We demonstrate an optical configuration to deliver high-intensity laser pulses with a tilted pulse front for velocity matching over the typical length of a gas jet. A laser pulse is diffracted from a grating to introduce angular dispersion, and the grating surface is imaged on the target using large demagnification. The laser pulse duration and tilt angle were measured at and near the image plane using two different techniques: second harmonic cross correlation and an interferometric method. We found that a temporal resolution on the order of 100 fs can be achieved over a range of approximately 1 mm around the image plane. (paper)

  18. Electro-optic sampling for time resolving relativistic ultrafast electron diffraction

    The Pegasus laboratory at UCLA features a state-of-the-art electron photoinjector capable of producing ultrashort (<100 fs) high-brightness electron bunches at energies of 3.75 MeV. These beams recently have been used to produce static diffraction patterns from scattering off thin metal foils, and it is foreseen to take advantage of the ultrashort nature of these bunches in future pump-probe time-resolved diffraction studies. In this paper, single shot 2-d electro-optic sampling is presented as a potential technique for time of arrival stamping of electron bunches used for diffraction. Effects of relatively low bunch charge (a few 10's of pC) and modestly relativistic beams are discussed and background compensation techniques to obtain high signal-to-noise ratio are explored. From these preliminary tests, electro-optic sampling is suitable to be a reliable nondestructive time stamping method for relativistic ultrafast electron diffraction at the Pegasus lab.

  19. Materials Properties and Solvated Electron Dynamics of Isolated Nanoparticles and Nanodroplets Probed with Ultrafast Extreme Ultraviolet Beams.

    Ellis, Jennifer L; Hickstein, Daniel D; Xiong, Wei; Dollar, Franklin; Palm, Brett B; Keister, K Ellen; Dorney, Kevin M; Ding, Chengyuan; Fan, Tingting; Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana; Jimenez, Jose L; Kapteyn, Henry C; Murnane, Margaret M

    2016-02-18

    We present ultrafast photoemission measurements of isolated nanoparticles in vacuum using extreme ultraviolet (EUV) light produced through high harmonic generation. Surface-selective static EUV photoemission measurements were performed on nanoparticles with a wide array of compositions, ranging from ionic crystals to nanodroplets of organic material. We find that the total photoelectron yield varies greatly with nanoparticle composition and provides insight into material properties such as the electron mean free path and effective mass. Additionally, we conduct time-resolved photoelectron yield measurements of isolated oleylamine nanodroplets, observing that EUV photons can create solvated electrons in liquid nanodroplets. Using photoemission from a time-delayed 790 nm pulse, we observe that a solvated electron is produced in an excited state and subsequently relaxes to its ground state with a lifetime of 151 ± 31 fs. This work demonstrates that femotosecond EUV photoemission is a versatile surface-sensitive probe of the properties and ultrafast dynamics of isolated nanoparticles. PMID:26807653

  20. Changes in microstructural parameters of NB4D2 silk fibres due to electron irradiation: X-ray line profile analysis

    Sangappa; S Asha; P Parameswara; R Somashekar

    2011-12-01

    The present study is concerned with changes of microcrystalline parameters in NB4D2 (Bombyx mori) silk fibres, due to electron irradiation. The irradiation process was performed in air at room temperature using 8 MeV electron beam at different dose rates: 0, 25, 50 and 75 kGy, respectively. X-ray recording of these irradiated samples and the line profile analysis were carried out. The crystal imperfection parameters such as crystallite size $\\langle N \\rangle$, lattice strain (g in %) and surface weighted crystallite size ($D_{s}$) were computed and compared with other physical parameters in order to asertain the changes that have crept into these irradiated fibres. Exponential, lognormal and Reinhold functions for the column length distributions have been used for the determination of these parameters.

  1. Relationships between the surface electronic and chemical properties of doped 4d and 5d late transition metal dioxides

    Xu, Zhongnan; Kitchin, John R., E-mail: jkitchin@andrew.cmu.edu [Department of Chemical Engineering, Carnegie Mellon University, 5000 Forbes Ave, Pittsburgh, Pennsylvania 15213 (United States)

    2015-03-14

    Density functional theory calculations were performed to elucidate the underlying physics describing the adsorption energies on doped late transition metal dioxide rutiles. Adsorption energies of atomic oxygen on doped rutiles M{sup D}-M{sup H}O{sub 2}, where transition metal M{sup D} is doped into M{sup H}O{sub 2}, were expressed in terms of a contribution from adsorption on the pure oxide of the dopant M{sup D} and perturbations to this adsorption energy caused by changing its neighboring metal cations and lattice parameters to that of the host oxide M{sup H}O{sub 2}, which we call the ligand and strain effects, respectively. Our analysis of atom projected density of states revealed that the t{sub 2g}-band center had the strongest correlation with adsorption energies. We show that charge transfer mediated shifts to the t{sub 2g}-band center describe the ligand effect, and the radii of the atomic orbitals of metal cations can predict the magnitude and direction of this charge transfer. Strain produces systematic shifts to all features of the atom projected density of states, but correlations between the strain effect and the electronic structure were dependent on the chemical identity of the metal cation. The slope of these correlations can be related to the idealized d-band filling. This work elucidates the underlying physics describing adsorption on doped late transition metal oxides and establishes a foundation for models that use known chemical properties for the prediction of reactivity.

  2. Test of theoretical models for ultrafast heterogeneous electron transfer with femtosecond two-photon photoemission data

    Lars Gundlach; Tobias Letzig; Frank Willig

    2009-09-01

    The energy distribution of electrons injected into acceptor states on the surface of TiO2 was measured with femtosecond two-photon photoemission. Shape and relative energetic position of these distribution curves with respect to the corresponding donor states, i.e. of perylene chromophores in the first excited singlet state attached via different bridge-anchor groups to the TiO2 surface, were compared with the predictions of different theoretical models for light-induced ultrafast heterogeneous electron transfer (HET). Gerischer’s early scenario for light-induced HET was considered and two recent explicit calculations, i.e. a fully quantum mechanical analytical model and a time-dependent density functional theory model based on molecular dynamics simulations for the vibrational modes were also considered. Based on the known vibrational structure in the photoionization spectrum of perylene in the gas phase and that measured in the linear absorption spectra of the perylene chromophores anchored on the TiO2 surface the energy distribution curves for the injected electrons were fitted assuming the excitation of the dominant 0.17 eV vibrational mode in the ionized perylene chromophore leading to a corresponding Franck-Condon dictated progression in the energy distribution curves. Each individual peak was fitted with a Voigt profile where the Lorentzian contribution was taken from the time-resolved HET data and the Gaussian contribution attributed to inhomogeneous broadening. The measured room temperature energy distribution curves for the injected electrons are explained with the fully quantum mechanical model for light-induced HET with the high energy, 0.17 eV, skeletal stretching mode excited in the ionized perylene chromophore. The corresponding energy distribution of the injected electrons is fully accommodated in acceptor states on the TiO2 surface fulfilling the wide band limit.

  3. Verifying 4D gated radiotherapy using time-integrated electronic portal imaging: a phantom and clinical study

    Slotman Ben J

    2007-08-01

    Full Text Available Abstract Background Respiration-gated radiotherapy (RGRT can decrease treatment toxicity by allowing for smaller treatment volumes for mobile tumors. RGRT is commonly performed using external surrogates of tumor motion. We describe the use of time-integrated electronic portal imaging (TI-EPI to verify the position of internal structures during RGRT delivery Methods TI-EPI portals were generated by continuously collecting exit dose data (aSi500 EPID, Portal vision, Varian Medical Systems when a respiratory motion phantom was irradiated during expiration, inspiration and free breathing phases. RGRT was delivered using the Varian RPM system, and grey value profile plots over a fixed trajectory were used to study object positions. Time-related positional information was derived by subtracting grey values from TI-EPI portals sharing the pixel matrix. TI-EPI portals were also collected in 2 patients undergoing RPM-triggered RGRT for a lung and hepatic tumor (with fiducial markers, and corresponding planning 4-dimensional CT (4DCT scans were analyzed for motion amplitude. Results Integral grey values of phantom TI-EPI portals correlated well with mean object position in all respiratory phases. Cranio-caudal motion of internal structures ranged from 17.5–20.0 mm on planning 4DCT scans. TI-EPI of bronchial images reproduced with a mean value of 5.3 mm (1 SD 3.0 mm located cranial to planned position. Mean hepatic fiducial markers reproduced with 3.2 mm (SD 2.2 mm caudal to planned position. After bony alignment to exclude set-up errors, mean displacement in the two structures was 2.8 mm and 1.4 mm, respectively, and corresponding reproducibility in anatomy improved to 1.6 mm (1 SD. Conclusion TI-EPI appears to be a promising method for verifying delivery of RGRT. The RPM system was a good indirect surrogate of internal anatomy, but use of TI-EPI allowed for a direct link between anatomy and breathing patterns.

  4. Verifying 4D gated radiotherapy using time-integrated electronic portal imaging: a phantom and clinical study

    Respiration-gated radiotherapy (RGRT) can decrease treatment toxicity by allowing for smaller treatment volumes for mobile tumors. RGRT is commonly performed using external surrogates of tumor motion. We describe the use of time-integrated electronic portal imaging (TI-EPI) to verify the position of internal structures during RGRT delivery TI-EPI portals were generated by continuously collecting exit dose data (aSi500 EPID, Portal vision, Varian Medical Systems) when a respiratory motion phantom was irradiated during expiration, inspiration and free breathing phases. RGRT was delivered using the Varian RPM system, and grey value profile plots over a fixed trajectory were used to study object positions. Time-related positional information was derived by subtracting grey values from TI-EPI portals sharing the pixel matrix. TI-EPI portals were also collected in 2 patients undergoing RPM-triggered RGRT for a lung and hepatic tumor (with fiducial markers), and corresponding planning 4-dimensional CT (4DCT) scans were analyzed for motion amplitude. Integral grey values of phantom TI-EPI portals correlated well with mean object position in all respiratory phases. Cranio-caudal motion of internal structures ranged from 17.5–20.0 mm on planning 4DCT scans. TI-EPI of bronchial images reproduced with a mean value of 5.3 mm (1 SD 3.0 mm) located cranial to planned position. Mean hepatic fiducial markers reproduced with 3.2 mm (SD 2.2 mm) caudal to planned position. After bony alignment to exclude set-up errors, mean displacement in the two structures was 2.8 mm and 1.4 mm, respectively, and corresponding reproducibility in anatomy improved to 1.6 mm (1 SD). TI-EPI appears to be a promising method for verifying delivery of RGRT. The RPM system was a good indirect surrogate of internal anatomy, but use of TI-EPI allowed for a direct link between anatomy and breathing patterns

  5. Accelerator-based Single-shot Ultrafast Transmission Electron Microscope with Picosecond Temporal Resolution and Nanometer Spatial Resolution

    Xiang, D; Zhang, J; Huang, X; Wang, L; Wang, X; Wan, W

    2014-01-01

    We present feasibility study of an accelerator-based ultrafast transmission electron microscope (u-TEM) capable of producing a full field image in a single-shot with simultaneous picosecond temporal resolution and nanometer spatial resolution. We study key physics related to performance of u-TEMs, and discuss major challenges as well as possible solutions for practical realization of u-TEMs. The feasibility of u-TEMs is confirmed through simulations using realistic electron beam parameters. We anticipate that u-TEMs with a product of temporal and spatial resolution beyond $10^{-19}~$m*s will open up new opportunities in probing matter at ultrafast temporal and ultrasmall spatial scales.

  6. Monitoring one-electron photo-oxidation of guanine in DNA crystals using ultrafast infrared spectroscopy

    Hall, James P.; Poynton, Fergus E.; Keane, Páraic M.; Gurung, Sarah P.; Brazier, John A.; Cardin, David J.; Winter, Graeme; Gunnlaugsson, Thorfinnur; Sazanovich, Igor V.; Towrie, Michael; Cardin, Christine J.; Kelly, John M.; Quinn, Susan J.

    2015-12-01

    To understand the molecular origins of diseases caused by ultraviolet and visible light, and also to develop photodynamic therapy, it is important to resolve the mechanism of photoinduced DNA damage. Damage to DNA bound to a photosensitizer molecule frequently proceeds by one-electron photo-oxidation of guanine, but the precise dynamics of this process are sensitive to the location and the orientation of the photosensitizer, which are very difficult to define in solution. To overcome this, ultrafast time-resolved infrared (TRIR) spectroscopy was performed on photoexcited ruthenium polypyridyl-DNA crystals, the atomic structure of which was determined by X-ray crystallography. By combining the X-ray and TRIR data we are able to define both the geometry of the reaction site and the rates of individual steps in a reversible photoinduced electron-transfer process. This allows us to propose an individual guanine as the reaction site and, intriguingly, reveals that the dynamics in the crystal state are quite similar to those observed in the solvent medium.

  7. Ultrafast terahertz probes of transient conducting and insulating phases in an electron-hole gas

    Kaindl, Robert A.; Carnahan, Marc A.; Hagele, Daniel; Lovenich, Reinhold; Chemla, Daniel S.

    2003-04-10

    Many-body systems in nature exhibit complexity and self-organization arising from seemingly simple laws. The long-range Coulomb interaction between electrical charges generates a plethora of bound states in matter, ranging from the hydrogen atom to complex biochemical structures. Semiconductors form an ideal laboratory for studying many-body interactions of quasi-particles among themselves and with lattice vibrations and light. Oppositely charged electron and hole quasi-particles can coexist in an ionized but correlated plasma, or form bound hydrogen-like pairs called excitons which strongly affect physical properties. The pathways between such states however remain elusive in near-visible optical experiments that detect a subset of excitons with vanishing center-of-mass momenta. In contrast, transitions between internal exciton levels which occur in the far-infrared at terahertz (10 s) frequencies are in dependent of this restriction suggesting their use as a novel pro be of pair dynamics. Here, we employ an ultrafast terahertz probe to directly investigate the dynamical interplay of optically-generated excitons and unbound electron-hole pairs in GaAs quantum wells. Our observations witness an unexpected quasi-instantaneous excitonic enhancement, reveal formation of insulating excitons on a hundred picosecond timescale and manifest conditions under which excitonic populations prevail.

  8. Vibrationally resolved optical spectra and ultrafast electronic relaxation dynamics of diamantane.

    Röhr, Merle I S; Mitrić, Roland; Petersen, Jens

    2016-03-28

    We present theoretical simulations of the vibrationally resolved photoabsorption and photoemission spectra of diamantane combined with nonadiabatic dynamics simulations in order to identify the state responsible for the measured photoluminescence of diamantane and to determine the mechanism and the time-scales of the electronic state relaxation. Diamantane is a prototype representative of the diamondoid class of hydrocarbons which have recently gained significant interest due to their unique electronic properties. This molecule is characterised by an almost dark first excited state, which therefore cannot be directly excited. Moreover, the calculated vertical transition from the geometrically relaxed first excited state to the ground state also bears no intensity. However, recent experiments suggest that the observed photoluminescence originates from the lowest excited state. We have performed spectral simulations in the frame of the Herzberg-Teller approximation for vibronic transitions, which goes beyond the Franck-Condon approximation of constant transition dipole moments and takes into account their linear dependence on the geometrical deformations. In this way, the available experimental spectrum could be fully reproduced, resolving the issue about the origin of the photoluminescence. Moreover, the photoemission from the first excited state also implies that ultrafast nonradiative processes have to take place after the initial excitation of the bright electronic states. We have determined the mechanism and time-scales of these relaxation processes by performing nonadiabatic dynamics simulations in the manifold of s- and p-type Rydberg excited states. The simulations demonstrate that the lowest excited electronic state of diamantane gains significant population from higher-lying states already after several hundreds of femtoseconds. Thus, our dynamics simulations combined with spectra calculated using the Herzberg-Teller approximation allow us to fully explain

  9. Polychromatic X-ray Beam from the Acceleration of Energetic Electrons in Ultrafast Laser-Produced Plasmas

    Albert, Félicie; Taphuoc, Kim; Shah, Rahul; Burgy, Frederic; Rousseau, Jean Philippe; Rousse, Antoine

    2007-01-01

    Polychromatic beams of hard X-rays from ultrafast laser plasma interaction are studied. Just as in a conventional synchrotron, electrons are accelerated and wiggled, but on a much shorter scale of a few millimeters. By focusing a 50 TW CPA laser system (30 fs duration) onto a helium gas jet, we obtained a polychromatic collimated beam (50 mrad) of X-ray radiation in the keV range. In addition, its perfect synchronization with the laser system, its ultrafast duration (≃30 fs) and its brightness (up to 108 photons/shot/solid angle at 0.1% BW) will make it applicable to both X-ray science and backlighting to address laboratory astrophysics research issues.

  10. Short electron bunch generation using single-cycle ultrafast electron guns

    Fallahi, Arya; Fakhari, Moein; Yahaghi, Alireza; Arrieta, Miguel; Kärtner, Franz X.

    2016-08-01

    We introduce a solution for producing ultrashort (˜fs ) high charge (˜pC ) from ultracompact guns utilizing single-cycle THz pulses. We show that the readily available THz pulses with energies as low as 20 μ J are sufficient to generate multi-10 keV electron bunches. Moreover, it is demonstrated that THz energies of 2 mJ are sufficient to generate relativistic electron bunches with higher than 2 MeV energy. The high acceleration gradients possible in the structures provide 30 fs electron bunches at 30 keV energy and 45 fs bunches at 2 MeV energy. These structures will underpin future devices for strong field THz physics in general and miniaturized electron guns, in which the high fields combined with the short pulse duration enable electron beams with ultrahigh brightness.

  11. Short Electron Bunch Generation Using Single-Cycle Ultrafast Electron Guns

    Fallahi, Arya; Yahaghi, Alireza; Arrieta, Miguel; Kärtner, Franz X

    2016-01-01

    We introduce a solution for producing ultrashort ($\\sim$fs) high charge ($\\sim$pC) from ultra-compact guns utilizing single-cycle THz pulses. We show that the readily available THz pulses with energies as low as 20 ?J are sufficient to generate multi-10 keV electron bunches. Moreover, It is demonstrated that THz energies of 2mJ are sufficient to generate relativistic electron bunches with higher than 2 MeV energy. The high acceleration gradients possible in the structures provide 30 fs electron bunches at 30 keV energy and 45 fs bunches at 2 MeV energy. These structures will underpin future devices for strong field THz physics in general and miniaturized electron guns, in which the high fields combined with the short pulse duration enable electron beams with ultrahigh brightness.

  12. Electronic Coupling Dependence of Ultrafast Interfacial Electron Transfer on Nanocrystalline Thin Films and Single Crystal

    Lian, Tianquan

    2014-04-22

    The long-term goal of the proposed research is to understand electron transfer dynamics in nanoparticle/liquid interface. This knowledge is essential to many semiconductor nanoparticle based devices, including photocatalytic waste degradation and dye sensitized solar cells.

  13. 4-D Photoacoustic Tomography

    Xiang, Liangzhong; Wang, Bo; Ji, Lijun; Jiang, Huabei

    2013-01-01

    Photoacoustic tomography (PAT) offers three-dimensional (3D) structural and functional imaging of living biological tissue with label-free, optical absorption contrast. These attributes lend PAT imaging to a wide variety of applications in clinical medicine and preclinical research. Despite advances in live animal imaging with PAT, there is still a need for 3D imaging at centimeter depths in real-time. We report the development of four dimensional (4D) PAT, which integrates time resolutions with 3D spatial resolution, obtained using spherical arrays of ultrasonic detectors. The 4D PAT technique generates motion pictures of imaged tissue, enabling real time tracking of dynamic physiological and pathological processes at hundred micrometer-millisecond resolutions. The 4D PAT technique is used here to image needle-based drug delivery and pharmacokinetics. We also use this technique to monitor 1) fast hemodynamic changes during inter-ictal epileptic seizures and 2) temperature variations during tumor thermal therapy.

  14. Structural, electronic and magnetic properties of Mo (4d)-based complex perovskites Ba{sub 2}MMoO{sub 6} (M=Cr and Fe)

    Musa Saad H E, M., E-mail: musa.1964@gmail.com [Department of Physics, College of Science, Qassim University, Buridah 51452 (Saudi Arabia); El-Hagary, M. [Physics Department, Faculty of Science, Helwan University, Helwan, Cairo (Egypt); Institut für Festkörperphysik, TU Wien, A-1040 Wien (Austria)

    2014-06-01

    We report a study of crystallographic parameters of the Mo-based complex perovskites Ba{sub 2}MMoO{sub 6} (M=Cr and Fe) obtained from analysis of X-ray diffraction (XRD) data and the electronic and magnetic properties prediction using the magnetic measurements and the full-potential linearized muffin–tin orbitals within the plane-wave approximation (LMTO–PLW). The Ba{sub 2}MMoO{sub 6} materials were prepared by the solid state reaction method. XRD analysis reveals that Ba{sub 2}MMoO{sub 6} crystalline in a cubic structure (space group Fm-3m) with lattice parameters (a=8.013 Å) for M=Cr and (a=8.061 Å) for M=Fe. XRD results present a matching of 98% with the theoretical results. The densities of states were calculated using the local spin density approximation (LSDA) and LSDA+U methods. LDOS results show a half-metallic-ferrimagnetic ground state for Ba{sub 2}MMoO{sub 6}, which is in majority due to the 4d-t{sub 2g} and 3d-t{sub 2g} characters. The structural, electronic and magnetic calculation results are in excellent agreement with the experimental and previous theoretical results. - Highlights: • Mo-based complex perovskites Ba{sub 2}MMoO{sub 6} (M=Cr and Fe) have been studied. • XRD analysis revealed Ba{sub 2}MMoO{sub 6} crystalline in cubic structures (Fm-3m). • Full-potential linear muffin–tin orbital (LMTO) calculations have been carried out. • The DOSs were calculated using the LSDA and correlated LSDA+U methods. • Ba{sub 2}MMoO{sub 6} (M=Cr and Fe) shows HM–FiM nature due to 3d-t{sub 2g}–4d-t{sub 2g} characters.

  15. High quality single shot ultrafast MeV electron diffraction from a photocathode radio-frequency gun

    A compact ultrafast electron diffractometer, consisting of an s-band 1.6 cell photocathode radio-frequency gun, a multi-function changeable sample chamber, and a sensitive relativistic electron detector, was built at Shanghai Jiao Tong University. High-quality single-shot transmission electron diffraction patterns have been recorded by scattering 2.5 MeV electrons off single crystalline gold and polycrystalline aluminum samples. The high quality diffraction pattern indicates an excellent spatial resolution, with the ratio of the diffraction ring radius over the ring rms width beyond 10. The electron pulse width is estimated to be about 300 fs. The high temporal and spatial resolution may open new opportunities in various areas of sciences

  16. Spectroscopic, electronic structure and natural bond analysis of 2-aminopyrimidine and 4-aminopyrazolo[3,4-d]pyrimidine: A comparative study

    Prabavathi, N.; Nilufer, A.; Krishnakumar, V.; Akilandeswari, L.

    2012-10-01

    The FTIR and FT-Raman spectra of 2-aminopyrimidine (2-AP) and 4-aminopyrazolo[3,4-d]pyrimidine (4-APP) has been recorded in the region 4000-400 and 3500-100 cm-1, respectively. The tautomeric stability, optimized geometry, frequency and intensity of the vibrational bands of 2-AP and 4-APP were obtained by the DFT level using 6-31G(d) and 6-31G(d,p) basis sets. The harmonic vibrational frequencies were calculated and the scaled values have been compared with experimental FTIR and FT-Raman spectra. A detailed interpretation of the infrared and Raman spectra of 2-AP and 4-APP are also reported based on total energy distribution (TED). The observed and the calculated frequencies are found to be in good agreement. The experimental spectra also coincide satisfactorily with those of theoretically simulated spectra. The 1H and 13C NMR spectra have been simulated using the gauge independent atomic orbital (GIAO) method. The theoretical UV-Vis spectrum of the compound using CIS method and the electronic properties, such as HOMO and LUMO energies, were performed by time-dependent DFT (TD-DFT) approach. The calculated HOMO and LUMO energies show that charge transfer occurs within molecule. The first order hyperpolarizability (β0) of these novel molecular system and related properties (β, α0 and Δα) of 2-AP and 4-APP are calculated using DFT/6-31G(d) method on the finite-field approach. The Mulliken charges, the values of electric dipole moment (μ) of the molecule were computed using DFT calculations. The change in electron density (ED) in the σ∗ antibonding orbitals and stabilization energies E(2) have been calculated by natural bond (NBO) analysis to give clear evidence of stabilization originating in the hyper conjugation of hydrogen-bonded interactions.

  17. Ultrafast gating of a mid-infrared laser pulse by a sub-pC relativistic electron beam

    In this paper we discuss a relative time-of-arrival measurement scheme between an electron beam and a mid-infrared laser pulse based on the electron-beam controlled transmission in semiconductor materials. This technique can be used as a time-stamping diagnostic in ultrafast electron diffraction or microscopy. In particular, our characterization of Germanium demonstrates that sub-ps time-of-arrival sensitivity could be achieved in a single shot and with very low charge beams (<1 pC). Detailed measurements as a function of the beam charge and the laser wavelength offer insights on the free carrier dynamics in the semiconductor upon excitation by the electron beam

  18. Ultrafast gating of a mid-infrared laser pulse by a sub-pC relativistic electron beam

    Cesar, D. B.; Musumeci, P. [Department of Physics and Astronomy, UCLA, Los Angeles, California 90095 (United States); Alesini, D. [INFN-LNF, Via E. Fermi, 40, 00044 Frascati, Roma (Italy)

    2015-12-21

    In this paper we discuss a relative time-of-arrival measurement scheme between an electron beam and a mid-infrared laser pulse based on the electron-beam controlled transmission in semiconductor materials. This technique can be used as a time-stamping diagnostic in ultrafast electron diffraction or microscopy. In particular, our characterization of Germanium demonstrates that sub-ps time-of-arrival sensitivity could be achieved in a single shot and with very low charge beams (<1 pC). Detailed measurements as a function of the beam charge and the laser wavelength offer insights on the free carrier dynamics in the semiconductor upon excitation by the electron beam.

  19. Dynamic Processes in Biology, Chemistry, and Materials Science: Opportunities for UltraFast Transmission Electron Microscopy - Workshop Summary Report

    Kabius, Bernd C.; Browning, Nigel D.; Thevuthasan, Suntharampillai; Diehl, Barbara L.; Stach, Eric A.

    2012-07-25

    This report summarizes a 2011 workshop that addressed the potential role of rapid, time-resolved electron microscopy measurements in accelerating the solution of important scientific and technical problems. A series of U.S. Department of Energy (DOE) and National Academy of Science workshops have highlighted the critical role advanced research tools play in addressing scientific challenges relevant to biology, sustainable energy, and technologies that will fuel economic development without degrading our environment. Among the specific capability needs for advancing science and technology are tools that extract more detailed information in realistic environments (in situ or operando) at extreme conditions (pressure and temperature) and as a function of time (dynamic and time-dependent). One of the DOE workshops, Future Science Needs and Opportunities for Electron Scattering: Next Generation Instrumentation and Beyond, specifically addressed the importance of electron-based characterization methods for a wide range of energy-relevant Grand Scientific Challenges. Boosted by the electron optical advancement in the last decade, a diversity of in situ capabilities already is available in many laboratories. The obvious remaining major capability gap in electron microscopy is in the ability to make these direct in situ observations over a broad spectrum of fast (µs) to ultrafast (picosecond [ps] and faster) temporal regimes. In an effort to address current capability gaps, EMSL, the Environmental Molecular Sciences Laboratory, organized an Ultrafast Electron Microscopy Workshop, held June 14-15, 2011, with the primary goal to identify the scientific needs that could be met by creating a facility capable of a strongly improved time resolution with integrated in situ capabilities. The workshop brought together more than 40 leading scientists involved in applying and/or advancing electron microscopy to address important scientific problems of relevance to DOE’s research

  20. Towards simultaneous measurements of electronic and structural properties in ultra-fast x-ray free electron laser absorption spectroscopy experiments

    The rapidly growing ultrafast science with X-ray lasers unveils atomic scale processes with unprecedented time resolution bringing the so called 'molecular movie' within reach. X-ray absorption spectroscopy is one of the most powerful x-ray techniques providing both local atomic order and electronic structure when coupled with ad-hoc theory. Collecting absorption spectra within few x-ray pulses is possible only in a dispersive setup. We demonstrate ultrafast time-resolved measurements of the LIII-edge x-ray absorption near-edge spectra of irreversibly laser excited Molybdenum using an average of only few x-ray pulses with a signal to noise ratio limited only by the saturation level of the detector. The simplicity of the experimental set-up makes this technique versatile and applicable for a wide range of pump-probe experiments, particularly in the case of non-reversible processes

  1. Ultrafast electron and energy transfer in dye-sensitized iron oxide and oxyhydroxide nanoparticles

    Gilbert, Benjamin; Katz, Jordan E.; Huse, Nils;

    2013-01-01

    An emerging area in chemical science is the study of solid-phase redox reactions using ultrafast time-resolved spectroscopy. We have used molecules of the photoactive dye 2′,7′-dichlorofluorescein (DCF) anchored to the surface of iron(iii) oxide nanoparticles to create iron(ii) surface atoms via...

  2. Design and implementation of electronics and data acquisition system for Ultra-Fast Flash Observatory

    Jung, A.; Ahmad, S.; Barrillon, P.;

    2013-01-01

    The Ultra-Fast Flash Observatory (UFFO) Pathfinder for Gamma-Ray Bursts (GRBs) consists of two telescopes. The UFFO Burst Alert & Trigger Telescope (UBAT) handles the detection and localization of GRBs, and the Slewing Mirror Telescope (SMT) conducts the measurement of the UV/optical afterglow. U...

  3. Molecular-structure control of ultrafast electron injection at cationic porphyrin-CdTe quantum dot interfaces

    Aly, Shawkat Mohammede

    2015-03-05

    Charge transfer (CT) at donor (D)/acceptor (A) interfaces is central to the functioning of photovoltaic and light-emitting devices. Understanding and controlling this process on the molecular level has been proven to be crucial for optimizing the performance of many energy-challenge relevant devices. Here, we report the experimental observations of controlled on/off ultrafast electron transfer (ET) at cationic porphyrin-CdTe quantum dot (QD) interfaces using femto- and nanosecond broad-band transient absorption (TA) spectroscopy. The time-resolved data demonstrate how one can turn on/off the electron injection from porphyrin to the CdTe QDs. With careful control of the molecular structure, we are able to tune the electron injection at the porphyrin-CdTe QD interface from zero to very efficient and ultrafast. In addition, our data demonstrate that the ET process occurs within our temporal resolution of 120 fs, which is one of the fastest times recorded for organic photovoltaics. © 2015 American Chemical Society.

  4. Ultrafast Photoinduced Electron Transfer and Charge Stabilization in Donor-Acceptor Dyads Capable of Harvesting Near-Infrared Light.

    Bandi, Venugopal; Gobeze, Habtom B; D'Souza, Francis

    2015-08-01

    To harvest energy from the near-infrared (near-IR) and infrared (IR) regions of the electromagnetic spectrum, which constitutes nearly 70 % of the solar radiation, there is a great demand for near-IR and IR light-absorbing sensitizers that are capable of undergoing ultrafast photoinduced electron transfer when connected to a suitable electron acceptor. Towards achieving this goal, in the present study, we report multistep syntheses of dyads derived from structurally modified BF2-chelated azadipyrromethene (ADP; to extend absorption and emission into the near-IR region) and fullerene as electron-donor and electron-acceptor entities, respectively. The newly synthesized dyads were fully characterized based on optical absorbance, fluorescence, geometry optimization, and electrochemical studies. The established energy level diagram revealed the possibility of electron transfer either from the singlet excited near-IR sensitizer or singlet excited fullerene. Femtosecond and nanosecond transient absorption studies were performed to gather evidence of excited state electron transfer and to evaluate the kinetics of charge separation and charge recombination processes. These studies revealed the occurrence of ultrafast photoinduced electron transfer leading to charge stabilization in the dyads, and populating the triplet states of ADP, benzanulated-ADP and benzanulated thiophene-ADP in the respective dyads, and triplet state of C60 in the case of BF2 -chelated dipyrromethene derived dyad during charge recombination. The present findings reveal that these sensitizers are suitable for harvesting light energy from the near-IR region of the solar spectrum and for building fast-responding optoelectronic devices operating under near-IR radiation input. PMID:26130432

  5. Effects of single atom doping on the ultrafast electron dynamics of M1Au24(SR)18 (M = Pd, Pt) nanoclusters

    Zhou, Meng; Qian, Huifeng; Sfeir, Matthew Y.; Nobusada, Katsuyuki; Jin, Rongchao

    2016-03-01

    Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M1@Au24(SR)18 (M = Pd, Pt; R = CH2CH2Ph) clusters using femtosecond visible and near infrared transient absorption spectroscopy. Three relaxation components are identified for both mono-doped clusters: (1) sub-picosecond relaxation within the M1Au12 core states; (2) core to shell relaxation in a few picoseconds; and (3) relaxation back to the ground state in more than one nanosecond. Despite similar relaxation pathways for the two doped nanoclusters, the coupling between the metal core and surface ligands is accelerated by over 30% in the case of the Pt dopant compared with the Pd dopant. Compared to Pd doping, the case of Pt doping leads to much more drastic changes in the steady state and transient absorption of the clusters, which indicates that the 5d orbitals of the Pt atom are more strongly mixed with Au 5d and 6s orbitals than the 4d orbitals of the Pd dopant. These results demonstrate that a single foreign atom can lead to entirely different excited state spectral features of the whole cluster compared to the parent Au25(SR)18 cluster. The detailed excited state dynamics of atomically precise Pd/Pt doped gold clusters help further understand their properties and benefit the development of energy-related applications.Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M1@Au24(SR)18 (M = Pd, Pt; R = CH2CH2Ph) clusters using femtosecond visible and near infrared

  6. Ultrafast coherent diffractive imaging of nanoparticles using X-ray free-electron laser radiation

    Coherent diffractive imaging with X-ray free-electron lasers (X-FEL) promises high-resolution structure determination of single microscopic particles without the need for crystallization. The diffraction signal of small samples can be very weak, a difficulty that can not be countered by merely increasing the number of photons because the sample would be damaged by a high absorbed radiation dose. Traditional X-ray crystallography avoids this problem by bringing many sample particles into a periodic arrangement, which amplifies the individual signals while distributing the absorbed dose. Depending on the sample, however, crystallization can be very difficult or even impossible. This thesis presents algorithms for a new imaging approach using X-FEL radiation that works with single, non-crystalline sample particles. X-FELs can deliver X-rays with a peak brilliance many orders of magnitude higher than conventional X-ray sources, compensating for their weak interaction cross sections. At the same time, FELs can produce ultra-short pulses down to a few femtoseconds. In this way it is possible to perform ultra-fast imaging, essentially ''freezing'' the atomic positions in time and terminating the imaging process before the sample is destroyed by the absorbed radiation. This thesis primarily focuses on the three-dimensional reconstruction of single (and not necessarily crystalline) particles using coherent diffractive imaging at X-FELs: in order to extract three-dimensional information from scattering data, two-dimensional diffraction patterns from many different viewing angles must be combined. Therefore, the diffraction signal of many identical sample copies in random orientations is measured. The main result of this work is a globally optimal algorithm that can recover the sample orientations solely based on the diffraction signal, enabling three-dimensional imaging for arbitrary samples. The problem of finding three-dimensional orientations is

  7. Ultrafast Excited-State Dynamics of Diketopyrrolopyrrole (DPP)-Based Materials: Static versus Diffusion-Controlled Electron Transfer Process

    Alsulami, Qana

    2015-06-25

    Singlet-to-triplet intersystem crossing (ISC) and photoinduced electron transfer (PET) of platinum(II) containing diketopyrrolopyrrole (DPP) oligomer in the absence and presence of strong electron-acceptor tetracyanoethylene (TCNE) were investigated using femtosecond and nanosecond transient absorption spectroscopy with broadband capabilities. The role of platinum(II) incorporation in those photophysical properties was evaluated by comparing the excited-state dynamics of DPP with and without the metal centers. The steady-state measurements reveal that platinum(II) incorporation facilitates dramatically the interactions between DPP-Pt(acac) and TCNE, resulting in charge transfer (CT) complex formation. The transient absorption spectra in the absence of TCNE reveal ultrafast ISC of DPP-Pt(acac) followed by their long-lived triplet state. In the presence of TCNE, PET from the excited DPP-Pt(acac) and DPP to TCNE, forming the radical ion pairs. The ultrafast PET which occurs statically from DPP-Pt(acac) to TCNE in picosecond regime, is much faster than that from DPP to TCNE (nanosecond time scale) which is diffusion-controlled process, providing clear evidence that PET rate is eventually controlled by the platinum(II) incorporation.

  8. ICT4D

    Coelho, Taiane Ritta

    2014-01-01

    Resumo: Este estudo se situa no campo de ICT4D (Information and Communication Technologies for Development), termo internacionalmente conhecido para discutir o uso das Tecnologias da Informação e Comunicação (TIC) para o desenvolvimento. O que motivou o pesquisador a estudar este tema foi a existência de um paradoxo: TIC são amplamente consideradas, por uns, como invenções que mudam a maneira como milhões de pessoas conduzem suas vidas e, por outros, como alargamento das relações de poder. E ...

  9. Novel Aspects of Materials Processing by Ultrafast Lasers: From Electronic to Biological and Cultural Heritage Applications

    Materials processing by ultrafast lasers offers several distinct possibilities for micro/nano scale applications. This is due to the unique characteristics of the laser-matter interactions involved, when sub-picosecond pulses are employed. Prospects arising will be discussed in the context of surface and in bulk laser induced modifications. In particular, examples of diverse applications including the development and functionalization of laser engineered surfaces, the laser transfer of biomolecules and the functionalization of 3D structures constructed by three-photon stereolithography will be presented. Furthermore, the removal of molecular substrates by ultrafast laser ablation will be discussed with emphasis placed on assessing the photochemical changes induced in the remaining bulk material. The results indicate that in femtosecond laser processing of organic materials, besides the well acknowledged morphological advantages, a second fundamental factor responsible for its success pertains to the selective chemical effects. This is crucial for the laser cleaning of sensitive painted artworks

  10. Effects of single atom doping on the ultrafast electron dynamics of M1Au24(SR)18 (M = Pd, Pt) nanoclusters.

    Zhou, Meng; Qian, Huifeng; Sfeir, Matthew Y; Nobusada, Katsuyuki; Jin, Rongchao

    2016-03-24

    Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M1@Au24(SR)18 (M = Pd, Pt; R = CH2CH2Ph) clusters using femtosecond visible and near infrared transient absorption spectroscopy. Three relaxation components are identified for both mono-doped clusters: (1) sub-picosecond relaxation within the M1Au12 core states; (2) core to shell relaxation in a few picoseconds; and (3) relaxation back to the ground state in more than one nanosecond. Despite similar relaxation pathways for the two doped nanoclusters, the coupling between the metal core and surface ligands is accelerated by over 30% in the case of the Pt dopant compared with the Pd dopant. Compared to Pd doping, the case of Pt doping leads to much more drastic changes in the steady state and transient absorption of the clusters, which indicates that the 5d orbitals of the Pt atom are more strongly mixed with Au 5d and 6s orbitals than the 4d orbitals of the Pd dopant. These results demonstrate that a single foreign atom can lead to entirely different excited state spectral features of the whole cluster compared to the parent Au25(SR)18 cluster. The detailed excited state dynamics of atomically precise Pd/Pt doped gold clusters help further understand their properties and benefit the development of energy-related applications. PMID:26967673

  11. Applications of Ultrafast Terahertz Pulses for Intra-ExcitonicSpectroscopy of Quasi-2D Electron-Hole Gases

    Kaindl, Robert A.; Carnahan, Marc A.; Hagele, Daniel; Chemla, D.S.

    2006-09-02

    Excitons are of fundamental interest and of importance foropto-electronic applications of bulk and nano-structured semiconductors.This paper discusses the utilization of ultrafast terahertz (THz) pulsesfor the study of characteristic low-energy excitations of photoexcitedquasi 2D electron-hole (e-h) gases. Optical-pump THz-probe spectroscopyat 250-kHz repetition rate is employed to detect characteristic THzsignatures of excitons and unbound e-h pairs in GaAs quantum wells.Exciton and free-carrier densities are extracted from the data using atwo-component model. We report the detailed THz response and pairdensities for different photoexcitation energies resonant to heavy-holeexcitons, light-hole excitons, or the continuum of unbound pairs. Suchexperiments can provide quantitative insights into wavelength, time, andtemperature dependence of the low-energy response and composition ofoptically excited e-h gases in low-dimensionalsemiconductors.

  12. Transition from ultrafast laser photo-electron emission to space-charge-limited current in a 1D gap

    A one-dimensional (1D) model has been constructed to study the transition of the time-dependent ultrafast laser photo-electron emission from a flat metallic surface to the space-charge-limited (SCL) current, including the effect of non-equilibrium laser heating on metals at the ultrafast time scale. At high laser field, it is found that the space charge (SC) effect cannot be ignored and the SCL current emission is reached at a lower value predicted by a short-pulse SCL current model that has assumed a time-independent emission process. The threshold of the laser field to reach the SCL regime is determined over a wide range of operating parameters. The calculated results agree well with particle-in-cell simulation results. It is found that the SC effect is more important for materials with lower work function like tungsten (4.4 eV) as compared with gold (5.4 eV). However, for a flat surface, both materials will reach the SC limited regime at sufficient high laser field such as >5 GV m−1 with a laser pulse length of 10 s to 100 fs. (paper)

  13. Ultrafast Magnetic Light

    Makarov, Sergey V; Krasnok, Alexander E; Belov, Pavel A

    2015-01-01

    We propose a novel concept for efficient dynamic tuning of optical properties of a high refractive index subwavelength nanoparticle with a magnetic Mie-type resonance by means of femtosecond laser radiation. This concept is based on ultrafast generation of electron-hole plasma within such nanoparticle, drastically changing its transient dielectric permittivity. This allows to manipulate by both electric and magnetic nanoparticle responses, resulting in dramatic changes of its extinction cross section and scattering diagram. Specifically, we demonstrate the effect of ultrafast switching-on a Huygens source in the vicinity of the magnetic dipole resonance. This approach enables to design ultrafast and compact optical switchers and modulators based on the "ultrafast magnetic light" concept.

  14. Quantum Nuclear Dynamics Pumped and Probed by Ultrafast Polarization Controlled Steering of a Coherent Electronic State in LiH.

    Nikodem, Astrid; Levine, R D; Remacle, F

    2016-05-19

    The quantum wave packet dynamics following a coherent electronic excitation of LiH by an ultrashort, polarized, strong one-cycle infrared optical pulse is computed on several electronic states using a grid method. The coupling to the strong field of the pump and the probe pulses is included in the Hamiltonian used to solve the time-dependent Schrodinger equation. The polarization of the pump pulse allows us to control the localization in time and in space of the nonequilibrium coherent electronic motion and the subsequent nuclear dynamics. We show that transient absorption, resulting from the interaction of the total molecular dipole with the electric fields of the pump and the probe, is a very versatile probe of the different time scales of the vibronic dynamics. It allows probing both the ultrashort, femtosecond time scale of the electronic coherences as well as the longer dozens of femtoseconds time scales of the nuclear motion on the excited electronic states. The ultrafast beatings of the electronic coherences in space and in time are shown to be modulated by the different periods of the nuclear motion. PMID:26928262

  15. Coherent wavepacket motion in an ultrafast electron transfer system monitored by femtosecond degenerate four-wave-mixing and pump–probe spectroscopy

    Highlights: • Coherent wavepacket motion was investigated for ultrafast electron transfer (ET) system. • Vibrations originating from ground and excited states were extracted with high accuracy. • The dephasing of the excited state vibration was accelerated by the ultrafast ET. - Abstract: Coherent nuclear wavepacket motions were monitored by three types of femtosecond time-resolved spectroscopy, namely, transient absorption measurement utilizing white-light supercontinuum (WC-TA), degenerate four-wave-mixing (DFWM), and pump–probe (PP) measurements, for an ultrafast intermolecular electron transfer (ET) system with a dye molecule, oxazine 1 (Ox1), dissolved in an electron donating solvent, N,N-dimethylaniline (DMA). Vibrational frequencies of the wavepacket motion in the excited and in the ground states were 560–562 and 567–569 cm−1, respectively, with only a few frequency difference of 5–9 cm−1, which were clearly distinguishable by the highly accurate measurements. In DMA, the excited state wavepacket motion declined with time constant of 160–240 fs which is somewhat longer than that of the ultrafast ET; 60–80 fs

  16. Coherent wavepacket motion in an ultrafast electron transfer system monitored by femtosecond degenerate four-wave-mixing and pump–probe spectroscopy

    Nagasawa, Yutaka, E-mail: nagasawa@chem.es.osaka-u.ac.jp [Division of Frontier Materials Science, Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531 (Japan); Center for Quantum Science and Technology under Extreme Conditions, Osaka University, Toyonaka, Osaka 560-8531 (Japan); PRESTO, Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012 (Japan); Yoneda, Yusuke; Nambu, Shohei; Muramatsu, Masayasu; Takeuchi, Eisuke; Tsumori, Hiroki; Morikawa, Soichiro [Division of Frontier Materials Science, Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531 (Japan); Katayama, Tetsuro [PRESTO, Japan Science and Technology Agency (JST), Kawaguchi, Saitama 332-0012 (Japan); Miyasaka, Hiroshi [Division of Frontier Materials Science, Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531 (Japan); Center for Quantum Science and Technology under Extreme Conditions, Osaka University, Toyonaka, Osaka 560-8531 (Japan)

    2014-10-17

    Highlights: • Coherent wavepacket motion was investigated for ultrafast electron transfer (ET) system. • Vibrations originating from ground and excited states were extracted with high accuracy. • The dephasing of the excited state vibration was accelerated by the ultrafast ET. - Abstract: Coherent nuclear wavepacket motions were monitored by three types of femtosecond time-resolved spectroscopy, namely, transient absorption measurement utilizing white-light supercontinuum (WC-TA), degenerate four-wave-mixing (DFWM), and pump–probe (PP) measurements, for an ultrafast intermolecular electron transfer (ET) system with a dye molecule, oxazine 1 (Ox1), dissolved in an electron donating solvent, N,N-dimethylaniline (DMA). Vibrational frequencies of the wavepacket motion in the excited and in the ground states were 560–562 and 567–569 cm{sup −1}, respectively, with only a few frequency difference of 5–9 cm{sup −1}, which were clearly distinguishable by the highly accurate measurements. In DMA, the excited state wavepacket motion declined with time constant of 160–240 fs which is somewhat longer than that of the ultrafast ET; 60–80 fs.

  17. Monitoring Ultrafast Chemical Dynamics by Time-Domain X-ray Photo- and Auger-Electron Spectroscopy.

    Gessner, Oliver; Gühr, Markus

    2016-01-19

    The directed flow of charge and energy is at the heart of all chemical processes. Extraordinary efforts are underway to monitor and understand the concerted motion of electrons and nuclei with ever increasing spatial and temporal sensitivity. The element specificity, chemical sensitivity, and temporal resolution of ultrafast X-ray spectroscopy techniques hold great promise to provide new insight into the fundamental interactions underlying chemical dynamics in systems ranging from isolated molecules to application-like devices. Here, we focus on the potential of ultrafast X-ray spectroscopy techniques based on the detection of photo- and Auger electrons to provide new fundamental insight into photochemical processes of systems with various degrees of complexity. Isolated nucleobases provide an excellent testing ground for our most fundamental understanding of intramolecular coupling between electrons and nuclei beyond the traditionally applied Born-Oppenheimer approximation. Ultrafast electronic relaxation dynamics enabled by the breakdown of this approximation is the major component of the nucleobase photoprotection mechanisms. Transient X-ray induced Auger electron spectroscopy on photoexcited thymine molecules provides atomic-site specific details of the extremely efficient coupling that converts potentially bond changing ultraviolet photon energy into benign heat. In particular, the time-dependent spectral shift of a specific Auger band is sensitive to the length of a single bond within the molecule. The X-ray induced Auger transients show evidence for an electronic transition out of the initially excited state within only ∼200 fs in contrast to theoretically predicted picosecond population trapping behind a reaction barrier. Photoinduced charge transfer dynamics between transition metal complexes and semiconductor nanostructures are of central importance for many emerging energy and climate relevant technologies. Numerous demonstrations of photovoltaic and

  18. Ultrafast optical rotations of electron spins in an InGaAs/GaAs quantum dot ensemble

    We report on fast optical rotation operations on electron spins in a quantum dots ensemble. The spins are initialized in the z direction (quantum dot growth and light propagation direction). The spin vector oscillates about a transversal magnetic field B till a ultrafast 2π-''control'' laser pulse induces rotations of the spins about the z axis. The 2π-control pulse rotates the spin without generating a new spin polarization. The rotation angle is determined by the photon energy detuning of the control pulse from the optical resonance. For the first time for optically controlled spins, spin echoes and extension of the dephasing time were seen. By combining the rotation about the two axis a spin rotations about arbitrary axis has been realized. This robust optically controlled single spin rotation gate provides the basis for single-qubit logic operations.

  19. Optimal control of ultrafast laser driven many-electron dynamics in a polyatomic molecule: N-methyl-6-quinolone

    Klamroth, Tillmann

    2006-04-01

    We report time-dependent configuration interaction singles calculations for the ultrafast laser driven many-electron dynamics in a polyatomic molecule, N-methyl-6-quinolone. We employ optimal control theory to achieve a nearly state-selective excitation from the S0 to the S1 state, on a time scale of a few (≈6) femtoseconds. The optimal control scheme is shown to correct for effects opposing a state-selective transition, such as multiphoton transitions and other, nonlinear phenomena, which are induced by the ultrashort and intense laser fields. In contrast, simple two-level π pulses are not effective in state-selective excitations when very short pulses are used. Also, the dependence of multiphoton and nonlinear effects on the number of states included in the dynamical simulations is investigated.

  20. Photoinduced Phase Transitions in α-, θ-, and κ-type ET Salts: Ultrafast Melting of the Electronic Ordering

    Shinichiro Iwai

    2012-05-01

    Full Text Available Photoinduced phase transitions in organic compounds with strong electron correlation ET [bis(ethylenedithio-tetrathiafulvalene-based salts α-(ET2I3, θ-(ET2RbZn(SCN4, κ-(d-ET2Cu[N(CN2Br] were discussed based, on time resolved optical pump-probe spectroscopy using ~150 fs mid-infrared pulse, 12 fs near infrared pulse, and sub-picosecond terahertz pulse. (i In charge-ordered insulators α-(ET2I3 and θ-(ET2RbZn(SCN4, we captured ultrafast snapshots of charge dynamics i.e., immediate (ca. 15 fs generation of a microscopic metallic state (or equivalently the microscopic melting of the charge order which is driven by the coherent oscillation (period; 18 fs of correlated electrons. Subsequently, condensation of the microscopic metallic state to the macroscopic scale occurs in α-(ET2I3. However, in θ-(ET2RbZn(SCN4, such condensation is prevented by the large potential barrier reflecting the structural difference between the insulator and metal; (ii In a Dimer–Mott insulator κ-(d-ET2Cu[N(CN2Br], photogeneration of the metallic state rises during ca. 1 ps that is much slower than the melting of charge order, because the photoinduced insulator to metal transition is driven by the intradimer molecular displacement in the dimer Mott insulator. The ultrafast dynamics of photoinduced insulator–metal transitions depend strongly on the molecular arrangement, reflecting various competing phases in the ET sheets.

  1. Soft Route to 4D Tomography

    Taillandier-Thomas, Thibault; Roux, Stéphane; Hild, François

    2016-07-01

    Based on the assumption that the time evolution of a sample observed by computed tomography requires many less parameters than the definition of the microstructure itself, it is proposed to reconstruct these changes based on the initial state (using computed tomography) and very few radiographs acquired at fixed intervals of time. This Letter presents a proof of concept that for a fatigue cracked sample its kinematics can be tracked from no more than two radiographs in situations where a complete 3D view would require several hundreds of radiographs. This 2 order of magnitude gain opens the way to a "computed" 4D tomography, which complements the recent progress achieved in fast or ultrafast computed tomography, which is based on beam brightness, detector sensitivity, and signal acquisition technologies.

  2. Excitation-wavelength-dependent, ultrafast photoinduced electron transfer in bisferrocene/BF2-chelated-azadipyrromethene/fullerene tetrads.

    Bandi, Venugopal; El-Khouly, Mohamed E; Ohkubo, Kei; Nesterov, Vladimir N; Zandler, Melvin E; Fukuzumi, Shunichi; D'Souza, Francis

    2013-05-27

    Donor-acceptor distance, orientation, and photoexcitation wavelength are key factors in governing the efficiency and mechanism of electron-transfer reactions both in natural and synthetic systems. Although distance and orientation effects have been successfully demonstrated in simple donor-acceptor dyads, revealing excitation-wavelength-dependent photochemical properties demands multimodular, photosynthetic-reaction-center model compounds. Here, we successfully demonstrate donor- acceptor excitation-wavelength-dependent, ultrafast charge separation and charge recombination in newly synthesized, novel tetrads featuring bisferrocene, BF2 -chelated azadipyrromethene, and fullerene entities. The tetrads synthesized using multistep synthetic procedure revealed characteristic optical, redox, and photo reactivities of the individual components and featured "closely" and "distantly" positioned donor-acceptor systems. The near-IR-emitting BF2-chelated azadipyrromethene acted as a photosensitizing electron acceptor along with fullerene, while the ferrocene entities acted as electron donors. Both tetrads revealed excitation-wavelength-dependent, photoinduced, electron-transfer events as probed by femtosecond transient absorption spectroscopy. That is, formation of the Fc(+)-ADP-C60(.-) charge-separated state upon C60 excitation, and Fc(+)-ADP(.-)-C60 formation upon ADP excitation is demonstrated. PMID:23554157

  3. Nitrogen plasma formation through terahertz-induced ultrafast electron field emission

    Iwaszczuk, Krzysztof; Zalkovskij, Maksim; Strikwerda, Andrew;

    2015-01-01

    Electron microscopy and electron diffraction techniques rely on electron sources. Those sources require strong electric fields to extract electrons from metals, either by the photoelectric effect, driven by multiphoton absorption of strong laser fields, or in the static field emission regime. Ter...

  4. Role of Macromolecular Structure in the Ultrafast Energy and Electron Transfer Dynamics of a Light-Harvesting Polymer.

    Morseth, Zachary A; Pho, Toan V; Gilligan, Alexander T; Dillon, Robert J; Schanze, Kirk S; Reynolds, John R; Papanikolas, John M

    2016-08-18

    Ultrafast energy and electron transfer (EnT and ET, respectively) are characterized in a light-harvesting assembly based on a π-conjugated polymer (poly(fluorene)) functionalized with broadly absorbing pendant organic isoindigo (iI) chromophores using a combination of femtosecond transient absorption spectroscopy and large-scale computer simulation. Photoexcitation of the π-conjugated polymer leads to near-unity quenching of the excitation through a combination of EnT and ET to the iI pendants. The excited pendants formed by EnT rapidly relax within 30 ps, whereas recombination of the charge-separated state formed following ET occurs within 1200 ps. A computer model of the excited-state processes is developed by combining all-atom molecular dynamics simulations, which provides a molecular-level view of the assembly structure, with a kinetic model that accounts for the multiple excited-state quenching pathways. Direct comparison of the simulations with experimental data reveals that the underlying structure has a dramatic effect on the partitioning between EnT and ET in the polymer assembly, where the distance and orientation of the pendants in relation to the backbone serve to direct the dominant quenching pathway. PMID:27433946

  5. A simple electron time-of-flight spectrometer for ultrafast vacuum ultraviolet photoelectron spectroscopy of liquid solutions

    We present a simple electron time of flight spectrometer for time resolved photoelectron spectroscopy of liquid samples using a vacuum ultraviolet (VUV) source produced by high-harmonic generation. The field free spectrometer coupled with the time-preserving monochromator for the VUV at the Artemis facility of the Rutherford Appleton Laboratory achieves an energy resolution of 0.65 eV at 40 eV with a sub 100 fs temporal resolution. A key feature of the design is a differentially pumped drift tube allowing a microliquid jet to be aligned and started at ambient atmosphere while preserving a pressure of 10−1 mbar at the micro channel plate detector. The pumping requirements for photoelectron (PE) spectroscopy in vacuum are presented, while the instrument performance is demonstrated with PE spectra of salt solutions in water. The capability of the instrument for time resolved measurements is demonstrated by observing the ultrafast (50 fs) vibrational excitation of water leading to temporary proton transfer

  6. Direct observation of ultrafast-electron-transfer reactions unravels high effectiveness of reductive DNA damage

    Nguyen, Jenny; Ma, Yuhan; Luo, Ting; Bristow, Robert G; Jaffray, David A; Lu, Qing-Bin

    2011-01-01

    Both water and electron-transfer reactions play important roles in chemistry, physics, biology, and the environment. Oxidative DNA damage is a well-known mechanism, whereas the relative role of reductive DNA damage is unknown. The prehydrated electron (), a novel species of electrons in water, is a fascinating species due to its fundamental importance in chemistry, biology, and the environment. is an ideal agent to observe reductive DNA damage. Here, we report both the first in situ femtosec...

  7. Tuning of Near- and Far-Field Properties of All-dielectric Dimer Nanoantennas via Ultrafast Electron-Hole Plasma Photoexcitation

    Baranov, Denis G; Krasnok, Alexander E; Belov, Pavel A; Alu, Andrea

    2016-01-01

    Achievement of all-optical ultrafast signal modulation and routing by a low-loss nanodevice is a crucial step towards an ultracompact optical chip with high performance. Here, we propose a specifically designed silicon dimer nanoantenna, which is tunable via photoexcitation of dense electron-hole plasma with ultrafast relaxation rate. Basing on this concept, we demonstrate the effect of beam steering up to 20 degrees via simple variation of incident intensity, being suitable for ultrafast light routing in an optical chip. The effect is demonstrated both in the visible and near-IR spectral regions for silicon and germanium based nanoantennas. We also reveal the effect of electron-hole plasma photoexcitation on local density of states (LDOS) in the dimer gap and find that the orientation averaged LDOS can be altered by 50\\%, whereas modification of the projected LDOS can be even more dramatic: almost 500\\% for transverse dipole orientation. Moreover, our analytical model sheds light on transient dynamics of the...

  8. Coherent phonons in CdSe quantum dots triggered by ultrafast electron transfer

    Wachtveitl J.

    2013-03-01

    Full Text Available The origin of coherent oscillations in CdSe quantum dots and in the CdSe/methylviologen electron transfer system is studied. In CdSe/methylviologen coherent phonons are triggered by the electron transfer from the quantum dot to methylviologen.

  9. Modeling time-coincident ultrafast electron transfer and solvation processes at molecule-semiconductor interfaces

    Kinetic models based on Fermi's Golden Rule are commonly employed to understand photoinduced electron transfer dynamics at molecule-semiconductor interfaces. Implicit in such second-order perturbative descriptions is the assumption that nuclear relaxation of the photoexcited electron donor is fast compared to electron injection into the semiconductor. This approximation breaks down in systems where electron transfer transitions occur on 100-fs time scale. Here, we present a fourth-order perturbative model that captures the interplay between time-coincident electron transfer and nuclear relaxation processes initiated by light absorption. The model consists of a fairly small number of parameters, which can be derived from standard spectroscopic measurements (e.g., linear absorbance, fluorescence) and/or first-principles electronic structure calculations. Insights provided by the model are illustrated for a two-level donor molecule coupled to both (i) a single acceptor level and (ii) a density of states (DOS) calculated for TiO2 using a first-principles electronic structure theory. These numerical calculations show that second-order kinetic theories fail to capture basic physical effects when the DOS exhibits narrow maxima near the energy of the molecular excited state. Overall, we conclude that the present fourth-order rate formula constitutes a rigorous and intuitive framework for understanding photoinduced electron transfer dynamics that occur on the 100-fs time scale

  10. Investigation of ultrafast electron dynamics of nickel film and micro-nano-structure film

    Weifeng Jin; Ming Zhou; Changlong Liu; Hui Wang; Huixia Liu; Naifei Ren

    2009-01-01

    The electron thermalization and relaxation processes in ferromagnetic nickel thin film and micro-nano-structure film have been studied by measuring the transient change after excitation by a femtosecond laser pulse. The measurements indicate that the electron thermalization time is between 18 and 47 fs. This is somewhat faster than the value reported before. And the thermalization time of the micro-nano-structure film is much longer than the nickel film. We deduce that it is caused by the discontinuity of the electron band close to the Fermi level in the micro-nano-structure nickel film.

  11. Laser-induced ultrafast electron emission from a field emission tip

    Barwick, B; Chandler-Smith, N; Corder, C; Strohaber, J; Uiterwaal, C; Barwick, Brett; Batelaan, Herman; Chandler-Smith, Nate; Corder, Chris; Strohaber, James; Uiterwaal, Cornelis

    2007-01-01

    We show that a field emission tip electron source that is triggered with a femtosecond laser pulse can generate electron pulses shorter than the laser pulse duration (~100 fs). The emission process is sensitive to a power law of the laser intensity, which supports an emission mechanism based on multiphoton absorption followed by over-the-barrier emission. Observed continuous transitions between power laws of different orders are indicative of field emission processes. We show that the source can also be operated so that thermionic emission processes become significant. Understanding these different emission processes is relevant for the production of sub-cycle electron pulses.

  12. Electronic structure near the Fermi level in the ferromagnetic semiconductor GaMnAs studied by ultrafast time-resolved light-induced reflectivity measurements

    Ishii, Tomoaki; Kawazoe, Tadashi; Hashimoto, Yusuke; Terada, Hiroshi; Muneta, Iriya; Ohtsu, Motoichi; Tanaka, Masaaki; Ohya, Shinobu

    2016-06-01

    Clarification of the electronic structure near the Fermi level is important in understanding the origin of ferromagnetism in the prototypical ferromagnetic semiconductor GaMnAs. Here, we perform ultrafast transient reflectivity spectra measurement, which is a powerful tool for selective detection of absorption edges in GaMnAs. The results show that the Fermi level of GaMnAs exists in the band gap. By using the Kramers-Kronig relation, we find the Mn-induced electronic states around the Fermi level, confirming that the ferromagnetism is stabilized by spin-polarized impurity-band holes.

  13. On the recollision-free excitation of krypton during ultrafast multi-electron tunnel ionization

    The probability of multiple ionization of krypton by 50 femtosecond circularly polarized laser pulses, independent of the optical focal geometry, has been obtained for the first time. The excellent agreement over the intensity range 100 TW cm-2 to 100 PW cm-2 with the recent predictions of Kornev et al (2003 Phys. Rev. A 68 043414) provides the first experimental confirmation that non-recollisional electronic excitation can occur in strong-field ionization. This is particularly true for higher stages of ionization, when the laser intensity exceeds 10 PW cm-2 as the energetic departure of the ionized electron(s) diabatically distorts the wavefunctions of the bound electrons. By scaling the probability of ionization by the focal volume, we discuss why this mechanism was not apparent in previous studies

  14. Ultrafast insulator-metal transition in VO2: interplay between coherent lattice motion and electronic correlations

    The multi-THz conductivity of VO2 recorded during a photoinduced insulator-metal transition directly reveals the femtosecond dynamics of V-V stretching modes and electronic correlations. The strongly correlated character of the electronic system leads to a transient behaviour of the conductivity that cannot be understood in a Born-Oppenheimer picture. Based on our measurements with a time resolution of 12 fs and recent theoretical simulations for the electronic structure in steady state, we suggest a novel qualitative model for the non-thermal phase transition. The extremely high speed for the photoinduced phase transition is elegantly explained via a directed wave packet motion in the electronically excited state of the dimer that transfers the crystal structure of the insulator into the configuration of the metallic phase. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  15. Roadmap on ultrafast optics

    Reid, Derryck T.; Heyl, Christoph M.; Thomson, Robert R.; Trebino, Rick; Steinmeyer, Günter; Fielding, Helen H.; Holzwarth, Ronald; Zhang, Zhigang; Del’Haye, Pascal; Südmeyer, Thomas; Mourou, Gérard; Tajima, Toshiki; Faccio, Daniele; Harren, Frans J. M.; Cerullo, Giulio

    2016-09-01

    The year 2015 marked the 25th anniversary of modern ultrafast optics, since the demonstration of the first Kerr lens modelocked Ti:sapphire laser in 1990 (Spence et al 1990 Conf. on Lasers and Electro-Optics, CLEO, pp 619–20) heralded an explosion of scientific and engineering innovation. The impact of this disruptive technology extended well beyond the previous discipline boundaries of lasers, reaching into biology labs, manufacturing facilities, and even consumer healthcare and electronics. In recognition of such a milestone, this roadmap on Ultrafast Optics draws together articles from some of the key opinion leaders in the field to provide a freeze-frame of the state-of-the-art, while also attempting to forecast the technical and scientific paradigms which will define the field over the next 25 years. While no roadmap can be fully comprehensive, the thirteen articles here reflect the most exciting technical opportunities presented at the current time in Ultrafast Optics. Several articles examine the future landscape for ultrafast light sources, from practical solid-state/fiber lasers and Raman microresonators to exotic attosecond extreme ultraviolet and possibly even zeptosecond x-ray pulses. Others address the control and measurement challenges, requiring radical approaches to harness nonlinear effects such as filamentation and parametric generation, coupled with the question of how to most accurately characterise the field of ultrafast pulses simultaneously in space and time. Applications of ultrafast sources in materials processing, spectroscopy and time-resolved chemistry are also discussed, highlighting the improvements in performance possible by using lasers of higher peak power and repetition rate, or by exploiting the phase stability of emerging new frequency comb sources.

  16. Relaxation and excitation electronic processes in dielectrics irradiated by ultrafast IR and VUV pulses

    We studied excitation and relaxation of electrons involved during interaction of visible and VUV femtosecond pulses with dielectrics. The generated population of hot electrons, having energy of few eV to few tens of eV above the bottom of the conduction band, is responsible of phenomena ranging to defect creation to optical breakdown. Owing to two techniques: photoemission and transient photoconductivity we improve the understanding of the The first photoemission experiments deal with dielectrics irradiated by 30 fs IR pulses. The photoemission spectra measured show a large population of electrons which energy rise up to 40 eV. We interpret this result in terms of a new absorption process: direct multi-photons inter-branch transitions. The 2. type of photoemission experiments are time resolved 'pump/probe' investigation. We study the relaxation of electrons excited by a VUV pulses. We used the high order harmonics (HOH) as light sources. We found surprisingly long decay time in the range of ps timescale. Last type of experiments is photoconductivity studies of diamond samples. Using HOH as light source we measure the displacement current induced by excited electrons in the conduction band. Those electrons relax mainly by impact ionisation creating secondary electrons. Hence by probing the number of electrons we were able to measure the efficiency of these relaxation processes. We observe a diminution of this efficiency when the energy of exciting photons is above 20 eV. Owing to Monte-Carlo simulation we interpret this result in terms of band structure effect. (author)

  17. Ultrafast Phase Transition in Vanadium Dioxide Driven by Hot-Electron Injection

    Prasankumar R. P.

    2013-03-01

    Full Text Available We present a novel all-optical method of triggering the phase transition in vanadium dioxide by means of ballistic electrons injected across the interface between a mesh of Au nanoparticles coveringd VO2 nanoislands. By performing non-degenerate pump-probe transmission spectroscopy on this hybrid plasmonic/phase-changing nanostructure, structural and electronic dynamics can be retrieved and compared.

  18. Laser-induced ultrafast electron emission from a field emission tip

    Barwick, Brett; Corder, Chris; Strohaber, James; Chandler-Smith, Nate; Uiterwaal, Cornelis; Batelaan, Herman

    2007-01-01

    We show that a field emission tip electron source that is triggered with a femtosecond laser pulse can generate electron pulses shorter than the laser pulse duration (~100 fs). The emission process is sensitive to a power law of the laser intensity, which supports an emission mechanism based on multiphoton absorption followed by over-the-barrier emission. Observed continuous transitions between power laws of different orders are indicative of field emission processes. We show that the source ...

  19. Finite-size and nonlinear effects on the ultrafast electron transport in thin metal films

    Manfredi, G.; Hervieux, P.-A.

    2005-10-01

    Self-consistent simulations of the electron dynamics and transport in thin metal films are performed using a semiclassical Vlasov-Poisson model. The Vlasov equation is solved using an accurate Eulerian scheme that preserves the fermionic character of the electron distribution. Although the thermodynamical properties of the ground state are accurately described by the bulk theory, the dynamical properties are strongly influenced by the finite size of the system and the presence of surfaces. Our results show that (i) heat transport is ballistic and occurs at a velocity close to the Fermi speed; (ii) after the excitation energy has been absorbed by the film, slow nonlinear oscillations appear, with a period proportional to the film thickness, which are attributed to nonequilibrium electrons bouncing back and forth on the film surfaces; (iii) except for trivial scaling factors, the above transport properties are insensitive to the excitation energy and the initial electron temperature. Finally, the coupling to the ion dynamics and the impact of electron-electron collisions are also investigated.

  20. Ultrafast Electron Transfer Kinetics in the LM Dimer of Bacterial Photosynthetic Reaction Center from Rhodobacter sphaeroides.

    Sun, Chang; Carey, Anne-Marie; Gao, Bing-Rong; Wraight, Colin A; Woodbury, Neal W; Lin, Su

    2016-06-23

    It has become increasingly clear that dynamics plays a major role in the function of many protein systems. One system that has proven particularly facile for studying the effects of dynamics on protein-mediated chemistry is the bacterial photosynthetic reaction center from Rhodobacter sphaeroides. Previous experimental and computational analysis have suggested that the dynamics of the protein matrix surrounding the primary quinone acceptor, QA, may be particularly important in electron transfer involving this cofactor. One can substantially increase the flexibility of this region by removing one of the reaction center subunits, the H-subunit. Even with this large change in structure, photoinduced electron transfer to the quinone still takes place. To evaluate the effect of H-subunit removal on electron transfer to QA, we have compared the kinetics of electron transfer and associated spectral evolution for the LM dimer with that of the intact reaction center complex on picosecond to millisecond time scales. The transient absorption spectra associated with all measured electron transfer reactions are similar, with the exception of a broadening in the QX transition and a blue-shift in the QY transition bands of the special pair of bacteriochlorophylls (P) in the LM dimer. The kinetics of the electron transfer reactions not involving quinones are unaffected. There is, however, a 4-fold decrease in the electron transfer rate from the reduced bacteriopheophytin to QA in the LM dimer compared to the intact reaction center and a similar decrease in the recombination rate of the resulting charge-separated state (P(+)QA(-)). These results are consistent with the concept that the removal of the H-subunit results in increased flexibility in the region around the quinone and an associated shift in the reorganization energy associated with charge separation and recombination. PMID:27243380

  1. X-Ray imaging of ultrafast magnetic reconnection driven by relativistic electrons

    Raymond, A.; McKelvey, A.; Zulick, C.; Maksimchuk, A.; Thomas, A. G. R.; Willingale, L.; Chykov, V.; Yanovsky, V.; Krushelnick, K.

    2015-05-01

    Evidence of magnetic reconnection (MR) events driven by relativistic electrons is observed between two high-intensity laser/plasma interaction sites. The two laser foci were on average 20um FWHM containing 50TW of power each, delivered with a split f/3 paraboloid onto copper foil targets at a focused intensity of 1019 W/cm2 with the HERCULES laser system. Cu K-alpha emissions from the interactions were imaged with a spherically bent Quartz crystal, and by motorizing one half of the paraboloid vertically the focal separation was varied between 0- 400um. Splitting the beam halves revealed an enhanced region between the foci with the highest a maximized K-alpha signal intensity at one inter-beam separation, evidencing inflow from relativistic electron driven MR. A filtered LANEX screen was imaged to search for outflow/jet electrons along the plane of the target surface and normal to the axis defined by the two spots, to calculate the electron temperature and to search for spatial profile nonuniformities potentially directly originating from reconnection events. Ongoing 2D and 3D PIC simulations are being conducted to better understand and model the measured electron outflow dynamics.

  2. Synthesis, optical properties and ultrafast electronic relaxation of metal (silver, gold, platinum) and manganese(2+)-doped zinc sulfide nanoparticles

    Smith, Brian Ampere

    Ultrafast transient absorption and time-dependent luminescence spectroscopy have been performed on metal (Ag, Au, Pt) and semiconductor (Mn2+ doped ZnS) nanoparticles respectively. In metal nanoparticles it was found that the decay dynamics exhibit a complex size and surface dependence. Specifically, the photoinduced dynamics show an exponential time constant that is longer than the same in bulk for particle sizes of 4-40 nm. When particle size is reduced further the plasmon band is drastically broadened and the relaxation time constant is similar to bulk. Upon reducing the size still further to only 13 atoms per cluster a much longer electronic relaxation is observed. These results are attributed to an intrinsic size dependent reduction in the electron-phonon coupling when particle size is reduced. This slows down the electronic relaxation compared to bulk. The increase in the number of surface collisions for very small particles increases the rate of electronic relaxation relative to larger particles. For particles on the order of 13 atoms the excitation is more singular in nature and the long relaxation is attributed to the fact that the excited species is a molecular as opposed to a fermi system. Also, the synthesis and luminescence decay kinetics of 1.2 nm Mn 2+ doped ZnS nanoclusters grown in reverse micelles are reported. The preparation method produces small particles with narrow size distribution and fluorescence bands near 400-450 nm and 585 nm. Time-dependent fluorescence decay measurements using picosecond, nanosecond and millisecond techniques reveal relaxation processes on all three time scales. In the doped sample, the red emission detected at 600 nm exhibits an 1-2 ms decay in addition to faster decays with time constants on the order of hundreds of ps, a few ns and tens of μs. While the slow decay is the same as that of bulk Mn 2+ doped ZnS, the fast decays are present for both doped and undoped samples and are unique to nanocluster ZnS, which are

  3. Ultrafast Electron Transfer at Organic Semiconductor Interfaces: Importance of Molecular Orientation

    Ayzner, Alexander L.

    2015-01-02

    © 2014 American Chemical Society. Much is known about the rate of photoexcited charge generation in at organic donor/acceptor (D/A) heterojunctions overaged over all relative arrangements. However, there has been very little experimental work investigating how the photoexcited electron transfer (ET) rate depends on the precise relative molecular orientation between D and A in thin solid films. This is the question that we address in this work. We find that the ET rate depends strongly on the relative molecular arrangement: The interface where the model donor compound copper phthalocyanine is oriented face-on with respect to the fullerene C60 acceptor yields a rate that is approximately 4 times faster than that of the edge-on oriented interface. Our results suggest that the D/A electronic coupling is significantly enhanced in the face-on case, which agrees well with theoretical predictions, underscoring the importance of controlling the relative interfacial molecular orientation.

  4. Ultrafast geometric manipulation of electron spin and detection of the geometric phase via Faraday rotation spectroscopy

    Li Xue Qian; Cen, L X; Zheng, H Z; Yan, Y J; Li, Xin-Qi; Hu, Cheng-Yong; Cen, Li-Xiang; Zheng, Hou-Zhi; Yan, YiJing

    2002-01-01

    Time-resolved Faraday rotation spectroscopy is currently exploited as a powerful technique to probe spin dynamics in semiconductors. We propose here an all-optical approach to geometrically manipulate electron spin and to detect the geometric phase by this type of extremely sensitive experiment. The global nature of the geometric phase can make the quantum manipulation more stable, which may find interesting application in quantum devices.

  5. Ultrafast electron transfer reactions initiated by excited CT states of push pull perylenes

    Miller, Scott E.; Zhao, Yongyu; Schaller, Richard; Mulloni, Viviana; Just, Eric M.; Johnson, Robert C.; Wasielewski, Michael R.

    2002-01-01

    Two new chromophores that absorb in the visible spectrum, the 9-( N-pyrrolidinyl)- and 9-( N-piperidinyl)perylene-3,4-dicarboximides, 5PMI and 6PMI, respectively, were synthesized and shown to possess lowest excited singlet states with about 70% charge transfer (CT) character. Changing the ring size of the cyclic amine from 5 to 6 significantly changes the energies of the CT states, as well as the redox potentials of the chromophores. These chromophores were linked to pyromellitimide (PI) and 1,8:4,5-naphthalenediimide (NI) electron acceptors using a single N-N bond between their respective imides to yield the corresponding donor-acceptor dyads 5PMI-PI, 5PMI-NI, 6PMI-PI, and 6PMI-NI. The donors and acceptors in these molecules are positioned relative to one another in a rod-like arrangement at fixed distances and restricted orientations. The rates of charge separation and recombination were measured using transient absorption spectroscopy. These chromophores were also used to prepare rigid donor-acceptor triads 5PMI-PI-NI and 6PMI-PI-NI, which display one- or two-step electron transfer mechanisms that depend on solvent polarity. These compounds exhibit a broad range of structure and media driven changes in electron transfer mechanism.

  6. Breaking the Attosecond, Angstrom and TV/M Field Barriers with Ultra-Fast Electron Beams

    Rosenzweig, James; Andonian, Gerard; Fukasawa, Atsushi; Hemsing, Erik; Marcus, Gabriel; Marinelli, Agostino; Musumeci, Pietro; O' Shea, Brendan; O' Shea, Finn; Pellegrini, Claudio; Schiller, David; Travish, Gil; /UCLA; Bucksbaum, Philip; Hogan, Mark; Krejcik, Patrick; /SLAC; Ferrario, Massimo; /INFN, Rome; Full, Steven; /Penn State U.; Muggli, Patric; /Southern California U.

    2012-06-22

    Recent initiatives at UCLA concerning ultra-short, GeV electron beam generation have been aimed at achieving sub-fs pulses capable of driving X-ray free-electron lasers (FELs) in single-spike mode. This use of very low Q beams may allow existing FEL injectors to produce few-100 attosecond pulses, with very high brightness. Towards this end, recent experiments at the LCLS have produced {approx}2 fs, 20 pC electron pulses. We discuss here extensions of this work, in which we seek to exploit the beam brightness in FELs, in tandem with new developments in cryogenic undulator technology, to create compact accelerator-undulator systems that can lase below 0.15 {angstrom}, or be used to permit 1.5 {angstrom} operation at 4.5 GeV. In addition, we are now developing experiments which use the present LCLS fs pulses to excite plasma wakefields exceeding 1 TV/m, permitting a table-top TeV accelerator for frontier high energy physics applications.

  7. Ultrafast electronic and vibrational dynamics in brominated aluminum corroles: Energy relaxation and triplet formation

    T. Stensitzki

    2016-07-01

    Full Text Available We combined femtosecond (fs VIS pump–IR probe spectroscopy with fs VIS pump–supercontinuum probe spectroscopy to characterize the photoreaction of the hexacoordinated Al(tpfc-Br8(py2 in a comprehensive way. Upon fs excitation at ∼400 nm in the Soret band, the excitation energy relaxes with a time constant of (250 ± 80 fs to the S2 and S1 electronic excited states. This is evident from the rise time of the stimulated emission signal in the visible spectral range. On the same time scale, narrowing of broad infrared signals in the C=C stretching region around 1500 cm−1 is observed. Energy redistribution processes are visible in the vibrational and electronic dynamics with time constants between ∼2 ps and ∼20 ps. Triplet formation is detected with a time constant of (95 ± 3 ps. This is tracked by the complete loss of stimulated emission. Electronic transition of the emerging triplet absorption band overlaps considerably with the singlet excited state absorption. In contrast, two well separated vibrational marker bands for triplet formation were identified at 1477 cm−1 and at 1508 cm−1. These marker bands allow a precise identification of triplet dynamics in corrole systems.

  8. Ultrafast electronic and vibrational dynamics in brominated aluminum corroles: Energy relaxation and triplet formation.

    Stensitzki, T; Yang, Y; Berg, A; Mahammed, A; Gross, Z; Heyne, K

    2016-07-01

    We combined femtosecond (fs) VIS pump-IR probe spectroscopy with fs VIS pump-supercontinuum probe spectroscopy to characterize the photoreaction of the hexacoordinated Al(tpfc-Br8)(py)2 in a comprehensive way. Upon fs excitation at ∼400 nm in the Soret band, the excitation energy relaxes with a time constant of (250 ± 80) fs to the S2 and S1 electronic excited states. This is evident from the rise time of the stimulated emission signal in the visible spectral range. On the same time scale, narrowing of broad infrared signals in the C=C stretching region around 1500 cm(-1) is observed. Energy redistribution processes are visible in the vibrational and electronic dynamics with time constants between ∼2 ps and ∼20 ps. Triplet formation is detected with a time constant of (95 ± 3) ps. This is tracked by the complete loss of stimulated emission. Electronic transition of the emerging triplet absorption band overlaps considerably with the singlet excited state absorption. In contrast, two well separated vibrational marker bands for triplet formation were identified at 1477 cm(-1) and at 1508 cm(-1). These marker bands allow a precise identification of triplet dynamics in corrole systems. PMID:27226980

  9. Electron diffraction using ultrafast electron bunches from a laser-wakefield accelerator at kHz repetition rate

    He, Z.-H; Thomas, A. G. R.; Beaurepaire, B; Nees, J. A.; Hou, B.; Malka, Victor; Krushelnick, K; Faure, Jérôme

    2013-01-01

    We show that electron bunches in the 50-100 keV range can be produced from a laser wake-field accelerator using 10 mJ, 35 fs laser pulses operating at 0.5 kHz. It is shown that using a solenoid magnetic lens, the electron bunch distribution can be shaped. The resulting transverse and longitudinal coherence is suitable for producing diffraction images from a polycrystalline 10 nm aluminum foil. The high repetition rate, the stability of the electron source and the fact that its uncorrelated bu...

  10. Endstation for ultrafast magnetic scattering experiments at the free-electron laser in Hamburg

    MÜller, L.; Gutt, C.; Eisebitt, S.; Kobs, A.; Hille, M.; Stickler, D.; Frömter, R.; Oepen, H.P.; Lüning, J.; Gruebel, Gerhard; Streit-Nierobisch, S.; Walther, M.; Schaffert, S.; Pfau, B.; Geilhufe, J.

    2013-01-01

    An endstation for pump–probe small-angle X-ray scattering (SAXS) experiments at the free-electron laser in Hamburg (FLASH) is presented. The endstation houses a solid-state absorber, optical incoupling for pump–probe experiments, time zero measurement, sample chamber, and detection unit. It can be used at all FLASH beamlines in the whole photon energy range offered by FLASH. The capabilities of the setup are demonstrated by showing the results of resonant magnetic SAXS measurements on cobalt-...

  11. Endstation for ultrafast magnetic scattering experiments at the free-electron laser in Hamburg.

    Müller, L; Gutt, C; Streit-Nierobisch, S; Walther, M; Schaffert, S; Pfau, B; Geilhufe, J; Büttner, F; Flewett, S; Günther, C M; Eisebitt, S; Kobs, A; Hille, M; Stickler, D; Frömter, R; Oepen, H P; Lüning, J; Grübel, G

    2013-01-01

    An endstation for pump-probe small-angle X-ray scattering (SAXS) experiments at the free-electron laser in Hamburg (FLASH) is presented. The endstation houses a solid-state absorber, optical incoupling for pump-probe experiments, time zero measurement, sample chamber, and detection unit. It can be used at all FLASH beamlines in the whole photon energy range offered by FLASH. The capabilities of the setup are demonstrated by showing the results of resonant magnetic SAXS measurements on cobalt-platinum multilayer samples grown on freestanding Si(3)N(4) membranes and pump-laser-induced grid structures in multilayer samples. PMID:23387667

  12. Ultrafast electron crystallography of the cooperative reaction path in vanadium dioxide

    Ding-Shyue Yang

    2016-05-01

    Full Text Available Time-resolved electron diffraction with atomic-scale spatial and temporal resolution was used to unravel the transformation pathway in the photoinduced structural phase transition of vanadium dioxide. Results from bulk crystals and single-crystalline thin-films reveal a common, stepwise mechanism: First, there is a femtosecond V−V bond dilation within 300 fs, second, an intracell adjustment in picoseconds and, third, a nanoscale shear motion within tens of picoseconds. Experiments at different ambient temperatures and pump laser fluences reveal a temperature-dependent excitation threshold required to trigger the transitional reaction path of the atomic motions.

  13. Endstation for ultrafast magnetic scattering experiments at the free-electron laser in Hamburg

    An endstation for pump–probe small-angle X-ray scattering (SAXS) experiments at the free-electron laser in Hamburg (FLASH) is presented. The endstation houses a solid-state absorber, optical incoupling for pump–probe experiments, time zero measurement, sample chamber, and detection unit. It can be used at all FLASH beamlines in the whole photon energy range offered by FLASH. The capabilities of the setup are demonstrated by showing the results of resonant magnetic SAXS measurements on cobalt-platinum multilayer samples grown on freestanding Si3N4 membranes and pump-laser-induced grid structures in multilayer samples.

  14. Ultrafast probing of the x-ray-induced lattice and electron dynamics in graphite at atomic-resolution

    Hau-Riege, S

    2010-10-07

    We used LCLS pulses to excite thin-film and bulk graphite with various different microstructures, and probed the ultrafast ion and electron dynamics through Bragg and x-ray Thomson scattering (XRTS). We pioneered XRTS at LCLS, making this technique viable for other users. We demonstrated for the first time that the LCLS can be used to characterize warm-dense-matter through Bragg and x-ray Thomson scattering. The warm-dense-matter conditions were created using the LCLS beam. Representative examples of the results are shown in the Figure above. In our experiment, we utilized simultaneously both Bragg and two Thomson spectrometers. The Bragg measurements as a function of x-ray fluence and pulse length allows us to characterize the onset of atomic motion at 2 keV with the highest resolution to date. The Bragg detector was positioned in back-reflection, providing us access to scattering data with large scattering vectors (nearly 4{pi}/{lambda}). We found a clear difference between the atomic dynamics for 70 and 300 fs pulses, and we are currently in the process of comparing these results to our models. The outcome of this comparison will have important consequences for ultrafast diffractive imaging, for which it is still not clear if atomic resolution can truly be achieved. The backward x-ray Thomson scattering data suggests that the average graphite temperature and ionization was 10 eV and 1.0, respectively, which agrees with our models. In the forward scattering data, we observed an inelastic feature in the Thomson spectrum that our models currently do not reproduce, so there is food for thought. We are in the process of writing these results up. Depending on if we can combine the Bragg and Thomson data or not, we plan to publish them in a single paper (e.g. Nature or Science) or as two separate papers (e.g. two Phys. Rev. Lett.). We will present the first analysis of the results at the APS Plasma Meeting in November 2010. We had a fantastic experience performing our

  15. Spot profile analysis and lifetime mapping in ultrafast electron diffraction: Lattice excitation of self-organized Ge nanostructures on Si(001

    T. Frigge

    2015-05-01

    Full Text Available Ultrafast high energy electron diffraction in reflection geometry is employed to study the structural dynamics of self-organized Germanium hut-, dome-, and relaxed clusters on Si(001 upon femtosecond laser excitation. Utilizing the difference in size and strain state the response of hut- and dome clusters can be distinguished by a transient spot profile analysis. Surface diffraction from {105}-type facets provide exclusive information on hut clusters. A pixel-by-pixel analysis of the dynamics of the entire diffraction pattern gives time constants of 40, 160, and 390 ps, which are assigned to the cooling time constants for hut-, dome-, and relaxed clusters.

  16. Ultrafast triggered transient energy storage by atomic layer deposition into porous silicon for integrated transient electronics

    Douglas, Anna; Muralidharan, Nitin; Carter, Rachel; Share, Keith; Pint, Cary L.

    2016-03-01

    Here we demonstrate the first on-chip silicon-integrated rechargeable transient power source based on atomic layer deposition (ALD) coating of vanadium oxide (VOx) into porous silicon. A stable specific capacitance above 20 F g-1 is achieved until the device is triggered with alkaline solutions. Due to the rational design of the active VOx coating enabled by ALD, transience occurs through a rapid disabling step that occurs within seconds, followed by full dissolution of all active materials within 30 minutes of the initial trigger. This work demonstrates how engineered materials for energy storage can provide a basis for next-generation transient systems and highlights porous silicon as a versatile scaffold to integrate transient energy storage into transient electronics.Here we demonstrate the first on-chip silicon-integrated rechargeable transient power source based on atomic layer deposition (ALD) coating of vanadium oxide (VOx) into porous silicon. A stable specific capacitance above 20 F g-1 is achieved until the device is triggered with alkaline solutions. Due to the rational design of the active VOx coating enabled by ALD, transience occurs through a rapid disabling step that occurs within seconds, followed by full dissolution of all active materials within 30 minutes of the initial trigger. This work demonstrates how engineered materials for energy storage can provide a basis for next-generation transient systems and highlights porous silicon as a versatile scaffold to integrate transient energy storage into transient electronics. Electronic supplementary information (ESI) available: (i) Experimental details for ALD and material fabrication, ellipsometry film thickness, preparation of gel electrolyte and separator, details for electrochemical measurements, HRTEM image of VOx coated porous silicon, Raman spectroscopy for VOx as-deposited as well as annealed in air for 1 hour at 450 °C, SEM and transient behavior dissolution tests of uniformly coated VOx on

  17. Ultrafast electron, lattice and spin dynamics on rare earth metal surfaces. Investigated with linear and nonlinear optical techniques

    Radu, I.E.

    2006-03-15

    This thesis presents the femtosecond laser-induced electron, lattice and spin dynamics on two representative rare-earth systems: The ferromagnetic gadolinium Gd(0001) and the paramagnetic yttrium Y(0001) metals. The employed investigation tools are the time-resolved linear reflectivity and second-harmonic generation, which provide complementary information about the bulk and surface/interface dynamics, respectively. The femtosecond laser excitation of the exchange-split surface state of Gd(0001) triggers simultaneously the coherent vibrational dynamics of the lattice and spin subsystems in the surface region at a frequency of 3 THz. The coherent optical phonon corresponds to the vibration of the topmost atomic layer against the underlying bulk along the normal direction to the surface. The coupling mechanism between phonons and magnons is attributed to the modulation of the exchange interaction J between neighbour atoms due to the coherent lattice vibration. This leads to an oscillatory motion of the magnetic moments having the same frequency as the lattice vibration. Thus these results reveal a new type of phonon-magnon coupling mediated by the modulation of the exchange interaction and not by the conventional spin-orbit interaction. Moreover, we show that coherent spin dynamics in the THz frequency domain is achievable, which is at least one order of magnitude faster than previously reported. The laser-induced (de)magnetization dynamics of the ferromagnetic Gd(0001) thin films have been studied. Upon photo-excitation, the nonlinear magneto-optics measurements performed in this work show a sudden drop in the spin polarization of the surface state by more than 50% in a <100 fs time interval. Under comparable experimental conditions, the time-resolved photoemission studies reveal a constant exchange splitting of the surface state. The ultrafast decrease of spin polarization can be explained by the quasi-elastic spin-flip scattering of the hot electrons among spin

  18. Femtosecond excitations in metallic nanostructures. From ultrafast light confinement to a local electron source

    Ropers, C.

    2007-07-11

    This thesis contributes to the understanding of optical excitations in metallic nanostructures. In experiments on selected model structures, the dynamics of these excitations and their electromagnetic spatial modes are investigated with femtosecond temporal and nanometer spatial resolution, respectively. Angle- and time-resolved transmission experiments on metallic thin film gratings demonstrate the dominant role resonant surface plasmon polaritons (SPPs) play in the optical properties of such structures. The lifetimes of these excitations are determined, and it is shown that coherent couplings among SPP-resonances result in drastic lifetime modifications. Near the visible part of the spectrum, subradiant SPP lifetimes of up to 200 femtoseconds are observed, which is considerably longer than previously expected for these structures. The spatial SPP mode profiles are imaged using a custom-built near-field optical microscope. The experiments reveal a direct correlation between the spatial mode structure and the dynamics of different SPP resonances. Coupling-induced SPP band gaps are identified as splittings into symmetric and antisymmetric surface modes. These findings allow for an interpretation of the near-field optical image contrast in terms of the contributions of different vectorial components of the electromagnetic near-field. A selective imaging of different electric and magnetic field components is demonstrated for various types of near-field probes. Furthermore, the excitation of SPPs in periodic structures is employed in a novel type of near-field tip. The resonant excitation of SPPs in a nanofabricated grating on the shaft of a sharp metallic tip results in their concentration at the tip apex. The final part of the thesis highlights the importance of optical field enhancements for the local generation of nonlinear optical signals at the apex of sharp metallic tips. Specifically, the observation of intense multiphoton electron emission after femtosecond

  19. Resonance fluorescence in ultrafast and intense x-ray free-electron-laser pulses

    Cavaletto, S M; Harman, Z; Kanter, E P; Southworth, S H; Young, L; Keitel, C H

    2012-01-01

    The spectrum of resonance fluorescence is calculated for a two-level system excited by an intense, ultrashort x-ray pulse made available for instance by free-electron lasers such as the Linac Coherent Light Source (LCLS). We allow for inner-shell hole decay widths and destruction of the system by further photoionization. This two-level description is employed to model neon cations strongly driven by x rays tuned to the $1s 2p^{-1}\\rightarrow 1s^{-1} 2p$ transition at 848 eV; the x rays induce Rabi oscillations which are so fast that they compete with Ne $1s$-hole decay. We predict resonance fluorescence spectra for two different scenarios: first, chaotic pulses based on the Self Amplified Spontaneous Emission principle, like those presently generated at XFEL facilities and, second, Gaussian pulses which will become available in the foreseeable future with self-seeding techniques. As an example of the exciting opportunities deriving from the use of seeding methods, we predict, in spite of above obstacles, the ...

  20. Response to 'Comment on 'Ultrafast electron optics: Propagation dynamics of femtosecond electron packets'' [J. Appl. Phys. 94, 803 (2003)

    In this reply, we address the main issues raised by Qian et al. regarding our recent article [J. Appl. Phys. 92, 1643 (2002)]. In particular, we reiterate the approximations used in the development of the mean-field model and demonstrate how the form used for the on-axis potential is applicable to the study of femtosecond electron packet propagation and is not in need of correction. We also repeat our assertion that the one-dimensional (1-D) fluid model developed by Qian et al. [J. Appl. Phys. 91, 462 (2002)] overestimates space-charge-induced pulse broadening and is in qualitative disagreement with femtosecond electron packet propagation dynamics. The key differences between the mean-field and 1-D fluid model are discussed and their range of applicability is clarified

  1. EDITORIAL: Ultrafast magnetization processes

    Hillebrands, Burkard

    2008-09-01

    This Cluster Issue of Journal of Physics D: Applied Physics is devoted to ultrafast magnetization processes. It reports on the scientific yield of the Priority Programme 1133 'Ultrafast Magnetization Processes' which was funded by the Deutsche Forschungsgemeinschaft in the period 2002-2008 in three successive two-year funding periods, supporting research of 17-18 groups in Germany. Now, at the end of this Priority Programme, the members feel that the achievements made in the course of the programme merit communication to the international scientific community in a concerted way. Therefore, each of the projects of the last funding period presents a key result in a published contribution to this Cluster Issue. The purpose of the funding by a Priority Programme is to advance knowledge in an emerging field of research through collaborative networked support over several locations. Priority Programmes are characterized by their enhanced quality of research through the use of new methods and forms of collaboration in emerging fields, by added value through interdisciplinary cooperation, and by networking. The aim of the Priority Programme 1133 'Ultrafast Magnetization Processes' may be well characterized by the call for projects in June 2001 after the programme was approved by the Deutsche Forschungsgemeinschaft: 'The aim of the priority programme is the achievement of a basic understanding of the temporal evolution of fast magnetization processes in magnetically ordered films, multilayers and micro-structured systems. The challenge lies in the advancement of the field of ultrafast magnetization processes into the regime of a few femtoseconds to nanoseconds, a topic not yet well explored. A general aim is to understand the fundamental mechanisms needed for applications in ultrafast magneto-electronic devices. The fundamental topic to be addressed is the response of the magnetization of small structures upon the application of pulsed magnetic fields, laser pulses or

  2. Instant Cinema 4D starter

    Kaminar, Aaron

    2013-01-01

    Get to grips with a new technology, understand what it is and what it can do for you, and then get to work with the most important features and tasks.This book is written in a friendly, practical style with lots of screenshots and help that will ensure you grow in confidence chapter by chapter.This book is recommended for artists that have experience in other 3D software packages, and who want to learn Cinema 4D. That being said, dedicated readers without experience in other 3D software should not be discouraged from reading this book to learn the basics of Cinema 4D as their first 3D package.

  3. Identification of ultrafast electronic and thermal processes during femtosecond laser ablation by means of surface topography investigations

    electronic system resulting in CE or SOR. These nanostructures due to localization of laser energy deposition in small areas provide a possible pathway from dense electronic excitation to atomic motion causing permanent structural modification. For moderate fluence regime surface elevations in the range of 20-200 nm in height and 100 nm-3μm in diameter are observed. These larger elevations are called bumps and are attributed to ultrafast melting (plasma formation), irradiated buildup of thermal stresses, diffusion, transformation and aggregation of primary defects. For high fluence regime where thermal processes start, craters and island like structures have been observed which are due to surface melting and resolidification. Surface topographical features of irradiated materials are well correlated with the structural changes explored by Raman spectroscopy. Ultrashort lasers have proven to be a powerful tool for many advanced technological applications e.g. two-photon material processing by evoking nonlinear processes in transparent materials. In this regards a practical example is presented in which nonlinear absorption properties are correlated with the surface and structural changes of an ultra short laser irradiated CR-39. Apart from features mentioned above, self-organized subwavelength ripples and classical ripples on Al, CaF2 and Si induced by laser pulses have been investigated by AFM under different experimental conditions. These features are attributed to the excitation of surface plasmon polaritons to induce a periodic enhancement of local fields in the surface layers. AFM investigations of the surface topography together with the characteristics of ejected particles observed with laser analytical methods yield coherent information and have widened the understanding of the processes involved. This is definitely a first step and has a large potential for further investigations: influence of the pulse-shape on the topography, identifying other possible processes

  4. Effects of different bridge/anchor groups on the mechanisms of ultrafast heterogeneous electron transfer in a dye/semiconductor system

    Neubauer, Antje; Szarko, Jodi; Dinkel, Carlo; Morbach, Guido; Socaciu-Siebert, Liana; Eichberger, Rainer; Willig, Frank [Hahn-Meitner-Institut, Glienicker Str. 100, D - 14109 Berlin (Germany)

    2007-07-01

    Two mechanisms for ultrafast heterogeneous electron transfer are known. For molecules bound to a TiO{sub 2} surface via a carboxylic anchor group the standard mechanism for photoinduced electron injection is widely accepted, where the chromophore of the organic dye is excited by light in a first step and the electron is injected from the excited state of the molecule in a second step. For dihydroxy compounds, where the two hydroxy groups bind to one Ti atom an alternative mechanism is known, the direct optical charge transfer. We investigated new perylene derivatives at nano-porous colloidal TiO{sub 2} films in order to clarify the mechanisms for those heterogeneous electron transfer reactions. In these systems the perylene molecule functions as electron donor, and the wide-band gap semiconductor TiO{sub 2} functions as electron acceptor. The perylene chromophores are bound via a hydroxyl group, catechol and two hydroxy groups as bridge/anchor groups. The spectral features of the linear absorption spectra in solution and attached to TiO{sub 2} give information concerning the dynamics and therefore the mechanisms for the electron transfer, which are supported by the short time constants for the electron injection of less than 30 fs measured with transient absorption spectroscopy.

  5. HII galaxies in 4D

    Telles, Eduardo

    2014-01-01

    HII galaxies are clumpy and their gas kinematics can be mapped to show the global turbulent motions and the effect of massive star evolution. The distribution of their physical conditions is homogeneous and oxygen abundance is uniform. The presence of nebular HeII 4868 line seems to be higher in a low abundance galaxy, implying a harder ionization power probably due to stars in low metallicity. Innovative methods of data cube analysis, namely PCA tomography (nicknamed 4D), seem promising in revealing additional information not detected with the standard methods. I review some of our own recent work on the 3D spectroscopy of HII galaxies.

  6. Ultrafast biophotonics

    Vasa, P

    2016-01-01

    This book presents emerging contemporary optical techniques of ultrafast science which have opened entirely new vistas for probing biological entities and processes. The spectrum reaches from time-resolved imaging and multiphoton microscopy to cancer therapy and studies of DNA damage. The book displays interdisciplinary research at the interface of physics and biology. Emerging topics on the horizon are also discussed, like the use of squeezed light, frequency combs and terahertz imaging as the possibility of mimicking biological systems. The book is written in a manner to make it readily accessible to researchers, postgraduate biologists, chemists, engineers, and physicists and students of optics, biomedical optics, photonics and biotechnology.

  7. PREFACE: Ultrafast biophotonics Ultrafast biophotonics

    Gu, Min; Reid, Derryck; Ben-Yakar, Adela

    2010-08-01

    The use of light to explore biology can be traced to the first observations of tissue made with early microscopes in the mid-seventeenth century, and has today evolved into the discipline which we now know as biophotonics. This field encompasses a diverse range of activities, each of which shares the common theme of exploiting the interaction of light with biological material. With the rapid advancement of ultrafast optical technologies over the last few decades, ultrafast lasers have increasingly found applications in biophotonics, to the extent that the distinctive new field of ultrafast biophotonics has now emerged, where robust turnkey ultrafast laser systems are facilitating cutting-edge studies in the life sciences to take place in everyday laboratories. The broad spectral bandwidths, precision timing resolution, low coherence and high peak powers of ultrafast optical pulses provide unique opportunities for imaging and manipulating biological systems. Time-resolved studies of bio-molecular dynamics exploit the short pulse durations from such lasers, while other applications such as optical coherence tomography benefit from the broad optical bandwidths possible by using super-continuum generation and additionally allowing for high speed imaging with speeds as high as 47 000 scans per second. Continuing progress in laser-system technology is accelerating the adoption of ultrafast techniques across the life sciences, both in research laboratories and in clinical applications, such as laser-assisted in situ keratomileusis (LASIK) eye surgery. Revolutionizing the field of optical microscopy, two-photon excitation fluorescence (TPEF) microscopy has enabled higher spatial resolution with improved depth penetration into biological specimens. Advantages of this nonlinear optical process include: reduced photo-interactions, allowing for extensive imaging time periods; simultaneously exciting multiple fluorescent molecules with only one excitation wavelength; and

  8. Ultrafast imaging the light-speed propagation of a focused femtosecond laser pulse in air and its ionized electron dynamics and plasma-induced pulse reshaping

    Yu, Yanwu; Jiang, Lan; Cao, Qiang; Shi, Xueshong; Wang, Qingsong; Wang, Guoyan; Lu, Yongfeng

    2016-03-01

    The light-speed propagation of a focused femtosecond (fs) laser pulse in air was recorded by a pump-probe shadowgraph imaging technique with femtosecond time resolution. The ultrafast dynamics of the laser-ionized electrons were studied, which revealed a strong reshaping of the laser field due to laser-air nonlinear interaction. The influence of laser fluence and focusing conditions on the pulse reshaping was studied, and it was found that: (1) double foci are formed due to the refocusing effect when the laser fluence is higher than 500 J/cm2 and the focusing numeric aperture (NA) is higher than 0.30; and (2) a higher NA focusing lens can better inhibit the prefocusing effect and nonlinear distortion in the Gaussian beam waist.

  9. Ultrafast electron transfer in all-carbon-based SWCNT-C60 donor-acceptor nanoensembles connected by poly(phenylene-ethynylene) spacers.

    Barrejón, Myriam; Gobeze, Habtom B; Gómez-Escalonilla, María J; Fierro, José Luis G; Zhang, Minfang; Yudasaka, Masako; Iijima, Sumio; D'Souza, Francis; Langa, Fernando

    2016-08-21

    Building all-carbon based functional materials for light energy harvesting applications could be a solution to tackle and reduce environmental carbon output. However, development of such all-carbon based donor-acceptor hybrids and demonstration of photoinduced charge separation in such nanohybrids is a challenge since in these hybrids part of the carbon material should act as an electron donating or accepting photosensitizer while the second part should fulfil the role of an electron acceptor or donor. In the present work, we have successfully addressed this issue by synthesizing covalently linked all-carbon-based donor-acceptor nanoensembles using single-walled carbon nanotubes (SWCNTs) as the donor and C60 as the acceptor. The donor-acceptor entities in the nanoensembles were connected by phenylene-ethynylene spacer units to achieve better electronic communication and to vary the distance between the components. These novel SWCNT-C60 nanoensembles have been characterized by a number of techniques, including TGA, FT-IR, Raman, AFM, absorbance and electrochemical methods. The moderate number of fullerene addends present on the side-walls of the nanotubes largely preserved the electronic structure of the nanotubes. The thermodynamic feasibility of charge separation in these nanoensembles was established using spectral and electrochemical data. Finally, occurrence of ultrafast electron transfer from the excited nanotubes in these donor-acceptor nanohybrids has been established by femtosecond transient absorption studies, signifying their utility in building light energy harvesting devices. PMID:27305145

  10. A layer-by-layer ZnO nanoparticle-PbS quantum dot self-assembly platform for ultrafast interfacial electron injection

    Eita, Mohamed Samir

    2014-08-28

    Absorbent layers of semiconductor quantum dots (QDs) are now used as material platforms for low-cost, high-performance solar cells. The semiconductor metal oxide nanoparticles as an acceptor layer have become an integral part of the next generation solar cell. To achieve sufficient electron transfer and subsequently high conversion efficiency in these solar cells, however, energy-level alignment and interfacial contact between the donor and the acceptor units are needed. Here, the layer-by-layer (LbL) technique is used to assemble ZnO nanoparticles (NPs), providing adequate PbS QD uptake to achieve greater interfacial contact compared with traditional sputtering methods. Electron injection at the PbS QD and ZnO NP interface is investigated using broadband transient absorption spectroscopy with 120 femtosecond temporal resolution. The results indicate that electron injection from photoexcited PbS QDs to ZnO NPs occurs on a time scale of a few hundred femtoseconds. This observation is supported by the interfacial electronic-energy alignment between the donor and acceptor moieties. Finally, due to the combination of large interfacial contact and ultrafast electron injection, this proposed platform of assembled thin films holds promise for a variety of solar cell architectures and other settings that principally rely on interfacial contact, such as photocatalysis. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. Ultrafast THz Saturable Absorption in Doped Semiconductors

    Turchinovich, Dmitry; Hoffmann, Matthias C.

    2011-01-01

    We demonstrate ultrafast THz saturable absorption in n-doped semiconductors by nonlinear THz time-domain spectroscopy. This effect is caused by the semiconductor conductivity modulation due to electron heating and satellite-valley scattering in strong THz fields.......We demonstrate ultrafast THz saturable absorption in n-doped semiconductors by nonlinear THz time-domain spectroscopy. This effect is caused by the semiconductor conductivity modulation due to electron heating and satellite-valley scattering in strong THz fields....

  12. Ultrafast Transmission Systems using Coherent Technology

    Ludwig, Reinhold; Richter, Thomas; Palushani, Evarist;

    2011-01-01

    We review recent progress in ultrafast transmission systems. Using coherent detection for simultaneous demultiplexing and demodulation enabled single channel serial 10.2Tb/s transmission over 29km as well as transmission impairment compensation far beyond electronic speed limits.......We review recent progress in ultrafast transmission systems. Using coherent detection for simultaneous demultiplexing and demodulation enabled single channel serial 10.2Tb/s transmission over 29km as well as transmission impairment compensation far beyond electronic speed limits....

  13. Direct probing of photoinduced electron transfer in a self-assembled biomimetic [2Fe2S]-hydrogenase complex using ultrafast vibrational spectroscopy.

    Li, Ping; Amirjalayer, Saeed; Hartl, František; Lutz, Martin; de Bruin, Bas; Becker, René; Woutersen, Sander; Reek, Joost N H

    2014-05-19

    A pyridyl-functionalized diiron dithiolate complex, [μ-(4-pyCH2-NMI-S2)Fe2(CO)6] (3, py = pyridine (ligand), NMI = naphthalene monoimide) was synthesized and fully characterized. In the presence of zinc tetraphenylporphyrin (ZnTPP), a self-assembled 3·ZnTPP complex was readily formed in CH2Cl2 by the coordination of the pyridyl nitrogen to the porphyrin zinc center. Ultrafast photoinduced electron transfer from excited ZnTPP to complex 3 in the supramolecular assembly was observed in real time by monitoring the ν(C≡O) and ν(C═O)NMI spectral changes with femtosecond time-resolved infrared (TRIR) spectroscopy. We have confirmed that photoinduced charge separation produced the monoreduced species by comparing the time-resolved IR spectra with the conventional IR spectra of 3(•-) generated by reversible electrochemical reduction. The lifetimes for the charge separation and charge recombination processes were found to be τCS = 40 ± 3 ps and τCR = 205 ± 14 ps, respectively. The charge recombination is much slower than that in an analogous covalent complex, demonstrating the potential of a supramolecular approach to extend the lifetime of the charge-separated state in photocatalytic complexes. The observed vibrational frequency shifts provide a very sensitive probe of the delocalization of the electron-spin density over the different parts of the Fe2S2 complex. The TR and spectro-electrochemical IR spectra, electron paramagnetic resonance spectra, and density functional theory calculations all show that the spin density in 3(•-) is delocalized over the diiron core and the NMI bridge. This delocalization explains why the complex exhibits low catalytic dihydrogen production even though it features a very efficient photoinduced electron transfer. The ultrafast porphyrin-to-NMI-S2-Fe2(CO)6 photoinduced electron transfer is the first reported example of a supramolecular Fe2S2-hydrogenase model studied by femtosecond TRIR spectroscopy. Our results show that TRIR

  14. Effect of Molecular Coupling on Ultrafast Electron-Transfer and Charge-Recombination Dynamics in a Wide-Gap ZnS Nanoaggregate Sensitized by Triphenyl Methane Dyes.

    Debnath, Tushar; Maity, Partha; Dana, Jayanta; Ghosh, Hirendra N

    2016-03-01

    Wide-band-gap ZnS nanocrystals (NCs) were synthesized, and after sensitizing the NCs with series of triphenyl methane (TPM) dyes, ultrafast charge-transfer dynamics was demonstrated. HRTEM images of ZnS NCs show the formation of aggregate crystals with a flower-like structure. Exciton absorption and lumimescence, due to quantum confinement of the ZnS NCs, appear at approximately 310 and 340 nm, respectively. Interestingly, all the TPM dyes (pyrogallol red, bromopyrogallol red, and aurin tricarboxylic acid) form charge-transfer complexes with the ZnS NCs, with the appearance of a red-shifted band. Electron injection from the photoexcited TPM dyes into the conduction band of the ZnS NCs is shown to be a thermodynamically viable process, as confirmed by steady-state and time-resolved emission studies. To unravel charge-transfer (both electron injection and charge recombination) dynamics and the effect of molecular coupling, femtosecond transient absorption studies were carried out in TPM-sensitized ZnS NCs. The electron-injection dynamics is pulse-width-limited in all the ZnS/TPM dye systems, however, the back electron transfer differs, depending on the molecular coupling of the sensitizers (TPM dyes). The detailed mechanisms for the above-mentioned processes are discussed. PMID:26548569

  15. Ultrafast electronic and vibrational dynamics of stabilized A state mutants of the green fluorescent protein (GFP): Snipping the proton wire

    Two blue absorbing and emitting mutants (S65G/T203V/E222Q and S65T at pH 5.5) of the green fluorescent protein (GFP) have been investigated through ultrafast time resolved infra-red (TRIR) and fluorescence spectroscopy. In these mutants, in which the excited state proton transfer reaction observed in wild-type GFP has been blocked, the photophysics are dominated by the neutral A state. It was found that the A* excited state lifetime is short, indicating that it is relatively less stabilised in the protein matrix than the anionic form. However, the lifetime of the A state can be increased through modifications to the protein structure. The TRIR spectra show that a large shifts in protein vibrational modes on excitation of the A state occurs in both these GFP mutants. This is ascribed to a change in H-bonding interactions between the protein matrix and the excited state

  16. Establishing a framework to implement 4D XCAT Phantom for 4D radiotherapy research

    Raj K Panta

    2012-01-01

    Conclusions: An integrated computer program has been developed to generate, review, analyse, process, and export the 4D XCAT images. A framework has been established to implement the 4D XCAT phantom for 4D RT research.

  17. Advances in 4D Radiation Therapy for Managing Respiration: Part I – 4D Imaging

    Hugo, Geoffrey D.; Rosu, Mihaela

    2012-01-01

    Techniques for managing respiration during imaging and planning of radiation therapy are reviewed, concentrating on free-breathing (4D) approaches. First, we focus on detailing the historical development and basic operational principles of currently-available “first generation” 4D imaging modalities: 4D computed tomography, 4D cone beam computed tomography, 4D magnetic resonance imaging, and 4D positron emission tomography. Features and limitations of these first generation systems are descri...

  18. Establishing a framework to implement 4D XCAT Phantom for 4D radiotherapy research

    Panta, Raj K.; Paul Segars; Fang-Fang Yin; Jing Cai

    2012-01-01

    Aims: To establish a framework to implement the 4D integrated extended cardiac torso (XCAT) digital phantom for 4D radiotherapy (RT) research. Materials and Methods: A computer program was developed to facilitate the characterization and implementation of the 4D XCAT phantom. The program can (1) generate 4D XCAT images with customized parameter files; (2) review 4D XCAT images; (3) generate composite images from 4D XCAT images; (4) track motion of selected region-of-interested (ROI); (5) c...

  19. Excited-state intramolecular hydrogen transfer (ESIHT) of 1,8-Dihydroxy-9,10-anthraquinone (DHAQ) characterized by ultrafast electronic and vibrational spectroscopy and computational modeling

    Mohammed, Omar F.

    2014-05-01

    We combine ultrafast electronic and vibrational spectroscopy and computational modeling to investigate the photoinduced excited-state intramolecular hydrogen-transfer dynamics in 1,8-dihydroxy-9,10-anthraquinone (DHAQ) in tetrachloroethene, acetonitrile, dimethyl sulfoxide, and methanol. We analyze the electronic excited states of DHAQ with various possible hydrogen-bonding schemes and provide a general description of the electronic excited-state dynamics based on a systematic analysis of femtosecond UV/vis and UV/IR pump-probe spectroscopic data. Upon photoabsorption at 400 nm, the S 2 electronic excited state is initially populated, followed by a rapid equilibration within 150 fs through population transfer to the S 1 state where DHAQ exhibits ESIHT dynamics. In this equilibration process, the excited-state population is distributed between the 9,10-quinone (S2) and 1,10-quinone (S1) states while undergoing vibrational energy redistribution, vibrational cooling, and solvation dynamics on the 0.1-50 ps time scale. Transient UV/vis pump-probe data in methanol also suggest additional relaxation dynamics on the subnanosecond time scale, which we tentatively ascribe to hydrogen bond dynamics of DHAQ with the protic solvent, affecting the equilibrium population dynamics within the S2 and S1 electronic excited states. Ultimately, the two excited singlet states decay with a solvent-dependent time constant ranging from 139 to 210 ps. The concomitant electronic ground-state recovery is, however, only partial because a large fraction of the population relaxes to the first triplet state. From the similarity of the time scales involved, we conjecture that the solvent plays a crucial role in breaking the intramolecular hydrogen bond of DHAQ during the S2/S1 relaxation to either the ground or triplet state. © 2014 American Chemical Society.

  20. Ultrafast electron transfer in all-carbon-based SWCNT-C60 donor-acceptor nanoensembles connected by poly(phenylene-ethynylene) spacers

    Barrejón, Myriam; Gobeze, Habtom B.; Gómez-Escalonilla, María J.; Fierro, José Luis G.; Zhang, Minfang; Yudasaka, Masako; Iijima, Sumio; D'Souza, Francis; Langa, Fernando

    2016-08-01

    Building all-carbon based functional materials for light energy harvesting applications could be a solution to tackle and reduce environmental carbon output. However, development of such all-carbon based donor-acceptor hybrids and demonstration of photoinduced charge separation in such nanohybrids is a challenge since in these hybrids part of the carbon material should act as an electron donating or accepting photosensitizer while the second part should fulfil the role of an electron acceptor or donor. In the present work, we have successfully addressed this issue by synthesizing covalently linked all-carbon-based donor-acceptor nanoensembles using single-walled carbon nanotubes (SWCNTs) as the donor and C60 as the acceptor. The donor-acceptor entities in the nanoensembles were connected by phenylene-ethynylene spacer units to achieve better electronic communication and to vary the distance between the components. These novel SWCNT-C60 nanoensembles have been characterized by a number of techniques, including TGA, FT-IR, Raman, AFM, absorbance and electrochemical methods. The moderate number of fullerene addends present on the side-walls of the nanotubes largely preserved the electronic structure of the nanotubes. The thermodynamic feasibility of charge separation in these nanoensembles was established using spectral and electrochemical data. Finally, occurrence of ultrafast electron transfer from the excited nanotubes in these donor-acceptor nanohybrids has been established by femtosecond transient absorption studies, signifying their utility in building light energy harvesting devices.Building all-carbon based functional materials for light energy harvesting applications could be a solution to tackle and reduce environmental carbon output. However, development of such all-carbon based donor-acceptor hybrids and demonstration of photoinduced charge separation in such nanohybrids is a challenge since in these hybrids part of the carbon material should act as an

  1. Impact of metal ions in porphyrin-based applied materials for visible-light photocatalysis: key information from ultrafast electronic spectroscopy.

    Kar, Prasenjit; Sardar, Samim; Alarousu, Erkki; Sun, Jingya; Seddigi, Zaki S; Ahmed, Saleh A; Danish, Ekram Y; Mohammed, Omar F; Pal, Samir Kumar

    2014-08-11

    Protoporphyrin IX-zinc oxide (PP-ZnO) nanohybrids have been synthesized for applications in photocatalytic devices. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and steady-state infrared, absorption, and emission spectroscopies have been used to analyze the structural details and optical properties of these nanohybrids. Time-resolved fluorescence and transient absorption techniques have been applied to study the ultrafast dynamic events that are key to photocatalytic activities. The photocatalytic efficiency under visible-light irradiation in the presence of naturally abundant iron(III) and copper(II) ions has been found to be significantly retarded in the former case, but enhanced in the latter case. More importantly, femtosecond (fs) transient absorption data have clearly demonstrated that the residence of photoexcited electrons from the sensitizer PP in the centrally located iron moiety hinders ground-state bleach recovery of the sensitizer, affecting the overall photocatalytic rate of the nanohybrid. The presence of copper(II) ions, on the other hand, offers additional stability against photobleaching and eventually enhances the efficiency of photocatalysis. In addition, we have also explored the role of UV light in the efficiency of photocatalysis and have rationalized our observations from femtosecond- to picosecond-resolved studies. PMID:25044047

  2. Impact of metal ions in porphyrin-based applied materials for visible-light photocatalysis: Key information from ultrafast electronic spectroscopy

    Kar, Prasenjit

    2014-07-10

    ProtoporphyrinIX-zinc oxide (PP-ZnO) nanohybrids have been synthesized for applications in photocatalytic devices. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and steady-state infrared, absorption, and emission spectroscopies have been used to analyze the structural details and optical properties of these nanohybrids. Time-resolved fluorescence and transient absorption techniques have been applied to study the ultrafast dynamic events that are key to photocatalytic activities. The photocatalytic efficiency under visible-light irradiation in the presence of naturally abundant iron(III) and copper(II) ions has been found to be significantly retarded in the former case, but enhanced in the latter case. More importantly, femtosecond (fs) transient absorption data have clearly demonstrated that the residence of photoexcited electrons from the sensitizer PP in the centrally located iron moiety hinders ground-state bleach recovery of the sensitizer, affecting the overall photocatalytic rate of the nanohybrid. The presence of copper(II) ions, on the other hand, offers additional stability against photobleaching and eventually enhances the efficiency of photocatalysis. In addition, we have also explored the role of UV light in the efficiency of photocatalysis and have rationalized our observations from femtosecond- to picosecond-resolved studies. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  3. An ultrafast terahertz probe of the transient evolution of the charged and neutral phase of photo-excited electron-hole gas in a monolayer semiconductor

    Liu, Xuefeng; Yu, Hongyi; Ji, Qingqing; Gao, Zhihan; Ge, Shaofeng; Qiu, Jun; Liu, Zhongfan; Zhang, Yanfeng; Sun, Dong

    2016-03-01

    We investigate the dynamical formation of an exciton from photo-excited electron-hole plasma and its subsequent decay dynamics in monolayer MoS2 grown by chemical vapor deposition (CVD) using ultrafast pump and terahertz probe spectroscopy. Different photo-excited electron-hole states are resolved based on their distinct responses to THz photon and decay lifetimes. The observed transient THz transmission can be fitted with two decay components: a fast component with a decay lifetime of 20 ps, which is attributed to the exciton lifetime, including its formation and subsequent intra-exciton relaxation; a slow component with an extremely long decay lifetime of several ns, possibly due to a long-lived dark exciton state. The relaxation dynamics are further supported by temperature and pump-fluence-dependent studies of the decay time constants. The sign of the transient THz observed in this experiment is the opposite of that measured in a recent parallel transient THz work on MoS2 [1]. The observed decay dynamics are also different, and the possible reasons for these discrepancies are discussed.

  4. 4-D OCT in Developmental Cardiology

    Jenkins, Michael W.; Rollins, Andrew M.

    Although strong evidence exists to suggest that altered cardiac function can lead to CHDs, few studies have investigated the influential role of cardiac function and biophysical forces on the development of the cardiovascular system due to a lack of proper in vivo imaging tools. 4-D imaging is needed to decipher the complex spatial and temporal patterns of biomechanical forces acting upon the heart. Numerous solutions over the past several years have demonstrated 4-D OCT imaging of the developing cardiovascular system. This chapter will focus on these solutions and explain their context in the evolution of 4-D OCT imaging. The first sections describe the relevant techniques (prospective gating, direct 4-D imaging, retrospective gating), while later sections focus on 4-D Doppler imaging and measurements of force implementing 4-D OCT Doppler. Finally, the techniques are summarized, and some possible future directions are discussed.

  5. Methods for studying the coherent 4D structural dynamics of free molecules and condensed state of matter

    Studies in the coupled 4D spatial and temporal continuum are necessary for understanding the dynamic features of molecular systems with a complex profile of the potential energy surface. The introduction of time sweep into diffraction methods and the development of principles for studying coherent processes have revealed new approaches to the analysis of the dynamics of wave packets, the intermediate products and the transition state of the reaction center, and short-lived compounds in gaseous and condensed media. The use of picosecond and femtosecond electron probe pulses, synchronized with excitation laser pulses, determined the development of ultrafast electron crystallography, time-resolved X-ray diffraction, and dynamic transmission electron microscopy (DTEM). One of the most promising applications of the developed diffraction methods is the characterization and visualization of the processes occurring upon the photoexcitation of free molecules and biological objects and the analysis of surface and thin films. The whole set of spectral and diffraction methods based on different physical principles, which are complementary and make it possible to perform the photoexcitation of nuclei and electrons and carry out diagnostics of their dynamics at ultrashort time sequences, reveal new possibilities for studies with the necessary integration of the “structure-dynamics-function” triad in chemistry, biology, and materials science.

  6. CINEMA 4D The Artist's Project Sourcebook

    McQuilkin, Kent

    2011-01-01

    Cinema 4D is a fully integrated 3D modeling, animation, and rendering package used extensively in the film, television, science, architecture, engineering and other industries. Generally ranked as the 3rd most widely-used 3Dapplication Cinema 4D is widely praised for its stability, speed and ease of use. Recent film and broadcast productions that have used Cinema 4D include Open Season, Monster House, Superman Returns, Polar Express, Monday Night Football. This third edition of Cinema 4D is updated to address the latest release of the application as well as its critically acclaimed MoGr

  7. The Verification of the Usefulness of Electronic Nose Based on Ultra-Fast Gas Chromatography and Four Different Chemometric Methods for Rapid Analysis of Spirit Beverages

    Śliwińska, Magdalena; Namieśnik, Jacek; Wardencki, Waldemar; Dymerski, Tomasz

    2016-01-01

    Spirit beverages are a diverse group of foodstuffs. They are very often counterfeited which cause the appearance of low quality products or wrongly labelled products on the market. It is important to find a proper quality control and botanical origin method enabling the same time preliminary check of the composition of investigated samples, which was the main goal of this work. For this purpose, the usefulness of electronic nose based on ultra-fast gas chromatography (fast GC e-nose) was verified. A set of 24 samples of raw spirits, 33 samples of vodkas, and 8 samples of whisky were analysed by fast GC e-nose. Four data analysis methods were used. The PCA was applied for the visualization of dataset, observation of the variation inside groups of samples, and selection of variables for the other three statistical methods. The SQC method was utilized to compare the quality of the samples. Both the DFA and SIMCA data analysis methods were used for discrimination of vodka, whisky, and spirits samples. The fast GC e-nose combined with four statistical methods can be used for rapid discrimination of raw spirits, vodkas, and whisky and in the same for preliminary determination of the composition of investigated samples.

  8. The Verification of the Usefulness of Electronic Nose Based on Ultra-Fast Gas Chromatography and Four Different Chemometric Methods for Rapid Analysis of Spirit Beverages

    Paulina Wiśniewska

    2016-01-01

    Full Text Available Spirit beverages are a diverse group of foodstuffs. They are very often counterfeited which cause the appearance of low quality products or wrongly labelled products on the market. It is important to find a proper quality control and botanical origin method enabling the same time preliminary check of the composition of investigated samples, which was the main goal of this work. For this purpose, the usefulness of electronic nose based on ultra-fast gas chromatography (fast GC e-nose was verified. A set of 24 samples of raw spirits, 33 samples of vodkas, and 8 samples of whisky were analysed by fast GC e-nose. Four data analysis methods were used. The PCA was applied for the visualization of dataset, observation of the variation inside groups of samples, and selection of variables for the other three statistical methods. The SQC method was utilized to compare the quality of the samples. Both the DFA and SIMCA data analysis methods were used for discrimination of vodka, whisky, and spirits samples. The fast GC e-nose combined with four statistical methods can be used for rapid discrimination of raw spirits, vodkas, and whisky and in the same for preliminary determination of the composition of investigated samples.

  9. The Verification of the Usefulness of Electronic Nose Based on Ultra-Fast Gas Chromatography and Four Different Chemometric Methods for Rapid Analysis of Spirit Beverages.

    Wiśniewska, Paulina; Śliwińska, Magdalena; Namieśnik, Jacek; Wardencki, Waldemar; Dymerski, Tomasz

    2016-01-01

    Spirit beverages are a diverse group of foodstuffs. They are very often counterfeited which cause the appearance of low quality products or wrongly labelled products on the market. It is important to find a proper quality control and botanical origin method enabling the same time preliminary check of the composition of investigated samples, which was the main goal of this work. For this purpose, the usefulness of electronic nose based on ultra-fast gas chromatography (fast GC e-nose) was verified. A set of 24 samples of raw spirits, 33 samples of vodkas, and 8 samples of whisky were analysed by fast GC e-nose. Four data analysis methods were used. The PCA was applied for the visualization of dataset, observation of the variation inside groups of samples, and selection of variables for the other three statistical methods. The SQC method was utilized to compare the quality of the samples. Both the DFA and SIMCA data analysis methods were used for discrimination of vodka, whisky, and spirits samples. The fast GC e-nose combined with four statistical methods can be used for rapid discrimination of raw spirits, vodkas, and whisky and in the same for preliminary determination of the composition of investigated samples. PMID:27446633

  10. Partially coherent ultrafast spectrography

    Bourassin-Bouchet, C.; Couprie, M.-E.

    2015-01-01

    Modern ultrafast metrology relies on the postulate that the pulse to be measured is fully coherent, that is, that it can be completely described by its spectrum and spectral phase. However, synthesizing fully coherent pulses is not always possible in practice, especially in the domain of emerging ultrashort X-ray sources where temporal metrology is strongly needed. Here we demonstrate how frequency-resolved optical gating (FROG), the first and one of the most widespread techniques for pulse characterization, can be adapted to measure partially coherent pulses even down to the attosecond timescale. No modification of experimental apparatuses is required; only the processing of the measurement changes. To do so, we take our inspiration from other branches of physics where partial coherence is routinely dealt with, such as quantum optics and coherent diffractive imaging. This will have important and immediate applications, such as enabling the measurement of X-ray free-electron laser pulses despite timing jitter. PMID:25744080

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

    Leitenstorfer A.

    2013-03-01

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

  12. Ultrafast insulator-metal transition in VO{sub 2}: interplay between coherent lattice motion and electronic correlations

    Leitenstorfer, A.; Kuebler, C.; Huber, R. [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Lopez, R.; Halabica, A.; Haglund, R.F. [Department of Physics and Astronomy, Vanderbilt University, Tennessee, Nashville (United States)

    2009-01-15

    The multi-THz conductivity of VO{sub 2} recorded during a photoinduced insulator-metal transition directly reveals the femtosecond dynamics of V-V stretching modes and electronic correlations. The strongly correlated character of the electronic system leads to a transient behaviour of the conductivity that cannot be understood in a Born-Oppenheimer picture. Based on our measurements with a time resolution of 12 fs and recent theoretical simulations for the electronic structure in steady state, we suggest a novel qualitative model for the non-thermal phase transition. The extremely high speed for the photoinduced phase transition is elegantly explained via a directed wave packet motion in the electronically excited state of the dimer that transfers the crystal structure of the insulator into the configuration of the metallic phase. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  13. On "New Massive" 4D Gravity

    Bergshoeff, Eric A; Rosseel, Jan; Townsend, Paul K

    2012-01-01

    We construct a four-dimensional (4D) gauge theory that propagates, unitarily, the five polarization modes of a massive spin-2 particle. These modes are described by a "dual" graviton gauge potential and the Lagrangian is 4th-order in derivatives. As the construction mimics that of 3D "new massive gravity", we call this 4D model (linearized) "new massive dual gravity". We analyse its massless limit, and discuss similarities to the Eddington-Schroedinger model.

  14. Ultrafast and Efficient Transport of Hot Plasmonic Electrons by Graphene for Pt Free, Highly Efficient Visible-Light Responsive Photocatalyst.

    Kumar, Dinesh; Lee, Ahreum; Lee, Taegon; Lim, Manho; Lim, Dong-Kwon

    2016-03-01

    We report that reduced graphene-coated gold nanoparticles (r-GO-AuNPs) are excellent visible-light-responsive photocatalysts for the photoconversion of CO2 into formic acid (HCOOH). The wavelength-dependent quantum and chemical yields of HCOOH shows a significant contribution of plasmon-induced hot electrons for CO2 photoconversion. Furthermore, the presence and reduced state of the graphene layers are critical parameters for the efficient CO2 photoconversion because of the electron mobility of graphene. With an excellent selectivity toward HCOOH (>90%), the quantum yield of HCOOH using r-GO-AuNPs is 1.52%, superior to that of Pt-coated AuNPs (quantum yield: 1.14%). This indicates that r-GO is a viable alternative to platinum metal. The excellent colloidal stability and photocatalytic stability of r-GO-AuNPs enables CO2 photoconversion under more desirable reaction conditions. These results highlight the role of reduced graphene layers as highly efficient electron acceptors and transporters to facilitate the use of hot electrons for plasmonic photocatalysts. The femtosecond transient spectroscopic analysis also shows 8.7 times higher transport efficiency of hot plasmonic electrons in r-GO-AuNPs compared with AuNPs. PMID:26854830

  15. Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser

    Highlights: •Development of the soft X-ray spectroscopy setup to probe surfaces using free electron laser. •Probing surface chemical reactions using free electron laser. •Optical laser pump and soft X-ray probe study on a sub-picosecond timescale. -- Abstract: We report on an experimental system designed to probe chemical reactions on solid surfaces on a sub-picosecond timescale using soft X-ray emission spectroscopy at the Linac Coherent Light Source (LCLS) free electron laser (FEL) at the SLAC National Accelerator Laboratory. We analyzed the O 1s X-ray emission spectra recorded from atomic oxygen adsorbed on a Ru(0 0 0 1) surface at a synchrotron beamline (SSRL, BL13-2) and an FEL beamline (LCLS, SXR). We have demonstrated conditions that provide negligible amount of FEL induced damage of the sample. In addition we show that the setup is capable of tracking the temporal evolution of electronic structure during a surface reaction of submonolayer quantities of CO molecules desorbing from the surface

  16. Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser

    Katayama, T.; Anniyev, T. [SIMES, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Beye, M. [SIMES, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Institute for Methods and Instrumentation in Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Wilhelm-Conrad-Röntgen Campus, Albert-Einstein-Str. 15, 12489 Berlin (Germany); Coffee, R. [Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Dell’Angela, M. [University of Hamburg and Center for Free Electron Laser Science, Luruper Chaussee 149, D-22761 Hamburg (Germany); Föhlisch, A. [Institute for Methods and Instrumentation in Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Wilhelm-Conrad-Röntgen Campus, Albert-Einstein-Str. 15, 12489 Berlin (Germany); Institut für Physik und Astronomie, Universität Potsdam, Karl-Liebknecht-Str. 24-25, 14476 Potsdam (Germany); Gladh, J. [Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 (Sweden); Kaya, S. [SIMES, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Krupin, O. [Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); European XFEL GmbH, Albert-Einstein-Ring 19, 22761 Hamburg (Germany); and others

    2013-04-15

    Highlights: •Development of the soft X-ray spectroscopy setup to probe surfaces using free electron laser. •Probing surface chemical reactions using free electron laser. •Optical laser pump and soft X-ray probe study on a sub-picosecond timescale. -- Abstract: We report on an experimental system designed to probe chemical reactions on solid surfaces on a sub-picosecond timescale using soft X-ray emission spectroscopy at the Linac Coherent Light Source (LCLS) free electron laser (FEL) at the SLAC National Accelerator Laboratory. We analyzed the O 1s X-ray emission spectra recorded from atomic oxygen adsorbed on a Ru(0 0 0 1) surface at a synchrotron beamline (SSRL, BL13-2) and an FEL beamline (LCLS, SXR). We have demonstrated conditions that provide negligible amount of FEL induced damage of the sample. In addition we show that the setup is capable of tracking the temporal evolution of electronic structure during a surface reaction of submonolayer quantities of CO molecules desorbing from the surface.

  17. Cooperative catalysis: electron-rich Fe-H complexes and DMAP, a successful "joint venture" for ultrafast hydrogen production.

    Rommel, Susanne; Hettmanczyk, Lara; Klein, Johannes E M N; Plietker, Bernd

    2014-08-01

    A series of defined iron-hydrogen complexes was prepared in a straightforward one-pot approach. The structure and electronic properties of such complexes were investigated by means of quantum-chemical analysis. These new complexes were then applied in the dehydrogenative silylation of methanol. The complex (dppp)(CO)(NO)FeH showed a remarkable activity with a TOF of more than 600 000 h(-1) of pure hydrogen gas within seconds. PMID:24807477

  18. Light-induced temperature jump causes power-dependent ultrafast kinetics of electrons generated in multiphoton ionization of liquid water

    Crowell, Robert A.; Lian, Rui; Shkrob, Ilya A.; Qian, Jun; Oulianov, Dmitri A.; Pommeret, Stanislas

    2004-01-01

    Picosecond geminate recombination kinetics for electrons generated by multiphoton ionization of liquid water become power dependent when the radiance of the excitation light is greater than 0.3-0.5 TW/cm^2 (the terawatt regime). To elucidate the mechanism of this power dependence, tri- 400 nm photon ionization of water has been studied using pump-probe laser spectroscopy on the pico- and femtosecond time scales. We suggest that the observed kinetic transformations are caused by a rapid temper...

  19. Progress in ultrafast intense laser science VII

    Normand, Didier; Yamanouchi, Kaoru

    2011-01-01

    The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed chapters authored by researchers at the forefront of each their own subfields of UILS. Every chapter begins with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance and attractions of the research topic at hand; these are followed by reports of cutting-edge discoveries. This seventh volume covers a broad range of topics from this interdisciplinary research field, focusing on the ionization of atoms and molecules, ultrafast responses of protons and electrons within a molecule, molecular alignment, high-order harmonics and attosecond pulse generation, and acceleration of electrons a...

  20. Ultrafast electrical injection of spin-polarized electrons in single self-organized InGaAs quantum dots

    The present thesis deals with the electrical injection of spin-polarized electrons in single InGaAs quantum dots in the nanosecond or even in the subnanosecond time range. Two different concepts with fundamentally different injection mechanisms were studied, namely the injection in a spin LED structure as well as the injection through a tunnel barrier in a pin diode with specially matched band structure. The readout of the spin information pursued via measurements of the electro- respectively photoluminescence emitted by the quantum dot.

  1. Representing Participation in ICT4D Projects

    Singh, J. P.; Flyverbom, Mikkel

    2016-01-01

    How do the discourses of participation inform deployment of information and communication technologies for development (ICT4D)? Discourses here mean narratives that assign roles to actors, and specify causes and outcomes for events. Based on the theory and practice of international development we...... identify two dimensions to participation and ICT4D: whether participation 1) is hierarchical/top-down or agent-driven/bottom-up, and 2) involves conflict or cooperation. Based on these dimensions we articulate four ideal types of discourse that permeate ICT and development efforts: stakeholder......-based discourses that emphasize consensus, networked efforts among actors collaborating in network arrangements, mobilization discourses that account for contestation over meanings of participation, and oppositional discourses from ׳grassroots׳ actors that also include conflict. We conclude that ICT4D efforts...

  2. Cinema 4D R13 Cookbook

    Szabo, Michael

    2012-01-01

    This book contains short recipes designed to effectively teach tools in the minimum amount of time. Each recipe hits on a topic that can be combined or incorporated with other recipes to give you the building blocks you need to start making great designs with Cinema 4D. Rather than demonstrating how to make a few specific and extensive projects, the recipes create a solid base of knowledge to help the reader understand the tools available to foster their own creativity. This book is for anyone who wants to quickly get up to speed with Cinema 4D to create 3D projects that run laps around simple

  3. 4D, N = 1 Supersymmetry Genomics (I)

    Gates, S J; MacGregor, B; Parker, J; Polo-Sherk, R; Rodgers, V G J; Wassink, L

    2009-01-01

    Presented in this paper the nature of the supersymmetrical representation theory behind 4D, N = 1 theories, as described by component fields, is investigated using the tools of Adinkras and Garden Algebras. A survey of familiar matter multiplets using these techniques reveals they are described by two fundamental valise Adinkras that are given the names of the cis-Valise (c-V) and the trans-Valise (t-V). A conjecture is made that all off-shell 4D, N = 1 component descriptions of supermultiplets are associated with two integers - the numbers of c-V and t-V Adinkras that occur in the representation.

  4. Direct observation of ultrafast many-body electron dynamics in a strongly-correlated ultracold Rydberg gas

    Takei, Nobuyuki; Genes, Claudiu; Pupillo, Guido; Goto, Haruka; Koyasu, Kuniaki; Chiba, Hisashi; Weidemüller, Matthias; Ohmori, Kenji

    2015-01-01

    Many-body interactions govern a variety of important quantum phenomena ranging from superconductivity and magnetism in condensed matter to solvent effects in chemistry. Understanding those interactions beyond mean field is a holy grail of modern sciences. AMO physics with advanced laser technologies has recently emerged as a new platform to study quantum many-body systems. One of its latest developments is the study of long-range interactions among ultracold particles to reveal the effects of many-body correlations. Rydberg atoms distinguish themselves by their large dipole moments and tunability of dipolar interactions. Most of ultracold Rydberg experiments have been performed with narrow-band lasers in the Rydberg blockade regime. Here we demonstrate an ultracold Rydberg gas in a complementary regime, where electronic coherence is created using a broadband picosecond laser pulse, thus circumventing the Rydberg blockade to induce strong many-body correlations. The effects of long-range Rydberg interactions h...

  5. Light-induced temperature jump causes power-dependent ultrafast kinetics of electrons generated in multiphoton ionization of liquid water

    Crowell, Robert A; Shkrob, Ilya A; Qian, Jun; Oulianov, Dmitri A; Pommeret, Stanislas

    2004-01-01

    Picosecond geminate recombination kinetics for electrons generated by multiphoton ionization of liquid water become power dependent when the radiance of the excitation light is greater than 0.3-0.5 TW/cm^2 (the terawatt regime). To elucidate the mechanism of this power dependence, tri- 400 nm photon ionization of water has been studied using pump-probe laser spectroscopy on the pico- and femtosecond time scales. We suggest that the observed kinetic transformations are caused by a rapid temperature jump in the sample. Such a jump is inherent to multiphoton ionization in the terawatt regime, when the absorption of the pump light along the optical path becomes very nonuniform. The heating of water is substantial (tens of degrees C) because the 3-photon quantum yield of the ionization is relatively low, ca. 0.42, and a large fraction of the excitation energy is released into the solvent bulk as heat. Evidence of the temperature jump is the observation of a red shift in the absorption spectrum of (thermalized) ele...

  6. New Insights into the Composition and Texture of Lunar Regolith Using Ultrafast Automated Electron-Beam Analysis

    Rickman, Doug; Wentworth, Susan J.; Schrader, Christian M.; Stoeser, Doug; Botha, Pieter WSK; Butcher, Alan R.; Horsch, Hanna E.; Benedictus, Aukje; Gottlieb, Paul; McKay, David

    2008-01-01

    Sieved grain mounts of Apollo 16 drive tube samples have been examined using QEMSCAN - an innovative electron beam technology. By combining multiple energy-dispersive X-ray detectors, fully automated control, and off-line image processing, to produce digital mineral maps of particles exposed on polished surfaces, the result is an unprecedented quantity of mineralogical and petrographic data, on a particle-by-particle basis. Experimental analysis of four size fractions (500-250 microns, 150-90 microns, 75-45 microns and < 20 microns), prepared from two samples (64002,374 and 64002,262), has produced a robust and uniform dataset which allows for the quantification of mineralogy; texture; particle shape, size and density; and the digital classification of distinct particle types in each measured sample. These preliminary data show that there is a decrease in plagioclase modal content and an opposing increase in glass modal content, with decreasing particle size. These findings, together with data on trace phases (metals, sulphides, phosphates, and oxides), provide not only new insights into the make-up of lunar regolith at the Apollo 16 landing site, but also key physical parameters which can be used to design lunar simulants, and compute Figures of Merit for each material produced.

  7. New Insights into the Composition and Texture of Lunar Regolith Using Ultrafast Automated Electron-Beam Analysis

    Rickman, Doug; Wentworth, Susan J.; Schrader, Christian M.; Stoeser, Doug; Botha, Pieter WSK; Butcher, Alan R.; Horsch, Hanna E.; Benedictus, Aukje; Gottlieb, Paul; McKay, David

    2008-01-01

    Sieved grain mounts of Apollo 16 drive tube samples have been examined using QEMSCAN - an innovative electron beam technology. By combining multiple energy-dispersive X-ray detectors, fully automated control, and off-line image processing, to produce digital mineral maps of particles exposed on polished surfaces, the result is an unprecedented quantity of mineralogical and petrographic data, on a particle-by-particle basis. Experimental analysis of four size fractions (500-250 microns, 150-90 microns, 75-45 microns and texture; particle shape, size and density; and the digital classification of distinct particle types in each measured sample. These preliminary data show that there is a decrease in plagioclase modal content and an opposing increase in glass modal content, with decreasing particle size. These findings, together with data on trace phases (metals, sulphides, phosphates, and oxides), provide not only new insights into the make-up of lunar regolith at the Apollo 16 landing site, but also key physical parameters which can be used to design lunar simulants, and compute Figures of Merit for each material produced.

  8. Constrained reconstructions for 4D intervention guidance

    Kuntz, J.; Flach, B.; Kueres, R.; Semmler, W.; Kachelrieß, M.; Bartling, S.

    2013-05-01

    Image-guided interventions are an increasingly important part of clinical minimally invasive procedures. However, up to now they cannot be performed under 4D (3D + time) guidance due to the exceedingly high x-ray dose. In this work we investigate the applicability of compressed sensing reconstructions for highly undersampled CT datasets combined with the incorporation of prior images in order to yield low dose 4D intervention guidance. We present a new reconstruction scheme prior image dynamic interventional CT (PrIDICT) that accounts for specific image features in intervention guidance and compare it to PICCS and ASD-POCS. The optimal parameters for the dose per projection and the numbers of projections per reconstruction are determined in phantom simulations and measurements. In vivo experiments in six pigs are performed in a cone-beam CT; measured doses are compared to current gold-standard intervention guidance represented by a clinical fluoroscopy system. Phantom studies show maximum image quality for identical overall doses in the range of 14 to 21 projections per reconstruction. In vivo studies reveal that interventional materials can be followed in 4D visualization and that PrIDICT, compared to PICCS and ASD-POCS, shows superior reconstruction results and fewer artifacts in the periphery with dose in the order of biplane fluoroscopy. These results suggest that 4D intervention guidance can be realized with today’s flat detector and gantry systems using the herein presented reconstruction scheme.

  9. Ultrafast cyclic voltammetry with asymmetrical potential scan

    Zhi Yong Guo; Xiang Qin Lin

    2008-01-01

    Based on the perfect ohmic drop compensation by online electronic positive feedback, ultrafast cyclic voltammetry withasymmetrical potential scan is achieved for the first time, with the reduction of anthracene acting as the test system. Compared withthe traditional cyclic voltammetry utilizing symmetrical triangular waveform as the excitation one, the new method allows a simplerapproach to mechanistic analysis of ultrafast chemical reactions coupled with a charge transfer. And perhaps more important, it alsoprovides a way to eliminate the interference of the adsorbed product in dynamic monitoring.

  10. Ultrafast supercontinuum fiber-laser based pump-probe scanning magneto-optical Kerr effect microscope for the investigation of electron spin dynamics in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution

    Henn, T.; Kiessling, T., E-mail: tobias.kiessling@physik.uni-wuerzburg.de; Ossau, W.; Molenkamp, L. W. [Physikalisches Institut (EP3), Universität Würzburg, 97074 Würzburg (Germany); Biermann, K.; Santos, P. V. [Paul-Drude-Institut für Festkörperelektronik, 10117 Berlin (Germany)

    2013-12-15

    We describe a two-color pump-probe scanning magneto-optical Kerr effect microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast “white light” supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains of two separate picosecond laser systems. The ability to independently tune the pump and probe wavelength enables the investigation of the influence of excitation energy on the optically induced electron spin dynamics in semiconductors. We demonstrate picosecond real-space imaging of the diffusive expansion of optically excited electron spin packets in a (110) GaAs quantum well sample to illustrate the capabilities of the instrument.

  11. Ultrafast supercontinuum fiber-laser based pump-probe scanning MOKE microscope for the investigation of electron spin dynamics in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution

    Henn, T; Ossau, W; Molenkamp, L W; Biermann, K; Santos, P V

    2013-01-01

    We describe a two-color pump-probe scanning magneto-optical Kerr effect (MOKE) microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast `white light' supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains of two separate picosecond laser systems. The ability to independently tune the pump and probe wavelength enables the investigation of the influence of excitation energy on the optically induced electron spin dynamics in semiconductors. We demonstrate picosecond real-space imaging of the diffusive expansion of optically excited electron spin packets in a (110) GaAs quantum well sample to illustrate the capabilities of t...

  12. High power ultrafast lasers

    Backus, S.; Durfee, C.G. III; Murnane, M.M.; Kapteyn, H.C. [Center for Ultrafast Optical Science, University of Michigan, Ann Arbor, Michigan 48109-2099 (United States)

    1998-03-01

    In this article, we review progress in the development of high peak-power ultrafast lasers, and discuss in detail the design issues which determine the performance of these systems. Presently, lasers capable of generating terawatt peak powers with unprecedented short pulse duration can now be built on a single optical table in a small-scale laboratory, while large-scale lasers can generate peak power of over a petawatt. This progress is made possible by the use of the chirped-pulse amplification technique, combined with the use of broad-bandwidth laser materials such as Ti:sapphire, and the development of techniques for generating and propagating very short (10{endash}30 fs) duration light pulses. We also briefly summarize some of the new scientific advances made possible by this technology, such as the generation of coherent femtosecond x-ray pulses, and the generation of MeV-energy electron beams and high-energy ions. {copyright} {ital 1998 American Institute of Physics.}

  13. Ultrafast laser calligraphy

    Kazansky, Peter G.; Yang, Weijia; Svirko, Yuri P.; Shimotsuma, Yasuhiko; Hirao, Kazuyuki

    2008-01-01

    Control of structural modifications inside transparent materials by varying the direction of pulse front tilt is demonstrated, achieving a calligraphic style of writing. Anisotropic ultrafast laser cavitation in the irradiated region is observed

  14. 4D, N=1 Supergravity Genomics

    Chappell, Isaac; Linch, William D; Parker, James; Randall, Stephen; Ridgway, Alexander; Stiffler, Kory

    2012-01-01

    The off-shell representation theory of 4D, $\\mathcal{N}=1$ supermultiplets can be categorized in terms of distinct irreducible graphical representations called adinkras. Recent evidence has emerged pointing to the existence of three such fundamental adinkras associated with distinct equivalence classes of a Coxeter group. A partial description of these adinkras is given in terms of two types, termed cis-and trans-adinkras (the latter being a degenerate doublet) in analogy to enantiomers in chemistry. Through a new and simple procedure that uses adinkras, we find the irreducible off-shell adinkra representations of 4D, $\\mathcal{N}=1$ supergravity, in the old-minimal, non-minimal, and conformal formulations. We categorize these representations in terms of their supersymmetry `enantiomer' numbers: the number of cis-($n_c$) and trans-($n_t$) adinkras in the representation.

  15. 4D, N=1 Supergravity Genomics

    Chappell, Isaac; Gates, Jr., S. James; Linch III, William D; Parker, James; Randall, Stephen; Ridgway, Alexander; Stiffler, Kory

    2012-01-01

    The off-shell representation theory of 4D, $\\mathcal{N}=1$ supermultiplets can be categorized in terms of distinct irreducible graphical representations called adinkras as part of a larger effort we call supersymmetry `genomics.' Recent evidence has emerged pointing to the existence of three such fundamental adinkras associated with distinct equivalence classes of a Coxeter group. A partial description of these adinkras is given in terms of two types, termed cis-and trans-adinkras (the latter...

  16. 4D image reconstruction for emission tomography

    An overview of the theory of 4D image reconstruction for emission tomography is given along with a review of the current state of the art, covering both positron emission tomography and single photon emission computed tomography (SPECT). By viewing 4D image reconstruction as a matter of either linear or non-linear parameter estimation for a set of spatiotemporal functions chosen to approximately represent the radiotracer distribution, the areas of so-called ‘fully 4D’ image reconstruction and ‘direct kinetic parameter estimation’ are unified within a common framework. Many choices of linear and non-linear parameterization of these functions are considered (including the important case where the parameters have direct biological meaning), along with a review of the algorithms which are able to estimate these often non-linear parameters from emission tomography data. The other crucial components to image reconstruction (the objective function, the system model and the raw data format) are also covered, but in less detail due to the relatively straightforward extension from their corresponding components in conventional 3D image reconstruction. The key unifying concept is that maximum likelihood or maximum a posteriori (MAP) estimation of either linear or non-linear model parameters can be achieved in image space after carrying out a conventional expectation maximization (EM) update of the dynamic image series, using a Kullback-Leibler distance metric (comparing the modeled image values with the EM image values), to optimize the desired parameters. For MAP, an image-space penalty for regularization purposes is required. The benefits of 4D and direct reconstruction reported in the literature are reviewed, and furthermore demonstrated with simple simulation examples. It is clear that the future of reconstructing dynamic or functional emission tomography images, which often exhibit high levels of spatially correlated noise, should ideally exploit these 4D

  17. 4D Lung Reconstruction with Phase Optimization

    Lyksborg, Mark; Paulsen, Rasmus; Brink, Carsten;

    2009-01-01

    This paper investigates and demonstrates a 4D lung CT reconstruction/registration method which results in a complete volumetric model of the lung that deforms according to a respiratory motion field. The motion field is estimated iteratively between all available slice samples and a reference...... than using an optimization which does not correct for phase errors. Knowing how the lung and any tumors located within the lung deforms is relevant in planning the treatment of lung cancer....

  18. Time-dependent multiconfiguration theory for ultrafast electronic dynamics of molecules in an intense laser field: Electron correlation and energy redistribution among natural orbitals

    We propose a new definition of molecular orbital energy in order to investigate the energetics of constituent molecular orbitals in the many-electron wave function calculated based on time-dependent multiconfiguration theory. It is shown that when energies are assigned to natural orbitals by a similar manner to that used in the Hartree-Fock theory, we can quantify a correction energy to the total electronic energy that represents electron correlation, and thus we can evaluate the time-dependence of the correlation energy. Our attempt is illustrated by numerical results on the time-dependence of the spatial density of the correlation energy and the orbital energies for a H2 molecule interacting with an intense, near-infrared laser field. We compared the energy ζj(t) supplied by the applied field with the net energy gain Δε-barj(t) for respective natural orbitals φj(t). φj and found that the natural orbitals with Δε-barj(t)>ζj(t) play a key role in the ionization process.

  19. SU-D-18C-01: A Novel 4D-MRI Technology Based On K-Space Retrospective Sorting

    Purpose: Current 4D-MRI techniques lack sufficient temporal/spatial resolution and consistent tumor contrast. To overcome these limitations, this study presents the development and initial evaluation of an entirely new framework of 4D-MRI based on k-space retrospective sorting. Methods: An important challenge of the proposed technique is to determine the number of repeated scans(NR) required to obtain sufficient k-space data for 4D-MRI. To do that, simulations using 29 cancer patients' respiratory profiles were performed to derive the relationship between data acquisition completeness(Cp) and NR, also relationship between NR(Cp=95%) and the following factors: total slice(NS), respiratory phase bin length(Lb), frame rate(fr), resolution(R) and image acquisition starting-phase(P0). To evaluate our technique, a computer simulation study on a 4D digital human phantom (XCAT) were conducted with regular breathing (fr=0.5Hz; R=256×256). A 2D echo planer imaging(EPI) MRI sequence were assumed to acquire raw k-space data, with respiratory signal and acquisition time for each k-space data line recorded simultaneously. K-space data was re-sorted based on respiratory phases. To evaluate 4D-MRI image quality, tumor trajectories were measured and compared with the input signal. Mean relative amplitude difference(D) and cross-correlation coefficient(CC) are calculated. Finally, phase-sharing sliding window technique was applied to investigate the feasibility of generating ultra-fast 4D-MRI. Result: Cp increased with NR(Cp=100*[1-exp(-0.19*NR)], when NS=30, Lb=100%/6). NR(Cp=95%) was inversely-proportional to Lb (r=0.97), but independent of other factors. 4D-MRI on XCAT demonstrated highly accurate motion information (D=0.67%, CC=0.996) with much less artifacts than those on image-based sorting 4D-MRI. Ultra-fast 4D-MRI with an apparent temporal resolution of 10 frames/second was reconstructed using the phase-sharing sliding window technique. Conclusions: A novel 4D

  20. Cinema 4D R14 cookbook

    Russell, Simon

    2013-01-01

    This book is written in a Cookbook style with short recipes designed to effectively teach tools in the minimum amount of time. Each recipe hits on a topic that can be combined or incorporated with other recipes to give you the building blocks you need to start making great designs with Cinema 4D. Rather than demonstrating how to make a few specific and extensive projects, the recipes create a solid base of knowledge to help the reader understand the tools available to foster their own creativity.This book is for professional artists working in architecture, design, production, or games and wan

  1. 4D, N = 1 Supersymmetry Genomics (II)

    Gates, S James; Hallett, Jared; Parker, James; Rodgers, Vincent G J; Stiffler, Kory

    2011-01-01

    We continue the development of a theory of off-shell supersymmetric representations analogous to that of compact Lie algebras such as SU(3). For off-shell 4D, N = 1 systems, quark-like representations have been identified [1] in terms of cis-Adinkras and trans-Adinkras and it has been conjectured that arbitrary representations are composites of $n_c$-cis and $n_t$-trans representations. Analyzing the real scalar and complex linear superfield multiplets, these "chemical enantiomer" numbers are found to be $n_c$ = $n_t$ = 1 and $n_c$ = 1, $n_t$ = 2, respectively.

  2. Active origami by 4D printing

    Recent advances in three dimensional (3D) printing technology that allow multiple materials to be printed within each layer enable the creation of materials and components with precisely controlled heterogeneous microstructures. In addition, active materials, such as shape memory polymers, can be printed to create an active microstructure within a solid. These active materials can subsequently be activated in a controlled manner to change the shape or configuration of the solid in response to an environmental stimulus. This has been termed 4D printing, with the 4th dimension being the time-dependent shape change after the printing. In this paper, we advance the 4D printing concept to the design and fabrication of active origami, where a flat sheet automatically folds into a complicated 3D component. Here we print active composites with shape memory polymer fibers precisely printed in an elastomeric matrix and use them as intelligent active hinges to enable origami folding patterns. We develop a theoretical model to provide guidance in selecting design parameters such as fiber dimensions, hinge length, and programming strains and temperature. Using the model, we design and fabricate several active origami components that assemble from flat polymer sheets, including a box, a pyramid, and two origami airplanes. In addition, we directly print a 3D box with active composite hinges and program it to assume a temporary flat shape that subsequently recovers to the 3D box shape on demand. (paper)

  3. Active origami by 4D printing

    Ge, Qi; Dunn, Conner K.; Qi, H. Jerry; Dunn, Martin L.

    2014-09-01

    Recent advances in three dimensional (3D) printing technology that allow multiple materials to be printed within each layer enable the creation of materials and components with precisely controlled heterogeneous microstructures. In addition, active materials, such as shape memory polymers, can be printed to create an active microstructure within a solid. These active materials can subsequently be activated in a controlled manner to change the shape or configuration of the solid in response to an environmental stimulus. This has been termed 4D printing, with the 4th dimension being the time-dependent shape change after the printing. In this paper, we advance the 4D printing concept to the design and fabrication of active origami, where a flat sheet automatically folds into a complicated 3D component. Here we print active composites with shape memory polymer fibers precisely printed in an elastomeric matrix and use them as intelligent active hinges to enable origami folding patterns. We develop a theoretical model to provide guidance in selecting design parameters such as fiber dimensions, hinge length, and programming strains and temperature. Using the model, we design and fabricate several active origami components that assemble from flat polymer sheets, including a box, a pyramid, and two origami airplanes. In addition, we directly print a 3D box with active composite hinges and program it to assume a temporary flat shape that subsequently recovers to the 3D box shape on demand.

  4. An ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle

    Gu Zhiguo; Yang Shuping [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China); Li Zaijun, E-mail: zaijunli@263.net [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China); Sun Xiulan [School of Food Science and Technology, Jiangnan University, Wuxi 214122 (China); Wang Guangli [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China); Fang Yinjun [Zhejiang Zanyu Technology Co., Ltd., Hangzhou 310009 (China); Liu Junkang [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China)

    2011-10-30

    Graphical abstract: We first reported an ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since promising their electrocatalytic synergy towards glucose was achieved, the biosensor showed high sensitivity (5762.8 nA nM{sup -1} cm{sup -2}), low detection limit (S/N = 3) (3 x 10{sup -12} M) and fast response time (0.045 s). - Abstract: The paper reported an ultrasensitive electrochemical biosensor for glucose which was based on CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since efficient electron transfer between glucose oxidase and the electrode was achieved, the biosensor showed high sensitivity (5762.8 nA nM{sup -1} cm{sup -2}), low detection limit (S/N = 3) (3 x 10{sup -12} M), fast response time (0.045 s), wide calibration range (from 1 x 10{sup -11} M to 1 x 10{sup -8} M) and good long-term stability (26 weeks). The apparent Michaelis-Menten constant of the glucose oxidase on the medium, 5.24 x 10{sup -6} mM, indicates excellent bioelectrocatalytic activity of the immobilized enzyme towards glucose oxidation. Moreover, the effects of omitting graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle were also investigated. The result showed sensitivity of the biosensor is 7.67-fold better if graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle are used. This could be ascribed to improvement of the conductivity between graphene nanosheets due to introduction of gold nanoparticles, ultrafast charge transfer from CdTe-CdS core-shell quantum dot to graphene nanosheets and gold nanoparticle due to unique electrochemical properties of the CdTe-CdS core-shell quantum dot and good biocompatibility of gold nanoparticle for glucose oxidase. The biosensor is of best sensitivity in all glucose

  5. An ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle

    Graphical abstract: We first reported an ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since promising their electrocatalytic synergy towards glucose was achieved, the biosensor showed high sensitivity (5762.8 nA nM-1 cm-2), low detection limit (S/N = 3) (3 x 10-12 M) and fast response time (0.045 s). - Abstract: The paper reported an ultrasensitive electrochemical biosensor for glucose which was based on CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since efficient electron transfer between glucose oxidase and the electrode was achieved, the biosensor showed high sensitivity (5762.8 nA nM-1 cm-2), low detection limit (S/N = 3) (3 x 10-12 M), fast response time (0.045 s), wide calibration range (from 1 x 10-11 M to 1 x 10-8 M) and good long-term stability (26 weeks). The apparent Michaelis-Menten constant of the glucose oxidase on the medium, 5.24 x 10-6 mM, indicates excellent bioelectrocatalytic activity of the immobilized enzyme towards glucose oxidation. Moreover, the effects of omitting graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle were also investigated. The result showed sensitivity of the biosensor is 7.67-fold better if graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle are used. This could be ascribed to improvement of the conductivity between graphene nanosheets due to introduction of gold nanoparticles, ultrafast charge transfer from CdTe-CdS core-shell quantum dot to graphene nanosheets and gold nanoparticle due to unique electrochemical properties of the CdTe-CdS core-shell quantum dot and good biocompatibility of gold nanoparticle for glucose oxidase. The biosensor is of best sensitivity in all glucose biosensors based on graphene nanomaterials up to now and has

  6. Ultrafast nonlinear optics

    Leburn, Christopher; Reid, Derryck

    2013-01-01

    The field of ultrafast nonlinear optics is broad and multidisciplinary, and encompasses areas concerned with both the generation and measurement of ultrashort pulses of light, as well as those concerned with the applications of such pulses. Ultrashort pulses are extreme events – both in terms of their durations, and also the high peak powers which their short durations can facilitate. These extreme properties make them powerful experiment tools. On one hand, their ultrashort durations facilitate the probing and manipulation of matter on incredibly short timescales. On the other, their ultrashort durations can facilitate high peak powers which can drive highly nonlinear light-matter interaction processes. Ultrafast Nonlinear Optics covers a complete range of topics, both applied and fundamental in nature, within the area of ultrafast nonlinear optics. Chapters 1 to 4 are concerned with the generation and measurement of ultrashort pulses. Chapters 5 to 7 are concerned with fundamental applications of ultrasho...

  7. Charge density wave dynamics from ultrafast XUV ARPES

    Frassetto F.

    2013-03-01

    Full Text Available Ultrafast angle–resolved XUV photoemission reveals the time- and momentum-dependent electronic structure of 1T–TaS2, a hybrid Mott and charge-density-wave insulator. Both electronic orderings melt well before the lattice responds, suggesting that electronic correlations play a role not just in the Mott localization but in the CDW ordering as well.

  8. ICT4D: A Computer Science Perspective

    Sutinen, Erkki; Tedre, Matti

    The term ICT4D refers to the opportunities of Information and Communication Technology (ICT) as an agent of development. Research in that field is often focused on evaluating the feasibility of existing technologies, mostly of Western or Far East Asian origin, in the context of developing regions. A computer science perspective is complementary to that agenda. The computer science perspective focuses on exploring the resources, or inputs, of a particular context and on basing the design of a technical intervention on the available resources, so that the output makes a difference in the development context. The modus operandi of computer science, construction, interacts with evaluation and exploration practices. An analysis of a contextualized information technology curriculum of Tumaini University in southern Tanzania shows the potential of the computer science perspective for designing meaningful information and communication technology for a developing region.

  9. Opening the Black Box of ICT4D: Advancing Our Understanding of ICT4D Partnerships

    Park, Sung Jin

    2013-01-01

    The term, Information and Communication Technologies for Development (ICT4D), pertains to programs or projects that strategically use ICTs (e.g. mobile phones, computers, and the internet) as a means toward the socio-economic betterment for the poor in developing contexts. Gaining the political and financial support of the international community…

  10. Ultrafast gas switching experiments

    We describe recent experiments which studied the physics of ultrafast gas breakdown under the extreme overvoltages which occur when a high pressure gas switch is pulse charged to hundreds of kV in 1 ns or less. The highly overvolted peaking gaps produce powerful electromagnetic pulses with risetimes Khz at > 100 kV/m E field

  11. Magnetic properties of 4d transition-metal clusters

    We analyze the stability of magnetic states obtained within the tight-binding model solved by molecular dynamics for cubo-octahedral (fcc) and icosahedral clusters of 3d (Ni and Co) and 4d (Pd, Rh, and Ru) transition metals. The magnetic states are stabilized by the Hund close-quote s rule exchange interaction between the d orbitals. Taking realistic parameters deduced from band structure calculations and spectroscopic data, we obtained saturated ferromagnetism for Ni13, Co13, and Pd13 clusters, while Rh13 fcc and Ru13 clusters are partially magnetic, with an antiferromagnetic orientation of the moments on the central atoms in Ru clusters. Our results for 4d transition-metal clusters agree qualitatively with the recent experimental data and with other calculations. Metastable magnetic clusters were identified in several situations. We found a dependence of the equilibrium lattice constant on the magnetization in the considered clusters which may be explained by the character of wave functions in the cluster electronic structure. copyright 1996 The American Physical Society

  12. Ultrafast excited state dynamics in 9,9'-bifluorenylidene.

    Conyard, Jamie; Heisler, Ismael A; Browne, Wesley R; Feringa, Ben L; Amirjalayer, Saeed; Buma, Wybren Jan; Woutersen, Sander; Meech, Stephen R

    2014-08-01

    9,9'-Bifluorenylidene has been proposed as an alternative and flexible electron acceptor in organic photovoltaic cells. Here we characterize its excited state properties and photokinetics, combining ultrafast fluorescence and transient IR measurements with quantum chemical calculations. The fluorescence decay is ultrafast (sub-100 fs) and remarkably independent of viscosity. This suggests that large scale structure change is not the primary relaxation mode. The ultrafast decay populates a dark state characterized by distinct vibrational and electronic spectra. This state decays with a 6 ps time constant to a hot ground state that ultimately populates the initial state with a 20 ps time constant; these times are also insensitive to solvent viscosity. No metastable intermediate structures are resolved in the photocycle after population of the dark state. The implications of these results for the operation of 9,9'-bifluorenylidene as an electron acceptor and as a potential molecular switch are discussed. PMID:25025227

  13. Influence of the electron-cation interaction on electron mobility in dye-sensitized ZnO and TiO.sub.2./sub. nanocrystals: a study using ultrafast terahertz spectroscopy

    Němec, Hynek; Rochford, J.; Taratula, O.; Galoppini, E.; Kužel, Petr; Polívka, T.; Yartsev, A.; Sundström, V.

    2010-01-01

    Roč. 104, č. 19 (2010), 197401/1-197401/4. ISSN 0031-9007 R&D Projects: GA ČR(CZ) GP202/09/P099; GA AV ČR(CZ) IAA100100902; GA MŠk LC512 Institutional research plan: CEZ:AV0Z10100520 Keywords : ultrafast dynamics * terahertz spectroscopy * semiconductor nanocrystals * dye-sensitized semiconductors Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 7.621, year: 2010

  14. Ultrafast spectroscopic imaging of exfoliated graphene

    Grancini, Giulia; Martino, Nicola; Petrozza, Annamaria; Lanzani, Guglielmo [Center for Nano Science and Technology rate at PoliMi, Istituto Italiano di Tecnologia, Via Giovanni Pascoli, 70/3, 20133 Milano (Italy); Bianchi, Massimiliano; Rizzi, Laura Giorgia; Sordan, Roman [L-NESS, Department of Physics, Polo di Como, Politecnico di Milano, Via Anzani 42, 22100 Como (Italy); Russo, Valeria [Department of Energetics, Politecnico di Milano, Via Lambruschini 4, 20156 Milano (Italy); Li Bassi, Andrea; Casari, Carlo Spartaco [Center for Nano Science and Technology rate at PoliMi, Istituto Italiano di Tecnologia, Via Giovanni Pascoli, 70/3, 20133 Milano (Italy); Department of Energetics, Politecnico di Milano, Via Lambruschini 4, 20156 Milano (Italy)

    2012-12-15

    In this paper we investigate the carrier cooling dynamics in graphene flakes exploiting ultrafast transient absorption imaging technique. This tool enables us to combine nanoscale spatial resolution and sub-picosecond (ps) time resolution. It provides many advantages over the standard transient absorption techniques because it directly investigates the excited state dynamics at a local scale that would be usually averaged out. The local dynamics show a photobleaching recovery in the first ps, assigned to cooling by electron-phonon scattering. We found that the photoexcited carrier dynamics is spatially uniform over the micrometer-sized exfoliated graphene layer. Ultrafast pump-probe technique is combined with an optical microscope to investigate the local excited state dynamics in graphene flakes. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  15. Ultrafast spectroscopic imaging of exfoliated graphene

    In this paper we investigate the carrier cooling dynamics in graphene flakes exploiting ultrafast transient absorption imaging technique. This tool enables us to combine nanoscale spatial resolution and sub-picosecond (ps) time resolution. It provides many advantages over the standard transient absorption techniques because it directly investigates the excited state dynamics at a local scale that would be usually averaged out. The local dynamics show a photobleaching recovery in the first ps, assigned to cooling by electron-phonon scattering. We found that the photoexcited carrier dynamics is spatially uniform over the micrometer-sized exfoliated graphene layer. Ultrafast pump-probe technique is combined with an optical microscope to investigate the local excited state dynamics in graphene flakes. (Copyright copyright 2012 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  16. Development operators on 4D moving object databases

    JUN Sung-woo; LEE Yang-koo; KIM Sang-ho; CHI Jeong-hee; RYU Keun-ho

    2004-01-01

    In this paper we propose four-dimensional (4D) operators, which can be used to deal with sequential changes of topological relationships between 4D moving objects and we call them 4D development operators. In contrast to the existing operators, we can apply the operators to real applications on 4D moving objects. We also propose a new approach to define them. The approach is based on a dimension-separated method, which considers x-y coordinates and z coordinates separately. In order to show the applicability of our operators, we show the algorithms for the proposed operators and development graph between 4D moving objects.

  17. Partially coherent ultrafast spectrography

    Bourassin-Bouchet, C.; Couprie, M.-E.

    2015-01-01

    Modern ultrafast metrology relies on the postulate that the pulse to be measured is fully coherent, that is, that it can be completely described by its spectrum and spectral phase. However, synthesizing fully coherent pulses is not always possible in practice, especially in the domain of emerging ultrashort X-ray sources where temporal metrology is strongly needed. Here we demonstrate how frequency-resolved optical gating (FROG), the first and one of the most widespread techniques for pulse c...

  18. Ultrafast Magnetization Dynamics

    Woodford, S.

    2008-01-01

    This thesis addresses ultrafast magnetization dynamics from a theoretical perspective. The manipulation of magnetization using the inverse Faraday effect has been studied, as well as magnetic relaxation processes in quantum dots. The inverse Faraday effect – the generation of a magnetic field by nonresonant, circularly polarized light – offers the possibility to control and reverse magnetization on a timescale of a few hundred femtoseconds. This is important both for the technological advant...

  19. 4+D digital engineering for advanced nuclear energy systems

    Nuclear power plants (NPPs) require massive quantity of data during the design, construction, operation, maintenance and decommissioning stages because of their special features like size, cost, radioactivity, and so forth. The system engineering thus calls for a fully automated way of managing the information flow spanning their life cycle. In line with practice in disciplines of naval architecture, aerospace engineering, and automotive manufacturing, the paper proposes total digital systems engineering based on three-dimensional (3D) computer-aided design (CAD) models. The signature in the proposal lies with the four-plus-dimensional (4+D) TechnologyTM, a critical know-how for digital management. The so-called OPIUM (Optimized Plant Integrated Ubiquitous Management) features a 4+D TechnologyTM for nuclear energy systems engineering. The technology proposed in the 3D space and time plus cost coordinates, i.e. 4+D, is the backbone of digital engineering in the nuclear systems design and management. Based on an integrated 3D configuration management system, OPIUM consists of solutions NOTUS (Nuclear Optimization Technique Ubiquitous System), VENUS (Virtual Engineering Nuclear Ubiquitous System), INUUS (Informatics Nuclear Utilities Ubiquitous System), JANUS (Junctional Analysis Numerical Ubiquitous System) and EURUS (Electronic Unit Research Ubiquitous System). These solutions will help initial simulation capability for NPPs to supply the crucial information. NOTUS contributes to reducing the construction cost of the NPPs by optimizing the component manufacturing procedure and the plant construction process. Planning and scheduling construction projects can thus benefit greatly by integrating traditional management techniques with digital process simulation visualization. The 3D visualization of construction processes and the resulting products intrinsically afford most of the advantages realized by incorporating a purely schedule level detail based the 4+D system

  20. Sex-differential genetic effect of phosphodiesterase 4D (PDE4D on carotid atherosclerosis

    Guo Yuh-Cherng

    2010-06-01

    Full Text Available Abstract Background The phosphodiesterase 4D (PDE4D gene was reported as a susceptibility gene to stroke. The genetic effect might be attributed to its role in modulating the atherogenic process in the carotid arteries. Using carotid intima-media thickness (IMT and plaque index as phenotypes, the present study sought to determine the influence of this gene on subclinical atherosclerosis. Methods Carotid ultrasonography was performed on 1013 stroke-free subjects who participated in the health screening programs (age 52.6 ± 12.2; 47.6% men. Genotype distribution was compared among the high-risk (plaque index ≥ 4, low-risk (index = 1-3, and reference (index = 0 groups. We analyzed continuous IMT data and further dichotomized IMT data using mean plus one standard deviation as the cutoff level. Because the plaque prevalence and IMT values displayed a notable difference between men and women, we carried out sex-specific analyses in addition to analyzing the overall data. Rs702553 at the PDE4D gene was selected because it conferred a risk for young stroke in our previous report. Previous young stroke data (190 cases and 211 controls with an additional 532 control subjects without ultrasonic data were shown as a cross-validation for the genetic effect. Results In the overall analyses, the rare homozygote of rs702553 led to an OR of 3.1 (p = 0.034 for a plaque index ≥ 4. When subjects were stratified by sex, the genetic effect was only evident in men but not in women. Comparing male subjects with plaque index ≥ 4 and those with plaque index = 0, the TT genotype was over-represented (27.6% vs. 13.4%, p = 0.008. For dichotomized IMT data in men, the TT genotype had an OR of 2.1 (p = 0.032 for a thicker IMT at the common carotid artery compared with the (AA + AT genotypes. In women, neither IMT nor plaque index was associated with rs702553. Similarly, SNP rs702553 was only significant in young stroke men (OR = 1.8, p = 0.025 but not in women (p = 0

  1. Dual-tip-enhanced ultrafast CARS nanoscopy

    Coherent anti-Stokes Raman scattering (CARS) and, in particular, femtosecond adaptive spectroscopic techniques (FAST CARS) have been successfully used for molecular spectroscopy and microscopic imaging. Recent progress in ultrafast nano-optics provides flexibility in generation and control of optical near fields, and holds promise to extend CARS techniques to the nanoscale. In this theoretical study, we demonstrate ultrafast subwavelentgh control of coherent Raman spectra of molecules in the vicinity of a plasmonic nanostructure excited by ultrashort laser pulses. The simulated nanostructure design provides localized excitation sources for CARS by focusing incident laser pulses into subwavelength hot spots via two self-similar nanolens antennas connected by a waveguide. Hot-spot-selective dual-tip-enhanced CARS (2TECARS) nanospectra of DNA nucleobases are obtained by simulating optimized pump, Stokes and probe near fields using tips, laser polarization- and pulse-shaping. This technique may be used to explore ultrafast energy and electron transfer dynamics in real space with nanometre resolution. (paper)

  2. Pros and cons for C4d as a biomarker

    Cohen, Danielle; Colvin, Robert B.; Mohamed R. Daha; Drachenberg, Cinthia B; Haas, Mark; Nickeleit, Volker; Salmon, Jane E.; Sis, Banu; ZHAO, Ming-Hui; Bruijn, Jan A.; Bajema, Ingeborg M.

    2012-01-01

    The introduction of C4d in daily clinical practice in the late nineties aroused an ever-increasing interest in the role of antibody-mediated mechanisms in allograft rejection. As a marker of classical complement activation, C4d made it possible to visualize the direct link between anti-donor antibodies and tissue injury at sites of antibody binding in a graft. With the expanding use of C4d worldwide several limitations of C4d were identified. For instance, in ABO-incompatible transplantations...

  3. Pros and cons for C4d as a biomarker.

    Cohen, Danielle; Colvin, Robert B; Daha, Mohamed R; Drachenberg, Cinthia B; Haas, Mark; Nickeleit, Volker; Salmon, Jane E; Sis, Banu; Zhao, Ming-Hui; Bruijn, Jan A; Bajema, Ingeborg M

    2012-04-01

    The introduction of C4d in daily clinical practice in the late nineties aroused an ever-increasing interest in the role of antibody-mediated mechanisms in allograft rejection. As a marker of classical complement activation, C4d made it possible to visualize the direct link between anti-donor antibodies and tissue injury at sites of antibody binding in a graft. With the expanding use of C4d worldwide several limitations of C4d were identified. For instance, in ABO-incompatible transplantations C4d is present in the majority of grafts but this seems to point at 'graft accommodation' rather than antibody-mediated rejection. C4d is now increasingly recognized as a potential biomarker in other fields where antibodies can cause tissue damage, such as systemic autoimmune diseases and pregnancy. In all these fields, C4d holds promise to detect patients at risk for the consequences of antibody-mediated disease. Moreover, the emergence of new therapeutics that block complement activation makes C4d a marker with potential to identify patients who may possibly benefit from these drugs. This review provides an overview of the past, present, and future perspectives of C4d as a biomarker, focusing on its use in solid organ transplantation and discussing its possible new roles in autoimmunity and pregnancy. PMID:22297669

  4. Ultrafast microchannel plate photomultipliers.

    Kume, H; Koyama, K; Nakatsugawa, K; Suzuki, S; Fatlowitz, D

    1988-03-15

    Performance characteristics of several new types of photomultiplier tubes (PMT) with microchannel plates (MCP) are presented in this paper. They are the MCP-PMT with 6-microm diam channels, MCP-PMT with an S-l photocathode, and MCP-PMT with multi (discrete) anode and gatable MCP-PMT. Important requirements of an optical detector for picosecond lasers, fluorescence measurements, and material analysis are low light detectability, ultrafast time response, and versatile operation including modulation. The basic configuration, characteristics, and practical results of these detectors are described. PMID:20531532

  5. Ultrafast Carrier Dynamics in the Large Magnetoresistance Material WTe$_{2}$

    Dai, Y. M.; Bowlan, J.; Li, H.; Miao, H; Wu, S. F.; Kong, W. D.; Shi, Y. G.; Trugman, S. A.; Zhu, J. -X.; H. Ding; Taylor, A. J.; Yarotski, D. A.; Prasankumar, R. P.

    2015-01-01

    Ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large magnetoresistance material WTe$_{2}$. Our experiments reveal a fast relaxation process occurring on a sub-picosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of $\\sim$5-15 picoseconds, is attributed to phonon-assisted electron-hole recombination. As the tempe...

  6. Ultrafast imaging of photoelectron packets generated from graphite surface

    Raman, Ramani K.; Tao, Zhensheng; Han, Tzong-Ru; Ruan, Chong-Yu

    2009-01-01

    We present an electron projection imaging method to study the ultrafast evolution of photoelectron density distribution and transient fields near the surface. The dynamical profile of the photoelectrons from graphite reveals an origin of a thermionic emission, followed by an adiabatic process leading to electron acceleration and cooling before a freely expanding cloud is established. The hot electron emission is found to couple with a surface charge dipole layer formation, with a sheet densit...

  7. Hard-X-Ray-Induced Multistep Ultrafast Dissociation

    Travnikova, Oksana; Marchenko, Tatiana; Goldsztejn, Gildas; Jänkälä, Kari; Sisourat, Nicolas; Carniato, Stéphane; Guillemin, Renaud; Journel, Loïc; Céolin, Denis; Püttner, Ralph; Iwayama, Hiroshi; Shigemasa, Eiji; Piancastelli, Maria Novella; Simon, Marc

    2016-05-01

    Creation of deep core holes with very short (τ ≤1 fs ) lifetimes triggers a chain of relaxation events leading to extensive nuclear dynamics on a few-femtosecond time scale. Here we demonstrate a general multistep ultrafast dissociation on an example of HCl following Cl 1 s →σ* excitation. Intermediate states with one or multiple holes in the shallower core electron shells are generated in the course of the decay cascades. The repulsive character and large gradients of the potential energy surfaces of these intermediates enable ultrafast fragmentation after the absorption of a hard x-ray photon.

  8. Fourier information optics for the ultrafast time domain.

    Weiner, Andrew M

    2008-02-01

    Ultrafast photonic signal processing based on Fourier optics principles offers exciting possibilities to go beyond the processing speeds of electronics technologies for applications in high-speed fiber communications and ultrawideband wireless. I review our recent work on processing of ultrafast optical signals via conversion between time, space, and optical frequency (Fourier) domains. Specific topics include optical arbitrary waveform generation, application of optical pulse shaping technologies for wavelength-parallel compensation of fiber transmission impairments and for experimental studies of optical code-division multiple-access communications, and application of photonic methods for precompensation of dispersion effects in wireless transmission of radio-frequency signals over ultrawideband antenna links. PMID:18239704

  9. Hard-X-Ray-Induced Multistep Ultrafast Dissociation.

    Travnikova, Oksana; Marchenko, Tatiana; Goldsztejn, Gildas; Jänkälä, Kari; Sisourat, Nicolas; Carniato, Stéphane; Guillemin, Renaud; Journel, Loïc; Céolin, Denis; Püttner, Ralph; Iwayama, Hiroshi; Shigemasa, Eiji; Piancastelli, Maria Novella; Simon, Marc

    2016-05-27

    Creation of deep core holes with very short (τ≤1  fs) lifetimes triggers a chain of relaxation events leading to extensive nuclear dynamics on a few-femtosecond time scale. Here we demonstrate a general multistep ultrafast dissociation on an example of HCl following Cl 1s→σ^{*} excitation. Intermediate states with one or multiple holes in the shallower core electron shells are generated in the course of the decay cascades. The repulsive character and large gradients of the potential energy surfaces of these intermediates enable ultrafast fragmentation after the absorption of a hard x-ray photon. PMID:27284654

  10. 32 CFR 1645.4 - Exclusion from Class 4-D.

    2010-07-01

    ... MINISTERS OF RELIGION § 1645.4 Exclusion from Class 4-D. A registrant is excluded from Class 4-D when his... duly ordained minister of religion in accordance with the ceremonial rite or discipline of a church... principles of religion and administer the ordinances of public worship, as embodied in the creed...

  11. Direct observation of the ultrafast electron transfer process in a polymer/fullerene blend. : Section Title: Physical Properties of Synthetic High Polymers

    Brabec, Ch J.; Zerza, G.; Sariciftci, N. S.; Cerullo, G.; Lanzani, G.; De Silvestri, S.; Hummelen, J. C.

    2001-01-01

    Optical studies on conjugated polymer-fullerene blends are performed with sub-10-fs temporal resoln. The photoinduced electron transfer process is directly monitored in the time domain, obtaining a forward electron transfer time const. of 45 fs. [on SciFinder(R)

  12. 9th International Symposium on Ultrafast Processes in Spectroscopy

    Silvestri, S; Denardo, G

    1996-01-01

    This volume is a collection of papers presented at the Ninth International Symposium on "Ultrafast Processes in Spectroscopy" (UPS '95) held at the International Centre for Theo­ retical Physics (ICTP), Trieste (Italy), October 30 -November 3, 1995. These meetings have become recognized as the major forum in Europe for discussion of new work in this rapidly moving field. The UPS'95 Conference in Trieste brought together a multidisciplinary group of researchers sharing common interests in the generation of ultrashort optical pulses and their application to studies of ultrafast phenomena in physics, chemistry, material science, electronics, and biology. It was attended by approximately 250 participants from 20 countries and the five-day program comprises more than 200 papers. The progress of both technology and applications in the field of ultrafast processes during these last years is truly remarkable. The advent of all solid state femtosecond lasers and the extension of laser wavelengths by frequency convers...

  13. Femtosecond laser studies of ultrafast intramolecular processes

    Hayden, C. [Sandia National Laboratories, Livermore, CA (United States)

    1993-12-01

    The goal of this research is to better understand the detailed mechanisms of chemical reactions by observing, directly in time, the dynamics of fundamental chemical processes. In this work femtosecond laser pulses are used to initiate chemical processes and follow the progress of these processes in time. The authors are currently studying ultrafast internal conversion and subsequent intramolecular relaxation in unsaturated hydrocarbons. In addition, the authors are developing nonlinear optical techniques to prepare and monitor the time evolution of specific vibrational motions in ground electronic state molecules.

  14. Ultrafast characterization of the electron injection from CdSe quantum dots and dye N719 co-sensitizers into TiO2 using sulfide based ionic liquid for enhanced long term stability

    Combination of inorganic quantum dots (QDs) and organic/metallorganic dyes as supracollectors nanocomposites could have an important role on the development of efficient photovoltaic devices based on the synergistic action of the hybrid-sensitizers. Here we have analyzed the combination of CdSe QDs and polypyridil N719 ruthenium dye. By ultrafast transient grating measurements we show that the cascading structure (type II) of this system takes full advantage to augment electron injection and hole regeneration efficiencies. Co-sensitized TiO2 electrodes lead to an improvement in charge separation, increasing the number of injected electrons from the CdSe QDs to the TiO2 as a consequence of the suppression of back reaction, by fast regeneration of holes by the dye action. The potentiality of this supracollector system has been verified in a complete cell configuration. Sulfide/polysulfide based ionic liquid in which both sensitizers (QD and dye) are stable has been employed as hole conducting media. In spite of the limited efficiencies of the analyzed cells, the higher photocurrents measured for CdSe/N719 co-sensitization compared to the cells sensitized using a single sensitizer constitutes a valid proof of the concept. Impedance spectroscopy unveiled the recombination limitation of the analyzed cells. On the other hand, ionic liquid exhibits an enhanced cell stability maintaining cell efficiency after one week and keeping it at 80% after 21 days. The reported results highlight a huge potential of the synergetic combination of QD and dyes for improving solar cell performance and of novel sulfide/polysulfide ionic liquid-based electrolytes for enhancing long term stability and sustainability of QD sensitizers

  15. Ultrafast transient absorption studies on photosystem I reaction centers from Chlamydomonas reinhardtii. 2: mutations near the P700 reaction center chlorophylls provide new insight into the nature of the primary electron donor.

    Holzwarth, Alfred R; Müller, Marc G; Niklas, Jens; Lubitz, Wolfgang

    2006-01-15

    The energy transfer and charge separation kinetics in several core Photosystem I particles of Chlamydomonas reinhardtii with point mutations around the PA and PB reaction center chlorophylls (Chls) have been studied using ultrafast transient absorption spectroscopy in the femtosecond to nanosecond time range to characterize the influence on the early electron transfer processes. The data have been analyzed in terms of kinetic compartment models. The adequate description of the transient absorption kinetics requires three different radical pairs in the time range up to approximately 100 ps. Also a charge recombination process from the first radical pair back to the excited state is present in all the mutants, as already shown previously for the wild-type (Müller, M. G., J. Niklas, W. Lubitz, and A. R. Holzwarth. 2003. Biophys. J. 85:3899-3922; and Holzwarth, A. R., M. G. Müller, J. Niklas, and W. Lubitz. 2005. J. Phys. Chem. B. 109:5903-59115). In all mutants, the primary charge separation occurs with the same effective rate constant within the error limits as in the wild-type (>350 ns(-1)), which implies an intrinsic rate constant of charge separation of hydrogen bond to the keto carbonyl of Chl PA, only a slight slowing down of the secondary electron transfer is observed. Finally for mutant A-W679A, which has the Trp near the PA Chl replaced, either no pronounced effect or, at best, a slight increase on the secondary electron transfer rate constants is observed. The effective charge recombination rate constant is modified in all mutants to some extent, with the strongest effect observed in mutant B-H656C. Our data strongly suggest that the Chls of the PA and PB pair, constituting what is traditionally called the "primary electron donor P700", are not oxidized in the first electron transfer process, but rather only in the secondary electron transfer step. We thus propose a new electron transfer mechanism for Photosystem I where the accessory Chl(s) function as

  16. Graphene in Ultrafast and Ultrastrong Laser Pulses

    Koochakikelardeh, Hamed; Apalkov, Vadym; Stockman, Mark

    2015-03-01

    We have shown that graphene subjected to an ultrafast (near-single-oscillation pulse) and strong (F ~ 1-3 V/Å) pulse exhibits fundamental behavior dramatically different from both insulators and metals. In such an ultrafast and ultrastrong field, the electron dynamics is coherent, in contrast to relatively long pulses (τ>100 fs) where the electron's dephasing becomes important leading to incoherent dynamics. Electron transfer from the valence band (VB) to the conduction band (CB) is deeply irreversible i.e., non-adiabatic, in which the residual CB population (after pulse ends) is close to the maximum one. The residual CB population as a function of wave vector is nonuniform with a few strongly localized spots near the Dirac points, at which the CB population is almost 100%. Furthermore, it is shown the direction of charge transfer depends on the pulse amplitude. Namely, at small pulse amplitude, =1 V/Å, it is in opposite direction of the pulse maximum (negative transferred charge). Consequently, in terms of charge transport, graphene at small pulse intensities behaves as a dielectric while at large intensities acts as a metal. These femtosecond currents and charge transfer in graphene may provide fundamental basis for detection and calibration of ultrashort intense laser pulses and are promising for petahertz information processing. This work was supported by U.S. Office of Naval Research No. N00014-13-1-0649 and NSF Grant No. ECCS-1308473.

  17. Fourteenth International Conference on Ultrafast Phenomena

    Kobayashi, Takayoshi; Kobayashi, Tetsuro; Nelson, Keith A; Silvestri, Sandro; Ultrafast Phenomena XIV

    2005-01-01

    Ultrafast Phenomena XIV presents the latest advances in ultrafast science, including ultrafast laser and measurement technology as well as studies of ultrafast phenomena. Pico-, femto-, and atosecond processes relevant in physics, chemistry, biology and engineering are presented. Ultrafast technology is now having a profound impact within a wide range of applications, among them imaging, material diagnostics, and transformation and high-speed optoelectronics. This book summarizes results presented at the 14th Ultrafast Phenomena Conference and reviews the state of the art in this important and rapidly advancing field.

  18. Sixteenth International Conference on Ultrafast Phenomena

    Corkum, Paul; Nelson, Keith A; Riedle, Eberhard; Schoenlein, Robert W; Ultrafast Phenomena XVI

    2009-01-01

    Ultrafast Phenomena XVI presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultrafast technology has a profound impact in a wide range of applications, amongst them biomedical imaging, chemical dynamics, frequency standards, material processing, and ultrahigh speed communications. This book summarizes the results presented at the 16th International Conference on Ultrafast Phenomena and provides an up-to-date view of this important and rapidly advancing field.

  19. Fifteenth International Conference on Ultrafast Phenomena

    Corkum, Paul; Miller, R. J. Dwayne; Weiner, Andrew M; Ultrafast Phenomena XV

    2007-01-01

    Ultrafast Phenomena XV presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond, and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultrafast technology has a profound impact in a wide range of applications, among them biomedical imaging, chemical dynamics, frequency standards, materials processing, and ultrahigh-speed communications. This book summarizes the results presented at the 15th International Conference on Ultrafast Phenomena and provides an up-to-date view of this important and rapidly advancing field.

  20. Attosecond delay of xenon $4d$ photoionization at the giant resonance and Cooper minimum

    Magrakvelidze, Maia; Chakraborty, Himadri S

    2016-01-01

    A Kohn-Sham time-dependent local-density-functional scheme is utilized to predict attosecond time delays of xenon 4d photoionization that involves the 4d giant dipole resonance and Cooper minimum. The fundamental effect of electron correlations to uniquely determine the delay at both regions is demonstrated. In particular, for the giant dipole resonance, the delay underpins strong collective effect, emulating the recent prediction at C60 giant plasmon resonance [T. Barillot et al, Phys. Rev. A 91, 033413 (2015)]. For the Cooper minimum, a qualitative similarity with a photorecombination experiment near argon 3p minimum [S. B. Schoun et al, Phys. Rev. Lett. 112, 153001 (2014)] is found. The result should encourage attosecond measurements of Xe 4d photoemission.

  1. Ultrafast Pulse Radiolysis Using a Terawatt Laser Wakefield Accelerator

    Oulianov, D A; Gosztola, D J; Korovyanko, O J; Rey de Castro, R C; Shkrob, I A; Crowell, Robert A.; Gosztola, David J.; Korovyanko, Oleg J.; Oulianov, Dmitri A.; Rey-de-Castro, Roberto C.; Shkrob, Ilya A.

    2006-01-01

    We report the first ultrafast pulse radiolysis transient absorption spectroscopy measurements from the Terawatt Ultrafast High Field Facility (TUHFF) at Argonne National Laboratory. TUHFF houses a 20 TW Ti:sapphire laser system that generates 2.5 nC sub-picosecond pulses of multi-MeV electrons at 10 Hz using laser wakefield acceleration. The system has been specifically optimized for kinetic measurements in a pump-probe fashion. This requires averaging over many shots which necessitates stable, reliable generation of electron pulses. The latter were used to generate excess electrons in pulse radiolysis of liquid water and concentrated solutions of perchloric acid. The hydronium ions in the acidic solutions react with the hydrated electrons resulting in the rapid decay of the transient absorbance at 800 nm on the picosecond time scale. Time resolution of a few picoseconds has been demonstrated. The current time resolution is determined primarily by the physical dimensions of the sample and the detection sensit...

  2. 4D-Var or Ensemble Kalman Filter

    Kalnay, E.; Li, H.; Yang, S.; Miyoshi, T.; Ballabrera, J.

    2007-05-01

    We consider the relative advantages of two advanced data assimilation systems, 4D-Var and ensemble Kalman filter (EnKF), currently in use or considered for operational implementation. We explore the impact of tuning assimilation parameters such as the assimilation window length and background error covariance in 4D-Var, the variance inflation in EnKF, and the effect of model errors and reduced observation coverage in both systems. For short assimilation windows EnKF gives more accurate analyses. Both systems reach similar levels of accuracy if long windows are used for 4D-Var, and for infrequent observations, when ensemble perturbations grow nonlinearly and become non-Gaussian, 4D-Var attains lower errors than EnKF. Results obtained with variations of EnKF using operational models and both simulated and real observations are reviewed. A table summarizes the pros and cons of the two methods.

  3. Motion management with phase-adapted 4D-optimization

    Nohadani, Omid; Seco, Joao; Bortfeld, Thomas

    2010-01-01

    Cancer treatment with ionizing radiation is often compromised by organ motion, in particular for lung cases. Motion uncertainties can significantly degrade an otherwise optimized treatment plan. We present a spatiotemporal optimization method, which takes into account all phases of breathing via the corresponding 4D-CTs and provides a 4D-optimal plan that can be delivered throughout all breathing phases. Monte Carlo dose calculations are employed to warrant for highest dosimetric accuracy, as...

  4. The Link between ICT4D and Modernization Theory

    Marlene Kunst

    2015-01-01

    Full Text Available For some decades western institutions have shared an enormous enthusiasm for Information and Communication Technologies for Development (ICT4D. Nevertheless, despite the field’s ever-increasing importance, research on it remains fragmented and lacks a theoretical foundation. By establishing a link between ICT4D and Modernization theory as one of the major development models, this paper aims to add some theoretical reflections to the body of existing research. Initially, a literature review of the most significant authors of Modernization theory serves as a theoretical base. Subsequently, empirical findings are systematized and embedded in the theoretical framework. The leading question is, whether ICT4D is connected to Modernization theory’s main lines of thought, both in theory and in the field. Modernization theory was chosen as a reference point, as even though it has frequently been marked as outdated, some argue that ICT4D has brought about its revival: Led by a technocratic mindset, actors in the field have indeed assumed ICTs to be context-free tools, which is one of the reasons why ICT4D has so far not been an unmitigated success. As there is a lack of systematic research on ICT4D, this paper is explorative in nature. It is certainly beyond the author’s scope to make any definite statements on how development cooperation has hitherto handled ICT4D, as the field is too complex. Instead, light will be shed on some trends that can be identified in the field of ICT4D to date.

  5. Play as Freedom : Implications for ICT4D

    Ferreira, Pedro

    2015-01-01

    Information and Communication Tech nologies for Development (ICT4D) deals with understanding the relationship between modern technology use and social and economic development. While play may not appear as an immediate concern to the field, a recent body of work has emerged questioning the role of play in ICT4D and the reasons behind its apparent dismissal. Some have even argued that aspects of pleasure and enjoyment get only marginal treatment within academic studies of technology more gener...

  6. The Link between ICT4D and Modernization Theory

    Marlene Kunst

    2015-01-01

    For some decades western institutions have shared an enormous enthusiasm for Information and Communication Technologies for Development (ICT4D). Nevertheless, despite the field’s ever-increasing importance, research on it remains fragmented and lacks a theoretical foundation. By establishing a link between ICT4D and Modernization theory as one of the major development models, this paper aims to add some theoretical reflections to the body of existing research. Initially, a lite...

  7. Ultrafast Surface Plasmonic Switch in Non-Plasmonic Metals

    Bévillon, E.; Colombier, J. P.; Recoules, V.; Zhang, H.; Li, C.; Stoian, R

    2015-01-01

    We demonstrate that ultrafast carrier excitation can drastically affect electronic structures and induce brief surface plasmonic response in non-plasmonic metals, potentially creating a plasmonic switch. Using first-principles molecular dynamics and Kubo-Greenwood formalism for laser-excited tungsten we show that carrier heating mobilizes d electrons into collective inter and intraband transitions leading to a sign flip in the imaginary optical conductivity, activating plasmonic properties fo...

  8. Reduced-order 4D-Var: a preconditioner for the Incremental 4D-Var data assimilation method

    Robert, Céline; Verron, Jacques

    2006-01-01

    This study demonstrates how the incremental 4D-Var data assimilation method can be applied efficiently preconditione d in an application to an oceanographic problem. The approach consists in performing a few iterations of the reduced-order 4D-Var prior to the incremental 4D-Var in the full space in order to achieve faster convergence. An application performed in the tropical Pacific Ocean, with assimilation of TAO temperature data, shows the method to be both feasible and efficient. It allows the global cost of the assimilation to be reduced by a factor of 2 without affecting the quality of the solution.

  9. 4-D-Var or ensemble Kalman filter?

    Kalnay, Eugenia; Li, Hong; Miyoshi, Takemasa; Yang, Shu-Chih; Ballabrera-Poy, Joaquim

    2007-10-01

    We consider the relative advantages of two advanced data assimilation systems, 4-D-Var and ensemble Kalman filter (EnKF), currently in use or under consideration for operational implementation. With the Lorenz model, we explore the impact of tuning assimilation parameters such as the assimilation window length and background error covariance in 4-D-Var, variance inflation in EnKF, and the effect of model errors and reduced observation coverage. For short assimilation windows EnKF gives more accurate analyses. Both systems reach similar levels of accuracy if long windows are used for 4-D-Var. For infrequent observations, when ensemble perturbations grow non-linearly and become non-Gaussian, 4-D-Var attains lower errors than EnKF. If the model is imperfect, the 4-D-Var with long windows requires weak constraint. Similar results are obtained with a quasi-geostrophic channel model. EnKF experiments made with the primitive equations SPEEDY model provide comparisons with 3-D-Var and guidance on model error and `observation localization'. Results obtained using operational models and both simulated and real observations indicate that currently EnKF is becoming competitive with 4-D-Var, and that the experience acquired with each of these methods can be used to improve the other. A table summarizes the pros and cons of the two methods.

  10. Ultra-fast computation of electronic spectra for large systems by tight-binding based simplified Tamm-Dancoff approximation (sTDA-xTB)

    Grimme, Stefan; Bannwarth, Christoph

    2016-08-01

    The computational bottleneck of the extremely fast simplified Tamm-Dancoff approximated (sTDA) time-dependent density functional theory procedure [S. Grimme, J. Chem. Phys. 138, 244104 (2013)] for the computation of electronic spectra for large systems is the determination of the ground state Kohn-Sham orbitals and eigenvalues. This limits such treatments to single structures with a few hundred atoms and hence, e.g., sampling along molecular dynamics trajectories for flexible systems or the calculation of chromophore aggregates is often not possible. The aim of this work is to solve this problem by a specifically designed semi-empirical tight binding (TB) procedure similar to the well established self-consistent-charge density functional TB scheme. The new special purpose method provides orbitals and orbital energies of hybrid density functional character for a subsequent and basically unmodified sTDA procedure. Compared to many previous semi-empirical excited state methods, an advantage of the ansatz is that a general eigenvalue problem in a non-orthogonal, extended atomic orbital basis is solved and therefore correct occupied/virtual orbital energy splittings as well as Rydberg levels are obtained. A key idea for the success of the new model is that the determination of atomic charges (describing an effective electron-electron interaction) and the one-particle spectrum is decoupled and treated by two differently parametrized Hamiltonians/basis sets. The three-diagonalization-step composite procedure can routinely compute broad range electronic spectra (0-8 eV) within minutes of computation time for systems composed of 500-1000 atoms with an accuracy typical of standard time-dependent density functional theory (0.3-0.5 eV average error). An easily extendable parametrization based on coupled-cluster and density functional computed reference data for the elements H-Zn including transition metals is described. The accuracy of the method termed sTDA-xTB is first

  11. Ultrafast Hierarchical OTDM/WDM Network

    Hideyuki Sotobayashi; Wataru Chujo; Takeshi Ozeki

    2003-01-01

    Ultrafast hierarchical OTDM/WDM network is proposed for the future core-network. We review its enabling technologies: C- and L-wavelength-band generation, OTDM-WDM mutual multiplexing format conversions, and ultrafast OTDM wavelengthband conversions.

  12. Ultrafast Mid-Infrared Nanoscopy of Strained Vanadium Dioxide Nanobeams.

    Huber, M A; Plankl, M; Eisele, M; Marvel, R E; Sandner, F; Korn, T; Schüller, C; Haglund, R F; Huber, R; Cocker, T L

    2016-02-10

    Long regarded as a model system for studying insulator-to-metal phase transitions, the correlated electron material vanadium dioxide (VO2) is now finding novel uses in device applications. Two of its most appealing aspects are its accessible transition temperature (∼341 K) and its rich phase diagram. Strain can be used to selectively stabilize different VO2 insulating phases by tuning the competition between electron and lattice degrees of freedom. It can even break the mesoscopic spatial symmetry of the transition, leading to a quasiperiodic ordering of insulating and metallic nanodomains. Nanostructuring of strained VO2 could potentially yield unique components for future devices. However, the most spectacular property of VO2-its ultrafast transition-has not yet been studied on the length scale of its phase heterogeneity. Here, we use ultrafast near-field microscopy in the mid-infrared to study individual, strained VO2 nanobeams on the 10 nm scale. We reveal a previously unseen correlation between the local steady-state switching susceptibility and the local ultrafast response to below-threshold photoexcitation. These results suggest that it may be possible to tailor the local photoresponse of VO2 using strain and thereby realize new types of ultrafast nano-optical devices. PMID:26771106

  13. Femtosecond magnetooptics and ultrafast magnetization reversal of ferromagnetic

    The model of ultrafast magnetic dynamics to describe the magnetization switching of ferromagnetics after the action of femtosecond laser pulses is proposed. The model suggests that processes of femtosecond duration are the property of orbital rather than spin magnetism. This assumption is shown not to contradict with the existing theoretical and experimental data. The equations for the description of the optical excitation of electrons in the Bloch model of ultrafast orbital dynamics in the electric dipole approximation are obtained. They have type of Bloch equations for the artificial vector. Its two components correspond to the electric polarization created by the electric field of the light wave. The third component is expressed through the orbital angular momentum of electrons. The analysis of solutions of these equations yielded the conditions under which the optical pump leaves non-equilibrium electron orbital angular momenta. The possibility of spin switching in the spin orbital field of nonequilibrium orbital momenta is discussed. - Highlights: • The ultrafast magnetic dynamics is caused by orbital rather than spin magnetism. • Action of femtosecond laser pump changes orbital electron state rather than spin one. • Optical excitation of electrons can be described by the equation for special vector V. • The vector V is composed of the electrical and orbital magnetic momenta of electrons. • The proposed model does not require a revision of the existing spin theory

  14. Rabi oscillations of Morris-Shore transformed $N$-state systems by elliptically polarized ultrafast laser pulses

    Kim, Hyosub; Lee, Han-gyeol; Ahn, Jaewook

    2015-01-01

    We present an experimental investigation of ultrafast-laser driven Rabi oscillations of atomic rubidium. Since the broadband spectrum of an ultrafast laser pulse simultaneously couples all the electronic hyperfine transitions between the excited and ground states, the complex excitation linkages involved with the D1 or D2 transition are energy degenerate. Here, by applying the Morris-Shore transformation, it is shown that this multi-state system is reduced to a set of independent two-state systems and dark states. In experiments performed by ultrafast laser interactions of atomic rubidium in the strong interaction regime, we demonstrate that the ultrafast dynamics of the considered multi-state system is governed by a sum of at most two decoupled Rabi oscillations when this system interacts with ultrafast laser pulses of any polarization state. We further show the implication of this result to possible controls of photo-electron polarizations.

  15. Resolution limits of ultrafast ultrasound localization microscopy

    Desailly, Yann; Pierre, Juliette; Couture, Olivier; Tanter, Mickael

    2015-11-01

    As in other imaging methods based on waves, the resolution of ultrasound imaging is limited by the wavelength. However, the diffraction-limit can be overcome by super-localizing single events from isolated sources. In recent years, we developed plane-wave ultrasound allowing frame rates up to 20 000 fps. Ultrafast processes such as rapid movement or disruption of ultrasound contrast agents (UCA) can thus be monitored, providing us with distinct punctual sources that could be localized beyond the diffraction limit. We previously showed experimentally that resolutions beyond λ/10 can be reached in ultrafast ultrasound localization microscopy (uULM) using a 128 transducer matrix in reception. Higher resolutions are theoretically achievable and the aim of this study is to predict the maximum resolution in uULM with respect to acquisition parameters (frequency, transducer geometry, sampling electronics). The accuracy of uULM is the error on the localization of a bubble, considered a point-source in a homogeneous medium. The proposed model consists in two steps: determining the timing accuracy of the microbubble echo in radiofrequency data, then transferring this time accuracy into spatial accuracy. The simplified model predicts a maximum resolution of 40 μm for a 1.75 MHz transducer matrix composed of two rows of 64 elements. Experimental confirmation of the model was performed by flowing microbubbles within a 60 μm microfluidic channel and localizing their blinking under ultrafast imaging (500 Hz frame rate). The experimental resolution, determined as the standard deviation in the positioning of the microbubbles, was predicted within 6 μm (13%) of the theoretical values and followed the analytical relationship with respect to the number of elements and depth. Understanding the underlying physical principles determining the resolution of superlocalization will allow the optimization of the imaging setup for each organ. Ultimately, accuracies better than the size

  16. ICT4D 2016: New Priorities for ICT4D Policy, Practice and WSIS in a Post-2015 World

    Heeks, R.

    2014-01-01

    In 2016, the Millennium Development Goals will be replaced by the post-2015 development agenda (PTDA). The foundational content is in place for this new agenda, which will be the single most-important force shaping the future of international development and, hence, the single most-important force shaping the future of information-and-communication-technology-for-development (ICT4D). In planning prospective ICT4D priorities, we should therefore pay close attention to the PTDA.This paper und...

  17. Semaphorin 4D Promotes Skeletal Metastasis in Breast Cancer

    Yang, Ying-Hua; Buhamrah, Asma; Schneider, Abraham; Lin, Yi-Ling; Zhou, Hua; Bugshan, Amr; Basile, John R.

    2016-01-01

    Bone density is controlled by interactions between osteoclasts, which resorb bone, and osteoblasts, which deposit it. The semaphorins and their receptors, the plexins, originally shown to function in the immune system and to provide chemotactic cues for axon guidance, are now known to play a role in this process as well. Emerging data have identified Semaphorin 4D (Sema4D) as a product of osteoclasts acting through its receptor Plexin-B1 on osteoblasts to inhibit their function, tipping the balance of bone homeostasis in favor of resorption. Breast cancers and other epithelial malignancies overexpress Sema4D, so we theorized that tumor cells could be exploiting this pathway to establish lytic skeletal metastases. Here, we use measurements of osteoblast and osteoclast differentiation and function in vitro and a mouse model of skeletal metastasis to demonstrate that both soluble Sema4D and protein produced by the breast cancer cell line MDA-MB-231 inhibits differentiation of MC3T3 cells, an osteoblast cell line, and their ability to form mineralized tissues, while Sema4D-mediated induction of IL-8 and LIX/CXCL5, the murine homologue of IL-8, increases osteoclast numbers and activity. We also observe a decrease in the number of bone metastases in mice injected with MDA-MB-231 cells when Sema4D is silenced by RNA interference. These results are significant because treatments directed at suppression of skeletal metastases in bone-homing malignancies usually work by arresting bone remodeling, potentially leading to skeletal fragility, a significant problem in patient management. Targeting Sema4D in these cancers would not affect bone remodeling and therefore could elicit an improved therapeutic result without the debilitating side effects. PMID:26910109

  18. Intense Cherenkov-type terahertz electromagnetic radiation from ultrafast laser-plasma interaction

    Hu Qiang-Lin; Liu Shi-Bing; Li Wei

    2008-01-01

    A Cherenkov-type terahertz electromagnetic radiation is revealed, which results efficiently from the collective effects in the time-domain of ultrafast pulsed electron current produced by ultrafast intense laser-plasma interaction.The emitted pulse waveform and spectrum, and the dependence of laser pulse parameters on the structure of the radiation field are investigated numerically. The condition of THz radiation generation in this regime and Cherenkov geometry of the radiation field are studied analytically.

  19. Vibrational Conical Intersections: Implications for Ultrafast Vibrational Dynamics

    Dawadi, Mahesh; Prasad Thapaliya, Bishnu; Bhatta, Ram; Perry, David

    2015-03-01

    The presence of conical intersections (CIs) between electronic potential energy surfaces is known to play a key role in ultrafast electronic relaxation in diverse circumstances. Recent reports have documented the existence of vibrational CIs connecting vibrationally adiabatic surfaces. Just as electronic CIs are now appreciated to be ubiquitous, controlling the rates of many photochemical processes, the present work on methanol and methyl mercaptan suggests that vibrational CIs may also be widespread, possibly controlling the outcome of some high-energy processes where vibrationally excited species are present. Other examples of vibrational CIs include the vibrational Jahn-Teller effect in C3V organic molecules and transition metal complexes. While the present work addresses only the couplings within bound molecules, the concept of vibrational CIs providing pathways for ultrafast relaxation also applies to molecular collisions. This work is supported by DOE (DEFG02-90ER14151).

  20. Attosecond Light and Science at the Time-scale of the Electron-Coherent X-Rays from Tabletop Ultrafast Lasers

    Murnane, Margaret (University of Colorado, Boulder and NIST)

    2010-03-31

    Ever since the invention of the laser 50 years ago and its application in nonlinear optics, scientists have been striving to extend coherent laser beams into the x-ray region of the spectrum. Very recently however, the prospects for tabletop coherent sources at very short wavelengths, even in the hard x-ray region of the spectrum at wavelengths < 1nm, have brightened considerably. This advance is possible by taking nonlinear optics techniques to an extreme - physics that is the direct result of a new ability to manipulate electrons on the fastest, attosecond, time-scales of our natural world. Several applications have already been demonstrated, including making a movie of how electrons rearrange in a chemical bond changes shape as a molecule breaks apart, following how fast a magnetic material can flip orientation, understanding how fast heat flows in a nanocircuit, or building a microscope without lenses. Nature 460, 1088 (2009); Science 317, 775 (2007); Physical Review Letters 103, 257402 (2009); Nature Materials 9, 26 (2010); Nature 463, 214 (2010); Science 322, 1207 (2008).

  1. Ultrafast strain engineering in complex oxide heterostructures

    Popovich, Paul; Caviglia, Andrea; Hu, Wanzheng; Bromberger, Hubertus; Singla, Rashmi; Mitrano, Matteo; Hoffmann, Matthias C.; Kaiser, Stefan; Foerst, Michael [Max-Planck Research Group for Structural Dynamics - Center for Free Electron Laser Science, University of Hamburg (Germany); Scherwitzl, Raoul; Zubko, Pavlo; Gariglio, Sergio; Triscone, Jean-Marc [Departement de Physique de la Matiere Condensee, University of Geneva, 24 Quai Ernest-Ansermet, 1211 Geneve 4, Geneva (Switzerland); Cavalleri, Andrea [Max-Planck Research Group for Structural Dynamics - Center for Free Electron Laser Science, University of Hamburg (Germany); Department of Physics, Clarendon Laboratory, University of Oxford (United Kingdom)

    2012-07-01

    The mechanical coupling between the substrate and the thin film is expected to be effective on the ultrafast timescale, and could be exploited for the dynamic control of materials properties. Here, we demonstrate that a large-amplitude mid-infrared field, made resonant with a stretching mode of the substrate, can switch the electronic properties of a thin film across an interface. Exploiting dynamic strain propagation between different components of a heterostructure, insulating antiferromagnetic NdNiO{sub 3} is driven through a prompt, five-order-of-magnitude increase of the electrical conductivity, with resonant frequency and susceptibility that is controlled by choice of the substrate material. Vibrational phase control, extended here to a wide class of heterostructures and interfaces, may be conductive to new strategies for electronic phase control at THz repetition rates.

  2. Imaging molecules from within: Ultrafast angström-scale structure determination of molecules via photoelectron holography using free-electron lasers

    Krasniqi, F.; Najjari, B.; Strüder, L.; Rolles, D.; Voitkiv, A.; Ullrich, J.

    2010-03-01

    A scheme based on (i) upcoming brilliant x-ray free-electron laser (FEL) sources, (ii) innovative energy and angular-dispersive large-area electron imagers, and (iii) the well-known photoelectron holography is elaborated that provides time-dependent three-dimensional structure determination of small to medium-sized molecules with Ångström spatial and femtosecond time resolution. Inducing molecular dynamics, wave-packet motion, dissociation, passage through conical intersections, or isomerization by a pump pulse this motion is visualized by the x-ray FEL probe pulse launching keV photoelectrons within a few femtoseconds from specific and well-defined sites, deep core levels of individual atoms, inside the molecule. On their way out, the photoelectrons are diffracted generating a hologram on the detector that encodes the molecular structure at the instant of photoionization, thus providing “femtosecond snapshot images of the molecule from within.” Detailed calculations in various approximations of increasing sophistication are presented and three-dimensional retrieval of the spatial structure of the molecule with Ångström spatial resolution is demonstrated. Due to the large photoabsorption cross sections the method extends x-ray-diffraction-based time-dependent structure investigations envisioned at FEL’s to new classes of samples that are not accessible by any other method. Among them are dilute samples in the gas phase such as aligned, oriented, or conformer-selected molecules, ultracold ensembles and/or molecular or cluster objects containing mainly light atoms that do not scatter x rays efficiently.

  3. Ultrafast Electron Transfer in Complexes of Doxorubicin with Human Telomeric G-Quadruplexes and GC Duplexes Probed by Femtosecond Fluorescence Spectroscopy.

    Changenet-Barret, Pascale; Gustavsson, Thomas; Markovitsi, Dimitra; Manet, Ilse

    2016-05-01

    Doxorubicin (DOX) is a natural anthracycline widely used in chemotherapy; its combined application as a chemotherapeutic and photodynamic agent has been recently proposed. In this context, understanding the photoinduced properties of DOX complexes with nucleic acids is crucial. Herein, the study of photoinduced electron transfer in DOX-DNA complexes by femtosecond fluorescence spectroscopy is reported. The behaviour of complexes with two model DNA structures, a G-quadruplex (G4) formed by the human telomeric sequence (Tel21) and a d(GC) duplex, is compared. The DOX affinity for these two sequences is similar. Although both 1:1 and 2:1 stoichiometries have been reported for DOX-G4 complexes, only 1:1 complexes form with the duplex. The steady-state absorption indicates a strong binding interaction with the duplex due to drug intercalation between the GC base pairs. In contrast, the interaction of DOX with Tel21 is much weaker and arises from drug binding on the G4 external faces at two independent binding sites. As observed for DOX-d(GC) complexes, fluorescence of the drug in the first binding site of Tel21 exhibits decays within a few picoseconds following a biphasic pattern; this is attributed to the existence of two drug conformations. The fluorescence of the drug in the second binding site of Tel21 shows slower decays within 150 ps. These timescales are consistent with electron transfer from the guanines to the excited drug, as favoured by the lower oxidation potential of the stacked guanines of G4 with respect to those in the duplex. PMID:26790038

  4. 19th International Conference on Ultrafast Phenomena

    Cundiff, Steven; Vivie-Riedle, Regina; Kuwata-Gonokami, Makoto; DiMauro, Louis

    2015-01-01

    This book presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond, and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultrafast technology has a profound impact in a wide range of applications, amongst them biomedical imaging, chemical dynamics, frequency standards, material processing, and ultrahigh-speed communications. This book summarizes the results presented at the 19th International Conference on Ultrafast Phenomena and provides an up-to-date view of this important and rapidly advancing field.

  5. Cold atom quantum emulation of ultrafast processes

    Rajagopal, Shankari; Geiger, Zachary; Fujiwara, Kurt; Singh, Kevin; Senaratne, Ruwan; Weld, David

    2016-05-01

    Pulsed lasers are an invaluable probe of fast electron dynamics in condensed matter systems. However, despite tremendous progress, physical limitations on lasers and a lack of exact theoretical models still limit the exploration of ultrafast processes in solids. We discuss a possible complementary approach, in which lattice-trapped cold neutral atoms driven far from equilibrium are used as a quantum emulator of ultrafast physics at sub-cycle timescales. The cold atom context is in many ways a natural choice for such experiments: equilibration timescales are more than ten orders of magnitude slower than those in solids, and strong driving forces are easily produced and manipulated. Our experimental approach uses ultracold strontium in optical traps. Multiple stable isotopes and a long-lived metastable state provide control over interaction strengths, while a narrow-linewidth transition expands the typical cold-atom toolbox of readout techniques. We discuss initial efforts in quantum emulation of tunnel ionization and development of a platform for more complicated endeavors, including the study of multiple-pulse sequences and recollision processes. We acknowledge support from the NSF GRFP, the AFOSR, the ARO and DURIP program, the Alfred P. Sloan Foundation, and the University of California Office of the President.

  6. Electronic structure near the Fermi level in the ferromagnetic semiconductor GaMnAs studied by ultrafast time-resolved light-induced reflectivity measurements

    Ishii, Tomoaki; Kawazoe, Tadashi; Hashimoto, Yusuke; Terada, Hiroshi; Muneta, Iriya; Ohtsu, Motoichi; Tanaka, Masaaki; Ohya, Shinobu

    The determination of the Fermi level (EF) position is important to understand the origin of the ferromagnetism in ferromagnetic semiconductor GaMnAs. The recent transient reflectivity (TR) spectroscopy measurement, which is potentially sensitive to the absorption edges, indicated that the EF exists in the valence band. However, the pump fluence in this study is rather high, and the accumulation of photo-carriers can shift the absorption edges. Thus, the definition of both the band gap and EF is obscure. Here, we have performed TR spectroscopy measurements on GaMnAs films with the pump fluence carefully controlled to suppress the accumulation of photo-carriers. The energy resolution of the TR spectrum was improved to 0.5 meV. The data shows light-induced change in the reflectivity spectra which is attributed to the band-gap renormalization and band filling. We have reproduced the observed TR spectra using the Kramers-Kronig relation and found the Mn-induced electronic states near the EF in the band gap. This work was partially supported by Grants-in-Aids for Scientific Research including Specially Promoted Research and Project for Developing Innovation Systems of MEXT.

  7. Beyond ICT4D: new media research in Uganda

    Lovink, G.

    2011-01-01

    Beyond ICT4D: New Media Research in Uganda is a collection of ethnographic reports from diverse perspectives of those living at the other end of the African ICT pyramid. Crucially, these texts refocus on the so-called "ICT4D" debate away from the standard western lens, which depicts users in the developing world as passive receivers of Western technological development, towards Ugandans whose use and production of technologies entail innovations from the ground up. It is this ‘other’ everyday...

  8. 4-D XRD for strain in many grains using triangulation

    Bale, Hrishikesh A.; Hanan, Jay C.; Tamura, Nobumichi

    2006-01-01

    Determination of the strains in a polycrystalline material using 4-D XRD reveals sub-grain and grain-to-grain behavior as a function of stress. Here 4-D XRD involves an experimental procedure using polychromatic micro-beam X-radiation (micro-Laue) to characterize polycrystalline materials in spatial location as well as with increasing stress. The in-situ tensile loading experiment measured strain in a model aluminum-sapphire metal matrix composite using the Advanced Light Source, Beam-li...

  9. The 4-D approach to visual control of autonomous systems

    Dickmanns, Ernst D.

    1994-01-01

    Development of a 4-D approach to dynamic machine vision is described. Core elements of this method are spatio-temporal models oriented towards objects and laws of perspective projection in a foward mode. Integration of multi-sensory measurement data was achieved through spatio-temporal models as invariants for object recognition. Situation assessment and long term predictions were allowed through maintenance of a symbolic 4-D image of processes involving objects. Behavioral capabilities were easily realized by state feedback and feed-foward control.

  10. 4D Multimodality Imaging of Citrobacter rodentium Infections in Mice

    Collins, James William; Meganck, Jeffrey A.; Kuo, Chaincy; Francis, Kevin P.; Frankel, Gad

    2013-01-01

    This protocol outlines the steps required to longitudinally monitor a bioluminescent bacterial infection using composite 3D diffuse light imaging tomography with integrated μCT (DLIT-μCT) and the subsequent use of this data to generate a four dimensional (4D) movie of the infection cycle. To develop the 4D infection movies and to validate the DLIT-μCT imaging for bacterial infection studies using an IVIS Spectrum CT, we used infection with bioluminescent C. rodentium, which causes self-limiti...

  11. Ultrafast time-resolved electron diffraction on adsorbate systems on silicon surfaces. Vibrational excitation in monllayers and dynamics of phase transitions

    In the present work ultra fast time resolved electron diffraction (TR-RHEED) at various adsorbate systems on silicon (Si) substrates was performed. Using the Debye-Waller-effect, the vibrational amplitude of the excited adsorbate atoms can be directly observed in the experiments as a function of time. For a coverage of 4/3 monolayers Lead (Pb) on Si(1 1 1) forms a (√(3) x √(3))-reconstruction. The transient intensity evolution of the diffraction spots is recorded in a TR-RHEED-experiment. After excitation with a fs-laser pulse the intensity decreases due to the Debye-Waller-effect. The temporal behavior of the de-excitation process can be described with two exponential functions: a short time constant of 100 ps and a long one of 2800 ps. The two time constants can be assigned to two different phonon modes of the Pb-adsorbate. The huge difference between the two time constants and thus difference in the coupling to the substrate is explained by the bonding geometry in the structural model. To confirm this possible explanation, further TR-RHEED-experiments for the (√(7) x √(3))-reconstruction of Pb on Si(1 1 1) were performed. The (√(7) x √(3))-reconstruction with a coverage of 1.2 monolayers shows comparable structural elements. The transient intensity evolution can be described with the identical two time constants. In addition, first experiments on the β (√(3) x √(3))-phase of Pb/Si(1 1 1) are presented. This β (√(3) x √(3))-reconstruction, with a coverage of 1/3 monolayers of Pb, shows a phase transition to a (3 x 3)-reconstruction, which was observed in the experiments. Further investigated adsorbate systems are: (√(3) x √(3))Ag/Si(1 1 1), (√(3) x √(3))In/Si(1 1 1), (√(31) x √(31))In/Si(1 1 1), and (√(3) x √(3))Bi/Si(1 1 1). In the second part of the present work the structural dynamics of strongly driven surface phase transitions was analysed for the first time with TR-RHEED. As a first modell system, the Si(0 0 1) c(4 x 2

  12. Silicon-chip-based ultrafast optical oscilloscope.

    Foster, Mark A; Salem, Reza; Geraghty, David F; Turner-Foster, Amy C; Lipson, Michal; Gaeta, Alexander L

    2008-11-01

    With the realization of faster telecommunication data rates and an expanding interest in ultrafast chemical and physical phenomena, it has become important to develop techniques that enable simple measurements of optical waveforms with subpicosecond resolution. State-of-the-art oscilloscopes with high-speed photodetectors provide single-shot waveform measurement with 30-ps resolution. Although multiple-shot sampling techniques can achieve few-picosecond resolution, single-shot measurements are necessary to analyse events that are rapidly varying in time, asynchronous, or may occur only once. Further improvements in single-shot resolution are challenging, owing to microelectronic bandwidth limitations. To overcome these limitations, researchers have looked towards all-optical techniques because of the large processing bandwidths that photonics allow. This has generated an explosion of interest in the integration of photonics on standard electronics platforms, which has spawned the field of silicon photonics and promises to enable the next generation of computer processing units and advances in high-bandwidth communications. For the success of silicon photonics in these areas, on-chip optical signal-processing for optical performance monitoring will prove critical. Beyond next-generation communications, silicon-compatible ultrafast metrology would be of great utility to many fundamental research fields, as evident from the scientific impact that ultrafast measurement techniques continue to make. Here, using time-to-frequency conversion via the nonlinear process of four-wave mixing on a silicon chip, we demonstrate a waveform measurement technology within a silicon-photonic platform. We measure optical waveforms with 220-fs resolution over lengths greater than 100 ps, which represent the largest record-length-to-resolution ratio (>450) of any single-shot-capable picosecond waveform measurement technique. Our implementation allows for single-shot measurements and uses

  13. Nonlinear Transient Dynamics of Photoexcited Silicon Nanoantenna for Ultrafast All-Optical Signal Processing

    Baranov, Denis G; Milichko, Valentin A; Kudryashov, Sergey I; Krasnok, Alexander E; Belov, Pavel A

    2016-01-01

    Optically generated electron-hole plasma in high-index dielectric nanostructures was demonstrated as a means of tuning of their optical properties. However, until now an ultrafast operation regime of such plasma driven nanostructures has not been attained. Here, we perform pump-probe experiments with resonant silicon nanoparticles and report on dense optical plasma generation near the magnetic dipole resonance with ultrafast (about 2.5 ps) relaxation rate. Basing on experimental results, we develop an analytical model describing transient response of a nanocrystalline silicon nanoparticle to an intense laser pulse and show theoretically that plasma induced optical nonlinearity leads to ultrafast reconfiguration of the scattering power pattern. We demonstrate 100 fs switching to unidirectional scattering regime upon irradiation of the nanoparticle by an intense femtosecond pulse. Our work lays the foundation for developing ultracompact and ultrafast all-optical signal processing devices.

  14. Ultrafast Surface Plasmonic Switch in Non-Plasmonic Metals

    Bévillon, E; Recoules, V; Zhang, H; Li, C; Stoian, R

    2015-01-01

    We demonstrate that ultrafast carrier excitation can drastically affect electronic structures and induce brief surface plasmonic response in non-plasmonic metals, potentially creating a plasmonic switch. Using first-principles molecular dynamics and Kubo-Greenwood formalism for laser-excited tungsten we show that carrier heating mobilizes d electrons into collective inter and intraband transitions leading to a sign flip in the imaginary optical conductivity, activating plasmonic properties for the initial non-plasmonic phase. The drive for the optical evolution can be visualized as an increasingly damped quasi-resonance at visible frequencies for pumping carriers across a chemical potential located in a d-band pseudo-gap with energy-dependent degree of occupation. The subsequent evolution of optical indices for the excited material is confirmed by time-resolved ultrafast ellipsometry. The large optical tunability extends the existence spectral domain of surface plasmons in ranges typically claimed in laser se...

  15. Partial photoionization cross-sections of rare earths metals in the region of the 4d resonance

    The partial photoionization cross-sections of the 4d-, 5p-, 4f-shells and the valence band of Ce, Pr, Nd, Eu and Gd are measured in the region of the 4d → 4f excitation. The sum is compared with the corresponding absorption spectrum in order to estimate the importance of different decay channels of the excited 4d94fsup(N+1) configurations. For the heavy rare earth metals, which show a large 4f multiplet splitting, we demonstrate that the coupling of the 4f ionization to the 4d → 4f excitations strongly depends on the particular (4fsup(N-1)) sup(2S+1)Lsub(J) - multiplet lines. This effect is also discussed for the 5p multiplet lines in Eu which arise from the coupling of the 5p hole with the 4f electrons. (orig.)

  16. 4d-polytopes described by Coxeter diagrams and quaternions

    4D-polytopes and their dual polytopes can be described as the orbits of the rank-4 Coxeter-Weyl groups. Their symmetries follow from the quaternionic descriptions of the rank-4 Coxeter-Dynkin diagrams. There exists a one to one correspondence between the finite subgroups of quaternions and the rank-4 Coxeter-Weyl groups.

  17. ARL4D - Wikipedia, the free encyclopedia [Gene Wiki

    Full Text Available ARL4D - Wikipedia, the free encyclopediaARL4DFrom Wikipedia, the free encyclopediaJump to:naviga ... of disease to interested scientists.[13][14][15]Male an d female an imals underwent a standardized phenotyp ... had decreased bone mineral content, heart weight, lean ... body mass and CD8-positive, alpha-beta memory T ce ...

  18. Medicoscapes: on mobile ubiquity effects and ICT4D

    Michelsen, Anders Ib

    2012-01-01

    The Article presents theoretical comments on the theme of ‘media ubiquity’, as an introduction to the presentation of an information and communication technology ‘4’ development (ICT4D) project in the Republic of Somaliland: The Somaliland Telemedical System for Psychiatry. This project is based on...

  19. Rise and fall of the 4d10→4d94f resonance in the Xe isoelectronic sequence

    The extreme ultraviolet photoabsorption spectrum of a laser-produced lanthanum plasma has been recorded and found to contain a number of discrete features in the 130-eV region. These have been analyzed as 4d10→4d9nf,np transitions in La3+. We show that the 4f transition, which is expected to be the strongest, is not in evidence. The reason is that this resonance, after the collapse of the 4f wave function, has a large autoionization width. We conclude that the 4f orbital in Ba2+ is only partially collapsed, which settles a long-standing discussion of this point

  20. 4D flow mri post-processing strategies for neuropathologies

    Schrauben, Eric Mathew

    4D flow MRI allows for the measurement of a dynamic 3D velocity vector field. Blood flow velocities in large vascular territories can be qualitatively visualized with the added benefit of quantitative probing. Within cranial pathologies theorized to have vascular-based contributions or effects, 4D flow MRI provides a unique platform for comprehensive assessment of hemodynamic parameters. Targeted blood flow derived measurements, such as flow rate, pulsatility, retrograde flow, or wall shear stress may provide insight into the onset or characterization of more complex neuropathologies. Therefore, the thorough assessment of each parameter within the context of a given disease has important medical implications. Not surprisingly, the last decade has seen rapid growth in the use of 4D flow MRI. Data acquisition sequences are available to researchers on all major scanner platforms. However, the use has been limited mostly to small research trials. One major reason that has hindered the more widespread use and application in larger clinical trials is the complexity of the post-processing tasks and the lack of adequate tools for these tasks. Post-processing of 4D flow MRI must be semi-automated, fast, user-independent, robust, and reliably consistent for use in a clinical setting, within large patient studies, or across a multicenter trial. Development of proper post-processing methods coupled with systematic investigation in normal and patient populations pushes 4D flow MRI closer to clinical realization while elucidating potential underlying neuropathological origins. Within this framework, the work in this thesis assesses venous flow reproducibility and internal consistency in a healthy population. A preliminary analysis of venous flow parameters in healthy controls and multiple sclerosis patients is performed in a large study employing 4D flow MRI. These studies are performed in the context of the chronic cerebrospinal venous insufficiency hypothesis. Additionally, a

  1. Building tomorrow's nuclear power plants with 4+D VR technology

    There continues to be an increasing demand of electricity around the globe to fuel the industrial growth and to promote the human welfare. The economic activities have brought about richness in our material and cultural lives, in which process the electric power has been at the heart of the versatile energy sources. In order to timely and competitively respond to rapidly changing energy environment in the twenty-first century there is a growing need to build the advanced nuclear power plants in the unlimited workspace of virtual reality (VR) prior to commissioning. One can then realistically evaluate their construction time and cost per varying methods and options available from the leading-edge technology. In particular a great deal of efforts have yet to be made for time- and cost-dependent plant simulation and dynamically coupled database construction in the VR space. The operator training and personnel education may also benefit from the VR technology. The present work is being proposed in the three-dimensional space and time plus cost coordinates, i. e. four plus dimensional (4+D) coordinates. The 4+D VR application will enable the nuclear industry to narrow the technological gap from the other leading industries that have long since been employing the VR engineering. The 4+D technology will help nurture public understanding of the special discipline of nuclear power plants. The technology will also facilitate public access to the knowledge on the nuclear science and engineering which has so far been monopolized by the academia, national laboratories and the heavy industry. The 4+D virtual design and construction will open up the new horizon for revitalization of the nuclear industry over the globe in the foreseeable future. Considering the long construction and operation time for the nuclear power plants, the preliminary VR simulation capability for the plants will supply the vital information not only for the actual design and construction of the engineered

  2. Ultrafast Spectroscopy of Semiconductor Devices

    Borri, Paola; Langbein, Wolfgang; Hvam, Jørn Marcher

    In this work we present an experimental technique for investigating ultrafast carrier dynamics in semiconductor optical amplifiers at room temperature. These dynamics, influenced by carrier heating, spectral hole-burning and two-photon absorption, are very important for device applications in inf...

  3. Ultrafast Spectroscopy of Semiconductor Devices

    Borri, Paola; Langbein, Wolfgang; Hvam, Jørn Marcher

    1999-01-01

    In this work we present an experimental technique for investigating ultrafast carrier dynamics in semiconductor optical amplifiers at room temperature. These dynamics, influenced by carrier heating, spectral hole-burning and two-photon absorption, are very important for device applications in...

  4. 4D MR imaging using robust internal respiratory signal

    Hui, CheukKai; Wen, Zhifei; Stemkens, Bjorn; Tijssen, R. H. N.; van den Berg, C. A. T.; Hwang, Ken-Pin; Beddar, Sam

    2016-05-01

    The purpose of this study is to investigate the feasibility of using internal respiratory (IR) surrogates to sort four-dimensional (4D) magnetic resonance (MR) images. The 4D MR images were constructed by acquiring fast 2D cine MR images sequentially, with each slice scanned for more than one breathing cycle. The 4D volume was then sorted retrospectively using the IR signal. In this study, we propose to use multiple low-frequency components in the Fourier space as well as the anterior body boundary as potential IR surrogates. From these potential IR surrogates, we used a clustering algorithm to identify those that best represented the respiratory pattern to derive the IR signal. A study with healthy volunteers was performed to assess the feasibility of the proposed IR signal. We compared this proposed IR signal with the respiratory signal obtained using respiratory bellows. Overall, 99% of the IR signals matched the bellows signals. The average difference between the end inspiration times in the IR signal and bellows signal was 0.18 s in this cohort of matching signals. For the acquired images corresponding to the other 1% of non-matching signal pairs, the respiratory motion shown in the images was coherent with the respiratory phases determined by the IR signal, but not the bellows signal. This suggested that the IR signal determined by the proposed method could potentially correct the faulty bellows signal. The sorted 4D images showed minimal mismatched artefacts and potential clinical applicability. The proposed IR signal therefore provides a feasible alternative to effectively sort MR images in 4D.

  5. Reflectivity enhancement in titanium by ultrafast XUV irradiation

    Bencivenga, F.; E. Principi; Giangrisostomi, E.; R. Cucini; Battistoni, A.; D'Amico, F.; Di Cicco, A; S. Di Fonzo; Filipponi, A.; Gessini, A.; R. Gunnella; Marsi, M.; L. Properzi; Saito, M; Masciovecchio, C.

    2014-01-01

    The study of highly photo-excited matter at solid state density is an emerging field of research, which is benefitting the development of free-electron-laser (FEL) technology. We report an extreme ultraviolet (XUV) reflectivity experiment from a titanium (Ti) sample irradiated with ultrafast seeded FEL pulses at variable incident photon fluence and frequency. Using a Drude formalism we relate the observed increase in reflectivity as a function of the excitation fluence to an increase in the p...

  6. Ultrafast charge localization in a stripe-phase nickelate

    Coslovich, Giacomo; Huber, Bernhard; Lee, Wei-Sheng; Sasagawa, Takao; Hussain, Zahid; Bechtel, Hans A.; Martin, Michael C.; Shen, Zhi-Xun; W. Schoenlein, Robert; A. Kaindl, Robert

    2013-08-30

    Self-organized electronically-ordered phases are a recurring feature in correlated materials, resulting in e.g. fluctuating charge stripes whose role in high-Tc superconductivity is under debate. However, the relevant cause-effect relations between real-space charge correlations and low-energy excitations remain hidden in time-averaged studies. Here, we reveal ultrafast charge localization and lattice vibrational coupling as dynamical precursors of stripe formation in the model compound La1.75Sr0.25NiO4, using ultrafast and equilibrium mid-infrared spectroscopy. The opening of a pseudogap at a crossover temperature T* far above long-range stripe formation establishes the onset of electronic localization which is accompanied by an enhanced Fano asymmetry of Ni-O stretch vibrations. Ultrafast excitation triggers a sub-picosecond dynamics exposing the synchronous modulation of electron-phonon coupling and charge localization. These results illuminate the role of localization in forming the pseudogap in nickelates, opening a path to understanding this mysterious phase in a broad class of complex oxides.

  7. Expression of Sema4D in patients with cerebral infarction and its clinical significance

    朱琳

    2012-01-01

    Objective To explore the expression and clinical significance of Semaphorin4D (Sema4D) mRNA in peripheral blood lymphocyte,Sema4D on platelet surface, soluble Sema4D (sSema4D) in plasma in patients with cerebral infarction. Methods Taking 299 patients with cerebral infarction

  8. An ultrafast silicon nanoplasmonic ballistic triode

    A nanoscale three terminal silicon based nanoplasmonic triode is proposed as a nanometer transistor. The device is suitable for monolithic integration with complementary-metal-oxide-semiconductor technology. Due to the highly spatially inhomogeneous, highly confined nanoplasmonic mode, electrons generated through two-photon absorption in the silicon are ponderomotively accelerated towards the copper anode producing an output current. Application of a negative grid voltage allows for control of the output current. The nanoplasmonic triode is able to achieve output current as high as 628 mA/μm on an ultrafast timescale of 150 fs in a compact footprint of 0.07 μm2. Reduction of the plasmonic field strength allows for a CMOS compatible current of 11.7 mA/μm. The results demonstrate the potential for the compact optical control of current useful for applications in high-speed, high current switching, and amplification

  9. Ultrafast dephasing of interband transitions in semiconductors

    2001-01-01

    Two basic types of dephasing mechanisms, carrier-carrier and carrier-phonon scattering including hole-hole and hole-phonon scattering are proposed in the theory of ultrafast polarization dephasing of continuum transitions in bulk semiconductors. The contribution of optical phonon scattering to the dephasing rate is the average of the scattering rates for electrons and holes. A weighting factor that reflects the change in the momentum of the particle in a collision is introduced into the usual integral of the carrier-carrier scattering rate to describe the contribution of carrier-carrier scattering to the dephasing rate for the case of static screening interaction. The theoretical calculations are in quantitative agreement with the reported experimental results.

  10. Impact of incorporating visual biofeedback in 4D MRI.

    To, David T; Kim, Joshua P; Price, Ryan G; Chetty, Indrin J; Glide-Hurst, Carri K

    2016-01-01

    Precise radiation therapy (RT) for abdominal lesions is complicated by respiratory motion and suboptimal soft tissue contrast in 4D CT. 4D MRI offers improved con-trast although long scan times and irregular breathing patterns can be limiting. To address this, visual biofeedback (VBF) was introduced into 4D MRI. Ten volunteers were consented to an IRB-approved protocol. Prospective respiratory-triggered, T2-weighted, coronal 4D MRIs were acquired on an open 1.0T MR-SIM. VBF was integrated using an MR-compatible interactive breath-hold control system. Subjects visually monitored their breathing patterns to stay within predetermined tolerances. 4D MRIs were acquired with and without VBF for 2- and 8-phase acquisitions. Normalized respiratory waveforms were evaluated for scan time, duty cycle (programmed/acquisition time), breathing period, and breathing regularity (end-inhale coefficient of variation, EI-COV). Three reviewers performed image quality assessment to compare artifacts with and without VBF. Respiration-induced liver motion was calculated via centroid difference analysis of end-exhale (EE) and EI liver contours. Incorporating VBF reduced 2-phase acquisition time (4.7 ± 1.0 and 5.4 ± 1.5 min with and without VBF, respectively) while reducing EI-COV by 43.8% ± 16.6%. For 8-phase acquisitions, VBF reduced acquisition time by 1.9 ± 1.6 min and EI-COVs by 38.8% ± 25.7% despite breathing rate remaining similar (11.1 ± 3.8 breaths/min with vs. 10.5 ± 2.9 without). Using VBF yielded higher duty cycles than unguided free breathing (34.4% ± 5.8% vs. 28.1% ± 6.6%, respectively). Image grading showed that out of 40 paired evaluations, 20 cases had equivalent and 17 had improved image quality scores with VBF, particularly for mid-exhale and EI. Increased liver excursion was observed with VBF, where superior-inferior, anterior-posterior, and left-right EE-EI displacements were 14.1± 5.8, 4.9 ± 2.1, and 1.5 ± 1.0 mm, respectively, with VBF compared to 11.9

  11. Ultrafast THz saturable absorption in doped semiconductors at room temperature

    Turchinovich, Dmitry; Hoffmann, M. V.

    2011-01-01

    Ultrafast Phenomena XVII presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond and attosecond processes relevant to applications in physics, chemistry, biology, and engineering....... Ultrafast technology has a profound impact in a wide range of applications, amongst them biomedical imaging, chemical dynamics, frequency standards, material processing, and ultrahigh speed communications. This book summarizes the results presented at the 17th International Conference on Ultrafast Phenomena...

  12. A brief review of the 2d/4d correspondences

    Tachikawa, Yuji

    2016-01-01

    An elementary introduction to the 2d/4d correspondences is given. After quickly reviewing the 2d q-deformed Yang-Mills theory and the Liouville theory, we will introduce 4d theories obtained by coupling trifundamentals to SU(2) gauge fields. We will then see concretely that the supersymmetric partition function of these theories on S^3 x S^1 and on S^4 is given respectively by the q-deformed Yang-Mills theory and the Liouville theory. After giving a short discussion on how this correspondence may be understood from the viewpoint of the 6d N=(2,0) theory, we conclude the review by enumerating future directions. Most of the technical points will be referred to more detailed review articles.

  13. Multireference Character for 4d Transition Metal-Containing Molecules.

    Wang, Jiaqi; Manivasagam, Sivabalan; Wilson, Angela K

    2015-12-01

    Four diagnostic criteria have been examined to identify the suitability of single-reference wave function-based quantum chemistry methods for a set of 118 4d transition metal species. These diagnostics include the weight of the leading configuration of the CASSCF wave function, C0(2); the Frobenius norm of the coupled cluster amplitude vector related to single excitations, T1; the matrix 2-norm of the coupled cluster T1 amplitude vector arising from coupled cluster calculations, D1; and the percent total atomization energy, %TAE, corresponding to a relationship between energies determined with CCSD and CCSD(T) calculations. New criteria, namely, T1 ≥ 0.045, D1 ≥ 0.120, and %TAE ≥ 10%, are herein proposed as a gauge for 4d transition metal-containing molecules to predict the possible need to employ multireference (MR) wave function-based methods to describe energetic and spectroscopic properties. PMID:26642991

  14. Construction Management Utilizing 4D CAD and Operations Simulation Methodologies

    ZHANG Jianping; ZHANG Yang; HU Zhenzhong; LU Ming

    2008-01-01

    The paper presents applications of simplified discrete-event simulation (SDESA), and 4D-GCPSU,to the National Stadium of the Beijing 2008 Olympics. Taking into account influential factors, e.g., resource, spatial condition, and the randomness of the construction process, the installation process of the steel- structure was simulated and optimized by using genetic algorithm (GA) optimization methodology. The op- erations simulation shortened the installation duration by 39 days (about 16% of the original total duration),guided the manufacturers to plan the construction processes, and provided specific suggestions on the en-try time of the installation components, resulting in resource allocation optimization, resource saving, and construction efficiency improvement. Combining with the optimized schedule, the 4D visualization environ- ment can discover time-space conflicts timely, and may assist project managers to reschedule the construc-tion activities in tune with the site layout and resource allocation.

  15. 4D, Script N = 1 supersymmetry genomics (I)

    Gates, S. James, Jr.; Gonzales, James; MacGregor, Boanne; Parker, James; Polo-Sherk, Ruben; Rodgers, Vincent G. J.; Wassink, Luke

    2009-12-01

    Presented in this paper the nature of the supersymmetrical representation theory behind 4D, Script N = 1 theories, as described by component fields, is investigated using the tools of Adinkras and Garden Algebras. A survey of familiar matter multiplets using these techniques reveals they are described by two fundamental valise Adinkras that are given the names of the cis-Valise (c-V) and the trans-Valise (t-V). A conjecture is made that all off-shell 4D, Script N = 1 component descriptions of supermultiplets are associated with two integers (nc, nt) — the numbers of c-V and t-V Adinkras that occur in the representation.

  16. ROER4D Sub-project 1 - Malaysia OER review

    Dhanarajan, Gajaraj; Arinto, Patricia

    2014-01-01

    The ROER4D project endeavours to cover at least three regions in the Global South, namely, South America, Sub-Saharan Africa, and South and South East Asia. However, background information on OER projects, policies and research and information on infrastructural, legal, socio-cultural and/or economic factors that might influence the adoption of OER in post-secondary education in these regions is incomplete despite the work of current projects. The project will provide background information o...

  17. 4d photoabsorption in Te V and Te VI

    The 4d photoabsorption spectra of Cd I-like Te V and the Ag I-like Te VI have been recorded in the 70-102 eV region using the dual-laser plasma technique. Discrete structure due to 4d→6p,nf (4≤n≤8) transitions have been observed in both ion stages. These have been identified with the aid of Hartree-Fock calculations. (author). Letter-to-the-editor

  18. Phosphodiesterase 4D gene polymorphisms in sudden sensorineural hearing loss.

    Chien, Chen-Yu; Tai, Shu-Yu; Wang, Ling-Feng; Hsi, Edward; Chang, Ning-Chia; Wang, Hsun-Mo; Wu, Ming-Tsang; Ho, Kuen-Yao

    2016-09-01

    The phosphodiesterase 4D (PDE4D) gene has been reported as a risk gene for ischemic stroke. The vascular factors are between the hypothesized etiologies of sudden sensorineural hearing loss (SSNHL), and this genetic effect might be attributed for its role in SSNHL. We hypothesized that genetic variants of the PDE4D gene are associated with susceptibility to SSNHL. We conducted a case-control study with 362 SSNHL cases and 209 controls. Three single nucleotide polymorphisms (SNPs) were selected. The genotypes were determined using TaqMan technology. Hardy-Weinberg equilibrium (HWE) was tested for each SNP, and genetic effects were evaluated according to three inheritance modes. We carried out sex-specific analysis to analyze the overall data. All three SNPs were in HWE. When subjects were stratified by sex, the genetic effect was only evident in females but not in males. The TT genotype of rs702553 exhibited an adjusted odds ratio (OR) of 3.83 (95 % confidence interval = 1.46-11.18) (p = 0.006) in female SSNHL. The TT genotype of SNP rs702553 was associated with female SSNHL under the recessive model (p = 0.004, OR 3.70). In multivariate logistic regression analysis, TT genotype of rs702553 was significantly associated with female SSNHL (p = 0.0043, OR 3.70). These results suggest that PDE4D gene polymorphisms influence the susceptibility for the development of SSNHL in the southern Taiwanese female population. PMID:26521189

  19. APPLICAZIONI 3D/4D GLOBALI: OLTRE TUTTE LE BARRIERE

    Deiana, Andrea

    2011-01-01

    Le soluzioni SkylineGlobe by Skyline Software Systems, Inc. si propongono come un ambiente utile all’integrazione di dati e sistemi provenienti da diverse piattaforme di ambito territoriale per l’acquisizione, la creazione, l’annotazione, la pubblicazione, l’erogazione, la visualizzazione, l’interrogazione e l’analisi di geodatasets in un ambiente 3D/4D di facile utilizzo, distribuzione e condivisione.

  20. ROER4D Sub-project 1 - India OER review

    Dhanarajan, Gajaraj; Arinto, Patricia

    2014-01-01

    The ROER4D project endeavours to cover at least three regions in the Global South, namely, South America, Sub-Saharan Africa, and South and South East Asia. However, background information on OER projects, policies and research and information on infrastructural, legal, socio-cultural and/or economic factors that might influence the adoption of OER in post-secondary education in these regions is incomplete despite the work of current projects. The project will provide background information o...

  1. Multivariable analysis of 2,4-d herbicide photocatalytic degradation

    LÓPEZ-VÁSQUEZ, ANDRÉS F.; JOSÉ A. COLINA-MÁRQUEZ; Machuca-Martínez, Fiderman

    2011-01-01

    The 2,4-D herbicide degradation of TiO2 suspensions in tap water was evaluated under artificial irradiation conditions. The response surface methodology (RSM) was applied to evaluate the effect of variables such as: catalyst concentration, herbicide concentration, pH, and the volumetric flow on the photocatalytic reaction in two kinds of photoreactors: flat plate and tubular reactor. The response variable was the pesticide mineralization expressed as the total organic carbon (TOC) removal per...

  2. Immersive 4D Interactive Visualization of Large-Scale Simulations

    Teuben, Peter; Hut, Piet; Levy, Stuart; Makino, Jun; McMillan, Steve; Zwart, Simon Portegies; Shara, Mike; Emmart, Carter

    2001-01-01

    In dense clusters a bewildering variety of interactions between stars can be observed, ranging from simple encounters to collisions and other mass-transfer encounters. With faster and special-purpose computers like GRAPE, the amount of data per simulation is now exceeding 1TB. Visualization of such data has now become a complex 4D data-mining problem, combining space and time, and finding interesting events in these large datasets. We have recently starting using the virtual reality simulator...

  3. Can Pions ``Smell'' 4D, N = 1 Supersymmetry?

    Gates, Jr., S. James

    1997-01-01

    We show how the usual chiral perturbation theory description of phenomenological pion physics admits an interpretation as a low-energy string-like model associated with QCD. By naive and straightforward generalization within the context of a new class of supersymmetrical models, it is shown that this string-like structure admits a 4D, N = 1 supersymmetrical extension. The presence of a WZNW term in the model implies modifications of certain higher order processes involving the ordinary SU(3) ...

  4. Autoadaptive phase-correlated (AAPC) reconstruction for 4D CBCT

    Bergner, Frank; Berkus, Timo; Oelhafen, Markus; Kunz, Patrik; Pan, Tinsu; Kachelrieß, Marc

    2009-01-01

    Purpose: Kilovoltage cone-beam computed tomography (CBCT) is widely used in image-guided radiation therapy for exact patient positioning prior to the treatment. However, producing time series of volumetric images (4D CBCT) of moving anatomical structures remains challenging. The presented work introduces a novel method, combining high temporal resolution inside anatomical regions with strong motion and image quality improvement in regions with little motion.

  5. Limits to Electron Beam Emittance from Stochastic Coulomb Interactions

    Dense electron beams can now be generated on an ultrafast timescale using laser driven photo-cathodes and these are used for a range of applications from ultrafast electron defraction to free electron lasers. Here we determine a lower bound to the emittance of an electron beam limited by fundamental stochastic Coulomb interactions.

  6. Limits to Electron Beam Emittance from Stochastic Coulomb Interactions

    Coleman-Smith, Christopher; Padmore, Howard A.; Wan, Weishi

    2008-08-22

    Dense electron beams can now be generated on an ultrafast timescale using laser driven photo-cathodes and these are used for a range of applications from ultrafast electron defraction to free electron lasers. Here we determine a lower bound to the emittance of an electron beam limited by fundamental stochastic Coulomb interactions.

  7. 4D remote sensing image coding with JPEG2000

    Muñoz-Gómez, Juan; Bartrina-Rapesta, Joan; Blanes, Ian; Jiménez-Rodríguez, Leandro; Aulí-Llinàs, Francesc; Serra-Sagristà, Joan

    2010-08-01

    Multicomponent data have become popular in several scientific fields such as forest monitoring, environmental studies, or sea water temperature detection. Nowadays, this multicomponent data can be collected more than one time per year for the same region. This generates different instances in time of multicomponent data, also called 4D-Data (1D Temporal + 1D Spectral + 2D Spatial). For multicomponent data, it is important to take into account inter-band redundancy to produce a more compact representation of the image by packing the energy into fewer number of bands, thus enabling a higher compression performance. The principal decorrelators used to compact the inter-band correlation redundancy are the Karhunen Loeve Transform (KLT) and Discrete Wavelet Transform (DWT). Because of the Temporal Dimension added, the inter-band redundancy among different multicomponent images is increased. In this paper we analyze the influence of the Temporal Dimension (TD) and the Spectral Dimension (SD) in 4D-Data in terms of coding performance for JPEG2000, because it has support to apply different decorrelation stages and transforms to the components through the different dimensions. We evaluate the influence to perform different decorrelators techniques to the different dimensions. Also we will assess the performance of the two main decorrelation techniques, KLT and DWT. Experimental results are provided, showing rate-distortion performances encoding 4D-Data using KLT and WT techniques to the different dimensions TD and SD.

  8. 4D-Flow validation, numerical and experimental framework

    Sansom, Kurt; Liu, Haining; Canton, Gador; Aliseda, Alberto; Yuan, Chun

    2015-11-01

    This work presents a group of assessment metrics of new 4D MRI flow sequences, an imaging modality that allows for visualization of three-dimensional pulsatile flow in the cardiovascular anatomy through time-resolved three-dimensional blood velocity measurements from cardiac-cycle synchronized MRI acquisition. This is a promising tool for clinical assessment but lacks a robust validation framework. First, 4D-MRI flow in a subject's stenotic carotid bifurcation is compared with a patient-specific CFD model using two different boundary condition methods. Second, Particle Image Velocimetry in a patient-specific phantom is used as a benchmark to compare the 4D-MRI in vivo measurements and CFD simulations under the same conditions. Comparison of estimated and measureable flow parameters such as wall shear stress, fluctuating velocity rms, Lagrangian particle residence time, will be discussed, with justification for their biomechanics relevance and the insights they can provide on the pathophysiology of arterial disease: atherosclerosis and intimal hyperplasia. Lastly, the framework is applied to a new sequence to provide a quantitative assessment. A parametric analysis on the carotid bifurcation pulsatile flow conditions will be presented and an accuracy assessment provided.

  9. High-temperature asymptotics of the 4d superconformal index

    Ardehali, Arash Arabi

    2016-01-01

    The superconformal index of a typical Lagrangian 4d SCFT is given by a special function known as an elliptic hypergeometric integral (EHI). The high-temperature limit of the index corresponds to the hyperbolic limit of the EHI. The hyperbolic limit of certain special EHIs has been analyzed by Eric Rains around 2006; extending Rains's techniques, we discover a surprisingly rich structure in the high-temperature limit of a (rather large) class of EHIs that arise as the superconformal index of unitary Lagrangian 4d SCFTs with non-chiral matter content. Our result has implications for $\\mathcal{N}=1$ dualities, the AdS/CFT correspondence, and supersymmetric gauge dynamics on $R^3\\times S^1$. We also investigate the high-temperature asymptotics of the large-N limit of the superconformal index of a class of holographic 4d SCFTs (described by toric quiver gauge theories with SU(N) nodes). We show that from this study a rather general solution to the problem of holographic Weyl anomaly in AdS$_5$/CFT$_4$ at the suble...

  10. Analytical methods for 2,4-D (Dichlorophenoxyacetic acid) determination

    The 2,4-D herbicide is one of the main pesticides for controlling the bad grass in crops such as the water undergrowth. In Mexico the allowed bound of this pesticide is 0.05 mg/l in water of 2,4-D so it is required to have methods trusts and exacts, which can used in order to detected low concentration of it. In this work we show some for the conventional techniques and for establishing the 2,4-D concentrations. The UV-Vis spectrometer and liquids chromatography due that they are the most common used nowadays. Beside, we introduce a now developed technique, which is based on the neutronic activation analysis. Though use of the UV-Vis spectrometer technique it was possible target the concentrations interval between 1 and 200 mg/l. In the liquids chromatography interval was between 0.1 and 0.9, and by the neutronic activation analysis the interval was between 0.01 and 200 mg/l. (Author)

  11. Ultrafast thermal dynamics of nano-ripples formation via laser double pulses excitation

    Du, Guangqing; Wu, Yanmin; Uddin, Noor; Yang, Qing; Chen, Feng; Lu, Yu; Bian, Hao; Hou, Xun

    2016-09-01

    The ultrafast thermal dynamics of nano-ripples formation on gold film via ultrafast laser double pulses excitation is theoretically investigated by numerical simulations. The non-equilibrium thermal modulations with respect to the electron and phonon energy transfers within gold film is proposed for predicting the nano-ripples formation. It is revealed that the nano-ripples contrast on gold film surface can be well controlled via tuning the pulse energy ratio, pulse separation and pulse exchange of ultrafast laser double-pulse. It is attributed to the tunable energy transfer routes between the electron thermal diffusion and the electron-phonon coupling via tuning double pulses parameters. The study provides theoretical basis for producing high-contrast ripples for a wide range application in the fields such as high-absorptive solar cells, surface friction devices and super-hydrophobic surface.

  12. 2,4-D impact on bacterial communities, and the activity and genetic potential of 2,4-D degrading communities in soil.

    Gonod, Laure Vieublé; Martin-Laurent, Fabrice; Chenu, Claire

    2006-12-01

    The key role of telluric microorganisms in pesticide degradation is well recognized but the possible relationships between the biodiversity of soil microbial communities and their functions still remain poorly documented. If microorganisms influence the fate of pesticides, pesticide application may reciprocally affect soil microorganisms. The objective of our work was to estimate the impact of 2,4-D application on the genetic structure of bacterial communities and the 2,4-D-degrading genetic potential in relation to 2,4-D mineralization. Experiments combined isotope measurements with molecular analyses. The impact of 2,4-D on soil bacterial populations was followed with ribosomal intergenic spacer analysis. The 2,4-D degrading genetic potential was estimated by real-time PCR targeted on tfdA sequences coding an enzyme specifically involved in 2,4-D mineralization. The genetic structure of bacterial communities was significantly modified in response to 2,4-D application, but only during the intense phase of 2,4-D biodegradation. This effect disappeared 7 days after the treatment. The 2,4-D degrading genetic potential increased rapidly following 2,4-D application. There was a concomitant increase between the tfdA copy number and the 14C microbial biomass. The maximum of tfdA sequences corresponded to the maximum rate of 2,4-D mineralization. In this soil, 2,4-D degrading microbial communities seem preferentially to use the tfd pathway to degrade 2,4-D. PMID:17117994

  13. A spectroelectrochemical cell for ultrafast two-dimensional infrared spectroscopy

    A spectroelectrochemical cell has been designed to combine electrochemistry and ultrafast two-dimensional infrared (2D-IR) spectroscopy, which is a powerful tool to extract structure and dynamics information on the femtosecond to picosecond time scale. Our design is based on a gold mirror with the dual role of performing electrochemistry and reflecting IR light. To provide the high optical surface quality required for laser spectroscopy, the gold surface is made by electron beam evaporation on a glass substrate. Electrochemical cycling facilitates in situ collection of ultrafast dynamics of redox-active molecules by means of 2D-IR. The IR beams are operated in reflection mode so that they travel twice through the sample, i.e., the signal size is doubled. This methodology is optimal for small sample volumes and successfully tested with the ferricyanide/ferrocyanide redox system of which the corresponding electrochemically induced 2D-IR difference spectrum is reported

  14. Ultrafast spectroscopy of quasiparticle dynamics in cuprate superconductors

    Ultrafast pump-probe spectroscopy is a powerful tool to study the nonequilibrium dynamics in high-Tc cuprate superconductors. The photo-induced quasiparticle (QP) dynamics revealed by pump-probe spectroscopy are sensitive to the near-Fermi level electronic structures. Here we review several selected examples to illustrate the enduring challenges including pairing glue, phase separation, and phase transitions in cuprate superconductors. We also present the data obtained on thin films of YBa2Cu3O7−δ in connection to these issues. - Highlights: • This paper reviews recent ultrafast spectroscopic study on cuprates. • Dynamics related to pairing glues and phase separations are summarized. • Mid-IR pulses enhance the coherent transport in underdoped cuprates. • Pump-probe data on the quasiparticle dynamics in YBCO films are presented

  15. Ultrafast photonic crystal optical switching

    GONG Qi-huang; HU Xiao-yong

    2006-01-01

    Photonic crystal,a novel and artificial photonic material with periodic dielectric distribution,possesses photonic bandgap and can control the propagation states of photons.Photonic crystal has been considered to be a promising candidate for the future integrated photonic devices.The properties and the fabrication method of photonic crystal are expounded.The progresses of the study of ultrafast photonic crystal optical switching are discussed in detail.

  16. ULTRASSONOGRAFIA GESTACIONAL 3D/4D EM PEQUENOS ANIMAIS

    Guilherme Fazan Rossi

    2015-06-01

    Full Text Available Esta revisión tiene como objetivo describir el uso actual de la ecografía tridimensional (3D/4D en obstetricia veterinários del pequeños animales. La ecografía tridimensional surgió en la década de 1950 y comenzó a tener una aplicación más amplia en las áreas de obstetricia y ginecología a principios de 1980. Esta técnica facilita 3D estudio volumétrico de ultrasonidos de órganos y las estructuras y permitir tercera plano de la imagen (plano coronal permite el cálculo volumétrico con mayor precisión, especialmente aquellos cuerpos de forma irregular. El método 4D se utiliza para evaluar las estructuras y funciones a través de la imagen de correlación espacio-temporal. Aun siendo una técnica disponible para más de 30 años en la medicina humana, en los estudios de veterinaria son necesarios para demostrar reciente y la especificidad y la sensibilidad de la técnica en la rutina de ultrasonido obstétrico de animales pequeños. A presente revisão tem por objetivo descrever as atuais utilizações da ultrassonografia tridimensional (US 3D/4D em obstetrícia veterinária de pequenos animais. A ultrassonografia tridimensional surgiu na década de 1950 e começou a ter maior aplicabilidade nas áreas de obstetrícia e ginecologia no início dos anos 1980. Essa técnica ultrassonográfica 3D facilita o estudo volumétrico de órgãos e estruturas e por permitir um terceiro plano da imagem (plano coronal possibilita o cálculo volumétrico mais precisamente, principalmente aqueles órgãos com formato irregular. A modalidade 4D é utilizada na avaliação de estruturas e funções via correlação imagem espaçotemporal. Mesmo sendo uma técnica disponível há mais de 30 anos em medicina humana, na veterinária os estudos são recentes e necessários para demonstrar a especificidade e sensibilidade da técnica ultrassonográfica na rotina da obstetrícia de pequenos animais. This review aims to describe the current use of three

  17. 4D Proton treatment planning strategy for mobile lung tumors

    Purpose: To investigate strategies for designing compensator-based 3D proton treatment plans for mobile lung tumors using four-dimensional computed tomography (4DCT) images. Methods and Materials: Four-dimensional CT sets for 10 lung cancer patients were used in this study. The internal gross tumor volume (IGTV) was obtained by combining the tumor volumes at different phases of the respiratory cycle. For each patient, we evaluated four planning strategies based on the following dose calculations: (1) the average (AVE) CT; (2) the free-breathing (FB) CT; (3) the maximum intensity projection (MIP) CT; and (4) the AVE CT in which the CT voxel values inside the IGTV were replaced by a constant density (AVERIGTV). For each strategy, the resulting cumulative dose distribution in a respiratory cycle was determined using a deformable image registration method. Results: There were dosimetric differences between the apparent dose distribution, calculated on a single CT dataset, and the motion-corrected 4D dose distribution, calculated by combining dose distributions delivered to each phase of the 4DCT. The AVERIGTV plan using a 1-cm smearing parameter had the best overall target coverage and critical structure sparing. The MIP plan approach resulted in an unnecessarily large treatment volume. The AVE and FB plans using 1-cm smearing did not provide adequate 4D target coverage in all patients. By using a larger smearing value, adequate 4D target coverage could be achieved; however, critical organ doses were increased. Conclusion: The AVERIGTV approach is an effective strategy for designing proton treatment plans for mobile lung tumors

  18. 4D seismic data acquisition method during coal mining

    In order to observe overburden media changes caused by mining processing, we take the fully-mechanized working face of the BLT coal mine in Shendong mine district as an example to develop a 4D seismic data acquisition methodology during coal mining. The 4D seismic data acquisition is implemented to collect 3D seismic data four times in different periods, such as before mining, during the mining process and after mining to observe the changes of the overburden layer during coal mining. The seismic data in the research area demonstrates that seismic waves are stronger in energy, higher in frequency and have better continuous reflectors before coal mining. However, all this is reversed after coal mining because the overburden layer has been mined, the seismic energy and frequency decrease, and reflections have more discontinuities. Comparing the records collected in the survey with those from newly mined areas and other records acquired in the same survey with the same geometry and with a long time for settling after mining, it clearly shows that the seismic reflections have stronger amplitudes and are more continuous because the media have recovered by overburden layer compaction after a long time of settling after mining. By 4D seismic acquisition, the original background investigation of the coal layers can be derived from the first records, then the layer structure changes can be monitored through the records of mining action and compaction action after mining. This method has laid the foundation for further research into the variation principles of the overburden layer under modern coal-mining conditions. (paper)

  19. Non-spherical particle generation from 4D optofluidic fabrication.

    Paulsen, Kevin S; Chung, Aram J

    2016-08-01

    Particles with non-spherical shapes can exhibit properties which are not available from spherical shaped particles. Complex shaped particles can provide unique benefits for areas such as drug delivery, tissue engineering, structural materials, and self-assembly building blocks. Current methods of creating complex shaped particles such as 3D printing, photolithography, and imprint lithography are limited by either slow speeds, shape limitations, or expensive processes. Previously, we presented a novel microfluidic flow lithography fabrication scheme combined with fluid inertia called optofluidic fabrication for the creation of complex shaped three-dimensional (3D) particles. This process was able to address the aforementioned limits and overcome two-dimensional shape limitations faced by traditional flow lithography methods; however, all of the created 3D particle shapes displayed top-down symmetry. Here, by introducing the time dimension into our existing optofluidic fabrication process, we break this top-down symmetry, generating fully asymmetric 3D particles where we termed the process: four-dimensional (4D) optofluidic fabrication. This 4D optofluidic fabrication is comprised of three sequential procedures. First, density mismatched precursor fluids flow past pillars within fluidic channels to manipulate the flow cross sections via fluid inertia. Next, the time dimension is incorporated by stopping the flow and allowing the denser fluids to settle by gravity to create asymmetric flow cross sections. Finally, the fluids are exposed to patterned ultraviolet (UV) light in order to polymerize fully asymmetric 3D-shaped particles. By varying inertial flow shaping, gravity-induced flow shaping, and UV light patterns, 4D optofluidic fabrication can create an infinite set of complex shaped asymmetric particles. PMID:27092661

  20. 4D micro-CT using fast prospective gating

    Guo, Xiaolian; Johnston, Samuel M.; Qi, Yi; Johnson, G. Allan; Badea, Cristian T.

    2012-01-01

    Micro-CT is currently used in preclinical studies to provide anatomical information. But, there is also significant interest in using this technology to obtain functional information. We report here a new sampling strategy for 4D micro-CT for functional cardiac and pulmonary imaging. Rapid scanning of free-breathing mice is achieved with fast prospective gating (FPG) implemented on a field programmable gate array. The method entails on-the-fly computation of delays from the R peaks of the ECG signals or the peaks of the respiratory signals for the triggering pulses. Projection images are acquired for all cardiac or respiratory phases at each angle before rotating to the next angle. FPG can deliver the faster scan time of retrospective gating (RG) with the regular angular distribution of conventional prospective gating for cardiac or respiratory gating. Simultaneous cardio-respiratory gating is also possible with FPG in a hybrid retrospective/prospective approach. We have performed phantom experiments to validate the new sampling protocol and compared the results from FPG and RG in cardiac imaging of a mouse. Additionally, we have evaluated the utility of incorporating respiratory information in 4D cardiac micro-CT studies with FPG. A dual-source micro-CT system was used for image acquisition with pulsed x-ray exposures (80 kVp, 100 mA, 10 ms). The cardiac micro-CT protocol involves the use of a liposomal blood pool contrast agent containing 123 mg I ml-1 delivered via a tail vein catheter in a dose of 0.01 ml g-1 body weight. The phantom experiment demonstrates that FPG can distinguish the successive phases of phantom motion with minimal motion blur, and the animal study demonstrates that respiratory FPG can distinguish inspiration and expiration. 4D cardiac micro-CT imaging with FPG provides image quality superior to RG at an isotropic voxel size of 88 µm and 10 ms temporal resolution. The acquisition time for either sampling approach is less than 5 min. The

  1. Exploring the Minimal 4D $\\mathcal{N}=1$ SCFT

    Poland, David

    2015-01-01

    We study the conformal bootstrap constraints for 4D $\\mathcal{N}=1$ superconformal field theories containing a chiral operator $\\phi$ and the chiral ring relation $\\phi^2=0$. Hints for a minimal interacting SCFT in this class have appeared in previous numerical bootstrap studies. We perform a detailed study of the properties of this conjectured theory, establishing that the corresponding solution to the bootstrap constraints contains a $\\text{U}(1)_R$ current multiplet and estimating the central charge and low-lying operator spectrum of this theory.

  2. MULTIVARIABLE ANALYSIS OF 2,4-D HERBICIDE PHOTOCATALYTIC DEGRADATION

    LÓPEZ-VÁSQUEZ, ANDRÉS F.; COLINA-MÁRQUEZ, JOSÉ A.; FIDERMAN MACHUCA-MARTÍNEZ

    2011-01-01

    La degradación del herbicida 2,4-D en suspensiones de TiO2 en agua real fue evaluada bajo condiciones de irradiación artificial. El análisis multivariable de metodología de superficie de respuesta (MSR), se aplicó para evaluar el efecto de variables como la concentración de catalizador y pesticida, el pH y el caudal volumétrico sobre la reacción fotocatalítica en dos fotorreactores catalíticos: placa plana y tubular. La variable de respuesta fue la mineralización del pesticida expresada como ...

  3. Beyond ICT4D: New Media in Uganda

    Lovink, G.W.

    2011-01-01

    This research project aims to pick up where Incommunicado left off, to look past conferences organized in the West, the debates sponsored by western organizations, and to instead look through the lens of the individual end users on the ground. This project aims to embed itself amongst the people living at the ‘bottom of the ICT pyramid’ and to look at the same discussion from their perspective. It is this ‘other’ point of view that is too often missing in the ICT4D debate, otherwise a valuabl...

  4. Magnetic Mass in 4D AdS Gravity

    Araneda, Rene; Miskovic, Olivera; Olea, Rodrigo

    2016-01-01

    We provide a fully-covariant expression for the diffeomorphic charge in 4D anti-de Sitter gravity, when the Gauss-Bonnet and Pontryagin terms are added to the action. The couplings of these topological invariants are such that the Weyl tensor and its dual appear in the on-shell variation of the action, and such that the action is stationary for asymptotic (anti) self-dual solutions in the Weyl tensor. In analogy with Euclidean electromagnetism, whenever the self-duality condition is global, both the action and the total charge are identically vanishing. Therefore, for such configurations the magnetic mass equals the Ashtekhar-Magnon-Das definition.

  5. Contextualised ICT4D: a Bottom-Up Approach

    Lund, Henrik Hautop; Sutinen, Erkki

    2010-01-01

    their own strengths to new levels by designing appropriate technologies with experts of technology and design. The bottomup approach requires a new kind of ICT education at the undergraduate level. An example of the development of a contextualized IT degree program at Tumaini University in Tanzania......The term ICT4D refers to the opportunities of Information and Communication Technology (ICT) as an agent of development. Much of the research in the field is based on evaluating the feasibility of existing technologies, mostly of Western or Asian origin, in the context of developing countries. In a...

  6. Multicolor 4D Fluorescence Microscopy using Ultrathin Bessel Light Sheets.

    Zhao, Teng; Lau, Sze Cheung; Wang, Ying; Su, Yumian; Wang, Hao; Cheng, Aifang; Herrup, Karl; Ip, Nancy Y; Du, Shengwang; Loy, M M T

    2016-01-01

    We demonstrate a simple and efficient method for producing ultrathin Bessel ('non-diffracting') light sheets of any color using a line-shaped beam and an annulus filter. With this robust and cost-effective technology, we obtained two-color, 3D images of biological samples with lateral/axial resolution of 250 nm/400 nm, and high-speed, 4D volume imaging of 20 μm sized live sample at 1 Hz temporal resolution. PMID:27189786

  7. Spin Dynamics during Ultrafast Optical Demagnetization

    Eisebitt, Stefan

    2015-03-01

    Magnetic order can be influenced on a sub-picosecund time scale via femtosecond optical pulses. In particular, demagnetization and switching can be triggered optically and while the applications e.g. for magnetic data storage are obvious, the underlying mechanisms are still under debate. We have investigated the contribution of electronic transport to optical demagnetization via pump-probe experiments at free-electron x-ray lasers. In ferromagnetic thin film multilayers with perpendicular anisotropy, optically excited electrons can move within a labyrinth domain network. Using x-ray magnetic circular dichroism (XMCD) as a contrast mechanism for small angle x-ray scattering to probe the local magnetization, we observe an ultrafast broadening of the domain walls, consistent with the existence of superdiffusive spin currents. Via pump-probe x-ray holographic imaging we obtain real space images of the local magnetization within the domain structure after pumping the system by a laterally confined excitation generated by an optical standing wave. With a temporal resolution of about 100 fs, we observe the propagation of a demagnetization front in real space, again consistent with the existence of superdiffusive spin currents. Support by BMBF in FSP-301 and 302 via Contracts 05K10KTB, 05K13KT3 and 05K13KT4 is gratefully acknowledged.

  8. Substrate dependent ultrafast dynamics in thin NiFe films

    Bosco, C. A. C.; Azevedo, A.; Acioli, L. H.

    2003-09-01

    We have studied the ultrafast electronic response of thin NiFe films by femtosecond transient reflectivity measurements. The experiments were performed on films with varying thicknesses, substrates, and pump fluences. It has been observed that for high excitation densities the electron cooling time depends strongly on the nature of the underlying substrate and we attribute our results to transport of hot carriers out of the excited region. In particular, we have observed that for NiFe over NiO, carrier transport should be less important than for NiFe over Si.

  9. Dielectronic recombination of the 4p and 4d open sub-shell tungsten ions

    Dielectronic recombination rate coefficients are given theoretically for several highly charged tungsten ions. As 4p open sub-shell ions, Ga-, Ge-, As-, Br-, Kr-like ions are considered. Rb-like ion is further considered as a 4d open sub-shell ion. Theoretical calculations are carried out using a relativistic atomic code FAC. The effect of configuration interaction is taking into account. Inner-shell electron excitations play a significant role for the dielectronic recombination process. Simple analytical formulae are given for the total rate coefficients by fitting to the presently obtained numerical results.

  10. Inhibitory concentrations of 2,4D and its possible intermediates in sulfate reducing biofilms

    Garcia-Cruz, Ulises [Department of Biotechnology, Environmental Science and Technology, Universidad Autonoma Metropolitana-Iztapalapa, Ave. San Rafael Atlixco 186, Vicentina, 09340 D.F. (Mexico); Celis, Lourdes B. [Division de Ciencias Ambientales, Instituto Potosino de Investigacion Cientifica y Tecnologica, Camino a la Presa San Jose 2055, Lomas 4a. Seccion, 78216 San Luis Potosi, S.L.P. (Mexico); Poggi, Hector [Department of Biotechnology and Bioengineering, CINVESTAV, Av. Instituto Politecnico Nacional 2508, Col. San Pedro Zacatenco, 07360 D.F. (Mexico); Meraz, Monica, E-mail: meraz@xanum.uam.mx [Department of Biotechnology, Environmental Science and Technology, Universidad Autonoma Metropolitana-Iztapalapa, Ave. San Rafael Atlixco 186, Vicentina, 09340 D.F. (Mexico)

    2010-07-15

    Different concentrations of the herbicide 2,4-dichlorophenoxyacetic acid (2,4D) and its possible intermediates such as 2,4-dichlorophenol (2,4DCP), 4-chlorophenol (4CP), 2-chlorophenol (2CP) and phenol, were assayed to evaluate the inhibitory effect on sulfate and ethanol utilization in a sulfate reducing biofilm. Increasing concentrations of the chlorophenolic compounds showed an adverse effect on sulfate reduction rate and ethanol conversion to acetate, being the intermediate 2,4DCP most toxic than the herbicide. The monochlorophenol 4CP (600 ppm) caused the complete cessation of sulfate reduction and ethanol conversion. The ratio of the electron acceptor to the electron donor utilized as well as the sulfate utilization volumetric rates, diminished when chlorophenols and phenol concentrations were increased, pointing out to the inhibition of the respiratory process and electrons transfer. The difference found in the IC{sub 50} values obtained was due to the chemical structure complexity of the phenolic compounds, the number of chlorine atoms as much as the chlorine atom position in the phenol ring. The IC{sub 50} values (ppm) indicated that the acute inhibition on the biofilm was caused by 2,4DCP (17.4) followed by 2,4D (29.0), 2CP (99.8), 4CP (108.0) and phenol (143.8).

  11. Inhibitory concentrations of 2,4D and its possible intermediates in sulfate reducing biofilms

    Different concentrations of the herbicide 2,4-dichlorophenoxyacetic acid (2,4D) and its possible intermediates such as 2,4-dichlorophenol (2,4DCP), 4-chlorophenol (4CP), 2-chlorophenol (2CP) and phenol, were assayed to evaluate the inhibitory effect on sulfate and ethanol utilization in a sulfate reducing biofilm. Increasing concentrations of the chlorophenolic compounds showed an adverse effect on sulfate reduction rate and ethanol conversion to acetate, being the intermediate 2,4DCP most toxic than the herbicide. The monochlorophenol 4CP (600 ppm) caused the complete cessation of sulfate reduction and ethanol conversion. The ratio of the electron acceptor to the electron donor utilized as well as the sulfate utilization volumetric rates, diminished when chlorophenols and phenol concentrations were increased, pointing out to the inhibition of the respiratory process and electrons transfer. The difference found in the IC50 values obtained was due to the chemical structure complexity of the phenolic compounds, the number of chlorine atoms as much as the chlorine atom position in the phenol ring. The IC50 values (ppm) indicated that the acute inhibition on the biofilm was caused by 2,4DCP (17.4) followed by 2,4D (29.0), 2CP (99.8), 4CP (108.0) and phenol (143.8).

  12. Untangling the contributions of image charge and laser profile for optimal photoemission of high-brightness electron beams

    Portman, J.; Zhang, H.; Makino, K.; Ruan, C. Y.; Berz, M.; Duxbury, P. M.

    2014-11-01

    Using our model for the simulation of photoemission of high brightness electron beams, we investigate the virtual cathode physics and the limits to spatio-temporal and spectroscopic resolution originating from the image charge on the surface and from the profile of the exciting laser pulse. By contrasting the effect of varying surface properties (leading to expanding or pinned image charge), laser profiles (Gaussian, uniform, and elliptical), and aspect ratios (pancake- and cigar-like) under different extraction field strengths and numbers of generated electrons, we quantify the effect of these experimental parameters on macroscopic pulse properties such as emittance, brightness (4D and 6D), coherence length, and energy spread. Based on our results, we outline optimal conditions of pulse generation for ultrafast electron microscope systems that take into account constraints on the number of generated electrons and on the required time resolution.

  13. Ultrafast Hierarchical OTDM/WDM Network

    Hideyuki Sotobayashi

    2003-12-01

    Full Text Available Ultrafast hierarchical OTDM/WDM network is proposed for the future core-network. We review its enabling technologies: C- and L-wavelength-band generation, OTDM-WDM mutual multiplexing format conversions, and ultrafast OTDM wavelengthband conversions.

  14. Avant-Garde Ultrafast Laser Writing

    Kazansky P. G.

    2013-11-01

    Full Text Available Ultrafast laser processing of transparent materials reveals new phenomena. Reviewed, are recent demonstrations of 5D optical memory, vortex polarization and Airy beam converters employing self-assembled nanostructuring, ultrafast laser calligraphy and polarization writing control using pulses with tilted front.

  15. Avant-Garde Ultrafast Laser Writing

    Kazansky P. G.; Beresna M.; Gecevičius M.

    2013-01-01

    Ultrafast laser processing of transparent materials reveals new phenomena. Reviewed, are recent demonstrations of 5D optical memory, vortex polarization and Airy beam converters employing self-assembled nanostructuring, ultrafast laser calligraphy and polarization writing control using pulses with tilted front.

  16. Nonlinear Optical Properties and Ultrafast Dynamics of Undoped and Doped Bulk SiC

    DING Jin-Liang; WANG Yao-Chuan; ZHOU Hui; CHEN Qiang; QIAN Shi-Xiong; FENG Zhe-Chuan; LU Wei-Jie

    2010-01-01

    @@ Ultrafast third-order nonlinear optical response of bulk 6H-SiC undoped and doped with different nitrogen concentrations are investigated utilizing ferntosecond Z-scan and optical Kerr effect(OKE)techniques at the wavelength of 800 nm.The Z-scan measurement shows that the third-order nonlinear optical susceptibilities of the doped samples are improved in comparison to the intrinsic sample.The 0KE results additionally reveal that the instantaneous nonlinear optical response of the sampies can be ascribed to the distortion of the electron cloud.The ultrafast transient spectroscopic measurements with the one-color and two-color pump-probe techniques demonstrate that the ultrafast recovery process in subpicosecond domain is induced by two-photon absorption process,while the slow relaxation component reflects the carrier dynamics of the excited electrons.

  17. 4D experience on Girassol Field block 17, Angola

    Lefeuvre, F.; Brechet, E.; Bertini, F.; Jourdan, J.M.; Cassou, G. [TOTAL S.A., Luanda (Angola); Dubucq, D. [TOTAL Angola, Luanda (Angola)

    2004-07-01

    The Girassol field is located in Angolan deep water of Block 17 and consists of large vertically stacked turbidities complexes. The reservoir extends over approximately 200 km{sup 2} and water depth ranges between 1300 and 1400 meters. In that context High Resolution 3D seismic became the most valuable tool to describe and monitor the reservoir. The field development plan took into account, through re-injection of the gas into the reservoir, Total environmental policy imposing the recycling of production gas. Monitoring of this injection was the main reason to shoot the first High Resolution 4D extremely early in the life of field. Despite the complexity of interpretation due to complex fluid situation and pressure effect, the results went way beyond expectations as the 4D images are of very high quality. Data has also been used to update and refine the reservoir flow model as well as to help deciding on the location of latest development wells. Other repeat surveys are scheduled, the next one before the end of 2004. The ultimate goal which we hope to reach in the very near future will be to use seismic-derived saturation and pressure changes to constrain the reservoir model during the history matching process. (author)

  18. Positive Energy Conditions in 4D Conformal Field Theory

    Farnsworth, Kara; Prilepina, Valentina

    2015-01-01

    We argue that all consistent 4D quantum field theories obey a spacetime-averaged weak energy inequality $\\langle T^{00} \\rangle \\ge -C/L^4$, where $L$ is the size of the smearing region, and $C$ is a positive constant that depends on the theory. If this condition is violated, the theory has states that are indistinguishable from states of negative total energy by any local measurement, and we expect instabilities or other inconsistencies. We apply this condition to 4D conformal field theories, and find that it places constraints on the OPE coefficients of the theory. The constraints we find are weaker than the "conformal collider" constraints of Hofman and Maldacena. We speculate that there may be theories that violate the Hofman-Maldacena bounds, but satisfy our bounds. In 3D CFTs, the only constraint we find is equivalent to the positivity of 2-point function of the energy-momentum tensor, which follows from unitarity. Our calculations are performed using momentum-space Wightman functions, which are remarka...

  19. Positive Energy Conditions in 4D Conformal Field Theory

    Farnsworth, Kara; Luty, Markus; Prilepina, Valentina

    2016-03-01

    We argue that all consistent 4D quantum field theories obey a spacetime-averaged weak energy inequality avgT00 >= - C /L4 , where L is the size of the smearing region, and C is a positive constant that depends on the theory. If this condition is violated, the theory has states that are indistinguishable from states of negative total energy by any local measurement, and we expect instabilities or other inconsistencies. We apply this condition to 4D conformal field theories, and find that it places constraints on the OPE coefficients of the theory. The constraints we find are weaker than the ``conformal collider'' constraints of Hofman and Maldacena. We speculate that there may be theories that violate the Hofman-Maldacena bounds, but satisfy our bounds. In 3D CFTs, the only constraint we find is equivalent to the positivity of 2-point function of the energy-momentum tensor, which follows from unitarity. Our calculations are performed using momentum-space Wightman functions, which are remarkably simple functions of momenta, and may be of interest in their own right.

  20. BPS black holes in gauged N = 4, D = 4 supergravity

    We find solutions of the bosonic sector of gauged N = 4, D = 4 SU(2) x SU(2) supergravity, which represent dilaton black holes with toroidal or spherical event horizons. The axion is consistently truncated, and the gauge group is broken to U(1) x U(1). The spherical black holes carry two electric and two magnetic abelian charges, whereas the toroidal holes have vanishing magnetic charges. The space-time metrics are warped products, and the manifolds turn out to be globally hyperbolic, in contrast to standard gauged supergravity ground states. It is shown that in the toroidal case, there are solutions preserving one quarter or one half of the supersymmetries, while for spherical topologies all supersymmetries are broken. In general, the toroidal BPS states represent naked singularities, but there is also a supersymmetric black hole with vanishing Hawking temperature. The ((1)/(2)) supersymmetric case arises for vanishing charges and mass, and represents the known domain wall solution of the Freedman-Schwarz model. It provides the background in which the black holes live. Finally, we use Chamseddine's and Volkov's Kaluza-Klein interpretation of gauged N = 4, D = 4 SU(2) x SU(2) supergravity to lift our solutions to ten and eleven dimensions and to consider them as solutions to the leading order equations of motion of the string/M-theory effective action

  1. 488-4D ASH LANDFILL CLOSURE CAP HELP MODELING

    Phifer, M.

    2014-11-17

    At the request of Area Completion Projects (ACP) in support of the 488-4D Landfill closure, the Savannah River National Laboratory (SRNL) has performed Hydrologic Evaluation of Landfill Performance (HELP) modeling of the planned 488-4D Ash Landfill closure cap to ensure that the South Carolina Department of Health and Environmental Control (SCDHEC) limit of no more than 12 inches of head on top of the barrier layer (saturated hydraulic conductivity of no more than 1.0E-05 cm/s) in association with a 25-year, 24-hour storm event is not projected to be exceeded. Based upon Weber 1998 a 25-year, 24-hour storm event at the Savannah River Site (SRS) is 6.1 inches. The results of the HELP modeling indicate that the greatest peak daily head on top of the barrier layer (i.e. geosynthetic clay liner (GCL) or high density polyethylene (HDPE) geomembrane) for any of the runs made was 0.079 inches associated with a peak daily precipitation of 6.16 inches. This is well below the SCDHEC limit of 12 inches.

  2. Gravitation in 4D Euclidean Space-Time Geometry

    Winkler, Franz-Guenter

    2007-01-01

    The Euclidean interpretation of special relativity provides an intuitive way to understand and derive the Lorentz transformations in the framework of a "natural" 4D Euclidean space-time geometry. In this article the conceptual basis for a purely metric generalization of the Euclidean view is laid. It consists of i) the assumption of spatial and directional variations of the speed of light (VSL), ii) a formulation of the principle of general covariance in 4D Euclidean geometry, and iii) a generally covariant motion law for point particles. For the gravitation model, which is developed on this basis, three out of four effects of the Schwarzschild solution are derived (shift of spectral lines, deflection of light, precession of perihelia of planetary orbits). The explanation of the Shapiro radar echo delay requires modifications of the space-time geometry of the sun's environment. The additional effects brought forth by the respective model entail a possible account of the coronal heating problem and thus make t...

  3. 2D/4D marker-free tumor tracking using 4D CBCT as the reference image

    Wang, Mengjiao; Sharp, Gregory C.; Rit, Simon; Delmon, Vivien; Wang, Guangzhi

    2014-05-01

    Tumor motion caused by respiration is an important issue in image-guided radiotherapy. A 2D/4D matching method between 4D volumes derived from cone beam computed tomography (CBCT) and 2D fluoroscopic images was implemented to track the tumor motion without the use of implanted markers. In this method, firstly, 3DCBCT and phase-rebinned 4DCBCT are reconstructed from cone beam acquisition. Secondly, 4DCBCT volumes and a streak-free 3DCBCT volume are combined to improve the image quality of the digitally reconstructed radiographs (DRRs). Finally, the 2D/4D matching problem is converted into a 2D/2D matching between incoming projections and DRR images from each phase of the 4DCBCT. The diaphragm is used as a target surrogate for matching instead of using the tumor position directly. This relies on the assumption that if a patient has the same breathing phase and diaphragm position as the reference 4DCBCT, then the tumor position is the same. From the matching results, the phase information, diaphragm position and tumor position at the time of each incoming projection acquisition can be derived. The accuracy of this method was verified using 16 candidate datasets, representing lung and liver applications and one-minute and two-minute acquisitions. The criteria for the eligibility of datasets were described: 11 eligible datasets were selected to verify the accuracy of diaphragm tracking, and one eligible dataset was chosen to verify the accuracy of tumor tracking. The diaphragm matching accuracy was 1.88 ± 1.35 mm in the isocenter plane and the 2D tumor tracking accuracy was 2.13 ± 1.26 mm in the isocenter plane. These features make this method feasible for real-time marker-free tumor motion tracking purposes.

  4. 2D/4D marker-free tumor tracking using 4D CBCT as the reference image

    Tumor motion caused by respiration is an important issue in image-guided radiotherapy. A 2D/4D matching method between 4D volumes derived from cone beam computed tomography (CBCT) and 2D fluoroscopic images was implemented to track the tumor motion without the use of implanted markers. In this method, firstly, 3DCBCT and phase-rebinned 4DCBCT are reconstructed from cone beam acquisition. Secondly, 4DCBCT volumes and a streak-free 3DCBCT volume are combined to improve the image quality of the digitally reconstructed radiographs (DRRs). Finally, the 2D/4D matching problem is converted into a 2D/2D matching between incoming projections and DRR images from each phase of the 4DCBCT. The diaphragm is used as a target surrogate for matching instead of using the tumor position directly. This relies on the assumption that if a patient has the same breathing phase and diaphragm position as the reference 4DCBCT, then the tumor position is the same. From the matching results, the phase information, diaphragm position and tumor position at the time of each incoming projection acquisition can be derived. The accuracy of this method was verified using 16 candidate datasets, representing lung and liver applications and one-minute and two-minute acquisitions. The criteria for the eligibility of datasets were described: 11 eligible datasets were selected to verify the accuracy of diaphragm tracking, and one eligible dataset was chosen to verify the accuracy of tumor tracking. The diaphragm matching accuracy was 1.88 ± 1.35 mm in the isocenter plane and the 2D tumor tracking accuracy was 2.13 ± 1.26 mm in the isocenter plane. These features make this method feasible for real-time marker-free tumor motion tracking purposes. (paper)

  5. Advanced Instrumentation for Ultrafast Science at the LCLS

    Berrah, Nora [Univ. of Connecticut, Storrs, CT (United States)

    2015-10-13

    This grant supported a Single Investigator and Small Group Research (SISGR) application to enable multi-user research in Ultrafast Science using the Linac Coherent Light Source (LCLS), the world’s first hard x-ray free electron laser (FEL) which lased for the first time at 1.5 Å on April 20, 2009. The goal of our proposal was to enable a New Era of Science by requesting funds to purchase and build Advanced Instrumentation for Ultrafast Science (AIUS), to utilize the intense, short x-ray pulses produced by the LCLS. The proposed instrumentation will allow peer review selected users to probe the ultrasmall and capture the ultrafast. These tools will expand on the investment already made in the construction of the light source and its instrumentation in both the LCLS and LUSI projects. The AIUS will provide researchers in the AMO, Chemical, Biological and Condensed Matter communities with greater flexibility in defining their scientific agenda at the LCLS. The proposed instrumentation will complement and significantly augment the present AMO instrument (funded through the LCLS project) through detectors and capabilities not included in the initial suite of instrumentation at the facility. We have built all of the instrumentations and they have been utilized by scientists. Please see report attached.

  6. Ultrafast Coherent Control and Characterization of Surface Reactions using FELs

    Ogasawara, Hirohito; Nordlund, Dennis a Nilsson, Anders; /SLAC, SSRL

    2005-09-30

    The microscopic understanding of reactions at surfaces requires an in-depth knowledge of the dynamics of elementary processes on an ultrafast timescale. This can be accomplished using an ultrafast excitation to initiate a chemical reaction and then probe the progression of the reaction with an ultrashort x-ray pulse from the FEL. There is a great potential to use atom-specific spectroscopy involving core levels to probe the chemical nature, structure and bonding of species on surfaces. The ultrashort electron pulse obtained in the linear accelerator to feed the X-ray FEL can also be used for generation of coherent synchrotron radiation in the low energy THz regime to be used as a pump. This radiation has an energy close to the thermal excitations of low-energy vibrational modes of molecules on surfaces and phonons in substrates. The coherent THz radiation will be an electric field pulse with a certain direction that can collectively manipulate atoms or molecules on surfaces. In this respect a chemical reaction can be initiated by collective atomic motion along a specific reaction coordinate. If the coherent THz radiation is generated from the same source as the X-ray FEL radiation, full-time synchronization for pump-probe experiments will be possible. The combination of THz and X-ray spectroscopy could be a unique opportunity for FEL facilities to conduct ultrafast chemistry studies at surfaces.

  7. Steady-state benchmarks of DK4D: A time-dependent, axisymmetric drift-kinetic equation solver

    The DK4D code has been written to solve a set of time-dependent, axisymmetric, finite-Larmor-radius drift-kinetic equations (DKEs) for the non-Maxwellian part of the electron and ion distribution functions using the full, linearized Fokker–Planck–Landau collision operator. The plasma is assumed to be in the low- to finite-collisionality regime, as is found in the cores of modern and future magnetic confinement fusion experiments. Each DKE is formulated such that the perturbed distribution function carries no net density, parallel momentum, or kinetic energy. Rather, these quantities are contained within the background Maxwellians and would be evolved by an appropriate set of extended magnetohydrodynamic (MHD) equations. This formulation allows for straight-forward coupling of DK4D to existing extended MHD time evolution codes. DK4D uses a mix of implicit and explicit temporal representations and finite element and spectral spatial representations. These, along with other computational methods used, are discussed extensively. Steady-state benchmarks are then presented comparing the results of DK4D to expected analytic results at low collisionality, qualitatively, and to the Sauter analytic fits for the neoclassical conductivity and bootstrap current, quantitatively. These benchmarks confirm that DK4D is capable of solving for the correct, gyroaveraged distribution function in stationary magnetic equilibria. Furthermore, the results presented demonstrate how the exact drift-kinetic solution varies with collisionality as a function of the magnetic moment and the poloidal angle

  8. Steady-state benchmarks of DK4D: A time-dependent, axisymmetric drift-kinetic equation solver

    Lyons, B. C. [Princeton University, Princeton, New Jersey 08544 (United States); Jardin, S. C. [Princeton Plasma Physics Laboratory, Princeton, New Jersey 08543-0451 (United States); Ramos, J. J. [Plasma Science and Fusion Center, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States)

    2015-05-15

    The DK4D code has been written to solve a set of time-dependent, axisymmetric, finite-Larmor-radius drift-kinetic equations (DKEs) for the non-Maxwellian part of the electron and ion distribution functions using the full, linearized Fokker–Planck–Landau collision operator. The plasma is assumed to be in the low- to finite-collisionality regime, as is found in the cores of modern and future magnetic confinement fusion experiments. Each DKE is formulated such that the perturbed distribution function carries no net density, parallel momentum, or kinetic energy. Rather, these quantities are contained within the background Maxwellians and would be evolved by an appropriate set of extended magnetohydrodynamic (MHD) equations. This formulation allows for straight-forward coupling of DK4D to existing extended MHD time evolution codes. DK4D uses a mix of implicit and explicit temporal representations and finite element and spectral spatial representations. These, along with other computational methods used, are discussed extensively. Steady-state benchmarks are then presented comparing the results of DK4D to expected analytic results at low collisionality, qualitatively, and to the Sauter analytic fits for the neoclassical conductivity and bootstrap current, quantitatively. These benchmarks confirm that DK4D is capable of solving for the correct, gyroaveraged distribution function in stationary magnetic equilibria. Furthermore, the results presented demonstrate how the exact drift-kinetic solution varies with collisionality as a function of the magnetic moment and the poloidal angle.

  9. 4th-International Symposium on Ultrafast Surface Science - Final Report

    Hrvoje Petek

    2005-01-26

    The 4-th International Symposium on Ultrafast Surface Dynamics (UDS4) was held at the Telluride Summer Research Center on June 22-27, 2003. The International Organizing Committee consisting of Hrvoje Petek (USA), Xiaoyang Zhu (USA), Pedro Echenique (Spain) and Maki Kawai (Japan) brought together a total of 51 participants 16 of whom were from Europe, 10 from Japan, and 25 from the USA. The focus of the conference was on ultrafast electron or light induced processes at well-defined surfaces. Ultrafast surface dynamics concerns the transfer of charge and energy at solid surfaces on the femtosecond time scale. These processes govern rates of fundamental steps in surface reactions, interfacial electron transfer in molecular electronics, and relaxation in spin transport. Recent developments in femtosecond laser technology make it possible to measure by a variety of nonlinear optical techniques directly in the time domain the microscopic rates underlying these interfacial processes. Parallel progress in scanning probe microscopy makes it possible at a single molecular level to perform the vibrational and electronic spectroscopy measurements, to induce reactions with tunneling electrons, and to observe their outcome. There is no doubt that successful development in the field of ultrafast surface dynamics will contribute to many important disciplines.

  10. Mapping motion from 4D-MRI to 3D-CT for use in 4D dose calculations: A technical feasibility study

    Purpose: Target sites affected by organ motion require a time resolved (4D) dose calculation. Typical 4D dose calculations use 4D-CT as a basis. Unfortunately, 4D-CT images have the disadvantage of being a “snap-shot” of the motion during acquisition and of assuming regularity of breathing. In addition, 4D-CT acquisitions involve a substantial additional dose burden to the patient making many, repeated 4D-CT acquisitions undesirable. Here the authors test the feasibility of an alternative approach to generate patient specific 4D-CT data sets. Methods: In this approach motion information is extracted from 4D-MRI. Simulated 4D-CT data sets [which the authors call 4D-CT(MRI)] are created by warping extracted deformation fields to a static 3D-CT data set. The employment of 4D-MRI sequences for this has the advantage that no assumptions on breathing regularity are made, irregularities in breathing can be studied and, if necessary, many repeat imaging studies (and consequently simulated 4D-CT data sets) can be performed on patients and/or volunteers. The accuracy of 4D-CT(MRI)s has been validated by 4D proton dose calculations. Our 4D dose algorithm takes into account displacements as well as deformations on the originating 4D-CT/4D-CT(MRI) by calculating the dose of each pencil beam based on an individual time stamp of when that pencil beam is applied. According to corresponding displacement and density-variation-maps the position and the water equivalent range of the dose grid points is adjusted at each time instance. Results: 4D dose distributions, using 4D-CT(MRI) data sets as input were compared to results based on a reference conventional 4D-CT data set capturing similar motion characteristics. Almost identical 4D dose distributions could be achieved, even though scanned proton beams are very sensitive to small differences in the patient geometry. In addition, 4D dose calculations have been performed on the same patient, but using 4D-CT(MRI) data sets based on

  11. Vertex Operators in 4D Quantum Gravity formulated as CFT

    Hamada, Ken-ji

    2010-01-01

    We study vertex operators in 4D conformal field theory derived from quantized gravity, whose dynamics is governed by the Weyl action and the Wess-Zumino action by Riegert. Conformal symmetry is equal to gauge symmetry of diffeomorphism, which mixes positive-metric and negative-metric modes of the gravitational field and thus these modes cannot be treated separately in physical operators. We explicitly construct gravitational vertex operators of the cosmological constant and the Ricci scalar, which are defined as space-time volume integrals of them are invariant under conformal transformations. Short distance singularities of these operator products are computed and it is shown that their coefficients have physically correct sign. Furthermore, we show that conformal algebra holds even in the system perturbed by the cosmological constant vertex operator, as in the case of the Liouville theory shown by Curtright and Thorn.

  12. Background-metric independent formulation of 4D quantum gravity

    Using the background-metric independence for the traceless mode as well as the conformal mode, 4D quantum gravity is described as a quantum field theory defined on a non-dynamical background metric. The measure then induces an action with four derivatives. So we think that fourth order gravity is essential and the Einstein-Hilbert term should be treated like a mass term. We introduce the dimensionless self-coupling constant t for the traceless mode. In this paper we study a model where the measure can be evaluated in the limit t → 0 exactly, using the background-metric independence for the conformal mode. The t-dependence of the measure is determined perturbatively using the background-metric independence for the traceless mode

  13. When chaos meets hyperchaos: 4D Rössler model

    Chaotic behavior is a common feature of nonlinear dynamics, as well as hyperchaos in high-dimensional systems. In numerical simulations of these systems it is quite difficult to distinguish one from another behavior in some situations, as the results are frequently quite “noisy”. We show that in such systems a global hyperchaotic invariant set is present giving rise to long hyperchaotic transient behaviors. This fact provides a mechanism for these noisy results. The coexistence of chaos and hyperchaos is proved via Computer-Assisted Proofs techniques. - Highlights: • The coexistence of chaos and hyperchaos in the 4D Rössler system is proved via Computer-Assisted Proofs techniques. • A global hyperchaotic invariant set is present giving rise to long hyperchaotic transient behaviors. • The long transient behaviors make difficult in numerical simulations to distinguish chaos from hyperchaos in some situations

  14. When chaos meets hyperchaos: 4D Rössler model

    Barrio, Roberto, E-mail: rbarrio@unizar.es [Departamento de Matemática Aplicada and IUMA, University of Zaragoza, E-50009 Zaragoza (Spain); Computational Dynamics group, University of Zaragoza, E-50009 Zaragoza (Spain); Angeles Martínez, M., E-mail: gelimc@unizar.es [Computational Dynamics group, University of Zaragoza, E-50009 Zaragoza (Spain); Serrano, Sergio, E-mail: sserrano@unizar.es [Departamento de Matemática Aplicada and IUMA, University of Zaragoza, E-50009 Zaragoza (Spain); Computational Dynamics group, University of Zaragoza, E-50009 Zaragoza (Spain); Wilczak, Daniel, E-mail: wilczak@ii.uj.edu.pl [Faculty of Mathematics and Computer Science, Jagiellonian University, Łojasiewicza 6, 30-348 Kraków (Poland)

    2015-10-09

    Chaotic behavior is a common feature of nonlinear dynamics, as well as hyperchaos in high-dimensional systems. In numerical simulations of these systems it is quite difficult to distinguish one from another behavior in some situations, as the results are frequently quite “noisy”. We show that in such systems a global hyperchaotic invariant set is present giving rise to long hyperchaotic transient behaviors. This fact provides a mechanism for these noisy results. The coexistence of chaos and hyperchaos is proved via Computer-Assisted Proofs techniques. - Highlights: • The coexistence of chaos and hyperchaos in the 4D Rössler system is proved via Computer-Assisted Proofs techniques. • A global hyperchaotic invariant set is present giving rise to long hyperchaotic transient behaviors. • The long transient behaviors make difficult in numerical simulations to distinguish chaos from hyperchaos in some situations.

  15. Immersive 4D Interactive Visualization of Large-Scale Simulations

    Teuben, P; Levy, S; Makino, J; McMillan, S; Zwart, S P; Shara, M M; Emmart, C; Teuben, Peter; Hut, Piet; Levy, Stuart; Makino, Jun; Millan, Steve Mc; Zwart, Simon Portegies; Shara, Mike; Emmart, Carter

    2001-01-01

    In dense clusters a bewildering variety of interactions between stars can be observed, ranging from simple encounters to collisions and other mass-transfer encounters. With faster and special-purpose computers like GRAPE, the amount of data per simulation is now exceeding 1TB. Visualization of such data has now become a complex 4D data-mining problem, combining space and time, and finding interesting events in these large datasets. We have recently starting using the virtual reality simulator, installed in the Hayden Planetarium in the American Museum for Natural History, to tackle some of these problem. This work (http://www.astro.umd.edu/nemo/amnh/) reports on our first ``observations'', modifications needed for our specific experiments, and perhaps field ideas for other fields in science which can benefit from such immersion. We also discuss how our normal analysis programs can be interfaced with this kind of visualization.

  16. Immersive 4-D Interactive Visualization of Large-Scale Simulations

    Teuben, P. J.; Hut, P.; Levy, S.; Makino, J.; McMillan, S.; Portegies Zwart, S.; Shara, M.; Emmart, C.

    In dense clusters a bewildering variety of interactions between stars can be observed, ranging from simple encounters to collisions and other mass-transfer encounters. With faster and special-purpose computers like GRAPE, the amount of data per simulation is now exceeding 1 TB. Visualization of such data has now become a complex 4-D data-mining problem, combining space and time, and finding interesting events in these large datasets. We have recently starting using the virtual reality simulator, installed in the Hayden Planetarium in the American Museum for Natural History, to tackle some of these problem. This work reports on our first ``observations,'' modifications needed for our specific experiments, and perhaps field ideas for other fields in science which can benefit from such immersion. We also discuss how our normal analysis programs can be interfaced with this kind of visualization.

  17. Towards 4D intervention guidance using compressed sensing

    Interventional radiology is nowadays usually guided with projection radiography using mono- or biplane systems. Due to the projective nature of this guidance imaging certain intraprocedural situations remain unclear. Although helpful, the use of 3D CT is limited due to radiation dose. Using advanced reconstruction techniques incorporating prior knowledge, one could overcome these limitations without exceeding dose limitations. Intervention guidance is especially appealing to those algorithms, because certain constrains apply to useful images in intervention guidance that vary relevantly from other CT applications. These are: key relevance of high contrast structures, sparse temporal updates and little relevance of absolute CT values. In this paper the principal usability of reconstruction algorithms for intervention guidance is tested. Compressed sensing algorithms PICCS and ASD-POCS are compared to the McKinnon-Bates and Feldkamp-Davis-Kress algorithm. Animal experiments as well as simulations are performed. An outlook towards 4D intervention guidance is provided. (orig.)

  18. 4D Script N = 2 supergravity and projective superspace

    Kuzenko, S. M.; Lindström, U.; Rocek, M.; Tartaglino-Mazzucchelli, G.

    2008-09-01

    This paper presents a projective superspace formulation for 4D Script N = 2 matter-coupled supergravity. We first describe a variant superspace realization for the Script N = 2 Weyl multiplet. It differs from that proposed by Howe in 1982 by the choice of the structure group (SO(3,1) × SU(2) versus SO(3,1) × U(2)), which implies that the super-Weyl transformations are generated by a covariantly chiral parameter instead of a real unconstrained one. We introduce various off-shell supermultiplets which are curved superspace analogues of the superconformal projective multiplets in global supersymmetry and which describe matter fields coupled to supergravity. A manifestly locally supersymmetric and super-Weyl invariant action principle is given. Off-shell locally supersymmetric nonlinear sigma models are presented in this new superspace.

  19. Seeing the unseen-bioturbation in 4D

    Delefosse, Matthieu; Kristensen, Erik; Crunelle, Diane;

    2015-01-01

    Understanding spatial and temporal patterns of bioirrigation induced by benthic fauna ventilation is critical given its significance on benthic nutrient exchange and biogeochemistry in coastal ecosystems. The quantification of this process challenges marine scientists because faunal activities and...... behaviors are concealed in an opaque sediment matrix. Here, we use a hybrid medical imaging technique, positron emission tomography and computed tomography (PET/CT) to provide a qualitative visual and fully quantitative description of bioirrigation in 4D (space and time). As a study case, we present images...... provide information that otherwise would require multiple methods. Furthermore, PET/CT scan is versatile as it can be used for a variety of benthic macrofauna species and sediment types and it provides information on burrow morphology or animal behavior. The lack of accessibility to the expensive...

  20. Parallel Wavefront Analysis for a 4D Interferometer

    Rao, Shanti R.

    2011-01-01

    This software provides a programming interface for automating data collection with a PhaseCam interferometer from 4D Technology, and distributing the image-processing algorithm across a cluster of general-purpose computers. Multiple instances of 4Sight (4D Technology s proprietary software) run on a networked cluster of computers. Each connects to a single server (the controller) and waits for instructions. The controller directs the interferometer to several images, then assigns each image to a different computer for processing. When the image processing is finished, the server directs one of the computers to collate and combine the processed images, saving the resulting measurement in a file on a disk. The available software captures approximately 100 images and analyzes them immediately. This software separates the capture and analysis processes, so that analysis can be done at a different time and faster by running the algorithm in parallel across several processors. The PhaseCam family of interferometers can measure an optical system in milliseconds, but it takes many seconds to process the data so that it is usable. In characterizing an adaptive optics system, like the next generation of astronomical observatories, thousands of measurements are required, and the processing time quickly becomes excessive. A programming interface distributes data processing for a PhaseCam interferometer across a Windows computing cluster. A scriptable controller program coordinates data acquisition from the interferometer, storage on networked hard disks, and parallel processing. Idle time of the interferometer is minimized. This architecture is implemented in Python and JavaScript, and may be altered to fit a customer s needs.

  1. Energy level properties of 4p{sup 6}4d{sup 3}, 4p{sup 6}4d{sup 2}4f, and 4p{sup 5}4d{sup 4} configurations of the W{sup 35+} ion

    Bogdanovich, P., E-mail: Pavelas.Bogdanovicius@tfai.vu.lt; Kisielius, R.

    2014-11-15

    The ab initio quasirelativistic Hartree–Fock method developed specifically for the calculation of spectroscopic parameters of heavy atoms and highly charged ions was used to derive spectral data for the multicharged tungsten ion W{sup 35+}. The configuration interaction method was applied to include the electron-correlation effects. The relativistic effects were taken into account in the Breit–Pauli approximation for quasirelativistic Hartree–Fock radial orbitals. The energy level spectra, radiative lifetimes τ, and Lande g-factors have been calculated for the 4p{sup 6}4d{sup 3}, 4p{sup 6}4d{sup 2}4f, and 4p{sup 5}4d{sup 4} configurations of the W{sup 35+} ion.

  2. Ultrafast dynamics of interfacial water

    Hsieh, C.-S.

    2014-01-01

    We survey the dynamics of the interfacial water at the air/water interface. We reveal that the ultrafast vibrational energy transfer dynamics and spectral diffusion of the OH stretch mode at the interface differs from those in the bulk significantly; the rotational motion is 3 times faster than in the bulk and energy relaxation is dominated by the rotational dynamics as well as the vibrational energy transfer from the free OH group to the H-bonded OH groups of a water molecule with the free O...

  3. Ultrafast vibrations of gold nanorings

    Kelf, T; Tanaka, Y; Matsuda, O;

    2011-01-01

    We investigate the vibrational modes of gold nanorings on a silica substrate with an ultrafast optical technique. By comparison with numerical simulations, we identify several resonances in the gigahertz range associated with axially symmetric deformations of the nanoring and substrate. We...... elucidate the corresponding mode shapes and find that the substrate plays an important role in determining the mode damping. This study demonstrates the need for a plasmonic nano-optics approach to understand the optical excitation and detection mechanisms for the vibrations of plasmonic nanostructures....

  4. Geometric validation of self-gating k-space-sorted 4D-MRI vs 4D-CT using a respiratory motion phantom

    Purpose: MRI is increasingly being used for radiotherapy planning, simulation, and in-treatment-room motion monitoring. To provide more detailed temporal and spatial MR data for these tasks, we have recently developed a novel self-gated (SG) MRI technique with advantage of k-space phase sorting, high isotropic spatial resolution, and high temporal resolution. The current work describes the validation of this 4D-MRI technique using a MRI- and CT-compatible respiratory motion phantom and comparison to 4D-CT. Methods: The 4D-MRI sequence is based on a spoiled gradient echo-based 3D projection reconstruction sequence with self-gating for 4D-MRI at 3 T. Respiratory phase is resolved by using SG k-space lines as the motion surrogate. 4D-MRI images are reconstructed into ten temporal bins with spatial resolution 1.56 × 1.56 × 1.56 mm3. A MRI-CT compatible phantom was designed to validate the performance of the 4D-MRI sequence and 4D-CT imaging. A spherical target (diameter 23 mm, volume 6.37 ml) filled with high-concentration gadolinium (Gd) gel is embedded into a plastic box (35 × 40 × 63 mm3) and stabilized with low-concentration Gd gel. The phantom, driven by an air pump, is able to produce human-type breathing patterns between 4 and 30 respiratory cycles/min. 4D-CT of the phantom has been acquired in cine mode, and reconstructed into ten phases with slice thickness 1.25 mm. The 4D images sets were imported into a treatment planning software for target contouring. The geometrical accuracy of the 4D MRI and CT images has been quantified using target volume, flattening, and eccentricity. The target motion was measured by tracking the centroids of the spheres in each individual phase. Motion ground-truth was obtained from input signals and real-time video recordings. Results: The dynamic phantom has been operated in four respiratory rate (RR) settings, 6, 10, 15, and 20/min, and was scanned with 4D-MRI and 4D-CT. 4D-CT images have target-stretching, partial

  5. Ultrafast dynamics and decoherence of quasiparticles in surface bands: Preasymptotic decay and dephasing of quasiparticle states

    Lazić, Predrag; Silkin, Vjaćeslav M.; Chulkov, Evgenij V.; Echenique, Pedro M.; Gumhalter, Branko

    2007-01-01

    We develop a many-body description of ultrafast electron dynamics in surface bands appropriate for studying relaxation of hot electrons and holes excited in the processes of one- and two-photon photoemission and inverse photoemission from surfaces. The description is based on the formalism for calculation of quasiparticle survival probabilities combined with self-consistent treatment of the electronic response of the system. We show that the calculation of survival amplitudes which carry info...

  6. Ultrafast Gain Dynamics in Quantum Dot Amplifiers: Theoretical Analysis and Experimental Investigations

    Poel, Mike van der; Gehrig, Edeltraud; Hess, Ortwin;

    2005-01-01

    Ultrafast gain dynamics in an optical amplifier with an active layer of self-organized quantum dots (QDs) emitting near 1.3$muhbox m$is characterized experimentally in a pump-probe experiment and modeled theoretically on the basis of QD Maxwell–Bloch equations. Experiment and theory are in good...... agreement and show ultrafast subpicoseconds gain recovery followed by a slower 5 ps recovery. This behavior is found to be mainly caused by longitudinal optical phonon scattering and strongly dependents on electronic structure and confinement energy of the dots. A low amplitude-phase coupling ($alpha...

  7. Ultrafast dynamics of copper nanoparticles embedded in soda-lime silicate glass fabricated by ion exchange

    Copper nanoparticles embedded in soda-lime glass were fabricated by ion exchange followed by thermal treatment in hydrogen. The ultrafast dynamics of the embedded Cu nanoparticles formed under different fabrication conditions were investigated by applying femtosecond pump-probe technique. Non-Fermi electrons were suggested to be dominant in the transient behavior of the nanocomposites far from surface plasmon resonance of Cu. The long ion-exchange processing time was found to benefit and improve the ultrafast response of the fabricated nanocomposites.

  8. Ultrafast reorganization of the hole charge created upon outer-valence ionization of porphyrins

    Highlights: ► Ultrafast electron dynamics following ionization of porphyrins is studied. ► Ionization spectra of the free-base porphyrin and Mg(II) porphyrin are analyzed. ► Hole charge created upon ionization spreads over the molecule in only few femtoseconds. ► This redistribution of the charge may predetermine the nuclear dynamics that follow. - Abstract: Based on elaborated ab initio calculations we first study the ionization spectra of the free-base porphyrin (H2-P) and Mg(II) porphyrin (Mg-P). Then we investigate the ultrafast electron dynamics following outer-valence ionization of these systems which constitutes the highlight of this paper. It is shown that the electron correlation effects are very strong in these systems giving rise to pronounced shake-down satellites in the outer-valence part of the ionization spectra. We show that due to these strong correlation effects the removal of an electron from the 3b1g orbital of H2-P and Mg-P leads to an ultrafast reorganization of the electronic cloud. After being initially localized on the B and D pyrrole rings, the hole charge created upon ionization spreads throughout the molecule in only few femtoseconds. In both systems the electron dynamics triggered by the ionization represent alternating ultrafast delocalizations and localizations of the charge. The results may also give a hint on the nuclear dynamics in the free-base and Mg(II) porphyrin radical cations that will follow the ultrafast charge migration.

  9. 4D Dynamic RNP Annual Interim Report-Year 1

    Finkelsztein, Daniel M.; Sturdy, James L.; Alaverdi, Omeed; Chung, William W.; Salvano, Daniel; Klooster, Joel; Hochwarth, Joachim K.

    2010-01-01

    This Annual Interim Report summarizes the activities led by Raytheon, in collaboration with GE Aviation and SAIC, and presents the results obtained during the first year of this research effort to expand the RNP concept to 4 dimensions relative to a dynamic frame of reference. Joint Program Development Office (JPDO)Concepts of Operations for the Next Generation Air Transportation System (NextGen) considers 4 Dimension Trajectory (4DT) procedures a key enabler to Trajectory Based Operations (TBO). The JPDO defines 4DT as a precise description of an aircraft path in space and time . While NextGen assumes that this path is defined within an Earth-reference frame, many 4DT procedure implementations will require an aircraft to precisely navigate relative to a moving reference such as another aircraft to form aggregate flows or a weather cell to allow for flows to shift. Current methods of implementing routes and flight paths rely on aircraft meeting a Required Navigation Performance (RNP) specification and being equipped with a monitoring and alerting capability to annunciate when the aircraft system is unable to meet the performance specification required for the operation. Since all aircraft today operate within the NAS relative to fixed reference points, the current RNP definition is deemed satisfactory. However, it is not well understood how the current RNP construct will support NextGen 4DT procedures where aircraft operate relative to each other or to other dynamic frames of reference. The objective of this research effort is to analyze candidate 4DT procedures from both an Air Navigation Service Provider (ANSP) and aircraft perspective, to identify their specific navigational requirements, assess the shortcomings of the current RNP construct to meet these requirements, to propose an extended 4 Dimensional Dynamic RNP (4D Dynamic RNP) construct that accounts for the dynamic spatial and temporal nature of the selected 4DT procedures, and finally, to design an

  10. On the use of EPID-based implanted marker tracking for 4D radiotherapy

    Four-dimensional (4D) radiotherapy delivery to dynamically moving tumors requires a real-time signal of the tumor position as a function of time so that the radiation beam can continuously track the tumor during the respiration cycle. The aim of this study was to develop and evaluate an electronic portal imaging device (EPID)-based marker-tracking system that can be used for real-time tumor targeting, or 4D radiotherapy. Three gold cylinders, 3 mm in length and 1 mm in diameter, were implanted in a dynamic lung phantom. The phantom range of motion was 4 cm with a 3-s 'breathing' period. EPID image acquisition parameters were modified, allowing image acquisition in 0.1 s. Images of the stationary and moving phantom were acquired. Software was developed to segment automatically the marker positions from the EPID images. Images acquired in 0.1 s displayed higher noise and a lower signal-noise ratio than those obtained using regular (>1 s) acquisition settings. However, the markers were still clearly visible on the 0.1-s images. The motion of the phantom blurred the images of the markers and further reduced the signal-noise ratio, though they could still be successfully segmented from the images in 10-30 ms of computation time. The positions of gold markers placed in the lung phantom were detected successfully, even for phantom velocities substantially higher than those observed for typical lung tumors. This study shows that using EPID-based marker tracking for 4D radiotherapy is feasible, however, changes in linear accelerator technology and EPID-based image acquisition as well as patient studies are required before this method can be implemented clinically

  11. Large lateral photovoltaic effect with ultrafast relaxation time in SnSe/Si junction

    Wang, Xianjie; Zhao, Xiaofeng; Hu, Chang; Zhang, Yang; Song, Bingqian; Zhang, Lingli; Liu, Weilong; Lv, Zhe; Zhang, Yu; Tang, Jinke; Sui, Yu; Song, Bo

    2016-07-01

    In this paper, we report a large lateral photovoltaic effect (LPE) with ultrafast relaxation time in SnSe/p-Si junctions. The LPE shows a linear dependence on the position of the laser spot, and the position sensitivity is as high as 250 mV mm-1. The optical response time and the relaxation time of the LPE are about 100 ns and 2 μs, respectively. The current-voltage curve on the surface of the SnSe film indicates the formation of an inversion layer at the SnSe/p-Si interface. Our results clearly suggest that most of the excited-electrons diffuse laterally in the inversion layer at the SnSe/p-Si interface, which results in a large LPE with ultrafast relaxation time. The high positional sensitivity and ultrafast relaxation time of the LPE make the SnSe/p-Si junction a promising candidate for a wide range of optoelectronic applications.

  12. The terahertz frontier for ultrafast coherent magnetic switching: Terahertz-induced demagnetization in ferromagnets

    Shalaby, Mostafa; Hauri, Christoph P

    2015-01-01

    The transition frequency between nonthermal coherent magnetic precessions and ultrafast demagnetization is arguably the most sought after answer in magnetism science and technology nowadays. So far, it is believed to be in the terahertz (THz) range. Here, using an ultra-intense low frequency THz bullet, and thin magnetic layers, we report on experimental evidences that fully coherent nonthermal THz magnetic switching may never be reachable in conventional ferromagnetic thin films. At high excitation intensities, while the spins still coherently precess with the THz magnetic field, the deposited THz energy initiates ultrafast demagnetization and ultimately material damage. These series of phenomena are found to take place simultaneously. The reported experiments set fundamental limits and raise questions on the coupling between electronic and magnetic systems and the associated structural dynamics on the ultrafast time scale.

  13. Ultrafast Optical Kerr Effect in Amorphous As2Se3 Film Induced by Ultrashort Laser Pulses

    刘启明; 米君; 钱士雄; 干福熹

    2002-01-01

    Nonresonant third-order nonlinear optical properties of amorphous As2Se3 films were investigated experimentally by the method of femtosecond optical heterodyne detection of the optical Kerr effect at 805 nm with 80 fs ultrafast pulses. The results have shown that the values of real and imaginary components of third-order susceptibility of amorphous As2Se3 films were 5.6×10-12 esu and -2.0×10-13 esu, respectively. Amorphous As2Se3 films demonstrated a very fast response time within 200fs. The ultrafast response and large third-order nonlinearity are attributed to the ultrafast distortion of the electron cloud of As2Se3 films.

  14. Pump-probe SAXS experiments on ultrafast demagnetization of magnetic multilayers

    We have investigated the ultrafast optical demagnetization of domain patterns in magnetic multilayers with perpendicular magnetic anisotropy in an infrared-pump x-ray-probe experiment. As a probe we used small angle x-ray scattering which, via x-ray magnetic circular dichroism at the Co M-edge, allows us to simultaneously obtain information on the magnitude of the local magnetization and the characteristic length scale of the magnetic domains. The free-electron laser source FLASH at Hamburg was tuned to deliver λ=20.9nm x-ray pulses of approx. 25 fs duration which were synchronized to an infrared fs laser for pump-probe experiments with sub-ps time resolution. In addition to ultrafast demagnetization, we observe sub-ps structural changes of the magnetic domain configuration. Models to explain this ultrafast structural change will be discussed.

  15. Ultrafast non-equilibrium dynamics in conventional and unconventional superconductors

    Schnyder, Andreas; Manske, Dirk [Max-Planck-Institut fuer Festkoerperforschung, Heisenbergstrasse 1, D-70569 Stuttgart (Germany)

    2010-07-01

    We present simulations of the ultrafast dynamics of conventional and unconventional superconductors using density-matrix theory. In particular, we study how the optical conductivity evolves in response to ultrashort optical pulses in the frequency range of the superconducting gap, i.e., in the terahertz regime. The dominant relaxation process is assumed to be due to electron-phonon collisions. Employing a second order cluster expansion and assuming that the phonons remain equilibrated, Boltzmann type equations for the dynamics of the quasiparticle occupations and coherences are derived. We apply our theoretical model to the study of non-equilibrium dynamics in the two-gap superconductor MgB{sub 2}.

  16. Driving magnetic order in a manganite by ultrafast lattice excitation.

    Forst, M.; Tobey, R. I.; Wall, S.; Bromberger, H.; Khanna, V.; Cavalieri, A. L.; Chuang, Y.-D.; Lee, W. S.; Moore, R.; Schlotter, W. F.; Turner, J. J.; Krupin, O.; Trigo, M.; Zheng, H.; Mitchell, J. F.; Dhesi, S. S.; Hill, J. P.; Cavalleri, A. (Materials Science Division); (Univ. Hamburg); (Brookhaven Nat. Lab.); (Fritz-Haber-Inst. Max Planck Soc.); (Univ. Oxford); (Lawrence Berkeley Lab.); (SLAC Nat. Accel. Lab.); (Stanford Univ.); (European XFEL); (Diamond Light Source)

    2011-01-01

    Femtosecond midinfrared pulses are used to directly excite the lattice of the single-layer manganite La{sub 0.5}Sr{sub 1.5}MnO{sub 4}. Magnetic and orbital orders, as measured by femtosecond resonant soft x-ray diffraction with an x-ray free-electron laser, are reduced within a few picoseconds. This effect is interpreted as a displacive exchange quench, a prompt shift in the equilibrium value of the magnetic- and orbital-order parameters after the lattice has been distorted. Control of magnetism through ultrafast lattice excitation may be of use for high-speed optomagnetism.

  17. Microwave photonic comb filter with ultra-fast tunability.

    Jiang, H Y; Yan, L S; Pan, Y; Pan, W; Luo, B; Zou, X H; Eggleton, B J

    2015-11-01

    A microwave comb filter with ultra-fast tunability is proposed based on the fundamental delay-line microwave photonic filter. The central frequency of the passband or stopband in such a filter can be rapidly adjusted, along with the independent tunability of the free spectral range (FSR). Experimental results show that the central frequency of the transfer function is electronically tuned with a frequency difference of half of the FSR at a speed of cognitive radio, and next-generation radar systems. PMID:26512477

  18. Multimaterial 4D Printing with Tailorable Shape Memory Polymers

    Ge, Qi; Sakhaei, Amir Hosein; Lee, Howon; Dunn, Conner K.; Fang, Nicholas X.; Dunn, Martin L.

    2016-08-01

    We present a new 4D printing approach that can create high resolution (up to a few microns), multimaterial shape memory polymer (SMP) architectures. The approach is based on high resolution projection microstereolithography (PμSL) and uses a family of photo-curable methacrylate based copolymer networks. We designed the constituents and compositions to exhibit desired thermomechanical behavior (including rubbery modulus, glass transition temperature and failure strain which is more than 300% and larger than any existing printable materials) to enable controlled shape memory behavior. We used a high resolution, high contrast digital micro display to ensure high resolution of photo-curing methacrylate based SMPs that requires higher exposure energy than more common acrylate based polymers. An automated material exchange process enables the manufacture of 3D composite architectures from multiple photo-curable SMPs. In order to understand the behavior of the 3D composite microarchitectures, we carry out high fidelity computational simulations of their complex nonlinear, time-dependent behavior and study important design considerations including local deformation, shape fixity and free recovery rate. Simulations are in good agreement with experiments for a series of single and multimaterial components and can be used to facilitate the design of SMP 3D structures.

  19. Multimaterial 4D Printing with Tailorable Shape Memory Polymers.

    Ge, Qi; Sakhaei, Amir Hosein; Lee, Howon; Dunn, Conner K; Fang, Nicholas X; Dunn, Martin L

    2016-01-01

    We present a new 4D printing approach that can create high resolution (up to a few microns), multimaterial shape memory polymer (SMP) architectures. The approach is based on high resolution projection microstereolithography (PμSL) and uses a family of photo-curable methacrylate based copolymer networks. We designed the constituents and compositions to exhibit desired thermomechanical behavior (including rubbery modulus, glass transition temperature and failure strain which is more than 300% and larger than any existing printable materials) to enable controlled shape memory behavior. We used a high resolution, high contrast digital micro display to ensure high resolution of photo-curing methacrylate based SMPs that requires higher exposure energy than more common acrylate based polymers. An automated material exchange process enables the manufacture of 3D composite architectures from multiple photo-curable SMPs. In order to understand the behavior of the 3D composite microarchitectures, we carry out high fidelity computational simulations of their complex nonlinear, time-dependent behavior and study important design considerations including local deformation, shape fixity and free recovery rate. Simulations are in good agreement with experiments for a series of single and multimaterial components and can be used to facilitate the design of SMP 3D structures. PMID:27499417

  20. 2,4-D and IAA Amino Acid Conjugates Show Distinct Metabolism in Arabidopsis

    Eyer, Luděk; Vain, Thomas; Pařízková, Barbora; Oklestkova, Jana; Barbez, Elke; Kozubíková, Hana; Pospíšil, Tomáš; Wierzbicka, Roksana; Kleine-Vehn, Jürgen; Fránek, Milan; Strnad, Miroslav; Robert, Stéphanie

    2016-01-01

    The herbicide 2,4-D exhibits an auxinic activity and therefore can be used as a synthetic and traceable analog to study auxin-related responses. Here we identified that not only exogenous 2,4-D but also its amide-linked metabolite 2,4-D-Glu displayed an inhibitory effect on plant growth via the TIR1/AFB auxin-mediated signaling pathway. To further investigate 2,4-D metabolite conversion, identity and activity, we have developed a novel purification procedure based on the combination of ion exchange and immuno-specific sorbents combined with a sensitive liquid chromatography-mass spectrometry method. In 2,4-D treated samples, 2,4-D-Glu and 2,4-D-Asp were detected at 100-fold lower concentrations compared to 2,4-D levels, showing that 2,4-D can be metabolized in the plant. Moreover, 2,4-D-Asp and 2,4-D-Glu were identified as reversible forms of 2,4-D homeostasis that can be converted to free 2,4-D. This work paves the way to new studies of auxin action in plant development. PMID:27434212

  1. Ultrafast CARS with Improved Spectral Resolution

    Lochbrunner S.

    2013-03-01

    Full Text Available Molecular vibrations are investigated by time and frequency resolved CARS applying ultrafast excitation and picosecond probing for high spectral resolution. Enhanced spectral structure and beating phenomena are demonstrated for coalescing Raman bands.

  2. A New Class of Ultrafast Photoswitchable Chromopeptides

    Cordes, Thorben; Riesselmann, Kerstin; Herre, Stefan; Rück-Braun, Karola; Zinth, Wolfgang; Corkum, Paul; Jonas, David M.; Miller, R.J. Dwayne; Weiner, Andrew M.

    2007-01-01

    The photochemical properties of a new ultrafast photoswitch based on hemithioindigo derivatives are investigated by transient absorption spectroscopy. The applicability as a trigger molecule for fast structural changes in small peptides is tested on a biologically relevant structure.

  3. Ultrafast Beam Switching Using Coupled VCSELs

    Ning, Cun-Zheng; Goorjian, Peter

    2001-01-01

    We propose a new approach to performing ultrafast beam switching using two coupled Vertical-Cavity Surface-Emitting Lasers (VCSELs). The strategy is demonstrated by numerical simulation, showing a beam switching of 10 deg at 42 GHz.

  4. Ultrafast charge dynamics in novel nanoparticles

    Al Otaify, Ali Abdullah

    2015-01-01

    The ultrafast charge dynamics in a number of nanostructured materials relevant to the production of renewable energy are investigated using ultrafast transient absorption spectroscopy. The materials include mercury telluride and cadmium mercury telluride quantum dots, and gold nanoparticles loaded on titanium dioxide colloidal spheres. The analysis of the resultant pump-induced transmittance change spectra and transients allow the determination of charge relaxation routes including multiple e...

  5. An ultrafast carbon nanotube terahertz polarisation modulator

    Docherty, Callum J.; Stranks, Samuel D.; Habisreutinger, Severin N.; Joyce, Hannah J.; Herz, Laura M.; Nicholas, Robin J.; Johnston, Michael B., E-mail: m.johnston@physics.ox.ac.uk [Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford OX1 3PU (United Kingdom)

    2014-05-28

    We demonstrate ultrafast modulation of terahertz radiation by unaligned optically pumped single-walled carbon nanotubes. Photoexcitation by an ultrafast optical pump pulse induces transient terahertz absorption in nanowires aligned parallel to the optical pump. By controlling the polarisation of the optical pump, we show that terahertz polarisation and modulation can be tuned, allowing sub-picosecond modulation of terahertz radiation. Such speeds suggest potential for semiconductor nanowire devices in terahertz communication technologies.

  6. Photonic-assisted ultrafast THz wireless access

    Yu, Xianbin; Chen, Ying; Galili, Michael;

    THz technology has been considered feasible for ultrafast wireless data communi- cation, to meet the increasing demand on next-generation fast wireless access, e.g., huge data file transferring and fast mobile data stream access. This talk reviews recent progress in high-speed THz wireless...... communications enabled by photonics technologies, as well as the needed technical breakthroughs for achieving ultrafast data rates beyond 100Gbit/s...

  7. Nonponderomotive electron acceleration in ultrashort surface-plasmon fields

    We investigate the nonponderomotive nature of ultrafast plasmonic electron acceleration in strongly decaying electromagnetic fields generated by few-cycle and single-cycle femtosecond laser pulses. We clearly identify the conditions contributing to nonponderomotive acceleration and establish fundamental scaling laws and carrier-envelope phase effects. These all-optically accelerated compact, femtosecond electron sources can be utilized in contemporary ultrafast methods.

  8. Insights into Ultrafast Demagnetization in Pseudogap Half-Metals

    Mann, Andreas; Walowski, Jakob; Münzenberg, Markus; Maat, Stefan; Carey, Matthew J.; Childress, Jeffrey R.; Mewes, Claudia; Ebke, Daniel; Drewello, Volker; Reiss, Günter; Thomas, Andy

    2012-10-01

    Interest in femtosecond demagnetization dynamics was sparked by Bigot’s experiment in 1996, which unveiled the elementary mechanisms that relate the electrons’ temperature to their spin order. Simultaneously, the application of fast demagnetization experiments has been demonstrated to provide key insight into technologically important systems such as high-spin-polarization metals, and consequently there is broad interest in further understanding the physics of these phenomena. To gain new and relevant insights, we performed ultrafast optical pump-probe experiments to characterize the demagnetization processes of highly spin-polarized magnetic thin films on a femtosecond time scale. Full spin polarization is obtained in half-metallic ferro- or ferrimagnets, where only one spin channel is populated at the Fermi level, whereas the other one exhibits a gap. In these materials, the spin-scattering processes is controlled via the electronic structure, and thus their ultrafast demagnetization is solely related to the spin polarization via a Fermi golden-rule model. Accordingly, a long demagnetization time correlates with a high spin polarization due to the suppression of the spin-flip scattering at around the Fermi level. Here we show that isoelectronic Heusler compounds (Co2MnSi, Co2MnGe, and Co2FeAl) exhibit a degree of spin polarization between 59% and 86%. We explain this behavior by considering the robustness of the gap against structural disorder. Moreover, we observe that CoFe-based pseudogap materials, such as partially ordered Co-Fe-Ge and Co-Fe-B alloys, can reach similar values of the spin polarization. By using the unique features of these metals we vary the number of possible spin-flip channels, which allows us to pinpoint and control the half-metals’ electronic structure and its influence on the elementary mechanisms of ultrafast demagnetization.

  9. 32 CFR 1630.43 - Class 4-D: Minister of religion.

    2010-07-01

    ... 32 National Defense 6 2010-07-01 2010-07-01 false Class 4-D: Minister of religion. 1630.43 Section... CLASSIFICATION RULES § 1630.43 Class 4-D: Minister of religion. In accord with part 1645 of this chapter any registrant shall be placed in Class 4-D who is a: (a) Duly ordained minister of religion; or (b)...

  10. Experimental and ab initio ultrafast carrier dynamics in plasmonic nanoparticles

    Brown, Ana M; Narang, Prineha; Schwartzberg, Adam M; Goddard, William A; Atwater, Harry A

    2016-01-01

    Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions which allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly non-thermal excited carriers and longer-lived thermalizing carriers.

  11. Experimenting with the GMAO 4D Data Assimilation

    Todling, R.; El Akkraoui, A.; Errico, R. M.; Guo, J.; Kim, J.; Kliest, D.; Parrish, D. F.; Suarez, M.; Trayanov, A.; Tremolet, Yannick; Whitaker, J.

    2012-01-01

    The Global Modeling and Assimilation Office (GMAO) has been working to promote its prototype four-dimensional variational (4DVAR) system to a version that can be exercised at operationally desirable configurations. Beyond a general circulation model (GeM) and an analysis system, traditional 4DV AR requires availability of tangent linear (TL) and adjoint (AD) models of the corresponding GeM. The GMAO prototype 4DVAR uses the finite-volume-based GEOS GeM and the Grid-point Statistical Interpolation (GSI) system for the first two, and TL and AD models derived ITom an early version of the finite-volume hydrodynamics that is scientifically equivalent to the present GEOS nonlinear GeM but computationally rather outdated. Specifically, the TL and AD models hydrodynamics uses a simple (I-dimensional) latitudinal MPI domain decomposition, which has consequent low scalability and prevents the prototype 4DV AR ITom being used in realistic applications. In the near future, GMAO will be upgrading its operational GEOS GCM (and assimilation system) to use a cubed-sphere-based hydrodynamics. This versions of the dynamics scales to thousands of processes and has led to a decision to re-derive the TL and AD models for this more modern dynamics, thus taking advantage of a two-dimensional MPI decomposition and improved scalability properties. With the aid of the Transformation of Algorithms in FORTRAN (l'AF) automatic adjoint generation tool and some hand-coding, a version of the cubed-sphere-based TL and AD models, with a simplified vertical diffusion scheme, is now available, enabling multiple configurations of standard implementations of 4DV AR in GEOS. Concurrent to this development, collaboration with the National Centers for Environmental Prediction (NCEP) and the Earth System Research Laboratory (ESRL) has allowed GMAO to implement a hybrid-ensemble capability within the GEOS data assimilation system. Both 3Dand 4D-ensemble capabilities are presently available thus allowing

  12. Predicting lower mantle heterogeneity from 4-D Earth models

    Flament, Nicolas; Williams, Simon; Müller, Dietmar; Gurnis, Michael; Bower, Dan J.

    2016-04-01

    basal layer ˜ 4% denser than ambient mantle. Increasing convective vigour (Ra ≈ 5 x 108) or decreasing the density of the basal layer decreases both the accuracy and sensitivity of the predicted lower mantle structure. References: D. J. Bower, M. Gurnis, N. Flament, Assimilating lithosphere and slab history in 4-D Earth models. Phys. Earth Planet. Inter. 238, 8-22 (2015). V. Lekic, S. Cottaar, A. Dziewonski, B. Romanowicz, Cluster analysis of global lower mantle tomography: A new class of structure and implications for chemical heterogeneity. Earth Planet. Sci. Lett. 357, 68-77 (2012).

  13. Ultra-fast dynamics in atoms and molecules during photoionization: from attoseconds to femtoseconds

    Månsson, Erik

    2014-01-01

    Treating the correlated behaviour of multiple particles is challenging for both theory and experiment. This thesis reports on a variety of experimental investigations aiming to advance the understanding of fundamental processes in atoms and molecules: double ionization, isomerization and dissociation. The emphasis lies on ultra-fast processes, where multiple electrons interact or nuclei move so rapidly that coupling between electronic and nuclear dynamics can not be neglected. Pulses ...

  14. PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

    Kono, Junichiro

    2013-02-01

    Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton-phonon and exciton-plasmon interactions; exciton-exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz-Keldysh effects; and non-perturbative light-mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section, and the

  15. "Plasmonic Antennas as Design Elements for Coherent Ultrafast Nanophotonics"

    Brinks, D.; Castro-Lopez, M.; Hildner, R.; van Hulst, N. F.

    2013-01-01

    Coherent broadband excitation of plasmons brings ultrafast photonics to the nanoscale. However, to fully leverage this potential for ultrafast nanophotonic applications, the capacity to engineer and control the ultrafast response of a plasmonic system at will is crucial. Here, we develop a framework for systematic control and measurement of ultrafast dynamics of near-field hotspots. We show deterministic design of the coherent response of plasmonic antennas at femtosecond timescales. Exploiti...

  16. Unraveling the Solid-Liquid-Vapor Phase Transition Dynamics at the Atomic Level with Ultrafast X-Ray Absorption Near-Edge Spectroscopy

    X-ray absorption near-edge spectroscopy (XANES) is a powerful probe of electronic and atomic structures in various media, ranging from molecules to condensed matter. We show how ultrafast time resolution opens new possibilities to investigate highly nonequilibrium states of matter including phase transitions. Based on a tabletop laser-plasma ultrafast x-ray source, we have performed a time-resolved (∼3 ps) XANES experiment that reveals the evolution of an aluminum foil at the atomic level, when undergoing ultrafast laser heating and ablation. X-ray absorption spectra highlight an ultrafast transition from the crystalline solid to the disordered liquid followed by a progressive transition of the delocalized valence electronic structure (metal) down to localized atomic orbitals (nonmetal--vapor), as the average distance between atoms increases.

  17. 4+D TechnologyTM for nuclear systems soft solutions

    The signature in the proposal lies with the NSSS (Nuclear Systems Soft Solutions). NSSS proposed in the 3-dimensional space and time plus cost coordinates, i.e. 4+ dimensional technology, is the backbone of digital engineering in the nuclear system design and management. The NSSS is empowered by Janus (Junctional Analysis Neo dynamic Unit Soft Power), NOTUS (Neo systemic Optimization Technical Unit Soft Power), Venus (Virtual Engineering Neo cybernetic Unit Soft Power), EURUS (Engineering Utilities Research Unit Soft Power) and INUUS (Informative Neo graphic Utilities Unit Soft Power). Janus extracts the geometric data directly from the computer-aided design CAD files to import to multidimensional computational fluid and structural dynamics codes. Janus uses the joint-CAD analysis methods to eliminate the necessity of any pre- and post- processors. Starting from the 3-dimensional CAD, NOTUS contributes to reducing the construction cost of the nuclear power plants by optimizing the component manufacturing procedure and the plant construction process. Planning and scheduling construction projects can thus benefit greatly by integrating traditional management techniques with digital process simulation visualization. The 3-dimensional visualization of construction processes and resulting products intrinsically afford most of the advantages realized by the 4+D technology. Problems with equipment positioning and manpower congestion in certain areas can readily be visualized prior to the actual operation, thus preventing accidents and safety problems such as collision between two machines and losses in productivity. Venus applied the virtual reality technology in nuclear industry. Virtual reality provides an interactive real time motion with sound and tactile and other forms of feedback. The management and workers can thus comprehend the work process crystal clear by visualizing precisely how activities relate to one another, whereby reducing conflicting interpretations

  18. Genetic and phenotypic diversity of 2,4-dichlorophenoxyacetic acid (2,4-D)-degrading bacteria isolated from 2,4-D-treated field soils.

    Ka, J O; Holben, W E; Tiedje, J M

    1994-01-01

    Forty-seven numerically dominant 2,4-dichlorophenoxyacetic acid (2,4-D)-degrading bacteria were isolated at different times from 1989 through 1992 from eight agricultural plots (3.6 by 9.1 m) which were either not treated with 2,4-D or treated with 2,4-D at three different concentrations. Isolates were obtained from the most dilute positive most-probable-number tubes inoculated with soil samples from the different plots on seven sampling dates over the 3-year period. The isolates were compare...

  19. Targeted disruption of the heat shock protein 20–phosphodiesterase 4D (PDE4D interaction protects against pathological cardiac remodelling in a mouse model of hypertrophy

    Tamara P. Martin

    2014-01-01

    Full Text Available Phosphorylated heat shock protein 20 (HSP20 is cardioprotective. Using human induced pluripotent stem cell-derived cardiomyocytes (hiPSC-CMs and a mouse model of pressure overload mediated hypertrophy, we show that peptide disruption of the HSP20–phosphodiesterase 4D (PDE4D complex results in attenuation of action potential prolongation and protection against adverse cardiac remodelling. The later was evidenced by improved contractility, decreased heart weight to body weight ratio, and reduced interstitial and perivascular fibrosis. This study demonstrates that disruption of the specific HSP20–PDE4D interaction leads to attenuation of pathological cardiac remodelling.

  20. Ultrafast laser spectroscopy in complex solid state materials

    Li, Tianqi [Iowa State Univ., Ames, IA (United States)

    2014-12-01

    This thesis summarizes my work on applying the ultrafast laser spectroscopy to the complex solid state materials. It shows that the ultrafast laser pulse can coherently control the material properties in the femtosecond time scale. And the ultrafast laser spectroscopy can be employed as a dynamical method for revealing the fundamental physical problems in the complex material systems.

  1. Acquiring 4D thoracic CT scans using a multislice helical method

    Respiratory motion degrades anatomic position reproducibility during imaging, necessitates larger margins during radiotherapy planning and causes errors during radiation delivery. Computed tomography (CT) scans acquired synchronously with the respiratory signal can be used to reconstruct 4D CT scans, which can be employed for 4D treatment planning to explicitly account for respiratory motion. The aim of this research was to develop, test and clinically implement a method to acquire 4D thoracic CT scans using a multislice helical method. A commercial position-monitoring system used for respiratory-gated radiotherapy was interfaced with a third generation multislice scanner. 4D cardiac reconstruction methods were modified to allow 4D thoracic CT acquisition. The technique was tested on a phantom under different conditions: stationary, periodic motion and non-periodic motion. 4D CT was also implemented for a lung cancer patient with audio-visual breathing coaching. For all cases, 4D CT images were successfully acquired from eight discrete breathing phases, however, some limitations of the system in terms of respiration reproducibility and breathing period relative to scanner settings were evident. Lung mass for the 4D CT patient scan was reproducible to within 2.1% over the eight phases, though the lung volume changed by 20% between end inspiration and end expiration (870 cm3). 4D CT can be used for 4D radiotherapy, respiration-gated radiotherapy, 'slow' CT acquisition and tumour motion studies

  2. Initial validation of 4D-model for a clinical PET scanner using the Monte Carlo code gate

    Building exposure computational models (ECM) of emission tomography (PET and SPECT) currently has several dedicated computing tools based on Monte Carlo techniques (SimSET, SORTEO, SIMIND, GATE). This paper is divided into two steps: (1) using the dedicated code GATE (Geant4 Application for Tomographic Emission) to build a 4D model (where the fourth dimension is the time) of a clinical PET scanner from General Electric, GE ADVANCE, simulating the geometric and electronic structures suitable for this scanner, as well as some phenomena 4D, for example, rotating gantry; (2) the next step is to evaluate the performance of the model built here in the reproduction of test noise equivalent count rate (NEC) based on the NEMA Standards Publication NU protocols 2-2007 for this tomography. The results for steps (1) and (2) will be compared with experimental and theoretical values of the literature showing actual state of art of validation. (author)

  3. Initial validation of 4D-model for a clinical PET scanner using the Monte Carlo code gate

    Vieira, Igor F.; Lima, Fernando R.A.; Gomes, Marcelo S., E-mail: falima@cnen.gov.b [Centro Regional de Ciencias Nucleares do Nordeste (CRCN-NE/CNEN-PE), Recife, PE (Brazil); Vieira, Jose W.; Pacheco, Ludimila M. [Instituto Federal de Educacao, Ciencia e Tecnologia (IFPE), Recife, PE (Brazil); Chaves, Rosa M. [Instituto de Radium e Supervoltagem Ivo Roesler, Recife, PE (Brazil)

    2011-07-01

    Building exposure computational models (ECM) of emission tomography (PET and SPECT) currently has several dedicated computing tools based on Monte Carlo techniques (SimSET, SORTEO, SIMIND, GATE). This paper is divided into two steps: (1) using the dedicated code GATE (Geant4 Application for Tomographic Emission) to build a 4D model (where the fourth dimension is the time) of a clinical PET scanner from General Electric, GE ADVANCE, simulating the geometric and electronic structures suitable for this scanner, as well as some phenomena 4D, for example, rotating gantry; (2) the next step is to evaluate the performance of the model built here in the reproduction of test noise equivalent count rate (NEC) based on the NEMA Standards Publication NU protocols 2-2007 for this tomography. The results for steps (1) and (2) will be compared with experimental and theoretical values of the literature showing actual state of art of validation. (author)

  4. Geometric validation of self-gating k-space-sorted 4D-MRI vs 4D-CT using a respiratory motion phantom

    Yue, Yong, E-mail: yong.yue@cshs.org; Yang, Wensha; McKenzie, Elizabeth; Tuli, Richard; Wallace, Robert; Fraass, Benedick [Department of Radiation Oncology, Cedars-Sinai Medical Center, Los Angeles, California 90048 (United States); Fan, Zhaoyang; Pang, Jianing [Department of Biomedical Sciences, Biomedical Imaging Research Institute, Cedars-Sinai Medical Center, Los Angeles, California 90048 (United States); Deng, Zixin; Li, Debiao [Department of Biomedical Sciences, Biomedical Imaging Research Institute, Cedars-Sinai Medical Center, Los Angeles, California 90048 and Department of Bioengineering, University of California, Los Angeles, California 90095 (United States)

    2015-10-15

    Purpose: MRI is increasingly being used for radiotherapy planning, simulation, and in-treatment-room motion monitoring. To provide more detailed temporal and spatial MR data for these tasks, we have recently developed a novel self-gated (SG) MRI technique with advantage of k-space phase sorting, high isotropic spatial resolution, and high temporal resolution. The current work describes the validation of this 4D-MRI technique using a MRI- and CT-compatible respiratory motion phantom and comparison to 4D-CT. Methods: The 4D-MRI sequence is based on a spoiled gradient echo-based 3D projection reconstruction sequence with self-gating for 4D-MRI at 3 T. Respiratory phase is resolved by using SG k-space lines as the motion surrogate. 4D-MRI images are reconstructed into ten temporal bins with spatial resolution 1.56 × 1.56 × 1.56 mm{sup 3}. A MRI-CT compatible phantom was designed to validate the performance of the 4D-MRI sequence and 4D-CT imaging. A spherical target (diameter 23 mm, volume 6.37 ml) filled with high-concentration gadolinium (Gd) gel is embedded into a plastic box (35 × 40 × 63 mm{sup 3}) and stabilized with low-concentration Gd gel. The phantom, driven by an air pump, is able to produce human-type breathing patterns between 4 and 30 respiratory cycles/min. 4D-CT of the phantom has been acquired in cine mode, and reconstructed into ten phases with slice thickness 1.25 mm. The 4D images sets were imported into a treatment planning software for target contouring. The geometrical accuracy of the 4D MRI and CT images has been quantified using target volume, flattening, and eccentricity. The target motion was measured by tracking the centroids of the spheres in each individual phase. Motion ground-truth was obtained from input signals and real-time video recordings. Results: The dynamic phantom has been operated in four respiratory rate (RR) settings, 6, 10, 15, and 20/min, and was scanned with 4D-MRI and 4D-CT. 4D-CT images have target

  5. Ultrafast palladium diffusion in germanium

    Tahini, Hassan Ali

    2015-01-01

    The slow transport of dopants through crystal lattices has hindered the development of novel devices. Typically atoms are contained within deep potential energy wells which necessitates multiple attempts to hop between minimum energy positions. This is because the bonds that constrain atoms are strongest at the minimum positions. As they hop between sites the bonds must be broken, only to re-form as the atoms slide into adjacent minima. Here we demonstrate that the Pd atoms introduced into the Ge lattice behave differently. They retain bonds as the atoms shift across so that at the energy maximum between sites Pd still exhibits strong bonding characteristics. This reduces the energy maximum to almost nothing (a migration energy of only 0.03 eV) and means that the transport of Pd through the Ge lattice is ultrafast. We scrutinize the bonding characteristics at the atomic level using quantum mechanical simulation tools and demonstrate why Pd behaves so differently to other metals we investigated (i.e. Li, Cu, Ag, Pt and Au). Consequently, this fundamental understanding can be extended to systems where extremely rapid diffusion is desired, such as radiation sensors, batteries and solid oxide fuel cells.

  6. Reflectivity enhancement in titanium by ultrafast XUV irradiation.

    Bencivenga, F; Principi, E; Giangrisostomi, E; Cucini, R; Battistoni, A; D'Amico, F; Di Cicco, A; Di Fonzo, S; Filipponi, A; Gessini, A; Gunnella, R; Marsi, M; Properzi, L; Saito, M; Masciovecchio, C

    2014-01-01

    The study of highly photo-excited matter at solid state density is an emerging field of research, which is benefitting the development of free-electron-laser (FEL) technology. We report an extreme ultraviolet (XUV) reflectivity experiment from a titanium (Ti) sample irradiated with ultrafast seeded FEL pulses at variable incident photon fluence and frequency. Using a Drude formalism we relate the observed increase in reflectivity as a function of the excitation fluence to an increase in the plasma frequency, which allows us to estimate the free electron density in the excited sample. The extreme simplicity of the experimental setup makes the present approach potentially a valuable complementary tool to determine the average ionization state of the excited sample, information of primary relevance for understanding the physics of matter under extreme conditions. PMID:24824987

  7. Measurement of the ultrafast temporal response of a plasmonic antenna

    A measurement on the temporal response of a plasmonic antenna at the femtosecond time scale is reported. The antenna consists of a square array of nanometer-size gold rods. The far-field dispersion of light reflected from the plasmonic antenna is found to be less than that of a 1.2 mm thick glass slide. Assuming a simple oscillating dipole model this implies that the near-field of the antenna may be used as an electron switch that responds faster than 20 fs. Alternatively, ultrafast electron diffraction may be used to investigate the near-field dynamics of the plasmonic antenna. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  8. Ultrafast coherent optical control of a single diamond spin

    Bassett, L. C.; Heremans, F. J.; Awschalom, D. D.; Burkard, G.

    2013-03-01

    As an optically addressable solid-state electronic spin, the nitrogen-vacancy (NV) center in diamond has great promise for applications in quantum information science and metrology. At temperatures below ~ 10 K, the NV center's optical fine structure facilitates coherent coupling between the electronic spin and light, providing the means for all-optical spin control and other applications in quantum optics. Here, using ultrafast optical pump-probe techniques, we investigate the interplay of orbital, vibrational, and spin dynamics on timescales ranging from femtoseconds to nanoseconds. These techniques provide a flexible and powerful probe of orbital dynamics in the NV center's optically excited state, and enable optical spin control with sub-picosecond resolution. Work supported by AFOSR, ARO, and DARPA.

  9. A new model of Pde4d deficiency: genetic knock-down of PDE4D enzyme in rats produces an antidepressant phenotype without spatial cognitive effects.

    Schaefer, T L; Braun, A A; Amos-Kroohs, R M; Williams, M T; Ostertag, E; Vorhees, C V

    2012-07-01

    Phosphodiesterases (PDEs) are a superfamily of intracellular second messenger cyclic nucleotide hydrolyzing enzymes composed of 12 families. The Pde4 family has been implicated in depression and cognition, and PDE4 inhibitors have been evaluated as antidepressants and possible cognitive enhancers. Pde4d(-/-) mice show an antidepressant phenotype and learning enhancement on some tests, but not others as do mice treated with PDE4 inhibitors. Here, we report for the first time the behavioral phenotype of a new Pde4d knock-down (KD) rat model of PDE4D deficiency. Consistent with other data on PDE4D deficiency, Pde4d KD rats showed depression resistance in the Porsolt forced swim test and hyperreactivity of the acoustic startle response with no differential response on prepulse inhibition, suggesting no sensorimotor gating defect. Pde4d KD rats also exhibited a small exploratory activity reduction but no difference following habituation, and no enhanced spatial learning or reference memory in the Morris water maze. A selective improvement in route-based learning in the Cincinnati water maze was seen as well as enhanced contextual and cued fear conditioning and a more rapid rate of cued extinction from their higher freezing level that declined to wild-type (WT) levels only after ∼20 extinction trials. The rat model confirms Pde4d's role in depression but not in spatial learning or memory enhancement and shows for the first time higher fear conditioning and altered extinction compared with controls. The new model provides a tool by which to better understand the role of PDE4D in neuropsychiatric disorders and for the development of alternate treatment approaches. PMID:22487514

  10. Progress in ultrafast intense laser science IX

    Midorikawa, Katsumi

    2013-01-01

    The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance and attractions of the research topic at hand; these are followed by reports of cutting-edge discoveries. This ninth volume covers a broad range of topics from this interdisciplinary research field, focusing on ultrafast molecular responses to an intense laser field, advanced techniques for attosecond pulse generation, atomic and molecular responses to attosecond pulses, photoelectron spectroscopy of atoms and molecules...

  11. Ultrafast nonlocal control of spontaneous emission

    Jin, Chao-Yuan; Swinkels, Milo Y; Hoang, Thang B; Midolo, Leonardo; van Veldhoven, Peter J; Fiore, Andrea

    2013-01-01

    Solid-state cavity quantum electrodynamics systems will form scalable nodes of future quantum networks, allowing the storage, processing and retrieval of quantum bits, where a real-time control of the radiative interaction in the cavity is required to achieve high efficiency. We demonstrate here the dynamic molding of the vacuum field in a coupled-cavity system to achieve the ultrafast nonlocal modulation of spontaneous emission of quantum dots in photonic crystal cavities, on a timescale of ~200 ps, much faster than their natural radiative lifetimes. This opens the way to the ultrafast control of semiconductor-based cavity quantum electrodynamics systems for application in quantum interfaces and to a new class of ultrafast lasers based on nano-photonic cavities.

  12. High-energy attosecond nanoplasmonic-based electron gun

    Greig, S. R.; Elezzabi, A. Y.

    2016-03-01

    We present the design of an ultrafast conical lens based nanoplasmonic electron gun. Through excitation with a radially polarized laser pulse, and a combination of magnetostatic and spatial filtering, high energy electron packets with attosecond durations can be achieved.

  13. Analysis of the 4d9-(4d86p + 4p54d10) transitions of Sb VII and the strongest transitions of the 4d9-4d84f array of Sb VII and Te VIII

    The spectra of antimony and tellurium were photographed in the 100-200 A region on grazing incidence spectrographs at Moscow, Russia and NIST, U.S.A. laboratories. The 4d9-[4d86p + 4p54d10] transition array of Sb VII was analyzed. 31 levels in Sb VII were established. 41 new lines in Sb VII belonging to the 4d9-(4p54d10 + 4d86p) transition array have been classified. Seven lines each in Sb VII and Te VIII belonging to the 4d9-4d84f transition array have been classified. Parametric least-squares-fitted calculations involving configuration interaction have been carried out to interpret the spectrum satisfactorily. (orig.)

  14. 3D ultrafast ultrasound imaging in vivo

    Very high frame rate ultrasound imaging has recently allowed for the extension of the applications of echography to new fields of study such as the functional imaging of the brain, cardiac electrophysiology, and the quantitative imaging of the intrinsic mechanical properties of tumors, to name a few, non-invasively and in real time. In this study, we present the first implementation of Ultrafast Ultrasound Imaging in 3D based on the use of either diverging or plane waves emanating from a sparse virtual array located behind the probe. It achieves high contrast and resolution while maintaining imaging rates of thousands of volumes per second. A customized portable ultrasound system was developed to sample 1024 independent channels and to drive a 32  ×  32 matrix-array probe. Its ability to track in 3D transient phenomena occurring in the millisecond range within a single ultrafast acquisition was demonstrated for 3D Shear-Wave Imaging, 3D Ultrafast Doppler Imaging, and, finally, 3D Ultrafast combined Tissue and Flow Doppler Imaging. The propagation of shear waves was tracked in a phantom and used to characterize its stiffness. 3D Ultrafast Doppler was used to obtain 3D maps of Pulsed Doppler, Color Doppler, and Power Doppler quantities in a single acquisition and revealed, at thousands of volumes per second, the complex 3D flow patterns occurring in the ventricles of the human heart during an entire cardiac cycle, as well as the 3D in vivo interaction of blood flow and wall motion during the pulse wave in the carotid at the bifurcation. This study demonstrates the potential of 3D Ultrafast Ultrasound Imaging for the 3D mapping of stiffness, tissue motion, and flow in humans in vivo and promises new clinical applications of ultrasound with reduced intra—and inter-observer variability. (fast track communication)

  15. Unlocking the Constraints of Cyanobacterial Productivity: Acclimations Enabling Ultrafast Growth

    Bernstein, Hans C.; McClure, Ryan S.; Hill, Eric A.; Markillie, Lye Meng; Chrisler, William B.; Romine, Margaret F.; McDermott, Jason E.; Posewitz, Matthew C.; Bryant, Donald A.; Konopka, Allan; Fredrickson, Jim K.; Beliaev, Alex S.

    2016-07-26

    Harnessing the metabolic potential of photosynthetic microbes for next-generation biotechnology objectives requires detailed scientific understanding of the physiological constraints and regulatory controls affecting carbon partitioning between biomass, metabolite storage pools, and bioproduct synthesis. We dissected the cellular mechanisms underlying the remarkable physiological robustness of the euryhaline unicellular cyanobacterium Synechococcus sp. strain PCC 7002 (Synechococcus 7002) and identify key mechanisms that allow cyanobacteria to achieve unprecedented photoautotrophic productivities (~2.5-h doubling time). Ultrafast growth of Synechococcus 7002 was supported by high rates of photosynthetic electron transfer and linked to significantly elevated transcription of precursor biosynthesis and protein translation machinery. Notably, no growth or photosynthesis inhibition signatures were observed under any of the tested experimental conditions. Finally, the ultrafast growth in Synechococcus 7002 was also linked to a 300% expansion of average cell volume. We hypothesize that this cellular adaptation is required at high irradiances to support higher cell division rates and reduce deleterious effects, corresponding to high light, through increased carbon and reductant sequestration.

  16. Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics.

    Lejman, Mariusz; Vaudel, Gwenaelle; Infante, Ingrid C; Chaban, Ievgeniia; Pezeril, Thomas; Edely, Mathieu; Nataf, Guillaume F; Guennou, Mael; Kreisel, Jens; Gusev, Vitalyi E; Dkhil, Brahim; Ruello, Pascal

    2016-01-01

    The ability to generate efficient giga-terahertz coherent acoustic phonons with femtosecond laser makes acousto-optics a promising candidate for ultrafast light processing, which faces electronic device limits intrinsic to complementary metal oxide semiconductor technology. Modern acousto-optic devices, including optical mode conversion process between ordinary and extraordinary light waves (and vice versa), remain limited to the megahertz range. Here, using coherent acoustic waves generated at tens of gigahertz frequency by a femtosecond laser pulse, we reveal the mode conversion process and show its efficiency in ferroelectric materials such as BiFeO3 and LiNbO3. Further to the experimental evidence, we provide a complete theoretical support to this all-optical ultrafast mechanism mediated by acousto-optic interaction. By allowing the manipulation of light polarization with gigahertz coherent acoustic phonons, our results provide a novel route for the development of next-generation photonic-based devices and highlight new capabilities in using ferroelectrics in modern photonics. PMID:27492493

  17. Atomic origin of ultrafast resistance switching in nanoscale electrometallization cells

    Onofrio, Nicolas; Guzman, David; Strachan, Alejandro

    2015-04-01

    Nanoscale resistance-switching cells that operate via the electrochemical formation and disruption of metallic filaments that bridge two electrodes are among the most promising devices for post-CMOS electronics. Despite their importance, the mechanisms that govern their remarkable properties are not fully understood, especially for nanoscale devices operating at ultrafast rates, limiting our ability to assess the ultimate performance and scalability of this technology. We present the first atomistic simulations of the operation of conductive bridging cells using reactive molecular dynamics with a charge equilibration method extended to describe electrochemical reactions. The simulations predict the ultrafast switching observed in these devices, with timescales ranging from hundreds of picoseconds to a few nanoseconds for devices consisting of Cu active electrodes and amorphous silica dielectrics and with dimensions corresponding to their scaling limit (cross-sections below 10 nm). We find that single-atom-chain bridges often form during device operation but that they are metastable, with lifetimes below a nanosecond. The formation of stable filaments involves the aggregation of ions into small metallic clusters, followed by a progressive chemical reduction as they become connected to the cathode. Contrary to observations in larger cells, the nanoscale conductive bridges often lack crystalline order. An atomic-level mechanistic understanding of the switching process provides guidelines for materials optimization for such applications and the quantitative predictions over an ensemble of devices provide insight into their ultimate scaling and performance.

  18. Ultrafast multiphoton transient absorption of {beta}-carotene

    Buckup, Tiago [Philipps University Marburg, Department of Chemistry, D-35043 Marburg (Germany); Ruprecht-Karls University Heidelberg, Physical-Chemistry Institute, D-69120 (Germany); Weigel, Alexander; Hauer, Juergen [Philipps University Marburg, Department of Chemistry, D-35043 Marburg (Germany); Motzkus, Marcus, E-mail: Marcus.Motzkus@pci.uni-heidelberg.de [Philipps University Marburg, Department of Chemistry, D-35043 Marburg (Germany); Ruprecht-Karls University Heidelberg, Physical-Chemistry Institute, D-69120 (Germany)

    2010-07-19

    Multiphoton spectroscopy is able to directly excite electronic states, which are one-photon forbidden. Under single photon conditions, such one-photon forbidden states are exclusively populated via internal relaxation. Hence, transient absorption with two-photon excitation has the potential of clarifying complex relaxation networks by using aimed excitation. In this work we exploited ultrafast two-photon spectroscopy to investigate the excitation of dark states of {beta}-carotene in solution. After direct excitation of the vibronic manifold of S{sub 1}(2A{sub g}{sup -}) from S{sub 0} via two-photon transition, the characteristic internal conversion via hot-S{sub 1} {yields} S{sub 1} {yields} S{sub 0} was observed in the respective spectral region. Additional slow dynamics in the blue-wing of excited-state absorption (ESA) and in the NIR were detected, which is not directly observable with one-photon excitation transient absorption. These features are associated here to resonant multiphoton processes, which lead simultaneously to ultrafast intersystem crossing between singlet and triplet systems as well as to excitation of doublet states. Furthermore, we identify a 340-400 fs relaxation component in the near-infrared region after two-photon resonant excitation and discuss the role of additional dark states (3A{sub g}{sup -} and 1B{sub u}{sup -}) in this process.

  19. Time-based Spacing for 4D Approaches using Speed-Profiles

    De Jong, P.M.A.; De Vos, K.; Borst, C; Van Paassen, M.M.; de Mulder, M.

    2011-01-01

    Two of the major projects in ATM development, SESAR and NextGen, both fore- cast the use of 4D trajectories as an intermediate phase in the development of full Performance Based Trajectories. Using 4D trajectories, the full positional and time coordinates of the aircraft are known throughout the planned trajectory. During approach, when reduced separation minimums are applied, the accuracy of this profile is most important to ensure a safe approach to the runway. One implementation of 4D appr...

  20. Neuroimmune semaphorin 4D is necessary for optimal lung allergic inflammation.

    Shanks, K; Nkyimbeng-Takwi, E H; Smith, E; Lipsky, M M; DeTolla, L J; Scott, D W; Keegan, A D; Chapoval, S P

    2013-12-01

    Neuroimmune semaphorin 4D (Sema4D) was found to be expressed and function in the nervous and immune systems. In the immune system, Sema4D is constitutively expressed on T cells and regulates T cell priming. In addition, it displays a stimulatory function on macrophages, DC, NK cells, and neutrophils. As all these cells are deeply involved in asthma pathology, we hypothesized that Sema4D plays a critical non-redundant regulatory role in allergic airway response. To test our hypothesis, we exposed Sema4D(-/-) and WT mice to OVA injections and challenges in the well-defined mouse model of OVA-induced experimental asthma. We observed a significant decrease in eosinophilic airway infiltration in allergen-treated Sema4D(-/-) mice relative to WT mice. This reduced allergic inflammatory response was associated with decreased BAL IL-5, IL-13, TGFβ1, IL-6, and IL-17A levels. In addition, T cell proliferation in OVA₃₂₃₋₃₃₉-restimulated Sema4D(-/-) cell cultures was downregulated. We also found increased Treg numbers in spleens of Sema4D(-/-) mice. However, airway hyperreactivity (AHR) to methacholine challenges was not affected by Sema4D deficiency in either acute or chronic experimental disease setting. Surprisingly, lung DC number and activation were not affected by Sema4D deficiency. These data provide a new insight into Sema4D biology and define Sema4D as an important regulator of Th2-driven lung pathophysiology and as a potential target for a combinatory disease immunotherapy. PMID:23911404