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Sample records for 4d ultrafast electron

  1. Ordered water structure at hydrophobic graphite interfaces observed by 4D, ultrafast electron crystallography

    Science.gov (United States)

    Yang, Ding-Shyue; Zewail, Ahmed H.

    2009-01-01

    Interfacial water has unique properties in various functions. Here, using 4-dimensional (4D), ultrafast electron crystallography with atomic-scale spatial and temporal resolution, we report study of structure and dynamics of interfacial water assembly on a hydrophobic surface. Structurally, vertically stacked bilayers on highly oriented pyrolytic graphite surface were determined to be ordered, contrary to the expectation that the strong hydrogen bonding of water on hydrophobic surfaces would dominate with suppressed interfacial order. Because of its terrace morphology, graphite plays the role of a template. The dynamics is also surprising. After the excitation of graphite by an ultrafast infrared pulse, the interfacial ice structure undergoes nonequilibrium “phase transformation” identified in the hydrogen-bond network through the observation of structural isosbestic point. We provide the time scales involved, the nature of ice-graphite structural dynamics, and relevance to properties related to confined water. PMID:19246378

  2. 4D scanning transmission ultrafast electron microscopy: Single-particle imaging and spectroscopy.

    Science.gov (United States)

    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.

  3. 4D scanning ultrafast electron microscopy: visualization of materials surface dynamics.

    Science.gov (United States)

    Mohammed, Omar F; Yang, Ding-Shyue; Pal, Samir Kumar; Zewail, Ahmed H

    2011-05-25

    The continuous electron beam of conventional scanning electron microscopes (SEM) limits the temporal resolution required for the study of ultrafast dynamics of materials surfaces. Here, we report the development of scanning ultrafast electron microscopy (S-UEM) as a time-resolved method with resolutions in both space and time. The approach is demonstrated in the investigation of the dynamics of semiconducting and metallic materials visualized using secondary-electron images and backscattering electron diffraction patterns. For probing, the electron packet was photogenerated from the sharp field-emitter tip of the microscope with a very low number of electrons in order to suppress space-charge repulsion between electrons and reach the ultrashort temporal resolution, an improvement of orders of magnitude when compared to the traditional beam-blanking method. Moreover, the spatial resolution of SEM is maintained, thus enabling spatiotemporal visualization of surface dynamics following the initiation of change by femtosecond heating or excitation. We discuss capabilities and potential applications of S-UEM in materials and biological science.

  4. 4D Electron Tomography

    Science.gov (United States)

    Kwon, Oh-Hoon; Zewail, Ahmed H.

    2010-06-01

    Electron tomography provides three-dimensional (3D) imaging of noncrystalline and crystalline equilibrium structures, as well as elemental volume composition, of materials and biological specimens, including those of viruses and cells. We report the development of 4D electron tomography by integrating the fourth dimension (time resolution) with the 3D spatial resolution obtained from a complete tilt series of 2D projections of an object. The different time frames of tomograms constitute a movie of the object in motion, thus enabling studies of nonequilibrium structures and transient processes. The method was demonstrated using carbon nanotubes of a bracelet-like ring structure for which 4D tomograms display different modes of motion, such as breathing and wiggling, with resonance frequencies up to 30 megahertz. Applications can now make use of the full space-time range with the nanometer-femtosecond resolution of ultrafast electron tomography.

  5. 4D Electron Tomography

    OpenAIRE

    Kwon, Oh-Hoon; Zewail, Ahmed H.

    2010-01-01

    Electron tomography provides three-dimensional (3D) imaging of noncrystalline and crystalline equilibrium structures, as well as elemental volume composition, of materials and biological specimens, including those of viruses and cells. We report the development of 4D electron tomography by integrating the fourth dimension (time resolution) with the 3D spatial resolution obtained from a complete tilt series of 2D projections of an object. The different time frames of tomograms constitute a mov...

  6. Scanning ultrafast electron microscopy.

    Science.gov (United States)

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

    2010-08-24

    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 which the pulse contains at most one or a few electrons, thus achieving imaging without the space-charge effect between electrons, and still in ten(s) of seconds. For imaging, the secondary electrons from surface structures are detected, as demonstrated here for material surfaces and biological specimens. By recording backscattered electrons, diffraction patterns from single crystals were also obtained. Scanning pulsed-electron microscopy with the acquired spatiotemporal resolutions, and its efficient heat-dissipation feature, is now poised to provide in situ 4D imaging and with environmental capability.

  7. Scanning ultrafast electron microscopy

    Science.gov (United States)

    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 which the pulse contains at most one or a few electrons, thus achieving imaging without the space-charge effect between electrons, and still in ten(s) of seconds. For imaging, the secondary electrons from surface structures are detected, as demonstrated here for material surfaces and biological specimens. By recording backscattered electrons, diffraction patterns from single crystals were also obtained. Scanning pulsed-electron microscopy with the acquired spatiotemporal resolutions, and its efficient heat-dissipation feature, is now poised to provide in situ 4D imaging and with environmental capability. PMID:20696933

  8. 4D electron microscopy: principles and applications.

    Science.gov (United States)

    Flannigan, David J; Zewail, Ahmed H

    2012-10-16

    achievable with short intense pulses containing a large number of electrons, however, are limited to tens of nanometers and nanoseconds, respectively. This is because Coulomb repulsion is significant in such a pulse, and the electrons spread in space and time, thus limiting the beam coherence. It is therefore not possible to image the ultrafast elementary dynamics of complex transformations. The challenge was to retain the high spatial resolution of a conventional TEM while simultaneously enabling the temporal resolution required to visualize atomic-scale motions. In this Account, we discuss the development of four-dimensional ultrafast electron microscopy (4D UEM) and summarize techniques and applications that illustrate the power of the approach. In UEM, images are obtained either stroboscopically with coherent single-electron packets or with a single electron bunch. Coulomb repulsion is absent under the single-electron condition, thus permitting imaging, diffraction, and spectroscopy, all with high spatiotemporal resolution, the atomic scale (sub-nanometer and femtosecond). The time resolution is limited only by the laser pulse duration and energy carried by the electron packets; the CCD camera has no bearing on the temporal resolution. In the regime of single pulses of electrons, the temporal resolution of picoseconds can be attained when hundreds of electrons are in the bunch. The applications given here are selected to highlight phenomena of different length and time scales, from atomic motions during structural dynamics to phase transitions and nanomechanical oscillations. We conclude with a brief discussion of emerging methods, which include scanning ultrafast electron microscopy (S-UEM), scanning transmission ultrafast electron microscopy (ST-UEM) with convergent beams, and time-resolved imaging of biological structures at ambient conditions with environmental cells.

  9. Four-dimensional ultrafast electron microscopy.

    Science.gov (United States)

    Lobastov, Vladimir A; Srinivasan, Ramesh; Zewail, Ahmed H

    2005-05-17

    Electron microscopy is arguably the most powerful tool for spatial imaging of structures. As such, 2D and 3D microscopies provide static structures with subnanometer and increasingly with angstrom-scale spatial resolution. Here we report the development of 4D ultrafast electron microscopy, whose capability imparts another dimension to imaging in general and to dynamics in particular. We demonstrate its versatility by recording images and diffraction patterns of crystalline and amorphous materials and images of biological cells. The electron packets, which were generated with femtosecond laser pulses, have a de Broglie wavelength of 0.0335 angstroms at 120 keV and have as low as one electron per pulse. With such few particles, doses of few electrons per square ångstrom, and ultrafast temporal duration, the long sought after but hitherto unrealized quest for ultrafast electron microscopy has been realized. Ultrafast electron microscopy should have an impact on all areas of microscopy, including biological imaging.

  10. Ultra-Fast Silicon Detectors for 4D tracking

    Science.gov (United States)

    Sola, V.; Arcidiacono, R.; Bellora, A.; Cartiglia, N.; Cenna, F.; Cirio, R.; Durando, S.; Ferrero, M.; Galloway, Z.; Gruey, B.; Freeman, P.; Mashayekhi, M.; Mandurrino, M.; Monaco, V.; Mulargia, R.; Obertino, M. M.; Ravera, F.; Sacchi, R.; Sadrozinski, H. F.-W.; Seiden, A.; Spencer, N.; Staiano, A.; Wilder, M.; Woods, N.; Zatserklyaniy, A.

    2017-02-01

    We review the progress toward the development of a novel type of silicon detectors suited for tracking with a picosecond timing resolution, the so called Ultra-Fast Silicon Detectors. The goal is to create a new family of particle detectors merging excellent position and timing resolution with GHz counting capabilities, very low material budget, radiation resistance, fine granularity, low power, insensitivity to magnetic field, and affordability. We aim to achieve concurrent precisions of ~ 10 ps and ~ 10 μm with a 50 μm thick sensor. Ultra-Fast Silicon Detectors are based on the concept of Low-Gain Avalanche Detectors, which are silicon detectors with an internal multiplication mechanism so that they generate a signal which is factor ~ 10 larger than standard silicon detectors.

  11. Ultrafast Science Opportunities with Electron Microscopy

    Energy Technology Data Exchange (ETDEWEB)

    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.

  12. Ultrafast dynamics of correlated electrons

    Energy Technology Data Exchange (ETDEWEB)

    Rettig, Laurenz

    2012-07-09

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

  13. 4D ultrafast ultrasound flow imaging: in vivo quantification of arterial volumetric flow rate in a single heartbeat

    Science.gov (United States)

    Correia, Mafalda; Provost, Jean; Tanter, Mickael; Pernot, Mathieu

    2016-12-01

    We present herein 4D ultrafast ultrasound flow imaging, a novel ultrasound-based volumetric imaging technique for the quantitative mapping of blood flow. Complete volumetric blood flow distribution imaging was achieved through 2D tilted plane-wave insonification, 2D multi-angle cross-beam beamforming, and 3D vector Doppler velocity components estimation by least-squares fitting. 4D ultrafast ultrasound flow imaging was performed in large volumetric fields of view at very high volume rate (>4000 volumes s-1) using a 1024-channel 4D ultrafast ultrasound scanner and a 2D matrix-array transducer. The precision of the technique was evaluated in vitro by using 3D velocity vector maps to estimate volumetric flow rates in a vessel phantom. Volumetric Flow rate errors of less than 5% were found when volumetric flow rates and peak velocities were respectively less than 360 ml min-1 and 100 cm s-1. The average volumetric flow rate error increased to 18.3% when volumetric flow rates and peak velocities were up to 490 ml min-1 and 1.3 m s-1, respectively. The in vivo feasibility of the technique was shown in the carotid arteries of two healthy volunteers. The 3D blood flow velocity distribution was assessed during one cardiac cycle in a full volume and it was used to quantify volumetric flow rates (375  ±  57 ml min-1 and 275  ±  43 ml min-1). Finally, the formation of 3D vortices at the carotid artery bifurcation was imaged at high volume rates.

  14. Development of Scanning Ultrafast Electron Microscope Capability.

    Energy Technology Data Exchange (ETDEWEB)

    Collins, Kimberlee Chiyoko [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Talin, Albert Alec [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Chandler, David W. [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Michael, Joseph R. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2016-11-01

    Modern semiconductor devices rely on the transport of minority charge carriers. Direct examination of minority carrier lifetimes in real devices with nanometer-scale features requires a measurement method with simultaneously high spatial and temporal resolutions. Achieving nanometer spatial resolutions at sub-nanosecond temporal resolution is possible with pump-probe methods that utilize electrons as probes. Recently, a stroboscopic scanning electron microscope was developed at Caltech, and used to study carrier transport across a Si p-n junction [ 1 , 2 , 3 ] . In this report, we detail our development of a prototype scanning ultrafast electron microscope system at Sandia National Laboratories based on the original Caltech design. This effort represents Sandia's first exploration into ultrafast electron microscopy.

  15. Ultrafast Time-Resolved Electron Diffraction with Megavolt Electron Beams

    Energy Technology Data Exchange (ETDEWEB)

    Hastings, J.B.; /SLAC; Rudakov, F.M.; /Brown U.; Dowell, D.H.; Schmerge, J.F.; /SLAC; Cardoza, J.D.; /Brown U.; Castro, J.M.; Gierman, S.M.; Loos, H.; /SLAC; Weber, P.M.; /Brown U.

    2006-10-24

    An rf photocathode electron gun is used as an electron source for ultrafast time-resolved pump-probe electron diffraction. We observed single-shot diffraction patterns from a 160 nm Al foil using the 5.4 MeV electron beam from the Gun Test Facility at the Stanford Linear Accelerator. Excellent agreement with simulations suggests that single-shot diffraction experiments with a time resolution approaching 100 fs are possible.

  16. Effects of electronic coherence in ultrafast spectroscopy

    Science.gov (United States)

    Bennett, Kochise

    Electronic dynamics takes place at the attosecond timescale. Recent technological advancements permit the creation of light pulses with durations in the attosecond regime, opening up the possibility of monitoring this ultrafast dynamics in real time. In particular, it becomes possible to observe the time-dependent interference between material electronic states, thus tracking the electronic energies temporally. This information, originating in the coherence terms in the electronic density matrix, can provide spectral information in the time-domain. Such an approach is particularly useful when the desired information is transient. In this thesis, we examine how electronic coherences contribute to photoelectron and a variety of x-ray Raman signals. We then utilize photoelectron spectroscopy and linear off-resonant Raman (TRUECARS) to track the dynamics of a model system by way of example.

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

    KAUST Repository

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.)

  19. Ultrafast Electron Dynamics in Solar Energy Conversion.

    Science.gov (United States)

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

    2017-08-23

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

  20. Ultrafast electron dynamics in gold nanoshells

    Science.gov (United States)

    Westcott, Sarah Linda

    2001-10-01

    In metallic nanostructures, the interaction of excited electrons with the nanostructure surface may result in electron relaxation dynamics that are significantly different than those predicted by electron-lattice coupling. These ultrafast electron dynamics were monitored by pump-probe measurements of the time-resolved change in transmission. Using femtosecond pulses from a cavity-dumped titanium-doped sapphire laser, two types of nanoparticles with a core-shell geometry were studied. Nanoshells are nanoparticles with a dielectric core surrounded by a continuous thin metal shell. For nanoshells, the plasmon resonance wavelength is tunable by changing the core and shell dimensions. For nanoshells with a gold sulfide core and a gold shell, two conditions were observed under which electron relaxation was different than predicted by electron-phonon coupling. First, electron relaxation occurred more rapidly for gold-gold sulfide nanoshells embedded in polymer films than for nanoshells dispersed in water, with lifetimes of 1.6 ps and 3 to 5 ps, respectively. Second, for nanoshells dispersed in water, the electron relaxation lifetime decreased with adsorption of p-aminobenzoic acid (to 1.7 ps) or aniline (to 1.9 ps) on the nanoshells. With adsorbed n-propylamine or p-mercaptobenzoic acid, electron relaxation transpired in 2.8 ps or 2.4 ps, respectively. Density functional theory calculations indicated that the molecules leading to the fastest electron relaxation possessed the largest induced dipole moments near a metal surface. Semicontinuous gold films grown around a silica nanoparticle core exhibited spectral and dynamical optical signatures of the percolation threshold. Compared to continuous shells, the electron dynamics in the semicontinuous shell layer were dramatically different as additional induced bleaching was observed in the first 500 fs. The observed dynamics are consistent with a rate equation model in which the electrons are initially excited in localized

  1. Ultrafast Imaging of Electronic Motion in Atoms and Molecules

    Science.gov (United States)

    2016-01-12

    AFRL-AFOSR-VA-TR-2016-0045 Ultrafast Imaging of Electronic Motion in Atoms and Molecules Martin Centurion UNIVERSITY OF NEBRSKA Final Report 01/12...Ultrafast Imaging of Electronic Motion in Atoms and Molecules 5a. CONTRACT NUMBER 5b. GRANT NUMBER FA9550-12-1-0149 5c. PROGRAM ELEMENT NUMBER 6...a gaseous target of atoms or molecules . An optical setup was designed and constructed to compensate for the blurring of the temporal resolution due

  2. Four-Dimensional Ultrafast Electron Microscopy: Insights into an Emerging Technique

    KAUST Repository

    Adhikari, Aniruddha

    2016-12-15

    Four-dimensional ultrafast electron microscopy (4D-UEM) is a novel analytical technique that aims to fulfill the long-held dream of researchers to investigate materials at extremely short spatial and temporal resolutions by integrating the excellent spatial resolution of electron microscopes with the temporal resolution of ultrafast femtosecond laser-based spectroscopy. The ingenious use of pulsed photoelectrons to probe surfaces and volumes of materials enables time-resolved snapshots of the dynamics to be captured in a way hitherto impossible by other conventional techniques. The flexibility of 4D-UEM lies in the fact that it can be used in both the scanning (S-UEM) and transmission (UEM) modes depending upon the type of electron microscope involved. While UEM can be employed to monitor elementary structural changes and phase transitions in samples using real-space mapping, diffraction, electron energy-loss spectroscopy, and tomography, S-UEM is well suited to map ultrafast dynamical events on materials surfaces in space and time. This review provides an overview of the unique features that distinguish these techniques and also illustrates the applications of both S-UEM and UEM to a multitude of problems relevant to materials science and chemistry.

  3. Four-Dimensional Ultrafast Electron Microscopy: Insights into an Emerging Technique.

    Science.gov (United States)

    Adhikari, Aniruddha; Eliason, Jeffrey K; Sun, Jingya; Bose, Riya; Flannigan, David J; Mohammed, Omar F

    2017-01-11

    Four-dimensional ultrafast electron microscopy (4D-UEM) is a novel analytical technique that aims to fulfill the long-held dream of researchers to investigate materials at extremely short spatial and temporal resolutions by integrating the excellent spatial resolution of electron microscopes with the temporal resolution of ultrafast femtosecond laser-based spectroscopy. The ingenious use of pulsed photoelectrons to probe surfaces and volumes of materials enables time-resolved snapshots of the dynamics to be captured in a way hitherto impossible by other conventional techniques. The flexibility of 4D-UEM lies in the fact that it can be used in both the scanning (S-UEM) and transmission (UEM) modes depending upon the type of electron microscope involved. While UEM can be employed to monitor elementary structural changes and phase transitions in samples using real-space mapping, diffraction, electron energy-loss spectroscopy, and tomography, S-UEM is well suited to map ultrafast dynamical events on materials surfaces in space and time. This review provides an overview of the unique features that distinguish these techniques and also illustrates the applications of both S-UEM and UEM to a multitude of problems relevant to materials science and chemistry.

  4. Ultrafast electron transport in graphene and magnetic nanostructures

    Science.gov (United States)

    Turchinovich, Dmitry

    2016-03-01

    Ultrafast terahertz spectroscopy is an ideal tool for observation of dynamics of charge, lattice and spin in solids on the most elementary timescale: in the regime ωτ ~ 1, where ω is the electromagnetic wave oscillation frequency, and τ is the characteristic timescale at which the fundamental phenomena in the three subsystems comprising the solid occur. In this paper two case studies will be discussed. (i) Ultrafast electron transport in graphene. We will show, that the free-carrier conductivity of graphene in arbitrary ultrafast, (sub-)picosecond electric fields is defined by the thermodynamic balance maintained within the electronic structure of graphene acting as thermalized electron gas. Within this simple thermodynamic picture, the electron gas quasi-instantaneously increases its temperature by absorbing the energy of driving ultrafast electric field, and at the same time cools down via a time-retarded, few picosecond-long process of phonon emission. The asymmetry in electron heating and cooling dynamics leads to heat accumulation in the electron population of graphene, concomitantly lowering the chemical potential for hotter electrons, and thereby reducing the intraband conductivity of graphene - an effect crucially important for understanding of ultrafast graphene transistors and photodetectors. (ii) We will also discuss the fundamental observation of spin-controlled electron conduction of Fermilevel electrons in ferromagnetic metals, and will directly quantify the Mott picture of conduction in ferromagnets - the effect directly employed in modern magnetic sensor technologies such as giant magnetoresistance.

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

    Directory of Open Access Journals (Sweden)

    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.

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

    Directory of Open Access Journals (Sweden)

    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. Development of an ultrafast electron source based on a cold-field emission gun for ultrafast coherent TEM

    Science.gov (United States)

    Caruso, Giuseppe Mario; Houdellier, Florent; Abeilhou, Pierre; Arbouet, Arnaud

    2017-07-01

    We report on the design of a femtosecond laser-driven electron source for ultrafast coherent transmission electron microscopy. The proposed architecture allows introducing an ultrafast laser beam inside the cold field emission source of a commercial TEM, aligning and focusing the laser spot on the apex of the nanoemitter. The modifications of the gun assembly do not deteriorate the performances of the electron source in conventional DC mode and allow easy switching between the conventional and ultrafast laser-driven emission modes. We describe here this ultrafast electron source and discuss its properties.

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

    KAUST Repository

    Shaheen, Basamat

    2017-05-17

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

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

    Directory of Open Access Journals (Sweden)

    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.

  10. Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses

    Science.gov (United States)

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

    2014-10-01

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

  11. Investigations of ultrafast dynamics in electronically excited alkylbenzenes

    Directory of Open Access Journals (Sweden)

    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. Structural preablation dynamics of graphite observed by ultrafast electron crystallography

    NARCIS (Netherlands)

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

    2008-01-01

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

  13. Photon gating in four-dimensional ultrafast electron microscopy.

    Science.gov (United States)

    Hassan, Mohammed T; Liu, Haihua; Baskin, John Spencer; Zewail, Ahmed H

    2015-10-20

    Ultrafast electron microscopy (UEM) is a pivotal tool for imaging of nanoscale structural dynamics with subparticle resolution on the time scale of atomic motion. Photon-induced near-field electron microscopy (PINEM), a key UEM technique, involves the detection of electrons that have gained energy from a femtosecond optical pulse via photon-electron coupling on nanostructures. PINEM has been applied in various fields of study, from materials science to biological imaging, exploiting the unique spatial, energy, and temporal characteristics of the PINEM electrons gained by interaction with a "single" light pulse. The further potential of photon-gated PINEM electrons in probing ultrafast dynamics of matter and the optical gating of electrons by invoking a "second" optical pulse has previously been proposed and examined theoretically in our group. Here, we experimentally demonstrate this photon-gating technique, and, through diffraction, visualize the phase transition dynamics in vanadium dioxide nanoparticles. With optical gating of PINEM electrons, imaging temporal resolution was improved by a factor of 3 or better, being limited only by the optical pulse widths. This work enables the combination of the high spatial resolution of electron microscopy and the ultrafast temporal response of the optical pulses, which provides a promising approach to attain the resolution of few femtoseconds and attoseconds in UEM.

  14. Dynamic diffraction effects and coherent breathing oscillations in ultrafast electron diffraction in layered 1T-TaSeTe

    Directory of Open Access Journals (Sweden)

    Linlin Wei

    2017-07-01

    Full Text Available Anisotropic lattice movements due to the difference between intralayer and interlayer bonding are observed in the layered transition-metal dichalcogenide 1T-TaSeTe following femtosecond laser pulse excitation. Our ultrafast electron diffraction investigations using 4D-transmission electron microscopy (4D-TEM clearly reveal that the intensity of Bragg reflection spots often changes remarkably due to the dynamic diffraction effects and anisotropic lattice movement. Importantly, the temporal diffracted intensity from a specific crystallographic plane depends on the deviation parameter s, which is commonly used in the theoretical study of diffraction intensity. Herein, we report on lattice thermalization and structural oscillations in layered 1T-TaSeTe, analyzed by dynamic diffraction theory. Ultrafast alterations of satellite spots arising from the charge density wave in the present system are also briefly discussed.

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

    Science.gov (United States)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  17. Ultrafast electron transport across nano gaps in nanowire circuits

    Energy Technology Data Exchange (ETDEWEB)

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

    KAUST Repository

    Khan, Jafar Iqbal

    2016-03-03

    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. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

    Science.gov (United States)

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

    2017-09-01

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

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

    CERN Document Server

    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

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

    Energy Technology Data Exchange (ETDEWEB)

    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 Photoinduced Electron Transfer from Peroxide Dianion.

    Science.gov (United States)

    Anderson, Bryce L; Maher, Andrew G; Nava, Matthew; Lopez, Nazario; Cummins, Christopher C; Nocera, Daniel G

    2015-06-18

    The encapsulation of peroxide dianion by hexacarboxamide cryptand provides a platform for the study of electron transfer of isolated peroxide anion. Photoinitiated electron transfer (ET) between freely diffusing Ru(bpy)3(2+) and the peroxide dianion occurs with a rate constant of 2.0 × 10(10) M(-1) s(-1). A competing electron transfer quenching pathway is observed within an ion pair. Picosecond transient spectroscopy furnishes a rate constant of 1.1 × 10(10) s(-1) for this first-order process. A driving force dependence for the ET rate within the ion pair using a series of Ru(bpy)3(2+) derivatives allows for the electronic coupling and reorganization energies to be assessed. The ET reaction is nonadiabatic and dominated by a large inner-sphere reorganization energy, in accordance with that expected for the change in bond distance accompanying the conversion of peroxide dianion to superoxide anion.

  3. Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Luo, Liang [Iowa State Univ., Ames, IA (United States)

    2015-01-01

    This thesis summarizes my work on using ultrafast laser pulses to study Terahertz (THz) electrodynamics of photonic and electronic nanostructures and microstructures. Ultrafast timeresolved (optical, NIR, MIR, THz) pump-probe spectroscopy setup has been successfully built, which enables me to perform a series of relevant experiments. Firstly, a novel high e ciency and compact THz wave emitter based on split-ring-resonators has been developed and characterized. The emitter can be pumped at any wavelength by tailoring the magnetic resonance and could generate gapless THz waves covering the entire THz band. Secondly, two kinds of new photonic structures for THz wave manipulation have been successfully designed and characterized. One is based on the 1D and 2D photo-imprinted di ractive elements. The other is based on the photoexcited double-split-ring-resonator metamaterials. Both structures are exible and can modulate THz waves with large tunability. Thirdly, the dark excitons in semiconducting singlewalled carbon nanotubes are studied by optical pump and THz probe spectroscopy, which provides the rst insights into the THz responses of nonequilibrium excitonic correlations and dynamics from the dark ground states in carbon nanotubes. Next, several on-going projects are brie y presented such as the study of ultrafast THz dynamics of Dirac fermions in topological insulator Bi2Se3 with Mid-infrared excitation. Finally, the thesis ends with a summary of the completed experiments and an outlook of the future plan.

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

    KAUST Repository

    Sun, Jingya

    2016-02-25

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

  5. Ultrafast dynamics of electrons at interfaces

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-05-03

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

  6. Structural determination and electronic properties of the 4d perovskite SrPdO3

    Science.gov (United States)

    He, Jiangang; Franchini, Cesare

    2014-01-01

    The structure and ground state electronic structure of the recently synthesized SrPdO3 perovskite [A. Galal et al. J. Power Sources 195, 3806 (2010), 10.1016/j.jpowsour.2009.12.091] have been studied by means of screened hybrid functional and the GW approximation with the inclusion of electron-hole interaction within the test-charge/test-charge scheme. By conducting a structural search based on lattice dynamics and group theoretical method we identify the orthorhombic phase with Pnma space group as the most stable crystal structure. The phase transition from the ideal cubic perovskite structure to the Pnma one is explained in terms of the simultaneous stabilization of the antiferrodistortive phonon modes R4+ and M3+. Our results indicate that SrPdO3 exhibits an insulating ground state, substantiated by a GW0 gap of about 1.1 eV. Spin polarized calculations suggest that SrPdO3 adopts a low spin state (t2g↑↓↑↓↑↓eg0), and is expected to exhibit spin excitations and spin state crossovers at finite temperature, analogous to the case of 3d isoelectronic LaCoO3. This would provide another playground for the study of spin state transitions in 4d oxides and an opportunity to design multifunctional materials based on the 4d Pnma building block.

  7. Adapting High Brightness Relativistic Electron Beams for Ultrafast Science

    Science.gov (United States)

    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. Probing Transient Electron Dynamics Using Ultrafast X Rays

    Science.gov (United States)

    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.

  9. Direct observation of the ultrafast electron transfer process in a polymer/fullerene blend

    NARCIS (Netherlands)

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

    2000-01-01

    Photoinduced electron transfer in organic molecules is an extensively investigated topic both because of fundamental interest in the photophysics and for applications to artificial photosynthesis. Highly efficient ultrafast electron transfer from photoexcited conjugated polymers to C60 has been

  10. Ultrafast modulation of electronic structure by coherent phonon excitations

    Science.gov (United States)

    Weisshaupt, J.; Rouzée, A.; Woerner, M.; Vrakking, M. J. J.; Elsaesser, T.; Shirley, E. L.; Borgschulte, A.

    2017-02-01

    Femtosecond x-ray absorption spectroscopy with a laser-driven high-harmonic source is used to map ultrafast changes of x-ray absorption by femtometer-scale coherent phonon displacements. In LiBH4, displacements along an Ag phonon mode at 10 THz are induced by impulsive Raman excitation and give rise to oscillatory changes of x-ray absorption at the Li K edge. Electron density maps from femtosecond x-ray diffraction data show that the electric field of the pump pulse induces a charge transfer from the BH4- to neighboring Li+ ions, resulting in a differential Coulomb force that drives lattice vibrations in this virtual transition state.

  11. Ultrafast Photoinduced Electron Transfer in Bimolecular Donor-Acceptor Systems

    KAUST Repository

    Alsulami, Qana A.

    2016-11-30

    The efficiency of photoconversion systems, such as organic photovoltaic (OPV) cells, is largely controlled by a series of fundamental photophysical processes occurring at the interface before carrier collection. A profound understanding of ultrafast interfacial charge transfer (CT), charge separation (CS), and charge recombination (CR) is the key determinant to improving the overall performances of photovoltaic devices. The discussion in this dissertation primarily focuses on the relevant parameters that are involved in photon absorption, exciton separation, carrier transport, carrier recombination and carrier collection in organic photovoltaic devices. A combination of steady-state and femtosecond broadband transient spectroscopies was used to investigate the photoinduced charge carrier dynamics in various donor-acceptor systems. Furthermore, this study was extended to investigate some important factors that influence charge transfer in donor-acceptor systems, such as the morphology, energy band alignment, electronic properties and chemical structure. Interestingly, clear correlations among the steady-state measurements, time-resolved spectroscopy results, grain alignment of the electron transporting layer (ETL), carrier mobility, and device performance are found. In this thesis, we explored the significant impacts of ultrafast charge separation and charge recombination at donor/acceptor (D/A) interfaces on the performance of a conjugated polymer PTB7-Th device with three fullerene acceptors: PC71BM, PC61BM and IC60BA. Time-resolved laser spectroscopy and high-resolution electron microscopy can illustrate the basis for fabricating solar cell devices with improved performances. In addition, we studied the effects of the incorporation of heavy metals into π-conjugated chromophores on electron transfer by monitoring the triplet state lifetime of the oligomer using transient absorption spectroscopy, as understanding the mechanisms controlling intersystem crossing and

  12. Ultrafast transmission electron microscopy using a laser-driven field emitter: femtosecond resolution with a high coherence electron beam

    CERN Document Server

    Feist, Armin; da Silva, Nara Rubiano; Danz, Thomas; Möller, Marcel; Priebe, Katharina E; Domröse, Till; Gatzmann, J Gregor; Rost, Stefan; Schauss, Jakob; Strauch, Stefanie; Bormann, Reiner; Sivis, Murat; Schäfer, Sascha; Ropers, Claus

    2016-01-01

    We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the G\\"ottingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9 {\\AA} focused beam diameter, 200 fs pulse duration and 0.6 eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free electron beams.

  13. Clocking the anisotropic lattice dynamics of multi-walled carbon nanotubes by four-dimensional ultrafast transmission electron microscopy

    Science.gov (United States)

    Cao, Gaolong; Sun, Shuaishuai; Li, Zhongwen; Tian, Huanfang; Yang, Huaixin; Li, Jianqi

    2015-02-01

    Recent advances in the four-dimensional ultrafast transmission electron microscope (4D-UTEM) with combined spatial and temporal resolutions have made it possible to directly visualize structural dynamics of materials at the atomic level. Herein, we report on our development on a 4D-UTEM which can be operated properly on either the photo-emission or the thermionic mode. We demonstrate its ability to obtain sequences of snapshots with high spatial and temporal resolutions in the study of lattice dynamics of the multi-walled carbon nanotubes (MWCNTs). This investigation provides an atomic level description of remarkable anisotropic lattice dynamics at the picosecond timescales. Moreover, our UTEM measurements clearly reveal that distinguishable lattice relaxations appear in intra-tubular sheets on an ultrafast timescale of a few picoseconds and after then an evident lattice expansion along the radial direction. These anisotropic behaviors in the MWCNTs are considered arising from the variety of chemical bonding, i.e. the weak van der Waals bonding between the tubular planes and the strong covalent sp2-hybridized bonds in the tubular sheets.

  14. Free electron laser-driven ultrafast rearrangement of the electronic structure in Ti

    Directory of Open Access Journals (Sweden)

    E. Principi

    2016-03-01

    Full Text Available High-energy density extreme ultraviolet radiation delivered by the FERMI seeded free-electron laser has been used to create an exotic nonequilibrium state of matter in a titanium sample characterized by a highly excited electron subsystem at temperatures in excess of 10 eV and a cold solid-density ion lattice. The obtained transient state has been investigated through ultrafast absorption spectroscopy across the Ti M2,3-edge revealing a drastic rearrangement of the sample electronic structure around the Fermi level occurring on a time scale of about 100 fs.

  15. Ultrafast Molecular Three-Electron Collective Auger Decay

    Science.gov (United States)

    Feifel, Raimund

    2016-06-01

    A new class of many-electron Auger transitions in atoms was initially proposed over 40 years ago, but the first tentative evidence for its real existence was only adduced by Lee et al. in 1993, on the basis of the resonant Auger spectrum of Kr. Using a multi-electron coincidence technique with synchrotron radiation, we unambiguously showed very recently that the transition suggested by Lee et al. in Kr really does take place, but with a rather small branching ratio. Related inter-atomic three-electron transitions in rare gas clusters were recently predicted by Averbukh and Kolorenc and demonstrated by Ouchi et al.. From consideration of the energy levels involved it seems that the basic three-electron process could occur in molecules too, wherever a double inner-valence shell vacancy lies at a higher energy than the molecular triple ionisation onset. Experiments on CH_3F reveal for the first time the existence of this new decay pathway there, and calculations show that despite its three-electron nature, its effective oscillator strength is orders of magnitudes higher than in atoms, allowing an efficient competition with both molecular dissociation and two-electron decay channels on the ultrafast time scale. The dramatic enhancement of the molecular three-electron Auger transition can be explained in terms of a partial breakdown of the molecular orbital picture of ionisation. We predict that the collective decay pathway will be significant in a wide variety of heteroatomic molecules ionised by extreme UV and soft X-rays, particularly at Free-Electron-Lasers where double inner-shell vacancies can be created efficiently by two-photon transitions. G.N. Ogurtsov et al., Sov. Phys. Tech. Phys. 15, 1656 (1971) and V.V. Afrosimov et al., JETP Lett. 21, 249 (1975). I. Lee, R. Wehlitz, U. Becker and M. Ya. Amusia, J. Phys. B: At. Mol. Opt. Phys. 26, L41 (1993). J.H.D. Eland, R.J. Squibb, M. Mucke, S. Zagorodskikh, P. Linusson, and R. Feifel, New J. Phys. 17, 122001 (2015). V

  16. Simultaneous investigation of ultrafast structural dynamics and transient electric field by sub-picosecond electron pulses

    Energy Technology Data Exchange (ETDEWEB)

    Li, Run-Ze; Zhu, Pengfei; Chen, Long; Chen, Jie, E-mail: jiec@sjtu.edu.cn, E-mail: jzhang1@sjtu.edu.cn; Sheng, Zheng-Ming; Zhang, Jie, E-mail: jiec@sjtu.edu.cn, E-mail: jzhang1@sjtu.edu.cn [Key Laboratory for Laser Plasmas (Ministry of Education) and Department of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240 (China); Cao, Jianming [Key Laboratory for Laser Plasmas (Ministry of Education) and Department of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240 (China); Physics Department and National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32310 (United States)

    2014-05-14

    The ultrafast structure dynamics and surface transient electric field, which are concurrently induced by laser excited electrons of an aluminum nanofilm, have been investigated simultaneously by the same transmission electron diffraction patterns. These two processes are found to be significantly different and distinguishable by tracing the time dependent changes of electron diffraction and deflection angles, respectively. This study also provides a practical means to evaluate simultaneously the effect of transient electric field during the study of structural dynamics under low pump fluence by transmission ultrafast electron diffraction.

  17. Ultrafast interatomic electronic decay in multiply excited clusters

    CERN Document Server

    Kuleff, Alexander I; Kopelke, Soeren; Cederbaum, Lorenz S

    2010-01-01

    An ultrafast mechanism belonging to the family of interatomic Coulombic decay (ICD) phenomena is proposed. When two excited species are present, an ultrafast energy transfer can take place bringing one of them to its ground state and ionizing the other one. It is shown that if large homoatomic clusters are exposed to an ultrashort and intense laser pulse whose photon energy is in resonance with an excitation transition of the cluster constituents, the large majority of ions will be produced by this ICD mechanism rather than by two-photon ionization. A related collective-ICD process that is operative in heteroatomic systems is also discussed.

  18. 4-d magnetism: Electronic structure and magnetism of some Mo-based alloys

    Science.gov (United States)

    Liu, Yong; Bose, S. K.; Kudrnovský, J.

    2017-02-01

    We report results of a first-principles density-functional study of alloys of the 4 d -element Mo with group IV elements Si, Ge and Sn in zinc blende (ZB) and rock salt (RS) structures. The study was motivated by a similar study of ours based on the 4 d -element Tc, which showed the presence of half-metallic states with integer magnetic moment (1μB) per formula unit in TcX (X=C, Si, Ge) alloys. The calculated Curie temperatures for the ferromagnetic (FM) phases were low, around or less than 300 K. Searching for the possibility of 4 d -based alloys with higher Curie temperatures we have carried out the study involving the elements Mo, Ru and Rh. Among these the most promising case appears to be that involving the element Mo. Among the MoX (X=Si, Ge, Sn) alloys in ZB and RS structures, both MoGe and MoSn in ZB structures are found to possess an integer magnetic moment of 2μB per formula unit. ZB MoSn can be classified as a marginal/weak half-metal or a spin gapless semiconductor, while ZB MoGe would be best described as a gapless magnetic semiconductor. The calculated Curie temperatures are in the range 300-700 K. Considering the theoretical uncertainty in the band gaps due not only to the treatment of exchange and correlation effects, but density functional theory itself, these classifications may change somewhat, but both merit investigation from the viewpoint of potential spintronic application. Based on their higher Curie temperatures, Mo-based alloys would serve such purpose better than the previously reported Tc-based ones.

  19. Ultrafast electron diffraction optimized for studying structural dynamics in thin films and monolayers

    NARCIS (Netherlands)

    Badali, D. S.; Gengler, R. Y. N.; Miller, R. J. D.

    2016-01-01

    A compact electron source specifically designed for time-resolved diffraction studies of free-standing thin films and monolayers is presented here. The sensitivity to thin samples is achieved by extending the established technique of ultrafast electron diffraction to the "medium" energy regime (1-10

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

    DEFF Research Database (Denmark)

    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...... electric field at the antenna tip. Using this method resonant properties of antennas fabricated on high resistivity silicon are investigated in the strong field regime. Decrease of antenna Q-factor due to ultrafast carrier multiplication in the substrate is observed....

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

    Science.gov (United States)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  3. 4d electron Ruthenate systems: their unique and new magnetic properties

    Science.gov (United States)

    Lee, Seungran; Shin, Yeongjae; Anwar, M. S.; Sugimoto, Yusuke; Lee, Mincheol; Kang, Sungjin; Yonezawa, Shingo; Maeno, Yoshiteru; Noh, Taewon

    The Ruddlesden-Popper series (PR) of Srn+1RunO3n+1 has attract much interest of their unique physical properties. Among them, SrRuO3 (n = ∞) (SRO) is the only ferromagnetic metallic oxide especially in Ru 4d transition metal oxides. Bulk SRO has orthorhombic structure showing the Curie temperature (TC) ~ 160 K. It is well known that RuO6 octahedral distortion plays critical roles in its mangetic properties. In film systems, such RuO6 octahedra can be easily controlled by strain-engineering. In this talk, with high quality SRO films fully strained (-1.7%-1%) using various substrates, we systematically studied their structural changes and associated magnetic properties. Compared to theoretical predictions, the structural changes can be explained, while the magnetic property changes cannot be understood. Surprisingly, when SRO113 is grown on its PR series of Sr2RuO4 (n=1) (SRO214) single crystal, the exact substrate of SRO214 magnetization results in strongly enhanced magnetization (M > 3 μB/Ru, TC ~ 160 K), which has never found SRO113 (001) since the low-spin configuration of SRO113 prevent M never exceed 2 μB/Ru. The mystery of M in SRO113 (especially SRO113/SRO214) will be further discussed.

  4. Ultrafast electronic relaxation of excited state vitamin B{sub 12} in the gas phase

    Energy Technology Data Exchange (ETDEWEB)

    Shafizadeh, Niloufar [Laboratoire de Photophysique Moleculaire, U.P.R. 3361 CNRS Bat 210, Universite de Paris-Sud, 91405 Orsay, Cedex (France)], E-mail: Niloufar.Shafizadeh@u-psud.fr; Poisson, Lionel; Soep, Benoit [Laboratoire Francis Perrin, CEA/DSM/DRECAM/SPAM - CNRS URA 2453, CEA Saclay, 91191 Gif-sur-Yvette Cedex (France)

    2008-06-23

    The time evolution of electronically excited vitamin B{sub 12} (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.

  5. Ultrafast electronic relaxation of excited state vitamin B 12 in the gas phase

    Science.gov (United States)

    Shafizadeh, Niloufar; Poisson, Lionel; Soep, Benoıˆt

    2008-06-01

    The time evolution of electronically excited vitamin B 12 (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.

  6. Graphene-layered steps and their fields visualized by 4D electron microscopy.

    Science.gov (United States)

    Park, Sang Tae; Yurtsever, Aycan; Baskin, John Spencer; Zewail, Ahmed H

    2013-06-04

    Enhanced image contrast has been seen at graphene-layered steps a few nanometers in height by means of photon-induced near-field electron microscopy (PINEM) using synchronous femtosecond pulses of light and electrons. The observed steps are formed by the edges of graphene strips lying on the surface of a graphene substrate, where the strips are hundreds of nanometers in width and many micrometers in length. PINEM measurements reflect the interaction of imaging electrons and induced (near) electric fields at the steps, and this leads to a much higher contrast than that achieved in bright-field transmission electron microscopy imaging of the same strips. Theory and numerical simulations support the experimental PINEM findings and elucidate the nature of the electric field at the steps formed by the graphene layers. These results extend the range of applications of the experimental PINEM methodology, which has previously been demonstrated for spherical, cylindrical, and triangular nanostructures, to shapes of high aspect ratio (rectangular strips), as well as into the regime of atomic layer thicknesses.

  7. Ultrafast quenching of electron-boson interaction and superconducting gap in a cuprate superconductor.

    Science.gov (United States)

    Zhang, Wentao; Hwang, Choongyu; Smallwood, Christopher L; Miller, Tristan L; Affeldt, Gregory; Kurashima, Koshi; Jozwiak, Chris; Eisaki, Hiroshi; Adachi, Tadashi; Koike, Yoji; Lee, Dung-Hai; Lanzara, Alessandra

    2014-01-01

    Ultrafast spectroscopy is an emerging technique with great promise in the study of quantum materials, as it makes it possible to track similarities and correlations that are not evident near equilibrium. Thus far, however, the way in which these processes modify the electron self-energy--a fundamental quantity describing many-body interactions in a material--has been little discussed. Here we use time- and angle-resolved photoemission to directly measure the ultrafast response of self-energy to near-infrared photoexcitation in high-temperature cuprate superconductor. Below the critical temperature of the superconductor, ultrafast excitations trigger a synchronous decrease of electron self-energy and superconducting gap, culminating in a saturation in the weakening of electron-boson coupling when the superconducting gap is fully quenched. In contrast, electron-boson coupling is unresponsive to ultrafast excitations above the critical temperature of the superconductor and in the metallic state of a related material. These findings open a new pathway for studying transient self-energy and correlation effects in solids.

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

    KAUST Repository

    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.

  9. Electronic structures and magnetic properties of 3d and 4d transition-metal impurities in ferromagnetic Fe

    CERN Document Server

    Park, J H; Min, B I; Cho, H S

    2000-01-01

    Employing the self-consistent local approach, the tight-binding linear-muffin-tin orbital recursion method, we have investigated the electronic structures and the magnetic properties of 3d and 4d transition-metal (TM) impurities in ferromagnetic bcc Fe. In both 3d and 4d TM impurities, virtual bound states appear and are characterized by a high density of states in the energy spectrum. The characters of the states are studied by calculating the bond order between interaction orbitals. For early TM impurities, the states at the impurity sites have more antibonding characters, while the states at neighboring Fe sites have more bonding characters. For late TM impurities, the situation is reversed. late TM impurities of both the 3d and the 4d TM series have the same magnetic ordering as the host Fe atoms whereas early TM impurities have magnetic moments antiparallel to that of the host. As for the Mn impurity, an inward relaxation of neighboring Fe atoms stabilizes the antiferromagnetic ordering with respect to t...

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

    CERN Document Server

    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.

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

    CERN Document Server

    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.

  12. Ultrafast Spin Density Wave Transition in Chromium Governed by Thermalized Electron Gas

    Science.gov (United States)

    Nicholson, C. W.; Monney, C.; Carley, R.; Frietsch, B.; Bowlan, J.; Weinelt, M.; Wolf, M.

    2016-09-01

    The energy and momentum selectivity of time- and angle-resolved photoemission spectroscopy is exploited to address the ultrafast dynamics of the antiferromagnetic spin density wave (SDW) transition photoexcited in epitaxial thin films of chromium. We are able to quantitatively extract the evolution of the SDW order parameter Δ through the ultrafast phase transition and show that Δ is governed by the transient temperature of the thermalized electron gas, in a mean field description. The complete destruction of SDW order on a sub-100 fs time scale is observed, much faster than for conventional charge density wave materials. Our results reveal that equilibrium concepts for phase transitions such as the order parameter may be utilized even in the strongly nonadiabatic regime of ultrafast photoexcitation.

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

    CERN Document Server

    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...

  14. Ultrafast time dynamics studies of periodic lattices with free electron laser radiation

    Energy Technology Data Exchange (ETDEWEB)

    Quevedo, W.; Busse, G.; Hallmann, J.; More, R.; Petri, M.; Rajkovic, I. [Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, 37077 Goettingen (Germany); Krasniqi, F.; Rudenko, A. [Max Planck Advanced Study Group at CFEL, Notkestrasse 85, 22607 Hamburg (Germany); Tschentscher, T. [European XFEL GmbH, Albert-Einstein-Ring 19, 22671 Hamburg (Germany); Stojanovic, N.; Duesterer, S.; Treusch, R.; Tolkiehn, M. [HASYLAB at DESY, Notkestrasse 85, 22607 Hamburg (Germany); Techert, S. [Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, 37077 Goettingen (Germany); Max Planck Advanced Study Group at CFEL, Notkestrasse 85, 22607 Hamburg (Germany)

    2012-11-01

    It has been proposed that radiation from free electron laser (FEL) at Hamburg (FLASH) can be used for ultrafast time-resolved x-ray diffraction experiments based on the near-infrared (NIR) pump/FEL probe scheme. Here, investigation probing the ultrafast structural dynamics of periodic nano-crystalline organic matter (silver behenate) with such a scheme is reported. Excitation with a femtosecond NIR laser leads to an ultrafast lattice modification which time evolution has been studied through the scattering of vacuum ultraviolet FEL pulses. The found effect last for 6 ps and underpins the possibility for studying nanoperiodic dynamics down to the FEL source time resolution. Furthermore, the possibility of extending the use of silver behenate (AgBh) as a wavelength and temporal calibration tool for experiments with soft x-ray/FEL sources is suggested.

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

    KAUST Repository

    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.

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

    DEFF Research Database (Denmark)

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

    2013-01-01

    –310 fs were found for all samples. Comparison between TA dynamics on uncoated and dye-sensitized hematite nanoparticles revealed the dye de-excitation pathway to consist of a competition between electron and energy transfer to the nanoparticles. We analyzed the TA data for hematite nanoparticles using...... a four-state model of the dye-sensitized system, finding electron and energy transfer to occur on the same ultrafast timescale. The interfacial electron transfer rates for iron oxides are very close to those previously reported for DCF-sensitized titanium dioxide (for which dye–oxide energy transfer...... photo-initiated interfacial electron transfer. This approach enables time-resolved study of the fate and mobility of electrons within the solid phase. However, complete analysis of the ultrafast processes following dye photoexcitation of the sensitized iron(iii) oxide nanoparticles has not been reported...

  17. Direct monitoring of ultrafast electron and hole dynamics in perovskite solar cells.

    Science.gov (United States)

    Piatkowski, Piotr; Cohen, Boiko; Javier Ramos, Francisco; Di Nunzio, Maria; Nazeeruddin, Mohammad Khaja; Grätzel, Michael; Ahmad, Shahzada; Douhal, Abderrazzak

    2015-06-14

    Organic-inorganic hybrid perovskite solar cells have emerged as cost effective efficient light-to-electricity conversion devices. Unravelling the time scale and the mechanisms that govern the charge carrier dynamics is of paramount importance for a clear understanding and further optimization of the perovskite based devices. For the classical FTO/bulk titania blocking layer/mesoporous titania/perovskite/Spiro-OMeTAD (FTO/TPS) cell, further detailed and systematic studies of the ultrafast events related to exciton generation, electron and hole transfer, ultrafast relaxation are still needed. We characterize the initial ultrafast processes attributed to the exciton-perovskite lattice interactions influenced by charge transfer to the electron and hole transporters that precede the exciton diffusion into free charge carriers occurring in the sensitizer. Time-resolved transient absorption studies of the FTO/perovskite and FTO/TPS samples under excitation at different wavelengths and at low fluence 2 (μJ cm(-2)) indicate the sub-picosecond electron and hole injection into titania and Spiro-OMeTAD, respectively. Furthermore, the power-dependent femtosecond transient absorption measurements support the ultrafast charge transfer and show strong Auger-type multiparticle interactions at early times. We reveal that the decays of the internal trap states are the same for both films, while those at surfaces differ. The contribution of the former in the recombination is small, thus increasing the survival probability of the charges in the excited perovskite.

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

    CERN Document Server

    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 ...

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

    Science.gov (United States)

    Battiato, Marco; Aguilera, Irene; Sánchez-Barriga, Jaime

    2017-07-17

    Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin-orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized G W +Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron-electron and electron-phonon scatterings. Taking the prototypical insulator Bi 2 Te 3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron-electron and electron-phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials.

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

    KAUST Repository

    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.

  1. Direct observation of ultrafast many-body electron dynamics in an ultracold Rydberg gas

    Science.gov (United States)

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

    2016-11-01

    Many-body correlations govern a variety of important quantum phenomena such as the emergence of superconductivity and magnetism. Understanding quantum many-body systems is thus one of the central goals of modern sciences. Here we demonstrate an experimental approach towards this goal by utilizing an ultracold Rydberg gas generated with a broadband picosecond laser pulse. We follow the ultrafast evolution of its electronic coherence by time-domain Ramsey interferometry with attosecond precision. The observed electronic coherence shows an ultrafast oscillation with a period of 1 femtosecond, whose phase shift on the attosecond timescale is consistent with many-body correlations among Rydberg atoms beyond mean-field approximations. This coherent and ultrafast many-body dynamics is actively controlled by tuning the orbital size and population of the Rydberg state, as well as the mean atomic distance. Our approach will offer a versatile platform to observe and manipulate non-equilibrium dynamics of quantum many-body systems on the ultrafast timescale.

  2. Proposed imaging of the ultrafast electronic motion in samples using x-ray phase-contrast

    CERN Document Server

    Dixit, Gopal; Santra, Robin

    2013-01-01

    Tracing the motion of electrons has enormous relevance to understanding ubiquitous phenomena in ultrafast science, such as the dynamical evolution of the electron density during complex chemical and biological processes. Scattering of ultrashort x-ray pulses from an electronic wavepacket would appear to be the most obvious approach to image the electronic motion in real-time and real-space with the notion that such scattering patterns, in the far-field regime, encode the instantaneous electron density of the wavepacket. However, recent results by Dixit {\\em et al.} [Proc. Natl. Acad. Sci. U.S.A., {\\bf 109}, 11636 (2012)] have put this notion into question and shown that the scattering in the far-field regime probes spatio-temporal density-density correlations. Here, we propose a possible way to image the instantaneous electron density of the wavepacket via ultrafast x-ray {\\em phase contrast imaging}. Moreover, we show that inelastic scattering processes, which plague ultrafast scattering in the far-field reg...

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

    Institute of Scientific and Technical Information of China (English)

    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.

  4. Ultrafast phase transition via catastrophic phonon collapse driven by plasmonic hot-electron injection.

    Science.gov (United States)

    Appavoo, Kannatassen; Wang, Bin; Brady, Nathaniel F; Seo, Minah; Nag, Joyeeta; Prasankumar, Rohit P; Hilton, David J; Pantelides, Sokrates T; Haglund, Richard F

    2014-03-12

    Ultrafast photoinduced phase transitions could revolutionize data-storage and telecommunications technologies by modulating signals in integrated nanocircuits at terahertz speeds. In quantum phase-changing materials (PCMs), microscopic charge, lattice, and orbital degrees of freedom interact cooperatively to modify macroscopic electrical and optical properties. Although these interactions are well documented for bulk single crystals and thin films, little is known about the ultrafast dynamics of nanostructured PCMs when interfaced to another class of materials as in this case to active plasmonic elements. Here, we demonstrate how a mesh of gold nanoparticles, acting as a plasmonic photocathode, induces an ultrafast phase transition in nanostructured vanadium dioxide (VO2) when illuminated by a spectrally resonant femtosecond laser pulse. Hot electrons created by optical excitation of the surface-plasmon resonance in the gold nanomesh are injected ballistically across the Au/VO2 interface to induce a subpicosecond phase transformation in VO2. Density functional calculations show that a critical density of injected electrons leads to a catastrophic collapse of the 6 THz phonon mode, which has been linked in different experiments to VO2 phase transition. The demonstration of subpicosecond phase transformations that are triggered by optically induced electron injection opens the possibility of designing hybrid nanostructures with unique nonequilibrium properties as a critical step for all-optical nanophotonic devices with optimizable switching thresholds.

  5. Design of an MeV ultra-fast electron diffraction experiment at Tsinghua university

    Institute of Scientific and Technical Information of China (English)

    LI Ren-Kai; TANG Chuan-Xiang; HUANG Wen-Hui; DU Ying-Chao; SHI Jia-Ru; YAN Li-Xin

    2009-01-01

    Time-resolved MeV ultra-fast electron difiraction(UED)is a powerful tool for structure dynamics studies.In this paper.we present a design of a MeV UED facility based on a photocathode RF gun at Tsinghua University.Electron beam qualities are optimized with numerical simulations,indicating that resolutions of 250 fs and 0.01 A.and bunch charge exceeding 105 electrons are expected with technically achievable machine parameters.Status of experiment preparation is also presented.

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

    Science.gov (United States)

    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.

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

    KAUST Repository

    Sun, Jingya

    2015-09-14

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

  8. Ultrafast electronic dynamics in laser-excited crystalline bismuth

    Directory of Open Access Journals (Sweden)

    Chekalin S.

    2013-03-01

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

  9. Non-thermal hot electrons ultrafastly generating hot optical phonons in graphite

    Science.gov (United States)

    Ishida, Y.; Togashi, T.; Yamamoto, K.; Tanaka, M.; Taniuchi, T.; Kiss, T.; Nakajima, M.; Suemoto, T.; Shin, S.

    2011-08-01

    Investigation of the non-equilibrium dynamics after an impulsive impact provides insights into couplings among various excitations. A two-temperature model (TTM) is often a starting point to understand the coupled dynamics of electrons and lattice vibrations: the optical pulse primarily raises the electronic temperature Tel while leaving the lattice temperature Tl low; subsequently the hot electrons heat up the lattice until Tel = Tl is reached. This temporal hierarchy owes to the assumption that the electron-electron scattering rate is much larger than the electron-phonon scattering rate. We report herein that the TTM scheme is seriously invalidated in semimetal graphite. Time-resolved photoemission spectroscopy (TrPES) of graphite reveals that fingerprints of coupled optical phonons (COPs) occur from the initial moments where Tel is still not definable. Our study shows that ultrafast-and-efficient phonon generations occur beyond the TTM scheme, presumably associated to the long duration of the non-thermal electrons in graphite.

  10. Ultrafast imprinting of topologically protected magnetic textures via pulsed electrons

    Science.gov (United States)

    Schäffer, A. F.; Dürr, H. A.; Berakdar, J.

    2017-07-01

    Short electron pulses are demonstrated to trigger and control magnetic excitations, even at low electron current densities. We show that the tangential magnetic field surrounding a picosecond electron pulse can imprint topologically protected magnetic textures such as skyrmions in a sample with a residual Dzyaloshinskii-Moriya spin-orbital coupling. Characteristics of the created excitations such as the topological charge can be steered via the duration and the strength of the electron pulses. The study points to a possible way for a spatiotemporally controlled generation of skyrmionic excitations.

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

    Science.gov (United States)

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1998-10-01

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

  13. Excitation of the 4d shell in Sb, Te, and BaF/sub 2/ with inelastic electron scattering: Collective or single particle

    Energy Technology Data Exchange (ETDEWEB)

    Franck, C.; Schnatterly, S.E.

    1982-06-01

    Simple models suggest that the momentum-transfer (q) dependence of inelastic electron scattering is sensitive to the difference between collective and single-particle behavior in atomic dynamics. We measured the energy centroid of the 4d continuum peak for 04d shells: Sb, Te, and BaF/sub 2/, and we find that a single-particle description is favored.

  14. Ultrafast static and diffusion-controlled electron transfer at Ag 29 nanocluster/molecular acceptor interfaces

    KAUST Repository

    Aly, Shawkat Mohammede

    2015-10-29

    Efficient absorption of visible light and a long-lived excited state lifetime of silver nanoclusters (Ag29 NCs) are integral properties for these new clusters to serve as light-harvesting materials. Upon optical excitation, electron injection at Ag29 NC/methyl viologen (MV2+) interfaces is very efficient and ultrafast. Interestingly, our femto- and nanosecond time-resolved results demonstrate clearly that both dynamic and static electron transfer mechanisms are involved in photoluminescence quenching of Ag29 NCs. © 2016 The Royal Society of Chemistry.

  15. Ultrafast electron diffraction optimized for studying structural dynamics in thin films and monolayers.

    Science.gov (United States)

    Badali, D S; Gengler, R Y N; Miller, R J D

    2016-05-01

    A compact electron source specifically designed for time-resolved diffraction studies of free-standing thin films and monolayers is presented here. The sensitivity to thin samples is achieved by extending the established technique of ultrafast electron diffraction to the "medium" energy regime (1-10 kV). An extremely compact design, in combination with low bunch charges, allows for high quality diffraction in a lensless geometry. The measured and simulated characteristics of the experimental system reveal sub-picosecond temporal resolution, while demonstrating the ability to produce high quality diffraction patterns from atomically thin samples.

  16. Ultrafast electron diffraction optimized for studying structural dynamics in thin films and monolayers

    Directory of Open Access Journals (Sweden)

    D. S. Badali

    2016-05-01

    Full Text Available A compact electron source specifically designed for time-resolved diffraction studies of free-standing thin films and monolayers is presented here. The sensitivity to thin samples is achieved by extending the established technique of ultrafast electron diffraction to the “medium” energy regime (1–10 kV. An extremely compact design, in combination with low bunch charges, allows for high quality diffraction in a lensless geometry. The measured and simulated characteristics of the experimental system reveal sub-picosecond temporal resolution, while demonstrating the ability to produce high quality diffraction patterns from atomically thin samples.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  19. Multiobjective optimizations of a novel cryocooled dc gun based ultrafast electron diffraction beam line

    Science.gov (United States)

    Gulliford, Colwyn; Bartnik, Adam; Bazarov, Ivan

    2016-09-01

    We present the results of multiobjective genetic algorithm optimizations of a single-shot ultrafast electron diffraction beam line utilizing a 225 kV dc gun with a novel cryocooled photocathode system and buncher cavity. Optimizations of the transverse projected emittance as a function of bunch charge are presented and discussed in terms of the scaling laws derived in the charge saturation limit. Additionally, optimization of the transverse coherence length as a function of final rms bunch length at the sample location have been performed for three different sample radii: 50, 100, and 200 μ m , for two final bunch charges: 1 05 electrons (16 fC) and 1 06 electrons (160 fC). Example optimal solutions are analyzed, and the effects of disordered induced heating estimated. In particular, a relative coherence length of Lc ,x/σx=0.27 nm /μ m was obtained for a final bunch charge of 1 05 electrons and final bunch length of σt≈100 fs . For a final charge of 1 06 electrons the cryogun produces Lc ,x/σx≈0.1 nm /μ m for σt≈100 - 200 fs and σx≥50 μ m . These results demonstrate the viability of using genetic algorithms in the design and operation of ultrafast electron diffraction beam lines.

  20. 10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources

    Science.gov (United States)

    Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

    2017-01-01

    Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today’s ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources.

  1. Transient optical response of ultrafast nonequilibrium excited metals: Effects of electron-electron contribution to collisional absorption

    CERN Document Server

    Colombier, Jean-Philippe; Audouard, Eric; Stoian, Razvan

    2008-01-01

    Approaching energy coupling in laser-irradiated metals, we point out the role of electron-electron collision as an efficient control factor for ultrafast optical absorption. The high degree of laser-induced electron-ion nonequilibrium drives a complex absorption pattern with consequences on the transient optical properties. Consequently, high electronic temperatures determine largely the collision frequency and establish a transition between absorptive regimes in solid and plasma phases. In particular, taking into account umklapp electron-electron collisions, we performed hydrodynamic simulations of the laser-matter interaction to calculate laser energy deposition during the electron-ion nonequilibrium stage and subsequent matter transformation phases. We observe strong correlations between optical and thermodynamic properties according to the experimental situations. A suitable connection between solid and plasma regimes is chosen in accordance with models that describe the behavior in extreme, asymptotic re...

  2. First-principles calculations of heat capacities of ultrafast laser-excited electrons in metals

    Science.gov (United States)

    Bévillon, E.; Colombier, J. P.; Recoules, V.; Stoian, R.

    2015-05-01

    Ultrafast laser excitation can induce fast increases of the electronic subsystem temperature. The subsequent electronic evolutions in terms of band structure and energy distribution can determine the change of several thermodynamic properties, including one essential for energy deposition; the electronic heat capacity. Using density functional calculations performed at finite electronic temperatures, the electronic heat capacities dependent on electronic temperatures are obtained for a series of metals, including free electron like, transition and noble metals. The effect of exchange and correlation functionals and the presence of semicore electrons on electronic heat capacities are first evaluated and found to be negligible in most cases. Then, we tested the validity of the free electron approaches, varying the number of free electrons per atom. This shows that only simple metals can be correctly fitted with these approaches. For transition metals, the presence of localized d electrons produces a strong deviation toward high energies of the electronic heat capacities, implying that more energy is needed to thermally excite them, compared to free sp electrons. This is attributed to collective excitation effects strengthened by a change of the electronic screening at high temperature.

  3. Ultrafast Molecular Imaging by Laser Induced Electron Diffraction

    CERN Document Server

    Peters, Michel; Cornaggia, Christian; Saugout, Sébastien; Charron, Eric; Keller, Arne; Atabek, Osman

    2010-01-01

    We address the feasibility of imaging geometric and orbital structure of a polyatomic molecule on an attosecond time-scale using the Laser Induced Electron Diffraction, LIED, technique [T. Zuo \\textit{et al.}, Chem. Phys. Lett. \\textbf{259}, 313 (1996)]. We present numerical results obtained for the CO$_2$ molecule using a single active electron model. The molecular geometry (bond-lengths) is determined within 3% of accuracy from a diffraction pattern which also reflects the nodal properties of the initial molecular orbital. Robustness of the structure determination is discussed with respect to vibrational and rotational motions with a complete interpretation of the laser-induced mechanisms.

  4. Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators

    Energy Technology Data Exchange (ETDEWEB)

    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.

  5. Ultrafast electron diffraction from laser-aligned molecules in the gas phase

    Science.gov (United States)

    Yang, Jie

    Ultrafast electron diffraction has emerged since the end of last century, and has become an increasingly important tool for revealing great details of molecular dynamics. In comparison to spectroscopic techniques, ultrafast electron diffraction directly probes time-resolved structure of target molecules, and therefore can potentially provide "molecular movies" of the reactions being studied. These molecular movies are critical for understanding and ultimately controlling the energy conversion pathways and efficiencies of photochemical processes. In this dissertation, I have focused on ultrafast electron diffraction from gas-phase molecules, and have investigated several long-standing challenges that have been preventing researchers from being able to achieve 3-D molecular movies of photochemical reactions. The first challenge is to resolve the full 3-D structure for molecules in the gas phase. The random orientation of molecules in the gas phase smears out the diffraction signal, which results in only 1-D structural information being accessible. The second challenge lies in temporal resolution. In order to resolve coherent nuclear motions on their natural time scale, a temporal resolution of ˜200 femtosecond or better is required. However, due to experimental limitations the shortest temporal resolution that had been achieved was only a few picoseconds in early 2000, by Zewail group from Caltech. The first challenge is tackled by laser-alignment. In the first half of the dissertation, I approach this method both theoretically and experimentally, and demonstrate that by using a short laser pulse to transiently align target molecules in space, 3-D molecular structure can be reconstructed ab-initio from diffraction patterns. The second half of the dissertation presents two experiments, both of which are important steps toward imaging coherent nuclear motions in real time during photochemical reactions. The first experiment simultaneously resolves molecular alignment

  6. Ultrafast Hot Electron Induced Phase Transitions in Vanadium Dioxide

    Directory of Open Access Journals (Sweden)

    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.

  7. Electron work function and surface energy of body-centered and face-centered cubic modifications of 4 d- and 5 d-metals

    Science.gov (United States)

    Aref'eva, L. P.; Shebzukhova, I. G.

    2016-07-01

    A technique for the evaluation of the electron work function of metallic single crystals and the electron work function anisotropy has been developed in the framework of the electron-statistical method. The surface energy and the electron work function have been calculated for crystal faces of allotropic modifications of 4 d- and 5 d-metals. A change in the electron work function due to the allotropic transformations has been estimated, and the periodic dependence of the electron work function has been determined. It has been shown that the results obtained using the proposed technique correlate with the available experimental data for polycrystals.

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

    Science.gov (United States)

    Timmers, Henry Robert

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

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

    Energy Technology Data Exchange (ETDEWEB)

    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

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

    CERN Document Server

    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.

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

    Science.gov (United States)

    Lorenz, U.; Kabachnik, N. M.; Weckert, E.; Vartanyants, I. A.

    2012-11-01

    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.

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

    Directory of Open Access Journals (Sweden)

    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.

  13. Alignment dependent ultrafast electron-nuclear dynamics in high-order harmonic generation

    CERN Document Server

    Li, Mu-Zi; Bian, Xue-Bin

    2016-01-01

    We investigated the high-order harmonic generation (HHG) process of diatomic molecular ion $\\mathrm{H}_2^+$ in non-Born-Oppenheimer approximations. The corresponding three-dimensional time-dependent Schr\\"odinger equation is solved with arbitrary alignment angles. It is found that the nuclear motion can lead to spectral modulation of HHG. Redshifts are unique in molecular HHG which decrease with the increase of alignment angles of the molecules and are sensitive to the initial vibrational states. It can be used to extract the ultrafast electron-nuclear dynamics and image molecular structure.

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

    Energy Technology Data Exchange (ETDEWEB)

    Chapman, H N; Bajt, S; Barty, A; Benner, W; Bogan, M; Frank, M; Hau-Riege, S; London, R; Marchesini, S; Spiller, E; Szoke, A; Woods, B; Boutet, S; Hodgson, K; Hajdu, J; Bergh, M; Burmeister, F; Caleman, C; Huldt, G; Maia, F; Seibert, M M; der Spoel, D v

    2006-08-22

    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.

  15. Ultrafast Electronic Band Gap Control in an Excitonic Insulator

    Science.gov (United States)

    Mor, Selene; Herzog, Marc; Golež, Denis; Werner, Philipp; Eckstein, Martin; Katayama, Naoyuki; Nohara, Minoru; Takagi, Hide; Mizokawa, Takashi; Monney, Claude; Stähler, Julia

    2017-08-01

    We report on the nonequilibrium dynamics of the electronic structure of the layered semiconductor Ta2NiSe5 investigated by time- and angle-resolved photoelectron spectroscopy. We show that below the critical excitation density of FC=0.2 mJ cm-2 , the band gap narrows transiently, while it is enhanced above FC . Hartree-Fock calculations reveal that this effect can be explained by the presence of the low-temperature excitonic insulator phase of Ta2 NiSe5 , whose order parameter is connected to the gap size. This work demonstrates the ability to manipulate the band gap of Ta2 NiSe5 with light on the femtosecond time scale.

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

    Science.gov (United States)

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

    2017-08-24

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

  17. Ultrafast spectroscopic investigations of cadmium chalcogenides: Nanoscale electronic relaxation and transfer

    Science.gov (United States)

    Spann, Bryan Thomas

    Harnessing solar energy more effectively remains one of the most important scientific challenges in recent history. Various strategies have been developed to capture the sun's energy to generate usable electricity. Recently, advances in chemistry have allowed researchers to synthesize semiconducting nanocrystals which show great promise in capturing and converting solar energy in a cheap and efficient way. In this dissertation, aspects of energy conversion processes in semiconducting nanocrystals are explored to elucidate their potential for photovoltaic applications. Various forms of linear and non-linear optical spectroscopy techniques were employed to explore electronic relaxation and transfer phenomena in nanoscale cadmium chalcogenide materials and heterojunctions. Ultrafast transient absorption studies were performed on various sizes of CdSe quantum dots (QDs) and quantum rods (QRs) with similar bandedge energies. These studies reviled that QRs have increased intraband relaxation times when compared with QDs as a result of an ultrafast formation of a 1D exciton along the elongated axis of the QR. The formation of the 1D exciton reduces the electron-to-hole scattering potential, consequently reducing the Auger thermalization mechanism. Furthermore, QD samples made in film form showed increased intraband relaxation times as a result of a hydrazine treatment which removed (in part) the organic ligands attached to the surface. As a result of removing the ligands, the ligand based relaxation pathway for the holes was also reduced, causing longer intraband relaxation. In addition to the studies on CdSe nanocrystals (NCs), ultrafast spectroscopy was used to study aspects of charge transfer in CdS -- TiO2 NC heterojunctions. This study revealed a means of increasing photo-induced ultrafast charge transfer in successive ionic layer adsorption and reaction (SILAR) CdS--TiO2 NC heterojunctions using pulsed laser sintering of TiO2 nanocrystals. The enhanced charge

  18. High-Mobility Two-Dimensional Electron Gases at ZnO/ZnMgO Interfaces for Ultra-Fast Electronics Applications

    Science.gov (United States)

    2014-11-17

    AFRL-AFOSR-UK-TR-2015-0007 High-mobility two-dimensional electron gases at ZnO /ZnMgO interfaces for ultra-fast electronics...two-dimensional electron gases at ZnO /ZnMgO interfaces for ultra-fast electronics applications 5a. CONTRACT NUMBER 5b. GRANT NUMBER FA8655-12...strain. This will necessitate the growth of a thin film of ZnO between the ZnO single crystal substrate and the ZnMgO thin film. 15

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

    Energy Technology Data Exchange (ETDEWEB)

    Wall, Simon [Univ. of Oxford (United Kingdom). Clarendon Lab.; Rini, Matteo [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Dhesi, Sarnjeet S. [Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.; Schoenlein, Robert W. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Cavalleri, Andrea [Univ. of Oxford (United Kingdom). Clarendon Lab.; Univ. of Hamburg (Germany). Max Planck Research Dept. for Structural Dynamics

    2011-02-24

    Here 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. Lastly, 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.

  20. Real-Time Observation of Cuprates Structural Dynamics by Ultrafast Electron Crystallography

    Directory of Open Access Journals (Sweden)

    F. Carbone

    2010-01-01

    Full Text Available The phonon-mediated attractive interaction between carriers leads to the Cooper pair formation in conventional superconductors. Despite decades of research, the glue holding Cooper pairs in high-temperature superconducting cuprates is still controversial, and the same is true for the relative involvement of structural and electronic degrees of freedom. Ultrafast electron crystallography (UEC offers, through observation of spatiotemporally resolved diffraction, the means for determining structural dynamics and the possible role of electron-lattice interaction. A polarized femtosecond (fs laser pulse excites the charge carriers, which relax through electron-electron and electron-phonon couplings, and the consequential structural distortion is followed diffracting fs electron pulses. In this paper, the recent findings obtained on cuprates are summarized. In particular, we discuss the strength and symmetry of the directional electron-phonon coupling in Bi2Sr2CaCu2O8+δ (BSCCO, as well as the c-axis structural instability induced by near-infrared pulses in La2CuO4 (LCO. The theoretical implications of these results are discussed with focus on the possibility of charge stripes being significant in accounting for the polarization anisotropy of BSCCO, and cohesion energy (Madelung calculations being descriptive of the c-axis instability in LCO.

  1. Exploration of ultra-fast electron dynamics using time-dependent R-matrix theory

    Science.gov (United States)

    van der Hart, Hugo; Rey, Hector; Hassouneh, Ola; Brown, Andrew

    2014-05-01

    When an atom is subjected to an intense laser field, the full atomic response can involve a collective response involving several electrons. This collective response will be affected by electron-electron repulsion, coupling the overall electron dynamics. In order to investigate this dynamics for a multi-electron system from first principles, we have developed time-dependent R-matrix theory. The theory applies the basic principles of R-matrix theory, in which all interactions between all electrons are taken into account close to the nucleus, but exchange interactions are neglected when one electron has become distanced from the parent atom. In this contribution, we will explain the basic principles of this theory and demonstrate its application to ultra-fast dynamics in C+, and harmonic generation in singly ionised noble-gas atoms. Both studies demonstrate that it is important to go beyond the single-active-electron approximation. This research has been supported by EPSRC UK, and by the EU Initial Training Network CORINF.

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

    Science.gov (United States)

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

    2014-02-11

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

  3. Ultrafast control of electron spin in a quantum dot using geometric phase

    Science.gov (United States)

    Malinovsky, V. S.; Rudin, S.

    2012-12-01

    We propose a scheme to perform arbitrary unitary operations on a single electron-spin qubit in a quantum dot. The design is solely based on the geometrical phase that the qubit state acquires after a cyclic evolution in the parameter space. The scheme is utilizing ultrafast linearly-chirped pulses providing adiabatic excitation of the qubit states and the geometric phase is fully controlled by the relative phase between pulses. The analytic expression of the evolution operator for the electron spin in a quantum dot, which provides a clear geometrical interpretation of the qubit dynamics is obtained. Using parameters of InGaN/GaN, GaN/AlN quantum dots we provide an estimate for the time scale of the qubit rotations and parameters of the external fields.

  4. Microbunching instability in relativistic electron bunches: direct observations of the microstructures using ultrafast YBCO detectors.

    Science.gov (United States)

    Roussel, E; Evain, C; Szwaj, C; Bielawski, S; Raasch, J; Thoma, P; Scheuring, A; Hofherr, M; Ilin, K; Wünsch, S; Siegel, M; Hosaka, M; Yamamoto, N; Takashima, Y; Zen, H; Konomi, T; Adachi, M; Kimura, S; Katoh, M

    2014-08-29

    Relativistic electron bunches circulating in accelerators are subjected to a dynamical instability leading to microstructures at millimeter to centimeter scale. Although this is a well-known fact, direct experimental observations of the structures, or the field that they emit, remained up to now an open problem. Here, we report the direct, shot-by-shot, time-resolved recording of the shapes (including envelope and carrier) of the pulses of coherent synchrotron radiation that are emitted, and that are a "signature" of the electron bunch microstructure. The experiments are performed on the UVSOR-III storage ring, using electrical field sensitive YBa2Cu3O(7-x) thin-film ultrafast detectors. The observed patterns are subjected to permanent drifts, that can be explained from a reasoning in phase space, using macroparticle simulations.

  5. Coherent oscillations of electrons in tunnel-coupled wells under ultrafast intersubband excitation

    Energy Technology Data Exchange (ETDEWEB)

    Hernandez-Cabrera, A [Departamento de FIsica Basica, Universidad de La Laguna, La Laguna 38206-Tenerife, Canary Islands (Spain); Aceituno, P [Departamento de FIsica Basica, Universidad de La Laguna, La Laguna 38206-Tenerife, Canary Islands (Spain); Vasko, F T [Institute of Semiconductor Physics, NAS of Ukraine, Kiev, 252650 (Ukraine)

    2004-07-28

    Ultrafast intersubband excitation of electrons in tunnel-coupled wells is studied in respect of its dependence on the structure parameters, the duration of the infrared pump and the detuning frequency. The temporal dependences of the photoinduced carrier concentration and dipole moment are obtained for two cases of transitions: from the single ground state to the tunnel-coupled excited states and from the tunnel-coupled states to the single excited state. The peculiarities of dephasing and population relaxation processes are also taken into account. The nonlinear regime of the response is also considered when the splitting energy between the tunnel-coupled levels is renormalized by the photoexcited electron concentration. The dependences of the period and the amplitude of oscillations on the excitation pulse are presented with a description of the damping of the nonlinear oscillations.

  6. Ultrafast electron-phonon coupling at the metal-dielectric interface

    Science.gov (United States)

    Yao, Qiaomu

    The pump-probe technique is an ultrafast spectroscopy method of detecting the dynamics of energy carriers such as electrons, phonons, and holes with transient thermal reflectance measurement. A laser beam is divided into a pump beam and probe beam with different wavelength or polarization and time delay. According to the transient reflectance result, this method could be applied to investigate the interaction between electron-phonon and electron-electron coupling with a high temporal resolution on the order of 10 femtoseconds. Energy transfer of photo-excited electrons in a metal film to the dielectric substrate at the metal-dielectric interface is important for understanding the ultrafast heat transfer process across the two materials. Many researches have been conducted in finding this energy transfer process in different materials. In this thesis, by measuring the transient reflectance variation, the two-temperature model (TTM) is used to analyze the interface metal electron and dielectric substrate coupling. In order to relate temperature to the reflectance change, a temperature and wavelength dependent Drude-Lorentz model was developed which represents the temperature dependent dielectric constant and can be used to calculate reflectance variation. Ultrafast pump-and-probe interband transition measurements on Au-Si samples were carried out, where the probe photon energy was chosen to be close to the interband transition threshold (ITT) of gold to minimize the influence of non-equilibrium or non-thermalized electrons on the optical response, and to increase the signal to noise ratio for reflectance change. In the experiment, different pump fluences have been used to test the transient reflectance variation on Au-Si samples of different thicknesses. The pump wavelength is taken as 800 nm while the probe wavelength is taken as 490 nm. A thick gold of 1000 nm thickness has been used to determine the electron-phonon coupling strength represented by a constant G 0

  7. Ultrafast electronic response of graphene to a strong and localized electric field

    Science.gov (United States)

    Gruber, Elisabeth; Wilhelm, Richard A.; Pétuya, Rémi; Smejkal, Valerie; Kozubek, Roland; Hierzenberger, Anke; Bayer, Bernhard C.; Aldazabal, Iñigo; Kazansky, Andrey K.; Libisch, Florian; Krasheninnikov, Arkady V.; Schleberger, Marika; Facsko, Stefan; Borisov, Andrei G.; Arnau, Andrés; Aumayr, Friedrich

    2016-12-01

    The way conduction electrons respond to ultrafast external perturbations in low dimensional materials is at the core of the design of future devices for (opto)electronics, photodetection and spintronics. Highly charged ions provide a tool for probing the electronic response of solids to extremely strong electric fields localized down to nanometre-sized areas. With ion transmission times in the order of femtoseconds, we can directly probe the local electronic dynamics of an ultrathin foil on this timescale. Here we report on the ability of freestanding single layer graphene to provide tens of electrons for charge neutralization of a slow highly charged ion within a few femtoseconds. With values higher than 1012 A cm-2, the resulting local current density in graphene exceeds previously measured breakdown currents by three orders of magnitude. Surprisingly, the passing ion does not tear nanometre-sized holes into the single layer graphene. We use time-dependent density functional theory to gain insight into the multielectron dynamics.

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

    Indian Academy of Sciences (India)

    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.

  9. Mapping multidimensional electronic structure and ultrafast dynamics with single-element detection and compressive sensing.

    Science.gov (United States)

    Spencer, Austin P; Spokoyny, Boris; Ray, Supratim; Sarvari, Fahad; Harel, Elad

    2016-01-25

    Compressive sensing allows signals to be efficiently captured by exploiting their inherent sparsity. Here we implement sparse sampling to capture the electronic structure and ultrafast dynamics of molecular systems using phase-resolved 2D coherent spectroscopy. Until now, 2D spectroscopy has been hampered by its reliance on array detectors that operate in limited spectral regions. Combining spatial encoding of the nonlinear optical response and rapid signal modulation allows retrieval of state-resolved correlation maps in a photosynthetic protein and carbocyanine dye. We report complete Hadamard reconstruction of the signals and compression factors as high as 10, in good agreement with array-detected spectra. Single-point array reconstruction by spatial encoding (SPARSE) Spectroscopy reduces acquisition times by about an order of magnitude, with further speed improvements enabled by fast scanning of a digital micromirror device. We envision unprecedented applications for coherent spectroscopy using frequency combs and super-continua in diverse spectral regions.

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

    Science.gov (United States)

    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.

  11. Imaging polyatomic molecules with ultrafast laser-induced electron diffraction (Conference Presentation)

    Science.gov (United States)

    Le, Anh-Thu; Lin, Chii-Dong

    2016-10-01

    Molecular structure determination of chemical reactions or processes has been one of the grand challenges in physics, chemistry, and biology. To image these processes, it typically requires sub-Angstrom spatial and femtosecond temporal resolutions. One of the standard imaging techniques, X-ray diffraction, however, currently suffers from temporal jitters and is available only at large facilities. Furthermore, it also suffers from very low elastic scattering cross sections, which make it difficult to apply to gas phase molecules. Another technique, ultrafast electron diffraction (UED), overcomes this low cross section problem, but the temporal resolution is still limited to hundreds of femtoseconds, mainly due to Coulomb repulsion in electron beam and velocity mismatch between laser-pump pulse and electron probe pulse in a typical pump-probe scheme. The recently proposed laser-induced electron diffraction (LIED) is based on two basic ideas. First, an electron wave packet can be generated from a target itself by an intense laser pulse and driven back within the subsequent half-cycle of the laser to rescatter from the parent ion, thus realizing a self-imaging process. Laser-free elastic differential cross sections (DCS) can then be extracted from high-energy electron spectra, as demonstrated by the Quantitative Rescattering theory (QRS). Second, the target structure information can be retrieved from the DCS. This retrieval is further simplified by using back-scattered electrons with collision energy of about 100 eV, for which the independent-atom model (IAM) can be employed to quite accurately simulate the DCS. Demonstration of ultrafast imaging with the LIED has been reported so far on simple diatomic molecules. Here we discuss recent progress in LIED with polyatomic molecules in two examples. The first one is aligned acetylene (C2H2) and the second one is benzene (C6H6). In both cases, two bond lengths, C-C and C-H have been successfully retrieved. For even more

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  13. Ultrafast electron and hole transfer in bulk heterojunctions of low-bandgap polymers

    Science.gov (United States)

    Kozlov, Oleg V.; Pavelyev, Vlad G.; de Gier, Hilde D.; Havenith, Remco W. A.; van Loosdrecht, Paul H. M.; Hummelen, Jan C.; Pshenichnikov, Maxim S.

    2016-12-01

    In modern bulk heterojunction (BHJ) organic solar cells, blends of low-bandgap polymer and [70]PCBM acceptor are used in the active layer. In this combination, the polymer absorbs photons from the red and near-IR parts of the solar spectrum, while the blue and near-UV photons are harvested by [70]PCBM. As a result, both electron transfer from polymer to [70]PCBM and hole transfer from [70]PCBM to polymer are of utmost importance in free charge generation and have to be optimized simultaneously. Here we study electron and hole transfer processes in BHJ blends of two low-bandgap polymers, BTT-DPP and PCPDTBT, by ultrafast photoinduced spectroscopy (PIA). By tracking the PIA dynamics, we observed substantially different charge separation pathways in BHJs of the two polymers with [70]PCBM. From the photoinduced anisotropy dynamics, we demonstrated that in the PCPDTBT:[70]PCBM system both electron and hole transfer processes are highly efficient, while in the BTTBPP:[ 70]PCBM electron transfer is blocked due to the unfortunate energy level alignment leaving hole transfer the only pathway to free charge generation. Calculations at the density functional theory level are used to gain more insight into our findings. The presented results highlight the importance of the energy level alignment on the charge separation process.

  14. Ultrafast Electron Transfer Between Dye and Catalyst on a Mesoporous NiO Surface.

    Science.gov (United States)

    Brown, Allison M; Antila, Liisa J; Mirmohades, Mohammad; Pullen, Sonja; Ott, Sascha; Hammarström, Leif

    2016-07-01

    The combination of molecular dyes and catalysts with semiconductors into dye-sensitized solar fuel devices (DSSFDs) requires control of efficient interfacial and surface charge transfer between the components. The present study reports on the light-induced electron transfer processes of p-type NiO films cosensitized with coumarin C343 and a bioinspired proton reduction catalyst, [FeFe](mcbdt)(CO)6 (mcbdt = 3-carboxybenzene-1,2-dithiolate). By transient optical spectroscopy we find that ultrafast interfacial electron transfer (τ ≈ 200 fs) from NiO to the excited C343 ("hole injection") is followed by rapid (t1/2 ≈ 10 ps) and efficient surface electron transfer from C343(-) to the coadsorbed [FeFe](mcbdt)(CO)6. The reduced catalyst has a clear spectroscopic signature that persists for several tens of microseconds, before charge recombination with NiO holes occurs. The demonstration of rapid surface electron transfer from dye to catalyst on NiO, and the relatively long lifetime of the resulting charge separated state, suggests the possibility to use these systems for photocathodes on DSSFDs.

  15. Calculation of Linear Dichroism in the Ce 4d-Core XAS and 4f Electronic State of CeRh3B2

    Science.gov (United States)

    Jo, Takeo; Imada, Shin

    1990-07-01

    Linear dichroism in Ce 4d-core photoabsorption for CeRh3B2 with a hexagonal structure is discussed on the basis of an impurity Anderson model. The model takes into account the hybridization between the 4f orbit and conduction band states, multiplets arising from electrostatic interactions between electrons and crystalline anisotropy. In the paramagnetic state of the compound, the difference in the multiplet structure of 4d XAS is calculated between two incident beams with polarizations parallel and perpendicular to the c-axis with varying the crystalline field to increase the occupancy of the 4f state with the azimuthal quantum number m{=}0. The result shows that the dichroism is a promising characteristic to check recent theoretical predictions on the occupancy of the 4f state with m{=}0 in CeRh3B2 and therefore, to measure the crystal anisotropy.

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

    Indian Academy of Sciences (India)

    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.

  17. Ultrafast studies of excess electrons in liquid acetonitrile: revisiting the solvated electron/solvent dimer anion equilibrium.

    Science.gov (United States)

    Doan, Stephanie C; Schwartz, Benjamin J

    2013-04-25

    We examine the ultrafast relaxation dynamics of excess electrons injected into liquid acetonitrile using air- and water-free techniques and compare our results to previous work on this system [Xia, C. et al. J. Chem. Phys. 2002, 117, 8855]. Excess electrons in liquid acetonitrile take on two forms: a "traditional" solvated electron that absorbs in the near-IR, and a solvated molecular dimer anion that absorbs weakly in the visible. We find that excess electrons initially produced via charge-transfer-to-solvent excitation of iodide prefer to localize as solvated electrons, but that there is a subsequent equilibration to form the dimer anion on an ~80 ps time scale. The spectral signature of this interconversion between the two forms of the excess electron is a clear isosbestic point. The presence of the isosbestic point makes it possible to fully deconvolute the spectra of the two species. We find that solvated molecular anion absorbs quite weakly, with a maximum extinction coefficient of ~2000 M(-1)cm(-1). With the extinction coefficient of the dimer anion in hand, we are also able to determine the equilibrium constant for the two forms of excess electron, and find that the molecular anion is favored by a factor of ~4. We also find that relatively little geminate recombination takes place, and that the geminate recombination that does take place is essentially complete within the first 20 ps. Finally, we show that the presence of small amounts of water in the acetonitrile can have a fairly large effect on the observed spectral dynamics, explaining the differences between our results and those in previously published work.

  18. New Quasi Low-Dimensional 4d and 5d Transition Metal Oxides with Correlated Electronic Properties - Synthesis and Characterizations

    Science.gov (United States)

    2016-02-17

    Strong Electron Hybridization and Fermi-to-Non-Fermi Liquid Transition in LaCu, Chemistry of Materials, (01 2015): 211. doi: 10.1021/cm503781s...Robert Paria Sena, Joke Hadermann, Gabriel Kotliar, Martha Greenblatt. Hole Doping and Structural Transformation in CsTl, Inorganic Chemistry , (02...PbMn(IV)TeO6: A New Noncentrosymmetric Layered Honeycomb Magnetic Oxide, Inorganic Chemistry , (02 2016): 1333. doi: 10.1021/acs.inorgchem.5b02677

  19. A systematic study of thermodynamic and transport properties of layered 4d and 5d correlated electron systemsph.d

    Science.gov (United States)

    Chikara, Shalinee

    Correlated electron materials have been at the forefront of condensed matter research in the past couple of decades. Correlation in materials, especially, with open d and f electronic shells often lead to very exciting and intriguing phenomenon like high temperature superconductivity, Mott metal-insulator transition, colossal magnetoresistance (CMR). This thesis focuses on triple-layered Sr4Ru3O10, Sr substituted double layered (Ca1 - xAx) 3Ru2O7 (A = Ba, Sr) and 5d system Sr2IrO4 and Sr3Ir2O7. Triple-layered Sr4Ru3O10 displays interesting phenomena ranging from quantum oscillations, tunneling magnetoresistance, unusual low temperature specific heat, strong spin-lattice coupling to switching behavior. The central feature, however, is the unique borderline magnetism: along the c-axis. Sr4Ru3O10 shows spontaneous ferromagnetism, indicating a strong Coulomb exchange interaction, U and a large density of states at the Fermi surface, g( EF), hence Ug(EF) ≥ 1 (Stoner criterion). But within the ab-plane it features a pronounced peak in magnetization and a first-order metamagnetic transition. The coexistence of the interlayer ferromagnetism and the intralayer metamagnetism makes Sr4Ru3O10 a really unique system. Also, in this thesis the spin-valve behavior exhibited by impurity doping at the Ca site by Ba and Sr in the double layered Ca3Ru2O 7 is reported. Spin valve effect is a phenomenon only realized in multilayer thin films. Here, spin valve is observed in bulk single crystals of impurity doped Ca3Ru2O7, Ca3(Ru 1-xCrx) 2O7 and (Ca1 - xAx) 3Ru2O7 (A = Ba, Sr). 5d Iridates are expected to be more metallic and less magnetic than their 3d and 4f counterparts because of the extended 5d orbitals. In marked contrast, many iridates are magnetic insulators with exotic properties. The focus in this thesis is on Sr2IrO4 which diplays a novel Jeff = 1=2 Mott state. Magnetic, electrical, and thermal measurements on single-crystals of Sr2IrO4, reveal a novel giant magneto

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

    Indian Academy of Sciences (India)

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

    Directory of Open Access Journals (Sweden)

    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.

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

    CERN Document Server

    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.

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

    Science.gov (United States)

    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.

  4. Evidences from electron momentum spectroscopy for ultra-fast charge transfers and structural reorganizations in a floppy molecule: Ethanol

    Energy Technology Data Exchange (ETDEWEB)

    Deleuze, Michael S; Hajgato, Balazs; Morini, Filippo, E-mail: michael.deleuze@uhasselt.b [Theoretical Chemistry, Department SBG, Hasselt University, Agoralaan Gebouw D, B-3590 Diepenbeek (Belgium)

    2009-11-01

    Calculations of electron momentum distributions employing advanced Dyson orbital theories and statistical thermodynamics beyond the RRHO approximation fail to quantitatively reproduce the outermost momentum profile inferred from experiments on ethanol employing high resolution Electron Momentum Spectroscopy [1]. Study of the influence of nuclear dynamics in the initial ground state and final ionized state indicates that this discrepancy between theory and experiment reflects a charge transfer occurring during an ultra-fast dissociation of the ethanol radical cation into a methyl radical and H{sub 2}C=O-H{sup +}.

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  6. 4D-QSAR investigation and pharmacophore identification of pyrrolo[2,1-c][1,4]benzodiazepines using electron conformational-genetic algorithm method.

    Science.gov (United States)

    Özalp, A; Yavuz, S Ç; Sabancı, N; Çopur, F; Kökbudak, Z; Sarıpınar, E

    2016-04-01

    In this paper, we present the results of pharmacophore identification and bioactivity prediction for pyrrolo[2,1-c][1,4]benzodiazepine derivatives using the electron conformational-genetic algorithm (EC-GA) method as 4D-QSAR analysis. Using the data obtained from quantum chemical calculations at PM3/HF level, the electron conformational matrices of congruity (ECMC) were constructed by EMRE software. The ECMC of the lowest energy conformer of the compound with the highest activity was chosen as the template and compared with the ECMCs of the lowest energy conformer of the other compounds within given tolerances to reveal the electron conformational submatrix of activity (ECSA, i.e. pharmacophore) by ECSP software. A descriptor pool was generated taking into account the obtained pharmacophore. To predict the theoretical activity and select the best subset of variables affecting bioactivities, the nonlinear least square regression method and genetic algorithm were performed. For four types of activity including the GI50, TGI, LC50 and IC50 of the pyrrolo[2,1-c][1,4] benzodiazepine series, the r(2)train, r(2)test and q(2) values were 0.858, 0.810, 0.771; 0.853, 0.848, 0.787; 0.703, 0.787, 0.600; and 0.776, 0.722, 0.687, respectively.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-01-01

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

  8. Single-shot, ultrafast diagnostics of light-speed plasma structures and accelerating GeV electrons

    Science.gov (United States)

    Chang, Yen-Yu; Shaw, Joseph M.; Welch, James; Weichman, Kathleen; Hannasch, Andrea; LaBerge, Maxwell; Henderson, Watson; Zgadzaj, Rafal; Bernstein, Aaron; Downer, Mike

    2017-03-01

    We have experimentally demonstrated ultrafast diagnostics to visualize the laser wakefield acceleration process in a single-shot mode. We measured the Faraday rotation of a probe pulse due to the magnetic field induced by GeV electrons in low-density plasmas. In addition, we improved the temporal resolution of Frequency Domain Streak Camera (FDSC) to ˜10 fs by broadening the bandwidth of the probe beam, enabling visualization of the bubble dynamics. A prototype experiment using the broad bandwidth FDSC was performed.

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

    Science.gov (United States)

    Gaudin, J; Fourment, C; Cho, B I; Engelhorn, K; Galtier, E; Harmand, M; Leguay, P M; Lee, H J; Nagler, B; Nakatsutsumi, M; Ozkan, C; Störmer, M; Toleikis, S; Tschentscher, Th; Heimann, P A; Dorchies, F

    2014-04-17

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-07-25

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

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

    KAUST Repository

    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.

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

    DEFF Research Database (Denmark)

    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...

  13. Ultrafast electron transfer from low band gap conjugated polymer to quantum dots in hybrid photovoltaic materials

    Science.gov (United States)

    Couderc, Elsa; Greaney, Matthew J.; Thornbury, William; Brutchey, Richard L.; Bradforth, Stephen E.

    2014-09-01

    Ultrafast transient absorption spectroscopy is used in conjunction with chemical doping experiments to study the photo-generation of charges in hybrid thin films composed of PCPDTBT and CdSe quantum dots. We show how we use chemical doping experiments to de-convolute the spectral signatures of the transient states in the near infrared.

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

    Energy Technology Data Exchange (ETDEWEB)

    Kassemeyer, Stephan

    2014-05-20

    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

  15. Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

    Science.gov (United States)

    Nagaya, K.; Motomura, K.; Kukk, E.; Fukuzawa, H.; Wada, S.; Tachibana, T.; Ito, Y.; Mondal, S.; Sakai, T.; Matsunami, K.; Koga, R.; Ohmura, S.; Takahashi, Y.; Kanno, M.; Rudenko, A.; Nicolas, C.; Liu, X.-J.; Zhang, Y.; Chen, J.; Anand, M.; Jiang, Y. H.; Kim, D.-E.; Tono, K.; Yabashi, M.; Kono, H.; Miron, C.; Yao, M.; Ueda, K.

    2016-04-01

    Understanding x-ray radiation damage is a crucial issue for both medical applications of x rays and x-ray free-electron-laser (XFEL) science aimed at molecular imaging. Decrypting the charge and fragmentation dynamics of nucleobases, the smallest units of a macro-biomolecule, contributes to a bottom-up understanding of the damage via cascades of phenomena following x-ray exposure. We investigate experimentally and by numerical simulations the ultrafast radiation damage induced on a nucleobase analogue (5-iodouracil) by an ultrashort (10 fs) high-intensity radiation pulse generated by XFEL at SPring-8 Angstrom Compact free electron Laser (SACLA). The present study elucidates a plausible underlying radiosensitizing mechanism of 5-iodouracil. This mechanism is independent of the exact composition of 5-iodouracil and thus relevant to other such radiosensitizers. Furthermore, we found that despite a rapid increase of the net molecular charge in the presence of iodine, and of the ultrafast release of hydrogen, the other atoms are almost frozen within the 10-fs duration of the exposure. This validates single-shot molecular imaging as a consistent approach, provided the radiation pulse used is brief enough.

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

    KAUST Repository

    Alsulami, Qana

    2015-06-25

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

  17. 4-D Photoacoustic Tomography

    Science.gov (United States)

    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.

  18. Evidence of apoptotic effects of 2,4-D and butachlor on walking catfish, Clarias batrachus, by transmission electron microscopy and DNA degradation studies.

    Science.gov (United States)

    Ateeq, Bushra; Farah, M Abul; Ahmad, Waseem

    2006-01-25

    Apoptosis or programmed cell death is characterized morphologically by chromatin condensation, cell shrinkage, fragmentation of the nucleus and cytoplasm, and consequently formation of apoptotic bodies. It has also been best characterized by the cleavage of DNA into nucleosomal size fragments of 180-200 bp or multiples of the same. Contrary to this, under extreme conditions, the cells were found to show adaptive response to apoptosis and unable to regulate their own death; necrosis is therefore predominantly observed. In the present study, we showed induction of apoptosis in Clarias batrachus due to sublethal concentration of 2,4-D and butachlor at multiple exposure time. The first phase of the study involved light microscopy (LM) and transmission electron microscopy (TEM) for ultrastructural abnormalities of the germinal tissues. While, in the second phase of the study, DNA degradation of blood and hepatic tissue was resolved on agarose gel electrophoresis. In histopathological studies, large numbers of stage II oocytes were noted for nuclear blebbing irrespective of the test chemical. Some of the butachlor-exposed oocytes showed vacuolation and electron dense cytoplasm along with thickened nuclear envelope, having close association with the lysosomes on the cytoplasmic side. Some oocytes undergo nuclear blebbing having inner dense core and translucent cytoplasm. Leydig cells were slightly hypertrophied and few appeared pycnotic, a process involving necrotic changes in which the cell nuclei were characterized by rounding up and condensation resulting in hyperchromatic staining or pycnosis. In testicular tissue, spermatogonial nuclei had irregular large clumps of heterochromatin adjoining the nuclear membrane indicating initial stage of apoptotic cell death. Electrophoretic separation resulted in a ladder pattern of blood DNA and smear like pattern of hepatic DNA. These results indicate that the above herbicides are able to induce apoptosis both at molecular as

  19. Comment on "Structural Preablation Dynamics of Graphite Observed by Ultrafast Electron Crystallography"

    OpenAIRE

    Park, Hyuk; Zuo, Jian-Min

    2010-01-01

    In a recent letter (F. Carbone, P. Baum, P. Rudolf, et al., Physical Review Letters 100, 2008), graphite is reported to undergo a c-axis contraction on the time scale of few picoseconds (ps) after ultrafast pulsed laser excitation. The velocity of lattice contraction depended on the laser fluence. Furthermore, the lattice contraction is followed by large, non-thermal, lattice expansion of several picometers (pm) after few hundreds of ps. These results were interpreted based on the position of...

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

    Energy Technology Data Exchange (ETDEWEB)

    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.

  1. Single-shot mega-electronvolt ultrafast electron diffraction for structure dynamic studies of warm dense matter

    Energy Technology Data Exchange (ETDEWEB)

    Mo, M. Z., E-mail: mmo09@slac.stanford.edu; Shen, X.; Chen, Z.; Li, R. K.; Dunning, M.; Zheng, Q.; Weathersby, S. P.; Reid, A. H.; Coffee, R.; Makasyuk, I.; Edstrom, S.; McCormick, D.; Jobe, K.; Hast, C.; Glenzer, S. H.; Wang, X. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Sokolowski-Tinten, K. [Faculty of Physics and Centre for Nanointegration Duisburg-Essen, University of Duisburg-Essen, Lotharstrasse 1, D-47048 Duisburg (Germany)

    2016-11-15

    We have developed a single-shot mega-electronvolt ultrafast-electron-diffraction system to measure the structural dynamics of warm dense matter. The electron probe in this system is featured by a kinetic energy of 3.2 MeV and a total charge of 20 fC, with the FWHM pulse duration and spot size at sample of 350 fs and 120 μm respectively. We demonstrate its unique capability by visualizing the atomic structural changes of warm dense gold formed from a laser-excited 35-nm freestanding single-crystal gold foil. The temporal evolution of the Bragg peak intensity and of the liquid signal during solid-liquid phase transition are quantitatively determined. This experimental capability opens up an exciting opportunity to unravel the atomic dynamics of structural phase transitions in warm dense matter regime.

  2. Excited states in electron-transfer reaction products: ultrafast relaxation dynamics of an isolated acceptor radical anion.

    Science.gov (United States)

    Horke, Daniel A; Roberts, Gareth M; Verlet, Jan R R

    2011-08-04

    The spectroscopy and ultrafast relaxation dynamics of excited states of the radical anion of a representative charge-transfer acceptor molecule, 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane, have been studied in the gas phase using time-resolved photoelectron spectroscopy. The photoelectron spectra reveal that at least two anion excited states are bound. Time-resolved studies show that both excited states are very short-lived and internally convert to the anion ground state, with the lower energy state relaxing within 200 fs and a near-threshold valence-excited state relaxing on a 60 fs time scale. These excited states, and in particular the valence-excited state, present efficient pathways for electron-transfer reactions in the highly exergonic inverted region which commonly displays rates exceeding predictions from electron-transfer theory.

  3. Ultrafast and nanoscale diodes

    Science.gov (United States)

    Zhang, Peng; Lau, Y. Y.

    2016-10-01

    Charge carrier transport across interfaces of dissimilar materials (including vacuum) is the essence of all electronic devices. Ultrafast charge transport across a nanometre length scale is of fundamental importance in the miniaturization of vacuum and plasma electronics. With the combination of recent advances in electronics, photonics and nanotechnology, these miniature devices may integrate with solid-state platforms, achieving superior performance. This paper reviews recent modelling efforts on quantum tunnelling, ultrafast electron emission and transport, and electrical contact resistance. Unsolved problems and challenges in these areas are addressed.

  4. Chapter 4 Electron transfer in respiratory complexes resolved by an ultra-fast freeze-quench approach.

    Science.gov (United States)

    Belevich, Nikolai P; Verkhovskaya, Marina L; Verkhovsky, Michael I

    2009-01-01

    The investigation of the molecular mechanism of the respiratory chain complexes requires determination of the time-dependent evolution of the catalytic cycle intermediates. The ultra-fast freeze-quench approach makes possible trapping such intermediates with consequent analysis of their chemical structure by means of different physical spectroscopic methods (e.g., EPR, optic, and Mössbauer spectroscopies). This chapter presents the description of a setup that allows stopping the enzymatic reaction in the time range from 100 microsec to tens of msec. The construction and production technology of the mixer head, ultra-fast freezing device, and accessories required for collecting a sample are described. Ways of solving a number of problems emerging on freezing of the reaction mixture and preparing the samples for EPR spectroscopy are proposed. The kinetics of electron transfer reaction in the first enzyme of the respiratory chain, Complex I (NADH: ubiquinone oxidoreductase), is presented as an illustration of the freeze-quench approach. Time-resolved EPR spectra indicating the redox state of FeS clusters of the wild-type and mutant (R274A in subunit NuoCD) Complex I from Escherichia coli are shown.

  5. Ultrafast Magnetic Light

    CERN Document Server

    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.

  6. Ultrafast internal conversion of excited cytosine via the lowest pipi electronic singlet state.

    Science.gov (United States)

    Merchán, Manuela; Serrano-Andrés, Luis

    2003-07-09

    Computational evidence at the CASPT2 level supports that the lowest excited state pipi* contributes to the S1/S0 crossing responsible for the ultrafast decay of singlet excited cytosine. The computed radiative lifetime, 33 ns, is consistent with the experimentally derived value, 40 ns. The nOpi* state does not play a direct role in the rapid repopulation of the ground state; it is involved in a S2/S1 crossing. Alternative mechanisms through excited states pisigma* or nNpi* are not competitive in cytosine.

  7. Probing ultrafast dynamics in electronic structure of epitaxial Gd(0 0 0 1) on W(1 1 0)

    Energy Technology Data Exchange (ETDEWEB)

    Beaulieu, Nathan [Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin BP 48, 91192 Gif-sur-Yvette Cedex (France); Malinowski, Gregory [Laboratoire de Physique des Solides, Université Paris Sud, Orsay (France); Bendounan, Azzedine; Silly, Mathieu G.; Chauvet, Christian [Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin BP 48, 91192 Gif-sur-Yvette Cedex (France); Krizmancic, Damjan [Instituto Officina dei Materiali (IOM)-CNR Laboratorio TASC, in Area Science Park S.S.14, Km 163.5, I-34149 Trieste (Italy); Sirotti, Fausto [Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin BP 48, 91192 Gif-sur-Yvette Cedex (France)

    2013-08-15

    Highlights: •Study of the magnetism of epitaxial Gd(0 0 0 1)/W(1 1 0). •Study of Gd(0 0 0 1) band structure as a function of the temperature. •Study of the Gd magnetism dynamics probing the M5 edge. -- Abstract: The electronic and magnetic properties of Gd have been studied using time- and angle-resolved photoelectron spectroscopy employing laser pump and synchrotron radiation probe pulses. The static temperature evolution of the valence band and more precisely, the 5d6s exchange splitting is reported. Ultrafast demagnetization is measured using dichroic resonant Auger spectroscopy. Remarkably, a complete demagnetization is observed followed up by a non-monotonic recovery that could be associated to magnetization oscillations.

  8. Tuning of magnetic optical response in a dielectric nanoparticle by ultrafast photo-injection of dense electron-hole plasma

    CERN Document Server

    Makarov, Sergey; Mukhin, Ivan; Mozharov, Alexey; Milichko, Valentin; Krasnok, Alexander; Belov, Pavel

    2015-01-01

    We propose a novel approach for efficient tuning of optical properties of a high refractive index subwavelength nanoparticle with a magnetic Mie-type resonance by means of femtosecond laser irradiation. This concept is based on ultrafast photo-injection of dense (>10^20 cm^-3) 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 scattering diagram and scattering cross section. We experimentally demonstrate 20 % tuning of reflectance of a single silicon nanoparticle by femtosecond laser pulses with wavelength in the vicinity of the magnetic dipole resonance. Such single-particle nanodevice enables to design fast and ultracompact optical switchers and modulators.

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

    Science.gov (United States)

    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.

  10. Space charge effect of the time-dependent ultrafast laser excited electron emission from a metal surface

    CERN Document Server

    Liu, Yangjie

    2013-01-01

    A model has been constructed to the study the transition of ultrafast laser excited electron emission from a metallic surface to the space charge limited (SCL) regime. By considering the time-dependent emission process by L. Wu et al. [Phys. Rev. B.78 224112 (2008)], we include the space charge effect which will affect the barrier at the emitting surface. At the high laser field, it is found that space charge effect cannot be ignored and the SCL current emission is reached. The threshold of the laser field to reach the SCL regime is determined. Our calculations agree well with particle-in-cell simulation results. This model is also compared with the classical short pulse SCL current model by A. Valfellset al. [Phys. Plasmas 9, 2377 (2002)].

  11. Triplet exciton dissociation and electron extraction in graphene-templated pentacene observed with ultrafast spectroscopy.

    Science.gov (United States)

    McDonough, Thomas J; Zhang, Lushuai; Roy, Susmit Singha; Kearns, Nicholas M; Arnold, Michael S; Zanni, Martin T; Andrew, Trisha L

    2017-02-08

    We compare the ultrafast dynamics of singlet fission and charge generation in pentacene films grown on glass and graphene. Pentacene grown on graphene is interesting because it forms large crystals with the long axis of the molecules "lying-down" (parallel to the surface). At low excitation fluence, spectra for pentacene on graphene contain triplet absorptions at 507 and 545 nm and no bleaching at 630 nm, which we show is due to the orientation of the pentacene molecules. We perform the first transient absorption anisotropy measurements on pentacene, observing negative anisotropy of the 507 and 545 nm peaks, consistent with triplet absorption. A broad feature at 853 nm, observed on both glass and graphene, is isotropic, suggesting hole absorption. At high fluence, there are additional features, whose kinetics and anisotropies are not explained by heating, that we assign to charge generation; we propose a polaron pair absorption at 614 nm. The lifetimes are shorter at high fluence for both pentacene on glass and graphene, indicative of triplet-triplet annihilation that likely enhances charge generation. The anisotropy decays more slowly for pentacene on graphene than on glass, in keeping with the smaller domain size observed via atomic force microscopy. Coherent acoustic phonons are observed for pentacene on graphene, which is a consequence of more homogeneous domains. Measuring the ultrafast dynamics of pentacene as a function of molecular orientation, fluence, and polarization provides new insight to previous spectral assignments.

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

    DEFF Research Database (Denmark)

    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...

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

    DEFF Research Database (Denmark)

    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...

  14. Role of thermal excitation in ultrafast energy transfer in chlorosomes revealed by two-dimensional electronic spectroscopy.

    Science.gov (United States)

    Jun, Sunhong; Yang, Cheolhee; Kim, Tae Wu; Isaji, Megumi; Tamiaki, Hitoshi; Ihee, Hyotcherl; Kim, Jeongho

    2015-07-21

    Chlorosomes are the largest light harvesting complexes in nature and consist of many bacteriochlorophyll pigments forming self-assembled J-aggregates. In this work, we use two-dimensional electronic spectroscopy (2D-ES) to investigate ultrafast dynamics of excitation energy transfer (EET) in chlorosomes and their temperature dependence. From time evolution of the measured 2D electronic spectra of chlorosomes, we directly map out the distribution of the EET rate among the manifold of exciton states in a 2D energy space. In particular, it is found that the EET rate varies gradually depending on the energies of energy-donor and energy-acceptor states. In addition, from comparative 2D-ES measurements at 77 K and room temperature, we show that the EET rate exhibits subtle dependence on both the exciton energy and temperature, demonstrating the effect of thermal excitation on the EET rate. This observation suggests that active thermal excitation at room temperature prevents the excitation trapping at low-energy states and thus promotes efficient exciton diffusion in chlorosomes at ambient temperature.

  15. Coherent phonon excitation and linear thermal expansion in structural dynamics and ultrafast electron diffraction of laser-heated metals

    Science.gov (United States)

    Tang, Jau

    2008-04-01

    In this study, we examine the ultrafast structural dynamics of metals induced by a femtosecond laser-heating pulse as probed by time-resolved electron diffraction. Using the two-temperature model and the Grüneisen relationship we calculate the electron temperature, phonon temperature, and impulsive force at each atomic site in the slab. Together with the Fermi-Pasta-Ulam anharmonic chain model we calculate changes of bond distance and the peak shift of Bragg spots or Laue rings. A laser-heated thin slab is shown to exhibit "breathing" standing-wave behavior, with a period equal to the round-trip time for sound wave and a wavelength twice the slab thickness. The peak delay time first increases linearly with the thickness (<70nm for aluminum and <200nm for gold), but becomes less dependent if further thickness increases. Coherent phonon excitation and propagation from the stressed bulk atoms due to impulsive forces as well as the linear thermal expansion due to lattice temperature jump are shown to contribute to the overall structural changes. Differences between these two mechanisms and their dependence on film thickness and other factors are discussed.

  16. A study of ultrafast electron diffusion kinetics in ultrashort-pulse laser ablation of metals

    Institute of Scientific and Technical Information of China (English)

    Yang Jian-Jun; Liu Wei-Wei; Zhu Xiao-Nong

    2007-01-01

    Temperature dependence of the electron diffusion in metallic targets, where the electron-electron collision is the dominant process, is investigated with the help of an extended two-temperature model. In sharp contrast to the low electron temperature case, where only the electron-phonon collisions are commonly considered, the electron diffusion process underlying the high electron temperatures evolves dramatically different in both temporal and spatial domains.Calculated results of the ablation yield at different pulse durations are presented for a copper plate impinged by ultrashort laser pulses with energy fluences ranging from 0.1 J/cm2 to 10 J/cm2. The excellent agreement between the simulation results and the experimental data indicates the significant role of electron-electron collisions in material ablations using intense ultrashort laser pulses.

  17. Direct spectroscopic evidence of ultrafast electron transfer from a low band gap polymer to CdSe quantum dots in hybrid photovoltaic thin films.

    Science.gov (United States)

    Couderc, Elsa; Greaney, Matthew J; Brutchey, Richard L; Bradforth, Stephen E

    2013-12-11

    Ultrafast transient absorption spectroscopy is used to study charge transfer dynamics in hybrid films composed of the low band gap polymer PCPDTBT and CdSe quantum dots capped with tert-butylthiol ligands. By selectively exciting the polymer, a spectral signature for electrons on the quantum dots appears on ultrafast time scales (≲ 65 fs), which indicates ultrafast electron transfer. From this time scale, the coupling between the polymer chains and the quantum dots is estimated to be J ≳ 17 meV. The reduced quantum dot acceptors exhibit an unambiguous spectral bleach signature, whose amplitude allows for the first direct calculation of the absolute electron transfer yield in a hybrid solar cell (82 ± 5%). We also show that a limitation of the hybrid system is rapid and measurable geminate recombination due to the small separation of the initial charge pair. The fast recombination is consistent with the internal quantum efficiency of the corresponding solar cell. We therefore have identified and quantified a main loss mechanism in this type of third generation solar cell.

  18. Ultrafast Charge Recombination Dynamics in Ternary Electron Donor-Acceptor Complexes: (Benzene)2-Tetracyanoethylene Complexes.

    Science.gov (United States)

    Chiu, Chih-Chung; Hung, Chih-Chang; Cheng, Po-Yuan

    2016-12-08

    The charge-transfer (CT) state relaxation dynamics of the binary (1:1) and ternary (2:1) benzene/tetracyanoethylene (BZ/TCNE) complexes are reported. Steady-state and ultrafast time-resolved broadband fluorescence (TRFL) spectra of TCNE dissolved in a series of BZ/CCl4 mixed solvents are measured to elucidate the spectroscopic properties of the BZ/TCNE complexes and their CT-state relaxation dynamics. Both steady-state and TRFL spectra exhibit marked BZ concentration dependences, which can be attributed to the formation of two types of 2:1 complexes in the ground and excited states. By combining with the density functional theory (DFT) calculations, it was concluded that the BZ concentration dependence of the absorption spectra is mainly due to the formation and excitation of the sandwich-type 2:1 ternary complexes, whereas the changes in fluorescence spectra at high BZ concentrations are due to the formation of the asymmetric-type 2:1 ternary complex CT1 state. A unified mechanism involving both direct excitation and secondary formation of the 2:1 complexes CT states are proposed to account for the observations. The equilibrium charge recombination (CR) time constant of the 1:1 CT1 state is determined to be ∼150 ps in CCl4, whereas that of the 2:1 DDA-type CT1 state becomes ∼70 ps in 10% BZ/CCl4 and ∼34 ps in pure BZ. The CR rates and the CT1-S0 energy gap of these complexes in different solvents exhibit a correlation conforming to the Marcus inverted region. It is concluded that partial charge resonance occurring between the two adjacent BZs in the asymmetric-type 2:1 CT1-state reduces the CR reaction exothermicity and increases the CR rate.

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

    Energy Technology Data Exchange (ETDEWEB)

    Arrell, C. A., E-mail: christopher.arrell@epfl.ch; Ojeda, J.; Mourik, F. van; Chergui, M. [Laboratory of Ultrafast Spectroscopy, ISIC, Station 6, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne (Switzerland); Sabbar, M.; Gallmann, L.; Keller, U. [Physics Department, ETH Zurich, 8093 Zurich (Switzerland); Okell, W. A.; Witting, T.; Siegel, T.; Diveki, Z.; Hutchinson, S.; Tisch, J. W.G.; Marangos, J. P. [Department of Physics, The Blackett Laboratory, Imperial College, London SW7 2AZ (United Kingdom); Chapman, R. T.; Cacho, C.; Rodrigues, N.; Turcu, I. C.E.; Springate, E. [Central Laser Facility, STFC Rutherford Appleton Laboratory, Oxon OX11 0QX (United Kingdom)

    2014-10-01

    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.

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

    CERN Document Server

    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...

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

    Science.gov (United States)

    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.

  2. Quantum computers based on electron spins controlled by ultrafast off-resonant single optical pulses.

    Science.gov (United States)

    Clark, Susan M; Fu, Kai-Mei C; Ladd, Thaddeus D; Yamamoto, Yoshihisa

    2007-07-27

    We describe a fast quantum computer based on optically controlled electron spins in charged quantum dots that are coupled to microcavities. This scheme uses broadband optical pulses to rotate electron spins and provide the clock signal to the system. Nonlocal two-qubit gates are performed by phase shifts induced by electron spins on laser pulses propagating along a shared waveguide. Numerical simulations of this scheme demonstrate high-fidelity single-qubit and two-qubit gates with operation times comparable to the inverse Zeeman frequency.

  3. Optical manipulation of ultrafast electron and nuclear motion on metal surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Petek, Hrvoje

    2009-12-02

    We study the unoccupied electronic structure and dynamics of chemisorbed atoms and molecules on metal surfaces by time resolved two-photon photoemission (TR-2PP). spectroscopy, low temperature scanning tunneling microscopy (LT-STM), and theory. Our research concerns simple atomic adsorbates such as alkali and alkaline earth atoms, which provide fundamentally important models for adsorbate-surface interactions, and more complex adsorbates such as fullerenes on noble metals, which illustrate emergent interfacial properties that derive from intrinsic molecular attributes, and moleculemolecule and molecule-surface interactions. Our goal is to understand how these interactions contribute to formation of the interfacial electronic structure, and how thus formed electronic properties affect interfacial phenomena of importance to energy transduction and storage. Moreover, we explore how the interfacial electronic excitation drives dynamical phenomena such as charge transfer and surface femtochemistry.

  4. Real Time Quantification of Ultrafast Photoinduced Bimolecular Electron Transfer Rate: Direct Probing of the Transient Intermediate.

    Science.gov (United States)

    Mukherjee, Puspal; Biswas, Somnath; Sen, Pratik

    2015-08-27

    Fluorescence quenching studies through steady-state and time-resolved measurements are inadequate to quantify the bimolecular electron transfer rate in bulk homogeneous solution due to constraints from diffusion. To nullify the effect of diffusion, direct evaluation of the rate of formation of a transient intermediate produced upon the electron transfer is essential. Methyl viologen, a well-known electron acceptor, produces a radical cation after accepting an electron, which has a characteristic strong and broad absorption band centered at 600 nm. Hence it is a good choice to evaluate the rate of photoinduced electron transfer reaction employing femtosecond broadband transient absorption spectroscopy. The time constant of the aforementioned process between pyrene and methyl viologen in methanol has been estimated to be 2.5 ± 0.4 ps using the same technique. The time constant for the backward reaction was found to be 14 ± 1 ps. These values did not change with variation of concentration of quencher, i.e., methyl viologen. Hence, we can infer that diffusion has no contribution in the estimation of rate constants. However, on changing the solvent from methanol to ethanol, the time constant of the electron transfer reaction has been found to increase and has accounted for the change in solvent reorganization energy.

  5. Roadmap on ultrafast optics

    Science.gov (United States)

    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.

  6. Theory of ultrafast photoinduced electron transfer from a bulk semiconductor to a quantum dot

    Energy Technology Data Exchange (ETDEWEB)

    Rasmussen, Andrew M., E-mail: andyras@gmail.com; Ramakrishna, S.; Weiss, Emily A.; Seideman, Tamar, E-mail: t-seideman@northwestern.edu [Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208-3113 (United States)

    2014-04-14

    This paper describes analytical and numerical results from a model Hamiltonian method applied to electron transfer (ET) from a quasicontinuum (QC) of states to a set of discrete states, with and without a mediating bridge. Analysis of the factors that determine ET dynamics yields guidelines for achieving high-yield electron transfer in these systems, desired for instance for applications in heterogeneous catalysis. These include the choice of parameters of the laser pulse that excites the initial state into a continuum electronic wavepacket and the design of the coupling between the bridge molecule and the donor and acceptor. The vibrational mode on a bridging molecule between donor and acceptor has an influence on the yield of electron transfer via Franck-Condon factors, even in cases where excited vibrational states are only transiently populated. Laser-induced coherence of the initial state as well as energetic overlap is crucial in determining the ET yield from a QC to a discrete state, whereas the ET time is influenced by competing factors from the coupling strength and the coherence properties of the electronic wavepacket.

  7. Enhancement of ultrafast electron photoemission from metallic nano antennas excited by a femtosecond laser pulse

    CERN Document Server

    Gubko, M A; Ionin, A A; Kudryashov, S I; Makarov, S V; Nathala, C S R; Rudenko, A A; Seleznev, L V; Sinitsyn, D V; Treshin, I V

    2013-01-01

    We have demonstrated for the first time that an array of nanoantennas (central nanotips inside sub-micron pits) on an aluminum surface, fabricated using a specific double-pulse femtosecond laser irradiation scheme, results in a 28-fold enhancement of the non-linear (three-photon) electron photoemission yield, driven by a third intense IR femtosecond laser pulse. The supporting numerical electrodynamic modeling indicates that the electron emission is increased not owing to a larger effective aluminum surface, but due to instant local electromagnetic field enhancement near the nanoantenna, contributed by both the tip's lightning rod effect and the focusing effect of the pit as a microreflector and annular edge as a plasmonic lens.

  8. Subwavelength ripples adjustment based on electron dynamics control by using shaped ultrafast laser pulse trains.

    Science.gov (United States)

    Jiang, Lan; Shi, Xuesong; Li, Xin; Yuan, Yanping; Wang, Cong; Lu, Yongfeng

    2012-09-10

    This study reveals that the periods, ablation areas and orientations of periodic surface structures (ripples) in fused silica can be adjusted by using designed femtosecond (fs) laser pulse trains to control transient localized electron dynamics and corresponding material properties. By increasing the pulse delays from 0 to 100 fs, the ripple periods are changed from ~550 nm to ~255 nm and the orientation is rotated by 90°. The nearwavelength/subwavelength ripple periods are close to the fundamental/second-harmonic wavelengths in fused silica respectively. The subsequent subpulse of the train significantly impacts free electron distributions generated by the previous subpulse(s), which might influence the formation mechanism of ripples and the surface morphology.

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

    KAUST Repository

    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.

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

    Directory of Open Access Journals (Sweden)

    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.

  11. Design and implementation of an optimal laser pulse front tilting scheme for ultrafast electron diffraction in reflection geometry with high temporal resolution

    Directory of Open Access Journals (Sweden)

    Francesco Pennacchio

    2017-07-01

    Full Text Available Ultrafast electron diffraction is a powerful technique to investigate out-of-equilibrium atomic dynamics in solids with high temporal resolution. When diffraction is performed in reflection geometry, the main limitation is the mismatch in group velocity between the overlapping pump light and the electron probe pulses, which affects the overall temporal resolution of the experiment. A solution already available in the literature involved pulse front tilt of the pump beam at the sample, providing a sub-picosecond time resolution. However, in the reported optical scheme, the tilted pulse is characterized by a temporal chirp of about 1 ps at 1 mm away from the centre of the beam, which limits the investigation of surface dynamics in large crystals. In this paper, we propose an optimal tilting scheme designed for a radio-frequency-compressed ultrafast electron diffraction setup working in reflection geometry with 30 keV electron pulses containing up to 105 electrons/pulse. To characterize our scheme, we performed optical cross-correlation measurements, obtaining an average temporal width of the tilted pulse lower than 250 fs. The calibration of the electron-laser temporal overlap was obtained by monitoring the spatial profile of the electron beam when interacting with the plasma optically induced at the apex of a copper needle (plasma lensing effect. Finally, we report the first time-resolved results obtained on graphite, where the electron-phonon coupling dynamics is observed, showing an overall temporal resolution in the sub-500 fs regime. The successful implementation of this configuration opens the way to directly probe structural dynamics of low-dimensional systems in the sub-picosecond regime, with pulsed electrons.

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

    Energy Technology Data Exchange (ETDEWEB)

    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

  13. Kinetics study of ultrafast electron transfer from sensitized dyes to silver halide microcrystals

    Institute of Scientific and Technical Information of China (English)

    Yang Shao-Peng; Fan Guo-Zhi; Fan Shan-Shan; Cao Ning; Li Xiao-Wei; Jiang Xiao-Li; Fu Guang-Sheng

    2006-01-01

    Spectral sensitization micromechanism of cyanine dyes J-aggregate adsorbed on the tabular and cubic AgBr microcrystals with different dye concentrations is studied by using picosecond time-resolved fluorescence spectroscopy,and the dependences of electron transfer and spectral efficiency sensitization on different conditions are analysed in detail. With the steady spectroscopy, the wavelengths of absorption and fluorescence of J-aggregate adsorbed on AgBr microcrystals are found to shift to red relative to dye monomer. The spectrum of fluorescence has a red shift relative to the absorption peak. With the time-resolved fluorescence spectroscopy, the fluorescence decay curves of cyanine dyes J-aggregate adsorbed on the tabular and cubic AgBr grains are found to be fitted well by a double-exponential decay function. The fitting curves consist of a fast and a slow component. Because of the large amplitude of the fast component, this fast decay should be attributable mainly to the electron transfer from J-aggregate of dye to a conduction band of AgBr.

  14. Ultrafast energy and electron transfers in structurally well addressable BODIPY-porphyrin-fullerene polyads.

    Science.gov (United States)

    Gao, Di; Aly, Shawkat M; Karsenti, Paul-Ludovic; Brisard, Gessie; Harvey, Pierre D

    2017-01-25

    Two electron transfer polyads built upon [C60]-[ZnP]-[BODIPY] (1) and [ZnP]-[ZnP](-[BODIPY])(-[C60]) (2), where [C60] = N-methyl-2-phenyl-3,4-fulleropyrrolidine, [BODIPY] = boron dipyrromethane, and [ZnP] = zinc(ii) porphyrin, were synthesized along with their corresponding energy transfer polyads [ZnP]-[BODIPY] (1a) and [ZnP]-[ZnP]-[BODIPY] (2a) as well as relevant models. These polyads were studied using cyclic voltammetry, DFT computations, steady state and time-resolved fluorescence spectroscopy, and fs transient absorption spectroscopy. The rates for energy transfer, kET, [BODIPY]* → [ZnP] are ∼2.8 × 10(10) s(-1) for both 1a and 2a, with an efficiency of 99%. Concurrently, the fast appearance of the [C60](-)˙ anion for 1 and 2 indicates that the charge separation occurs on the 20-30 ps timescale with the rates of electron transfer, ket, [ZnP]*/[C60] → [ZnP](+)˙/[C60](-)˙ of ∼0.9 × 10(10) to ∼3.8 × 10(10) s(-1). The latter value is among the fastest for these types of polyads. Conversely, the charge recombination operates on the ns timescale. These rates are comparable to or faster than those reported for other more flexible [C60]-[ZnP]-[BODIPY] polyads, which can be rationalized by the donor-acceptor separations.

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

    Directory of Open Access Journals (Sweden)

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

    Energy Technology Data Exchange (ETDEWEB)

    Radu, I.E.

    2006-03-15

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

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

    Science.gov (United States)

    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

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

    Energy Technology Data Exchange (ETDEWEB)

    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. Ultrafast electron kinetics in short pulse laser-driven dense hydrogen

    Science.gov (United States)

    Zastrau, U.; Sperling, P.; Fortmann-Grote, C.; Becker, A.; Bornath, T.; Bredow, R.; Döppner, T.; Fennel, T.; Fletcher, L. B.; Förster, E.; Göde, S.; Gregori, G.; Harmand, M.; Hilbert, V.; Laarmann, T.; Lee, H. J.; Ma, T.; Meiwes-Broer, K. H.; Mithen, J. P.; Murphy, C. D.; Nakatsutsumi, M.; Neumayer, P.; Przystawik, A.; Skruszewicz, S.; Tiggesbäumker, J.; Toleikis, S.; White, T. G.; Glenzer, S. H.; Redmer, R.; Tschentscher, T.

    2015-11-01

    Dense cryogenic hydrogen is heated by intense femtosecond infrared laser pulses at intensities of {10}15-{10}16 W cm-2. Three-dimensional particle-in-cell (PIC) simulations predict that this heating is limited to the skin depth, causing an inhomogeneously heated outer shell with a cold core and two prominent temperatures of about 25 and 40 {eV} for simulated delay times up to +70 {fs} after the laser pulse maximum. Experimentally, the time-integrated emitted bremsstrahlung in the spectral range of 8-18 nm was corrected for the wavelength-dependent instrument efficiency. The resulting spectrum cannot be fit with a single temperature bremsstrahlung model, and the best fit is obtained using two temperatures of about 13 and 30 eV. The lower temperatures in the experiment can be explained by missing energy-loss channels in the simulations, as well as the inclusion of hot, non-Maxwellian electrons in the temperature calculation. We resolved the time-scale for laser-heating of hydrogen, and PIC results for laser-matter interaction were successfully tested against the experiment data.

  20. Ultrafast probing of ejection dynamics of Rydberg atoms and molecular fragments from electronically excited helium nanodroplets.

    Science.gov (United States)

    Bünermann, Oliver; Kornilov, Oleg; Haxton, Daniel J; Leone, Stephen R; Neumark, Daniel M; Gessner, Oliver

    2012-12-07

    The ejection dynamics of Rydberg atoms and molecular fragments from electronically excited helium nanodroplets are studied with time-resolved extreme ultraviolet ion imaging spectroscopy. At excitation energies of 23.6 ± 0.2 eV, Rydberg atoms in n = 3 and n = 4 states are ejected on different time scales and with significantly different kinetic energy distributions. Specifically, n = 3 Rydberg atoms are ejected with kinetic energies as high as 0.85 eV, but their appearance is delayed by approximately 200 fs. In contrast, n = 4 Rydberg atoms appear within the time resolution of the experiment with considerably lower kinetic energies. Major features in the Rydberg atom kinetic energy distributions for both principal quantum numbers can be described within a simple elastic scattering model of localized perturbed atomic Rydberg atoms that are expelled from the droplet due to their repulsive interaction with the surrounding helium bath. Time-dependent kinetic energy distributions of He(2) (+) and He(3) (+) ions are presented that support the formation of molecular ions in an indirect droplet ionization process and the ejection of neutral Rydberg dimers on a similar time scale as the n = 3 Rydberg atoms.

  1. Ultrafast laser induced electronic and structural modifications in bulk fused silica

    Science.gov (United States)

    Mishchik, K.; D'Amico, C.; Velpula, P. K.; Mauclair, C.; Boukenter, A.; Ouerdane, Y.; Stoian, R.

    2013-10-01

    Ultrashort laser pulses can modify the inner structure of fused silica, generating refractive index changes varying from soft positive (type I) light guiding forms to negative (type II) values with void presence and anisotropic sub-wavelength modulation. We investigate electronic and structural material changes in the type I to type II transition via coherent and incoherent secondary light emission reflecting free carrier behavior and post-irradiation material relaxation in the index change patterns. Using phase contrast microscopy, photoluminescence, and Raman spectroscopy, we determine in a space-resolved manner defect formation, redistribution and spatial segregation, and glass network reorganization paths in conditions marking the changeover between type I and type II photoinscription regimes. We first show characteristic patterns of second harmonic generation in type I and type II traces, indicating the collective involvement of free carriers and polarization memory. Second, incoherent photoemission from resonantly and non-resonantly excited defect states reveals accumulation of non-bridging oxygen hole centers (NBOHCs) in positive index domains and oxygen deficiency centers (ODCs) with O2- ions segregation in void-like regions and in the nanostructured domains, reflecting the interaction strength. Complementary Raman investigations put into evidence signatures of the different environments where photo-chemical densification (bond rearrangements) and mechanical effects can be indicated. NBOHCs setting in before visible index changes serve as precursors for subsequent compaction build-up, indicating a scenario of cold, defect-assisted densification for the soft type I irradiation regime. Additionally, we observe hydrodynamic effects and severe bond-breaking in type II zones with indications of phase transition. These observations illuminate densification paths in fused silica in low power irradiation regimes, and equally in energetic ranges, characterized by

  2. From Femtochemistry to 4D Microscopy

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    To celebrate the 10th anniversary of the Nobel Prize for Femtochemistry,the field is overviewed with several classic examples and the new extension to Femtobiology. The revolutionary breakthrough in 4D electron microscopy is briefly introduced here and a new age to structural dynamics is rising on the horizon,an exciting time and a great opportunity for China and for the world.

  3. Excited states in electron-transfer reaction products : ultrafast relaxation dynamics of an isolated acceptor radical anion.

    OpenAIRE

    D. A. Horke; Roberts, G.M.; Verlet, J. R. R.

    2011-01-01

    The spectroscopy and ultrafast relaxation dynamics of excited states of the radical anion of a representative charge-transfer acceptor molecule, 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane, have been studied in the gas phase using time-resolved photoelectron spectroscopy. The photoelectron spectra reveal that at least two anion excited states are bound. Time-resolved studies show that both excited states are very short-lived and internally convert to the anion ground state, with the ...

  4. CHY formulae in 4d

    CERN Document Server

    Zhang, Yong

    2016-01-01

    In this paper, we develop a rather general way to reduce integrands with polarisation involved in the Cachazo-He-Yuan formulae, such as the reduced Pfaffian and its compactification, as well as the new object for F3 amplitude. We prove that the reduced Pfaffian vanishes unless on a certain set of solutions. It leads us to build up the 4d CHY formulae using spinors, which strains off many useless solutions. The supersymmetrization is straightforward and may provide a hint to understanding ambitwistor string in 4d.

  5. Ultrafast Optical Electronics Center

    Science.gov (United States)

    1990-08-28

    probe beam, while the longitudinal crystal, fabricated of deuterated potassium dihydrogen phosphate (KD*P), is used to measure field components that are...clad between 0.1 4am p+ cap layer and a I .m n buffer layer grown on top of the semi- insulating (SI) substrate. Tunneling is only possible through the...Twenty-five periods of the double-QW structure were grown on an n -type GaAs substrate and n -type GaAs buffer layer. A semitransparent Al Schottky 11 CF

  6. Ultrafast, Light-Induced Electron Transfer in a Perylene Diimide Chromophore-Donor Assembly on TiO 2

    Energy Technology Data Exchange (ETDEWEB)

    Brennaman, M. Kyle; Norris, Michael R.; Gish, Melissa K.; Grumstrup, Erik M.; Alibabaei, Leila; Ashford, Dennis L.; Lapides, Alexander M.; Papanikolas, John M.; Templeton, Joseph L.; Meyer, Thomas J.

    2015-12-03

    Surface-bound, perylenediimide (PDI)-based molecular assemblies have been synthesized on nanocrystalline TiO2 by reaction of a dianhydride with a surface-bound aniline and succinimide bonding. In a second step, the Fe(II) polypyridyl complex [FeII(tpy-PhNH2)2]2+ was added to the outside of the film, also by succinimide bonding. Ultrafast transient absorption measurements in 0.1 M HClO4 reveal that electron injection into TiO2 by 1PDI* does not occur, but rather leads to the ultrafast formation of the redox-separated pair PDI•+,PDI•–, which decays with complex kinetics (τ1 = 0.8 ps, τ2 = 15 ps, and τ3 = 1500 ps). With the added Fe(II) polypyridyl complex, rapid (<25 ps) oxidation of Fe(II) by the PDI•+,PDI•– redox pair occurs to give Fe(III),PDI•– persisting for >400 μs in the film environment.

  7. Temperature dependence of the hydrated electron's excited-state relaxation. II. Elucidating the relaxation mechanism through ultrafast transient absorption and stimulated emission spectroscopy

    Science.gov (United States)

    Farr, Erik P.; Zho, Chen-Chen; Challa, Jagannadha R.; Schwartz, Benjamin J.

    2017-08-01

    The structure of the hydrated electron, particularly whether it exists primarily within a cavity or encompasses interior water molecules, has been the subject of much recent debate. In Paper I [C.-C. Zho et al., J. Chem. Phys. 147, 074503 (2017)], we found that mixed quantum/classical simulations with cavity and non-cavity pseudopotentials gave different predictions for the temperature dependence of the rate of the photoexcited hydrated electron's relaxation back to the ground state. In this paper, we measure the ultrafast transient absorption spectroscopy of the photoexcited hydrated electron as a function of temperature to confront the predictions of our simulations. The ultrafast spectroscopy clearly shows faster relaxation dynamics at higher temperatures. In particular, the transient absorption data show a clear excess bleach beyond that of the equilibrium hydrated electron's ground-state absorption that can only be explained by stimulated emission. This stimulated emission component, which is consistent with the experimentally known fluorescence spectrum of the hydrated electron, decreases in both amplitude and lifetime as the temperature is increased. We use a kinetic model to globally fit the temperature-dependent transient absorption data at multiple temperatures ranging from 0 to 45 °C. We find the room-temperature lifetime of the excited-state hydrated electron to be 137 ±40 fs, in close agreement with recent time-resolved photoelectron spectroscopy (TRPES) experiments and in strong support of the "non-adiabatic" picture of the hydrated electron's excited-state relaxation. Moreover, we find that the excited-state lifetime is strongly temperature dependent, changing by slightly more than a factor of two over the 45 °C temperature range explored. This temperature dependence of the lifetime, along with a faster rate of ground-state cooling with increasing bulk temperature, should be directly observable by future TRPES experiments. Our data also suggest

  8. Exploring the time-scale of photo-initiated interfacial electron transfer through first-principles interpretation of ultrafast X-ray spectroscopy (Presentation Recording)

    Science.gov (United States)

    Prendergast, David; Pemmaraju, Sri Chaitanya Das

    2015-09-01

    With the advent of X-ray free electron lasers and table-top high-harmonic-generation X-ray sources, we can now explore changes in electronic structure on ultrafast time scales -- at or less than 1ps. Transient X-ray spectroscopy of this kind provides a direct probe of relevant electronic levels related to photoinitiated processes and associated interfacial electron transfer as the initial step in solar energy conversion. However, the interpretation of such spectra is typically fraught with difficulty, especially since we rarely have access to spectral standards for nonequilibrium states. To this end, direct first-principles simulations of X-ray absorption spectra can provide the necessary connection between measurements and reliable models of the atomic and electronic structure. We present examples of modeling excited states of materials interfaces relevant to solar harvesting and their corresponding X-ray spectra in either photoemission or absorption modalities. In this way, we can establish particular electron transfer mechanisms to reveal detailed working principles of materials systems in solar applications and provide insight for improved efficiency.

  9. OSA Proceedings on Ultrafast Electronics and Optoelectronics Held in San Francisco, California on January 25 -27, 1993. Volume 14,

    Science.gov (United States)

    1993-01-27

    extrinsic = (1 + iiB )-I for (PR ýc 1 colft-or capacitance Cc, and the parasitic resistances, 2 e2e-•S e-i𔄃 for TB > 1 R•, Rc•, and R~x. where 9PB... extrinsic capacitance , Cc. = 0. In this case, the common-emitter output impedance, unilateral gain can be reduced to the following form: 76 Ultrafast...Challenges (invited) .......... 56 Robert W. Keyes and Mark B. Ketchen Ultra-Deep Submicron Si MOSFETs with fT Exceeding 100 GHz (invited

  10. Instant Cinema 4D starter

    CERN Document Server

    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.

  11. Chaos synchronization between two different 4D hyperchaotic Chen systems

    Institute of Scientific and Technical Information of China (English)

    Liu Yang-Zheng; Jiang Chang-Sheng; Lin Chang-Sheng; Jiang Yao-Mei

    2007-01-01

    This paper presents chaos synchronization between two different four-dimensional (4D) hyperchaotic Chen systems by nonlinear feedback control laws.A modified 4D hyperchaotic Chen system is obtained by changing the nonlinear function of the 4D hyperchaotic Chen system,furthermore,an electronic circuit to realize two different 4D hyperchaotic Chen systems is designed.With nonlinear feedback control method,chaos synchronization between two different 4D hyperchaotic Chen systems is achieved.Based on the stability theory,the functions of the nonlinear feedback control for synchronization of two different 4D hyperchaotic Chen systems is derived,the range of feedback gains is determined.Numerical simulations are shown to verify the theoretical results.

  12. Ultrafast biophotonics

    CERN Document Server

    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.

  13. Semiclassical study of quantum coherence and isotope effects in ultrafast electron transfer reactions coupled to a proton and a phonon bath.

    Science.gov (United States)

    Venkataraman, Charulatha

    2011-11-28

    The linearized semiclassical initial value representation is employed to describe ultrafast electron transfer processes coupled to a phonon bath and weakly coupled to a proton mode. The goal of our theoretical investigation is to understand the influence of the proton on the electronic dynamics in various bath relaxation regimes. More specifically, we study the impact of the proton on coherences and analyze if the coupling to the proton is revealed in the form of an isotope effect. This will be important in distinguishing reactions in which the proton does not undergo significant rearrangement from those in which the electron transfer is accompanied by proton transfer. Unlike other methodologies widely employed to describe nonadiabatic electron transfer, this approach treats the electronic and nuclear degrees of freedom consistently. However, due to the linearized approximation, quantum interference effects are not captured accurately. Our study shows that at small phonon bath reorganization energies, coherent oscillations and isotope effect are observed in both slow and fast bath regimes. The coherences are more substantially damped by deuterium in comparison to the proton. Further, in contrast to the dynamics of the spin-boson model, the coherences are not long-lived. At large bath reorganization energies, the decay is incoherent in the slow and fast bath regimes. In this case, the extent of the isotope effect depends on the relative relaxation timescales of the proton mode and the phonon bath. The isotope effect is magnified for baths that relax on picosecond timescales in contrast to baths that relax in femtoseconds.

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

    KAUST Repository

    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.

  15. A general method for baseline-removal in ultrafast electron powder diffraction data using the dual-tree complex wavelet transform

    Science.gov (United States)

    René de Cotret, Laurent P.; Siwick, Bradley J.

    2016-01-01

    The general problem of background subtraction in ultrafast electron powder diffraction (UEPD) is presented with a focus on the diffraction patterns obtained from materials of moderately complex structure which contain many overlapping peaks and effectively no scattering vector regions that can be considered exclusively background. We compare the performance of background subtraction algorithms based on discrete and dual-tree complex (DTCWT) wavelet transforms when applied to simulated UEPD data on the M1–R phase transition in VO2 with a time-varying background. We find that the DTCWT approach is capable of extracting intensities that are accurate to better than 2% across the whole range of scattering vector simulated, effectively independent of delay time. A Python package is available. PMID:28083543

  16. Through-Space Ultrafast Photoinduced Electron Transfer Dynamics of a C 70 -Encapsulated Bisporphyrin Covalent Organic Polyhedron in a Low-Dielectric Medium

    Energy Technology Data Exchange (ETDEWEB)

    Ortiz, Michael; Cho, Sung; Niklas, Jens; Kim, Seonah; Poluektov, Oleg G.; Zhang, Wei; Rumbles, Garry; Park, Jaehong

    2017-03-16

    Ultrafast photoinduced electron transfer (PIET) dynamics of a C70-encapsulated bisporphyrin covalent organic polyhedron hybrid (C70@COP-5) is studied in a nonpolar toluene medium with fluorescence and transient absorption spectroscopies. This structurally rigid donor (D)-acceptor (A) molecular hybrid offers a new platform featuring conformationally predetermined cofacial D-A orientation with a fixed edge-to-edge separation, REE (2.8 A), without the aid of covalent bonds. Sub-picosecond PIET (tET = 0.4 ps) and very slow charge recombination (tCR ~600 ps) dynamics are observed. The origin of these dynamics is discussed in terms of enhanced D-A coupling (V = 675 cm-1) and extremely small reorganization energy (..lambda.. ~ 0.18 eV), induced by the intrinsic structural rigidity of the C70@COP-5 complex.

  17. A general method for baseline-removal in ultrafast electron powder diffraction data using the dual-tree complex wavelet transform

    Directory of Open Access Journals (Sweden)

    Laurent P. René de Cotret

    2017-07-01

    Full Text Available The general problem of background subtraction in ultrafast electron powder diffraction (UEPD is presented with a focus on the diffraction patterns obtained from materials of moderately complex structure which contain many overlapping peaks and effectively no scattering vector regions that can be considered exclusively background. We compare the performance of background subtraction algorithms based on discrete and dual-tree complex (DTCWT wavelet transforms when applied to simulated UEPD data on the M1–R phase transition in VO2 with a time-varying background. We find that the DTCWT approach is capable of extracting intensities that are accurate to better than 2% across the whole range of scattering vector simulated, effectively independent of delay time. A Python package is available.

  18. Ultrafast THz Saturable Absorption in Doped Semiconductors

    DEFF Research Database (Denmark)

    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....

  19. PREFACE: Ultrafast biophotonics Ultrafast biophotonics

    Science.gov (United States)

    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

  20. Carotenoids as electron or excited-state energy donors in artificial photosynthesis: an ultrafast investigation of a carotenoporphyrin and a carotenofullerene dyad.

    Science.gov (United States)

    Pillai, Smitha; Ravensbergen, Janneke; Antoniuk-Pablant, Antaeres; Sherman, Benjamin D; van Grondelle, Rienk; Frese, Raoul N; Moore, Thomas A; Gust, Devens; Moore, Ana L; Kennis, John T M

    2013-04-07

    Photophysical investigations of molecular donor-acceptor systems have helped elucidate many details of natural photosynthesis and revealed design principles for artificial photosynthetic systems. To obtain insights into the factors that govern the partition between excited-state energy transfer (EET) and electron transfer (ET) processes among carotenoids and tetrapyrroles and fullerenes, we have designed artificial photosynthetic dyads that are thermodynamically poised to favor ET over EET processes. The dyads were studied using transient absorption spectroscopy with ∼100 femtosecond time resolution. For dyad , a carotenoporphyrin, excitation to the carotenoid S2 state induces ultrafast ET, competing with internal conversion (IC) to the carotenoid S1 state. In addition, the carotenoid S1 state gives rise to ET. In contrast with biological photosynthesis and many artificial photosynthetic systems, no EET at all was detected for this dyad upon carotenoid S2 excitation. Recombination of the charge separated state takes place in hundreds of picoseconds and yields a triplet state, which is interpreted as a triplet delocalized between the porphyrin and carotenoid moieties. In dyad , a carotenofullerene, excitation of the carotenoid in the S2 band results in internal conversion to the S1 state, ET and probably EET to fullerene on ultrafast timescales. From the carotenoid S1 state EET to fullerene occurs. Subsequently, the excited-state fullerene gives rise to ET from the carotenoid to the fullerene. Again, the charge separated state recombines in hundreds of picoseconds. The results illustrate that for a given rate of EET, the ratio of ET to EET can be controlled by adjusting the driving force for electron transfer.

  1. Ultrafast forward and backward electron transfer dynamics of coumarin 337 in hydrogen-bonded anilines as studied with femtosecond UV-pump/IR-probe spectroscopy.

    Science.gov (United States)

    Ghosh, Hirendra N; Verma, Sandeep; Nibbering, Erik T J

    2011-02-10

    Femtosecond infrared spectroscopy is used to study both forward and backward electron transfer (ET) dynamics between coumarin 337 (C337) and the aromatic amine solvents aniline (AN), N-methylaniline (MAN), and N,N-dimethylaniline (DMAN), where all the aniline solvents can donate an electron but only AN and MAN can form hydrogen bonds with C337. The formation of a hydrogen bond with AN and MAN is confirmed with steady state FT-IR spectroscopy, where the C═O stretching vibration is a direct marker mode for hydrogen bond formation. Transient IR absorption measurements in all solvents show an absorption band at 2166 cm(-1), which has been attributed to the C≡N stretching vibration of the C337 radical anion formed after ET. Forward electron transfer dynamics is found to be biexponential with time constants τ(ET)(1) = 500 fs, τ(ET)(2) = 7 ps in all solvents. Despite the presence of hydrogen bonds of C337 with the solvents AN and MAN, no effect has been found on the forward electron transfer step. Because of the absence of an H/D isotope effect on the forward electron transfer reaction of C337 in AN, hydrogen bonds are understood to play a minor role in mediating electron transfer. In contrast, direct π-orbital overlap between C337 and the aromatic amine solvents causes ultrafast forward electron transfer dynamics. Backward electron transfer dynamics, in contrast, is dependent on the solvent used. Standard Marcus theory explains the observed backward electron transfer rates.

  2. HII galaxies in 4D

    CERN Document Server

    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.

  3. Jet-cooled fluorescence excitation spectra and carbonyl wagging and ring-puckering potential energy functions of cyclobutanone and its 2,2,4,4-d4 isotopomer in the S1(n,π*) electronic excited state

    Science.gov (United States)

    Zhang, Jian; Chiang, Whe-Yi; Laane, Jaan

    1994-03-01

    The jet-cooled fluorescence excitation spectra of cyclobutanone and its 2,2,4,4-d4 isotopomer have been recorded in the 305-335 nm region. The electronic band origin of the d0 molecule for the S1(n,π*) state of A2 symmetry occurs at 30 292 cm-1 (30 265 cm-1 for the d4 molecule). The observed spectra consisting of more than 50 bands for each isotopomer involve ν7, ν8, and ν9 (the three A1 ring vibrations) as well as ν20(C=O in-plane wag), ν26 (C=O out-of-plane wag), and ν27 (ring puckering). Five bands associated with the excited vibrational states of ν26 in the S1(n,π*) electronic state were observed for each isotopic species, and these were used to determine the one-dimensional potential energy functions for the C=O out-of-plane wagging. The C=O wagging angle was determined to be 39° and the barrier to inversion is 2149 cm-1 (2188 cm-1 for the deuteride). For the ring-puckering in the S1 state the lowest three vibrational energy spacings were found to be 106, 166, and 185 cm-1 as compared to values of 35, 57, and 65 cm-1 in the S0 ground state. Several ring-puckering potential energy functions with varying degrees of asymmetry are capable of reproducing the observed results. In all cases, however, the v=0 puckering state lies above any barrier to planarity. A two-dimensional potential function which fits the observed data was also determined in terms of the wagging and puckering coordinates.

  4. Ultrafast electron dynamics in the topological insulator Bi{sub 2}Se{sub 3} studied by time-resolved photoemission spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Sobota, J.A.; Yang, S.-L. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Geballe Laboratory for Advanced Materials, Department ofApplied Physics, Stanford University, Stanford, CA 94305 (United States); Department of Physics, Stanford University, Stanford, CA 94305 (United States); Leuenberger, D. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Geballe Laboratory for Advanced Materials, Department ofApplied Physics, Stanford University, Stanford, CA 94305 (United States); Kemper, A.F. [Lawrence Berkeley National Lab, 1 Cyclotron Road, Berkeley, CA 94720 (United States); Analytis, J.G. [Department of Physics, University of California, Berkeley, CA 94720 (United States); Fisher, I.R. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Geballe Laboratory for Advanced Materials, Department ofApplied Physics, Stanford University, Stanford, CA 94305 (United States); Kirchmann, P.S., E-mail: kirchman@stanford.edu [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Devereaux, T.P. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025 (United States); Geballe Laboratory for Advanced Materials, Department ofApplied Physics, Stanford University, Stanford, CA 94305 (United States); and others

    2014-08-15

    We characterize the topological insulator Bi{sub 2}Se{sub 3} using time- and angle-resolved photoemission spectroscopy. By employing two-photon photoemission, a complete picture of the unoccupied electronic structure from the Fermi level up to the vacuum level is obtained. We demonstrate that the unoccupied states host a second Dirac surface state which can be resonantly excited by 1.5 eV photons. We then study the ultrafast relaxation processes following optical excitation. We find that they culminate in a persistent non-equilibrium population of the first Dirac surface state, which is maintained by a meta-stable population of the bulk conduction band. Finally, we perform a temperature-dependent study of the electron–phonon scattering processes in the conduction band, and find the unexpected result that their rates decrease with increasing sample temperature. We develop a model of phonon emission and absorption from a population of electrons, and show that this counter-intuitive trend is the natural consequence of fundamental electron–phonon scattering processes. This analysis serves as an important reminder that the decay rates extracted by time-resolved photoemission are not in general equal to single electron scattering rates, but include contributions from filling and emptying processes from a continuum of states.

  5. E4D_RT

    Energy Technology Data Exchange (ETDEWEB)

    2016-03-22

    Time-lapse ERT imaging for monitoring both natural and engineered subsurface processes has advanced rapidly over the past 15-20 years. However, imaging results generally required a significant amount of manual and computational effort, and therefore were not available while the process was occurring. Although the value of real-time imaging was recognized, several obstacles prevented it's implementation. E4D_RT addresses these obstacles by 1) providing specialized algorithms that negate the need for user intervention, thereby automating the time-lapse data processing steps, 2) linking field data collection systems with parallel supercomputing systems via wireless data transfer link, and 3) addressing the computational burdens by utilizing distributed memory supercomputing resources, thereby enabling rapid data processing and imaging results.

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

    KAUST Repository

    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.

  7. Imaging ultrafast excited state pathways in transition metal complexes by X-ray transient absorption and scattering using X-ray free electron laser source

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Lin X.; Shelby, Megan L.; Lestrange, Patrick J.; Jackson, Nicholas E.; Haldrup, Kristoffer; Mara, Michael W.; Stickrath, Andrew B.; Zhu, Diling; Lemke, Henrik; Chollet, Matthieu; Hoffman, Brian M.; Li, Xiaosong

    2016-01-01

    This report will describe our recent studies of transition metal complex structural dynamics on the fs and ps time scales using an X-ray free electron laser source, Linac Coherent Light Source (LCLS). Ultrafast XANES spectra at the Ni K-edge of nickel(II) tetramesitylporphyrin (NiTMP) were successfully measured for optically excited state at a timescale from 100 fs to 50 ps, providing insight into its sub-ps electronic and structural relaxation processes. Importantly, a transient reduced state Ni(I) (π, 3dx2-y2) electronic state is captured through the interpretation of a short-lived excited state absorption on the low-energy shoulder of the edge, which is aided by the computation of X-ray transitions for postulated excited electronic states. The observed and computed inner shell to valence orbital transition energies demonstrate and quantify the influence of electronic configuration on specific metal orbital energies. A strong influence of the valence orbital occupation on the inner shell orbital energies indicates that one should not use the transition energy from 1s to other orbitals to draw conclusions about the d-orbital energies. For photocatalysis, a transient electronic configuration could influence d-orbital energies up to a few eV and any attempt to steer the reaction pathway should account for this to ensure that external energies can be used optimally in driving desirable processes. NiTMP structural evolution and the influence of the porphyrin macrocycle conformation on relaxation kinetics can be likewise inferred from this study.

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

    Science.gov (United States)

    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

  9. Ultrafast technologies for photonic networks

    Science.gov (United States)

    Prucnal, Paul R.; Baby, Varghese; Xu, Lei; Glesk, Ivan

    2004-10-01

    Considerable progress has been in the last decade in the fields of photonic networks and ultra-fast optics. The past few years has seen the widespread use of wavelength division multiplexing (WDM) to provide enormous point-to-point capacity in the backbone and metro area networks. Remarkable progress in electronics, in terms of both costs and performance speeds, has to some extent alleviated the 'electronic bottleneck'. Developments in fiber-optics such as novel fiber types and Raman amplification have opened up additional wavelength regions of operation resulting in great expansion of usable fiber bandwidth. There exist unique opportunities for ultrafast technologies - a subject of much interest in the last decade and reaching a point of maturity - to complement these advances and spark the next generation networks. In our talk, we will mention two networking environments very different from WDM - (1) optical time division multiplexing (OTDM) and (2) optical code division multiple access (OCDMA). We will look at the potential of both these scenarios for different applications, focusing in particular on the latter as an approach that provides maximum flexibility to utilize the immense bandwidth of the optical fiber. We will also describe various ultra-fast technologies that have been developed e.g. .high repetition rate pulsed lasers, ultra-fast optical switches, time delay elements etc. which have a direct relevance to both these types of networks.

  10. 飞秒电子衍射系统的设计%Design of an Ultra-fast Electron Diffraction System

    Institute of Scientific and Technical Information of China (English)

    吴建军; 田进寿; 王俊锋; 邹玮; 赛小锋; 赵宝升; 刘运全; 梁文锡; 张杰

    2006-01-01

    研发的超快电子衍射系统由超快电子枪、样品室、超快读出系统、电源系统,以及真空系统等组成,该超快电子衍射系统具有较高的时间分辩能力和较强的探测能力.光电阴极是蒸镀于MgFB2窗上的35 nm的银膜,该阴极对266 nm的紫外光比较敏感,有较高的量子效率,又具有很好的化学稳定性.用短磁聚焦系统来实现对光电子的聚焦,有两对偏转板,其中的一对在测量时间脉宽时用作扫描板.用双MCP探测器来增强电子图像的强度,其增益在104以上,具有单电子探测能力.系统的总时间脉宽设计为358 fs.%The designed electron diffraction system consists of an ultra-fast electron gun,a sample chamber,a readout system,a power supply system,and a vacuum system,and it bears such unique characteristics as high energy,high temporal resolution,and high detection capacity.The photocathode is of a 35 nm Ag film deposited on an MgF2 glass disk,and it is sensitive to ultraviolet light with wavelength of 266 nm.A magnetic lens is used to focus the electrons.Two pairs of electric deflection plates are used in the X and Y directions respectively to control the movement of the electrons,and one pair of them will act as a scanning plate while measuring the pulse width of electrons.The sample chamber is made of stainless steel,and in the middle of the chamber there is a specimen holder,capable of shifting in three dimensions and turning around its axis.The diffraction pattern recording system has a very high detecting efficiency,and even a single electron could be detected.A cascade MCP detector is used to ensure an electron gain reached to 104.The electron gun is in a vacuum system of 10-4 Pa.The whole gun is shielded by a μ-metal sheath.The designed temporal resolution of the ultra-fast electron diffraction system (UED) is about 358 fs.

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

    KAUST Repository

    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.

  12. Ultrafast electron diffraction technique and its applications%超快电子衍射技术及其应用∗

    Institute of Scientific and Technical Information of China (English)

    裴敏洁; 齐大龙; 齐迎朋; 贾天卿; 张诗按; 孙真荣

    2015-01-01

    The real-time observation of atomic motion in space and time is of great importance for natural science research. Ultrafast electron diffraction (UED) technique, which is equipped with both the high temporal resolution of femtosecond laser pulses and the high spatial resolution of electron diffraction, can provide an effective approach to study the structural change of matter in atomic scale. In this review, we make an introduction of the development history, experimental methods, related applications and future prospects of UED technique.%时间和空间上实时观测原子运动对于自然科学研究有着非常重大的意义,而超快电子衍射(UED)技术同时具备飞秒激光脉冲的高时间分辨特性和电子衍射技术的高空间特性,可以为实时观测原子级分辨尺度物质的结构变化提供一种有效工具。本文综述了超快电子衍射技术的发展历史、实验方法以及相关应用,并且展望了超快电子衍射技术未来的发展。

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

    Science.gov (United States)

    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. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  14. Remarkably High Conversion Efficiency of Inverted Bulk Heterojunction Solar Cells: From Ultrafast Laser Spectroscopy and Electron Microscopy to Device Fabrication and Optimization

    KAUST Repository

    Alsulami, Qana

    2016-04-10

    In organic donor-acceptor systems, ultrafast interfacial charge transfer (CT), charge separation (CS), and charge recombination (CR) are key determinants of the overall performance of photovoltaic devices. However, a profound understanding of these photophysical processes at device interfaces remains superficial, creating a major bottleneck that circumvents advancements and the optimization of these solar cells. Here, results from time-resolved laser spectroscopy and high-resolution electron microscopy are examined to provide the fundamental information necessary to fabricate and optimize organic solar cell devices. In real time, CT and CS are monitored at the interface between three fullerene acceptors (FAs) (PC71BM, PC61BM, and IC60BA) and the PTB7-Th donor polymer. Femtosecond transient absorption (fs-TA) data demonstrates that photoinduced electron transfer from the PTB7-Th polymer to each FA occurs on the sub-picosecond time scale, leading to the formation of long-lived radical ions. It is also found that the power conversion efficiency improves from 2% in IC60BA-based solar cells to >9% in PC71BM-based devices, in support of our time-resolved results. The insights reported in this manuscript provide a clear understanding of the key variables involved at the device interface, paving the way for the exploitation of efficient CS and subsequently improving the photoconversion efficiency. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. Ultrafast pulse generation with black phosphorus

    CERN Document Server

    Li, Diao; Karvonen, Lasse; Ye, Guojun; Lipsanen, Harri; Chen, Xianhui; Sun, Zhipei

    2015-01-01

    Black phosphorus has been recently rediscovered as a new and interesting two-dimensional material due to its unique electronic and optical properties. Here, we study the linear and nonlinear optical properties of black phosphorus thin films, indicating that both linear and nonlinear optical properties are anisotropic and can be tuned by the film thickness. Then we employ the nonlinear optical property of black phosphorus for ultrafast (pulse duration down to ~786 fs in mode-locking) and large-energy (pulse energy up to >18 nJ in Q-switching) pulse generation in fiber lasers at the near-infrared telecommunication band ~1.5 {\\mu}m. Our results underscore relatively large optical nonlinearity in black phosphorus and its prospective for ultrafast pulse generation, paving the way to black phosphorus based nonlinear and ultrafast photonics applications (e.g., ultrafast all-optical switches/modulators, frequency converters etc.).

  16. 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.

    Science.gov (United States)

    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.

  17. 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

    Directory of Open Access Journals (Sweden)

    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.

  18. Reply to “Comment on ‘Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions’ ”

    Directory of Open Access Journals (Sweden)

    Emrah Turgut

    2013-09-01

    Full Text Available In the following, we show that the conclusions of our article titled “Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions” are correct. The Comment of Vodungbo et al. argues that a unique determination of the refractive index variation over time is not possible using the data set presented in our paper. Furthermore, it was suggested that the lack of uniqueness allows for the possibility of a very specific time-dependent trajectory of the refractive index in the complex plane that could give rise to a large nonmagnetic modulation of the measured asymmetry, in spite of a negligible change in the s-polarized reflectivity. In this Reply, we conclusively show that any nonmagnetic contribution to the measured asymmetry is indeed negligible (<2%, below the noise level of the magnetic-asymmetry measurements. First, we use a few additional measurements to unambiguously rule out the presence of any nonmagnetic contributions to the signal. Second, we show that the scenario proposed by Vodungbo et al. would require both exotic time and energy dependences of the refractive index near the M edge that are extremely unlikely (virtually impossible in real materials. Thus, the conclusions of our original article are preserved.

  19. EDITORIAL: Ultrafast magnetization processes

    Science.gov (United States)

    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

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

    Directory of Open Access Journals (Sweden)

    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.

  1. AIMS simulation study of ultrafast electronically nonadiabatic chemistry of methyl azide and UV-VIS spectroscopic study of azido-based energetic plasticizer bis(1,3-diazido prop-2-yl)malonate

    Science.gov (United States)

    Ghosh, Jayanta; Banerjee, Shaibal; Bhattacharya, Atanu

    2017-09-01

    To gain insight into the ultrafast electronically nonadiabatic chemistry of azido-based energetic plasticizer, we have explored the nonadiabatic chemical dynamics of an azido-based model analog molecule, methyl azide (MAz), using ab initio multiple spawning (AIMS) simulation and electronic structure theory calculations. Molecular nitrogen (N2) is predicted to be the initial product of MAz following its electronic excitation to the S1 electronically excited state. AIMS-based simulation reveals that electronically excited azido-based molecules undergo extremely fast (approximately in 40 femtoseconds) relaxation to the ground state via the (S1/S0)CI conical intersection. Furthermore, this relaxation process involves the Nsbnd N bond elongation along with the bending of N3 moiety. This is the first report on the electronically non-adiabatic chemical dynamics (in ultrafast time domain) of methyl azide. Finally, using ultraviolet-visible (UV-VIS) spectroscopy, we comment on the electronically nonadiabatic chemistry of azido-based energetic plasticizer, bis(1,3-diazido prop-2-yl)malonate.

  2. Partially coherent ultrafast spectrography.

    Science.gov (United States)

    Bourassin-Bouchet, C; Couprie, M-E

    2015-03-06

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Ishchenko, A. A., E-mail: aischenko@yasenevo.ru [Moscow State Technological University (Russian Federation); Bagratashvili, V. N. [Russian Academy of Sciences, Institute of Laser and Information Technologies (Russian Federation); Avilov, A. S. [Russian Academy of Sciences, Shubnikov Institute of Crystallography (Russian Federation)

    2011-09-15

    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.

  4. Semiconductors Under Ion Radiation: Ultrafast Electron-Ion Dynamics in Perfect Crystals and the Effect of Defects

    Science.gov (United States)

    Lee, Cheng-Wei; Schleife, André

    Stability and safety issues have been challenging difficulties for materials and devices under radiation such as solar panels in outer space. On the other hand, radiation can be utilized to modify materials and increase their performance via focused-ion beam patterning at nano-scale. In order to grasp the underlying processes, further understanding of the radiation-material and radiation-defect interactions is required and inevitably involves the electron-ion dynamics that was traditionally hard to capture. By applying Ehrenfest dynamics based on time-dependent density functional theory, we have been able to perform real-time simulation of electron-ion dynamics in MgO and InP/GaP. By simulating a high-energy proton penetrating the material, the energy gain of electronic system can be interpreted as electronic stopping power and the result is compared to existing data. We also study electronic stopping in the vicinity of defects: for both oxygen vacancy in MgO and interface of InP/GaP superlattice, electronic stopping shows strong dependence on the velocity of the proton. To study the energy transfer from electronic system to lattice, simulations of about 100 femto-seconds are performed and we analyze the difference between Ehrenfest and Born-Oppenheimer molecular dynamics.

  5. 4-D OCT in Developmental Cardiology

    Science.gov (United States)

    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.

  6. Natural dyes adsorbed on TiO2 nanowire for photovoltaic applications: enhanced light absorption and ultrafast electron injection.

    Science.gov (United States)

    Meng, Sheng; Ren, Jun; Kaxiras, Efthimios

    2008-10-01

    We investigate the electronic coupling between a TiO2 nanowire and a natural dye sensitizer, using state-of-the-art time-dependent first-principles calculations. The model dye molecule, cyanidin, is deprotonated into the quinonoidal form upon adsorption on the wire surface. This results in its highest occupied molecular orbital (HOMO) being located in the middle of the TiO2 bandgap and its lowest unoccupied molecular orbital (LUMO) being close to the TiO2 conduction band minimum (CBM), leading to greatly enhanced visible light absorption with two prominent peaks at 480 and 650 nm. We find that excited electrons are injected into the TiO2 conduction band within a time scale of 50 fs with negligible electron-hole recombination and energy dissipation, even though the dye LUMO is located 0.1-0.3 eV lower than the CBM of the TiO2 nanowire.

  7. Ultrafast fluorescence quenching dynamics of Atto655 in the presence of N-acetyltyrosine and N-acetyltryptophan in aqueous solution: proton-coupled electron transfer versus electron transfer.

    Science.gov (United States)

    Zhang, Ying; Yuan, Shuwei; Lu, Rong; Yu, Anchi

    2013-06-20

    We studied the ultrafast fluorescence quenching dynamics of Atto655 in the presence of N-acetyltyrosine (AcTyr) and N-acetyltryptophan (AcTrp) in aqueous solution with femtosecond transient absorption spectroscopy. We found that the charge-transfer rate between Atto655 and AcTyr is about 240 times smaller than that between Atto655 and AcTrp. The pH value and D2O dependences of the excited-state decay kinetics of Atto655 in the presence of AcTyr and AcTrp reveal that the quenching of Atto655 fluorescence by AcTyr in aqueous solution is via a proton-coupled electron-transfer (PCET) process and that the quenching of Atto655 fluorescence by AcTrp in aqueous solution is via an electron-transfer process. With the version of the semiclassical Marcus ET theory, we derived that the electronic coupling constant for the PCET reaction between Atto655 and AcTyr in aqueous solution is 8.3 cm(-1), indicating that the PCET reaction between Atto655 and AcTyr in aqueous solution is nonadiabatic.

  8. CINEMA 4D The Artist's Project Sourcebook

    CERN Document Server

    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

  9. Substitutional 4d and 5d impurities in graphene.

    Science.gov (United States)

    Alonso-Lanza, Tomás; Ayuela, Andrés; Aguilera-Granja, Faustino

    2016-08-21

    We describe the structural and electronic properties of graphene doped with substitutional impurities of 4d and 5d transition metals. The adsorption energies and distances for 4d and 5d metals in graphene show similar trends for the later groups in the periodic table, which are also well-known characteristics of 3d elements. However, along earlier groups the 4d impurities in graphene show very similar adsorption energies, distances and magnetic moments to the 5d ones, which can be related to the influence of the 4d and 5d lanthanide contraction. Surprisingly, within the manganese group, the total magnetic moment of 3 μB for manganese is reduced to 1 μB for technetium and rhenium. We find that compared with 3d elements, the larger size of the 4d and 5d elements causes a high degree of hybridization with the neighbouring carbon atoms, reducing spin splitting in the d levels. It seems that the magnetic adjustment of graphene could be significantly different if 4d or 5d impurities are used instead of 3d impurities.

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

    Science.gov (United States)

    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.

  11. Ultrafast Relaxation Dynamics of Photoexcited Heme Model Compounds: Observation of Multiple Electronic Spin States and Vibrational Cooling.

    Science.gov (United States)

    Govind, Chinju; Karunakaran, Venugopal

    2017-04-13

    Hemin is a unique model compound of heme proteins carrying out variable biological functions. Here, the excited state relaxation dynamics of heme model compounds in the ferric form are systematically investigated by changing the axial ligand (Cl/Br), the peripheral substituent (vinyl/ethyl-meso), and the solvent (methanol/DMSO) using femtosecond pump-probe spectroscopy upon excitation at 380 nm. The relaxation time constants of these model compounds are obtained by global analysis. Excited state deactivation pathway of the model compounds comprising the decay of the porphyrin excited state (S*) to ligand to metal charge transfer state (LMCT, τ1), back electron transfer from metal to ligand (MLCT, τ2), and relaxation to the ground state through different electronic spin states of iron (τ3 and τ4) are proposed along with the vibrational cooling processes. This is based on the excited state absorption spectral evolution, similarities between the transient absorption spectra of the ferric form and steady state absorption spectra of the low-spin ferrous form, and the data analysis. The observation of an increase of all the relaxation time constants in DMSO compared to the methanol reflects the stabilization of intermediate states involved in the electronic relaxation. The transient absorption spectra of met-myoglobin are also measured for comparison. Thus, the transient absorption spectra of these model compounds reveal the involvement of multiple iron spin states in the electronic relaxation dynamics, which could be an alternative pathway to the ground state beside the vibrational cooling processes and associated with the inherent features of the heme b type.

  12. Ultra-fast framing camera tube

    Science.gov (United States)

    Kalibjian, Ralph

    1981-01-01

    An electronic framing camera tube features focal plane image dissection and synchronized restoration of the dissected electron line images to form two-dimensional framed images. Ultra-fast framing is performed by first streaking a two-dimensional electron image across a narrow slit, thereby dissecting the two-dimensional electron image into sequential electron line images. The dissected electron line images are then restored into a framed image by a restorer deflector operated synchronously with the dissector deflector. The number of framed images on the tube's viewing screen is equal to the number of dissecting slits in the tube. The distinguishing features of this ultra-fast framing camera tube are the focal plane dissecting slits, and the synchronously-operated restorer deflector which restores the dissected electron line images into a two-dimensional framed image. The framing camera tube can produce image frames having high spatial resolution of optical events in the sub-100 picosecond range.

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

    Science.gov (United States)

    Hugo, Geoffrey D.; Rosu, Mihaela

    2014-01-01

    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 described, including necessity of breathing surrogates for 4D image reconstruction, assumptions made in acquisition and reconstruction about the breathing pattern, and commonly-observed artifacts. Both established and developmental methods to deal with these limitations are detailed. Finally, strategies to construct 4D targets and images and, alternatively, to compress 4D information into static targets and images for radiation therapy planning are described. PMID:22784929

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

    CERN Document Server

    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...

  15. Ultrafast cyclic voltammetry with asymmetrical potential scan

    Institute of Scientific and Technical Information of China (English)

    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.

  16. 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

    CERN Document Server

    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...

  17. Ultrafast science using Laser Wakefield Accelerators

    Science.gov (United States)

    Thomas, Alec G. R.

    2016-10-01

    Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have considerable benefits for ultrafast science. Laser wakefield acceleration provides radiation pulses that have femtosecond duration and intrinsic synchronisation with the laser source, allowing for pump-probe measurements with unprecedented temporal resolution. These pulses can be used to study ultrafast dynamical phenomena in plasma and dense material, such as transient magnetic fields, rapidly evolving plasma dynamics and crystal lattice oscillations. In this talk, I will review recent experiments in laser wakefield acceleration and energetic photon generation using the laser systems HERCULES and Lambda-Cubed at the University of Michigan and their use for capturing the dynamics of laser-pumped samples. Studies of the electron beam hosing instability and the generation of annular phase space distributions increase X-ray flux while maintaining its femtosecond duration. Single-shot, spectrally resolved absorption measurements in laser pumped foils can be made on ultrafast timescales using this broadband photon source. Ultrafast electron radiography is able to temporally resolve relativistically expanding magnetic fields in high-intensity laser-solid interactions and the evolution of electric fields in low density plasma. Time-resolved electron diffraction captures structural dynamics in crystalline silicon. I will also discuss the technological needs for and potential impact of such revolutionary compact radiation sources for ultrafast science in the future. US Air Force Office of Scientific Research under Award Number FA9550-12-1-0310, the US National Science Foundation Grants No. 1054164, 0935197, 1535628 and 0810979, US Department of Energy Grant No. DE-NA0002372 and Army Research Office Grant No. W911NF1.

  18. 4D Bioprinting for Biomedical Applications.

    Science.gov (United States)

    Gao, Bin; Yang, Qingzhen; Zhao, Xin; Jin, Guorui; Ma, Yufei; Xu, Feng

    2016-09-01

    3D bioprinting has been developed to effectively and rapidly pattern living cells and biomaterials, aiming to create complex bioconstructs. However, placing biocompatible materials or cells into direct contact via bioprinting is necessary but insufficient for creating these constructs. Therefore, '4D bioprinting' has emerged recently, where 'time' is integrated with 3D bioprinting as the fourth dimension, and the printed objects can change their shapes or functionalities when an external stimulus is imposed or when cell fusion or postprinting self-assembly occurs. In this review, we highlight recent developments in 4D bioprinting technology. Additionally, we review the uses of 4D bioprinting in tissue engineering and drug delivery. Finally, we discuss the major roadblocks to this approach, together with possible solutions, to provide future perspectives on this technology.

  19. Global 4-D trajectory optimization for spacecraft

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    Global 4-D trajectory(x,y,z,t)is optimized for a spacecraft,which is launched from the Earth to fly around the Sun,just as star-drift of 1437 asteroids in the solar system.The spacecraft trajectory is controlled by low thrust.The performance index of optimal trajectory is to maximize the rendezvous times with the intermediate asteroids,and also maximize the final mass.This paper provides a combined algorithm of global 4-D trajectory optimization.The algorithm is composed of dynamic programming and two-point-boundary algorithm based on optimal control theory.The best 4-D trajectory is obtained:the spacecraft flies passing 55 asteroids,and rendezvous with(following or passing again)asteroids for 454 days,and finally rendezvous with the asteroid 2005SN25 on the day 60521(MJD),the final mass of the spacecraft is 836.53 kg.

  20. Cinema 4D R13 Cookbook

    CERN Document Server

    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

  1. Representing Participation in ICT4D Projects

    DEFF Research Database (Denmark)

    Singh, J. P.; Flyverbom, Mikkel

    2016-01-01

    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......, depending on the context of their implementation, are permeated by multiple discourses about participation. Our four ideal types of participation discourses are, therefore, useful starting points to discuss the intricate dynamics of participation in ICT4D projects....

  2. Ultrafast dynamics of neutral superexcited Oxygen: A direct measurement of the competition between autoionization and predissociation

    CERN Document Server

    Timmers, Henry; Sandhu, Arvinder

    2012-01-01

    Using ultrafast extreme ultraviolet pulses, we performed a direct measurement of the relaxation dynamics of neutral superexcited states corresponding to the nl\\sigma_g(c^4\\Sigma_u^-) Rydberg series of O_2. An XUV attosecond pulse train was used to create a temporally localized Rydberg wavepacket and the ensuing electronic and nuclear dynamics were probed using a time-delayed femtosecond near-infrared pulse. We investigated the competing predissociation and autoionization mechanisms for superexcited molecules and found that autoionization is dominant for the low n Rydberg states. We measured an autoionization lifetime of 92+/-6 fs and 180+/-10 fs for (5s,4d)\\sigma_g and (6s,5d)\\sigma_g Rydberg state groups respectively. We determine that the disputed neutral dissociation lifetime for the \

  3. Deconvolution of ultrafast kinetic data with inverse filtering

    Energy Technology Data Exchange (ETDEWEB)

    Banyasz, Akos [Department of Physical Chemistry, Eoetvoes University, P.O. Box 32, H-1518 Budapest 112 (Hungary); Research Institute for Solid State Physics and Optics, Hungarian Academy of Sciences, P.O. Box 49, H-1525 Budapest (Hungary); Matyus, Edit [Department of Physical Chemistry, Eoetvoes University, P.O. Box 32, H-1518 Budapest 112 (Hungary); Keszei, Erno [Department of Physical Chemistry, Eoetvoes University, P.O. Box 32, H-1518 Budapest 112 (Hungary)]. E-mail: keszei@chem.elte.hu

    2005-02-01

    Due to limitations of pulse widths in ultrafast laser or electron pulse kinetic measurements, in the case of subpicosecond characteristic times of the studied reactions, deconvolution with the pulses always distorts the kinetic signal. Here, we describe inverse filtering based on Fourier transformations to deconvolve measured ultrafast kinetic data without evoking a particular kinetic mechanism. Deconvolution methods using additional Wiener filtering or two-parameter regularization are found to give reliable results for simulated as well as experimental data.

  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

    Energy Technology Data Exchange (ETDEWEB)

    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. Ultrafast infrared spectroscopy in photosynthesis.

    Science.gov (United States)

    Di Donato, Mariangela; Groot, Marie Louise

    2015-01-01

    In recent years visible pump/mid-infrared (IR) probe spectroscopy has established itself as a key technology to unravel structure-function relationships underlying the photo-dynamics of complex molecular systems. In this contribution we review the most important applications of mid-infrared absorption difference spectroscopy with sub-picosecond time-resolution to photosynthetic complexes. Considering several examples, such as energy transfer in photosynthetic antennas and electron transfer in reaction centers and even more intact structures, we show that the acquisition of ultrafast time resolved mid-IR spectra has led to new insights into the photo-dynamics of the considered systems and allows establishing a direct link between dynamics and structure, further strengthened by the possibility of investigating the protein response signal to the energy or electron transfer processes. This article is part of a Special Issue entitled: Vibrational spectroscopies and bioenergetic systems.

  6. Perspective: Ultrafast magnetism and THz spintronics

    Energy Technology Data Exchange (ETDEWEB)

    Walowski, Jakob; Münzenberg, Markus [Institut für Physik, Ernst-Moritz-Arndt-Universität Greifswald, 17489 Greifswald (Germany)

    2016-10-14

    This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

  7. Perspective: Ultrafast magnetism and THz spintronics

    Science.gov (United States)

    Walowski, Jakob; Münzenberg, Markus

    2016-10-01

    This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

  8. Interactive animation of 4D performance capture.

    Science.gov (United States)

    Casas, Dan; Tejera, Margara; Guillemaut, Jean-Yves; Hilton, Adrian

    2013-05-01

    A 4D parametric motion graph representation is presented for interactive animation from actor performance capture in a multiple camera studio. The representation is based on a 4D model database of temporally aligned mesh sequence reconstructions for multiple motions. High-level movement controls such as speed and direction are achieved by blending multiple mesh sequences of related motions. A real-time mesh sequence blending approach is introduced, which combines the realistic deformation of previous nonlinear solutions with efficient online computation. Transitions between different parametric motion spaces are evaluated in real time based on surface shape and motion similarity. Four-dimensional parametric motion graphs allow real-time interactive character animation while preserving the natural dynamics of the captured performance.

  9. 4D Lung Reconstruction with Phase Optimization

    DEFF Research Database (Denmark)

    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 vol...... 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.......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...

  10. Ultrafast nonlinear optics

    CERN Document Server

    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...

  11. 4D image reconstruction for emission tomography

    Science.gov (United States)

    Reader, Andrew J.; Verhaeghe, Jeroen

    2014-11-01

    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

  12. Cinema 4D R14 cookbook

    CERN Document Server

    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

  13. 4D geomorphological evolution of intertropical islands

    Science.gov (United States)

    Pastier, Anne-Morwenn; Bezos, Antoine; Husson, Laurent; Pedoja, Kevin; Arias, Camilo; Elliot, Mary; Lacroix, Pascal; Imran, Andi Muhammad

    2017-04-01

    Coral reef terraces record joint variations of sea level and surface elevation. U/Th ratings on corals along with topographic/bathymetric profiles and eustatic reconstitutions allow to locally determine the vertical rate of ground motion, while numerical modelling of reef sequences allows to unravel the processes controlling the architecture of sequences, and high-resolution DEMs facilitates the detailed mapping of the sequences of reef terraces. Alltogether, these methods allow to extrapolate the local vertical rates towards an unprecedented resolution for 4D kinematics. We applied our method to uplifting islands of the tectonically active Buton Archipelago, SE Sulawesi, Indonesia. The area undergoes a general uplift revealed by the ubiquitous occurrence of uplifted and folded reef sequences. We dated some 40 samples using U/Th, acquired sonar and dGPS profiles, and constructed high-res DEMs (Pleiades). Local vertical rates (from 0.2 to 0.28 mm/yr) were determined. Detailed geomorphological mapping of the lateral variations of the terraces are converted into time and space variations of uplift rates. Extrapolating the higher, undated terraces permits to reconstruct the overall 4D geomorphology history over the last Ma. In turns, these results give a unique view on the structural kinematics.

  14. Supercurrent anomalies in 4d SCFTs

    Science.gov (United States)

    Papadimitriou, Ioannis

    2017-07-01

    We use holographic renormalization of minimal N=2 gauged supergravity in order to derive the general form of the quantum Ward identities for 3d N=2 and 4d N=1 superconformal theories on general curved backgrounds, including an arbitrary fermionic source for the supercurrent. The Ward identities for 4d N=1 theories contain both bosonic and fermionic global anomalies, which we determine explicitly up to quadratic order in the supercurrent source. The Ward identities we derive apply to any superconformal theory, independently of whether it admits a holographic dual, except for the specific values of the a and c anomaly coefficients, which are equal due to our starting point of a two-derivative bulk supergravity theory. We show that the fermionic anomalies lead to an anomalous transformation of the supercurrent under rigid supersymmetry on backgrounds admitting Killing spinors, even if all superconformal anomalies are numerically zero on such backgrounds. The anomalous transformation of the supercurrent under rigid supersymmetry leads to an obstruction to the Q-exactness of the stress tensor in supersymmetric vacua, and may have implications for the applicability of localization techniques. We use this obstruction to the Q-exactness of the stress tensor, together with the Ward identities, in order to determine the general form of the stress tensor and R-current one-point functions in supersymmetric vacua, which allows us to obtain general expressions for the supersymmetric Casimir charges and partition function.

  15. Active origami by 4D printing

    Science.gov (United States)

    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.

  16. Qualitative characteristics and comparison of volatile fraction of vodkas made from different botanical materials by comprehensive two-dimensional gas chromatography and the electronic nose based on the technology of ultra-fast gas chromatography.

    Science.gov (United States)

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

    2017-03-01

    Vodka is a spirit-based beverage made from ethyl alcohol of agricultural origin. At present, increasingly more vodka brands have labels that specify the botanical origin of the product. Until now, the techniques for distinguishing between vodkas of different botanical origin have been costly, time-consuming and insufficient for making a distinction between vodka produced from similar raw materials. Therefore, it is of utmost importance to find a fast and relatively inexpensive technique for conducting such tests. In the present study, we employed comprehensive two-dimensional gas chromatography (GC×GC) and an electronic nose based on the technology of ultra-fast GC with chemometric methods such as partial least square discriminant analysis, discriminant function analysis and soft independent modeling of class analogy. Both techniques allow a distinction between the vodkas produced from different raw materials. In the case of GC×GC, the differences between vodkas were more noticeable than in the analysis by electronic nose; however, the electronic nose allowed the significantly faster analysis of vodkas. © 2016 Society of Chemical Industry. © 2016 Society of Chemical Industry.

  17. Four-dimensional electron microscopy.

    Science.gov (United States)

    Zewail, Ahmed H

    2010-04-09

    The discovery of the electron over a century ago and the realization of its dual character have given birth to one of the two most powerful imaging instruments: the electron microscope. The electron microscope's ability to resolve three-dimensional (3D) structures on the atomic scale is continuing to affect different fields, including materials science and biology. In this Review, we highlight recent developments and inventions made by introducing the fourth dimension of time in electron microscopy. Today, ultrafast electron microscopy (4D UEM) enables a resolution that is 10 orders of magnitude better than that of conventional microscopes, which are limited by the video-camera rate of recording. After presenting the central concept involved, that of single-electron stroboscopic imaging, we discuss prototypical applications, which include the visualization of complex structures when unfolding on different length and time scales. The developed UEM variant techniques are several, and here we illucidate convergent-beam and near-field imaging, as well as tomography and scanning-pulse microscopy. We conclude with current explorations in imaging of nanomaterials and biostructures and an outlook on possible future directions in space-time, 4D electron microscopy.

  18. Imaging the Temporal Evolution of Molecular Orbitals during Ultrafast Dissociation

    Science.gov (United States)

    Sann, H.; Havermeier, T.; Müller, C.; Kim, H.-K.; Trinter, F.; Waitz, M.; Voigtsberger, J.; Sturm, F.; Bauer, T.; Wallauer, R.; Schneider, D.; Weller, M.; Goihl, C.; Tross, J.; Cole, K.; Wu, J.; Schöffler, M. S.; Schmidt-Böcking, H.; Jahnke, T.; Simon, M.; Dörner, R.

    2016-12-01

    We investigate the temporal evolution of molecular frame angular distributions of Auger electrons emitted during ultrafast dissociation of HCl following a resonant single-photon excitation. The electron emission pattern changes its shape from that of a molecular σ orbital to that of an atomic p state as the system evolves from a molecule into two separated atoms.

  19. Advances in 4D radiation therapy for managing respiration: part II - 4D treatment planning.

    Science.gov (United States)

    Rosu, Mihaela; Hugo, Geoffrey D

    2012-12-01

    The development of 4D CT imaging technology made possible the creation of patient models that are reflective of respiration-induced anatomical changes by adding a temporal dimension to the conventional 3D, spatial-only, patient description. This had opened a new venue for treatment planning and radiation delivery, aimed at creating a comprehensive 4D radiation therapy process for moving targets. Unlike other breathing motion compensation strategies (e.g. breath-hold and gating techniques), 4D radiotherapy assumes treatment delivery over the entire respiratory cycle - an added bonus for both patient comfort and treatment time efficiency. The time-dependent positional and volumetric information holds the promise for optimal, highly conformal, radiotherapy for targets experiencing movements caused by respiration, with potentially elevated dose prescriptions and therefore higher cure rates, while avoiding the uninvolved nearby structures. In this paper, the current state of the 4D treatment planning is reviewed, from theory to the established practical routine. While the fundamental principles of 4D radiotherapy are well defined, the development of a complete, robust and clinically feasible process still remains a challenge, imposed by limitations in the available treatment planning and radiation delivery systems. Copyright © 2012. Published by Elsevier GmbH.

  20. Advances in 4D Radiation Therapy for Managing Respiration: Part II – 4D Treatment Planning

    Science.gov (United States)

    Rosu, Mihaela; Hugo, Geoffrey D.

    2014-01-01

    The development of 4D CT imaging technology made possible the creation of patient models that are reflective of respiration-induced anatomical changes by adding a temporal dimension to the conventional 3D, spatial-only, patient description. This had opened a new venue for treatment planning and radiation delivery, aimed at creating a comprehensive 4D radiation therapy process for moving targets. Unlike other breathing motion compensation strategies (e.g. breath-hold and gating techniques), 4D radiotherapy assumes treatment delivery over the entire respiratory cycle – an added bonus for both patient comfort and treatment time efficiency. The time-dependent positional and volumetric information holds the promise for optimal, highly conformal, radiotherapy for targets experiencing movements caused by respiration, with potentially elevated dose prescriptions and therefore higher cure rates, while avoiding the uninvolved nearby structures. In this paper, the current state of the 4D treatment planning is reviewed, from theory to the established practical routine. While the fundamental principles of 4D radiotherapy are well defined, the development of a complete, robust and clinically feasible process still remains a challenge, imposed by limitations in the available treatment planning and radiation delivery systems. PMID:22796324

  1. Ultrafast spectroscopic imaging of exfoliated graphene

    Energy Technology Data Exchange (ETDEWEB)

    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)

  2. Theoretical study on decay of the 4d core-excited states of Cs Ⅲ

    Institute of Scientific and Technical Information of China (English)

    Ding Xiao-Bin; Dong Chen-Zhong; Stephan Fritzsche

    2008-01-01

    In a recent XUV photoabsorption spectrum of Cs Ⅲ ions by Cummings and O'Sullivan [2001 J. Phys. B 34 199], rather large linewidths were found for the 4d 95s25p6 - 4d 105s25p5 transition which are quite in disagreement with corresponding quasi-relativistic multiconfiguration Hartree-Fock (MCHF) calculation. In the present work, a detailed multiconfiguration Dirac-Fock study has been carried out to explore this discrepancy. Owing to the detailed consid- eration of electron correlation effects, some 'forbidden' Auger decay channels, such as 4d 105s25p35d and 4d105s05p6, would become 'open'. As a result, remarkable improvement of the linewidths has been obtained in our calculation. Furthermore, the theoretical Auger spectrum of the 4d 95s25p6 core-excited states of Cs Ⅲ ions is given in the present work.

  3. Ultrafast exciton formation at the ZnO(1010) surface.

    Science.gov (United States)

    Deinert, J-C; Wegkamp, D; Meyer, M; Richter, C; Wolf, M; Stähler, J

    2014-08-01

    We study the ultrafast quasiparticle dynamics in and below the ZnO conduction band using femtosecond time-resolved two-photon photoelectron spectroscopy. Above band gap excitation causes hot electron relaxation by electron-phonon scattering down to the Fermi level E_{F} followed by ultrafast (200 fs) formation of a surface exciton (SX). Transient screening of the Coulomb interaction reduces the SX formation probability at high excitation densities near the Mott limit. Located just below the surface, the SX are stable with regard to hydrogen-induced work function modifications and thus the ideal prerequisite for resonant energy transfer applications.

  4. Ultrafast magnetization dynamics

    OpenAIRE

    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...

  5. Ptychographic ultrafast pulse reconstruction

    CERN Document Server

    Spangenberg, D; Brügmann, M H; Feurer, T

    2014-01-01

    We demonstrate a new ultrafast pulse reconstruction modality which is somewhat reminiscent of frequency resolved optical gating but uses a modified setup and a conceptually different reconstruction algorithm that is derived from ptychography. Even though it is a second order correlation scheme it shows no time ambiguity. Moreover, the number of spectra to record is considerably smaller than in most other related schemes which, together with a robust algorithm, leads to extremely fast convergence of the reconstruction.

  6. Ultrafast Magnetization Dynamics

    OpenAIRE

    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...

  7. Ultrafast photophysics of transition metal complexes.

    Science.gov (United States)

    Chergui, Majed

    2015-03-17

    The properties of transition metal complexes are interesting not only for their potential applications in solar energy conversion, OLEDs, molecular electronics, biology, photochemistry, etc. but also for their fascinating photophysical properties that call for a rethinking of fundamental concepts. With the advent of ultrafast spectroscopy over 25 years ago and, more particularly, with improvements in the past 10-15 years, a new area of study was opened that has led to insightful observations of the intramolecular relaxation processes such as internal conversion (IC), intersystem crossing (ISC), and intramolecular vibrational redistribution (IVR). Indeed, ultrafast optical spectroscopic tools, such as fluorescence up-conversion, show that in many cases, intramolecular relaxation processes can be extremely fast and even shorter than time scales of vibrations. In addition, more and more examples are appearing showing that ultrafast ISC rates do not scale with the magnitude of the metal spin-orbit coupling constant, that is, that there is no heavy-atom effect on ultrafast time scales. It appears that the structural dynamics of the system and the density of states play a crucial role therein. While optical spectroscopy delivers an insightful picture of electronic relaxation processes involving valence orbitals, the photophysics of metal complexes involves excitations that may be centered on the metal (called metal-centered or MC) or the ligand (called ligand-centered or LC) or involve a transition from one to the other or vice versa (called MLCT or LMCT). These excitations call for an element-specific probe of the photophysics, which is achieved by X-ray absorption spectroscopy. In this case, transitions from core orbitals to valence orbitals or higher allow probing the electronic structure changes induced by the optical excitation of the valence orbitals, while also delivering information about the geometrical rearrangement of the neighbor atoms around the atom of

  8. Resolving Ultrafast Heating of Dense Cryogenic Hydrogen

    Science.gov (United States)

    Zastrau, U.; Sperling, P.; Harmand, M.; Becker, A.; Bornath, T.; Bredow, R.; Dziarzhytski, S.; Fennel, T.; Fletcher, L. B.; Förster, E.; Göde, S.; Gregori, G.; Hilbert, V.; Hochhaus, D.; Holst, B.; Laarmann, T.; Lee, H. J.; Ma, T.; Mithen, J. P.; Mitzner, R.; Murphy, C. D.; Nakatsutsumi, M.; Neumayer, P.; Przystawik, A.; Roling, S.; Schulz, M.; Siemer, B.; Skruszewicz, S.; Tiggesbäumker, J.; Toleikis, S.; Tschentscher, T.; White, T.; Wöstmann, M.; Zacharias, H.; Döppner, T.; Glenzer, S. H.; Redmer, R.

    2014-03-01

    We report on the dynamics of ultrafast heating in cryogenic hydrogen initiated by a ≲300 fs, 92 eV free electron laser x-ray burst. The rise of the x-ray scattering amplitude from a second x-ray pulse probes the transition from dense cryogenic molecular hydrogen to a nearly uncorrelated plasmalike structure, indicating an electron-ion equilibration time of ˜0.9 ps. The rise time agrees with radiation hydrodynamics simulations based on a conductivity model for partially ionized plasma that is validated by two-temperature density-functional theory.

  9. Ultrafast probes of coherent oscillations in Fe-based superconductors

    Energy Technology Data Exchange (ETDEWEB)

    Kim, K. W. [Dept. of Physics, Chungbuk National University, Cheongju (Korea, Republic of)

    2017-03-15

    Forefront ultrafast experimental techniques have recently proven their potential as new approaches to understand materials based on non-equilibrium dynamics in the time domain. The time domain approach is useful especially in disentangling complicated coupling among charge, spin and lattice degrees of freedom. Various ultrafast experiments on Fe-based superconductors have observed strong coherent oscillations of an A1g phonon mode of arsenic ions, which shows strong coupling to the electronic and magnetic states. This paper reviews the recent reports of ultrafast studies on Fe-based superconductor with a focus on the coherent oscillations. Experimental results with ultrashort light sources from the terahertz-infrared pulses to the hard X-rays from a free electron laser will be presented.

  10. Role of Electron-Driven Proton-Transfer Processes in the Ultrafast Deactivation of Photoexcited Anionic 8-oxoGuanine-Adenine and 8-oxoGuanine-Cytosine Base Pairs.

    Science.gov (United States)

    Wu, Xiuxiu; Karsili, Tolga N V; Domcke, Wolfgang

    2017-01-14

    It has been reported that 8-oxo-7,8-dihydro-guanosine (8-oxo-G), which is the main product of oxidative damage of DNA, can repair cyclobutane pyrimidine dimer (CPD) lesions when incorporated into DNA or RNA strands in proximity to such lesions. It has therefore been suggested that the 8-oxo-G nucleoside may have been a primordial precursor of present-day flavins in DNA or RNA repair. Because the electron transfer leading to the splitting of a thymine-thymine pair in a CPD lesion occurs in the photoexcited state, a reasonably long excited-state lifetime of 8-oxo-G is required. The neutral (protonated) form of 8-oxo-G exhibits a very short (sub-picosecond) intrinsic excited-state lifetime which is unfavorable for repair. It has therefore been argued that the anionic (deprotonated) form of 8-oxo-G, which exhibits a much longer excited-state lifetime, is more likely to be a suitable cofactor for DNA repair. Herein, we have investigated the exited-state quenching mechanisms in the hydrogen-bonded complexes of deprotonated 8-oxo-G(-) with adenine (A) and cytosine (C) using ab initio wave-function-based electronic-structure calculations. The calculated reaction paths and potential-energy profiles reveal the existence of barrierless electron-driven inter-base proton-transfer reactions which lead to low-lying S₁/S₀ conical intersections. The latter can promote ultrafast excited-state deactivation of the anionic base pairs. While the isolated deprotonated 8-oxo-G(-) nucleoside may have been an efficient primordial repair cofactor, the excited states of the 8-oxo-G(-)-A and 8-oxo-G(-)-C base pairs are likely too short-lived to be efficient electron-transfer repair agents.

  11. A capacitive sensor for 2,4-D determination in water based on 2,4-D imprinted polypyrrole coated pencil electrode

    Science.gov (United States)

    Prusty, Arun Kumar; Bhand, Sunil

    2017-03-01

    A capacitive sensor for 2,4-dichloro phenoxy acetic acid(2,4-D) determination in drinking water has been developed using molecularly imprinted polypyrrole on pencil graphite electrode (PGE). Molecular imprinted polymer (MIP) coated PGE was prepared by electropolymerization of pyrrole via chronopotentiometry in the presence of 2,4-D as the template molecule. The prepared electrodes were characterized by field emission gun-scanning electron microscopy, cyclic voltammetry, and electrochemical impedance spectroscopy (EIS). The capacitance change of MIP electrode was measured in the presence of 2,4-D using EIS. The developed capacitive sensor exhibited a linear range 0.06-1.25 µg l-1 2,4-D with limit of detection of 0.02 µg l-1 and good selectivity towards 2,4-D in water with recovery from 92 to 110%. The results suggest the viable applicability of the MIP/PGE based sensor for the determination of the 2,4-D in water samples.

  12. An ultrafast look at Au nanoclusters.

    Science.gov (United States)

    Yau, Sung Hei; Varnavski, Oleg; Goodson, Theodore

    2013-07-16

    In the past 20 years, researchers studying nanomaterials have uncovered many new and interesting properties not found in bulk materials. Extensive research has focused on metal nanoparticles (>3 nm) because of their potential applications, such as in molecular electronics, image markers, and catalysts. In particular, the discovery of metal nanoclusters (properties for nanomaterials are intriguing, because for metal nanosystems in this size regime both size and shape determine electronic properties. Remarkably, changes in the optical properties of nanomaterials have provided tremendous insight into the electronic structure of nanoclusters. The success of synthesizing monolayer protected clusters (MPCs) in the condensed phase has allowed scientists to probe the metal core directly. Au MPCs have become the "gold" standard in nanocluster science, thanks to the rigorous structural characterization already accomplished. The use of ultrafast laser spectroscopy on MPCs in solution provides the benefit of directly studying the chemical dynamics of metal nanoclusters (core), and their nonlinear optical properties. In this Account, we investigate the optical properties of MPCs in the visible region using ultrafast spectroscopy. Based on fluorescence up-conversion spectroscopy, we propose an emission mechanism for these nanoclusters. These clusters behave differently from nanoparticles in terms of emission lifetimes as well as two-photon cross sections. Through further investigation of the transient (excited state) absorption, we have found many unique phenomena of nanoclusters, such as quantum confinement effects and vibrational breathing modes. In summary, based on the differences in the optical properties, the distinction between nanoclusters and nanoparticles appears at a size near 2.2 nm. This is consistent with simulations from a free-electron model proposed for MPCs. The use of ultrafast techniques on these nanoclusters can answer many of the fundamental questions about

  13. Mixed Potential Energy Surfaces of the Ultrafast Isomerization of Retinal in Bacteriorhodopsin

    Directory of Open Access Journals (Sweden)

    Prokhorenko Valentyn I.

    2013-03-01

    Full Text Available We observe, using electronic two-dimensional photon echo spectroscopy, that the cis and trans potential energy surfaces of the ultrafast isomerization of retinal in bacteriorhodopsin are mixed via the hydrogen out of plane (HOOP mode.

  14. LUX - A recirculating linac-based ultrafast X-ray source

    Energy Technology Data Exchange (ETDEWEB)

    Corlett, J.N.; Barletta, W.A.; DeSantis, S.; Doolittle, L.; Fawley, W.M.; Green, M.A.; Heimann, P.; Leone, S.R.; Lidia, S.; Li, D.; Parmigiani, F.; Ratti, A.; Robinson, K.; Schoenlein, R.; Staples, J.; Wan, W.; Wells, R.; Wilcox, R.; Wolski, A.; Zholents, A.

    2003-08-01

    We describe the design of a proposed source of ultra-fast synchrotron radiation x-ray pulses based on a recirculating superconducting linac, with an integrated array of ultrafast laser systems. The source produces x-ray pulses with duration of 10-50 fs at a 10 kHz repetition rate, with tunability from EUV to hard x-ray regimes, and optimized for the study of ultra-fast dynamics. A high-brightness rf photocathode provides electron bunches. An injector linac accelerates the beam to the 100 MeV range, and is followed by four passes through a 700 MeV recirculating linac. Ultrafast hard x-ray pulses are obtained by a combination of electron bunch manipulation, transverse temporal correlation of the electrons, and x-ray pulse compression. EUV and soft x-ray pulses as short as 10 fs are generated in a harmonic-cascade free electron laser scheme.

  15. 17 CFR 260.4d-8 - Content.

    Science.gov (United States)

    2010-04-01

    ... 17 Commodity and Securities Exchanges 3 2010-04-01 2010-04-01 false Content. 260.4d-8 Section 260.4d-8 Commodity and Securities Exchanges SECURITIES AND EXCHANGE COMMISSION (CONTINUED) GENERAL RULES AND REGULATIONS, TRUST INDENTURE ACT OF 1939 Rules Under Section 304 § 260.4d-8 Content. (a)...

  16. 17 CFR 260.4d-8 - Content.

    Science.gov (United States)

    2012-04-01

    ... 17 Commodity and Securities Exchanges 3 2012-04-01 2012-04-01 false Content. 260.4d-8 Section 260.4d-8 Commodity and Securities Exchanges SECURITIES AND EXCHANGE COMMISSION (CONTINUED) GENERAL RULES AND REGULATIONS, TRUST INDENTURE ACT OF 1939 Rules Under Section 304 § 260.4d-8 Content. (a) Each...

  17. Stoner versus Heisenberg: Ultrafast exchange reduction and magnon generation during laser-induced demagnetization

    Science.gov (United States)

    Turgut, Emrah; Zusin, Dmitriy; Legut, Dominik; Carva, Karel; Knut, Ronny; Shaw, Justin M.; Chen, Cong; Tao, Zhensheng; Nembach, Hans T.; Silva, Thomas J.; Mathias, Stefan; Aeschlimann, Martin; Oppeneer, Peter M.; Kapteyn, Henry C.; Murnane, Margaret M.; Grychtol, Patrik

    2016-12-01

    Understanding how the electronic band structure of a ferromagnetic material is modified during laser-induced demagnetization on femtosecond time scales has been a long-standing question in condensed matter physics. Here, we use ultrafast high harmonics to measure time-, energy-, and angle-resolved M -edge magnetic asymmetry spectra for Co films after optical pumping to induce ultrafast demagnetization. This provides a complete data set that we can compare with advanced ab initio magneto-optical calculations. Our analysis identifies that the dominant mechanisms contributing to ultrafast demagnetization on time scales up to several picoseconds are a transient reduction in the exchange splitting and the excitation of ultrafast magnons. Surprisingly, we find that the magnon contribution to ultrafast demagnetization is already strong on subpicosecond time scales, while the reduction in exchange splitting persists to several picoseconds.

  18. Integrated Graphene-Based Optoelectronic Devices Used for Ultrafast Optical-THz Photodetectors, Modulators and Emitters

    Science.gov (United States)

    2015-04-03

    AFRL-RV-PS- AFRL-RV-PS- TR-2015-0083 TR-2015-0083 INTEGRATED GRAPHENE -BASED OPTOELECTRONIC DEVICES USED FOR ULTRAFAST OPTICAL-THZ PHOTODETECTORS...From - To) 7 Nov 2011 – 12 Feb 2012 4. TITLE AND SUBTITLE Integrated Graphene -Based Optoelectronic Devices Used for Ultrafast Optical-THz...quasiparticles in graphene electrons, phlasmons and electron-hole pairs with the ultimate goal to convert them into or be extracted from terahertz

  19. Ultrafast AMO physics at the LCLS x-ray FEL

    Directory of Open Access Journals (Sweden)

    Bucksbaum P.H.

    2013-08-01

    Full Text Available The Linac Coherent Light Source at the SLAC National Accelerator Laboratory, Stanford University, began operation in 2009 as the world's first hard x-ray free electron laser. Early experiments have concentrated on atomic physics, and have demonstrated several key features of the ultrafast high field x-ray-atom interaction. This paper reviews some of these early results.

  20. Photodegradation of 2,4-D induced by NO₂(-) in aqueous solutions: the role of NO₂.

    Science.gov (United States)

    Yu, Chunyan; Wang, Hua; Liu, Xuan; Quan, Xie; Chen, Shuo; Zhang, Jianlin; Zhang, Peng

    2014-07-01

    To elucidate the effect of nitrite ion (NO₂(-)) on the photodegradation of organic pollutants, a 300 W mercury lamp and Pyrex tubes restricting the transmission of wavelengths below 290 nm were used to simulate sunlight, and the photodegradation processes of 2,4-dichlorophenoxyacetic acid (2,4-D) with different concentrations of NO₂(-) in freshwater and seawater were studied. The effect of reactive oxygen species (ROS) on the photolysis of 2,4-D was also demonstrated using electron paramagnetic resonance (EPR). The results indicated that the 2,4-D photolysis reaction followed the first-order kinetics in freshwater and seawater under different concentrations of NO₂(-). Meanwhile, the photochemical reaction rate of 2,4-D increased with increasing concentration of NO₂(-). When the concentration of NO₂(-) was lower than 23 mg/L, the photodegradation rate of 2,4-D in seawater was higher than that in freshwater. However, when the concentration of NO₂(-) was reached 230 mg/L, 2,4-D degradation slowed down in seawater. It was important to note that EPR spectra showed NO₂ radical was generated in the NO₂(-) solution under simulated sunlight irradiation, indicating that 2,4-D photodegradation could be induced by NO₂. These results show the key role of NO₂(-) in photochemistry and are helpful for better understanding of the phototransformation of environmental contaminants in natural aquatic systems. Copyright © 2014. Published by Elsevier B.V.

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

    NARCIS (Netherlands)

    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)

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

    NARCIS (Netherlands)

    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)

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

    Science.gov (United States)

    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.

  4. Development operators on 4D moving object databases

    Institute of Scientific and Technical Information of China (English)

    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.

  5. Comprehensive Studies of Ultrafast Laser Excited Warm Dense Gold

    Science.gov (United States)

    Chen, Zhijiang; Mo, Mianzhen; Russell, Brandon; Tsui, Ying; Wang, Xijie; Ng, Andrew; Glenzer, Siegfried

    2016-10-01

    Isochoric excitation of solids by ultrafast laser pulses is an important approach to generate warm dense matter in laboratory. Electrical conductivity, structural dynamics and lattice stabilities are the most important properties in ultrafast laser excited warm dense matter. To investigate these properties, we have developed multiple advanced capabilities at SLAC recently, including the measurement of semi-DC electrical conductivity with ultrafast THz radiation, the study of solid and liquid structural dynamics by ultrafast electron diffraction (UED), and the investigation of lattice stability using frequency domain interferometry (FDI) on both front and rear surfaces. Due to the non-reversible nature in exciting solid to warm dense matter, all these diagnostics are implemented with single-shot approaches, reducing the uncertainties due to shot-to-shot fluctuations. In this talk, we will introduce these novel capabilities and present some highlighted studies in warm dense gold, which was uniformly excited by ultrafast laser pulses at 400nm. We appreciate the supports from DOE FES under FWP #100182.

  6. Ultrafast scanning tunneling microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Botkin, D.A. [California Univ., Berkeley, CA (United States). Dept. of Physics]|[Lawrence Berkeley Lab., CA (United States)

    1995-09-01

    I have developed an ultrafast scanning tunneling microscope (USTM) based on uniting stroboscopic methods of ultrafast optics and scanned probe microscopy to obtain nanometer spatial resolution and sub-picosecond temporal resolution. USTM increases the achievable time resolution of a STM by more than 6 orders of magnitude; this should enable exploration of mesoscopic and nanometer size systems on time scales corresponding to the period or decay of fundamental excitations. USTM consists of a photoconductive switch with subpicosecond response time in series with the tip of a STM. An optical pulse from a modelocked laser activates the switch to create a gate for the tunneling current, while a second laser pulse on the sample initiates a dynamic process which affects the tunneling current. By sending a large sequence of identical pulse pairs and measuring the average tunnel current as a function of the relative time delay between the pulses in each pair, one can map the time evolution of the surface process. USTM was used to measure the broadband response of the STM`s atomic size tunnel barrier in frequencies from tens to hundreds of GHz. The USTM signal amplitude decays linearly with the tunnel junction conductance, so the spatial resolution of the time-resolved signal is comparable to that of a conventional STM. Geometrical capacitance of the junction does not appear to play an important role in the measurement, but a capacitive effect intimately related to tunneling contributes to the measured signals and may limit the ultimate resolution of the USTM.

  7. 9th International Symposium on Ultrafast Processes in Spectroscopy

    CERN Document Server

    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...

  8. Ultrafast Multiphoton Thermionic Photoemission from Graphite

    Science.gov (United States)

    Tan, Shijing; Argondizzo, Adam; Wang, Cong; Cui, Xuefeng; Petek, Hrvoje

    2017-01-01

    Electronic heating of cold crystal lattices in nonlinear multiphoton excitation can transiently alter their physical and chemical properties. In metals where free electron densities are high and the relative fraction of photoexcited hot electrons is low, the effects are small, but in semimetals, where the free electron densities are low and the photoexcited densities can overwhelm them, the intense femtosecond laser excitation can induce profound changes. In semimetal graphite and its derivatives, strong optical absorption, weak screening of the Coulomb potential, and high cohesive energy enable extreme hot electron generation and thermalization to be realized under femtosecond laser excitation. We investigate the nonlinear interactions within a hot electron gas in graphite through multiphoton-induced thermionic emission. Unlike the conventional photoelectric effect, within about 25 fs, the memory of the excitation process, where resonant dipole transitions absorb up to eight quanta of light, is erased to produce statistical Boltzmann electron distributions with temperatures exceeding 5000 K; this ultrafast electronic heating causes thermionic emission to occur from the interlayer band of graphite. The nearly instantaneous thermalization of the photoexcited carriers through Coulomb scattering to extreme electronic temperatures characterized by separate electron and hole chemical potentials can enhance hot electron surface femtochemistry, photovoltaic energy conversion, and incandescence, and drive graphite-to-diamond electronic phase transition.

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

    Directory of Open Access Journals (Sweden)

    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

  10. Femtosecond laser studies of ultrafast intramolecular processes

    Energy Technology Data Exchange (ETDEWEB)

    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.

  11. Ultrafast graphene-based broadband THz detector

    CERN Document Server

    Mittendorff, Martin; Kamann, Josef; Eroms, Jonathan; Weiss, Dieter; Schneider, Harald; Helm, Manfred

    2013-01-01

    We present an ultrafast graphene-based detector, working in the THz range at room temperature. A logarithmic-periodic antenna is coupled to a graphene flake that is produced by exfoliation on SiO2. The detector was characterized with the free-electron laser FELBE for wavelengths from 8 um to 220 um. The detector rise time is 50 ps in the wavelength range from 30 um to 220 um. Autocorrelation measurements exploiting the nonlinear photocurrent response at high intensities reveal an intrinsic response time below 10 ps. This detector has a high potential for characterizing temporal overlaps, e. g. in two-color pump-probe experiments.

  12. Motion4D-library extended

    Science.gov (United States)

    Müller, Thomas

    2011-06-01

    The new version of the Motion4D-library now also includes the integration of a Sachs basis and the Jacobi equation to determine gravitational lensing of pointlike sources for arbitrary spacetimes.New version program summaryProgram title: Motion4D-libraryCatalogue identifier: AEEX_v3_0Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEEX_v3_0.htmlProgram obtainable from: CPC Program Library, Queen's University, Belfast, N. IrelandLicensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.htmlNo. of lines in distributed program, including test data, etc.: 219 441No. of bytes in distributed program, including test data, etc.: 6 968 223Distribution format: tar.gzProgramming language: C++Computer: All platforms with a C++ compilerOperating system: Linux, WindowsRAM: 61 MbytesClassification: 1.5External routines: Gnu Scientic Library (GSL) (http://www.gnu.org/software/gsl/)Catalogue identifier of previous version: AEEX_v2_0Journal reference of previous version: Comput. Phys. Comm. 181 (2010) 703Does the new version supersede the previous version?: YesNature of problem: Solve geodesic equation, parallel and Fermi-Walker transport in four-dimensional Lorentzian spacetimes. Determine gravitational lensing by integration of Jacobi equation and parallel transport of Sachs basis.Solution method: Integration of ordinary differential equations.Reasons for new version: The main novelty of the current version is the extension to integrate the Jacobi equation and the parallel transport of the Sachs basis along null geodesics. In combination, the change of the cross section of a light bundle and thus the gravitational lensing effect of a spacetime can be determined. Furthermore, we have implemented several new metrics.Summary of revisions: The main novelty of the current version is the integration of the Jacobi equation and the parallel transport of the Sachs basis along null geodesics. The corresponding set of equations readd2xμdλ2=-Γρ

  13. Magnetic Dichroism in the 4d-Core Photoabsorption for the Mixed Valent Ferromagnet CeRh3B2

    Science.gov (United States)

    Jo, Takeo; Imada, Shin

    1989-06-01

    The Ce 4d-core X-ray absorption spectrum (4d XAS) of the mixed valent ferromagnet CeRh3B2 is calculated based on the impurity Anderson model incorporated with electron-electron (or core hole) interactions described by the Slater integrals. The ferromagnetic ordering is taken into account by the molecular field acting on the 4f electron of the impurity atom. The difference in the 4d XAS between the right-hand and left-hand circularly polarized incident photons is predicted to be very remarkable, even for the magnetization of ˜ 1 μB per Ce atom.

  14. Role of the middle residue in the triple tryptophan electron transfer chain of DNA photolyase: ultrafast spectroscopy of a Trp-->Phe mutant.

    Science.gov (United States)

    Lukacs, Andras; Eker, André P M; Byrdin, Martin; Villette, Sandrine; Pan, Jie; Brettel, Klaus; Vos, Marten H

    2006-08-17

    Photoreduction of the semi-reduced flavin adenine dinucleotide cofactor FADH* in DNA photolyase from Escherichia coli into FADH- involves three tryptophan (W) residues that form a closely spaced electron-transfer chain FADH*-W382-W359-W306. To investigate this process, we have constructed a mutant photolyase in which W359 is replaced by phenylalanine (F). Monitoring its photoproducts by femtosecond spectroscopy, the excited-state FADH* was found to decay in approximately 30 ps, similar as in wild type (WT) photolyase. In contrast to WT, however, in W359F mutant photolyase the ground-state FADH* fully recovered virtually concomitantly with the decay of its excited state and, despite the presence of the primary electron donor W382, no measurable flavin reduction was observed at any time. Thus, W359F photolyase appears to behave like many other flavoproteins, where flavin excited states are quenched by very short-lived oxidation of aromatic residues. Our analysis indicates that both charge recombination of the primary charge separation state FADH-W382*+ and (in WT) electron transfer from W359 to W382*+ occur with time constants FADH* electron-transfer step. Our results provide a first experimental indication that electron transfer between aromatic residues can take place on the time scale of approximately 10(-12) s.

  15. Ultrafast Graphene Photonics and Optoelectronics

    Science.gov (United States)

    2017-04-14

    structures that consist of a sheet of graphene and a plasma substrate such as a metal, a doped semiconductor, or another graphene layer. Using these...AFRL-AFOSR-JP-TR-2017-0032 Ultrafast Graphene Photonics and Optoelectronics Kuang-Hsiung Wu National Chiao Tung University Final Report 04/14/2017...DATES COVERED (From - To) 18 Apr 2013 to 17 Apr 2016 4. TITLE AND SUBTITLE Ultrafast Graphene Photonics and Optoelectronics 5a.  CONTRACT NUMBER 5b

  16. Ultrafast electron relaxation in superconducting Bi(2)Sr(2)CaCu(2)O(8+delta) by time-resolved photoelectron spectroscopy.

    Science.gov (United States)

    Perfetti, L; Loukakos, P A; Lisowski, M; Bovensiepen, U; Eisaki, H; Wolf, M

    2007-11-09

    Time-resolved photoelectron spectroscopy is employed to study the dynamics of photoexcited electrons in optimally doped Bi{2}Sr{2}CaCu{2}O{8+delta} (Bi-2212). Hot electrons thermalize in less than 50 fs and dissipate their energy on two distinct time scales (110 fs and 2 ps). These are attributed to the generation and subsequent decay of nonequilibrium phonons, respectively. We conclude that 20% of the total lattice modes dominate the coupling strength and estimate the second momentum of the Eliashberg coupling function lambdaOmega{0}{2}=360+/-30 meV{2}. For the typical phonon energy of copper-oxygen bonds (Omega{0} approximately 40-70 meV), this results in an average electron-phonon coupling lambda<0.25.

  17. Imaging ultrafast excited state pathways in transition metal complexes by X-ray transient absorption and scattering using X-ray free electron laser source

    DEFF Research Database (Denmark)

    Chen, Lin X; Shelby, Megan L; Lestrange, Patrick J

    2016-01-01

    orbital energies. A strong influence of the valence orbital occupation on the inner shell orbital energies indicates that one should not use the transition energy from 1s to other orbitals to draw conclusions about the d-orbital energies. For photocatalysis, a transient electronic configuration could...

  18. Structures and ultrafast dynamics of interfacial water assemblies on smooth hydrophobic surfaces

    Science.gov (United States)

    Yang, Ding-Shyue; He, Xing

    2017-09-01

    Using time-averaged and ultrafast electron diffraction, structures and ultrafast dynamics of interfacial water assemblies on smooth hydrophobic surfaces are reported. The lack of hydrophilic interaction and topographical template effect from the support surface leads to the formation of small, mostly randomly-oriented, ice crystallites with the cubic structure. Dynamically, following the substrate photoexcitation, interfacial water assemblies undergo four stages of changes-ultrafast melting, nonequilibrium isotropic phase transformation, annealing, and restructuring-which are closely correlated with the substrate dynamics. The connectivity and cooperative nature of the hydrogen-bonded network is considered crucial for water assemblies to withstand large structural motions without sublimation on ultrashort times.

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

    Science.gov (United States)

    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

  20. Ultrafast X-Ray Coherent Control

    Energy Technology Data Exchange (ETDEWEB)

    Reis, David

    2009-05-01

    This main purpose of this grant was to develop the nascent eld of ultrafast x-ray science using accelerator-based sources, and originally developed from an idea that a laser could modulate the di racting properties of a x-ray di racting crystal on a fast enough time scale to switch out in time a shorter slice from the already short x-ray pulses from a synchrotron. The research was carried out primarily at the Advanced Photon Source (APS) sector 7 at Argonne National Laboratory and the Sub-Picosecond Pulse Source (SPPS) at SLAC; in anticipation of the Linac Coherent Light Source (LCLS) x-ray free electron laser that became operational in 2009 at SLAC (all National User Facilities operated by BES). The research centered on the generation, control and measurement of atomic-scale dynamics in atomic, molecular optical and condensed matter systems with temporal and spatial resolution . It helped develop the ultrafast physics, techniques and scienti c case for using the unprecedented characteristics of the LCLS. The project has been very successful with results have been disseminated widely and in top journals, have been well cited in the eld, and have laid the foundation for many experiments being performed on the LCLS, the world's rst hard x-ray free electron laser.

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

    CERN Document Server

    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.

  2. Experimental Characterizations of 4-D Transverse Phase-Space of a Compressed Beam

    CERN Document Server

    Zhou, Feng; Andonian, Gerard; Ben-Zvi, Ilan; Cline, David B; Murokh, Alex; Rosenzweig, James E; Yakimenko, Vitaly

    2005-01-01

    Coherent synchrotron radiation can significantly distort beam phase spaces in longitudinal direction and bending plane through a bunch compressor. A tomography technique is used to reconstruct transverse phase space of electron beam. Transverse 4-D phase spaces are systematically measured at UCLA/ATF compressor and their characteristics with different bunch compression conditions are analyzed.

  3. Biokinetic Analysis and Metabolic Fate of 2,4-D in 2,4-D-Resistant Soybean (Glycine max).

    Science.gov (United States)

    Skelton, Joshua J; Simpson, David M; Peterson, Mark A; Riechers, Dean E

    2017-07-26

    The Enlist weed control system allows the use of 2,4-D in soybean but slight necrosis in treated leaves may be observed in the field. The objectives of this research were to measure and compare uptake, translocation, and metabolism of 2,4-D in Enlist (E, resistant) and non-AAD-12 transformed (NT, sensitive) soybeans. The adjuvant from the Enlist Duo herbicide formulation (ADJ) increased 2,4-D uptake (36%) and displayed the fastest rate of uptake (U50= 0.2 h) among treatments. E soybean demonstrated a faster rate of 2,4-D metabolism (M50= 0.2 h) compared to NT soybean, but glyphosate did not affect 2,4-D metabolism. Metabolites of 2,4-D in E soybean were qualitatively different than NT. Applying 2,4-D-ethylhexyl ester instead of 2,4-D choline (a quaternary ammonium salt) eliminated visual injury to E soybean, likely due to the time required for initial de-esterification and bioactivation. Excessive 2,4-D acid concentrations in E soybean resulting from ADJ-increased uptake may significantly contribute to foliar injury.

  4. A Time Domain Impedance Probe For Ultra-Fast Measurements of Electron Parameters in the Ionosphere: Results From A NASA USIP Experiment

    Science.gov (United States)

    Clark, D. C.; Spencer, E. A.; Gollapalli, R.; Kerrigan, B.

    2016-12-01

    A plasma impedance probe is used to obtain plasma parameters in the ionosphere by measuring the magnitude, shape and location of resonances in the frequency spectrum when a probe structure is driven with RF excitation. We have designed and developed a new Time Domain Impedance Probe (TDIP) capable of making measurements of absolute electron density and electron neutral collision frequency at temporal and spatial resolutions not previously attained. A single measurement can be made in a time as short as 100 microseconds, which yields much higher spatial resolution than a frequency sweep method. This method essentially consists of applying a small amplitude time limited voltage signal into a probe and measuring the resulting current response. The frequency bandwidth of the voltage signal is selected in order that the electron plasma resonances are observable. A prototype of the new instrument was flown at 08:45 EST on March 1 2016 on a NASA Undergraduate Student Instrument Progam (USIP) sounding rocket launched out of Wallops Flight Facility (Flight time was around 20 minutes). Here we analyze the data from the sounding rocket experiment, using an adaptive system identification technique to compare the measured data with analytical formulas obtained from a theoretical consideration of the time domain response. The analytical formula is calibrated to a plasma fluid finite difference time domain (PFFDTD) numerical computation before using it to analyze the rocket data from 85 km to 170 km on both upleg and downleg. Our results show that the technique works as advertised, but several issues including payload charging and signal rectification remains to be resolved. A plasma impedance probe is used to obtain plasma parameters in the ionosphere by measuring the magnitude, shape and location of resonances in the frequency spectrum when a probe structure is driven with RF excitation. We have designed and developed a new Time Domain Impedance Probe (TDIP) capable of making

  5. 3D/4D ultrasound registration of bone

    CERN Document Server

    Schers, Jonathan; Daanen, Vincent; Fouard, Céline; Plaskos, Christopher; Kilian, Pascal

    2008-01-01

    This paper presents a method to reduce the invasiveness of Computer Assisted Orthopaedic Surgery (CAOS) using ultrasound. In this goal, we need to develop a method for 3D/4D ultrasound registration. The premilinary results of this study suggest that the development of a robust and ``realtime'' 3D/4D ultrasound registration is feasible.

  6. Beyond ICT4D: new media research in Uganda

    NARCIS (Netherlands)

    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

  7. 32 CFR 1645.4 - Exclusion from Class 4-D.

    Science.gov (United States)

    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...

  8. Beyond ICT4D: new media research in Uganda

    NARCIS (Netherlands)

    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 dev

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

    Institute of Scientific and Technical Information of China (English)

    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.

  10. Enhanced rate performance of flexible and stretchable linear supercapacitors based on polyaniline@Au@carbon nanotube with ultrafast axial electron transport

    Science.gov (United States)

    Xu, Jiang; Ding, Jianning; Zhou, Xiaoshuang; Zhang, Yang; Zhu, Wenjun; Liu, Zunfen; Ge, Shanhai; Yuan, Ningyi; Fang, Shaoli; Baughman, Ray H.

    2017-02-01

    Linear supercapacitors suffer a severe loss of capacity at high rates due to the trade-off of radial ion diffusion and axial electron transport. Optimizing axial conductivity of electrodes is a key to circumvent this trade-off. We report here the synthesis of Au nanograin decorated aligned multiwall carbon nanotube (CNT) sheets, followed by the incorporation of polyaniline (PANI). The embedded Au nanograins results in fast radial ion diffusion and enhance axial electron transport in the linear electrodes. The flexible linear solid supercapacitor fabricated by twisting two PANI@Au@CNT yarns exhibits an outstanding electrochemical performance with a total volumetric capacitance of ∼6 F cm-3 at scan rate up to 10 V s-1. Diameter of the electrode has little effect on volumetric capacitance even at high scan rates because of its high electrical conductivity. Highly stretchable supercapacitors with high rate performance and excellent cycling and stretching stability have been also fabricated using buckled linear electrodes made by wrapping PANI@Au@CNT sheet on elastic rubber fibers. The stretchable linear supercapacitor possesses a stable total volumetric capacitance of up to ∼0.2 F cm-3 at scan rate of 1 V s-1 and at 400% strain, and remarkable capacitance retention of about 95% over 1000 stretch/release cycles.

  11. 4D Cellular Automaton Track Finder in the CBM Experiment

    Science.gov (United States)

    Akishina, Valentina; Kisel, Ivan

    2016-11-01

    The CBM experiment (FAIR/GSI, Darmstadt, Germany) will focus on the measurement of rare probes at interaction rates up to 10MHz with data flow of up to 1 TB/s. It requires a novel read-out and data-acquisition concept with self-triggered electronics and free-streaming data. In this case resolving different collisions is a non-trivial task and event building must be performed in software online. That requires full online event reconstruction and selection not only in space, but also in time, so-called 4D event building and selection. This is a task of the First-Level Event Selection (FLES). The FLES reconstruction and selection package consists of several modules: track finding, track fitting, short-lived particles finding, event building and event selection. The Cellular Automaton (CA) track finder algorithm was adapted towards time-based reconstruction. In this article, we describe in detail the modification done to the algorithm, as well as the performance of the developed time-based CA approach.

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

    Science.gov (United States)

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

    2016-05-04

    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.

  13. Ultrafast Imaging using Spectral Resonance Modulation.

    Science.gov (United States)

    Huang, Eric; Ma, Qian; Liu, Zhaowei

    2016-04-28

    CCD cameras are ubiquitous in research labs, industry, and hospitals for a huge variety of applications, but there are many dynamic processes in nature that unfold too quickly to be captured. Although tradeoffs can be made between exposure time, sensitivity, and area of interest, ultimately the speed limit of a CCD camera is constrained by the electronic readout rate of the sensors. One potential way to improve the imaging speed is with compressive sensing (CS), a technique that allows for a reduction in the number of measurements needed to record an image. However, most CS imaging methods require spatial light modulators (SLMs), which are subject to mechanical speed limitations. Here, we demonstrate an etalon array based SLM without any moving elements that is unconstrained by either mechanical or electronic speed limitations. This novel spectral resonance modulator (SRM) shows great potential in an ultrafast compressive single pixel camera.

  14. Ultrafast carriers dynamics in filled-skutterudites

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Liang; Xu, Xianfan, E-mail: xxu@purdue.edu [School of Mechanical Engineering and Birck Nanotechnology Center, Purdue University, West Lafayette, Indiana 47907 (United States); Salvador, James R. [Chemical and Materials Systems Laboratory, GM Global R and D, Warren, Michigan 48090 (United States)

    2015-06-08

    Carrier dynamics of filled-skutterudites, an important class of thermoelectric materials, is investigated using ultrafast optical spectroscopy. By tuning the wavelength of the probe laser, charge transfers at different electronic energy levels are interrogated. Analysis based on the Kramers-Kronig relation explains the complex spectroscopy data, which is mainly due to band filling caused by photo-excited carriers and free carrier absorption. The relaxation time of hot carriers is found to be about 0.4–0.6 ps, depending on the electronic energy level, and the characteristic time for carrier-phonon equilibrium is about 0.95 ps. These studies of carrier dynamics, which fundamentally determines the transport properties of thermoelectric material, can provide guidance for the design of materials.

  15. Ultrafast carriers dynamics in filled-skutterudites

    Science.gov (United States)

    Guo, Liang; Xu, Xianfan; Salvador, James R.

    2015-06-01

    Carrier dynamics of filled-skutterudites, an important class of thermoelectric materials, is investigated using ultrafast optical spectroscopy. By tuning the wavelength of the probe laser, charge transfers at different electronic energy levels are interrogated. Analysis based on the Kramers-Kronig relation explains the complex spectroscopy data, which is mainly due to band filling caused by photo-excited carriers and free carrier absorption. The relaxation time of hot carriers is found to be about 0.4-0.6 ps, depending on the electronic energy level, and the characteristic time for carrier-phonon equilibrium is about 0.95 ps. These studies of carrier dynamics, which fundamentally determines the transport properties of thermoelectric material, can provide guidance for the design of materials.

  16. Ultrafast spectroscopy studies on the mechanism of electron transfer and energy conversion in the isolated pseudo ginseng, water hyacinth and spinach chloroplasts

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    The spectroscopy characteristics and the fluorescence lifetime for the chloroplasts isolated from the pseudo ginseng, water hyacinth and spinach plant leaves have been studied by absorption spectra, low temperature steady-state fluorescence spectroscopy and single photon counting measurement under the same conditions and by the same methods. The similarity of the absorption spectra for the chloroplasts at room temperature suggests that different plants can efficiently absorb light of the same wavelength. The fluorescence decays in PS II measured at the natural QA state for the chloroplasts have been fitted by a three-exponential kinetic model. The three fluorescence lifetimes are 30, 274 and 805 ps for the pseudo ginseng chloroplast; 138, 521 and 1494 ps for the water hyacinth chloroplast; 197, 465 and 1459 ps for the spinach chloroplast, respectively. The slow lifetime fluorescence component is assigned to a collection of associated light harvesting Chl a/b proteins, the fast lifetime component to the reaction center of PS II and the middle lifetime component to the delay fluorescence of recombination of and Pheo-. The excitation energy conversion efficiency (η) in PS II RC is defined and calculated on the basis of the 20 ps electron transfer time constant model, 60%, 87% and 91% for the pseudo ginseng, water hyacinth and spinach chloroplasts, respectively. This interesting result is in unconformity with what is assumed to be 100% efficiency in PS II RC. Our result in this work stands in line with the 20 ps electron transfer time constant in PS II rather sound and the water hyacinth plant grows slower than the spinach plant does as envisaged on the efficiency. But, our results predict that those plants can perform highly efficient transfer of photo-excitation energy from the light-harvesting pigment system to the reaction center (closely to 100%). The conclusion contained in this paper reveals the plant growth characteristics expressed in the primary processes of

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

    Science.gov (United States)

    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.

  18. 19th International Conference on Ultrafast Phenomena

    CERN Document Server

    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.

  19. Ultrafast nanoimprint lithography (Invited Paper)

    Science.gov (United States)

    Xia, Qiangfei; Chou, Stephen Y.

    2005-04-01

    Both ultrafast thermal and photocurable nanoimprint lithography (NIL) are studied and high fidelity transfers of nanopatterns from molds to resists have been achieved. In ultrafast thermal NIL, we use a single excimer laser pulse to melt a NIL resist polymer and imprint it using a fused silica mold. The entire imprint process, from melting the polymer to completion of the imprint, takes less than 200 ns. This technique, termed laser assisted nanoimprint lithography (LAN), has patterned nanostructures in various polymer films with high fidelity over the entire mold area. In LAN, the short laser pulse is absorbed primarily by the resist and the laser energy is minute, hence substrate heating and distortion are negligible. In ultrafast photocurable NIL, a flash lamp (pulse width 94 μs) is used to crosslink photo curable resists over a 4 in. wafer with high uniformity by a single pulse. The significant reduction of the heating of the substrate and mold will greatly benefit overlay alignment.

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

    CERN Document Server

    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 infrared and UV-vis studies of the photochemistry of methoxycarbonylphenyl azides in solution.

    Science.gov (United States)

    Xue, Jiadan; Luk, Hoi Ling; Eswaran, S V; Hadad, Christopher M; Platz, Matthew S

    2012-06-07

    The photochemistry of 4-methoxycarbonylphenyl azide (2a), 2-methoxycarbonylphenyl azide (3a), and 2-methoxy-6-methoxycarbonylphenyl azide (4a) were studied by ultrafast time-resolved infrared (IR) and UV-vis spectroscopies in solution. Singlet nitrenes and ketenimines were observed and characterized for all three azides. Isoxazole species 3g and 4g are generated after photolysis of 3a and 4a, respectively, in acetonitrile. Triplet nitrene 4e formation correlated with the decay of singlet nitrene 4b. The presence of water does not change the chemistry or kinetics of singlet nitrenes 2b and 3b, but leads to protonation of 4b to produce nitrenium ion 4f. Singlet nitrenes 2b and 3b have lifetimes of 2 ns and 400 ps, respectively, in solution at ambient temperature. The singlet nitrene 4b in acetonitrile has a lifetime of about 800 ps, and reacts with water with a rate constant of 1.9 × 10(8) L·mol(-1)·s(-1) at room temperature. These results indicate that a methoxycarbonyl group at either the para or ortho positions has little influence on the ISC rate, but that the presence of a 2-methoxy group dramatically accelerates the ISC rate relative to the unsubstituted phenylnitrene. An ortho-methoxy group highly stabilizes the corresponding nitrenium ion and favors its formation in aqueous solvents. This substituent has little influence on the ring-expansion rate. These results are consistent with theoretical calculations for the various intermediates and their transition states. Cyclization from the nitrene to the azirine intermediate is favored to proceed toward the electron-deficient ester group; however, the higher energy barrier is the ring-opening process, that is, azirine to ketenimine formation, rendering the formation of the ester-ketenimine (4d') to be less favorable than the isomeric MeO-ketenimine (4d).

  2. SU-D-BRB-01: 4D-CT Lung Ventilation Images Vary with 4D-CT Sorting Techniques.

    Science.gov (United States)

    Yamamoto, T; Kabus, S; Lorenz, C; Johnston, E; Maxim, P; Loo, B; Keall, P

    2012-06-01

    4D-CT ventilation imaging is a novel promising technique for lung functional imaging and has potential as a biomarker for radiation pneumonitis, but has not been validated in human subjects. The current 4D- CT technique with phase-based sorting results in artifacts at an alarmingly high frequency (90%), which may introduce variations into ventilation calculations. The purpose of this study was to quantify the variability of 4D- CT ventilation imaging to 4D-CT sorting techniques. Two 4D-CT images were generated from the same data set by: (1) phase-based; (2) anatomic similarity- and abdominal displacement-based sorting for five patients. Two ventilation image sets (V_phase and V_anat) were then calculated by deformable image registration of peak-exhale and peak-inhale4D-CT images and quantification of regional volume change based on Hounsfield unit change. The variability of 4D-CT ventilation imaging wasquantified using the voxel-based Spearman rank correlation coefficients and Dice similarity coefficients (DSC) for the spatial overlap of segmented low- functional lung regions. The relationship between the abdominal motionrange variation and ventilation variation was also assessed using linearregression. Furthermore, the correlations between V_phase or V_anat and SPECT ventilation images (assumed ground-truth) were compared. In general, displacement- and anatomic similarity-based sorting reduced 4D- CT artifacts compared to phase-based sorting. The voxel-based correlationsbetween V_phase and V_anat were only moderate (range, 0.57-0.77). The DSCs for the low-functional lung regions were moderate to substantial (0.58-0.70). The relationship between the motion range variation and ventilation variation was strong on average (R2=0.79±0.25), suggesting that ventilation variations are related to 4D-CT artifacts. Vanat was found to improve correlations with SPECT ventilation images compared to V_phase. 4D-CT ventilation images vary markedly with 4D-CT sorting techniques. 4

  3. 4D Applications of GIS in Construction Management

    Directory of Open Access Journals (Sweden)

    A. Chaitanya Kumar

    2017-01-01

    Full Text Available Construction industries broadly involve different set of construction activities which are to be executed as per schedule and the major software used for scheduling is PRIMAVERA and Microsoft Project (MSP. But the software still lacks a feature of providing spatial aspects of information in construction schedule. Recently, advanced technology like 4D GIS plays a major role in overcoming the limitation of the software. 4D GIS technology includes integration of 2D drawings from AutoCAD and schedules prepared in PRIMAVERA software. In the present study, a multistair residential building has been selected. ARCMAP 10.2 is used for interlinking of schedules as well as drawings and ARCSCENE has been used for developing 4D view. This linkage between scheduled activities and respective drawings in GIS helps in identifying construction sequences and also in detecting logical errors that occur in project schedules. The developed 4D view provides better visualization of construction progress of a project.

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

    CERN Document Server

    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.

  5. Ultrafast collinear scattering and carrier multiplication in graphene.

    Science.gov (United States)

    Brida, D; Tomadin, A; Manzoni, C; Kim, Y J; Lombardo, A; Milana, S; Nair, R R; Novoselov, K S; Ferrari, A C; Cerullo, G; Polini, M

    2013-01-01

    Graphene is emerging as a viable alternative to conventional optoelectronic, plasmonic and nanophotonic materials. The interaction of light with charge carriers creates an out-of-equilibrium distribution, which relaxes on an ultrafast timescale to a hot Fermi-Dirac distribution, that subsequently cools emitting phonons. Although the slower relaxation mechanisms have been extensively investigated, the initial stages still pose a challenge. Experimentally, they defy the resolution of most pump-probe setups, due to the extremely fast sub-100 fs carrier dynamics. Theoretically, massless Dirac fermions represent a novel many-body problem, fundamentally different from Schrödinger fermions. Here we combine pump-probe spectroscopy with a microscopic theory to investigate electron-electron interactions during the early stages of relaxation. We identify the mechanisms controlling the ultrafast dynamics, in particular the role of collinear scattering. This gives rise to Auger processes, including charge multiplication, which is key in photovoltage generation and photodetectors.

  6. Ultrafast Surface Plasmonic Switch in Non-Plasmonic Metals

    CERN Document Server

    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...

  7. C4d staining as immunohistochemical marker in inflammatory myopathies.

    Science.gov (United States)

    Pytel, Peter

    2014-10-01

    The diagnosis of an inflammatory myopathy is often established based on basic histologic studies. Additional immunohistochemical studies are sometimes required to support the diagnosis and the classification of inflammatory myopathies. Staining for major histocompatibility complex 1 (MHC1) often shows increased sarcolemmal labeling in inflammatory myopathies. Endomysial capillary staining C5b-9 (membrane attack complex) is a feature that is reported as frequently associated with dermatomyositis. Immunohistochemical staining for C4d is widely used for various applications including the assessment of antibody-mediated rejection after solid organ transplantation. In the context of dermatomyositis, C4d staining has been described in skin biopsies but not in muscle biopsies. A total of 32 muscle biopsy specimens were examined. The hematoxylin and eosin-stained slides were reviewed, and immunohistochemical studies for MHC1, C5b-9, and C4d were conducted. The staining observed for C5b-9 and C4d was compared. Overall, the staining pattern for C4d mirrored the one observed for C5b-9 in the examined muscle biopsy specimens. There was high and statistically significant (P<0.0001) correlation between the staining seen with these 2 antibodies. Both antibodies labeled the cytoplasm of degenerating necrotic myofibers. In addition, both antibodies showed distinct endomysial capillary labeling in a subset of dermatomyositis. Areas with perifascicular atrophy often exhibited the most prominent vascular labeling for C4d and C5b-9. In conclusion, C4d and C5b-9 show similar expression patterns in muscle biopsies of patients with inflammatory myopathies and both highlight the presence of vascular labeling associated with dermatomyositis. C4d antibodies are widely used and may offer an alternative for C5b-9 staining.

  8. 4D Printing with Mechanically Robust, Thermally Actuating Hydrogels.

    Science.gov (United States)

    Bakarich, Shannon E; Gorkin, Robert; in het Panhuis, Marc; Spinks, Geoffrey M

    2015-06-01

    A smart valve is created by 4D printing of hydrogels that are both mechanically robust and thermally actuating. The printed hydrogels are made up of an interpenetrating network of alginate and poly(N-isopropylacrylamide). 4D structures are created by printing the "dynamic" hydrogel ink alongside other static materials. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  9. Ultrafast Spectroscopy of Semiconductor Devices

    DEFF Research Database (Denmark)

    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...

  10. Ultrafast vibrations of gold nanorings

    DEFF Research Database (Denmark)

    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...

  11. Ultrafast charge localization in a stripe-phase nickelate

    Energy Technology Data Exchange (ETDEWEB)

    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.

  12. Semaphorin 4D Promotes Skeletal Metastasis in Breast Cancer.

    Science.gov (United States)

    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.

  13. Semaphorin 4D Promotes Skeletal Metastasis in Breast Cancer.

    Directory of Open Access Journals (Sweden)

    Ying-Hua Yang

    Full Text Available 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.

  14. Ultra-fast silicon detectors (UFSD)

    Science.gov (United States)

    Sadrozinski, H. F.-W.; Anker, A.; Chen, J.; Fadeyev, V.; Freeman, P.; Galloway, Z.; Gruey, B.; Grabas, H.; John, C.; Liang, Z.; Losakul, R.; Mak, S. N.; Ng, C. W.; Seiden, A.; Woods, N.; Zatserklyaniy, A.; Baldassarri, B.; Cartiglia, N.; Cenna, F.; Ferrero, M.; Pellegrini, G.; Hidalgo, S.; Baselga, M.; Carulla, M.; Fernandez-Martinez, P.; Flores, D.; Merlos, A.; Quirion, D.; Mikuž, M.; Kramberger, G.; Cindro, V.; Mandić, I.; Zavrtanik, M.

    2016-09-01

    We report on measurements on Ultra-Fast Silicon Detectors (UFSD) which are based on Low-Gain Avalanche Detectors (LGAD). They are n-on-p sensors with internal charge multiplication due to the presence of a thin, low-resistivity diffusion layer below the junction, obtained with a highly doped implant. We have performed several beam tests with LGAD of different gain and report the measured timing resolution, comparing it with laser injection and simulations. For the 300 μm thick LGAD, the timing resolution measured at test beams is 120 ps while it is 57 ps for IR laser, in agreement with simulations using Weightfield2. For the development of thin sensors and their readout electronics, we focused on the understanding of the pulse shapes and point out the pivotal role the sensor capacitance plays.

  15. Ultra-fast silicon detectors (UFSD)

    Energy Technology Data Exchange (ETDEWEB)

    Sadrozinski, H.F.-W., E-mail: hartmut@ucsc.edu [SCIPP, Univ. of California Santa Cruz, CA 95064 (United States); Anker, A.; Chen, J.; Fadeyev, V.; Freeman, P.; Galloway, Z.; Gruey, B.; Grabas, H.; John, C.; Liang, Z.; Losakul, R.; Mak, S.N.; Ng, C.W.; Seiden, A.; Woods, N.; Zatserklyaniy, A. [SCIPP, Univ. of California Santa Cruz, CA 95064 (United States); Baldassarri, B.; Cartiglia, N.; Cenna, F.; Ferrero, M. [Univ. of Torino and INFN, Torino (Italy); and others

    2016-09-21

    We report on measurements on Ultra-Fast Silicon Detectors (UFSD) which are based on Low-Gain Avalanche Detectors (LGAD). They are n-on-p sensors with internal charge multiplication due to the presence of a thin, low-resistivity diffusion layer below the junction, obtained with a highly doped implant. We have performed several beam tests with LGAD of different gain and report the measured timing resolution, comparing it with laser injection and simulations. For the 300 μm thick LGAD, the timing resolution measured at test beams is 120 ps while it is 57 ps for IR laser, in agreement with simulations using Weightfield2. For the development of thin sensors and their readout electronics, we focused on the understanding of the pulse shapes and point out the pivotal role the sensor capacitance plays.

  16. Moduli instability in warped compactification - 4D effective theory approach

    CERN Document Server

    Arroja, F; Arroja, Frederico; Koyama, Kazuya

    2006-01-01

    We consider a 5D BPS dilatonic two brane model which reduces to the Randall-Sundrum model or the Horava-Witten theory for a particular choice of parameters. Recently new dynamical solutions were found by Chen et al., which describe a moduli instability of the warped geometry. Using a 4D effective theory derived by solving the 5D equations of motion, based on the gradient expansion method, we show that the exact solution of Chen et. al. can be reproduced within the 4D effective theory and we identify the origin of the moduli instability. We revisit the gradient expansion method with a new metric ansatz to clarify why the 4D effective theory solution can be lifted back to an exact 5D solution. Finally we argue against a recent claim that the 4D effective theory allows a much wider class of solutions than the 5D theory and provide a way to lift solutions in the 4D effective theory to 5D solutions perturbatively in terms of small velocities of the branes.

  17. True 4D Image Denoising on the GPU

    Science.gov (United States)

    Eklund, Anders; Andersson, Mats; Knutsson, Hans

    2011-01-01

    The use of image denoising techniques is an important part of many medical imaging applications. One common application is to improve the image quality of low-dose (noisy) computed tomography (CT) data. While 3D image denoising previously has been applied to several volumes independently, there has not been much work done on true 4D image denoising, where the algorithm considers several volumes at the same time. The problem with 4D image denoising, compared to 2D and 3D denoising, is that the computational complexity increases exponentially. In this paper we describe a novel algorithm for true 4D image denoising, based on local adaptive filtering, and how to implement it on the graphics processing unit (GPU). The algorithm was applied to a 4D CT heart dataset of the resolution 512  × 512  × 445  × 20. The result is that the GPU can complete the denoising in about 25 minutes if spatial filtering is used and in about 8 minutes if FFT-based filtering is used. The CPU implementation requires several days of processing time for spatial filtering and about 50 minutes for FFT-based filtering. The short processing time increases the clinical value of true 4D image denoising significantly. PMID:21977020

  18. Ultrafast thermal dynamics of nano-ripples formation via laser double pulses excitation

    Science.gov (United States)

    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.

  19. Combined convective and diffusive simulations: VERB-4D comparison with 17 March 2013 Van Allen Probes observations

    Science.gov (United States)

    Shprits, Yuri Y.; Kellerman, Adam C.; Drozdov, Alexander Y.; Spence, Harlan E.; Reeves, Geoffrey D.; Baker, Daniel N.

    2015-11-01

    This study is focused on understanding the coupling between different electron populations in the inner magnetosphere and the various physical processes that determine evolution of electron fluxes at different energies. Observations during the 17 March 2013 storm and simulations with a newly developed Versatile Electron Radiation Belt-4D (VERB-4D) are presented. Analysis of the drift trajectories of the energetic and relativistic electrons shows that electron trajectories at transitional energies with a first invariant on the scale of ~100 MeV/G may resemble ring current or relativistic electron trajectories depending on the level of geomagnetic activity. Simulations with the VERB-4D code including convection, radial diffusion, and energy diffusion are presented. Sensitivity simulations including various physical processes show how different acceleration mechanisms contribute to the energization of energetic electrons at transitional energies. In particular, the range of energies where inward transport is strongly influenced by both convection and radial diffusion are studied. The results of the 4-D simulations are compared to Van Allen Probes observations at a range of energies including source, seed, and core populations of the energetic and relativistic electrons in the inner magnetosphere.

  20. 4d N=1 from 6d (1,0)

    CERN Document Server

    Razamat, Shlomo S; Zafrir, Gabi

    2016-01-01

    We study the geometry of 4d N=1 SCFT's arising from compactification of 6d (1,0) SCFT's on a Riemann surface. We show that the conformal manifold of the resulting theory is characterized, in addition to moduli of complex structure of the Riemann surface, by the choice of a connection for a vector bundle on the surface arising from flavor symmetries in 6d. We exemplify this by considering the case of 4d N=1 SCFT's arising from M5 branes probing Z_k singularity compactified on a Riemann surface. In particular, we study in detail the four dimensional theories arising in the case of two M5 branes on Z_2 singularity. We compute the conformal anomalies and indices of such theories in 4d and find that they are consistent with expectations based on anomaly and the moduli structure derived from the 6 dimensional perspective.

  1. 4-D-Var or ensemble Kalman filter?

    OpenAIRE

    Kalnay, Eugenia; LI, HONG; Miyoshi, Takemasa; Yang, Shu-Chih; Ballabrera-Poy, Joaquim

    2007-01-01

    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 a...

  2. Influence of the electron-cation interaction on electron mobility in dye-sensitized ZnO and TiO2 nanocrystals: a study using ultrafast terahertz spectroscopy.

    Science.gov (United States)

    Nemec, H; Rochford, J; Taratula, O; Galoppini, E; Kuzel, P; Polívka, T; Yartsev, A; Sundström, V

    2010-05-14

    Charge transport and recombination in nanostructured semiconductors are poorly understood key processes in dye-sensitized solar cells. We have employed time-resolved spectroscopies in the terahertz and visible spectral regions supplemented with Monte Carlo simulations to obtain unique information on these processes. Our results show that charge transport in the active solar cell material can be very different from that in nonsensitized semiconductors, due to strong electrostatic interaction between injected electrons and dye cations at the surface of the semiconductor nanoparticle. For ZnO, this leads to formation of an electron-cation complex which causes fast charge recombination and dramatically decreases the electron mobility even after the dissociation of the complex. Sensitized TiO2 does not suffer from this problem due to its high permittivity efficiently screening the charges.

  3. A spectroelectrochemical cell for ultrafast two-dimensional infrared spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    El Khoury, Youssef; Van Wilderen, Luuk J. G. W.; Vogt, Tim; Winter, Ernst; Bredenbeck, Jens, E-mail: bredenbeck@biophysik.uni-frankfurt.org, E-mail: bredenbeck@biophysik.uni-frankfurt.de [Institut für Biophysik, Johann Wolfgang Goethe-Universität, Max-von-Laue-Strasse 1, 60438 Frankfurt (Germany)

    2015-08-15

    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.

  4. A spectroelectrochemical cell for ultrafast two-dimensional infrared spectroscopy

    Science.gov (United States)

    El Khoury, Youssef; Van Wilderen, Luuk J. G. W.; Vogt, Tim; Winter, Ernst; Bredenbeck, Jens

    2015-08-01

    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.

  5. Ultrafast spectroscopy of quasiparticle dynamics in cuprate superconductors

    Energy Technology Data Exchange (ETDEWEB)

    Li, Wei [National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093 (China); Zhang, Chunfeng, E-mail: cfzhang@nju.edu.cn [National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093 (China); Wang, Xiaoyong [National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093 (China); Chakhalian, Jak, E-mail: jchakhal@uark.edu [Department of Physics, University of Arkansas, Fayetteville, AR 72701 (United States); Xiao, Min, E-mail: mxiao@uark.edu [National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093 (China); Department of Physics, University of Arkansas, Fayetteville, AR 72701 (United States)

    2015-02-15

    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 YBa{sub 2}Cu{sub 3}O{sub 7−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.

  6. Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency.

    Science.gov (United States)

    Li, Chi; Zhou, Xu; Zhai, Feng; Li, Zhenjun; Yao, Fengrui; Qiao, Ruixi; Chen, Ke; Cole, Matthew Thomas; Yu, Dapeng; Sun, Zhipei; Liu, Kaihui; Dai, Qing

    2017-08-01

    Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow ultrafast dynamics to be characterized in materials. However, the pursuit of simultaneous ultimate spatial and temporal resolution of microscopy and spectroscopy is largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. Field-driven photoemission from metal tips provides high light-phase synchronization, but suffers large electron energy spreads (3-100 eV) as driven by a long wavelength laser (>800 nm). Here, ultrafast electron emission from carbon nanotubes (≈1 nm radius) excited by a 410 nm femtosecond laser is realized in the field-driven regime. In addition, the emitted electrons have great monochromaticity with energy spread as low as 0.25 eV. This great performance benefits from the extraordinarily high field enhancement and great stability of carbon nanotubes, superior to metal tips. The new nanotube-based ultrafast electron source opens exciting prospects for extending current characterization to sub-femtosecond temporal resolution as well as sub-nanometer spatial resolution. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  7. Ultrafast spectroscopy of semiconducting and multiferroic materials

    Science.gov (United States)

    Lou, Shitao

    In this thesis, we have used ultrafast spectroscopy to study the optical properties of two semiconductors, GaAs and Ge, and one hexagonal multiferroic material, LuMnO3. Both semiconductor and multiferroic materials are of great importance technologically and economically. By using ultrafast spectroscopy, we obtained time resolved electron and phonon dynamics directly, which is unavailable by conventional optical methods. Electron-hole pairs, coherent phonon oscillations and an optical coherence response are excited when femtosecond laser pulses interact with either GaAs or Ge crystals. The coherent phonon mode excited in GaAs/Ge is of T 2/T2g symmetry as determined by probe beam polarization analysis. The pump polarization dependence of the phonon oscillation is consistent with the transient stimulated Raman scattering (TSRS) mechanism. From the pump polarization dependence of the phonon oscillation, we have identified two excitation mechanisms contributing to the coherent phonon in GaAs, one is consistent with TSRS, and the other is consistent with screening effect of photoexcited electrons. The femtosecond laser pulse, with 800 nm center wavelength and polarized perpendicular to the c axis of LuMnO3, excites a narrow intra-atomic dxy, x2--y2 to d3z2--r2 transition in Mn. This excitation results in a transient reflectivity change for light of the same wavelength and polarization, by partial saturation of the transition. The relaxation time of this electronic excitation is about 1 ps. Furthermore, the electronic excitation resonantly excites a coherent optical phonon with A1 symmetry (TO: 118 cm--1 and LO: 120 cm --1), involving Lu ions motion along the c-axis, which is identified to be the soft mode driving the ferroelectric transition. A remarkable reversal of the sign of the oscillation amplitude (pi phase shift) of the reflectivity curve was observed upon comparing longitudinal optical (LO) with transverse optical (TO) mode geometries. The phase reversal is

  8. Comparison of C4d detection on erythrocytes and PTC-C4d to histological signs of antibody-mediated rejection in kidney transplantation.

    Science.gov (United States)

    Haidar, F; Kisserli, A; Tabary, T; McGregor, B; Noel, L H; Réveil, B; Toupance, O; Rieu, P; Thervet, E; Legendre, C; Morelon, E; Issa, N; Cohen, J H M

    2012-06-01

    C4d on erythrocytes (EC4d), C4d peritubular capillary deposition (PTC-C4d) staining and histology were compared in a cross-sectional cohort of 146 renal allograft biopsies (132 patients). EC4d levels paralleled PTC-C4d staining, but were more predictive of peritubular capillaritis (PTC). Donor-specific antibodies (DSA), PTC-C4d, EC4d and PTC were analyzed in an independent longitudinal follow-up cohort (96 biopsies, 76 patients). Seventy-six samples were PTC and EC4d concordant, 11 positive and 65 negative, 7 PTC-EC4d+ and 13 PTC+EC4d-. EC4d levels were related to DSA occurrence. With ABMR defined by PTC and DSA, all apparently discordant patients, EC4d negative, were correctly reassigned comparing EC4d level curves with rejection kinetics, with positive EC4d samples predating biopsy or late biopsies compared with ABMR flare-ups. All EC4d-positive patients without PTC or DSA had permanent high EC4d levels unrelated to rejection. EC4d was more abundant in PTC-positive (mean = 108.5%± 3.4; n = 50) than PTC-negative samples (mean = 88.1%± 1.3; n= 96; p PTC-C4d and EC4d for PTC were, respectively, 75%, 79%; 64%, 76% (p < 0.05); 28%, 46% (p < 0.05) and 93%, 94%. Values were similar for DSA. A noninvasive blood test, EC4d, and particularly longitudinally monitoring EC4d levels, may increase surrogate ABMR testing options. © Copyright 2012 The American Society of Transplantation and the American Society of Transplant Surgeons.

  9. Photonic metasurfaces for spatiotemporal and ultrafast light control

    Science.gov (United States)

    Shaltout, Amr Mohammad Emadeldin Abdelmaksoud

    The emergence of photonic metasurfaces - planar arrays of nano-antennas - has enabled a new paradigm of light control through wave-front engineering. Space-gradient metasurfaces induce spatially varying phase and/or polarization to propagating light. As a consequence, photons propagating through space-gradient metasurfaces can be engineered to undergo a change to their momentum, angular momentum and/or spin states. In our study, we implement metasurface-based devices that break the spin symmetry of light to obtain Photonic Spin Hall Effect (PSHE). We utilized PSHE to design a real-time circular dichroism spectrometer, a device vital in bio-sensing, and an optical rotator used in secure quantum communications. In addition, we developed metasurface based Fabry--Perot nano-cavities, which go beyond the diffraction limit of light, a requirement to enhance photonic spontaneous emission using the Purcell effect. In addition, we demonstrate that the field of flat photonics is further empowered by utilizing time-gradient metasurfaces with dynamic responses to propagating light. A new genus of optical devices and physical effects can be realized. Photons experience inelastic interactions with time-varying metasurfaces resulting in a Doppler-like wavelength-shift. Furthermore, Snell's relations are modified to a more universal form not limited by Lorentz reciprocity, hence meeting all the requirements to build magnetic-free optical isolators. Finally, we construct the concept of ultrafast metasurfaces. We integrate spatial interference methodology delivered by metasurfaces and temporal interference of phase-locked frequency-comb provided by ultrafast technology. This leads to generation of coherent 4D space-time optical patterns, which is implemented to achieve ultrafast laser beam steering over hundred-picosecond scale.

  10. Oscillator strengths and branching fractions of 4d75p-4d75s Rh II transitions

    Science.gov (United States)

    Bouazza, Safa

    2017-01-01

    This work reports semi-empirical determination of oscillator strengths, transition probabilities and branching fractions for Rh II 4d75p-4d75s transitions in a wide wavelength range. The angular coefficients of the transition matrix, beforehand obtained in pure SL coupling with help of Racah algebra are transformed into intermediate coupling using eigenvector amplitudes of these two configuration levels determined for this purpose; The transition integral was treated as free parameter in the least squares fit to experimental oscillator strength (gf) values found in literature. The extracted value: 5s|r1|4d75p> =2.7426 ± 0.0007 is slightly smaller than that computed by means of ab-initio method. Subsequently to oscillator strength evaluations, transition probabilities and branching fractions were deduced and compared to those obtained experimentally or through another approach like pseudo-relativistic Hartree-Fock model including core-polarization effects.

  11. Enterococcus faecalis promotes osteoclastogenesis and semaphorin 4D expression.

    Science.gov (United States)

    Wang, Shuai; Deng, Zuhui; Seneviratne, Chaminda J; Cheung, Gary S P; Jin, Lijian; Zhao, Baohong; Zhang, Chengfei

    2015-10-01

    Enterococcus faecalis is considered a major bacterial pathogen implicated in endodontic infections and contributes considerably to periapical periodontitis. This study aimed to investigate the potential mechanisms by which E. faecalis accounts for the bone destruction in periapical periodontitis in vitro. Osteoclast precursor RAW264.7 cells were treated with E. faecalis ATCC 29212 and a wild strain of E. faecalis derived clinically from an infected root canal. The results showed that, to some extent, E. faecalis induced the RAW264.7 cells to form tartrate-resistant acid phosphatase (TRAP)-positive multinucleated osteoclast-like cells. This pathogen markedly stimulated RAW264.7 cells to express semaphorin 4D (Sema4D), which inhibits bone formation. Once RAW264.7 cells were primed by low-dose receptor activator of nuclear factor-kappa B ligand (RANKL), E. faecalis could significantly increase the production of TRAP-positive multinucleated cells and up-regulate the expression of osteoclast-specific markers, including NFATc1, TRAP and cathepsin K. Both p38 and ERK1/2 MAPK signaling pathways were activated by E. faecalis in RANKL-primed RAW264.7 cells, and meanwhile the expression of Sema4D was highly increased. In conclusion, E. faecalis may greatly contribute to the bone resorption in periapical periodontitis by promoting RANKL-dependent osteoclastogenesis and expression of Sema4D through activation of p38 and ERK1/2 MAPK signaling pathways.

  12. Ultrafast photonic crystal optical switching

    Institute of Scientific and Technical Information of China (English)

    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.

  13. Ultrafast Dynamics of Energetic Materials

    Science.gov (United States)

    2014-01-23

    make tens of thousands of shocks on the same sample. As shown in Fig. 5, the original sample used a monolayer of nitrobenzoic acid ( NBA ). Also...there is a few micrometer thick polymer tamping layer. The NBA molecule is an EM simulant with a nitro group. We are focused on the nitro groups due...in Fig. 5d. We have 13 Fig.5. Sample construction for ultrafast shock vibrational spectroscopy. A monolayer of NBA is deposited onto a metal

  14. 4D flow mri post-processing strategies for neuropathologies

    Science.gov (United States)

    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

  15. 4D MR imaging using robust internal respiratory signal

    Science.gov (United States)

    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.

  16. SU-E-T-790: Validation of 4D Measurement-Guided Dose Reconstruction (MGDR) with OCTAVIUS 4D System

    Energy Technology Data Exchange (ETDEWEB)

    Lee, V; Leung, R; Wong, M; Law, G; Lee, K; Tung, S; Chan, M [Tuen Mun Hospital, Hong Kong, Hong Kong (S.A.R) (Hong Kong); Blanck, O [University Clinic Schleswig-Holstein, Kiel, Kiel (Germany)

    2015-06-15

    Purpose: To validate the MGDR of OCTAVIUS 4D system (PTW, Freiburg, Germany) for quality assurance (QA) of volumetric-modulated arc radiotherapy (VMAT). Methods: 4D-MGDR measurements were divided into two parts: 1) square fields from 2×2 to 25×25 cm{sup 2} at 0°, 10° and 45° gantry, and 2) 8 VMAT plans (5 nasopharyngeal and 3 prostate) collapsed to gantry 40° in QA mode in Monaco v5.0 (Elekta, CMS, Maryland Heights, MO) were delivered on the OCTAVIUS 4D phantom with the OCTAVIUS 1500 detector plane perpendicular to either the incident beam to obtain the reconstructed dose (OCTA4D) or the 0° gantry axis to obtain the raw doses (OCTA3D) in Verisoft 6.1 (PTW, Freiburg, Germany). Raw measurements of OCTA3D were limited to < 45° gantry to avoid >0.5% variation of detector angular response with respect to 0° gantry as determined previously. Reconstructed OCTA4D and raw OCTA3D doses for all plans were compared at the same detector plane using γ criteria of 2% (local dose)/2mm and 3%/3mm criteria. Results: At gantry 0° and 10°, the γ results for all OCTA4D on detector plane coinciding with OCTA3D were over 90% at 2%/2mm except for the largest field (25×25 cm{sup 2} ) showing >88%. For square field at 45° gantry, γ passing rate is > 90% for fields smaller than 15x 15cm2 but < 80% for field size of 20 x20 cm{sup 2} upward. For VMAT, γ results showed 94% and 99% passing rate at 2%/2mm and 3%/3mm, respectively. Conclusion: OCTAVIUS 4D system has compromised accuracy in reconstructing dose away from the central beam axis, possibly due to the off-axis softening correction and errors of the percent depth dose data necessary as input for MGDR. Good results in VMAT delivery suggested that the system is relatively reliable for VMAT with small segments.

  17. Ultrafast Hierarchical OTDM/WDM Network

    Directory of Open Access Journals (Sweden)

    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.

  18. Avant-Garde Ultrafast Laser Writing

    Directory of Open Access Journals (Sweden)

    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.

  19. Ultrafast THz saturable absorption in doped semiconductors at room temperature

    DEFF Research Database (Denmark)

    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. Ultraf...... and provides an up-to-date view of this important and rapidly advancing field....

  20. Construction Management Utilizing 4D CAD and Operations Simulation Methodologies

    Institute of Scientific and Technical Information of China (English)

    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.

  1. 4D embryonic cardiography using gated optical coherence tomography

    Science.gov (United States)

    Jenkins, M. W.; Rothenberg, F.; Roy, D.; Nikolski, V. P.; Hu, Z.; Watanabe, M.; Wilson, D. L.; Efimov, I. R.; Rollins, A. M.

    2006-01-01

    Simultaneous imaging of very early embryonic heart structure and function has technical limitations of spatial and temporal resolution. We have developed a gated technique using optical coherence tomography (OCT) that can rapidly image beating embryonic hearts in four-dimensions (4D), at high spatial resolution (10-15 μm), and with a depth penetration of 1.5 - 2.0 mm that is suitable for the study of early embryonic hearts. We acquired data from paced, excised, embryonic chicken and mouse hearts using gated sampling and employed image processing techniques to visualize the hearts in 4D and measure physiologic parameters such as cardiac volume, ejection fraction, and wall thickness. This technique is being developed to longitudinally investigate the physiology of intact embryonic hearts and events that lead to congenital heart defects.

  2. A brief review of the 2d/4d correspondences

    CERN Document Server

    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.

  3. 4D Art: corpos reais e virtuais, uma realidade aumentada

    Directory of Open Access Journals (Sweden)

    Michel Lemieux

    2016-05-01

    Full Text Available A companhia canadense 4D Art fascina o olhar do público e interroga seus sentidos de realidade e presença pela interação cênica dos movimentos de corpos reais e virtuais. Para compreender os processos de criação da cena multimídia de 4D Art, apresenta-se uma entrevista exclusiva realizada com os diretores artísticos Michel Lemieux e Victor Pilon. As motivações artísticas do jogo real e virtual, os procedimentos empregados na criação das figuras virtuais e os desafios enfrentados pelos atores aparecem nas palavras dos criadores.

  4. 4d SCFTs from negative-degree line bundles

    CERN Document Server

    Nardoni, Emily

    2016-01-01

    We construct 4d $\\mathcal{N}=1$ quantum field theories by compactifying the (2,0) theories on a Riemann surface with genus $g$ and $n$ punctures, where the normal bundle decomposes into a sum of two line bundles with possibly negative degrees $p$ and $q$. Until recently, the only available field-theoretic constructions required the line bundle degrees to be nonnegative, although supergravity solutions were constructed in the literature for the zero-puncture case for all $p$ and $q$. Here, we provide field-theoretic constructions and computations of the central charges of 4d $\\mathcal{N}=1$ SCFTs that are the IR limit of M5-branes wrapping a surface with general $p$ or $q$ negative, for general genus $g$ and number of maximal punctures $n$.

  5. Topological wave functions and the 4D-5D lift

    CERN Document Server

    Gao, Peng

    2008-01-01

    We revisit the holomorphic anomaly equations satisfied by the topological string amplitude from the perspective of the 4D-5D lift, in the context of ``magic'' N=2 supergravity theories. In particular, we interpret the Gopakumar-Vafa relation between 5D black hole degeneracies and the topological string amplitude as the result of a canonical transformation from 4D to 5D charges. Moreover we use the known Bekenstein-Hawking entropy of 5D black holes to constrain the asymptotic behavior of the topological wave function at finite topological coupling but large K\\"ahler classes. In the process, some subtleties in the relation between 5D black hole degeneracies and the topological string amplitude are uncovered, but not resolved. Finally we extend these considerations to the putative one-parameter generalization of the topological string amplitude, and identify the canonical transformation as a Weyl reflection inside the 3D duality group.

  6. Expression of Sema4D in patients with cerebral infarction and its clinical significance

    Institute of Scientific and Technical Information of China (English)

    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

  7. Ultrafast Coherent Control and Characterization of Surface Reactions using FELs

    Energy Technology Data Exchange (ETDEWEB)

    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.

  8. Advanced Instrumentation for Ultrafast Science at the LCLS

    Energy Technology Data Exchange (ETDEWEB)

    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.

  9. Compact ultrafast orthogonal acceleration time-of-flight mass spectrometer for on-line gas analysis by electron impact ionization and soft single photon ionization using an electron beam pumped rare gas excimer lamp as VUV-light source.

    Science.gov (United States)

    Mühlberger, F; Saraji-Bozorgzad, M; Gonin, M; Fuhrer, K; Zimmermann, R

    2007-11-01

    Orthogonal acceleration time-of-flight mass spectrometers (oaTOFMS), which are exhibiting a pulsed orthogonal extraction of ion bunches into the TOF mass analyzer from a continuous primary ion beam, are well-suited for continuous ionization methods such as electron impact ionization (EI). Recently an electron beam pumped rare gas excimer lamp (EBEL) was introduced, which emits intensive vacuum UV (VUV) radiation at, e.g., 126 nm (argon excimer) and is well suited as the light source for soft single photon ionization (SPI) of organic molecules. In this paper, a new compact oaTOFMS system which allows switching between SPI, using VUV-light from an EBEL-light source, and conventional EI is described. With the oaTOFMS system, EBEL-SPI and EI mass spectral transients can be recorded at very high repetition rates (up to 100 kHz), enabling high duty cycles and therefore good detection efficiencies. By using a transient recorder card with the capability to perform on-board accumulation of the oaTOF transients, final mass spectra with a dynamic range of 106 can be saved to the hard disk at a rate of 10 Hz. As it is possible to change the ionization modes (EI and SPI) rapidly, a comprehensive monitoring of complex gases with highly dynamic compositions, such as cigarette smoke, is possible. In this context, the EI based mass spectra address the bulk composition (compounds such as water, oxygen, carbon dioxide, etc. in the up to percentage concentration range) as well as some inorganic trace gases such as argon, sulfur dioxide, etc. down to the low ppm level. The EBEL-SPI mass spectra on the other hand are revealing the organic composition down to the lower ppb concentration range.

  10. Phosphodiesterase 4D gene polymorphisms in sudden sensorineural hearing loss.

    Science.gov (United States)

    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.

  11. Analysis of 4D Var Data Assimilation Application Issues

    Science.gov (United States)

    Trailovic, L.; Etherton, B.; Harrop, C.; Govett, M.

    2016-12-01

    This paper summarizes the challenges encountered with our ongoing development and use of a software system designed to facilitate exploration of computational optimizations and strategies for Data Assimilation (DA). The software system is designed and constructed from scratch using modern software development methods and tools, though it incorporates components of pre-existing systems where appropriate. We present results of experiments that employ this system to test approaches for assimilation of observations using a four-dimensional variational (4D Var) scheme. We propose a modular DA system software architecture and demonstrate its utility using a set of models of varying realism and complexity. The software system design and implementation was initially tested and validated using a simple chaotic atmospheric model. A Quasi-Geostrophic (QG) atmospheric model was used to conduct DA experiments of increased difficulty and to validate the software design at larger scales of model complexity. Our QG DA study focused on 2016 winter weather data where a Nature run was used to represent the "true" state of the atmosphere and observations, whereas observation error covariance and observation operator were adapted from pre-existing DA systems. To increase performance, a parallel-in-time algorithm was applied to solve the proposed 4D Var data assimilation problem. That is, the assimilation window was divided into multiple sub-intervals, which allowed for parallelization of the cost function and gradient computations. Continuity equations of the solution were added as constraints across interval boundaries. This approach produced a different formulation of the variational data assimilation problem than weakly constrained 4D Var. We explored a combination of serial and parallel 4D Var algorithms to increase performance.

  12. 4D tropospheric tomography using GPS slant wet delays

    Directory of Open Access Journals (Sweden)

    A. Flores

    Full Text Available Tomographic techniques are successfully applied to obtain 4D images of the tropospheric refractivity in a local dense network of global positioning system (GPS receivers. We show here how GPS data are processed to obtain the tropospheric slant wet delays and discuss the validity of the processing. These slant wet delays are the observables in the tomographic processing. We then discuss the inverse problem in 4D tropospheric tomography making extensive use of simulations to test the system and define the resolution and the impact of noise. Finally, we use data from the Kilauea network in Hawaii for February 1, 1997, and a local 4×4×40 voxel grid on a region of 400 km2 and 15 km in height to produce the corresponding 4D wet refractivity fields, which are then validated using forecast analysis from the European Center for Medium Range Weather Forecast (ECMWF. We conclude that tomographic techniques can be used to monitor the troposphere in time and space.

    Key words: Radio science (remote sensing; instruments and techniques

  13. 4D-Flow validation, numerical and experimental framework

    Science.gov (United States)

    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.

  14. Coherent ultrafast charge transfer in an organic photovoltaic blend.

    Science.gov (United States)

    Falke, Sarah Maria; Rozzi, Carlo Andrea; Brida, Daniele; Maiuri, Margherita; Amato, Michele; Sommer, Ephraim; De Sio, Antonietta; Rubio, Angel; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph

    2014-05-30

    Blends of conjugated polymers and fullerene derivatives are prototype systems for organic photovoltaic devices. The primary charge-generation mechanism involves a light-induced ultrafast electron transfer from the light-absorbing and electron-donating polymer to the fullerene electron acceptor. Here, we elucidate the initial quantum dynamics of this process. Experimentally, we observed coherent vibrational motion of the fullerene moiety after impulsive optical excitation of the polymer donor. Comparison with first-principle theoretical simulations evidences coherent electron transfer between donor and acceptor and oscillations of the transferred charge with a 25-femtosecond period matching that of the observed vibrational modes. Our results show that coherent vibronic coupling between electronic and nuclear degrees of freedom is of key importance in triggering charge delocalization and transfer in a noncovalently bound reference system. Copyright © 2014, American Association for the Advancement of Science.

  15. Control and mapping ultrafast plasmons with PEEM

    Science.gov (United States)

    Ji, Boyu; Qin, Jiang; Lang, Peng; Koya, Alemayehu Nana; Hao, Zuoqiang; Song, Xiaowei; Lin, Jingquan

    2016-11-01

    We report the direct imaging of plasmon on the tips of nano-prisms in a bowtie structure excited by 7 fs laser pulses and probing of ultrafast plasmon dynamics by combining the pump-probe technology with three-photon photoemission electron microscopy. A series of images of the evolution of local surface plasmon modes on different tips of the bowtie are obtained by the time-resolved three-photon photoemission electron microscopy, and the result discloses that plasmon excitation is dominated by the interference of the pump and probe pulses within the first 13 fs of the delay time, and thereafter the individual plasmon starts to oscillate on its own characteristic resonant frequencies. On the other hand, control of the near-field distribution was realized by variation of the phase delay of two orthogonally polarized 200fs laser pulses. The experimental results of the optical near-field distribution control are well reproduced by finite-difference time-domain simulations and understood by linear combination of electric charge distribution of the bowtie by s- and p- polarized light illumination. In addition, an independent shift of the excitation position or the phase of the near-field can be realized by coherent control of two orthogonally polarized fs laser pulses.

  16. Ultrafast endocytosis at mouse hippocampal synapses

    Science.gov (United States)

    Watanabe, Shigeki; Rost, Benjamin R.; Camacho-Pérez, Marcial; Davis, M. Wayne; Söhl-Kielczynski, Berit; Rosenmund, Christian; Jorgensen, Erik M.

    2013-12-01

    To sustain neurotransmission, synaptic vesicles and their associated proteins must be recycled locally at synapses. Synaptic vesicles are thought to be regenerated approximately 20s after fusion by the assembly of clathrin scaffolds or in approximately 1s by the reversal of fusion pores via `kiss-and-run' endocytosis. Here we use optogenetics to stimulate cultured hippocampal neurons with a single stimulus, rapidly freeze them after fixed intervals and examine the ultrastructure using electron microscopy--`flash-and-freeze' electron microscopy. Docked vesicles fuse and collapse into the membrane within 30ms of the stimulus. Compensatory endocytosis occurs within 50 to 100ms at sites flanking the active zone. Invagination is blocked by inhibition of actin polymerization, and scission is blocked by inhibiting dynamin. Because intact synaptic vesicles are not recovered, this form of recycling is not compatible with kiss-and-run endocytosis; moreover, it is 200-fold faster than clathrin-mediated endocytosis. It is likely that `ultrafast endocytosis' is specialized to restore the surface area of the membrane rapidly.

  17. Ultrafast vibrations of gold nanorings

    DEFF Research Database (Denmark)

    Kelf, T; Tanaka, Y; Matsuda, O;

    2011-01-01

    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.......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...

  18. Ultrafast quenching of ring closure in molecular switches, self-assembled on gold nanoparticles

    NARCIS (Netherlands)

    Hania, Ralph; Pugžlys, Audrius; Kudernac, Tibor; Jonkman, Harry; Duppen, Koos; DeSilvestri, S.; Kobayashi, T.; Kobayashi, T.; Nelson, K.A.; Okada, T.

    2005-01-01

    We report the ultrafast quenching of the ring-closure reaction in BTE-based photochromic switches self-assembled on gold nanoparticles. The photoinduced population dynamics of the switches reveals that the electronic states of the switch molecules are strongly mixed with the states of the gold

  19. LUX — A Recirculating Linac-based Ultrafast X-ray Source

    Science.gov (United States)

    Corlett, J. N.; Barletta, W. A.; DeSantis, S.; Doolittle, L.; Fawley, W. M.; Green, M. A.; Heimann, P.; Leone, S. R.; Lidia, S.; Li, D.; Parmigiani, F.; Ratti, A.; Robinson, K.; Schoenlein, R.; Staples, J.; Wan, W.; Wells, R.; Wilcox, R.; Wolski, A.; Zholents, A.

    2004-05-01

    We describe the design of a proposed source of ultra-fast synchrotron radiation x-ray pulses based on a recirculating superconducting linac, with an integrated array of ultrafast laser systems. The source produces x-ray pulses with duration of 10-50 fs at a 10 kHz repetition rate, with tunability from EUV to hard x-ray regimes, and optimized for the study of ultra-fast dynamics. A high-brightness rf photocathode provides electron bunches. An injector linac accelerates the beam to the 100 MeV range, and is followed by four passes through a 700 MeV recirculating linac. Ultrafast hard x-ray pulses are obtained by a combination of electron bunch manipulation, transverse temporal correlation of the electrons, and x-ray pulse compression. EUV and soft x-ray pulses as short as 10 fs are generated in a harmonic-cascade free electron laser scheme. We describe the facility major systems and peformance.

  20. Ultrafast quenching of ring closure in molecular switches, self-assembled on gold nanoparticles

    NARCIS (Netherlands)

    Hania, Ralph; Pugžlys, Audrius; Kudernac, Tibor; Jonkman, Harry; Duppen, Koos; DeSilvestri, S.; Kobayashi, T.; Kobayashi, T.; Nelson, K.A.; Okada, T.

    2005-01-01

    We report the ultrafast quenching of the ring-closure reaction in BTE-based photochromic switches self-assembled on gold nanoparticles. The photoinduced population dynamics of the switches reveals that the electronic states of the switch molecules are strongly mixed with the states of the gold parti

  1. Decoupling Bulk and Surface Contributions in Water- Splitting Photocatalysts by In Situ Ultrafast Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Appavoo, Kannatassen [Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Mingzhao, Liu [Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Black, Charles T. [Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Sfeir, Matthew Y. [Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials

    2015-05-10

    By performing ultrafast emission spectroscopy in an operating, bias-controlled photoelectrochemical cell, we distinguish between bulk (charge transport) and surface (chemical reaction) recombination processes in a nanostructured photocatalyst and correlate its electronic properties directly with its incident-photon-to-current efficiency.

  2. Efeitos do 2,4-D, em laranjeira baianinha Effects of 2,4-D on the baianinha orange

    Directory of Open Access Journals (Sweden)

    Ody Rodriguez

    1960-01-01

    Full Text Available Com o objetivo de conhecer a reação da laranjeira Baianinha à aplicação de 2,4-D, principalmente com relação à queda de frutas, executamos um experimento de pulverização de plantas com solução deste hormônio sintético, na Estação Experimental de Limeira, zona de maior densidade citrícola do Estado de São Paulo. Tôdas as concentrações do ácido, usadas no experimento, causaram modificações nos caracteres normais da laranjeira (Citrus sinensis Osb. As fôlhas, flôres e frutas sofreram modificações mais ou menos acentuadas, de acordo com a concentração do produto, os resultados permitindo contra-indicar pulverizações com 2,4-D nas condições apresentadas; mostram também, que as modificações atribuídas ao hormônio só se produziram durante a safra em que se fizeram os tratamentos. São apresentados dados das produções, do aumento de pêso das frutas e de queda das mesmas e das fôlhas, bem como ilustrações das principais modificações ocorridas nas frutas. A aplicação do 2,4-D causou decréscimo linear do número de frutas, proporcional as dosagens do hormônio. Como conseqüência houve aumento do seu pêso médio. Êste fato pode ser de utilidade para outras variedades cítricas, quando houver interesse no aumento de tamanho das frutas.The reaction of the Baianinha orange (Citrus sinensis Osb., a Brazilian hud sport of the Washington Navel, to applications of 2,4-D was studied at the Limeira Agr. Exp. Sta., São Paulo. All concentrations of this hormonial herbicide used in the tests induced some modifications of the normal characteristics of the plants when compared with the controls. The leaves, flowers, and fruits were the plant parts most affected by the treatments. Some of the morphological changes induced on the fruits tend to confirm the view that the Baia orange originated as a mutation from the Seleta variety. Data obtained on the yield, weight per fruit, and fruit drop indicate that application

  3. ULTRASSONOGRAFIA GESTACIONAL 3D/4D EM PEQUENOS ANIMAIS

    Directory of Open Access Journals (Sweden)

    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

  4. Ablation and ultrafast dynamics of zinc selenide under femtosecond laser irradiation

    Institute of Scientific and Technical Information of China (English)

    Xiaofeng Wang; Tianqing Jia; Xiaoxi Li; Chengbin Li; Donghai Feng; Haiyi Sun; Shizhen Xu; Zhizhan Xu

    2005-01-01

    The ablation in zinc selenide (ZnSe) crystal is studied by using 150-fs, 800-nm laser system. The images of the ablation pit measured by scanning electronic microscope (SEM) show no thermal stress and melting dynamics. The threshold fluence is measured to be 0.7 J/cm2. The ultrafast ablation dynamics is studied by using pump and probe method. The result suggests that optical breakdown and ultrafast melting take place in ZnSe irradiated under femtosecond laser pulses.

  5. Fast GPU based adaptive filtering of 4D echocardiography.

    Science.gov (United States)

    Broxvall, Mathias; Emilsson, Kent; Thunberg, Per

    2012-06-01

    Time resolved three-dimensional (3D) echocardiography generates four-dimensional (3D+time) data sets that bring new possibilities in clinical practice. Image quality of four-dimensional (4D) echocardiography is however regarded as poorer compared to conventional echocardiography where time-resolved 2D imaging is used. Advanced image processing filtering methods can be used to achieve image improvements but to the cost of heavy data processing. The recent development of graphics processing unit (GPUs) enables highly parallel general purpose computations, that considerably reduces the computational time of advanced image filtering methods. In this study multidimensional adaptive filtering of 4D echocardiography was performed using GPUs. Filtering was done using multiple kernels implemented in OpenCL (open computing language) working on multiple subsets of the data. Our results show a substantial speed increase of up to 74 times, resulting in a total filtering time less than 30 s on a common desktop. This implies that advanced adaptive image processing can be accomplished in conjunction with a clinical examination. Since the presented GPU processor method scales linearly with the number of processing elements, we expect it to continue scaling with the expected future increases in number of processing elements. This should be contrasted with the increases in data set sizes in the near future following the further improvements in ultrasound probes and measuring devices. It is concluded that GPUs facilitate the use of demanding adaptive image filtering techniques that in turn enhance 4D echocardiographic data sets. The presented general methodology of implementing parallelism using GPUs is also applicable for other medical modalities that generate multidimensional data.

  6. Phase and amplitude binning for 4D-CT imaging

    Science.gov (United States)

    Abdelnour, A. F.; Nehmeh, S. A.; Pan, T.; Humm, J. L.; Vernon, P.; Schöder, H.; Rosenzweig, K. E.; Mageras, G. S.; Yorke, E.; Larson, S. M.; Erdi, Y. E.

    2007-07-01

    We compare the consistency and accuracy of two image binning approaches used in 4D-CT imaging. One approach, phase binning (PB), assigns each breathing cycle 2π rad, within which the images are grouped. In amplitude binning (AB), the images are assigned bins according to the breathing signal's full amplitude. To quantitate both approaches we used a NEMA NU2-2001 IEC phantom oscillating in the axial direction and at random frequencies and amplitudes, approximately simulating a patient's breathing. 4D-CT images were obtained using a four-slice GE Lightspeed CT scanner operating in cine mode. We define consistency error as a measure of ability to correctly bin over repeated cycles in the same field of view. Average consistency error μe ± σe in PB ranged from 18% ± 20% to 30% ± 35%, while in AB the error ranged from 11% ± 14% to 20% ± 24%. In PB nearly all bins contained sphere slices. AB was more accurate, revealing empty bins where no sphere slices existed. As a proof of principle, we present examples of two non-small cell lung carcinoma patients' 4D-CT lung images binned by both approaches. While AB can lead to gaps in the coronal images, depending on the patient's breathing pattern, PB exhibits no gaps but suffers visible artifacts due to misbinning, yielding images that cover a relatively large amplitude range. AB was more consistent, though often resulted in gaps when no data existed due to patients' breathing pattern. We conclude AB is more accurate than PB. This has important consequences to treatment planning and diagnosis.

  7. Phase and amplitude binning for 4D-CT imaging

    Energy Technology Data Exchange (ETDEWEB)

    Abdelnour, A F [US Patent and Trademark Office, Alexandria, VA (United States); Nehmeh, S A [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Pan, T [M.D. Anderson Cancer Center, Houston, TX (United States); Humm, J L [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Vernon, P [GE Healthcare Technologies, Waukesha, WI (United States); Schoeder, H [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Rosenzweig, K E [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Mageras, G S [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Yorke, E [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Larson, S M [Memorial Sloan-Kettering Cancer Center, New York, NY (United States); Erdi, Y E [Memorial Sloan-Kettering Cancer Center, New York, NY (United States)

    2007-07-21

    We compare the consistency and accuracy of two image binning approaches used in 4D-CT imaging. One approach, phase binning (PB), assigns each breathing cycle 2{pi} rad, within which the images are grouped. In amplitude binning (AB), the images are assigned bins according to the breathing signal's full amplitude. To quantitate both approaches we used a NEMA NU2-2001 IEC phantom oscillating in the axial direction and at random frequencies and amplitudes, approximately simulating a patient's breathing. 4D-CT images were obtained using a four-slice GE Lightspeed CT scanner operating in cine mode. We define consistency error as a measure of ability to correctly bin over repeated cycles in the same field of view. Average consistency error {mu}{sub e} {+-} {sigma}{sub e} in PB ranged from 18% {+-} 20% to 30% {+-} 35%, while in AB the error ranged from 11% {+-} 14% to 20% {+-} 24%. In PB nearly all bins contained sphere slices. AB was more accurate, revealing empty bins where no sphere slices existed. As a proof of principle, we present examples of two non-small cell lung carcinoma patients' 4D-CT lung images binned by both approaches. While AB can lead to gaps in the coronal images, depending on the patient's breathing pattern, PB exhibits no gaps but suffers visible artifacts due to misbinning, yielding images that cover a relatively large amplitude range. AB was more consistent, though often resulted in gaps when no data existed due to patients' breathing pattern. We conclude AB is more accurate than PB. This has important consequences to treatment planning and diagnosis.

  8. Linear and ultrafast nonlinear plasmonics of single nano-objects

    Science.gov (United States)

    Crut, Aurélien; Maioli, Paolo; Vallée, Fabrice; Del Fatti, Natalia

    2017-03-01

    Single-particle optical investigations have greatly improved our understanding of the fundamental properties of nano-objects, avoiding the spurious inhomogeneous effects that affect ensemble experiments. Correlation with high-resolution imaging techniques providing morphological information (e.g. electron microscopy) allows a quantitative interpretation of the optical measurements by means of analytical models and numerical simulations. In this topical review, we first briefly recall the principles underlying some of the most commonly used single-particle optical techniques: near-field, dark-field, spatial modulation and photothermal microscopies/spectroscopies. We then focus on the quantitative investigation of the surface plasmon resonance (SPR) of metallic nano-objects using linear and ultrafast optical techniques. While measured SPR positions and spectral areas are found in good agreement with predictions based on Maxwell’s equations, SPR widths are strongly influenced by quantum confinement (or, from a classical standpoint, surface-induced electron scattering) and, for small nano-objects, cannot be reproduced using the dielectric functions of bulk materials. Linear measurements on single nano-objects (silver nanospheres and gold nanorods) allow a quantification of the size and geometry dependences of these effects in confined metals. Addressing the ultrafast response of an individual nano-object is also a powerful tool to elucidate the physical mechanisms at the origin of their optical nonlinearities, and their electronic, vibrational and thermal relaxation processes. Experimental investigations of the dynamical response of gold nanorods are shown to be quantitatively modeled in terms of modifications of the metal dielectric function enhanced by plasmonic effects. Ultrafast spectroscopy can also be exploited to unveil hidden physical properties of more complex nanosystems. In this context, two-color femtosecond pump–probe experiments performed on

  9. 4D micro-CT using fast prospective gating

    Science.gov (United States)

    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

  10. Seeing the unseen-bioturbation in 4D

    DEFF Research Database (Denmark)

    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...

  11. Actively triggered 4d cone-beam CT acquisition

    Energy Technology Data Exchange (ETDEWEB)

    Fast, Martin F.; Wisotzky, Eric [German Cancer Research Center (DKFZ), Im Neuenheimer Feld 280, D-69120 Heidelberg (Germany); Oelfke, Uwe; Nill, Simeon [Joint Department of Physics, The Institute of Cancer Research and The Royal Marsden NHS Foundation Trust, Downs Road, Sutton, Surrey SM2 5PT (United Kingdom)

    2013-09-15

    Purpose: 4d cone-beam computed tomography (CBCT) scans are usually reconstructed by extracting the motion information from the 2d projections or an external surrogate signal, and binning the individual projections into multiple respiratory phases. In this “after-the-fact” binning approach, however, projections are unevenly distributed over respiratory phases resulting in inefficient utilization of imaging dose. To avoid excess dose in certain respiratory phases, and poor image quality due to a lack of projections in others, the authors have developed a novel 4d CBCT acquisition framework which actively triggers 2d projections based on the forward-predicted position of the tumor.Methods: The forward-prediction of the tumor position was independently established using either (i) an electromagnetic (EM) tracking system based on implanted EM-transponders which act as a surrogate for the tumor position, or (ii) an external motion sensor measuring the chest-wall displacement and correlating this external motion to the phase-shifted diaphragm motion derived from the acquired images. In order to avoid EM-induced artifacts in the imaging detector, the authors devised a simple but effective “Faraday” shielding cage. The authors demonstrated the feasibility of their acquisition strategy by scanning an anthropomorphic lung phantom moving on 1d or 2d sinusoidal trajectories.Results: With both tumor position devices, the authors were able to acquire 4d CBCTs free of motion blurring. For scans based on the EM tracking system, reconstruction artifacts stemming from the presence of the EM-array and the EM-transponders were greatly reduced using newly developed correction algorithms. By tuning the imaging frequency independently for each respiratory phase prior to acquisition, it was possible to harmonize the number of projections over respiratory phases. Depending on the breathing period (3.5 or 5 s) and the gantry rotation time (4 or 5 min), between ∼90 and 145

  12. 4D Flow MRI in Neuroradiology: Techniques and Applications.

    Science.gov (United States)

    Pereira, Vitor Mendes; Delattre, Benedicte; Brina, Olivier; Bouillot, Pierre; Vargas, Maria Isabel

    2016-04-01

    Assessment of the intracranial flow is important for the understanding and management of cerebral vascular diseases. From brain aneurysms and arteriovenous malformations lesions to intracranial and cervical stenosis, the appraisal of the blood flow can be crucial and influence positively on patients' management. The determination of the intracranial hemodynamics and the collateral pattern seems to play to a major role in the management of these lesions. 4D flow magnetic resonance imaging is a noninvasive phase contrast derived method that has been developed and applied in neurovascular diseases. It has a great potential if followed by further technical improvements and comprehensive and systematic clinical studies.

  13. Realistic CT simulation using the 4D XCAT phantom.

    Science.gov (United States)

    Segars, W P; Mahesh, M; Beck, T J; Frey, E C; Tsui, B M W

    2008-08-01

    The authors develop a unique CT simulation tool based on the 4D extended cardiac-torso (XCAT) phantom, a whole-body computer model of the human anatomy and physiology based on NURBS surfaces. Unlike current phantoms in CT based on simple mathematical primitives, the 4D XCAT provides an accurate representation of the complex human anatomy and has the advantage, due to its design, that its organ shapes can be changed to realistically model anatomical variations and patient motion. A disadvantage to the NURBS basis of the XCAT, however, is that the mathematical complexity of the surfaces makes the calculation of line integrals through the phantom difficult. They have to be calculated using iterative procedures; therefore, the calculation of CT projections is much slower than for simpler mathematical phantoms. To overcome this limitation, the authors used efficient ray tracing techniques from computer graphics, to develop a fast analytic projection algorithm to accurately calculate CT projections directly from the surface definition of the XCAT phantom given parameters defining the CT scanner and geometry. Using this tool, realistic high-resolution 3D and 4D projection images can be simulated and reconstructed from the XCAT within a reasonable amount of time. In comparison with other simulators with geometrically defined organs, the XCAT-based algorithm was found to be only three times slower in generating a projection data set of the same anatomical structures using a single 3.2 GHz processor. To overcome this decrease in speed would, therefore, only require running the projection algorithm in parallel over three processors. With the ever decreasing cost of computers and the rise of faster processors and multi-processor systems and clusters, this slowdown is basically inconsequential, especially given the vast improvement the XCAT offers in terms of realism and the ability to generate 3D and 4D data from anatomically diverse patients. As such, the authors conclude

  14. 4D-QSAR: Perspectives in Drug Design

    Directory of Open Access Journals (Sweden)

    Carolina H. Andrade

    2010-05-01

    Full Text Available Drug design is a process driven by innovation and technological breakthroughs involving a combination of advanced experimental and computational methods. A broad variety of medicinal chemistry approaches can be used for the identification of hits, generation of leads, as well as to accelerate the optimization of leads into drug candidates. The quantitative structure–activity relationship (QSAR formalisms are among the most important strategies that can be applied for the successful design new molecules. This review provides a comprehensive review on the evolution and current status of 4D-QSAR, highlighting present challenges and new opportunities in drug design.

  15. Gender matters: Female perspectives in ICT4D research

    CSIR Research Space (South Africa)

    Light, A

    2010-12-01

    Full Text Available phrases for greetings, introductions and providing training feedback (e.g. ?Very good!?). In many cases, she played the role of a comically lost in translation foreigner, encouraging participants to correct her in order to foster interaction. Slightly... on differences between men and women in the roles and opportunities which affect technology usage [19]. A number of ICT4D solutions focus on women?s empowerment or welfare as First Days [6] and microfinance beneficiaries [17], while Human Computer Interaction...

  16. Medicoscapes: on mobile ubiquity effects and ICT4D

    DEFF Research Database (Denmark)

    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 ...... perspective. It will ponder issues of collective imagination as exerted by way of such effects, i.e. in cultural forms that emerge out of media-roles in the ‘complex connectivity’ in globalisation processes....

  17. Inhibitory concentrations of 2,4D and its possible intermediates in sulfate reducing biofilms

    Energy Technology Data Exchange (ETDEWEB)

    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).

  18. Large lateral photovoltaic effect with ultrafast relaxation time in SnSe/Si junction

    Science.gov (United States)

    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.

  19. Pump-probe SAXS experiments on ultrafast demagnetization of magnetic multilayers

    Energy Technology Data Exchange (ETDEWEB)

    Pfau, B.; Schaffert, S.; Mohanty, J.; Geilhufe, J.; Flewett, S.; Eisebitt, S. [IOAP, Technische Universitaet Berlin (Germany); Buettner, F. [IOAP, Technische Universitaet Berlin (Germany); Paul Scherrer Institut, Villigen (Switzerland); Mueller, L.; Gutt, C.; Al-Shemmary, A.; Duesterer, S.; Redlin, H.; Gruebel, G. [HASYLAB, DESY, Hamburg (Germany); Vodungbo, B. [ENSTA ParisTech, Ecole Polytechnique, Palaiseau (France); Luening, J. [Universite Pierre et Marie Curie, Paris (France); Stickler, D.; Froemter, R.; Oepen, H.P. [Universitaet Hamburg (Germany); Schlotter, W.F. [LCLS, SLAC, Menlo Park (United States)

    2011-07-01

    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 {lambda}=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.

  20. Driving magnetic order in a manganite by ultrafast lattice excitation.

    Energy Technology Data Exchange (ETDEWEB)

    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.

  1. Cancer Incidence of 2,4-D Production Workers

    Directory of Open Access Journals (Sweden)

    Marcia Lee

    2011-09-01

    Full Text Available Despite showing no evidence of carcinogenicity in laboratory animals, the herbicide 2,4-dichlorophenoxyacetic acid (2,4-D has been associated with non-Hodgkin lymphoma (NHL in some human epidemiology studies, albeit inconsistently. We matched an existing cohort of 2,4-D manufacturing employees with cancer registries in three US states resulting in 244 cancers compared to 276 expected cases. The Standardized Incidence Ratio (SIR for the 14 NHL cases was 1.36 (95% Confidence Interval (CI 0.74–2.29. Risk estimates were higher in the upper cumulative exposure and duration subgroups, yet not statistically significant. There were no clear patterns of NHL risk with period of hire and histology subtypes. Statistically significant results were observed for prostate cancer (SIR = 0.74, 95% CI 0.57–0.94, and “other respiratory” cancers (SIR = 3.79, 95% CI 1.22–8.84; 4 of 5 cases were mesotheliomas. Overall, we observed fewer cancer cases than expected, and a non statistically significant increase in the number of NHL cases.

  2. 488-4D ASH LANDFILL CLOSURE CAP HELP MODELING

    Energy Technology Data Exchange (ETDEWEB)

    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.

  3. Exploration of 4D MRI blood flow using stylistic visualization.

    Science.gov (United States)

    van Pelt, Roy; Oliván Bescós, Javier; Breeuwer, Marcel; Clough, Rachel E; Gröller, M Eduard; ter Haar Romenij, Bart; Vilanova, Anna

    2010-01-01

    Insight into the dynamics of blood-flow considerably improves the understanding of the complex cardiovascular system and its pathologies. Advances in MRI technology enable acquisition of 4D blood-flow data, providing quantitative blood-flow velocities over time. The currently typical slice-by-slice analysis requires a full mental reconstruction of the unsteady blood-flow field, which is a tedious and highly challenging task, even for skilled physicians. We endeavor to alleviate this task by means of comprehensive visualization and interaction techniques. In this paper we present a framework for pre-clinical cardiovascular research, providing tools to both interactively explore the 4D blood-flow data and depict the essential blood-flow characteristics. The framework encompasses a variety of visualization styles, comprising illustrative techniques as well as improved methods from the established field of flow visualization. Each of the incorporated styles, including exploded planar reformats, flow-direction highlights, and arrow-trails, locally captures the blood-flow dynamics and may be initiated by an interactively probed vessel cross-section. Additionally, we present the results of an evaluation with domain experts, measuring the value of each of the visualization styles and related rendering parameters.

  4. 4D experience on Girassol Field block 17, Angola

    Energy Technology Data Exchange (ETDEWEB)

    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)

  5. 4-D XRD for strain in many grains using triangulation

    Energy Technology Data Exchange (ETDEWEB)

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

    2006-12-31

    Determination of the strains in a polycrystalline materialusing 4-D XRD reveals sub-grain and grain-to-grain behavior as a functionof stress. Here 4-D XRD involves an experimental procedure usingpolychromatic micro-beam X-radiation (micro-Laue) to characterizepolycrystalline materials in spatial location as well as with increasingstress. The in-situ tensile loading experiment measured strain in a modelaluminum-sapphire metal matrix composite using the Advanced Light Source,Beam-line 7.3.3. Micro-Laue resolves individual grains in thepolycrystalline matrix. Results obtained from a list of grains sorted bycrystallographic orientation depict the strain states within and amongindividual grains. Locating the grain positions in the planeperpendicular to the incident beam is trivial. However, determining theexact location of grains within a 3-D space is challenging. Determiningthe depth of the grains within the matrix (along the beam direction)involved a triangulation method tracing individual rays that producespots on the CCD back to the point of origin. Triangulation wasexperimentally implemented by simulating a 3-D detector capturingmultiple diffraction images while increasing the camera to sampledistance. Hence by observing the intersection of rays from multiple spotsbelonging to the corresponding grain, depth is calculated. Depthresolution is a function of the number of images collected, grain to beamsize ratio, and the pixel resolution of the CCD. The 4DXRD methodprovides grain morphologies, strain behavior of each grain, andinteractions of the matrix grains with each other and the centrallylocated single crystal fiber.

  6. Positive Energy Conditions in 4D Conformal Field Theory

    CERN Document Server

    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...

  7. Positive energy conditions in 4D conformal field theory

    Science.gov (United States)

    Farnsworth, Kara; Luty, Markus A.; Prilepina, Valentina

    2016-10-01

    We argue that all consistent 4D quantum field theories obey a spacetime-averaged weak energy inequality ≥ - 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. 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.

  8. Quantum Hooke's law to classify pulse laser induced ultrafast melting.

    Science.gov (United States)

    Hu, Hao; Ding, Hepeng; Liu, Feng

    2015-02-03

    Ultrafast crystal-to-liquid phase transition induced by femtosecond pulse laser excitation is an interesting material's behavior manifesting the complexity of light-matter interaction. There exist two types of such phase transitions: one occurs at a time scale shorter than a picosecond via a nonthermal process mediated by electron-hole plasma formation; the other at a longer time scale via a thermal melting process mediated by electron-phonon interaction. However, it remains unclear what material would undergo which process and why? Here, by exploiting the property of quantum electronic stress (QES) governed by quantum Hooke's law, we classify the transitions by two distinct classes of materials: the faster nonthermal process can only occur in materials like ice having an anomalous phase diagram characterized with dTm/dP melting temperature and P is pressure, above a high threshold laser fluence; while the slower thermal process may occur in all materials. Especially, the nonthermal transition is shown to be induced by the QES, acting like a negative internal pressure, which drives the crystal into a "super pressing" state to spontaneously transform into a higher-density liquid phase. Our findings significantly advance fundamental understanding of ultrafast crystal-to-liquid phase transitions, enabling quantitative a priori predictions.

  9. Technology and applications of ultrafast fiber lasers

    Science.gov (United States)

    Lang, Marion; Hellerer, Thomas; Stuhler, Juergen

    2012-03-01

    We briefly review the key technology of modern fiber based femtosecond laser sources summarizing advantages and disadvantages of different mode-locking solutions. A description of possible extensions of a FemtoFiber-type modelocked Er-doped fiber laser oscillator (1560 nm) reveals the flexibility with respect to wavelength coverage (488 nm .. 2200 nm) and pulse duration (10 fs .. 10 ps). The resulting FemtoFiber family and its versions for instrument integration allow one to use these state-of-the-art light sources in many important applications, e.g. THz spectroscopy and microscopy. We show that, depending on the fiber laser model and the THz emitter, THz radiation can be produced with 4-10 THz bandwidth and detected with up to 60 dB signal-to-noise ratio (SNR). Electronically controlled optical scanning (ECOPS) - a unique method for fast, precise and comfortable sampling of the THz pulse or other pump-probe experiments - is described and recommended for efficient data acquisition. As examples for modern microscopy with ultrafast fiber lasers we present results of two-photon fluorescence, coherent microscopy techniques (SHG/THG/CARS) and fluorescence lifetime imaging (FLIM).

  10. Cavity-Enhanced Ultrafast Spectroscopy: Ultrafast Meets Ultrasensitive

    Science.gov (United States)

    Allison, Thomas K.; Reber, Melanie Roberts; Chen, Yuning

    2016-06-01

    Ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D-spectroscopy, are widely used across many disciplines. However, these techniques are typically restricted to optically thick samples, such as solids and liquid solutions. Using a frequency comb laser and optical cavities, we present a new technique for performing ultrafast optical spectroscopy with high sensitivity, enabling work in dilute gas-phase molecular beams. Resonantly enhancing the probe pulses, we demonstrate transient absorption measurements with a detection limit of ΔOD = 2 × 10-10 (1 × 10-9/√{Hz}). Resonantly enhancing the pump pulses allows us to produce a high excitation fraction at high repetition-rate, so that signals can be recorded from samples with optical densities as low as OD ≈ 10-8, or column densities oise performance of CE-TAS. (a), Transient absorption measurements taken with reduced gas flow and perpendicular polarizations. The red dots represent the average of 60 consecutive scans taken over a 1 hour period. Black curves are every 10th scan from the data set. Inset: Zoom-in around 0.8 ps delay. Error bars represent the uncertainty in the mean. (b), The green squares show the average of the Allan deviations obtained independently for each delay point. Error bars here are the standard deviation (not the uncertainty in the mean) of this ensemble, to represent the spread in the data. The blue diamond is the average of the error bars of (a), along with their standard deviation. The grey line has a slope of -1/2 on the log-log plot, the expected slope for white noise performance

  11. SU-E-T-202: Comparison of 4D-Measurement-Guided Dose Reconstructions (MGDR) with COMPASS and OCTAVIUS 4D System

    Energy Technology Data Exchange (ETDEWEB)

    Leung, R; Wong, M; Lee, V; Law, G; Lee, K; Tung, S; Chan, M [Tuen Mun Hospital, Hong Kong, Hong Kong (China); Blanck, O [University Clinic Schleswig-Holstein, Kiel (Germany)

    2015-06-15

    Purpose: To cross-validate the MGDR of COMPASS (IBA dosimetry, GmbH, Germany) and OCTAVIUS 4D system (PTW, Freiburg, Germany). Methods: Volumetric-modulated arc plans (5 head-and-neck and 3 prostate) collapsed to 40° gantry on the OCTAVIUS 4D phantom in QA mode on Monaco v5.0 (Elekta, CMS, Maryland Heights, MO) were delivered on a Elekta Agility linac. This study was divided into two parts: (1) error-free measurements by gantry-mounted EvolutionXX 2D array were reconstructed in COMPASS (IBA dosimetry, GmbH, Germany), and by OCTAVIUS 1500 array in Versoft v6.1 (PTW, Freiburg, Germany) to obtain the 3D doses (COM4D and OCTA4D). COM4D and OCTA4D were compared to the raw measurement (OCTA3D) at the same detector plane for which OCTAVIUS 1500 was perpendicular to 0° gantry axis while the plans were delivered at gantry 40°; (2) beam steering errors of energy (Hump=-2%) and symmetry (2T=+2%) were introduced during the delivery of 5 plans to compare the MGDR doses COM4D-Hump (COM4D-2T), OCTA4D-Hump (OCTA4D-2T), with raw doses OCTA3D-Hump (OCTA3D-2T) and with OCTA3D to assess the error reconstruction and detection ability of MGDR tools. All comparisons used Υ-criteria of 2%(local dose)/2mm and 3%/3mm. Results: Averaged Υ passing rates were 85% and 96% for COM4D,and 94% and 99% for OCTA4D at 2%/2mm and 3%/3mm criteria respectively. For error reconstruction, COM4D-Hump (COM4D-2T) showed 81% (93%) at 2%/2mm and 94% (98%) at 3%/3mm, while OCTA4D-Hump (OCTA4D-2T) showed 96% (96%) at 2%/2mm and 99% (99%) at 3%/3mm. For error detection, OCTA3D doses were compared to COM4D-Hump (COM4D-2T) showing Υ passing rates of 93% (93%) at 2%/2mm and 98% (98%), and to OCTA4D-Hump (OCTA4D -2T) showing 94% (99%) at 2%/2mm and 81% (96%) at 3%/3mm, respectively. Conclusion: OCTAVIUS MGDR showed better agreement to raw measurements in both error- and error-free comparisons. COMPASS MGDR deviated from the raw measurements possibly owing to beam modeling uncertainty.

  12. Toward 4D Nanoprinting with Tip-Induced Organic Surface Reactions.

    Science.gov (United States)

    Carbonell, Carlos; Braunschweig, Adam B

    2017-02-21

    Future nanomanufacturing tools will prepare organic materials with complex four-dimensional (4D) structure, where the position (x, y, z) and chemical composition within a volume is controlled with sub-1 μm spatial resolution. Such tools could produce substrates that mimic biological interfaces, like the cell surface or the extracellular matrix, whose topology and chemical complexity combine to direct some of the most sophisticated biological events. The control of organic materials at the nanoscale-level of spatial resolution could revolutionize the assembly of next generation optical and electronic devices or substrates for tissue engineering or enable fundamental biological or material science investigations. Organic chemistry provides the requisite control over the orientation and position of matter within a nanoscale reference frame through the formation of new covalent bonds. Several challenges however preclude the integration of organic chemistry with conventional nanomanufacturing approaches, namely most nanolithography platforms would denature or destroy delicate organic and biologically active matter, confirming covalent bond formation at interfaces remains difficult, and finally, only a small handful of the reactions used to transform molecules in solution have been validated on surfaces. Thus, entirely new approaches, where organic transformations and spatial control are considered equally important contributors, are needed to create 4D organic nanoprinting platforms. This Account describes efforts from our group to reconcile nanolithography, and specifically massively parallel scanning probe lithography (SPL), with organic chemistry to further the goal of 4D organic nanoprinting. Massively parallel SPL involves arrays of elastomeric pyramids mounted onto piezoelectric actuators, and creates patterns with feature diameters below 50 nm by using the pyramidal tips for either the direct deposition of ink or the localized delivery of energy to a surface

  13. 4D XCAT phantom for multimodality imaging research

    Energy Technology Data Exchange (ETDEWEB)

    Segars, W. P.; Sturgeon, G.; Mendonca, S.; Grimes, Jason; Tsui, B. M. W. [Department of Radiology, Carl E. Ravin Advanced Imaging Laboratories, Duke University Medical Center, 2424 Erwin Road, Hock Plaza, Suite 302, Durham, North Carolina 27705 (United States); Department of Radiology, Carl E. Ravin Advanced Imaging Laboratories, Duke University Medical Center, 2424 Erwin Road, Hock Plaza, Suite 302, Durham, North Carolina 27705 and Department of Biomedical Engineering, University of North Carolina, Chapel Hill, North Carolina 27599 (United States); Department of Radiology, Carl E. Ravin Advanced Imaging Laboratories, Duke University Medical Center, 2424 Erwin Road, Hock Plaza, Suite 302, Durham, North Carolina 27705 (United States); The Russell H. Morgan Department of Radiology and Radiological Science, Johns Hopkins Medical Institutions, Baltimore, Maryland 21287 (United States)

    2010-09-15

    Purpose: The authors develop the 4D extended cardiac-torso (XCAT) phantom for multimodality imaging research. Methods: Highly detailed whole-body anatomies for the adult male and female were defined in the XCAT using nonuniform rational B-spline (NURBS) and subdivision surfaces based on segmentation of the Visible Male and Female anatomical datasets from the National Library of Medicine as well as patient datasets. Using the flexibility of these surfaces, the Visible Human anatomies were transformed to match body measurements and organ volumes for a 50th percentile (height and weight) male and female. The desired body measurements for the models were obtained using the PEOPLESIZE program that contains anthropometric dimensions categorized from 1st to the 99th percentile for US adults. The desired organ volumes were determined from ICRP Publication 89 [ICRP, ''Basic anatomical and physiological data for use in radiological protection: reference values,'' ICRP Publication 89 (International Commission on Radiological Protection, New York, NY, 2002)]. The male and female anatomies serve as standard templates upon which anatomical variations may be modeled in the XCAT through user-defined parameters. Parametrized models for the cardiac and respiratory motions were also incorporated into the XCAT based on high-resolution cardiac- and respiratory-gated multislice CT data. To demonstrate the usefulness of the phantom, the authors show example simulation studies in PET, SPECT, and CT using publicly available simulation packages. Results: As demonstrated in the pilot studies, the 4D XCAT (which includes thousands of anatomical structures) can produce realistic imaging data when combined with accurate models of the imaging process. With the flexibility of the NURBS surface primitives, any number of different anatomies, cardiac or respiratory motions or patterns, and spatial resolutions can be simulated to perform imaging research. Conclusions: With the

  14. Ultrafast dynamics during the photoinduced phase transition in VO2

    Science.gov (United States)

    Wegkamp, Daniel; Stähler, Julia

    2015-12-01

    The phase transition of VO2 from a monoclinic insulator to a rutile metal, which occurs thermally at TC = 340 K, can also be driven by strong photoexcitation. The ultrafast dynamics during this photoinduced phase transition (PIPT) have attracted great scientific attention for decades, as this approach promises to answer the question of whether the insulator-to-metal (IMT) transition is caused by electronic or crystallographic processes through disentanglement of the different contributions in the time domain. We review our recent results achieved by femtosecond time-resolved photoelectron, optical, and coherent phonon spectroscopy and discuss them within the framework of a selection of latest, complementary studies of the ultrafast PIPT in VO2. We show that the population change of electrons and holes caused by photoexcitation launches a highly non-equilibrium plasma phase characterized by enhanced screening due to quasi-free carriers and followed by two branches of non-equilibrium dynamics: (i) an instantaneous (within the time resolution) collapse of the insulating gap that precedes charge carrier relaxation and significant ionic motion and (ii) an instantaneous lattice potential symmetry change that represents the onset of the crystallographic phase transition through ionic motion on longer timescales. We discuss the interconnection between these two non-thermal pathways with particular focus on the meaning of the critical fluence of the PIPT in different types of experiments. Based on this, we conclude that the PIPT threshold identified in optical experiments is most probably determined by the excitation density required to drive the lattice potential change rather than the IMT. These considerations suggest that the IMT can be driven by weaker excitation, predicting a transiently metallic, monoclinic state of VO2 that is not stabilized by the non-thermal structural transition and, thus, decays on ultrafast timescales.

  15. Analysis of phase space topologies for models of 4D betatronic motion in view of 4D beam splitting

    CERN Document Server

    Percival, Benjamin

    2015-01-01

    The novel technique of multiturn extraction is used to ll the Super Proton Synchrotron (SPS) at CERN with a high-intensity proton beam delivered by the Proton Synchrotron (PS). This technique involves manipulating nonlinear fields of sextupoles and octupoles in the PS to trap the beam into stable islands in the transverse phase space. By varying the tunes slowly and crossing a resonance condition it is possible to trap particles by means of stable structures. This generates a number of well-dened beamlets, which may be extracted over a number of turns proportional to the order of the resonance that is crossed and its stability. In this report, the theoretical background of how to construct the Normal Form of a 4D map incorporating a sextupolar and an octupolar eld contribution that act on a particle in our beam close to a 4th order difference resonance is detailed. A Hamiltonian will be analysed after transforming from a 4D to a 2D system using a canonical transformation, which allows us to visualise the isla...

  16. Imaging of aortic valve dynamics in 4D OCT

    Directory of Open Access Journals (Sweden)

    Schnabel Christian

    2015-09-01

    Full Text Available The mechanical components of the heart, especially the valves and leaflets, are enormous stressed during lifetime. Therefore, those structures undergo different pathophysiological tissue transformations which affect cardiac output and in consequence living comfort of affected patients. These changes may lead to calcific aortic valve stenosis (AVS, the major heart valve disease in humans. The knowledge about changes of the dynamic behaviour during the course of this disease and the possibility of early stage diagnosis is of particular interest and could lead to the development of new treatment strategies and drug based options of prevention or therapy. 4D optical coherence tomography (OCT in combination with high-speed video microscopy were applied to characterize dynamic behaviour of the murine aortic valve and to characterize dynamic properties during artificial stimulation. We present a promising tool to investigate the aortic valve dynamics in an ex vivo disease model with a high spatial and temporal resolution using a multimodal imaging setup.

  17. Medicoscapes: on mobile ubiquity effects and ICT4D

    DEFF Research Database (Denmark)

    Michelsen, Anders Ib

    2012-01-01

    on use of resources of the global civil society emerging in global ‘transformations’ related to migration, media and ‘the social work of the imagination’. Whereas much new media debate departs from the assumption of media ubiquity affecting our notions of reality, the article will attempt a different...... perspective. It will ponder issues of collective imagination as exerted by way of such effects, i.e. in cultural forms that emerge out of media-roles in the ‘complex connectivity’ in globalisation processes.......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...

  18. 4D fast tracking for experiments at high luminosity LHC

    Science.gov (United States)

    Neri, N.; Cardini, A.; Calabrese, R.; Fiorini, M.; Luppi, E.; Marconi, U.; Petruzzo, M.

    2016-11-01

    The full exploitation of the physics potential of the high luminosity LHC is a big challenge that requires new instrumentation and innovative solutions. We present here a conceptual design and simulation studies of a fast timing pixel detector with embedded real-time tracking capabilities. The system is conceived to operate at 40 MHz event rate and to reconstruct tracks in real-time, using precise space and time 4D information of the hit, for fast trigger decisions. This work is part of an R&D project aimed at building an innovative tracking detector with superior time (10 ps) and position (10 μm) resolutions to be used in very harsh radiation environments, for the ultimate flavour physics experiment at the high luminosity phase of the LHC.

  19. 4D GPR Experiments--Towards the Virtual Lysimeter

    Science.gov (United States)

    Grasmueck, M.; Viggiano, D. A.; Day-Lewis, F. D.; Drasdis, J. B.; Kruse, S. E.; Or, D.

    2006-05-01

    In-situ monitoring of infiltration, water flow and retention in the vadose zone currently rely primarily on invasive methods, which irreversibly disturb original soil structure and alter its hydrologic behavior in the vicinity of the measurement. For example, use of lysimeters requires extraction and repacking of soil samples, and time- domain reflectometry (TDR) requires insertion of probes into the soil profile. This study investigates the use of repeated high-density 3D ground penetrating radar surveys (also known as 4D GPR) as a non-invasive alternative for detailed visualization and quantification of water flow in the vadose zone. Evaluation of the 4D GPR method was based on a series of controlled point-source water injection experiments into undisturbed beach sand deposits at Crandon Park in Miami, Florida. The goal of the GPR surveys was to image the shape and evolution of a wet-bulb as it propagates from the injection points (~0.5 m) towards the water table at 2.2 m depth. The experimental design was guided by predictive modeling using Hydrus 2D and finite-difference GPR waveform codes. Input parameters for the modeling were derived from hydrologic and electromagnetic characterization of representative sand samples. Guided by modeling results, we injected 30 to 40 liters of tap water through plastic-cased boreholes with slotted bottom sections (0.1 m) located 0.4 to 0.6 m below the surface. During and after injection, an area of 25 m2 was surveyed every 20 minutes using 250 and 500 MHz antennas with a grid spacing of 0.05 x 0.025 m. A total of 20 3D GPR surveys were completed over 3 infiltration sites. To confirm wet-bulb shapes measured by GPR, we injected 2 liters of "brilliant blue" dye (~100 mg/l) along with a saline water tracer towards the end of one experiment. After completion of GPR scanning, a trench was excavated to examine the distribution of the saltwater and dye using TDR and visual inspection, respectively. Preliminary analysis of the 4D GPR

  20. When chaos meets hyperchaos: 4D Rössler model

    Energy Technology Data Exchange (ETDEWEB)

    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.

  1. (Delta a) curiosities in some 4d susy RG flows

    CERN Document Server

    Amariti, Antonio

    2012-01-01

    We explore some curiosities in 4d susy RG flows. One issue is that the compelling candidate a-function, from a-maximization with Lagrange multipliers, has a `strange branch," with reversed RG flow properties, monotonically increasing instead of decreasing. The branch flip to the strange branch occurs where a double-trace deformation Delta W=O ^2 passes through marginality, reminiscent of the condition for the chiral symmetry breaking, out of the conformal window transition in non-susy gauge theories. The second issue arises from Higgsing vevs for IR-free fields, which sometimes superficially violate the a-theorem. The resolution is that some vevs trigger marginal or irrelevant interactions, leading to Delta a=0 and decoupled dilaton on a subspace of the moduli space of vacua. This is contrary to classical intuition about Higgsing. This phenomenon often (but not always) correlates with negative R-charge for the Higgsing chiral operator.

  2. Euclidean 4d exact solitons in a Skyrme type model

    Energy Technology Data Exchange (ETDEWEB)

    Ferreira, L.A. [Instituto de Fisica de Sao Carlos, IFSC/USP, Universidade de Sao Paulo, Caixa Postal 369, CEP 13560-970 Sao Carlos, SP (Brazil) and Instituto de Fisica Teorica, IFT/UNESP, Universidade Estadula Paulista, Rua Pamplona 145, 01405-900 Sao Paulo, SP (Brazil)]. E-mail: laf@if.sc.usp.br

    2005-01-27

    We introduce a Skyrme type, four-dimensional Euclidean field theory made of a triplet of scalar fields n->, taking values on the sphere S{sup 2}, and an additional real scalar field {phi}, which is dynamical only on a three-dimensional surface embedded in R{sup 4}. Using a special ansatz we reduce the 4d non-linear equations of motion into linear ordinary differential equations, which lead to the construction of an infinite number of exact soliton solutions with vanishing Euclidean action. The theory possesses a mass scale which fixes the size of the solitons in way which differs from Derrick's scaling arguments. The model may be relevant to the study of the low energy limit of pure SU(2) Yang-Mills theory.

  3. Myocardial motion and function assessment using 4D images

    Science.gov (United States)

    Shi, Peng-Cheng; Robinson, Glynn P.; Duncan, James S.

    1994-09-01

    This paper describes efforts aimed at more objectively and accurately quantifying the local, regional and global function of the left ventricle (LV) of the heart from 4D image data. Using our shape-based image analysis methods, point-wise myocardial motion vector fields between successive image frames through the entire cardiac cycle will be computed. Quantitative LV motion, thickening, and strain measurements will then be established from the point correspondence maps. In the paper, we will also briefly describe an in vivo experimental model which uses implanted imaging-opaque markers to validate the results of our image analysis methods. Finally, initial experimental results using image sequences from two different modalities will be presented.

  4. Contextualised ICT4D: a Bottom-Up Approach

    DEFF Research Database (Denmark)

    Lund, Henrik Hautop; Sutinen, Erkki

    2010-01-01

    . In a certain way, this agenda can be understood as a topdown approach which transfers technology in a hierarchical way to actual users. Complementary to the traditional approach, a bottom-up approach starts by identifying communities that are ready to participate in a process to use technology to transform......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...... 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 shows...

  5. ULTRASSONOGRAFIA GESTACIONAL 3D/4D EM PEQUENOS ANIMAIS

    OpenAIRE

    2015-01-01

    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 may...

  6. QED Corrections to the 4p - 4d Transition Energies of Copperlike Heavy Ions

    Energy Technology Data Exchange (ETDEWEB)

    Chen, M H; Cheng, K T; Johnson, W R; Sapirstein, J

    2006-08-21

    Quantum electrodynamic (QED) corrections to 4p-4d transition energies of several copper-like ions with Z = 70-92 are calculated non-perturbatively in strong external fields to all orders in binding corrections. Dirac-Kohn-Sham potentials are used to account for screening and core-relaxation effects. For the 4p{sub 1/2}-4d{sub 3/2} transition in copperlike bismuth, thorium and uranium, results are in good agreement with empirical QED corrections deduced from differences between transition energies obtained from recent high-precision electron-beam ion-trap (EBIT) measurements and those calculated with the relativistic many-body perturbation theory (RMBPT). These comparisons provide sensitive tests of QED corrections for high angular momentum states in many-electron heavy ions and illustrate the importance of core-relaxation corrections. Comparisons are also made with other theories and with experiment on the 4s-4p transition energies of high-Z Cu-like ions as accuracy checks of the present RMBPT and QED calculations.

  7. Scattering vector mesons in D4-D8 holographic QCD

    Energy Technology Data Exchange (ETDEWEB)

    Boschi-Filho, Henrique; Braga, Nelson; Ballon Bayona, C.A.; Torres, Marcus A.C. [Universidade Federal do Rio de Janeiro (UFRJ), RJ (Brazil)

    2009-07-01

    Full text. Sakai and Sugimoto authored one of the most successful string top-down models in describing real QCD, the D4-D8 brane model of holographic QCD. This model succeeds in exhibiting chiral symmetry breaking and confinement.A drawback of this model is that all massive hadrons have their masses set by the Kaluza-Klein compactification scale and we would have to work at energy scales below 1 GeV in order to describe a four dimensional physics. Still, they were able to find pion form factors and pion in agreement with experiment at scale of 1 GeV and above. They also calculate pion quadratic square radius in check with experiment, from a formula that depends on the entire Kaluza-Klein tower of excited pion states. Their model also realizes vector meson dominance (VMD) in electromagnetic interaction as proposed by Sakurai in the sixties. 5D gauge fields from flavor symmetry provides a zoo of mesons (scalar, pseudo-scalar, vector and pseudo-vector) and instanton configurations of such fields are interpreted as baryon fields. Inspired by the results of pion form factors and pion quadratic radius predicted in close agreement with experiment, we further calculate vector and axial vector mesons {psi}(z) wave functions, form factors, we discuss about its Q{sup -2} power behavior at large virtuosity (Q{sup 2}), and we check necessary relations between coupling constants and masses (superconvergence) that grants such power behavior of form factors. We compare our results with what is found in bottom-up hard wall and soft wall models and discuss the problems of the D4-D8 model. (author)

  8. Parallel Wavefront Analysis for a 4D Interferometer

    Science.gov (United States)

    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.

  9. Ultrafast spectroscopy of quantum dots

    CERN Document Server

    Foo, E

    2001-01-01

    exchange-correlation interactions among the confined carriers inside the dots are suggested to be responsible. A density functional calculation for BGR of the ground state transition shows good agreement with our experimental results, especially in the high dot occupancy regime. Many-particle state scattering gives rise to large homogeneous spectral broadening of the PL peaks, from which an intradot relaxation time approx 300 fs is estimated. This observation supports the results obtained by direct excitation of carriers within the QDs. Femtosecond time-resolved photoluminescence measured by frequency up-conversion has been used to investigate carrier dynamics in InAs/GaAs self-assembled quantum dots (QDs). Our results reveal ultrafast carrier relaxation and sequential state filling. Carrier relaxation is proposed to occur by Auger-type processes, and the sequential state filling suggests that intradot relaxation is much faster than carrier capture from the InAs wetting layer. Measurements obtained by direct ...

  10. Steady-state benchmarks of DK4D: A time-dependent, axisymmetric drift-kinetic equation solver

    Energy Technology Data Exchange (ETDEWEB)

    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.

  11. Experimental and Ab Initio Ultrafast Carrier Dynamics in Plasmonic Nanoparticles

    Science.gov (United States)

    Brown, Ana M.; Sundararaman, Ravishankar; Narang, Prineha; Schwartzberg, Adam M.; Goddard, William A.; Atwater, Harry A.

    2017-02-01

    Ultrafast pump-probe measurements of plasmonic nanostructures probe the nonequilibrium 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 that 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 nonthermal excited carriers and longer-lived thermalizing carriers.

  12. Experimental and ab initio ultrafast carrier dynamics in plasmonic nanoparticles

    CERN Document Server

    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.

  13. Investigation on the effect of exposure time on scintillator afterglow for ultra-fast tomography acquisition

    Science.gov (United States)

    Zefreh, K. Z.; Welford, F. M.; Sijbers, Jan

    2016-12-01

    Thanks to the ultra-fast endstation of the TOMCAT beamline, it is possible to do a tomographic scan with a sub-second temporal resolution which allows following dynamic processes in 4D (3D space + time). This ultra- high-rate tomography acquisition, exploiting the distinctive peculiarities of synchrotron radiation, provides nondestructive investigation of many dynamic processes which were not possible in the past. For example a continuous tensile test has been conducted recently in-situ for the first time with a frequency of 20 tomograms per second (20 Hz acquisition frequency). In the ultra-fast endstation a scintillator is used to convert X-ray to visible photons that can be detected by the camera. However, this conversion is not ideal and the scintillator response decays exponentially with afterglow. Afterglow can cause resolution degradation and artifacts (such as ring and band) especially with high rotation speed. On the other hand, to achieve a higher scan speed, thicker scintillators are more common because they result in higher emission intensities that can compensate the short exposure time in fast scans. However, the resolution deteriorates as the scintillator's thickness increases and thicker scintillators show higher afterglow. Performing many ultra-fast scans at the TOMCAT beamline with different acquisition rate, we demonstrate how the exposure time effects on the projection data and reconstructed images. Using two different thicknesses of LAG scintillator we also investigate the afterglow artifacts for different acquisition rate and exposure time.

  14. Respiratory triggered 4D cone-beam computed tomography: A novel method to reduce imaging dose

    Science.gov (United States)

    Cooper, Benjamin J.; O’Brien, Ricky T.; Balik, Salim; Hugo, Geoffrey D.; Keall, Paul J.

    2013-01-01

    Purpose: A novel method called respiratory triggered 4D cone-beam computed tomography (RT 4D CBCT) is described whereby imaging dose can be reduced without degrading image quality. RT 4D CBCT utilizes a respiratory signal to trigger projections such that only a single projection is assigned to a given respiratory bin for each breathing cycle. In contrast, commercial 4D CBCT does not actively use the respiratory signal to minimize image dose. Methods: To compare RT 4D CBCT with conventional 4D CBCT, 3600 CBCT projections of a thorax phantom were gathered and reconstructed to generate a ground truth CBCT dataset. Simulation pairs of conventional 4D CBCT acquisitions and RT 4D CBCT acquisitions were developed assuming a sinusoidal respiratory signal which governs the selection of projections from the pool of 3600 original projections. The RT 4D CBCT acquisition triggers a single projection when the respiratory signal enters a desired acquisition bin; the conventional acquisition does not use a respiratory trigger and projections are acquired at a constant frequency. Acquisition parameters studied were breathing period, acquisition time, and imager frequency. The performance of RT 4D CBCT using phase based and displacement based sorting was also studied. Image quality was quantified by calculating difference images of the test dataset from the ground truth dataset. Imaging dose was calculated by counting projections. Results: Using phase based sorting RT 4D CBCT results in 47% less imaging dose on average compared to conventional 4D CBCT. Image quality differences were less than 4% at worst. Using displacement based sorting RT 4D CBCT results in 57% less imaging dose on average, than conventional 4D CBCT methods; however, image quality was 26% worse with RT 4D CBCT. Conclusions: Simulation studies have shown that RT 4D CBCT reduces imaging dose while maintaining comparable image quality for phase based 4D CBCT; image quality is degraded for displacement based RT 4D

  15. Multimaterial 4D Printing with Tailorable Shape Memory Polymers

    Science.gov (United States)

    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.

  16. 4D ANIMATION RECONSTRUCTION FROM MULTI-CAMERA COORDINATES TRANSFORMATION

    Directory of Open Access Journals (Sweden)

    J. P. Jhan

    2016-06-01

    Full Text Available Reservoir dredging issues are important to extend the life of reservoir. The most effective and cost reduction way is to construct a tunnel to desilt the bottom sediment. Conventional technique is to construct a cofferdam to separate the water, construct the intake of tunnel inside and remove the cofferdam afterwards. In Taiwan, the ZengWen reservoir dredging project will install an Elephant-trunk Steel Pipe (ETSP in the water to connect the desilting tunnel without building the cofferdam. Since the installation is critical to the whole project, a 1:20 model was built to simulate the installation steps in a towing tank, i.e. launching, dragging, water injection, and sinking. To increase the construction safety, photogrammetry technic is adopted to record images during the simulation, compute its transformation parameters for dynamic analysis and reconstruct the 4D animations. In this study, several Australis© coded targets are fixed on the surface of ETSP for auto-recognition and measurement. The cameras orientations are computed by space resection where the 3D coordinates of coded targets are measured. Two approaches for motion parameters computation are proposed, i.e. performing 3D conformal transformation from the coordinates of cameras and relative orientation computation by the orientation of single camera. Experimental results show the 3D conformal transformation can achieve sub-mm simulation results, and relative orientation computation shows the flexibility for dynamic motion analysis which is easier and more efficiency.

  17. MULTIVARIABLE ANALYSIS OF 2,4-D HERBICIDE PHOTOCATALYTIC DEGRADATION

    Directory of Open Access Journals (Sweden)

    ANDRÉS F. LÓPEZ-VÁSQUEZ

    2011-01-01

    Full Text Available 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 porcentaje de degradación de carbono orgánico total (COT después de cuatro horas de irradiación. Para el fotorreactor tubular, los cuatro factores tuvieron la misma significancia sobre la degradación, mientras que para el fotorreactor de placa plana inclinada, sólo la concentración de catalizador y el pH tuvieron significancia. La MSR fue una técnica adecuada para obtener parámetros de operación óptimos de un proceso fotocatalítico con un reactor específico y dentro de un rango de estudio determinado.

  18. Multimaterial 4D Printing with Tailorable Shape Memory Polymers.

    Science.gov (United States)

    Ge, Qi; Sakhaei, Amir Hosein; Lee, Howon; Dunn, Conner K; Fang, Nicholas X; Dunn, Martin L

    2016-08-08

    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. Cardy Formula for 4d SUSY Theories and Localization

    CERN Document Server

    Di Pietro, Lorenzo

    2016-01-01

    We study 4d $\\mathcal{N}=1$ supersymmetric theories on a compact Euclidean manifold of the form $S^1 \\times\\mathcal{M}_3$. Partition functions of gauge theories on this background can be computed using localization, and explicit formulas have been derived for different choices of the compact manifold $\\mathcal{M}_3$. Taking the limit of shrinking $S^1$, we present a general formula for the limit of the localization integrand, derived by simple effective theory considerations, generalizing the result of arXiv:1512.03376. The limit is given in terms of an effective potential for the holonomies around the $S^1$, whose minima determine the asymptotic behavior of the partition function. If the potential is minimized in the origin, where it vanishes, the partition function has a Cardy-like behavior fixed by $\\mathrm{Tr}(R)$, while a nontrivial minimum gives a shift in the coefficient. In all the examples that we consider, the origin is a minimum iff $\\mathrm{Tr}(R) \\leq 0$.

  20. 4D Near-Field Source Localization Using Cumulant

    Directory of Open Access Journals (Sweden)

    Zhao Feng

    2007-01-01

    Full Text Available This paper proposes a new cumulant-based algorithm to jointly estimate four-dimensional (4D source parameters of multiple near-field narrowband sources. Firstly, this approach proposes a new cross-array, and constructs five high-dimensional Toeplitz matrices using the fourth-order cumulants of some properly chosen sensor outputs; secondly, it forms a parallel factor (PARAFAC model in the cumulant domain using these matrices, and analyzes the unique low-rank decomposition of this model; thirdly, it jointly estimates the frequency, two-dimensional (2D directions-of-arrival (DOAs, and range of each near-field source from the matrices via the low-rank three-way array (TWA decomposition. In comparison with some available methods, the proposed algorithm, which efficiently makes use of the array aperture, can localize sources using sensors. In addition, it requires neither pairing parameters nor multidimensional search. Simulation results are presented to validate the performance of the proposed method.

  1. 4D Near-Field Source Localization Using Cumulant

    Directory of Open Access Journals (Sweden)

    Junying Zhang

    2007-01-01

    Full Text Available This paper proposes a new cumulant-based algorithm to jointly estimate four-dimensional (4D source parameters of multiple near-field narrowband sources. Firstly, this approach proposes a new cross-array, and constructs five high-dimensional Toeplitz matrices using the fourth-order cumulants of some properly chosen sensor outputs; secondly, it forms a parallel factor (PARAFAC model in the cumulant domain using these matrices, and analyzes the unique low-rank decomposition of this model; thirdly, it jointly estimates the frequency, two-dimensional (2D directions-of-arrival (DOAs, and range of each near-field source from the matrices via the low-rank three-way array (TWA decomposition. In comparison with some available methods, the proposed algorithm, which efficiently makes use of the array aperture, can localize N−3 sources using N sensors. In addition, it requires neither pairing parameters nor multidimensional search. Simulation results are presented to validate the performance of the proposed method.

  2. A dynamic 4D probabilistic atlas of the developing brain.

    Science.gov (United States)

    Kuklisova-Murgasova, Maria; Aljabar, Paul; Srinivasan, Latha; Counsell, Serena J; Doria, Valentina; Serag, Ahmed; Gousias, Ioannis S; Boardman, James P; Rutherford, Mary A; Edwards, A David; Hajnal, Joseph V; Rueckert, Daniel

    2011-02-14

    Probabilistic atlases are widely used in the neuroscience community as a tool for providing a standard space for comparison of subjects and as tissue priors used to enhance the intensity-based classification of brain MRI. Most efforts so far have focused on static brain atlases either for adult or pediatric cohorts. In contrast to the adult brain the rapid growth of the neonatal brain requires an age-specific spatial probabilistic atlas to provide suitable anatomical and structural information. In this paper we describe a 4D probabilistic atlas that allows dynamic generation of prior tissue probability maps for any chosen stage of neonatal brain development between 29 and 44 gestational weeks. The atlas is created from the segmentations of 142 neonatal subjects at different ages using a kernel-based regression method and provides prior tissue probability maps for six structures - cortex, white matter, subcortical grey matter, brainstem, cerebellum and cerebro-spinal fluid. The atlas is publicly available at www.brain-development.org.

  3. Bounds in 4D conformal field theories with global symmetry

    Energy Technology Data Exchange (ETDEWEB)

    Rattazzi, Riccardo; Vichi, Alessandro [Institut de Theorie des Phenomenes Physiques, EPFL, CH-1015 Lausanne (Switzerland); Rychkov, Slava [Laboratoire de Physique Theorique, Ecole Normale Superieure, and Faculte de Physique, Universite Pierre et Marie Curie (France)

    2011-01-21

    We explore the constraining power of OPE associativity in 4D conformal field theory with a continuous global symmetry group. We give a general analysis of crossing symmetry constraints in the 4-point function ({phi}{phi}{phi}{dagger}{phi}{dagger}), where {phi} is a primary scalar operator in a given representation R. These constraints take the form of 'vectorial sum rules' for conformal blocks of operators whose representations appear in RxR and Rx R-bar . The coefficients in these sum rules are related to the Fierz transformation matrices for the RxRx R-bar x R-bar invariant tensors. We show that the number of equations is always equal to the number of symmetry channels to be constrained. We also analyze in detail two cases-the fundamental of SO(N) and the fundamental of SU(N). We derive the vectorial sum rules explicitly, and use them to study the dimension of the lowest singlet scalar in the {phi} x {phi}{dagger} OPE. We prove the existence of an upper bound on the dimension of this scalar. The bound depends on the conformal dimension of {phi} and approaches 2 in the limit dim({Phi}){yields}1. For several small groups, we compute the behavior of the bound at dim({Phi})>1. We discuss implications of our bound for the conformal technicolor scenario of electroweak symmetry breaking.

  4. Unlocking the Constraints of Cyanobacterial Productivity: Acclimations Enabling Ultrafast Growth

    Energy Technology Data Exchange (ETDEWEB)

    Bernstein, Hans C.; McClure, Ryan S.; Hill, Eric A.; Markillie, Lye Meng; Chrisler, William B.; Romine, Margie F.; McDermott, Jason E.; Posewitz, Matthew C.; Bryant, Donald A.; Konopka, Allan E.; Fredrickson, James K.; Beliaev, Alexander S.

    2016-07-26

    ABSTRACT

    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 cyanobacteriumSynechococcussp. strain PCC 7002 (Synechococcus7002) and identify key mechanisms that allow cyanobacteria to achieve unprecedented photoautotrophic productivities (~2.5-h doubling time). Ultrafast growth ofSynechococcus7002 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 inSynechococcus7002 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.

    IMPORTANCEEfficient coupling between photosynthesis and productivity is central to the development of biotechnology based on solar energy. Therefore, understanding the factors constraining maximum rates of carbon processing is necessary to identify regulatory mechanisms and devise strategies to overcome productivity constraints. Here, we interrogate the molecular mechanisms that operate at a systems level to allow cyanobacteria to achieve ultrafast growth. This was done by considering growth and photosynthetic kinetics with global transcription patterns. We have delineated

  5. Observation of ultrafast charge migration in an amino acid

    Science.gov (United States)

    Calegari, Francesca

    2014-05-01

    Electron transfer within a single molecule is the fundamental step of many biological processes and chemical reactions. It plays a crucial role in catalysis, DNA damage, photosynthesis and photovoltaics. The investigation of this process has been the subject of considerable research effort. Electron transfer driven by solely electronic correlations is well known as ``charge migration'' and it occurs in a few femtoseconds. In this work we present the first observation of ultrafast charge migration in the amino acid phenylalanine using XUV attosecond pulses. Neutral molecules were produced in gas phase by heating a thin metallic foil with a CW laser. Phenylalanine molecules were irradiated by a 250-as pump pulse with photon energy in the range 16-35 eV, followed by a 4-fs VIS/NIR probe pulse. The produced parent and fragment ions were then extracted into a linear TOF device for mass analysis. The main contributions in the mass spectrum correspond to the parent ion M + (165 Da), the immonium ion (M-COOH = 120), the backbone of the amino acid (M-R = 74) and the phenyl groups (R = 91, R + H = 92). A small peak at 60 can be assigned to the doubly charged immonium ion. Pump-probe measurements evidenced an exponential decay of the yield of fragment 60 with a time constant of 30 fs. This ultrashort time constant suggests that the dication dynamics is initiated by ionization of an inner-valence electron. By increasing the temporal resolution of the measurement we were able to observe a clear modulation of the yield with a periodicity of a few femtoseconds. This ultrafast dynamics can only be associated with purely electronic processes, thus constituting a clear experimental evidence of charge migration in biomolecules.

  6. Ultrafast laser spectroscopy in complex solid state materials

    Energy Technology Data Exchange (ETDEWEB)

    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.

  7. Ultrafast carrier dynamics in type II ZnSe/CdS/ZnSe nanobarbells.

    Science.gov (United States)

    Hewa-Kasakarage, Nishshanka N; El-Khoury, Patrick Z; Tarnovsky, Alexander N; Kirsanova, Maria; Nemitz, Ian; Nemchinov, Alexander; Zamkov, Mikhail

    2010-04-27

    We employ femtosecond transient absorption spectroscopy to get an insight into ultrafast processes occurring at the interface of type II ZnSe/CdS heterostructured nanocrystals fabricated via colloidal routes and comprising a barbell-like arrangement of ZnSe tips and CdS nanorods. Our study shows that resonant excitation of ZnSe tips results in an unprecedently fast transfer of excited electrons into CdS domains of nanobarbells (ZnSe tips (tau(h)= 95 ps). A qualitative thermodynamic description of observed electron processes within the classical limit of Marcus theory was used to identify a specific charge transfer regime associated with the ultrafast electron injection into CdS. Potential photocatalytic applications of the observed fast separation of carriers along the main axis of ZnSe/CdS barbells are discussed.

  8. The essential role of hypusine in eukaryotic translation initiation factor 4D (eIF-4D). Purification of eIF-4D and its precursors and comparison of their activities.

    Science.gov (United States)

    Park, M H

    1989-11-05

    Eukaryotic translation initiation factor 4D (eIF-4D) is the only protein known to contain the amino acid, hypusine [N epsilon-(4-amino-2-hydroxybutyl)lysine]. This unusual amino acid is formed post-translationally by modification of a single specific lysine residue in an eIF-4D precursor protein. Two separate eIF-4D precursors, each of which contains a lysine residue in place of the hypusine residue and each of which thereby serves as a protein substrate for the hypusine modification, were purified from DL-2-difluoromethylornithine-treated Chinese hamster ovary cells by means of a five-step procedure. These two precursors termed PI and PII both have apparent molecular masses of approximately 17 kDa, indistinguishable from that of eIF-4D, but exhibit more acidic isoelectric points (5.1 and 5.25 for PI and PII, respectively, compared with 5.37 for eIF-4D). These physical characteristics, together with other properties, indicate that eIF-4D differs from PII only in possessing the hypusine residue in place of a lysine residue, whereas an additional structural difference exists between PI and eIF-4D. eIF-4D from CHO cells provides a significant enhancement of methionyl-puromycin synthesis, a model assay for translation initiation. Neither PI nor PII stimulates this in vitro system. These findings are the first direct evidence that hypusine is essential for the biological activity of eIF-4D.

  9. Biofilm vs. Planktonic Lifestyle: Consequences for Pesticide 2,4-D Metabolism by Cupriavidus necator JMP134

    Science.gov (United States)

    Lerch, Thomas Z.; Chenu, Claire; Dignac, Marie F.; Barriuso, Enrique; Mariotti, André

    2017-01-01

    The development of bacterial biofilms in natural environments may alter important functions, such as pollutant bioremediation by modifying both the degraders' physiology and/or interactions within the matrix. The present study focuses on the influence of biofilm formation on the metabolism of a pesticide, 2,4-dichlorophenoxyacetic acid (2,4-D), by Cupriavidus necator JMP134. Pure cultures were established in a liquid medium with 2,4-D as a sole carbon source with or without sand grains for 10 days. Bacterial numbers and 2,4-D concentrations in solution were followed by spectrophotometry, the respiration rate by gas chromatography and the surface colonization by electron microscopy. In addition, isotopic techniques coupled with Fatty Acid Methyl Ester (FAME) profiling were used to determine possible metabolic changes. After only 3 days, approximately 80% of the cells were attached to the sand grains and microscopy images showed that the porous medium was totally clogged by the development of a biofilm. After 10 days, there was 25% less 2,4-D in the solution in samples with sand than in control samples. This difference was due to (1) a higher (+8%) mineralization of 2,4-D by sessile bacteria and (2) a retention (15%) of 2,4-D in the biofilm matrix. Besides, the amount of carbohydrates, presumably constituting the biofilm polysaccharides, increased by 63%. Compound-specific isotope analysis revealed that the FAME isotopic signature was less affected by the biofilm lifestyle than was the FAME composition. These results suggest that sessile bacteria differ more in their anabolism than in their catabolism compared to their planktonic counterparts. This study stresses the importance of considering interactions between microorganisms and their habitat when studying pollutant dynamics in porous media. PMID:28588567

  10. Biofilm vs. Planktonic Lifestyle: Consequences for Pesticide 2,4-D Metabolism by Cupriavidus necator JMP134.

    Science.gov (United States)

    Lerch, Thomas Z; Chenu, Claire; Dignac, Marie F; Barriuso, Enrique; Mariotti, André

    2017-01-01

    The development of bacterial biofilms in natural environments may alter important functions, such as pollutant bioremediation by modifying both the degraders' physiology and/or interactions within the matrix. The present study focuses on the influence of biofilm formation on the metabolism of a pesticide, 2,4-dichlorophenoxyacetic acid (2,4-D), by Cupriavidus necator JMP134. Pure cultures were established in a liquid medium with 2,4-D as a sole carbon source with or without sand grains for 10 days. Bacterial numbers and 2,4-D concentrations in solution were followed by spectrophotometry, the respiration rate by gas chromatography and the surface colonization by electron microscopy. In addition, isotopic techniques coupled with Fatty Acid Methyl Ester (FAME) profiling were used to determine possible metabolic changes. After only 3 days, approximately 80% of the cells were attached to the sand grains and microscopy images showed that the porous medium was totally clogged by the development of a biofilm. After 10 days, there was 25% less 2,4-D in the solution in samples with sand than in control samples. This difference was due to (1) a higher (+8%) mineralization of 2,4-D by sessile bacteria and (2) a retention (15%) of 2,4-D in the biofilm matrix. Besides, the amount of carbohydrates, presumably constituting the biofilm polysaccharides, increased by 63%. Compound-specific isotope analysis revealed that the FAME isotopic signature was less affected by the biofilm lifestyle than was the FAME composition. These results suggest that sessile bacteria differ more in their anabolism than in their catabolism compared to their planktonic counterparts. This study stresses the importance of considering interactions between microorganisms and their habitat when studying pollutant dynamics in porous media.

  11. Biofilm vs. Planktonic Lifestyle: Consequences for Pesticide 2,4-D Metabolism by Cupriavidus necator JMP134

    Directory of Open Access Journals (Sweden)

    Thomas Z. Lerch

    2017-05-01

    Full Text Available The development of bacterial biofilms in natural environments may alter important functions, such as pollutant bioremediation by modifying both the degraders' physiology and/or interactions within the matrix. The present study focuses on the influence of biofilm formation on the metabolism of a pesticide, 2,4-dichlorophenoxyacetic acid (2,4-D, by Cupriavidus necator JMP134. Pure cultures were established in a liquid medium with 2,4-D as a sole carbon source with or without sand grains for 10 days. Bacterial numbers and 2,4-D concentrations in solution were followed by spectrophotometry, the respiration rate by gas chromatography and the surface colonization by electron microscopy. In addition, isotopic techniques coupled with Fatty Acid Methyl Ester (FAME profiling were used to determine possible metabolic changes. After only 3 days, approximately 80% of the cells were attached to the sand grains and microscopy images showed that the porous medium was totally clogged by the development of a biofilm. After 10 days, there was 25% less 2,4-D in the solution in samples with sand than in control samples. This difference was due to (1 a higher (+8% mineralization of 2,4-D by sessile bacteria and (2 a retention (15% of 2,4-D in the biofilm matrix. Besides, the amount of carbohydrates, presumably constituting the biofilm polysaccharides, increased by 63%. Compound-specific isotope analysis revealed that the FAME isotopic signature was less affected by the biofilm lifestyle than was the FAME composition. These results suggest that sessile bacteria differ more in their anabolism than in their catabolism compared to their planktonic counterparts. This study stresses the importance of considering interactions between microorganisms and their habitat when studying pollutant dynamics in porous media.

  12. Staggered Multiple-PRF Ultrafast Color Doppler.

    Science.gov (United States)

    Posada, Daniel; Poree, Jonathan; Pellissier, Arnaud; Chayer, Boris; Tournoux, Francois; Cloutier, Guy; Garcia, Damien

    2016-06-01

    Color Doppler imaging is an established pulsed ultrasound technique to visualize blood flow non-invasively. High-frame-rate (ultrafast) color Doppler, by emissions of plane or circular wavefronts, allows severalfold increase in frame rates. Conventional and ultrafast color Doppler are both limited by the range-velocity dilemma, which may result in velocity folding (aliasing) for large depths and/or large velocities. We investigated multiple pulse-repetition-frequency (PRF) emissions arranged in a series of staggered intervals to remove aliasing in ultrafast color Doppler. Staggered PRF is an emission process where time delays between successive pulse transmissions change in an alternating way. We tested staggered dual- and triple-PRF ultrafast color Doppler, 1) in vitro in a spinning disc and a free jet flow, and 2) in vivo in a human left ventricle. The in vitro results showed that the Nyquist velocity could be extended to up to 6 times the conventional limit. We found coefficients of determination r(2) ≥ 0.98 between the de-aliased and ground-truth velocities. Consistent de-aliased Doppler images were also obtained in the human left heart. Our results demonstrate that staggered multiple-PRF ultrafast color Doppler is efficient for high-velocity high-frame-rate blood flow imaging. This is particularly relevant for new developments in ultrasound imaging relying on accurate velocity measurements.

  13. Digit ratio (2D:4D) and hand preference for writing in the BBC Internet Study.

    Science.gov (United States)

    Manning, J T; Peters, M

    2009-09-01

    The ratio of the length of the second to the fourth digit (2D:4D) may be negatively correlated with prenatal testosterone. Hand preference has been linked with prenatal testosterone and 2D:4D. Here we show that 2D:4D is associated with hand preference for writing in a large internet sample (n>170,000) in which participants self-reported their finger lengths. We replicated a significant association between right 2D:4D and writing hand preference (low right 2D:4D associated with left hand preference) as well as a significant correlation between writing hand preference and the difference between left and right 2D:4D or Dr-l (low Dr-l associated with left hand preference). A new significant correlation between left 2D:4D and writing hand preference was also shown (high left 2D:4D associated with left hand preference). There was a clear interaction between writing hand preference and 2D:4D: The left 2D:4D was significantly larger than the right 2D:4D in male and female left-handed writers, and the right hand 2D:4D was significantly larger than the left hand 2D:4D in male and female right-handed writers.

  14. 4D measurement system for automatic location of anatomical structures

    Science.gov (United States)

    Witkowski, Marcin; Sitnik, Robert; Kujawińska, Małgorzata; Rapp, Walter; Kowalski, Marcin; Haex, Bart; Mooshake, Sven

    2006-04-01

    Orthopedics and neurosciences are fields of medicine where the analysis of objective movement parameters is extremely important for clinical diagnosis. Moreover, as there are significant differences between static and dynamic parameters, there is a strong need of analyzing the anatomical structures under functional conditions. In clinical gait analysis the benefits of kinematical methods are undoubted. In this paper we present a 4D (3D + time) measurement system capable of automatic location of selected anatomical structures by locating and tracing the structures' position and orientation in time. The presented system is designed to help a general practitioner in diagnosing selected lower limbs' dysfunctions (e.g. knee injuries) and also determine if a patient should be directed for further examination (e.g. x-ray or MRI). The measurement system components are hardware and software. For the hardware part we adapt the laser triangulation method. In this way we can evaluate functional and dynamic movements in a contact-free, non-invasive way, without the use of potentially harmful radiation. Furthermore, opposite to marker-based video-tracking systems, no preparation time is required. The software part consists of a data acquisition module, an image processing and point clouds (point cloud, set of points described by coordinates (x, y, z)) calculation module, a preliminary processing module, a feature-searching module and an external biomechanical module. The paper briefly presents the modules mentioned above with the focus on the feature-searching module. Also we present some measurement and analysis results. These include: parameters maps, landmarks trajectories in time sequence and animation of a simplified model of lower limbs.

  15. Ultrafast disk lasers and amplifiers

    Science.gov (United States)

    Sutter, Dirk H.; Kleinbauer, Jochen; Bauer, Dominik; Wolf, Martin; Tan, Chuong; Gebs, Raphael; Budnicki, Aleksander; Wagenblast, Philipp; Weiler, Sascha

    2012-03-01

    Disk lasers with multi-kW continuous wave (CW) output power are widely used in manufacturing, primarily for cutting and welding applications, notably in the automotive industry. The ytterbium disk technology combines high power (average and/or peak power), excellent beam quality, high efficiency, and high reliability with low investment and operating costs. Fundamental mode picosecond disk lasers are well established in micro machining at high throughput and perfect precision. Following the world's first market introduction of industrial grade 50 W picosecond lasers (TruMicro 5050) at the Photonics West 2008, the second generation of the TruMicro series 5000 now provides twice the average power (100 W at 1030 nm, or 60 W frequency doubled, green output) at a significantly reduced footprint. Mode-locked disk oscillators achieve by far the highest average power of any unamplified lasers, significantly exceeding the 100 W level in laboratory set-ups. With robust long resonators their multi-microjoule pulse energies begin to compete with typical ultrafast amplifiers. In addition, significant interest in disk technology has recently come from the extreme light laser community, aiming for ultra-high peak powers of petawatts and beyond.

  16. Ultrafast palladium diffusion in germanium

    KAUST Repository

    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.

  17. Ultrafast dephasing of interband transitions in semiconductors

    Institute of Scientific and Technical Information of China (English)

    ZHANG; Haichao

    2001-01-01

    [1]Becker, P. C., Fragnito, H. L., Brito, C. C. H. et al., Femtosecond photon echoes from band-to-band transitions in GaAs, Phys. Rev. Lett., 1988, 61: 1647—1649.[2]Lin, W. Z., Schoenlein, R. W., Fujimoto, J. G. et al., Femtosecond absorption saturation of hot carriers in GaAs and AlGaAs, IEEE JQE, 1988, 24: 267—275.[3]Gurevich, V. L., Muradov, M. I., Parshin, D. A., On the theory of femtosecond photon echoes from band-to -band transitions in semiconductors, Europhys. Lett., 1990, 12(4): 375—379.[4]Sayed, K. E., Bányai, L., Haug, H., Coulomb quantum kinetics and optical dephasing on the femtosecond time scale, Phys. Rev. B, 1994, 50:1541—1550.[5]Arlt, S., Siegner, U., Kunde, J. et al., Ultrafast dephasing of continuum transitions in bulk semiconductors, Phys. Rev. B, 1999, 59: 14860—14863.[6]Hügel, W. A., Heinrich, M. F., Wegener, M. et al., Photon echoes from semiconductor band-to -band continuum transitions in the regime of Coulomb quantum kinetics, Phys. Rev. Lett., 1999, 83(16): 3313—3316.[7]Scott, D. C., Binder, R., Koch, S. W., Ultrafast dephasing through acoustic plasmon undamping in nonequilibrium electron-hole plasmas, Phys. Rev. Lett., 1992, 69(2): 347—350.[8]Binder, R., Scott, D., Paul, A. E. et al., Carrier-carrier scattering and optical dephasing in highly excited semiconductors, Phys. Rev., B 1991, 45: 1107—1114.[9]Schilp, J., Kuhn, T., Mahler, G., Electron-phonon quantum kinetics in pulse-excited semiconductors: Memory and renormalization effects, Phys. Rev. B, 1994, 50: 5435—5447.[10]Snoke, D. W., Density dependence of electron scattering at low density, Phys. Rev., B 1994, 50: 11583—11591.[11]Leitenstorfer, A., Lohner, A., Rick, K. et al., Excitonic and free-carrier polarizations of bulk GaAs studied by femtosecond coherent spectroscopy, Phys. Rev., 1994B 49: 16372—16380.[12]Zhang, H. C., Wen, J. H., Guo, B. Hole-hole scattering of photoexcited heavy-holes in GaAs, Acta Physica

  18. Degradation of 2,4-D herbicide by microorganisms isolated from Brazilian contaminated soil

    National Research Council Canada - National Science Library

    Silva, Tatiane M; Stets, Maria I; Mazzetto, André M; Andrade, Fabiana D; Pileggi, Sônia A. V; Fávero, Paulo R; Cantú, Marcelo D; Carrilho, Emanuel; Carneiro, Paulo I.B; Pileggi, Marcos

    2007-01-01

    The aim of this work was to isolate microorganisms from Brazilian soil contaminated with 2,4-D herbicide, and analyze the efficiency for 2,4D degradation, using high-performance liquid chromatography (HPLC...

  19. Progress in ultrafast intense laser science IX

    CERN Document Server

    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...

  20. Ultrafast structural dynamics of perovskite superlattices

    Energy Technology Data Exchange (ETDEWEB)

    Woerner, M.; Korff Schmising, C. von; Zhavoronkov, N.; Elsaesser, T. [Max-Born-Institut fuer Nichtlineare Optik und Kurzzeitspektroskopie, Berlin (Germany); Bargheer, M. [Universitaet Potsdam, Institut fuer Physik und Astronomie, Potsdam (Germany); Vrejoiu, I.; Hesse, D.; Alexe, M. [Max-Planck-Institut fuer Mikrostrukturphysik, Halle (Germany)

    2009-07-15

    Femtosecond X-ray diffraction provides direct insight into the ultrafast reversible lattice dynamics of materials with a perovskite structure. Superlattice (SL) structures consisting of a sequence of nanometer-thick layer pairs allow for optically inducing a tailored stress profile that drives the lattice motions and for limiting the influence of strain propagation on the observed dynamics. We demonstrate this concept in a series of diffraction experiments with femtosecond time resolution, giving detailed information on the ultrafast lattice dynamics of ferroelectric and ferromagnetic superlattices. Anharmonically coupled lattice motions in a SrRuO{sub 3}/PbZr{sub 0.2}Ti{sub 0.8}O{sub 3} (SRO/PZT) SL lead to a switch-off of the electric polarizations on a time scale of the order of 1 ps. Ultrafast magnetostriction of photoexcited SRO layers is demonstrated in a SRO/SrTiO{sub 3} (STO) SL. (orig.)

  1. Unlocking the Constraints of Cyanobacterial Productivity: Acclimations Enabling Ultrafast Growth

    Directory of Open Access Journals (Sweden)

    Hans C. Bernstein

    2016-07-01

    Full Text Available 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.

  2. Atomic origin of ultrafast resistance switching in nanoscale electrometallization cells.

    Science.gov (United States)

    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.

  3. Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

    Science.gov (United States)

    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

    2016-08-01

    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.

  4. Diffraction of quantum dots reveals nanoscale ultrafast energy localization.

    Science.gov (United States)

    Vanacore, Giovanni M; Hu, Jianbo; Liang, Wenxi; Bietti, Sergio; Sanguinetti, Stefano; Zewail, Ahmed H

    2014-11-12

    Unlike in bulk materials, energy transport in low-dimensional and nanoscale systems may be governed by a coherent "ballistic" behavior of lattice vibrations, the phonons. If dominant, such behavior would determine the mechanism for transport and relaxation in various energy-conversion applications. In order to study this coherent limit, both the spatial and temporal resolutions must be sufficient for the length-time scales involved. Here, we report observation of the lattice dynamics in nanoscale quantum dots of gallium arsenide using ultrafast electron diffraction. By varying the dot size from h = 11 to 46 nm, the length scale effect was examined, together with the temporal change. When the dot size is smaller than the inelastic phonon mean-free path, the energy remains localized in high-energy acoustic modes that travel coherently within the dot. As the dot size increases, an energy dissipation toward low-energy phonons takes place, and the transport becomes diffusive. Because ultrafast diffraction provides the atomic-scale resolution and a sufficiently high time resolution, other nanostructured materials can be studied similarly to elucidate the nature of dynamical energy localization.

  5. Resolving and Controlling Photoinduced Ultrafast Solvation in the Solid State.

    Science.gov (United States)

    Delor, Milan; McCarthy, Dannielle G; Cotts, Benjamin L; Roberts, Trevor D; Noriega, Rodrigo; Devore, David D; Mukhopadhyay, Sukrit; De Vries, Timothy S; Ginsberg, Naomi S

    2017-09-07

    Solid-state solvation (SSS) is a solid-state analogue of solvent-solute interactions in the liquid state. Although it could enable exceptionally fine control over the energetic properties of solid-state devices, its molecular mechanisms have remained largely unexplored. We use ultrafast transient absorption and optical Kerr effect spectroscopies to independently track and correlate both the excited-state dynamics of an organic emitter and the polarization anisotropy relaxation of a small polar dopant embedded in an amorphous polystyrene matrix. The results demonstrate that the dopants are able to rotationally reorient on ultrafast time scales following light-induced changes in the electronic configuration of the emitter, minimizing the system energy. The solid-state dopant-emitter dynamics are intrinsically analogous to liquid-state solvent-solute interactions. In addition, tuning the dopant/polymer pore ratio offers control over solvation dynamics by exploiting molecular-scale confinement of the dopants by the polymer matrix. Our findings will enable refined strategies for tuning optoelectronic material properties using SSS and offer new strategies to investigate mobility and disorder in heterogeneous solid and glassy materials.

  6. 32 CFR 1630.43 - Class 4-D: Minister of religion.

    Science.gov (United States)

    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) Regular...

  7. 2,4-D removal via denitrification using volatile fatty acids.

    Science.gov (United States)

    He, X; Wareham, D G

    2011-01-01

    Many countries have waters contaminated with both herbicides and nitrates; however, information is limited with respect to removal rates for combined nitrate and herbicide elimination. This research investigates the removal of 2,4-D via denitrification, with a particular emphasis on the effect of adding naturally generated volatile fatty acids (VFAs). The acids were produced from an acid-phase anaerobic digester with a mean VFA concentration of 3153±801 mg/L (as acetic acid). Initially, 2,4-D degrading bacteria were developed in an SBR fed with both sewage and 2,4-D (30-100 mg/L). Subsequent denitrification batch tests demonstrated that the specific denitrification rate increased from 0.0119±0.0039 using 2,4-D alone to 0.0192±0.0079 g NO₃-N/g VSS per day, when 2,4-D was combined with natural VFAs from the digester. Similarly, the specific 2,4-D consumption rate increased from 0.0016±0.0009 using 2,4-D alone to 0.0055±0.0021 g 2,4-D/g VSS per day, when using 2,4-D plus natural VFAs. Finally, a parallel increase in the percent 2,4-D removal was observed, rising from 28.33±11.88 using 2,4-D alone to 54.17±21.89 using 2,4-D plus natural VFAs.

  8. Predicting lower mantle heterogeneity from 4-D Earth models

    Science.gov (United States)

    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).

  9. Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging

    Science.gov (United States)

    Cocker, Tyler L.; Peller, Dominik; Yu, Ping; Repp, Jascha; Huber, Rupert

    2016-11-01

    Watching a single molecule move on its intrinsic timescale has been one of the central goals of modern nanoscience, and calls for measurements that combine ultrafast temporal resolution with atomic spatial resolution. Steady-state experiments access the requisite spatial scales, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution. But tracking the intrinsic dynamics of a single molecule directly in the time domain faces the challenge that interactions with the molecule must be confined to a femtosecond time window. For individual nanoparticles, such ultrafast temporal confinement has been demonstrated by combining scanning tunnelling microscopy with so-called lightwave electronics, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on timescales faster even than a single cycle of light. Here we build on ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state. It thereby removes a single electron from an individual pentacene molecule’s highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record approximately 100-femtosecond snapshot images of the orbital structure with sub-ångström spatial resolution, and to reveal, through pump/probe measurements, coherent molecular vibrations at terahertz frequencies directly in the time domain. We anticipate that the combination of lightwave electronics and the atomic resolution of our approach will open the door to visualizing ultrafast photochemistry and the operation of molecular electronics on the single-orbital scale.

  10. Progress in ultrafast intense laser science XI

    CERN Document Server

    Yamanouchi, Kaoru; Martin, Philippe

    2014-01-01

    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

  11. Progress in ultrafast intense laser science

    CERN Document Server

    Yamanouchi, Kaoru; Mathur, Deepak

    2014-01-01

    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

  12. Ultrafast Nonlinear Signal Processing in Silicon Waveguides

    DEFF Research Database (Denmark)

    Oxenløwe, Leif Katsuo; Mulvad, Hans Christian Hansen; Hu, Hao;

    2012-01-01

    We describe recent demonstrations of exploiting highly nonlinear silicon waveguides for ultrafast optical signal processing. We describe wavelength conversion and serial-to-parallel conversion of 640 Gbit/s data signals and 1.28 Tbit/s demultiplexing and all-optical sampling.......We describe recent demonstrations of exploiting highly nonlinear silicon waveguides for ultrafast optical signal processing. We describe wavelength conversion and serial-to-parallel conversion of 640 Gbit/s data signals and 1.28 Tbit/s demultiplexing and all-optical sampling....

  13. Ultrafast Terahertz Conductivity of Photoexcited Nanocrystalline Silicon

    DEFF Research Database (Denmark)

    Cooke, David; MacDonald, A. Nicole; Hryciw, Aaron;

    2007-01-01

    The ultrafast transient ac conductivity of nanocrystalline silicon films is investigated using time-resolved terahertz spectroscopy. While epitaxial silicon on sapphire exhibits a free carrier Drude response, silicon nanocrystals embedded in glass show a response that is best described by a class......The ultrafast transient ac conductivity of nanocrystalline silicon films is investigated using time-resolved terahertz spectroscopy. While epitaxial silicon on sapphire exhibits a free carrier Drude response, silicon nanocrystals embedded in glass show a response that is best described...

  14. New Aspects of Photocurrent Generation at Graphene pn Junctions Revealed by Ultrafast Optical Measurements

    Science.gov (United States)

    Aivazian, Grant; Sun, Dong; Jones, Aaron; Ross, Jason; Yao, Wang; Cobden, David; Xu, Xiaodong

    2012-02-01

    The remarkable electrical and optical properties of graphene make it a promising material for new optoelectronic applications. However, one important, but so far unexplored, property is the role of hot carriers in charge and energy transport at graphene interfaces. Here we investigate the photocurrent (PC) dynamics at a tunable graphene pn junction using ultrafast scanning PC microscopy. Pump-probe measurements show a temperature dependent relaxation time of photogenerated carriers that increases from 1.5ps at 290K to 4ps at 20K; while the amplitude of the PC is independent of the lattice temperature. These observations imply that it is hot carriers, not phonons, which dominate ultrafast energy transport. Gate dependent measurements show many interesting features such as pump induced saturation, enhancement, and sign reversal of probe generated PC. These observations reveal that the underlying PC mechanism is a combination of the thermoelectric and built-in electric field effects. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (˜500 GHz) for graphene-based photodetectors.

  15. Curvatronics with bilayer graphene in an effective $4D$ spacetime

    CERN Document Server

    Cariglia, M; Perali, A

    2016-01-01

    We show that in AB stacked bilayer graphene low energy excitations around the semimetallic points are described by massless, four dimensional Dirac fermions. There is an effective reconstruction of the 4 dimensional spacetime, including in particular the dimension perpendicular to the sheet, that arises dynamically from the physical graphene sheet and the interactions experienced by the carriers. The effective spacetime is the Eisenhart-Duval lift of the dynamics experienced by Galilei invariant L\\'evy-Leblond spin $\\frac{1}{2}$ particles near the Dirac points. We find that changing the intrinsic curvature of the bilayer sheet induces a change in the energy level of the electronic bands, switching from a conducting regime for negative curvature to an insulating one when curvature is positive. In particular, curving graphene bilayers allows opening or closing the energy gap between conduction and valence bands, a key effect for electronic devices. Thus using curvature as a tunable parameter opens the way for t...

  16. Ultrafast infrared studies of complex ligand rearrangements in solution

    Energy Technology Data Exchange (ETDEWEB)

    Payne, Christine K. [Univ. of California, Berkeley, CA (United States)

    2003-01-01

    The complete description of a chemical reaction in solution depends upon an understanding of the reactive molecule as well as its interactions with the surrounding solvent molecules. Using ultrafast infrared spectroscopy it is possible to observe both the solute-solvent interactions and the rearrangement steps which determine the overall course of a chemical reaction. The topics addressed in these studies focus on reaction mechanisms which require the rearrangement of complex ligands and the spectroscopic techniques necessary for the determination of these mechanisms. Ligand rearrangement is studied by considering two different reaction mechanisms for which the rearrangement of a complex ligand constitutes the most important step of the reaction. The first system concerns the rearrangement of a cyclopentadienyl ring as the response of an organometallic complex to a loss of electron density. This mechanism, commonly referred to as ''ring slip'', is frequently cited to explain reaction mechanisms. However, the ring slipped intermediate is too short-lived to be observed using conventional methods. Using a combination of ultrafast infrared spectroscopy and electronic structure calculations it has been shown that the intermediate exists, but does not form an eighteen-electron intermediate as suggested by traditional molecular orbital models. The second example examines the initial steps of alkyne polymerization. Group 6 (Cr, Mo, W) pentacarbonyl species are generated photolytically and used to catalyze the polymerization of unsaturated hydrocarbons through a series of coordination and rearrangement steps. Observing this reaction on the femto- to millisecond timescale indicates that the initial coordination of an alkyne solvent molecule to the metal center results in a stable intermediate that does not rearrange to form the polymer precursor. This suggests that polymerization requires the dissociation of additional carbonyl ligands before

  17. Ultrafast infrared studies of complex ligand rearrangements in solution

    Energy Technology Data Exchange (ETDEWEB)

    Payne, Christine K.

    2003-05-31

    The complete description of a chemical reaction in solution depends upon an understanding of the reactive molecule as well as its interactions with the surrounding solvent molecules. Using ultrafast infrared spectroscopy it is possible to observe both the solute-solvent interactions and the rearrangement steps which determine the overall course of a chemical reaction. The topics addressed in these studies focus on reaction mechanisms which require the rearrangement of complex ligands and the spectroscopic techniques necessary for the determination of these mechanisms. Ligand rearrangement is studied by considering two different reaction mechanisms for which the rearrangement of a complex ligand constitutes the most important step of the reaction. The first system concerns the rearrangement of a cyclopentadienyl ring as the response of an organometallic complex to a loss of electron density. This mechanism, commonly referred to as ''ring slip'', is frequently cited to explain reaction mechanisms. However, the ring slipped intermediate is too short-lived to be observed using conventional methods. Using a combination of ultrafast infrared spectroscopy and electronic structure calculations it has been shown that the intermediate exists, but does not form an eighteen-electron intermediate as suggested by traditional molecular orbital models. The second example examines the initial steps of alkyne polymerization. Group 6 (Cr, Mo, W) pentacarbonyl species are generated photolytically and used to catalyze the polymerization of unsaturated hydrocarbons through a series of coordination and rearrangement steps. Observing this reaction on the femto- to millisecond timescale indicates that the initial coordination of an alkyne solvent molecule to the metal center results in a stable intermediate that does not rearrange to form the polymer precursor. This suggests that polymerization requires the dissociation of additional carbonyl ligands before

  18. Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer.

    Science.gov (United States)

    Athanasopoulos, Stavros; Alfonso Hernandez, Laura; Beljonne, David; Fernandez-Alberti, Sebastian; Tretiak, Sergei

    2017-04-06

    Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S2 → S1 internal conversion process, revealing an efficient unidirectional donor → acceptor energy-transfer process. Detailed analysis of the excited-state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S2-S1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition.

  19. Excited states in DNA strands investigated by ultrafast laser spectroscopy.

    Science.gov (United States)

    Chen, Jinquan; Zhang, Yuyuan; Kohler, Bern

    2015-01-01

    Ultrafast laser experiments on carefully selected DNA model compounds probe the effects of base stacking, base pairing, and structural disorder on excited electronic states formed by UV absorption in single and double DNA strands. Direct π-orbital overlap between two stacked bases in a dinucleotide or in a longer single strand creates new excited states that decay orders of magnitude more slowly than the generally subpicosecond excited states of monomeric bases. Half or more of all excited states in single strands decay in this manner. Ultrafast mid-IR transient absorption experiments reveal that the long-lived excited states in a number of model compounds are charge transfer states formed by interbase electron transfer, which subsequently decay by charge recombination. The lifetimes of the charge transfer states are surprisingly independent of how the stacked bases are oriented, but disruption of π-stacking, either by elevating temperature or by adding a denaturing co-solvent, completely eliminates this decay channel. Time-resolved emission measurements support the conclusion that these states are populated very rapidly from initial excitons. These experiments also reveal the existence of populations of emissive excited states that decay on the nanosecond time scale. The quantum yield of these states is very small for UVB/UVC excitation, but increases at UVA wavelengths. In double strands, hydrogen bonding between bases perturbs, but does not quench, the long-lived excited states. Kinetic isotope effects on the excited-state dynamics suggest that intrastrand electron transfer may couple to interstrand proton transfer. By revealing how structure and non-covalent interactions affect excited-state dynamics, on-going experimental and theoretical studies of excited states in DNA strands can advance understanding of fundamental photophysics in other nanoscale systems.

  20. Synthesis and characterization of zinc oxide nanorods and its photocatalytic activities towards degradation of 2,4-D.

    Science.gov (United States)

    Meenakshi, G; Sivasamy, A

    2017-01-01

    Semiconductor zinc oxide nanorods (NRZnO) were prepared by sol-gel technique using zinc acetate as the precursor and ammonia as the precipitating agent. The prepared photocatalyst were characterized by X-ray diffraction (XRD), Fourier Transform Infrared (FTIR), UV-Visible diffuse reflectance spectroscopy (UV-Vis-DRS), X-ray photoelectron spectroscopy (XPS), Field Emission-Scanning Electron Microscopy (FE-SEM), Atomic Force Microscopy (AFM), High Resolution-Tunneling Microscope (HR-TEM), Brunauer, Emmett and Teller (BET) and electron paramagnetic resonance spectroscopy (EPR) analysis. Particle size of the prepared photocatalyst was established by XRD and FE-SEM analysis. The morphology and the formation of uniform NRZnO was controlled by the temperature, entire concentration of precursors, duration of aging process. High surface roughness and porosity confirmed by AFM analysis. Band gap energy of the synthesized photocatalyst (3.2eV) was determined by using diffuse reflectance spectroscopy. The in-situ production of OH radicals by the prepared photocatalyst was confirmed by electron paramagnetic resonance spectroscopy (EPR) spin trapping technique. The photocatalytic activity of prepared NRZnO was evaluated by photo degradation of 2, 4-dichlorophenoxyacetic acid (2, 4-D) under UV and visible light irradiations. Experimental parameter such as effect of pH, catalyst dosage, initial 2, 4- D concentrations and addition of different electrolytes on the degradation of 2, 4-D was also studied in detail. Neutral pH was found to be the optimum and catalyst dosage of 30mg/10ml resulted in higher percentage of degradation. The photo degraded samples were analyzed by chemical oxygen demand (COD) analysis, UV-Visible spectroscopy. Reusability of the prepared photocatalyst was tested upto three cycles without affecting its performance. The experimental shown the rate of degradation follows pseudo-first order rate kinetics with respect to 2, 4 D. Copyright © 2016 Elsevier Inc