Science.gov

Sample records for 4d ultrafast electron

  1. 4D multiple-cathode ultrafast electron microscopy

    PubMed Central

    Baskin, John Spencer; Liu, Haihua; Zewail, Ahmed H.

    2014-01-01

    Four-dimensional multiple-cathode ultrafast electron microscopy is developed to enable the capture of multiple images at ultrashort time intervals for a single microscopic dynamic process. The dynamic process is initiated in the specimen by one femtosecond light pulse and probed by multiple packets of electrons generated by one UV laser pulse impinging on multiple, spatially distinct, cathode surfaces. Each packet is distinctly recorded, with timing and detector location controlled by the cathode configuration. In the first demonstration, two packets of electrons on each image frame (of the CCD) probe different times, separated by 19 picoseconds, in the evolution of the diffraction of a gold film following femtosecond heating. Future elaborations of this concept to extend its capabilities and expand the range of applications of 4D ultrafast electron microscopy are discussed. The proof-of-principle demonstration reported here provides a path toward the imaging of irreversible ultrafast phenomena of materials, and opens the door to studies involving the single-frame capture of ultrafast dynamics using single-pump/multiple-probe, embedded stroboscopic imaging. PMID:25006261

  2. Perspective: 4D ultrafast electron microscopy--Evolutions and revolutions.

    PubMed

    Shorokhov, Dmitry; Zewail, Ahmed H

    2016-02-28

    In this Perspective, the evolutionary and revolutionary developments of ultrafast electron imaging are overviewed with focus on the "single-electron concept" for probing methodology. From the first electron microscope of Knoll and Ruska [Z. Phys. 78, 318 (1932)], constructed in the 1930s, to aberration-corrected instruments and on, to four-dimensional ultrafast electron microscopy (4D UEM), the developments over eight decades have transformed humans' scope of visualization. The changes in the length and time scales involved are unimaginable, beginning with the micrometer and second domains, and now reaching the space and time dimensions of atoms in matter. With these advances, it has become possible to follow the elementary structural dynamics as it unfolds in real time and to provide the means for visualizing materials behavior and biological functions. The aim is to understand emergent phenomena in complex systems, and 4D UEM is now central for the visualization of elementary processes involved, as illustrated here with examples from past achievements and future outlook. PMID:26931672

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

    NASA Astrophysics Data System (ADS)

    Shorokhov, Dmitry; Zewail, Ahmed H.

    2016-02-01

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

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

    PubMed

    Yurtsever, Aycan; Zewail, Ahmed H

    2009-10-30

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

  5. 4D scanning transmission ultrafast electron microscopy: Single-particle imaging and spectroscopy.

    PubMed

    Ortalan, Volkan; Zewail, Ahmed H

    2011-07-20

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

  6. On the dynamical nature of the active center in a single-site photocatalyst visualized by 4D ultrafast electron microscopy

    PubMed Central

    Yoo, Byung-Kuk; Su, Zixue; Thomas, John Meurig; Zewail, Ahmed H.

    2016-01-01

    Understanding the dynamical nature of the catalytic active site embedded in complex systems at the atomic level is critical to developing efficient photocatalytic materials. Here, we report, using 4D ultrafast electron microscopy, the spatiotemporal behaviors of titanium and oxygen in a titanosilicate catalytic material. The observed changes in Bragg diffraction intensity with time at the specific lattice planes, and with a tilted geometry, provide the relaxation pathway: the Ti4+=O2− double bond transformation to a Ti3+−O1− single bond via the individual atomic displacements of the titanium and the apical oxygen. The dilation of the double bond is up to 0.8 Å and occurs on the femtosecond time scale. These findings suggest the direct catalytic involvement of the Ti3+−O1− local structure, the significance of nonthermal processes at the reactive site, and the efficient photo-induced electron transfer that plays a pivotal role in many photocatalytic reactions. PMID:26729878

  7. 4D microvascular imaging based on ultrafast Doppler tomography.

    PubMed

    Demené, Charlie; Tiran, Elodie; Sieu, Lim-Anna; Bergel, Antoine; Gennisson, Jean Luc; Pernot, Mathieu; Deffieux, Thomas; Cohen, Ivan; Tanter, Mickael

    2016-02-15

    4D ultrasound microvascular imaging was demonstrated by applying ultrafast Doppler tomography (UFD-T) to the imaging of brain hemodynamics in rodents. In vivo real-time imaging of the rat brain was performed using ultrasonic plane wave transmissions at very high frame rates (18,000 frames per second). Such ultrafast frame rates allow for highly sensitive and wide-field-of-view 2D Doppler imaging of blood vessels far beyond conventional ultrasonography. Voxel anisotropy (100 μm × 100 μm × 500 μm) was corrected for by using a tomographic approach, which consisted of ultrafast acquisitions repeated for different imaging plane orientations over multiple cardiac cycles. UFT-D allows for 4D dynamic microvascular imaging of deep-seated vasculature (up to 20 mm) with a very high 4D resolution (respectively 100 μm × 100 μm × 100 μm and 10 ms) and high sensitivity to flow in small vessels (>1 mm/s) for a whole-brain imaging technique without requiring any contrast agent. 4D ultrasound microvascular imaging in vivo could become a valuable tool for the study of brain hemodynamics, such as cerebral flow autoregulation or vascular remodeling after ischemic stroke recovery, and, more generally, tumor vasculature response to therapeutic treatment. PMID:26555279

  8. Four-dimensional ultrafast electron microscopy

    PubMed Central

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

    2005-01-01

    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 ångstrom-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 Å 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. PMID:15883380

  9. Single-electron pulses for ultrafast diffraction

    PubMed Central

    Aidelsburger, M.; Kirchner, F. O.; Krausz, F.; Baum, P.

    2010-01-01

    Visualization of atomic-scale structural motion by ultrafast electron diffraction and microscopy requires electron packets of shortest duration and highest coherence. We report on the generation and application of single-electron pulses for this purpose. Photoelectric emission from metal surfaces is studied with tunable ultraviolet pulses in the femtosecond regime. The bandwidth, efficiency, coherence, and electron pulse duration are investigated in dependence on excitation wavelength, intensity, and laser bandwidth. At photon energies close to the cathode’s work function, the electron pulse duration shortens significantly and approaches a threshold that is determined by interplay of the optical pulse width and the acceleration field. An optimized choice of laser wavelength and bandwidth results in sub-100-fs electron pulses. We demonstrate single-electron diffraction from polycrystalline diamond films and reveal the favorable influences of matched photon energies on the coherence volume of single-electron wave packets. We discuss the consequences of our findings for the physics of the photoelectric effect and for applications of single-electron pulses in ultrafast 4D imaging of structural dynamics. PMID:21041681

  10. Attosecond electron pulses for 4D diffraction and microscopy

    PubMed Central

    Baum, Peter; Zewail, Ahmed H.

    2007-01-01

    In this contribution, we consider the advancement of ultrafast electron diffraction and microscopy to cover the attosecond time domain. The concept is centered on the compression of femtosecond electron packets to trains of 15-attosecond pulses by the use of the ponderomotive force in synthesized gratings of optical fields. Such attosecond electron pulses are significantly shorter than those achievable with extreme UV light sources near 25 nm (≈50 eV) and have the potential for applications in the visualization of ultrafast electron dynamics, especially of atomic structures, clusters of atoms, and some materials. PMID:18000040

  11. 4D electron microscopy visualization of anisotropic atomic motions in carbon nanotubes.

    PubMed

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

    2012-06-01

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

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

    PubMed

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

    2016-07-01

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

  13. Ultrafast Electron Diffraction: How It Works

    SciTech Connect

    2015-08-05

    A new technology at SLAC uses high-energy electrons to unravel motions in materials that are faster than a tenth of a trillionth of a second, opening up new research opportunities in ultrafast science.

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

    PubMed

    Flannigan, David J; Zewail, Ahmed H

    2010-05-12

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

  15. Ultrafast Dynamics of Electrons in Ammonia

    NASA Astrophysics Data System (ADS)

    Vöhringer, Peter

    2015-04-01

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

  16. Ultrafast dynamics of electrons in ammonia.

    PubMed

    Vöhringer, Peter

    2015-04-01

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

  17. Bridge mediated ultrafast heterogeneous electron transfer

    NASA Astrophysics Data System (ADS)

    Ramakrishna, S.; Willig, F.; May, V.

    2002-01-01

    Bridge mediated photoinduced ultrafast heterogeneous electron transfer (ET) from a molecularly anchored chromophore to a semiconductor surface is modelled theoretically. The continuum levels of the semiconductor substrate are taken into account in the numerical calculations via a polynomial expansion. Electron transfer for the direct injection case in the strong coupling limit is studied and compared with cases where intermediate bridging states are successively introduced to weaken the effective electronic coupling. The role of vibronic coherences in the strong electronic coupling limit as well as in off-resonant bridge mediated electron transfer is also discussed.

  18. Structure and Dynamics with Ultrafast Electron Microscopes

    NASA Astrophysics Data System (ADS)

    Siwick, Bradley

    In this talk I will describe how combining ultrafast lasers and electron microscopes in novel ways makes it possible to directly `watch' the time-evolving structure of condensed matter, both at the level of atomic-scale structural rearrangements in the unit cell and at the level of a material's nano- microstructure. First, I will briefly describe my group's efforts to develop ultrafast electron diffraction using radio- frequency compressed electron pulses in the 100keV range, a system that rivals the capabilities of xray free electron lasers for diffraction experiments. I will give several examples of the new kinds of information that can be gleaned from such experiments. In vanadium dioxide we have mapped the detailed reorganization of the unit cell during the much debated insulator-metal transition. In particular, we have been able to identify and separate lattice structural changes from valence charge density redistribution in the material on the ultrafast timescale. In doing so we uncovered a previously unreported optically accessible phase/state of vanadium dioxide that has monoclinic crystallography like the insulator, but electronic structure and properties that are more like the rutile metal. We have also combined these dynamic structural measurements with broadband ultrafast spectroscopy to make detailed connections between structure and properties for the photoinduced insulator to metal transition. Second, I will show how dynamic transmission electron microscopy (DTEM) can be used to make direct, real space images of nano-microstructural evolution during laser-induced crystallization of amorphous semiconductors at unprecedented spatio-temporal resolution. This is a remarkably complex process that involves several distinct modes of crystal growth and the development of intricate microstructural patterns on the nanosecond to ten microsecond timescales all of which can be imaged directly with DTEM.

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

    PubMed

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

    2016-07-13

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

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

    SciTech Connect

    Hastings, J.B.; Rudakov, F.M.; Dowell, D.H.; Schmerge, J.F.; Cardoza, J.D.; Castro, J.M.; Gierman, S.M.; Loos, H.; 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.

  1. Ultrafast electronic dynamics driven by nuclear motion

    NASA Astrophysics Data System (ADS)

    Vendrell, Oriol

    2016-05-01

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

  2. A pulsed electron gun for ultrafast electron diffraction at surfaces.

    PubMed

    Janzen, A; Krenzer, B; Heinz, O; Zhou, P; Thien, D; Hanisch, A; Meyer Zu Heringdorf, F-J; von der Linde, D; Horn von Hoegen, M

    2007-01-01

    The construction of a pulsed electron gun for ultrafast reflection high-energy electron diffraction experiments at surfaces is reported. Special emphasis is placed on the characterization of the electron source: a photocathode, consisting of a 10 nm thin Au film deposited onto a sapphire substrate. Electron pulses are generated by the illumination of the film with ultraviolet laser pulses of femtosecond duration. The photoelectrons are emitted homogeneously across the photocathode with an energy distribution of 0.1 eV width. After leaving the Au film, the electrons are accelerated to kinetic energies of up to 15 keV. Focusing is accomplished by an electrostatic lens. The temporal resolution of the experiment is determined by the probing time of the electrons traveling across the surface which is about 30 ps. However, the duration of the electron pulses can be reduced to less than 6 ps. PMID:17503932

  3. Probing Structural and Electronic Dynamics with Ultrafast Electron Microscopy

    SciTech Connect

    Plemmons, DA; Suri, PK; Flannigan, DJ

    2015-05-12

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

  4. Imaging population transfer in atoms with ultrafast electron pulses

    NASA Astrophysics Data System (ADS)

    Shao, Hua-Chieh; Starace, Anthony F.

    2016-05-01

    Ultrafast electron diffraction and microscopy have made significant progress recently in investigating atomic-scale structural dynamics in gas-phase and condensed materials. With these advances, direct imaging of electronic motions in atoms and molecules by ultrafast electron diffraction is anticipated. We propose imaging a laser-driven coherent population transfer in lithium atoms by femtosecond ultrafast electron pulses. Valuable information and insight can be obtained from studying such a system in order to refine ultrafast electron techniques and to interpret experimental results. Adiabatic passage by level crossing is used to transfer the electron population from the 2 s to the 2 p state. Our simulations demonstrate the ability of ultrafast electron diffraction to image this population transfer, as the time-dependent diffraction images reflect the electronic motion in the scattering intensity and angular distribution. Furthermore, asymmetric diffraction patterns indicate that even the relative phases of the electronic wave function can be resolved, provided there is sufficient temporal resolution. This work has been supported in part by DOE Award No. DE-SC0012193 [H.-C.S.] and by NSF Grant No. PHYS-1505492 [A.F.S.].

  5. Ultrafast electron transport in graphene and magnetic nanostructures

    NASA Astrophysics Data System (ADS)

    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.

  6. Space charge effects in ultrafast electron diffraction and imaging

    SciTech Connect

    Tao Zhensheng; Zhang He; Duxbury, P. M.; Berz, Martin; Ruan, Chong-Yu

    2012-02-15

    Understanding space charge effects is central for the development of high-brightness ultrafast electron diffraction and microscopy techniques for imaging material transformation with atomic scale detail at the fs to ps timescales. We present methods and results for direct ultrafast photoelectron beam characterization employing a shadow projection imaging technique to investigate the generation of ultrafast, non-uniform, intense photoelectron pulses in a dc photo-gun geometry. Combined with N-particle simulations and an analytical Gaussian model, we elucidate three essential space-charge-led features: the pulse lengthening following a power-law scaling, the broadening of the initial energy distribution, and the virtual cathode threshold. The impacts of these space charge effects on the performance of the next generation high-brightness ultrafast electron diffraction and imaging systems are evaluated.

  7. Fast-electron-impact study on excitations of 4d electron of xenon

    NASA Astrophysics Data System (ADS)

    Zhang, Xin; Liu, Ya-Wei; Peng, Yi-Geng; Xu, Long-Quan; Ni, Dong-Dong; Kang, Xu; Wang, Yang-Yang; Qi, Yue-Ying; Zhu, Lin-Fan

    2015-12-01

    The electron energy loss spectrum of the 4d excitations of xenon was measured at an incident electron energy of 1500 eV and a scattering angle of 6°. Besides the optically allowed transitions of and the optically forbidden transitions of and were observed. The measured features are assigned with the help of the calculation by the Cowan Code. The line profile parameters of both optically allowed transitions and optically forbidden ones were determined and compared with the previous available data. It is found that the natural widths of both dipole-allowed and dipole-forbidden excitations are approximately identical, which means the spectator transitions dominate the resonant Auger effect for both dipole-allowed and dipole-forbidden transitions. Project supported by the National Natural Science Foundation of China (Grant Nos. U1332204, 11274291, 11504361, and 11320101003).

  8. Ultrafast spectroscopy of correlated electron systems

    NASA Astrophysics Data System (ADS)

    Schmid, Benjamin Andrew

    This dissertation attempts to illuminate and expand our understanding of charge dynamics in a number of different semiconductor materials, in particular the behavior of electron-hole pairs which are correlated via the long-range Coulomb interaction. Terahertz spectroscopy gives us direct access to probe the fundamental excitations of quasiparticles in a wide range of materials systems. By probing the low-energy excitations of materials on short time scales, one can learn a great deal about their quasiparticles and dynamics as well as explore new tools for their manipulation. Carriers in semiconductors, existing either as bound electron-hole pairs or "free" carriers (or both), are particularly amenable to this avenue of study. The internal structure of excitons in semiconductors lies energetically in the far- to mid-infrared. Free carriers moving under the influence of a free-space electric field reveal much about themselves. By exploiting this unique window, one can both characterize and manipulate these systems in novel ways, as well as seek to understand the physics of new materials. I study the ferromagnetic semiconductor gallium manganese phosphide (GaMnP) to better understand the role of charge carriers in the origins of ferromagnetism. By applying the tools of terahertz spectroscopy, I am able to make contact free measurements of hole populations in a novel GaMnP film. I exploit THz spectroscopy to provide a direct gauge of bound and unbound pair densities in gallium arsenide quantum wells, enabling the observation of the excitonic fine structure as it evolves under high-density conditions. And finally I have observed for the first time stimulated emission of far-infrared radiation from internal transitions in excitons in the semiconductor Cu 2O. Broadband THz spectroscopy is employed to directly map out the ultrafast dynamics, spectral positions, and line broadenings of intra-excitonic transitions. This work has opened up new possibilities for the quantum

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

    PubMed

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

    2016-05-01

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

  10. Breaking resolution limits in ultrafast electron diffraction and microscopy

    PubMed Central

    Baum, Peter; Zewail, Ahmed H.

    2006-01-01

    Ultrafast electron microscopy and diffraction are powerful techniques for the study of the time-resolved structures of molecules, materials, and biological systems. Central to these approaches is the use of ultrafast coherent electron packets. The electron pulses typically have an energy of 30 keV for diffraction and 100–200 keV for microscopy, corresponding to speeds of 33–70% of the speed of light. Although the spatial resolution can reach the atomic scale, the temporal resolution is limited by the pulse width and by the difference in group velocities of electrons and the light used to initiate the dynamical change. In this contribution, we introduce the concept of tilted optical pulses into diffraction and imaging techniques and demonstrate the methodology experimentally. These advances allow us to reach limits of time resolution down to regimes of a few femtoseconds and, possibly, attoseconds. With tilted pulses, every part of the sample is excited at precisely the same time as when the electrons arrive at the specimen. Here, this approach is demonstrated for the most unfavorable case of ultrafast crystallography. We also present a method for measuring the duration of electron packets by autocorrelating electron pulses in free space and without streaking, and we discuss the potential of tilting the electron pulses themselves for applications in domains involving nuclear and electron motions. PMID:17056711

  11. Photon gating in four-dimensional ultrafast electron microscopy

    PubMed Central

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

    2015-01-01

    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. PMID:26438835

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

    SciTech Connect

    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.

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

    PubMed

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

    2015-07-01

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

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

    SciTech Connect

    Weathersby, S. P.; Brown, G.; Chase, T. F.; Coffee, R.; Corbett, J.; Eichner, J. P.; Frisch, J. C.; Fry, A. R.; Gühr, M.; Hartmann, N.; Hast, C.; Hettel, R.; Jobe, R. K.; Jongewaard, E. N.; Lewandowski, J. R.; Li, R. K. Lindenberg, A. M.; Makasyuk, I.; May, J. E.; McCormick, D.; and others

    2015-07-15

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

  15. Ultrafast electron transport across nano gaps in nanowire circuits

    SciTech Connect

    Potma, Eric O.

    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.

  16. rf streak camera based ultrafast relativistic electron diffraction.

    PubMed

    Musumeci, P; Moody, J T; Scoby, C M; Gutierrez, M S; Tran, T

    2009-01-01

    We theoretically and experimentally investigate the possibility of using a rf streak camera to time resolve in a single shot structural changes at the sub-100 fs time scale via relativistic electron diffraction. We experimentally tested this novel concept at the UCLA Pegasus rf photoinjector. Time-resolved diffraction patterns from thin Al foil are recorded. Averaging over 50 shots is required in order to get statistics sufficient to uncover a variation in time of the diffraction patterns. In the absence of an external pump laser, this is explained as due to the energy chirp on the beam out of the electron gun. With further improvements to the electron source, rf streak camera based ultrafast electron diffraction has the potential to yield truly single shot measurements of ultrafast processes. PMID:19191429

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

    PubMed

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

    2009-07-10

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

  18. Ultrafast Electron Diffractive Voltammetry:. General Formalism and Applications

    NASA Astrophysics Data System (ADS)

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

    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 photoemission. We show that voltammetry contribution associated with photoemission has a long decay tail and plays a more significant role in the nanosecond timescale, whereas the ultrafast voltammetry are dominated by local charge transfer, such as surface charging and molecular charge transport at nanostructured interfaces. We also discuss the general applicability of the diffractive voltammetry as an integral part of quantitative ultrafast electron diffraction methodology in researching different types of interfaces having distinctive surface diffraction and boundary conditions.

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

    NASA Astrophysics Data System (ADS)

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

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

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

    SciTech Connect

    Feng, L. W.; Lin, L.; Huang, S. L.; Quan, S. W.; Hao, J. K.; Zhu, F.; Wang, F.; Liu, K. X.; Jiang, T.; Zhu, P. F.; Fu, F.; Wang, R.; Zhao, L.; Xiang, D.

    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.

  1. Ultrafast electron diffraction from aligned molecules

    SciTech Connect

    Centurion, Martin

    2015-08-17

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

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

    NASA Astrophysics Data System (ADS)

    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.

  3. Prospects for Electron Imaging with Ultrafast Time Resolution

    SciTech Connect

    Armstrong, M R; Reed, B W; Torralva, B R; Browning, N D

    2007-01-26

    Many pivotal aspects of material science, biomechanics, and chemistry would benefit from nanometer imaging with ultrafast time resolution. Here we demonstrate the feasibility of short-pulse electron imaging with t10 nanometer/10 picosecond spatio-temporal resolution, sufficient to characterize phenomena that propagate at the speed of sound in materials (1-10 kilometer/second) without smearing. We outline resolution-degrading effects that occur at high current density followed by strategies to mitigate these effects. Finally, we present a model electron imaging system that achieves 10 nanometer/10 picosecond spatio-temporal resolution.

  4. Nanofluidics. Observing liquid flow in nanotubes by 4D electron microscopy.

    PubMed

    Lorenz, Ulrich J; Zewail, Ahmed H

    2014-06-27

    Nanofluidics involves the study of fluid transport in nanometer-scale structures. We report the direct observation of fluid dynamics in a single zinc oxide nanotube with the high spatial and temporal resolution of four-dimensional (4D) electron microscopy. The nanotube is filled with metallic lead, which we melt in situ with a temperature jump induced by a heating laser pulse. We then use a short electron pulse to create an image of the ensuing dynamics of the hot liquid. Single-shot images elucidate the mechanism of irreversible processes, whereas stroboscopic diffraction patterns provide the heating and cooling rates of single nanotubes. The temporal changes of the images enable studies of the viscous friction involved in the flow of liquid within the nanotube, as well as studies of mechanical processes such as those that result in the formation of extrusions. PMID:24970082

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

    PubMed

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

    2016-03-17

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

  6. Ultrafast studies of coexisting electronic order in cuprate superconductors

    NASA Astrophysics Data System (ADS)

    Hinton, James; Thewalt, Eric; Alpichshev, Zhanybek; Sternbach, Aaron; McLeod, Alex; Ji, L.; Veit, Mike; Dorrow, Chelsey; Koralek, Jake; Xhao, Xudong; Barisic, Neven; Kemper, Alexander; Gedik, Nuh; Greven, Martin; Basov, Dimitri; Orenstein, Joe

    The cuprate family of high temperature superconductors displays a variety of electronic phases which emerge when charge carriers are added to the antiferromagnetic parent compound. These electronic phases are characterized by subtle differences in the low energy electronic excitations. Ultrafast time-resolved reflectivity (TRR) provides an ideal tool for investigating the cuprate phase diagram, as small changes in the electronic structure can produce significant contrast in the non-equilibrium reflectivity. Here we present TRR measurements of cuprate superconductors, focusing on the model single-layer cuprate HgBa2CuO4+δ. We observe a cusp-like feature in the quasiparticle lifetime near the superconducting transition temperature Tc. This feature can be understood using a model of coherently-mixed charge-density wave and superconducting pairing. We propose extending this technique to the nanoscale using ultrafast scattering scanning near-field microscopy (u-SNOM). This will allow us to explore how these electronic phases coexist and compete in real-space.

  7. Cardiac function and perfusion dynamics measured on a beat-by-beat basis in the live mouse using ultra-fast 4D optoacoustic imaging

    NASA Astrophysics Data System (ADS)

    Ford, Steven J.; Deán-Ben, Xosé L.; Razansky, Daniel

    2015-03-01

    The fast heart rate (~7 Hz) of the mouse makes cardiac imaging and functional analysis difficult when studying mouse models of cardiovascular disease, and cannot be done truly in real-time and 3D using established imaging modalities. Optoacoustic imaging, on the other hand, provides ultra-fast imaging at up to 50 volumetric frames per second, allowing for acquisition of several frames per mouse cardiac cycle. In this study, we combined a recently-developed 3D optoacoustic imaging array with novel analytical techniques to assess cardiac function and perfusion dynamics of the mouse heart at high, 4D spatiotemporal resolution. In brief, the heart of an anesthetized mouse was imaged over a series of multiple volumetric frames. In another experiment, an intravenous bolus of indocyanine green (ICG) was injected and its distribution was subsequently imaged in the heart. Unique temporal features of the cardiac cycle and ICG distribution profiles were used to segment the heart from background and to assess cardiac function. The 3D nature of the experimental data allowed for determination of cardiac volumes at ~7-8 frames per mouse cardiac cycle, providing important cardiac function parameters (e.g., stroke volume, ejection fraction) on a beat-by-beat basis, which has been previously unachieved by any other cardiac imaging modality. Furthermore, ICG distribution dynamics allowed for the determination of pulmonary transit time and thus additional quantitative measures of cardiovascular function. This work demonstrates the potential for optoacoustic cardiac imaging and is expected to have a major contribution toward future preclinical studies of animal models of cardiovascular health and disease.

  8. Ultrafast dynamics of electrons at interfaces

    SciTech Connect

    McNeill, Jason D.

    1999-05-03

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

  9. Electronic/photonic interfaces for ultrafast data processing.

    SciTech Connect

    Overberg, Mark E.; Geib, Kent Martin; Serkland, Darwin Keith; Hsu, Alan Yuan-Chun; Keeler, Gordon Arthur; Finnegan, Patrick Sean

    2008-09-01

    This report summarizes a 3-month program that explored the potential areas of impact for electronic/photonic integration technologies, as applied to next-generation data processing systems operating within 100+ Gb/s optical networks. The study included a technology review that targeted three key functions of data processing systems, namely receive/demultiplexing/clock recovery, data processing, and transmit/multiplexing. Various technical approaches were described and evaluated. In addition, we initiated the development of high-speed photodetectors and hybrid integration processes, two key elements of an ultrafast data processor. Relevant experimental results are described herein.

  10. Mechanisms for Ultrafast Nonradiative Relaxation in Electronically Excited Eumelanin Constituents

    PubMed Central

    Meng, Sheng; Kaxiras, Efthimios

    2008-01-01

    We investigate the relaxation dynamics of melanin model constituents including monomers, dimers, and tetramers, upon excitation, using state-of-the-art, time-dependent, density functional theory calculations. The results explain the ability of these molecules to transform photon energy into thermal energy in a remarkably short timescale of ∼100 fs. We find that after electronic excitation by light absorption, ultrafast energy conversion takes place through two novel mechanisms: proton transfer on a timescale of 110 fs and state mixing upon oligomerization on a timescale of <50 fs. These results are in good agreement with available experiments and help elucidate melanin's role in photoprotection against ultraviolet radiation. PMID:18676639

  11. Adapting High Brightness Relativistic Electron Beams for Ultrafast Science

    NASA Astrophysics Data System (ADS)

    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

  12. Probing Transient Electron Dynamics Using Ultrafast X Rays

    NASA Astrophysics Data System (ADS)

    Bucksbaum, Philip

    2016-05-01

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

  13. Ultrafast electron relaxation dynamics in coupled metal nanoparticles in aggregates.

    PubMed

    Jain, Prashant K; Qian, Wei; El-Sayed, Mostafa A

    2006-01-12

    We report the effect of aggregation in gold nanoparticles on their ultrafast electron-phonon relaxation dynamics measured by femtosecond transient absorption pump-probe spectroscopy. UV-visible extinction and transient absorption of the solution-stable aggregates of gold nanoparticles show a broad absorption in the 550-700-nm region in addition to the isolated gold nanoparticle plasmon resonance. This broad red-shifted absorption can be attributed to contributions from gold nanoparticle aggregates with different sizes and/or different fractal structures. The electron-phonon relaxation, reflected as a fast decay component of the transient bleach, is found to depend on the probe wavelength, suggesting that each wavelength interrogates one particular subset of the aggregates. As the probe wavelength is changed from 520 to 635 nm across the broad aggregate absorption, the rate of electron-phonon relaxation increases. The observed trend in the hot electron lifetimes can be explained on the basis of an increased overlap of the electron oscillation frequency with the phonon spectrum and enhanced interfacial electron scattering, with increasing extent of aggregation. The experimental results strongly suggest the presence of intercolloid electronic coupling within the nanoparticle aggregates, besides the well-known dipolar plasmon coupling. PMID:16471511

  14. 4D-QSAR analysis and pharmacophore modeling: electron conformational-genetic algorithm approach for penicillins.

    PubMed

    Yanmaz, Ersin; Sarıpınar, Emin; Şahin, Kader; Geçen, Nazmiye; Çopur, Fatih

    2011-04-01

    4D-QSAR studies were performed on a series of 87 penicillin analogues using the electron conformational-genetic algorithm (EC-GA) method. In this EC-based method, each conformation of the molecular system is described by a matrix (ECMC) with both electron structural parameters and interatomic distances as matrix elements. Multiple comparisons of these matrices within given tolerances for high active and low active penicillin compounds allow one to separate a smaller number of matrix elements (ECSA) which represent the pharmacophore groups. The effect of conformations was investigated building model 1 and 2 based on ensemble of conformers and single conformer, respectively. GA was used to select the most important descriptors and to predict the theoretical activity of the training (74 compounds) and test (13 compounds, commercial penicillins) sets. The model 1 for training and test sets obtained by optimum 12 parameters gave more satisfactory results (R(training)(2)=0.861, SE(training)=0.044, R(test)(2)=0.892, SE(test)=0.099, q(2)=0.702, q(ext1)(2)=0.777 and q(ext2)(2)=0.733) than model 2 (R(training)(2)=0.774, SE(training)=0.056, R(test)(2)=0.840, SE(test)=0.121, q(2)=0.514, q(ext1)(2)=0.641 and q(ext2)(2)=0.570). To estimate the individual influence of each of the molecular descriptors on biological activity, the E statistics technique was applied to the derived EC-GA model. PMID:21419636

  15. Special issue on ultrafast electron and molecular dynamics

    NASA Astrophysics Data System (ADS)

    Martin, Fernando; Hishikawa, Akiyoshi; Vrakking, Marc

    2014-06-01

    In the last few years, the advent of novel experimental and theoretical approaches has made possible the investigation of (time-resolved) molecular dynamics in ways not anticipated before. Experimentally, the introduction of novel light sources such as high-harmonic generation (HHG) and XUV/x-ray free electron lasers, and the emergence of novel detection strategies, such as time-resolved electron/x-ray diffraction and the fully coincident detection of electrons and fragment ions in reaction microscopes, has significantly expanded the arsenal of available techniques, and has taken studies of molecular dynamics into new domains of spectroscopic, spatial and temporal resolution, the latter including first explorations into the attosecond domain, thus opening completely new avenues for imaging electronic and nuclear dynamics in molecules. Along the way, particular types of molecular dynamics, e.g., dynamics around conical intersections, have gained an increased prominence, sparked by the realization of the essential role that this dynamics plays in relaxation pathways in important bio-molecular systems. In the short term, this will allow one to uncover and control the dynamics of elementary chemical processes such as, e.g., ultrafast charge migration, proton transfer, isomerization or multiple ionization, and to address new key questions about the role of attosecond coherent electron dynamics in chemical reactivity. The progress on the theoretical side has been no less impressive. Novel generations of supercomputers and a series of novel computational strategies have allowed nearly exact calculations in small molecules, as well as highly successful approximate calculations in large, polyatomic molecules, including biomolecules. Frequent and intensive collaborations involving both theory and experiment have been essential for the progress that has been accomplished. The special issue 'Ultrafast electron and molecular dynamics' seeks to provide an overview of the current

  16. Nonequilibrium phase transitions in cuprates observed by ultrafast electron crystallography.

    PubMed

    Gedik, Nuh; Yang, Ding-Shyue; Logvenov, Gennady; Bozovic, Ivan; Zewail, Ahmed H

    2007-04-20

    Nonequilibrium phase transitions, which are defined by the formation of macroscopic transient domains, are optically dark and cannot be observed through conventional temperature- or pressure-change studies. We have directly determined the structural dynamics of such a nonequilibrium phase transition in a cuprate superconductor. Ultrafast electron crystallography with the use of a tilted optical geometry technique afforded the necessary atomic-scale spatial and temporal resolutions. The observed transient behavior displays a notable "structural isosbestic" point and a threshold effect for the dependence of c-axis expansion (Deltac) on fluence (F), with Deltac/F = 0.02 angstrom/(millijoule per square centimeter). This threshold for photon doping occurs at approximately 0.12 photons per copper site, which is unexpectedly close to the density (per site) of chemically doped carriers needed to induce superconductivity. PMID:17446397

  17. Sub-fs electron pulses for ultrafast electron diffraction

    NASA Astrophysics Data System (ADS)

    Fill, Ernst; Veisz, Laszlo; Apolonski, Alexander; Krausz, Ferenc

    2006-11-01

    We present a new concept for an electron gun generating subrelativistic electron pulses with a duration down to the attosecond range. It is based on a cylindrical RF cavity (a so-called pill-box cavity) oscillating in its TM010 eigenmode with a photocathode triggered by a fs-laser pulse. Injecting electrons at an appropriate phase of the RF cycle compensates for their initial velocities and time delays and makes the electrons arrive at a target in a sub-fs temporal window. Such electron pulses will allow nuclear motion and electronic dynamics to be studied on an attosecond time scale.

  18. Kikuchi ultrafast nanodiffraction in four-dimensional electron microscopy.

    PubMed

    Yurtsever, Aycan; Zewail, Ahmed H

    2011-02-22

    Coherent atomic motions in materials can be revealed using time-resolved X-ray and electron Bragg diffraction. Because of the size of the beam used, typically on the micron scale, the detection of nanoscale propagating waves in extended structures hitherto has not been reported. For elastic waves of complex motions, Bragg intensities contain all polarizations and they are not straightforward to disentangle. Here, we introduce Kikuchi diffraction dynamics, using convergent-beam geometry in an ultrafast electron microscope, to selectively probe propagating transverse elastic waves with nanoscale resolution. It is shown that Kikuchi band shifts, which are sensitive only to the tilting of atomic planes, reveal the resonance oscillations, unit cell angular amplitudes, and the polarization directions. For silicon, the observed wave packet temporal envelope (resonance frequency of 33 GHz), the out-of-phase temporal behavior of Kikuchi's edges, and the magnitude of angular amplitude (0.3 mrad) and polarization elucidate the nature of the motion: one that preserves the mass density (i.e., no compression or expansion) but leads to sliding of planes in the antisymmetric shear eigenmode of the elastic waveguide. As such, the method of Kikuchi diffraction dynamics, which is unique to electron imaging, can be used to characterize the atomic motions of propagating waves and their interactions with interfaces, defects, and grain boundaries at the nanoscale. PMID:21245348

  19. Ultrafast Structural Dynamics of Tertiary Amines upon Electronic Excitation

    NASA Astrophysics Data System (ADS)

    Cheng, Xinxin; Minitti, Michael P.; Deb, Sanghamitra; Zhang, Yao; Budarz, James; Weber, Peter M.

    2011-06-01

    The structural response of several tertiary amines to electronic excitation has been investigated using Rydberg Fingerprint Spectroscopy. The 3p Rydberg states are reached by excitation with a 5.93 eV photon while 3s states are populated by electronic relaxation from 3p state. We observe binding energy shifts on ultrafast time scales in all peaks that reflect the structural change of the molecular ion cores. The shifts are in the range of 15 meV to 30 meV, within time scales of less than 500 fs, depending on the specific molecular systems and the nature of the electronic state. In cases where the p states are spectrally separate, the trends of the energy shifts are different for the p_z and p_x_y Rydberg states whereas the p_z and s states are similar. This suggests that the response of the Rydberg states to structural displacements depends on the symmetry. Very fast binding energy shifts, observed on sub-picosecond time scales, are attributed to the structural adjustment from a pyramidal to a planar structure upon Rydberg excitation. The quantitative values of the binding energy shifts can also be affected by laser chirp, which we model using simulations.

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

    PubMed Central

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

    2015-01-01

    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. PMID:25672762

  1. Ultrafast electron optics: Propagation dynamics of femtosecond electron packets

    NASA Astrophysics Data System (ADS)

    Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E.; Miller, R. J. Dwayne

    2002-08-01

    Time-resolved electron diffraction harbors great promise for resolving the fastest chemical processes with atomic level detail. The main obstacles to achieving this real-time view of a chemical reaction are associated with delivering short electron pulses with sufficient electron density to the sample. In this article, the propagation dynamics of femtosecond electron packets in the drift region of a photoelectron gun are investigated with an N-body numerical simulation and mean-field model. It is found that space-charge effects can broaden the electron pulse to many times its original length and generate many eV of kinetic energy bandwidth in only a few nanoseconds. There is excellent agreement between the N-body simulation and the mean-field model for both space-charge induced temporal and kinetic energy distribution broadening. The numerical simulation also shows that the redistribution of electrons inside the packet results in changes to the pulse envelope and the development of a spatially linear axial velocity distribution. These results are important for (or have the potential to impact on) the interpretation of time-resolved electron diffraction experiments and can be used in the design of photoelectron guns and streak tubes with temporal resolution of several hundred femtoseconds.

  2. Attosecond electron emission probes of ultrafast nanolocalized fields

    NASA Astrophysics Data System (ADS)

    Kling, Matthias

    2011-05-01

    Ongoing experimental and theoretical work on the temporal and spatial characterization of nanolocalized plasmonic fields will be presented. Because of their broad spectral bandwidth, plasmons in metal nanoparticles undergo ultrafast dynamics with timescales as short as a few hundred attoseconds. So far, the spatiotemporal dynamics of optical fields localized on the nanoscale has been hidden from direct access in the real space and time domain. Our ultimate goal is to characterize the nanoplasmonic fields not only on a nanometer spatial scale but also on ~100 attosecond temporal scale. Information about the nanoplasmonic fields, which are excited by few-cycle laser pulses with stable electric field waveform, can be obtained by the measurement of photoemitted electrons. We will present recent results on the large acceleration of recollision electrons in nanolocalized fields near dielectric nanoparticles following the excitation by 5-fs near-infrared laser pulses with controlled electric field waveforms. This work has been carried out in collaboration with Th. Fennel (University of Rostock), E. Ruehl (FU Berlin), and M.I. Stockman (GSU Atlanta). We acknowledge support by the DFG via Emmy-Noether program and SPP1391.

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

    PubMed

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

    2016-08-10

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

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

    NASA Astrophysics Data System (ADS)

    Filippetto, D.; Qian, H.

    2016-05-01

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

  5. Effects of 3d and 4d transition metal substitutional impurities on the electronic properties of CrO2

    NASA Astrophysics Data System (ADS)

    Williams, M. E.; Sims, H.; Mazumdar, D.; Butler, W. H.

    2012-12-01

    We present first-principles-based density functional theory calculations of the electronic and magnetic structure of CrO2 with 3d and 4d substitutional impurities. We find that the half-metallicity of CrO2 remains intact for the ground state of all of the calculated substitutions. We also observe two periodic trends as a function of the number of valence electrons: if the substituted atom has six or fewer valence electrons, the number of down spin electrons associated with the impurity ion is zero, resulting in ferromagnetic alignment of the impurity magnetic moment with the magnetization of the CrO2 host. For substituent atoms with eight to ten valence electrons (with the exception of Ni), the number of down-spin electrons contributed by the impurity ion remains fixed at three as the number contributed to the majority increases from one to three resulting in antiferromagnetic alignment between impurity moment and host magnetization. In impurities with seven valence electrons, the zero down-spin and threse down-spin configurations are very close in energy. At 11 valence electrons, the energy is minimized when the substituent ion contributes five down-spin electrons. The moments on the 4d impurities, particularly Nb and Mo, tend to be delocalized compared with those of the 3ds.

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

    PubMed Central

    Principi, E.; Giangrisostomi, E.; Cucini, R.; Bencivenga, F.; Battistoni, A.; Gessini, A.; Mincigrucci, R.; Saito, M.; Di Fonzo, S.; D'Amico, F.; Di Cicco, A.; Gunnella, R.; Filipponi, A.; Giglia, A.; Nannarone, S.; Masciovecchio, C.

    2015-01-01

    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. PMID:26798835

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

    SciTech Connect

    Dixit, Gopal; Santra, Robin

    2013-04-07

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

  8. Quantum effects in ultrafast electron transfers within cryptochromes.

    PubMed

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

    2016-08-21

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

  9. Probing the ultrafast electron transfer at the CuPc/Au(111) interface

    SciTech Connect

    Chen Wei; Wang Li; Qi Dongchen; Chen Shi; Gao Xingyu; Wee, Andrew Thye Shen

    2006-05-01

    Core-hole clock spectroscopy and near-edge x-ray-absorption fine structure measurements have been used to investigate the ultrafast electron transfer dynamics at the Copper(II) phthalocyanine (CuPc)/Au(111) interface. It was found that the strong electronic coupling between the first layer of CuPc molecules and Au(111) substrate favors ultrafast electron transfer from the lowest unoccupied molecular orbital of the CuPc molecules to the conduction band of Au(111) in the time scale of {approx}6 fs. In contrast, the intermolecular electron transfer within multilayers of CuPc molecules via the weak van der Waals interaction was much slower.

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

    SciTech Connect

    Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha Ropers, Claus

    2015-11-07

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

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

    NASA Astrophysics Data System (ADS)

    Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha; Ropers, Claus

    2015-11-01

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

  12. Ultrafast electron microscopy and diffraction with laser-driven field emitters

    NASA Astrophysics Data System (ADS)

    Ropers, Claus

    2015-03-01

    Ultrafast structural dynamics in solids and nanostructures can be investigated by an increasing number of sophisticated electron and x-ray diffraction techniques. Electrons are particularly suited for this purpose, exhibiting high scattering cross-sections and allowing for beam control by versatile electrostatic or magnetic lens systems. The capabilities of time-resolved electron imaging techniques critically depend on the employed source of laser-driven ultrashort electron pulses. Nanoscopic sources offer exceptional possibilities for the generation of electron probe pulses with very short durations and high spatial beam coherence. In this talk, I will discuss recent progress in the development of ultrafast electron microscopy and diffraction based on nanoscopic photocathodes. In particular, we implemented ultrafast low-energy electron diffraction (ULEED) and ultrafast transmission electron microscopy (UTEM) driven by nonlinear photoemission from field emission tips. ULEED enables the study of structural changes with high temporal resolution and ultimate surface sensitivity, at sub-keV electron energies. As a first application of this technique, we studied the structural phase transition in a stripe-like polymer superstructure on freestanding monolayer graphene. An advanced UTEM instrument was realized by custom modifications of a standard transmission electron microscope, leading to electron focal spot sizes in the microscope's sample plane of about 10 nm and electron pulse durations of less than 700 fs. Utilizing these features, we investigate the quantum-coherent interaction between the ultrashort electron pulse and the optical near-field of an illuminated nanostructure. Finally, further applications and prospects of ultrafast electron imaging, diffraction and spectroscopy using nanoscale field emitters will be discussed.

  13. 4d electron Ruthenate systems: their unique and new magnetic properties

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed Central

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

    2013-01-01

    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. PMID:23690572

  15. Laser-induced short-range disorder in aluminum revealed by ultrafast electron diffuse scattering

    SciTech Connect

    Zhu, Pengfei; Chen, Jie; Li, Runze; Chen, Long; Cao, Jianming; Sheng, Zhengming; Zhang, Jie

    2013-12-02

    We report ultrafast electron diffuse scattering intensity (DSI) measurement in order to study the structural response of aluminum to femtosecond laser excitation. In this measurement, the evolutions of DSI and Bragg peak intensities after the laser excitation are measured and compared in the time domain. Their differences suggest that two kinds of lattice disorder, short-range and long-range, are triggered simultaneously. The former, induced by electron excitation, arises and decays with a faster rate than the latter which is subject to lattice heating. The results presented show that the time-resolved DSI measurements provide complementary insights to the ultrafast diffraction measurements.

  16. Imaging of alignment and structural changes of carbon disulfide molecules using ultrafast electron diffraction.

    PubMed

    Yang, Jie; Beck, Joshua; Uiterwaal, Cornelis J; Centurion, Martin

    2015-01-01

    Imaging the structure of molecules in transient-excited states remains a challenge due to the extreme requirements for spatial and temporal resolution. Ultrafast electron diffraction from aligned molecules provides atomic resolution and allows for the retrieval of structural information without the need to rely on theoretical models. Here we use ultrafast electron diffraction from aligned molecules and femtosecond laser mass spectrometry to investigate the dynamics in carbon disulfide following the interaction with an intense femtosecond laser pulse. We observe that the degree of alignment reaches an upper limit at laser intensities below the ionization threshold, and find evidence of structural deformation, dissociation and ionization at higher laser intensities. PMID:26337631

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

    NASA Astrophysics Data System (ADS)

    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.

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

    SciTech Connect

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

    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.

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

    NASA Astrophysics Data System (ADS)

    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.

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

    NASA Astrophysics Data System (ADS)

    Suzuki, Toshinori

    2014-06-01

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

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

    SciTech Connect

    Quevedo, W.; Busse, G.; Hallmann, J.; More, R.; Petri, M.; Rajkovic, I.; Krasniqi, F.; Rudenko, A.; Tschentscher, T.; Stojanovic, N.; Duesterer, S.; Treusch, R.; Tolkiehn, M.; Techert, S.

    2012-11-01

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

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

    PubMed

    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. PMID:25972103

  3. Ultrafast static and diffusion-controlled electron transfer at Ag29 nanocluster/molecular acceptor interfaces.

    PubMed

    Aly, Shawkat M; AbdulHalim, Lina G; Besong, Tabot M D; Soldan, Giada; Bakr, Osman M; Mohammed, Omar F

    2016-03-14

    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 (MV(2+)) 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. PMID:26548942

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

    NASA Astrophysics Data System (ADS)

    Qiu, Weihong; Li, Tanping; Zhang, Luyuan; Yang, Yi; Kao, Ya-Ting; Wang, Lijuan; Zhong, Dongping

    2008-06-01

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

  5. Discrete Chromatic Aberrations Arising from Photoinduced Electron-Photon Interactions in Ultrafast Electron Microscopy.

    PubMed

    Plemmons, Dayne A; Flannigan, David J

    2016-05-26

    In femtosecond ultrafast electron microscopy (UEM) experiments, the initial excitation period is composed of spatiotemporal overlap of the temporally commensurate pump photon pulse and probe photoelectron packet. Generation of evanescent near-fields at the nanostructure specimens produces a dispersion relation that enables coupling of the photons (ℏω = 2.4 eV, for example) and freely propagating electrons (200 keV, for example) in the near-field. Typically, this manifests as discrete peaks occurring at integer multiples (n) of the photon energy in the low-loss/gain region of electron-energy spectra (i.e., at 200 keV ± nℏω eV). Here, we examine the UEM imaging resolution implications of the strong inelastic near-field interactions between the photons employed in optical excitation and the probe photoelectrons. We find that the additional photoinduced energy dispersion occurring when swift electrons pass through intense evanescent near-fields results in a discrete chromatic aberration that limits the spatial resolving power to several angstroms during the excitation period. PMID:27111530

  6. Simultaneous observation of ultrafast structural dynamics and transient electrical field by picosecond electron pulses

    NASA Astrophysics Data System (ADS)

    Li, Run-Ze; Zhu, Pengfei; Chen, Long; Chen, Jie; Cao, Jianming; Sheng, Zheng-Ming; Zhang, Jie

    2014-03-01

    Ultrafast electron diffraction and microscopy are very promising methods to study transient structural dynamics with atomic spatial-temporal resolution. However, in these laser-pump electron-probe studies of structural dynamics, a transient electric field induced by laser excitation of the sample could deflect probing electrons, which may eventually leads to a misinterpretation of the diffraction data. Here, picosecond structural dynamics and transient surface electric field evolution, excited by femtosecond laser interaction with a metallic thin film, have been observed simultaneously in real time by ultrashort electron pulses in a transmission configuration. By tracing time dependent changes of electron diffraction and deflection angles, these two processes are found to be significantly different and distinguishable in their temporal behavior. This observation provides an effective approach to extract the otherwise obscured ultrafast structural dynamics and may help to improve the spatiotemporal resolution in ultrafast electron diffraction and microscopy studies. This work was supported by the National Basic Research Program of China and the National Natural Science Foundation of China.

  7. Experimental demonstration of high quality MeV ultrafast electron diffraction.

    PubMed

    Li, Renkai; Tang, Chuanxiang; Du, Yingchao; Huang, Wenhui; Du, Qiang; Shi, Jiaru; Yan, Lixin; Wang, Xijie

    2009-08-01

    The simulation optimization and an experimental demonstration of improved performances of mega-electron-volt ultrafast electron diffraction (MeV UED) are reported in this paper. Using ultrashort high quality electron pulses from an S-band photocathode rf gun and a polycrystalline aluminum foil as the sample, we experimentally demonstrated an improved spatial resolution of MeV UED, in which the Debye-Scherrer rings of the (111) and (200) planes were clearly resolved. This result showed that MeV UED is capable to achieve an atomic level spatial resolution and a approximately 100 fs temporal resolution simultaneously, and will be a unique tool for ultrafast structural dynamics studies. PMID:19725647

  8. Quantum coherent optical phase modulation in an ultrafast transmission electron microscope

    NASA Astrophysics Data System (ADS)

    Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob; Yalunin, Sergey V.; Schäfer, Sascha; Ropers, Claus

    2015-05-01

    Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven `quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

  9. Dynamics of ultrafast photoinduced heterogeneous electron transfer, implications for recent solar energy conversion scenarios

    NASA Astrophysics Data System (ADS)

    Gundlach, Lars; Burfeindt, Bernd; Mahrt, Jürgen; Willig, Frank

    2012-08-01

    The general case of a heterogeneous electron transfer reaction is realized by ultrafast electron transfer from a photo-excited molecule to a wide continuum of electronic acceptor states. Two different theoretical model calculations addressing the injection dynamics have recently been presented. The first scenario predicts a wide energy distribution for the injected electron via excitations of high-energy vibrational modes in the ionized molecule, whereas the second scenario ascribes the width to thermal fluctuations. We present experimental data at different temperatures and identify the valid injection scenario for perylene/TiO2 systems. The results are discussed in view of recent solar energy conversion scenarios.

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

    NASA Astrophysics Data System (ADS)

    Okhrimenko, Albert N.

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

  11. Tuning ultrafast electron thermalization pathways in a van der Waals heterostructure

    NASA Astrophysics Data System (ADS)

    Ma, Qiong; Andersen, Trond I.; Nair, Nityan L.; Gabor, Nathaniel M.; Massicotte, Mathieu; Lui, Chun Hung; Young, Andrea F.; Fang, Wenjing; Watanabe, Kenji; Taniguchi, Takashi; Kong, Jing; Gedik, Nuh; Koppens, Frank H. L.; Jarillo-Herrero, Pablo

    2016-05-01

    Ultrafast electron thermalization--the process leading to carrier multiplication via impact ionization, and hot-carrier luminescence--occurs when optically excited electrons in a material undergo rapid electron-electron scattering to redistribute excess energy and reach electronic thermal equilibrium. Owing to extremely short time and length scales, the measurement and manipulation of electron thermalization in nanoscale devices remains challenging even with the most advanced ultrafast laser techniques. Here, we overcome this challenge by leveraging the atomic thinness of two-dimensional van der Waals (vdW) materials to introduce a highly tunable electron transfer pathway that directly competes with electron thermalization. We realize this scheme in a graphene-boron nitride-graphene (G-BN-G) vdW heterostructure, through which optically excited carriers are transported from one graphene layer to the other. By applying an interlayer bias voltage or varying the excitation photon energy, interlayer carrier transport can be controlled to occur faster or slower than the intralayer scattering events, thus effectively tuning the electron thermalization pathways in graphene. Our findings, which demonstrate a means to probe and directly modulate electron energy transport in nanoscale materials, represent a step towards designing and implementing optoelectronic and energy-harvesting devices with tailored microscopic properties.

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

    PubMed

    Sun, Jingya; Melnikov, Vasily A; Khan, Jafar I; Mohammed, Omar F

    2015-10-01

    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. PMID:26722888

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

    PubMed

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

    2015-10-01

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

  14. Ultrafast electron crystallography: transient structures of molecules, surfaces, and phase transitions.

    PubMed

    Ruan, Chong-Yu; Vigliotti, Franco; Lobastov, Vladimir A; Chen, Songye; Zewail, Ahmed H

    2004-02-01

    The static structure of macromolecular assemblies can be mapped out with atomic-scale resolution by using electron diffraction and microscopy of crystals. For transient nonequilibrium structures, which are critical to the understanding of dynamics and mechanisms, both spatial and temporal resolutions are required; the shortest scales of length (0.1-1 nm) and time (10(-13) to 10(-12) s) represent the quantum limit, the nonstatistical regime of rates. Here, we report the development of ultrafast electron crystallography for direct determination of structures with submonolayer sensitivity. In these experiments, we use crystalline silicon as a template for different adsorbates: hydrogen, chlorine, and trifluoroiodomethane. We observe the coherent restructuring of the surface layers with subangstrom displacement of atoms after the ultrafast heat impulse. This nonequilibrium dynamics, which is monitored in steps of 2 ps (total change ultrafast electron crystallography tabletop methodology. PMID:14745037

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

    PubMed

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

    2016-05-01

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

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

    NASA Astrophysics Data System (ADS)

    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.

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

    NASA Astrophysics Data System (ADS)

    Herink, Georg; Ropers, Claus

    2015-09-01

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

  18. Ultrafast Carrier Dynamics and Hot Electron Extraction in Tetrapod-Shaped CdSe Nanocrystals.

    PubMed

    Jing, Pengtao; Ji, Wenyu; Yuan, Xi; Qu, Songnan; Xie, Renguo; Ikezawa, Michio; Zhao, Jialong; Li, Haibo; Masumoto, Yasuaki

    2015-04-22

    The ultrafast carrier dynamics and hot electron extraction in tetrapod-shaped CdSe nanocrystals was studied by femtosecond transient absorption (TA) spectroscopy. The carriers relaxation process from the higher electronic states (CB2, CB3(2), and CB4) to the lowest electronic state (CB1) was demonstrated to have a time constant of 1.04 ps, resulting from the spatial electron transfer from arms to a core. The lowest electronic state in the central core exhibited a long decay time of 5.07 ns in agreement with the reported theoretical calculation. The state filling mechanism and Coulomb blockade effect in the CdSe tetrapod were clearly observed in the pump-fluence-dependent transient absorption spectra. Hot electrons were transferred from arm states into the electron acceptor molecules before relaxation into core states. PMID:25838148

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

    NASA Astrophysics Data System (ADS)

    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.

  20. Ultrafast Electron Transfer in Photosynthesis: Reduced Pheophytin and Quinone Interaction Mediated by Conical Intersections

    NASA Astrophysics Data System (ADS)

    Olaso-González, Gloria; Merchán, Manuela; Serrano-Andrés, Luis

    2007-12-01

    The mechanism of electron transfer (ET) from reduced pheophytin (Pheo-) to the primary stable photosynthetic acceptor, a quinone (Q) molecule, is addressed by using high-level ab initio computations and realistic molecular models. The results reveal that the ET process involving the (Pheo-+Q) and (Pheo+Q-) oxidation states can be essentially seen as an ultrafast radiationless transition between the two hypersurfaces taking place via conical intersections (CIs) and it is favoured when the topology of the interacting moieties make possible some overlap between the lowest occupied molecular orbitals (LUMO) of the two systems. Thus, it is anticipated that large scale motions, which are difficult to monitor experimentally, may actually occur in the photosynthetic reaction centers of bacteria, algae, and higher plants, to fulfil the observed ultrafast ET processes.

  1. Laser Alignment as a Route to Ultrafast Control of Electron Transport through Junctions

    SciTech Connect

    Reuter, Matthew G; Ratner, Mark A.; Seideman, Tamar

    2012-01-01

    We consider the extension of ultrafast laser alignment schemes to surface-adsorbed molecules, where the laser field coerces the molecule to reorient itself relative to the surface. When probed by a scanning tunneling microscope tip, this reorientation modifies the tip-molecule distance, and thus the tunneling current, suggesting a route to an ultrafast, nanoscale current switch. In addition to exploring the controllability of adsorbed molecules by moderately intense laser fields and discussing the fundamental differences of alignment behavior between surface-adsorbed molecules and gas phase molecules, we computationally investigate the quality of orientation with respect to field intensity, field duration, and the location of the tip. Overall, the molecule moves directly to its oriented configuration, which is reasonably insensitive to the tip location. These results collectively suggest the efficacy of using laser alignment schemes to control electron transport through junctions.

  2. Characterization of fast photoelectron packets in weak and strong laser fields in ultrafast electron microscopy.

    PubMed

    Plemmons, Dayne A; Tae Park, Sang; Zewail, Ahmed H; Flannigan, David J

    2014-11-01

    The development of ultrafast electron microscopy (UEM) and variants thereof (e.g., photon-induced near-field electron microscopy, PINEM) has made it possible to image atomic-scale dynamics on the femtosecond timescale. Accessing the femtosecond regime with UEM currently relies on the generation of photoelectrons with an ultrafast laser pulse and operation in a stroboscopic pump-probe fashion. With this approach, temporal resolution is limited mainly by the durations of the pump laser pulse and probe electron packet. The ability to accurately determine the duration of the electron packets, and thus the instrument response function, is critically important for interpretation of dynamics occurring near the temporal resolution limit, in addition to quantifying the effects of the imaging mode. Here, we describe a technique for in situ characterization of ultrashort electron packets that makes use of coupling with photons in the evanescent near-field of the specimen. We show that within the weakly-interacting (i.e., low laser fluence) regime, the zero-loss peak temporal cross-section is precisely the convolution of electron packet and photon pulse profiles. Beyond this regime, we outline the effects of non-linear processes and show that temporal cross-sections of high-order peaks explicitly reveal the electron packet profile, while use of the zero-loss peak becomes increasingly unreliable. PMID:25151361

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

    NASA Astrophysics Data System (ADS)

    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.

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

    SciTech Connect

    Ge, Nien-Hui

    1998-10-01

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

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

    SciTech Connect

    Szekely, Joshua E.; Seideman, Tamar

    2014-07-28

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

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

    NASA Astrophysics Data System (ADS)

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

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

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

    PubMed

    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. PMID:27226978

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

    PubMed Central

    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 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. PMID:27226978

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

    PubMed Central

    van der Veen, Renske M.; Penfold, Thomas J.; Zewail, Ahmed H.

    2015-01-01

    We demonstrate ultrafast core-electron energy-loss spectroscopy in four-dimensional electron microscopy as an element-specific probe of nanoscale dynamics. We apply it to the study of photoexcited graphite with femtosecond and nanosecond resolutions. The transient core-loss spectra, in combination with ab initio molecular dynamics simulations, reveal the elongation of the carbon-carbon bonds, even though the overall behavior is a contraction of the crystal lattice. A prompt energy-gap shrinkage is observed on the picosecond time scale, which is caused by local bond length elongation and the direct renormalization of band energies due to temperature-dependent electron–phonon interactions. PMID:26798793

  10. Ultrafast electronic readout of diamond nitrogen-vacancy centres coupled to graphene.

    PubMed

    Brenneis, Andreas; Gaudreau, Louis; Seifert, Max; Karl, Helmut; Brandt, Martin S; Huebl, Hans; Garrido, Jose A; Koppens, Frank H L; Holleitner, Alexander W

    2015-02-01

    Non-radiative transfer processes are often regarded as loss channels for an optical emitter because they are inherently difficult to access experimentally. Recently, it has been shown that emitters, such as fluorophores and nitrogen-vacancy centres in diamond, can exhibit a strong non-radiative energy transfer to graphene. So far, the energy of the transferred electronic excitations has been considered to be lost within the electron bath of the graphene. Here we demonstrate that the transferred excitations can be read out by detecting corresponding currents with a picosecond time resolution. We detect electronically the spin of nitrogen-vacancy centres in diamond and control the non-radiative transfer to graphene by electron spin resonance. Our results open the avenue for incorporating nitrogen-vacancy centres into ultrafast electronic circuits and for harvesting non-radiative transfer processes electronically. PMID:25437746

  11. Electronically induced structure transformations in graphite & silver, studied using ultrafast electron crystallography

    NASA Astrophysics Data System (ADS)

    Raman, Ramani K.

    Electronically induced structure transformations are a unique class of phenomena in which material transformation can be effected by impulsive excitation of the electronic system, often resulting in exotic structural phases and transformation pathways inaccessible to thermodynamic channels. Using ultrafast electron crystallography (UEC), we have directly observed such photodinduced atomic dynamics in two systems - graphite and silver nanocrystals (Ag NC) that appear to be driven by the strong coupling between the laser excitation and lattice perturbations in the form of strongly coupled optical phonons and laser induced electron redistribution. In graphite, structural changes resulting from photoexcitation with p-polarized, near-IR, femtosecond laser pulses are observed to lead to the nonthermal creation of a transient state with sp3 like bonding characteristics. At laser fluences approaching, but below the damage threshold, the average inter-layer spacing contracts along with creation of new inter-layer distances at ≈ 2 A while the lattice is only moderately heated. The advantage of using electrons (which carry a charge) as a probe is demonstrated, as it reveals the transformation to be driven by a hitherto unobserved surface dipole field, observed here via a Coulomb refraction shift of the scattered electrons within the sub-surface region. Ab initio density functional theory calculations are employed to relate these structural changes to a nonthermal heating of the electrons, followed by a photoinduced charge separation causing a compressive Coulomb stress. To quantify the role and dynamics of electrons emitted from photoexcited surfaces, a novel 'point-projection method' is introduced, capable of directly imaging the spatiotemporal evolution of such photoemitted electron bunches. The method is shown to provide sufficient sensitivity to image electron bunches (as small as 1010 e/cm3) and permit quantitative investigation of the electron emission from

  12. Quantum coherent optical phase modulation in an ultrafast transmission electron microscope.

    PubMed

    Feist, Armin; Echternkamp, Katharina E; Schauss, Jakob; Yalunin, Sergey V; Schäfer, Sascha; Ropers, Claus

    2015-05-14

    Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven 'quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers. PMID:25971512

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

    PubMed

    Masih, Dilshad; Aly, Shawkat M; Usman, Anwar; Alarousu, Erkki; Mohammed, Omar F

    2015-04-14

    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 π-π 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. PMID:25751714

  14. Photoinduced phase transitions in vanadium dioxide revealed by ultrafast electron diffraction and mid-infrared spectroscopy

    NASA Astrophysics Data System (ADS)

    Tiwari, Kunal; Morrison, Vance; Chatelain, Robert; Hendaoui, Ali; Bruhacs, Andrew; Chaker, Mohamed; Siwick, Bradley

    2015-03-01

    The complex interplay between strong electron-electron correlations and structural distortions is thought to determine the electronic properties of many oxides, but the respective role of these two contributions is often difficult to determine. We report combined radio-frequency compressed ultrafast electron diffraction (RF-UED) and infrared transmissivity experiments in which we directly monitor and separate the lattice and charge density reorganizations associated with the optically induced semiconductor-to-metal phase transition in vanadium dioxide. These studies have uncovered a previously unreported photoinduced transition to a metastable phase retaining the periodic lattice distortion characteristic of the insulating phase, but differing by a reorganization of charge density along the vanadium dimer chains and a transition to metal-like mid IR optical properties. These results demonstrate that UED is able to follow details of both lattice and electronic structural dynamics on the ultrafast timescale. Supported by Natural Sciences and Engineering Research Council of Canada, the Canada Foundation for Innovation, the Canada Research Chairs program, NSERC PGS-D and CGS-D fellowships, and Fonds de Récherche du Québec-Nature et Technologies.

  15. Imaging of isolated molecules with ultrafast electron pulses.

    PubMed

    Hensley, Christopher J; Yang, Jie; Centurion, Martin

    2012-09-28

    Imaging isolated molecules in three dimensions with atomic resolution is important for elucidating complex molecular structures and intermediate states in molecular dynamics. This goal has so far remained elusive due to the random orientation of molecules in the gas phase. We show that three-dimensional structural information can be retrieved from multiple electron diffraction patterns of aligned molecules. The molecules are aligned impulsively with a femtosecond laser pulse and probed with a femtosecond electron pulse two picoseconds later, when the degree of alignment reaches a maximum. PMID:23030087

  16. Ultrafast Diagnostics for Electron Beams from Laser Plasma Accelerators

    SciTech Connect

    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.

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

    NASA Astrophysics Data System (ADS)

    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

  18. Ultrafast electron transfer via a bridge-extended donor orbital

    NASA Astrophysics Data System (ADS)

    Ernstorfer, R.; Gundlach, L.; Felber, S.; Storck, W.; Eichberger, R.; Zimmermann, C.; Willig, F.

    Electron transfer from the excited aromatic donor perylene to TiO2 occurred with 10 fs time constant via the conjugated -CH=CH- bridge unit compared to 57 fs in the presence of the saturated -CH2-CH2- bridge unit.

  19. DC photoelectron gun parameters for ultrafast electron microscopy.

    PubMed

    Berger, Joel A; Hogan, John T; Greco, Michael J; Schroeder, W Andreas; Nicholls, Alan W; Browning, Nigel D

    2009-08-01

    We present a characterization of the performance of an ultrashort laser pulse driven DC photoelectron gun based on the thermionic emission gun design of Togawa et al. [Togawa, K., Shintake, T., Inagaki, T., Onoe, K. & Tanaka, T. (2007). Phys Rev Spec Top-AC 10, 020703]. The gun design intrinsically provides adequate optical access and accommodates the generation of approximately 1 mm2 electron beams while contributing negligible divergent effects at the anode aperture. Both single-photon (with up to 20,000 electrons/pulse) and two-photon photoemission are observed from Ta and Cu(100) photocathodes driven by the harmonics (approximately 4 ps pulses at 261 nm and approximately 200 fs pulses at 532 nm, respectively) of a high-power femtosecond Yb:KGW laser. The results, including the dependence of the photoemission efficiency on the polarization state of the drive laser radiation, are consistent with expectations. The implications of these observations and other physical limitations for the development of a dynamic transmission electron microscope with sub-1 nm.ps space-time resolution are discussed. PMID:19575831

  20. A compact streak camera for 150 fs time resolved measurement of bright pulses in ultrafast electron diffraction.

    PubMed

    Kassier, G H; Haupt, K; Erasmus, N; Rohwer, E G; von Bergmann, H M; Schwoerer, H; Coelho, S M M; Auret, F D

    2010-10-01

    We have developed a compact streak camera suitable for measuring the duration of highly charged subrelativistic femtosecond electron bunches with an energy bandwidth in the order of 0.1%, as frequently used in ultrafast electron diffraction (UED) experiments for the investigation of ultrafast structural dynamics. The device operates in accumulation mode with 50 fs shot-to-shot timing jitter, and at a 30 keV electron energy, the full width at half maximum temporal resolution is 150 fs. Measured durations of pulses from our UED gun agree well with the predictions from the detailed charged particle trajectory simulations. PMID:21034115

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

    NASA Astrophysics Data System (ADS)

    Essert, Sven; Schneider, Hans Christian

    2011-12-01

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

  2. Ultrafast electron trapping in ligand-exchanged quantum dot assemblies.

    PubMed

    Turk, Michael E; Vora, Patrick M; Fafarman, Aaron T; Diroll, Benjamin T; Murray, Christopher B; Kagan, Cherie R; Kikkawa, James M

    2015-02-24

    We use time-integrated and time-resolved photoluminescence and absorption to characterize the low-temperature optical properties of CdSe quantum dot solids after exchanging native aliphatic ligands for thiocyanate and subsequent thermal annealing. In contrast to trends established at room temperature, our data show that at low temperature the band-edge absorptive bleach is dominated by 1S3/2h hole occupation in the quantum dot interior. We find that our ligand treatments, which bring enhanced interparticle coupling, lead to faster surface state electron trapping, a greater proportion of surface-related photoluminescence, and decreased band-edge photoluminescence lifetimes. PMID:25635923

  3. Ultrafast molecular imaging by laser-induced electron diffraction

    SciTech Connect

    Peters, M.; Nguyen-Dang, T. T.; Cornaggia, C.; Saugout, S.; Charron, E.; Keller, A.; Atabek, O.

    2011-05-15

    We address the feasibility of imaging geometric and orbital structures of a polyatomic molecule on an attosecond time scale using the laser-induced electron diffraction (LIED) technique. We present numerical results for the highest molecular orbitals of the CO{sub 2} molecule excited by a near-infrared few-cycle laser pulse. 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 XUV spectroscopy: Unveiling the nature of electronic couplings in molecular dynamics

    NASA Astrophysics Data System (ADS)

    Timmers, Henry Robert

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

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

    PubMed

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

    2015-09-01

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

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

    PubMed Central

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

    2015-01-01

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

  8. Ultrafast Electron Diffraction Tomography for Structure Determination of the New Zeolite ITQ-58.

    PubMed

    Simancas, Jorge; Simancas, Raquel; Bereciartua, Pablo J; Jorda, Jose L; Rey, Fernando; Corma, Avelino; Nicolopoulos, Stavros; Pratim Das, Partha; Gemmi, Mauro; Mugnaioli, Enrico

    2016-08-17

    In this work a new ultrafast data collection strategy for electron diffraction tomography is presented that allows reducing data acquisition time by one order of magnitude. This methodology minimizes the radiation damage of beam-sensitive materials, such as microporous materials. This method, combined with the precession of the electron beam, provides high quality data enabling the determination of very complex structures. Most importantly, the implementation of this new electron diffraction methodology is easily affordable in any modern electron microscope. As a proof of concept, we have solved a new highly complex zeolitic structure named ITQ-58, with a very low symmetry (triclinic) and a large unit cell volume (1874.6 Å(3)), containing 16 silicon and 32 oxygen atoms in its asymmetric unit, which would be very difficult to solve with the state of the art techniques. PMID:27478889

  9. Ablation of GaAs by Intense, Ultrafast Electronic Excitation from Highly Charged Ions

    SciTech Connect

    Schenkel, T.; Hamza, A.V.; Barnes, A.V.; Schneider, D.H.; Banks, J.C.; Doyle, B.L.

    1998-09-01

    We have measured total ablation rates and secondary ion yields from undoped GaAs(100) interacting with slow (v=6.6{times}10{sup 5} m /s) , very highly charged ions. Ablation rates increase strongly as a function of projectile charge. Some 1400thinspthinsptarget atoms are removed when a single Th{sup 70+} ion deposits a potential energy of 152.6thinspthinspkeV within a few femtoseconds into a nanometer-sized target volume. We discuss models for ablation of semiconductors by intense, ultrafast electronic excitation. {copyright} {ital 1998} {ital The American Physical Society}

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

    SciTech Connect

    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.

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

    NASA Astrophysics Data System (ADS)

    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

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

    PubMed

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

    2012-11-01

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

  13. Optical Probing of Ultrafast Electronic Decay in Bi and Sb with Slow Phonons

    NASA Astrophysics Data System (ADS)

    Li, J. J.; Chen, J.; Reis, D. A.; Fahy, S.; Merlin, R.

    2013-01-01

    Illumination with laser sources leads to the creation of excited electronic states of particular symmetries, which can drive isosymmetric vibrations. Here, we use a combination of ultrafast stimulated and cw spontaneous Raman scattering to determine the lifetime of A1g and Eg electronic coherences in Bi and Sb. Our results both shed new light on the mechanisms of coherent phonon generation and represent a novel way to probe extremely fast electron decoherence rates. The Eg state, resulting from an unequal distribution of carriers in three equivalent band regions, is extremely short lived. Consistent with theory, the lifetime of its associated driving force reaches values as small as 2 (6) fs for Bi (Sb) at 300 K.

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

    SciTech Connect

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

    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.

  15. Effect of donor orientation on ultrafast intermolecular electron transfer in coumarin-amine systems.

    PubMed

    Singh, P K; Nath, S; Bhasikuttan, A C; Kumbhakar, M; Mohanty, J; Sarkar, S K; Mukherjee, T; Pal, H

    2008-09-21

    Effect of donor amine orientation on nondiffusive ultrafast intermolecular electron transfer (ET) reactions in coumarin-amine systems has been investigated using femtosecond fluorescence upconversion measurements. Intermolecular ET from different aromatic and aliphatic amines used as donor solvents to the excited coumarin-151 (C151) acceptor occurs with ultrafast rates such that the shortest fluorescence lifetime component (tau(1)) is the measure of the fastest ET rate (tau(1)=tau(ET) (fast)=(k(ET) (fast))(-1)), assigned to the C151-amine contact pairs in which amine donors are properly oriented with respect to C151 to maximize the acceptor-donor electronic coupling (V(el)). It is interestingly observed that as the amine solvents are diluted by suitable diluents (either keeping solvent dielectric constant similar or with increasing dielectric constant), the tau(1) remains almost in the similar range as long as the amine dilution does not cross a certain critical limit, which in terms of the amine mole fraction (x(A)) is found to be approximately 0.4 for aromatic amines and approximately 0.8 for aliphatic amines. Beyond these dilutions in the two respective cases of the amine systems, the tau(1) values are seen to increase very sharply. The large difference in the critical x(A) values involving aromatic and aliphatic amine donors has been rationalized in terms of the largely different orientational restrictions for the ET reactions as imposed by the aliphatic (n-type) and aromatic (pi-type) nature of the amine donors [A. K. Satpati et al., J. Mol. Struct. 878, 84 (2008)]. Since the highest occupied molecular orbital (HOMO) of the n-type aliphatic amines is mostly centralized at the amino nitrogen, only some specific orientations of these amines with respect to the close-contact acceptor dye [also of pi-character; A. K. Satpati et al., J. Mol. Struct. 878, 84 (2008) and E. W. Castner et al., J. Phys. Chem. A 104, 2869 (2000)] can give suitable V(el) and thus

  16. Ultrafast interfacial electron transfer from the excited state of anchored molecules into a semiconductor

    NASA Astrophysics Data System (ADS)

    Gundlach, L.; Ernstorfer, R.; Willig, F.

    Ultrafast heterogeneous electron transfer (HET) from the excited singlet state of the large organic chromophore perylene into the inorganic semiconductor rutile TiO 2 was investigated with femtosecond time-resolved two-photon photoemission (TR-2PPE). The strength of the electronic interaction between the chromophore and the semiconductor was varied by inserting different anchor/bridge groups that functioned either as electronic wire or electronic tunnelling barrier. Both anchor groups, i.e. carboxylic and phosphonic acid, formed strong chemical bonds at the TiO 2 surface. The perylene chromophore with the different anchor/bridge groups was adsorbed from solution in a dedicated ultra-high-vacuum (UHV) chamber. The adsorption geometry of the chromophore perylene was determined from angle and polarization dependent two-photon photoemission (2PPE) signals and was found to be very different for the two different anchor/bridge groups. The measured adsorption geometries are compatible with recent DFT (density functional theory) calculations by P. Persson and co-workers [M. Nilsing, S. Lunell, P. Persson, L. Ojamäe, Phosphonic acid adsorption at the TiO 2 anatase (1 0 1) surface investigated by periodic hybrid HF-DFT computations, Surf. Sci. 582 (2005) 49-60]. Two different processes contributed to the TR-2PPE transients, firstly electron transfer from the chromophore to the electronic acceptor states on the surface and secondly escape of the electrons from the surface into the bulk of the semiconductor. The latter escape process was measured separately by making the interfacial electron injection process instantaneous when the chromophore catechol was employed in place of the perylene compounds. The thus measured electron escape behavior was governed by the same time constants that have recently been predicted by Prezhdo and coworkers from time dependent DFT calculations [W.R. Duncan, W.M. Stier, O.V. Prezhdo, Ab initio nonadiabatic molecular dynamics of the ultrafast

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

    PubMed

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

    2016-07-28

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  19. Ultrafast Surface-Enhanced Raman Probing of the Role of Hot Electrons in Plasmon-Driven Chemistry.

    PubMed

    Brandt, Nathaniel C; Keller, Emily L; Frontiera, Renee R

    2016-08-18

    Hot electrons generated through plasmonic excitations in metal nanostructures show great promise for efficiently driving chemical reactions with light. However, the lifetime, yield, and mechanism of action of plasmon-generated hot electrons involved in a given photocatalytic process are not well understood. Here, we develop ultrafast surface-enhanced Raman scattering (SERS) as a direct probe of plasmon-molecule interactions in the plasmon-catalyzed dimerization of 4-nitrobenzenethiol to p,p'-dimercaptoazobenzene. Ultrafast SERS probing of these molecular reporters in plasmonic hot spots reveals transient Fano resonances, which we attribute to near-field coupling of Stokes-shifted photons to hot electron-driven metal photoluminescence. Surprisingly, we find that hot spots that yield more photoluminescence are much more likely to drive the reaction, which indirectly proves that plasmon-generated hot electrons induce the photochemistry. These ultrafast SERS results provide insight into the relative reactivity of different plasmonic hot spot environments and quantify the ultrafast lifetime of hot electrons involved in plasmon-driven chemistry. PMID:27488515

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

    SciTech Connect

    Alperovich, Igor; Smolentsev, Grigory; Moonshiram, Dooshaye; Jurss, Jonah W.; Concepcion, Javier J.; Meyer, Thomas J.; Soldatov, Alexander; Pushkar, Yulia

    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.

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

    PubMed

    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. PMID:25215987

  2. Infrared PINEM developed by diffraction in 4D UEM

    PubMed Central

    Liu, Haihua; Baskin, John Spencer; Zewail, Ahmed H.

    2016-01-01

    The development of four-dimensional ultrafast electron microscopy (4D UEM) has enabled not only observations of the ultrafast dynamics of photon–matter interactions at the atomic scale with ultrafast resolution in image, diffraction, and energy space, but photon–electron interactions in the field of nanoplasmonics and nanophotonics also have been captured by the related technique of photon-induced near-field electron microscopy (PINEM) in image and energy space. Here we report a further extension in the ongoing development of PINEM using a focused, nanometer-scale, electron beam in diffraction space for measurements of infrared-light-induced PINEM. The energy resolution in diffraction mode is unprecedented, reaching 0.63 eV under the 200-keV electron beam illumination, and separated peaks of the PINEM electron-energy spectrum induced by infrared light of wavelength 1,038 nm (photon energy 1.2 eV) have been well resolved for the first time, to our knowledge. In a comparison with excitation by green (519-nm) pulses, similar first-order PINEM peak amplitudes were obtained for optical fluence differing by a factor of more than 60 at the interface of copper metal and vacuum. Under high fluence, the nonlinear regime of IR PINEM was observed, and its spatial dependence was studied. In combination with PINEM temporal gating and low-fluence infrared excitation, the PINEM diffraction method paves the way for studies of structural dynamics in reciprocal space and energy space with high temporal resolution. PMID:26848135

  3. Ultrafast probing of transient electric fields from optical field ionized plasmas using picosecond electron deflectometry

    NASA Astrophysics Data System (ADS)

    He, Zhaohan; Nees, John; Hou, Bixue; Krushelnick, Karl; Thomas, Alec

    2015-11-01

    Femtosecond bunches of electrons with relativistic to ultra-relativistic energies can be robustly produced in laser plasma wakefield accelerators (LWFA). Scaling the electron energy down to sub-relativistic and MeV level using a millijoule laser system will make such electron source a promising candidate for ultrafast electron diffraction (UED) the applications due to the intrinsic short bunch duration and perfect synchronization with optical pump. Electrons with sub-relativistic (~100 keV) energies can be used to probe transient electric field generated in laser plasmas with very high sensitivity. In a proof-of-principle experiment, we measured field evolution from plasma produced by focusing femtosecond laser pulses into a gas jet at intensities up to 1017 W/cm2. Due to the energy spread in laser plasma generated electrons, dipole magnets are used to record a streaked electron image such that the temporal evolution can be mapped in a single shot. This technique allows for probing irreversible processes such as melting of crystalline samples.

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

    NASA Astrophysics Data System (ADS)

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

    2015-11-01

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

  5. Ultrafast electronic state conversion at room temperature utilizing hidden state in cuprate ladder system

    PubMed Central

    Fukaya, R.; Okimoto, Y.; Kunitomo, M.; Onda, K.; Ishikawa, T.; Koshihara, S.; Hashimoto, H.; Ishihara, S.; Isayama, A.; Yui, H.; Sasagawa, T.

    2015-01-01

    Photo-control of material properties on femto- (10−15) and pico- (10−12) second timescales at room temperature has been a long-sought goal of materials science. Here we demonstrate a unique ultrafast conversion between the metallic and insulating state and the emergence of a hidden insulating state by tuning the carrier coherence in a wide temperature range in the two-leg ladder superconductor Sr14-xCaxCu24O41 through femtosecond time-resolved reflection spectroscopy. We also propose a theoretical scenario that can explain the experimental results. The calculations indicate that the holes injected by the ultrashort light reduce the coherence among the inherent hole pairs and result in suppression of conductivity, which is opposite to the conventional photocarrier-doping mechanism. By using trains of ultrashort laser pulses, we successively tune the carrier coherence to within 1 picosecond. Control of hole-pair coherence is shown to be a realistic strategy for tuning the electronic state on ultrafast timescales at room temperature. PMID:26481604

  6. Ultrafast Coherent Control of a Single Electron Spin in a Quantum Dot

    NASA Astrophysics Data System (ADS)

    Mikkelsen, Maiken H.

    2009-03-01

    Practical quantum information processing schemes require fast single-qubit operations. For spin-based qubits, this involves performing arbitrary coherent rotations of the spin state on timescales much faster than the spin coherence time. While we recently demonstrated the ability to initialize and monitor the evolution of single spins in quantum dots (QDs)ootnotetextM. H. Mikkelsen, J. Berezovsky, N. G. Stoltz, L. A. Coldren, D. D. Awschalom, Nature Physics 3, 770 (2007); J. Berezovsky, M. H. Mikkelsen, O. Gywat, N. G. Stoltz, L. A. Coldren, and D. D. Awschalom, Science 314, 1916 (2006)., here we present an all-optical scheme for ultrafast manipulation of these states through arbitrary angles. The GaAs QDs are embedded in a diode structure to allow controllable charging of the QDs and positioned within a vertical optical cavity to enhance the small single spin signal. By applying off-resonant optical pulses, we coherently rotate a single electron spin in a QD up to π radians on picosecond timescales ootnotetextJ. Berezovsky, M. H. Mikkelsen, N. G. Stoltz, L. A. Coldren, D. D. Awschalom, Science 320, 349 (2008)..We directly observe this spin manipulation using time-resolved Kerr rotation spectroscopy at T=10K. Measurements of the spin rotation as a function of laser detuning and intensity confirm that the optical Stark effect is the operative mechanism and the results are well-described by a model including the electron-nuclear spin interaction. Using short tipping pulses, this technique enables one to perform a large number of operations within the coherence time. This ability to perform arbitrary single-qubit operations enables sequential all-optical initialization, ultrafast control and detection of a single electron spin for quantum information purposes.

  7. Single substitutional nitrogen defects revealed as electron acceptor states in diamond using ultrafast spectroscopy

    NASA Astrophysics Data System (ADS)

    Ulbricht, R.; van der Post, S. T.; Goss, J. P.; Briddon, P. R.; Jones, R.; Khan, R. U. A.; Bonn, M.

    2011-10-01

    We report on the carrier dynamics and recombination pathways of photogenerated electrons in type Ib synthetic diamond using ultrafast spectroscopic techniques. Samples with controlled amounts of nitrogen defects were grown using the high-pressure high-temperature (HPHT) method. Electrons were excited from single substitutional nitrogen defects into the conduction band via an ultrashort pulse from a frequency-doubled Ti-sapphire laser. Using time-resolved terahertz time-domain spectroscopy, we determined the mobility of the photoexcited electrons and monitored their recombination dynamics, at temperatures ranging from cryogenic temperatures to room temperature. The electron mobility was observed to be limited by scattering with neutral nitrogen impurity defects (Ns0). Electrons were observed to predominantly recombine into neutral nitrogen states rather than their original ionized nitrogen defects, thereby creating negatively charged nitrogen states (Ns-). The creation of Ns- states is confirmed experimentally by tracking the localized vibrational modes (LVM) of nitrogen defects during the electron recombination process using visible pump-infrared probe transient spectroscopy. We observe a transient infrared absorption feature at 1349 cm-1 that can be assigned to the LVM of Ns-. Density functional calculations are carried out to determine the LVMs of nitrogen in various charge states, and we find a ˜10 cm-1 upward shift of the mode on passing from Ns0 to Ns-, in agreement with experimental observations.

  8. Ultrafast optical control of electron spins in quantum wells and quantum dots

    NASA Astrophysics Data System (ADS)

    Carter, Samuel G.; Economou, Sophia E.; Shabaev, Andrew; Kennedy, Thomas A.; Bracker, Allan S.; Reinecke, Thomas L.; Chen, Zhigang; Cundiff, Steven T.

    2010-02-01

    Using two-color time-resolved Faraday rotation and ellipticity, we demonstrate ultrafast optical control of electron spins in GaAs quantum wells and InAs quantum dots. In quantum wells, a magnetic-field induced electron spin polarization is manipulated by off-resonant pulses. By measuring the amplitude and phase of the spin polarization as a function of pulse detuning, we observe the two competing optical processes: real excitation, which generates a spin polarization through excitation of electron-hole pairs; and virtual excitation, which can manipulate a spin polarization through a stimulated Raman process without exciting electron-hole pairs. In InAs quantum dots, the spin coherence time is much longer, so that the effect of many repetitions of the pump pulses is important. Through real excitation, the pulse train efficiently polarizes electron spins that precess at multiples of the laser repetition frequency, leading to a "mode-locking" phenomenon. Through virtual excitation, the spins can be partially rotated toward the magnetic field direction, leading to a sensitive dependence of the spin orientation on the precession frequency and detuning. The electron spin dynamics strongly influence the nuclear spin dynamics as well, leading to directional control of the nuclear polarization distribution.

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

    PubMed Central

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

    2016-01-01

    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. PMID:26804546

  10. Experimental facility for two- and three-dimensional ultrafast electron beam x-ray computed tomography

    NASA Astrophysics Data System (ADS)

    Stürzel, T.; Bieberle, M.; Laurien, E.; Hampel, U.; Barthel, F.; Menz, H.-J.; Mayer, H.-G.

    2011-02-01

    An experimental facility is described, which has been designed to perform ultrafast two-dimensional (2D) and three-dimensional (3D) electron beam computed tomographies. As a novelty, a specially designed transparent target enables tomography with no axial offset for 2D imaging and high axial resolution 3D imaging employing the cone-beam tomography principles. The imaging speed is 10 000 frames per second for planar scanning and more than 1000 frames per second for 3D imaging. The facility serves a broad spectrum of potential applications; primarily, the study of multiphase flows, but also in principle nondestructive testing or small animal imaging. In order to demonstrate the aptitude for these applications, static phantom experiments at a frame rate of 2000 frames per second were performed. Resulting spatial resolution was found to be 1.2 mm and better for a reduced temporal resolution.

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

    PubMed

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

    2016-08-18

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

  12. Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser

    PubMed Central

    Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; Cottone, Grazia; Glownia, James Michael; Zhu, Diling; Chollet, Mathieu; Ihee, Hyotcherl; Cupane, Antonio; Cammarata, Marco

    2015-01-01

    Light absorption can trigger biologically relevant protein conformational changes. The light-induced structural rearrangement at the level of a photoexcited chromophore is known to occur in the femtosecond timescale and is expected to propagate through the protein as a quake-like intramolecular motion. Here we report direct experimental evidence of such ‘proteinquake’ observed in myoglobin through femtosecond X-ray solution scattering measurements performed at the Linac Coherent Light Source X-ray free-electron laser. An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes damped oscillations with a ~3.6-picosecond time period. Our results unambiguously show how initially localized chemical changes can propagate at the level of the global protein conformation in the picosecond timescale. PMID:25832715

  13. Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser

    DOE PAGESBeta

    Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; Cottone, Grazia; Glownia, James Michael; Zhu, Diling; Chollet, Mathieu; Ihee, Hyotcherl; KAIST, Daejeon; Cupane, Antonio; et al

    2015-04-02

    Light absorption can trigger biologically relevant protein conformational changes. The light induced structural rearrangement at the level of a photoexcited chromophore is known to occur in the femtosecond timescale and is expected to propagate through the protein as a quake-like intramolecular motion. Here we report direct experimental evidence of such ‘proteinquake’ observed in myoglobin through femtosecond X-ray solution scattering measurements performed at the Linac Coherent Light Source X-ray free-electron laser. An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes damped oscillations withmore » a ~3.6-picosecond time period. Our results unambiguously show how initially localized chemical changes can propagate at the level of the global protein conformation in the picosecond timescale.« less

  14. Ultrafast myoglobin structural dynamics observed with an X-ray free-electron laser

    SciTech Connect

    Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; Cottone, Grazia; Glownia, James Michael; Zhu, Diling; Chollet, Mathieu; Ihee, Hyotcherl; KAIST, Daejeon; Cupane, Antonio; Cammarata, Marco

    2015-04-02

    Light absorption can trigger biologically relevant protein conformational changes. The light induced structural rearrangement at the level of a photoexcited chromophore is known to occur in the femtosecond timescale and is expected to propagate through the protein as a quake-like intramolecular motion. Here we report direct experimental evidence of such ‘proteinquake’ observed in myoglobin through femtosecond X-ray solution scattering measurements performed at the Linac Coherent Light Source X-ray free-electron laser. An ultrafast increase of myoglobin radius of gyration occurs within 1 picosecond and is followed by a delayed protein expansion. As the system approaches equilibrium it undergoes damped oscillations with a ~3.6-picosecond time period. Our results unambiguously show how initially localized chemical changes can propagate at the level of the global protein conformation in the picosecond timescale.

  15. Direct observation of the transition state of ultrafast electron transfer reaction of a radiosensitizing drug bromodeoxyuridine

    SciTech Connect

    Wang, C.-R.; Hu, A.; Lu, Q.-B.

    2006-06-28

    Replacement of thymidine in DNA by bromodeoxyuridine (BrdU) has long been known to enhance DNA damage and cell death induced by ionizing/UV radiation, but the mechanism of action of BrdU at the molecular level is poor understood. Using time-resolved femtosecond laser spectroscopy, we obtain the real-time observation of the transition state of the ultrafast electron transfer (ET) reaction of BrdU with the precursor to the hydrated electron, which is a general product in ionizing/UV radiation. The results show that the ET reaction is completed within 0.2 picosecond (ps) after the electronic excitation, leading to the formation of a transition state BrdU*{sup -} with a lifetime of {approx}1.5 ps that then dissociates into Br{sup -} and a high reactive radical dU{sup *}. The present results can greatly enhance our understanding not only of the mechanism of BrdU as a radio-/photosensitizer but of the role of prehydrated electrons in electron-initiated processes in biological and environmental systems.

  16. Direct observation of the transition state of ultrafast electron transfer reaction of a radiosensitizing drug bromodeoxyuridine

    NASA Astrophysics Data System (ADS)

    Wang, C.-R.; Hu, A.; Lu, Q.-B.

    2006-06-01

    Replacement of thymidine in DNA by bromodeoxyuridine (BrdU) has long been known to enhance DNA damage and cell death induced by ionizing/UV radiation, but the mechanism of action of BrdU at the molecular level is poor understood. Using time-resolved femtosecond laser spectroscopy, we obtain the real-time observation of the transition state of the ultrafast electron transfer (ET) reaction of BrdU with the precursor to the hydrated electron, which is a general product in ionizing/UV radiation. The results show that the ET reaction is completed within 0.2picosecond (ps) after the electronic excitation, leading to the formation of a transition state BrdU*- with a lifetime of ˜1.5ps that then dissociates into Br- and a high reactive radical dU*. The present results can greatly enhance our understanding not only of the mechanism of BrdU as a radio-/photosensitizer but of the role of prehydrated electrons in electron-initiated processes in biological and environmental systems.

  17. Ultrafast coupling of coherent phonons with a nonequilibrium electron-hole plasma in GaAs

    NASA Astrophysics Data System (ADS)

    Basak, Amlan Kumar; Petek, Hrvoje; Ishioka, Kunie; Thatcher, Evan M.; Stanton, Christopher J.

    2015-03-01

    We present a joint experimental theoretical study of the coupling of coherent phonons in bulk GaAs with a nonequilibrium electron-hole plasma following photoexcitation at the E1 gap by ultrafast laser pulses. In contrast to prior coherent phonon experiments where photoexcitation across the E0 gap generated electrons in the Γ valley, for the E1 gap excitation, the majority of the electrons are generated in the satellite L valleys. This leads to a drastically different situation from the previous studies because the damping of electrons is now faster due to the higher scattering rates in the L valley, and, in addition, the diffusion of carriers has a significant effect on the plasma response due to the shorter optical absorption depth of the pump-probe light. Reflectivity measurements show coherent phonon-plasmon oscillations, whose frequencies lie between the transverse and longitudinal optical phonon frequencies due to the heavy damping and change with time due to the diffusion of the plasma. We analyze the experimental data with a theoretical model that describes the time and density-dependent coupling of the coherent phonon and the electron-hole plasma as the photoexcited carriers diffuse into the sample on a subpicosecond time scale. The calculated phonon-plasmon dynamics qualitatively reproduce the experimentally observed time-dependent frequency.

  18. Resolving the role of femtosecond heated electrons in ultrafast spin dynamics

    PubMed Central

    Mendil, J.; Nieves, P.; Chubykalo-Fesenko, O.; Walowski, J.; Santos, T.; Pisana, S.; Münzenberg, M.

    2014-01-01

    Magnetization manipulation is essential for basic research and applications. A fundamental question is, how fast can the magnetization be reversed in nanoscale magnetic storage media. When subject to an ultrafast laser pulse, the speed of the magnetization dynamics depends on the nature of the energy transfer pathway. The order of the spin system can be effectively influenced through spin-flip processes mediated by hot electrons. It has been predicted that as electrons drive spins into the regime close to almost total demagnetization, characterized by a loss of ferromagnetic correlations near criticality, a second slower demagnetization process takes place after the initial fast drop of magnetization. By studying FePt, we unravel the fundamental role of the electronic structure. As the ferromagnet Fe becomes more noble in the FePt compound, the electronic structure is changed and the density of states around the Fermi level is reduced, thereby driving the spin correlations into the limit of critical fluctuations. We demonstrate the impact of the electrons and the ferromagnetic interactions, which allows a general insight into the mechanisms of spin dynamics when the ferromagnetic state is highly excited, and identifies possible recording speed limits in heat-assisted magnetization reversal. PMID:24496221

  19. Ultrafast demagnetization after femtosecond laser pulses: Transfer of angular momentum from the electronic system to magnetoelastic spin-phonon modes

    NASA Astrophysics Data System (ADS)

    Tsatsoulis, T.; Illg, C.; Haag, M.; Mueller, B. Y.; Zhang, L.; Fähnle, M.

    2016-04-01

    During ultrafast demagnetization after the excitation of ferromagnetic films with femtosecond laser pulses, the angular momentum of the electronic system is transferred to the lattice via electron-phonon scatterings. The actual amount of transfer is calculated for Ni and Fe by considering spin-phonon eigenmodes, which have a sharp angular momentum. Because the considered Hamiltonian is not isotropic, the total angular momentum is not conserved.

  20. Ultra-fast electron capture by electrosterically-stabilized gold nanoparticles

    NASA Astrophysics Data System (ADS)

    Ghandi, Khashayar; Findlater, Alexander D.; Mahimwalla, Zahid; MacNeil, Connor S.; Awoonor-Williams, Ernest; Zahariev, Federico; Gordon, Mark S.

    2015-07-01

    Ultra-fast pre-solvated electron capture has been observed for aqueous solutions of room-temperature ionic liquid (RTIL) surface-stabilized gold nanoparticles (AuNPs; ~9 nm). The extraordinarily large inverse temperature dependent rate constants (ke ~ 5 × 1014 M-1 s-1) measured for the capture of electrons in solution suggest electron capture by the AuNP surface that is on the timescale of, and therefore in competition with, electron solvation and electron-cation recombination reactions. The observed electron transfer rates challenge the conventional notion that radiation induced biological damage would be enhanced in the presence of AuNPs. On the contrary, AuNPs stabilized by non-covalently bonded ligands demonstrate the potential to quench radiation-induced electrons, indicating potential applications in fields ranging from radiation therapy to heterogeneous catalysis.Ultra-fast pre-solvated electron capture has been observed for aqueous solutions of room-temperature ionic liquid (RTIL) surface-stabilized gold nanoparticles (AuNPs; ~9 nm). The extraordinarily large inverse temperature dependent rate constants (ke ~ 5 × 1014 M-1 s-1) measured for the capture of electrons in solution suggest electron capture by the AuNP surface that is on the timescale of, and therefore in competition with, electron solvation and electron-cation recombination reactions. The observed electron transfer rates challenge the conventional notion that radiation induced biological damage would be enhanced in the presence of AuNPs. On the contrary, AuNPs stabilized by non-covalently bonded ligands demonstrate the potential to quench radiation-induced electrons, indicating potential applications in fields ranging from radiation therapy to heterogeneous catalysis. Electronic supplementary information (ESI) available: Calculations and procedure for the synthesis and determination of the gold nanoparticle concentration, μSR sample preparation, determination of rate constants for electron

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

    SciTech Connect

    Scoby, C. M.; Musumeci, P.; Moody, J.; Gutierrez, M.; Tran, T.

    2009-01-22

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

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

    PubMed

    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. PMID:27314570

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

    PubMed

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

    2011-07-19

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

  4. Electronic and quantum dynamical insight into the ultrafast proton transfer of 1-hydroxy-2-acetonaphthone

    SciTech Connect

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

    2007-08-28

    The ultrafast proton-transfer dynamics of 1-hydroxy-2-acetonaphthone has been theoretically analyzed in the ground and first singlet excited electronic states by density functional theory calculations and quantum dynamics. The potential energies obtained in the ground electronic state reveal that the proton-transfer process does not lead to a stable keto tautomer unless the transfer of the hydrogen from the enol form is accompanied by an internal rotation of the newly formed O-H bond. Calculations in the first singlet excited electronic state point to a very low barrier for the formation of the keto tautomer. The analysis of the calculated frequencies of the two tautomers in the excited state unveils a coupling of the skeletal motions (low frequency modes) with the proton-transfer process, as it has been stated from time-resolved experiments. The electronic energies obtained by the time-dependent density functional theory formalism have been fitted to a monodimensional potential energy surface in order to perform an exact quantum dynamics study of the process. Our results show that the proton-transfer process is completed within 25.5 fs, in remarkable good agreement with experiments.

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

    NASA Astrophysics Data System (ADS)

    Zhang, Ping; Yang, Jie; Centurion, Martin

    2014-08-01

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

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

    PubMed

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

    2016-02-18

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

  7. Ultrafast Electron and Ion Dynamics in Strong-Field-Ionized Liquid Water

    NASA Astrophysics Data System (ADS)

    Loh, Zhi-Heng; Li, Jialin; Nie, Zhaogang; Zheng, Yi Ying; Dong, Shuo; Low, Pei Jiang

    2016-05-01

    The ionization of liquid water functions as the principal trigger for a myriad of phenomena that are relevant to radiation chemistry and biology. The earliest events that follow the ionization of water, however, remain relatively unknown. Here, femtosecond coherence spectroscopy is combined with polarization anisotropy measurements to elucidate the ultrafast electron and ion dynamics in ionized water. The results show that strong-field ionization of liquid water produces an aligned p electron distribution. Furthermore oscillations observed in the polarization anisotropy are suggestive of valence electron motion in the highly reactive H2 O+ radical cation, whose lifetime with respect to proton transfer is found to be 196 +/- 5 fs. Coherent intermolecular motions that signal initial solvent reorganization and subsequent long-lived ballistic proton transport that involves the H3 O+ end-product are also detected in the time domain. These results offer new insight into the elementary dynamics of ionized liquid water. This work is supported by the Ministry of Education (MOE2014-T2-2-052), A*Star (122-PSF-0011), and the Nanyang Assistant Professorship.

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

    NASA Astrophysics Data System (ADS)

    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

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

    NASA Astrophysics Data System (ADS)

    Silva, Carlos

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

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

    SciTech Connect

    Xu, Zhongnan; Kitchin, John R.

    2015-03-14

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    PubMed

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

    2015-12-01

    To understand the molecular origins of diseases caused by ultraviolet and visible light, and also to develop photodynamic therapy, it is important to resolve the mechanism of photoinduced DNA damage. Damage to DNA bound to a photosensitizer molecule frequently proceeds by one-electron photo-oxidation of guanine, but the precise dynamics of this process are sensitive to the location and the orientation of the photosensitizer, which are very difficult to define in solution. To overcome this, ultrafast time-resolved infrared (TRIR) spectroscopy was performed on photoexcited ruthenium polypyridyl-DNA crystals, the atomic structure of which was determined by X-ray crystallography. By combining the X-ray and TRIR data we are able to define both the geometry of the reaction site and the rates of individual steps in a reversible photoinduced electron-transfer process. This allows us to propose an individual guanine as the reaction site and, intriguingly, reveals that the dynamics in the crystal state are quite similar to those observed in the solvent medium. PMID:26587711

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

    SciTech Connect

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

    2003-04-10

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

  14. Formation of hot-electron ensembles quasiequilibrated in momentum space by ultrafast momentum scattering of highly excited hot electrons photoinjected into the Γ valley of GaAs

    NASA Astrophysics Data System (ADS)

    Tanimura, Hiroshi; Kanasaki, Jun'ichi; Tanimura, Katsumi; Sjakste, Jelena; Vast, Nathalie; Calandra, Matteo; Mauri, Francesco

    2016-04-01

    We study ultrafast scattering dynamics of hot electrons photoinjected with high excess energies in the Γ valley of the conduction band of GaAs, using time- and angle-resolved photoemission spectroscopy and ab initio calculations. At ultrafast rates of the order of 10 fs, the packets in the Γ valley are transformed into hot-electron ensembles (HEEs) quasiequilibrated in momentum space but not in energy space. The energy relaxation of the HEEs takes place as a whole on a longer time scale with rates dependent only on the excess energy, irrespective of the momenta of hot electrons. Both momentum scattering and energy relaxation are ruled by the electron-phonon interaction.

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

    PubMed

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

    2016-03-28

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

  16. 4D-QSAR investigation and pharmacophore identification of pyrrolo[2,1-c][1,4]benzodiazepines using electron conformational-genetic algorithm method.

    PubMed

    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. PMID:27121415

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

    NASA Astrophysics Data System (ADS)

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

    2007-01-01

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

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

    NASA Astrophysics Data System (ADS)

    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.

  19. Ultrafast dynamics of multiple exciton harvesting in the CdSe-ZnO system: electron injection versus Auger recombination.

    PubMed

    Zídek, Karel; Zheng, Kaibo; Abdellah, Mohamed; Lenngren, Nils; Chábera, Pavel; Pullerits, Tõnu

    2012-12-12

    We study multiple electron transfer from a CdSe quantum dot (QD) to ZnO, which is a prerequisite for successful utilization of multiple exciton generation for photovoltaics. By using ultrafast time-resolved spectroscopy we observe competition between electron injection into ZnO and quenching of multiexcitons via Auger recombination. We show that fast electron injection dominates over biexcitonic Auger recombination and multiple electrons can be transferred into ZnO. A kinetic component with time constant of a few tens of picoseconds was identified as the competition between injection of the second electron from a doubly excited QD and a trion Auger recombination. Moreover, we demonstrate that the multiexciton harvesting efficiency changes significantly with QD size. Within a narrow QD diameter range from 2 to 4 nm, the efficiency of electron injection from a doubly excited QD can vary from 30% to 70% in our system. PMID:23163524

  20. Ultrafast Decay of the Solvated Electron in a Neat Polar Solvent: The Unusual Case of Propylene Carbonate.

    PubMed

    Le Caër, Sophie; Ortiz, Daniel; Marignier, Jean-Louis; Schmidhammer, Uli; Belloni, Jacqueline; Mostafavi, Mehran

    2016-01-01

    The behavior of carbonates is critical for a detailed understanding of aging phenomena in Li-ion batteries. Here we study the first reaction stages of propylene carbonate (PC), a cyclical carbonate, by picosecond pulse radiolysis. An absorption band with a maximum around 1360 nm is observed at 20 ps after the electron pulse and is shifted to 1310 nm after 50 ps. This band presents the features of a solvated electron absorption band, the solvation lasting up to 50 ps. Surprisingly, in this polar solvent, the solvated electron follows an ultrafast decay and disappears with a half time of 360 ps. This is attributed to the formation of a radical anion PC(-•). The yield of the solvated electron is low, suggesting that the radical anions are mainly directly produced from presolvated electrons. These results demonstrate that the initial electron transfers mechanisms are strongly different in linear compared with cyclical carbonates. PMID:26706441

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

    SciTech Connect

    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.

  2. 4-D Photoacoustic Tomography

    PubMed Central

    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. PMID:23346370

  3. 4-D Photoacoustic Tomography

    NASA Astrophysics Data System (ADS)

    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.

  4. Non-Markovian response of ultrafast coherent electronic ring currents in chiral aromatic molecules in a condensed phase

    NASA Astrophysics Data System (ADS)

    Mineo, H.; Lin, S. H.; Fujimura, Y.; Xu, J.; Xu, R. X.; Yan, Y. J.

    2013-12-01

    Results of a theoretical study on non-Markov response for femtosecond laser-driven coherent ring currents in chiral aromatic molecules embedded in a condensed phase are presented. Coherent ring currents are generated by coherent excitation of a pair of quasi-degenerated π-electronic excited states. The coherent electronic dynamical behaviors are strongly influenced by interactions between the electronic system and phonon bath in a condensed phase. Here, the bath correlation time is not instantaneous but should be taken to be a finite time in ultrashort time-resolved experiments. In such a case, Markov approximation breaks down. A hierarchical master equation approach for an improved semiclassical Drude dissipation model was adopted to examine the non-Markov effects on ultrafast coherent electronic ring currents of (P)-2,2'-biphenol in a condensed phase. Time evolution of the coherent ring current derived in the hierarchical master equation approach was calculated and compared with those in the Drude model in the Markov approximation and in the static limit. The results show how non-Markovian behaviors in quantum beat signals of ring currents depend on the Drude bath damping constant. Effects of temperatures on ultrafast coherent electronic ring currents are also clarified.

  5. Non-Markovian response of ultrafast coherent electronic ring currents in chiral aromatic molecules in a condensed phase

    SciTech Connect

    Mineo, H.; Lin, S. H.; Fujimura, Y.; Xu, J.; Xu, R. X.; Yan, Y. J.

    2013-12-07

    Results of a theoretical study on non-Markov response for femtosecond laser-driven coherent ring currents in chiral aromatic molecules embedded in a condensed phase are presented. Coherent ring currents are generated by coherent excitation of a pair of quasi-degenerated π-electronic excited states. The coherent electronic dynamical behaviors are strongly influenced by interactions between the electronic system and phonon bath in a condensed phase. Here, the bath correlation time is not instantaneous but should be taken to be a finite time in ultrashort time-resolved experiments. In such a case, Markov approximation breaks down. A hierarchical master equation approach for an improved semiclassical Drude dissipation model was adopted to examine the non-Markov effects on ultrafast coherent electronic ring currents of (P)-2,2{sup ′}-biphenol in a condensed phase. Time evolution of the coherent ring current derived in the hierarchical master equation approach was calculated and compared with those in the Drude model in the Markov approximation and in the static limit. The results show how non-Markovian behaviors in quantum beat signals of ring currents depend on the Drude bath damping constant. Effects of temperatures on ultrafast coherent electronic ring currents are also clarified.

  6. Non-Markovian response of ultrafast coherent electronic ring currents in chiral aromatic molecules in a condensed phase.

    PubMed

    Mineo, H; Lin, S H; Fujimura, Y; Xu, J; Xu, R X; Yan, Y J

    2013-12-01

    Results of a theoretical study on non-Markov response for femtosecond laser-driven coherent ring currents in chiral aromatic molecules embedded in a condensed phase are presented. Coherent ring currents are generated by coherent excitation of a pair of quasi-degenerated π-electronic excited states. The coherent electronic dynamical behaviors are strongly influenced by interactions between the electronic system and phonon bath in a condensed phase. Here, the bath correlation time is not instantaneous but should be taken to be a finite time in ultrashort time-resolved experiments. In such a case, Markov approximation breaks down. A hierarchical master equation approach for an improved semiclassical Drude dissipation model was adopted to examine the non-Markov effects on ultrafast coherent electronic ring currents of (P)-2,2'-biphenol in a condensed phase. Time evolution of the coherent ring current derived in the hierarchical master equation approach was calculated and compared with those in the Drude model in the Markov approximation and in the static limit. The results show how non-Markovian behaviors in quantum beat signals of ring currents depend on the Drude bath damping constant. Effects of temperatures on ultrafast coherent electronic ring currents are also clarified. PMID:24320379

  7. Ultrafast photoinduced electron transfer reactions in supramolecular arrays: Studies of electronic coupling and solvation

    SciTech Connect

    Wasielewski, M.R.; Wiederrecht, G.P.; Svec, W.A.

    1993-05-01

    Research in our laboratory focuses on developing supramolecular arrays that produce long-lived charge separation by limiting the electronic coupling between the separated charges, and on the role of solvation in determining the rates and energetics of photoinitiated electron transfer reactions. Arrays have been developed that closely mimic the electronic coupling that was observed only for long-lived radical pairs produced in photosynthetic glassy solids. A series of 36 fixed-distance donor-acceptor molecules using porphyrin donors, triptycene spacers, and 9 different acceptors has been prepared; these are used to probe the dependence of photoinduced charge separation rates on free energy of reaction as a function of solvent both in liquid and solid solution. Data were obtained on rates of charge separation in dioxane, MTHF, butyronitrile, toluene, chlorobenzene, and benzonitrile.

  8. Ultrafast photoinduced electron transfer reactions in supramolecular arrays: Studies of electronic coupling and solvation

    SciTech Connect

    Wasielewski, M.R.; Wiederrecht, G.P.; Svec, W.A.

    1993-01-01

    Research in our laboratory focuses on developing supramolecular arrays that produce long-lived charge separation by limiting the electronic coupling between the separated charges, and on the role of solvation in determining the rates and energetics of photoinitiated electron transfer reactions. Arrays have been developed that closely mimic the electronic coupling that was observed only for long-lived radical pairs produced in photosynthetic glassy solids. A series of 36 fixed-distance donor-acceptor molecules using porphyrin donors, triptycene spacers, and 9 different acceptors has been prepared; these are used to probe the dependence of photoinduced charge separation rates on free energy of reaction as a function of solvent both in liquid and solid solution. Data were obtained on rates of charge separation in dioxane, MTHF, butyronitrile, toluene, chlorobenzene, and benzonitrile.

  9. Ultrafast Excitation of an Inner-Shell Electron by Laser-Induced Electron Recollision

    NASA Astrophysics Data System (ADS)

    Deng, Yunpei; Zeng, Zhinan; Jia, Zhengmao; Komm, Pavel; Zheng, Yinhui; Ge, Xiaochun; Li, Ruxin; Marcus, Gilad

    2016-02-01

    Extreme ultraviolet attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe subfemtosecond dynamics in atoms, molecules, and solids. However, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray (ℏω >300 eV ) attosecond bursts. A way around this problem is to use the recolliding electron to directly initiate the desired inner-shell process, instead of using the currently low flux x-ray attosecond sources. Such an excitation process occurs in a subfemtosecond time scale, and may provide the necessary "pump" step in a pump-probe experiment. Here we used a few cycle infrared (λ0≈1800 nm ) source and observed direct evidence for inner-shell excitations through the laser-induced electron recollision process. It is the first step toward time-resolved core-hole studies in the keV energy range with subfemtosecond time resolution.

  10. Ultrafast Excitation of an Inner-Shell Electron by Laser-Induced Electron Recollision.

    PubMed

    Deng, Yunpei; Zeng, Zhinan; Jia, Zhengmao; Komm, Pavel; Zheng, Yinhui; Ge, Xiaochun; Li, Ruxin; Marcus, Gilad

    2016-02-19

    Extreme ultraviolet attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe subfemtosecond dynamics in atoms, molecules, and solids. However, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray (ℏω>300  eV) attosecond bursts. A way around this problem is to use the recolliding electron to directly initiate the desired inner-shell process, instead of using the currently low flux x-ray attosecond sources. Such an excitation process occurs in a subfemtosecond time scale, and may provide the necessary "pump" step in a pump-probe experiment. Here we used a few cycle infrared (λ_{0}≈1800  nm) source and observed direct evidence for inner-shell excitations through the laser-induced electron recollision process. It is the first step toward time-resolved core-hole studies in the keV energy range with subfemtosecond time resolution. PMID:26943536

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

    PubMed

    Fu, Feichao; Liu, Shengguang; Zhu, Pengfei; Xiang, Dao; Zhang, Jie; Cao, Jianming

    2014-08-01

    A compact ultrafast electron diffractometer, consisting of an s-band 1.6 cell photocathode radio-frequency gun, a multi-function changeable sample chamber, and a sensitive relativistic electron detector, was built at Shanghai Jiao Tong University. High-quality single-shot transmission electron diffraction patterns have been recorded by scattering 2.5 MeV electrons off single crystalline gold and polycrystalline aluminum samples. The high quality diffraction pattern indicates an excellent spatial resolution, with the ratio of the diffraction ring radius over the ring rms width beyond 10. The electron pulse width is estimated to be about 300 fs. The high temporal and spatial resolution may open new opportunities in various areas of sciences. PMID:25173270

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

    SciTech Connect

    Fu, Feichao; Liu, Shengguang; Zhu, Pengfei; Xiang, Dao Zhang, Jie; Cao, Jianming

    2014-08-15

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

  13. Photoinduced ultrafast interfacial electron transfer probed with two-photon-photoemission

    NASA Astrophysics Data System (ADS)

    Gundlach, Lars; Ernstorfer, Ralph; Willig, Frank

    2007-09-01

    Ultrafast heterogeneous electron transfer (HET) from the excited singlet state of the organic chromophore perylene into the inorganic semiconductor rutile TiO II was investigated with femtosecond time-resolved two-photon photoemission (2PPE). With 2PPE one can address adsorbates at coverages far below a monolayer on single crystal surfaces. With the same chromophore perylene fixed with different anchor and bridge groups at the surface of rutile TiO II(110) the corresponding 2PPE transients revealed the relevant parameters that characterize the contributing processes. Instantaneous optical injection on one hand and slow injection over a long distance on the other hand were realized. Direct optical charge transfer was realized with the chromophore catechol that is known to form a charge transfer complex with Ti atoms on the surface of TiO II. The slow injection cases were realized by inserting rigid molecular bridges. Comparison of the different 2PPE signals with corresponding transient absorption (TA) signals for the identical systems revealed the physical processes and time scales that control the 2PPE transients. On the surface of the single crystals only one long time constant was measured via 2PPE also in the case of a long rigid bridge/anchor group in contrast to a broad distribution of time constants observed for the same molecules anchored in the nm-size cavities of an anatase TiO II film measured via TA. The broad distribution of time constants in the latter measurements can be attributed to different microscopic environments giving rise to different distances between the chromophore and the nearest TiO II wall.

  14. Ultrafast heterogeneous electron transfer reactions: Comparative theoretical studies on time- and frequency-domain data

    NASA Astrophysics Data System (ADS)

    Wang, Luxia; Willig, Frank; May, Volkhard

    2006-01-01

    Recent theoretical studies on linear absorption spectra of dye-semiconductor systems [perylene attached to nanostructured TiO2, L. Wang et al., J. Phys. Chem. B 109, 9589 (2005)] are extended here in different respects. Since the systems show ultrafast photoinduced heterogeneous electron transfer the time-dependent formulation used to compute the absorbance is also applied to calculate the temporal evolution of the sub-100fs charge injection dynamics after a 10fs laser-pulse excitation. These studies complement our recent absorption spectra fit for two perylene bridge-anchor group TiO2 systems. Moreover, the time-dependent formulation of the absorbance is confronted with a frequency-domain description. The latter underlines the central importance of the self-energy caused by the coupling of the dye levels to the semiconductor band continuum. The used model is further applied to study the effect of different parameters such as (1) the dependence on the reorganization energies of the involved intramolecular transitions, (2) the effect of changing the transfer integral which couples the excited dye state with the band continuum, and (3) the effect of the concrete form of the semiconductor band density of states. Emphasis is also put on the case where the charge injection level of the dye is near or somewhat below the band edge. This nicely demonstrates the change from a structureless absorption to a well-resolved vibrational progression including characteristic shifts of the absorption lines which are a direct measure for the dye-semiconductor coupling.

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

    PubMed

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

    2012-10-01

    The FTIR and FT-Raman spectra of 2-aminopyrimidine (2-AP) and 4-aminopyrazolo[3,4-d]pyrimidine (4-APP) has been recorded in the region 4000-400 and 3500-100 cm(-1), respectively. The tautomeric stability, optimized geometry, frequency and intensity of the vibrational bands of 2-AP and 4-APP were obtained by the DFT level using 6-31G(d) and 6-31G(d,p) basis sets. The harmonic vibrational frequencies were calculated and the scaled values have been compared with experimental FTIR and FT-Raman spectra. A detailed interpretation of the infrared and Raman spectra of 2-AP and 4-APP are also reported based on total energy distribution (TED). The observed and the calculated frequencies are found to be in good agreement. The experimental spectra also coincide satisfactorily with those of theoretically simulated spectra. The (1)H and (13)C NMR spectra have been simulated using the gauge independent atomic orbital (GIAO) method. The theoretical UV-Vis spectrum of the compound using CIS method and the electronic properties, such as HOMO and LUMO energies, were performed by time-dependent DFT (TD-DFT) approach. The calculated HOMO and LUMO energies show that charge transfer occurs within molecule. The first order hyperpolarizability (β(0)) of these novel molecular system and related properties (β, α(0) and Δα) of 2-AP and 4-APP are calculated using DFT/6-31G(d) method on the finite-field approach. The Mulliken charges, the values of electric dipole moment (μ) of the molecule were computed using DFT calculations. The change in electron density (ED) in the σ(∗) antibonding orbitals and stabilization energies E(2) have been calculated by natural bond (NBO) analysis to give clear evidence of stabilization originating in the hyper conjugation of hydrogen-bonded interactions. PMID:22683558

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

    NASA Astrophysics Data System (ADS)

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

    2012-10-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

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

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

    SciTech Connect

    Cesar, D. B.; Musumeci, P.; Alesini, D.

    2015-12-21

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

  19. Two-Dimensional Electronic Spectroscopy Reveals Ultrafast Downhill Energy Transfer in Photosystem I Trimers of the Cyanobacterium Thermosynechococcus elongatus.

    PubMed

    Anna, Jessica M; Ostroumov, Evgeny E; Maghlaoui, Karim; Barber, James; Scholes, Gregory D

    2012-12-20

    Two-dimensional electronic spectroscopy (2DES) was used to investigate the ultrafast energy-transfer dynamics of trimeric photosystem I of the cyanobacterium Thermosynechococcus elongatus. We demonstrate the ability of 2DES to resolve dynamics in a large pigment-protein complex containing ∼300 chromophores with both high frequency and time resolution. Monitoring the waiting-time-dependent changes of the line shape of the inhomogeneously broadened Qy(0-0) transition, we directly observe downhill energy equilibration on the 50 fs time scale. PMID:26291095

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

    SciTech Connect

    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

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

    DOE PAGESBeta

    Gaudin, J.; Fourment, C.; Cho, B. I.; Engelhorn, K.; Galtier, E.; Harmand, M.; Leguay, P. M.; Lee, H. J.; Nagler, B.; Nakatsutsumi, M.; et al

    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 ofmore » 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.« less

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

    SciTech Connect

    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.

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

    PubMed Central

    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.

    2014-01-01

    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. PMID:24740172

  4. Real-time observation of multiexcitonic states in ultrafast singlet fission using coherent 2D electronic spectroscopy.

    PubMed

    Bakulin, Artem A; Morgan, Sarah E; Kehoe, Tom B; Wilson, Mark W B; Chin, Alex W; Zigmantas, Donatas; Egorova, Dassia; Rao, Akshay

    2016-01-01

    Singlet fission is the spin-allowed conversion of a spin-singlet exciton into a pair of spin-triplet excitons residing on neighbouring molecules. To rationalize this phenomenon, a multiexcitonic spin-zero triplet-pair state has been hypothesized as an intermediate in singlet fission. However, the nature of the intermediate states and the underlying mechanism of ultrafast fission have not been elucidated experimentally. Here, we study a series of pentacene derivatives using ultrafast two-dimensional electronic spectroscopy and unravel the origin of the states involved in fission. Our data reveal the crucial role of vibrational degrees of freedom coupled to electronic excitations that facilitate the mixing of multiexcitonic states with singlet excitons. The resulting manifold of vibronic states drives sub-100 fs fission with unity efficiency. Our results provide a framework for understanding singlet fission and show how the formation of vibronic manifolds with a high density of states facilitates fast and efficient electronic processes in molecular systems. PMID:26673260

  5. Real-time observation of multiexcitonic states in ultrafast singlet fission using coherent 2D electronic spectroscopy

    NASA Astrophysics Data System (ADS)

    Bakulin, Artem A.; Morgan, Sarah E.; Kehoe, Tom B.; Wilson, Mark W. B.; Chin, Alex W.; Zigmantas, Donatas; Egorova, Dassia; Rao, Akshay

    2016-01-01

    Singlet fission is the spin-allowed conversion of a spin-singlet exciton into a pair of spin-triplet excitons residing on neighbouring molecules. To rationalize this phenomenon, a multiexcitonic spin-zero triplet-pair state has been hypothesized as an intermediate in singlet fission. However, the nature of the intermediate states and the underlying mechanism of ultrafast fission have not been elucidated experimentally. Here, we study a series of pentacene derivatives using ultrafast two-dimensional electronic spectroscopy and unravel the origin of the states involved in fission. Our data reveal the crucial role of vibrational degrees of freedom coupled to electronic excitations that facilitate the mixing of multiexcitonic states with singlet excitons. The resulting manifold of vibronic states drives sub-100 fs fission with unity efficiency. Our results provide a framework for understanding singlet fission and show how the formation of vibronic manifolds with a high density of states facilitates fast and efficient electronic processes in molecular systems.

  6. Ultrafast electronic deactivation dynamics of the inosine dimer--a model case for H-bonded purine bases.

    PubMed

    Röttger, Katharina; Sönnichsen, Frank D; Temps, Friedrich

    2013-08-01

    The structural properties and ultrafast electronic deactivation dynamics of the inosine dimer in CHCl3 have been investigated by two-dimensional (1)H NMR and static FTIR spectroscopy and by femtosecond time-resolved transient absorption spectroscopy, respectively. The (1)H NMR and IR spectra show the formation of a well-defined, symmetric dimer with an association equilibrium constant of KI·I = 690 ± 100 M(-1). The excited-state dynamics after photoexcitation at λpump = 260 nm monitored by ultrafast absorption spectroscopy show great similarity with those of the monomer inosine in an aqueous solution and are governed by a decay time of τ = 90 ± 10 fs, which is one of the shortest electronic lifetimes of all nucleobases and nucleobase dimers studied so far. On the basis of these observations, the inosine dimer is expected to follow a similar relaxation pathway as the monomer, involving an out-of-plane deformation of the six-membered ring. The importance of the C(2) position for the electronic deactivation of hypoxanthine and guanine is discussed. The obtained well-determined structure and straightforward dynamics qualify the inosine dimer as an excellent reference case for more complicated systems such as the G·G dimer and the G·C and A·T Watson-Crick pairs. PMID:23788062

  7. Probing in Space and Time the Nuclear Motion Driven by Nonequilibrium Electronic Dynamics in Ultrafast Pumped N2.

    PubMed

    Ajay, J; Šmydke, J; Remacle, F; Levine, R D

    2016-05-19

    An ultrafast electronic excitation of N2 in the vacuum ultraviolet creates a nonstationary coherent linear superposition of interacting valence and Rydberg states resulting in a net oscillating dipole moment. There is therefore a linear response to an electrical field that can be queried by varying the time delay between the pump and a second optical probe pulse. Both the pump and probe pulses are included in our computation as part of the Hamiltonian, and the time-dependent wave function for both electronic and nuclear dynamics is computed using a grid representation for the internuclear coordinate. Even on an ultrafast time scale there are several processes that can be discerned beyond the expected coherence oscillations. In particular, the coupling between the excited valence and Rydberg states of the same symmetry is very evident and can be directly probed by varying the delay between pulse and probe. For quite a number of vibrations the nuclear motion does not dephase the electronic disequilibrium. However, the nuclear motion does modulate the dipolar response by taking the wave packet in and out of the Franck-Condon region and by its strong influence on the coupling of the Rydberg and valence states. A distinct isotope effect arises from the dependence of the interstate coupling on the nuclear mass. PMID:26937745

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

    PubMed

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

    2015-08-01

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

  9. Ultrafast spin-switching of a ferrimagnetic alloy at room temperature traced by resonant magneto-optical Kerr effect using a seeded free electron laser.

    PubMed

    Yamamoto, Sh; Taguchi, M; Someya, T; Kubota, Y; Ito, S; Wadati, H; Fujisawa, M; Capotondi, F; Pedersoli, E; Manfredda, M; Raimondi, L; Kiskinova, M; Fujii, J; Moras, P; Tsuyama, T; Nakamura, T; Kato, T; Higashide, T; Iwata, S; Yamamoto, S; Shin, S; Matsuda, I

    2015-08-01

    Ultrafast magnetization reversal of a ferrimagnetic metallic alloy GdFeCo was investigated by time-resolved resonant magneto-optical Kerr effect measurements using a seeded free electron laser. The GdFeCo alloy was pumped by a linearly polarized optical laser pulse, and the following temporal evolution of the magnetization of Fe in GdFeCo was element-selectively traced by a probe free electron laser pulse with a photon energy tuned to the Fe M-edge. The results have been measured using rotating analyzer ellipsometry method and confirmed magnetization switching caused by ultrafast heating. PMID:26329205

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

  11. Ultrafast single-electron transfer in coupled quantum dots driven by a few-cycle chirped pulse

    SciTech Connect

    Yang, Wen-Xing; Chen, Ai-Xi; Bai, Yanfeng; Lee, Ray-Kuang

    2014-04-14

    We theoretically study the ultrafast transfer of a single electron between the ground states of a coupled double quantum dot (QD) structure driven by a nonlinear chirped few-cycle laser pulse. A time-dependent Schrödinger equation without the rotating wave approximation is solved numerically. We demonstrate numerically the possibility to have a complete transfer of a single electron by choosing appropriate values of chirped rate parameters and the intensity of the pulse. Even in the presence of the spontaneous emission and dephasing processes of the QD system, high-efficiency coherent transfer of a single electron can be obtained in a wide range of the pulse parameters. Our results illustrate the potential to utilize few-cycle pulses for the excitation in coupled quantum dot systems through the nonlinear chirp parameter control, as well as a guidance in the design of experimental implementation.

  12. Ultrafast photoinduced electron transfer in the micelle and the gel phase of a PEO-PPO-PEO triblock copolymer

    SciTech Connect

    Mandal, Ujjwal; Ghosh, Subhadip; Dey, Shantanu; Adhikari, Aniruddha; Bhattacharyya, Kankan

    2008-04-28

    Ultrafast photoinduced electron transfer (PET) from N,N-dimethylaniline (DMA) to coumarin dyes is studied in the micelle and the gel phase of a triblock copolymer, (PEO){sub 20}-(PPO){sub 70}-(PEO){sub 20} (Pluronic P123) by picosecond and femtosecond emission spectroscopies. The rate of PET in a P123 micelle and gel is found to be nonexponential and faster than the slow components of solvation dynamics. In a P123 micelle and gel, PET occurs on multiple time scales ranging from a subpicosecond time scale to a few nanoseconds. In the gel phase, the highest rate constant (9.3x10{sup 9} M{sup -1} s{sup -1}) of ET for C152 is about two times higher than that (3.8x10{sup 9} M{sup -1} s{sup -1}) observed in micelle phase. The ultrafast components of electron transfer (ET) exhibits a bell shaped dependence with the free energy change which is similar to the Marcus inversion. Possible reasons for slower PET in P123 micelle compared to other micelles and relative to P123 gel are discussed.

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

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed

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

    2016-03-24

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

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

    SciTech Connect

    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.

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

    DOE PAGESBeta

    Mo, M. Z.; Shen, X.; Chen, Z.; Li, R. K.; Dunning, M.; Sokolowski-Tinten, K.; Zheng, Q.; Weathersby, S. P.; Reid, A. H.; Coffee, R.; et al

    2016-08-04

    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.more » This experimental capability opens up an exciting opportunity to unravel the atomic dynamics of structural phase transitions in warm dense matter regime« less

  17. Water-Stable, Hydroxamate Anchors for Functionalization of TiO2 Surfaces with Ultrafast Interfacial Electron Transfer

    SciTech Connect

    McNamara, W.R.; Milot, R.L.; Song, H.; Snoeberger III, R.C.; Batista, Victor S.; Schmuttenmaer, C.A.; Brudvig, Gary W; Crabtree, Robert H

    2010-01-01

    A novel class of derivatized hydroxamic acid linkages for robust sensitization of TiO{sub 2} nanoparticles (NPs) under various aqueous conditions is described. The stability of linkages bound to metal oxides under various conditions is important in developing photocatalytic cells which incorporate transition metal complexes for solar energy conversion. In order to compare the standard carboxylate anchor to hydroxamates, two organic dyes differing only in anchoring groups were synthesized and attached to TiO{sub 2} NPs. At acidic, basic, and close to neutral pH, hydroxamic acid linkages resist detachment compared to the labile carboxylic acids. THz spectroscopy was used to compare ultrafast interfacial electron transfer (IET) into the conduction band of TiO{sub 2} for both linkages and found similar IET characteristics. Observable electron injection and stronger binding suggest that hydroxamates are a suitable class of anchors for designing water stable molecules for functionalizing TiO{sub 2}.

  18. Ultrafast coherent dynamics of Rydberg electrons bound in the image potential near a single metallic nano-object (Presentation Recording)

    NASA Astrophysics Data System (ADS)

    Robin, Jörg; Vogelsang, Jan; Nagy, Benedek J.; Gross, Petra; Lienau, Christoph

    2015-09-01

    Image potential states are well established surface states of metallic films [1]. For a single metallic nanostructure these surface states can be localized in the near-field arising from illumination by a strong laser field. Thus single metallic nanostructures offer the unique possibility to study quantum systems with both high spatial and ultrafast temporal resolution. Here, we investigate the dynamics of Rydberg states localized to a sharp metallic nanotaper. For this purpose we realized a laser system delivering few-cycle pulses tunable over a wide wavelength range [2]. Pulses from a regenerative titanium:sapphire amplifier generate a white light continuum, from which both a proportion in the visible and in the infrared are amplified in two non-collinear optical parametric amplification (NOPA) stages. Difference frequency generation (DFG) of both stages provides pulses in the near-infrared. With a precisely delayed sequence of few-cycle pulses centered around 600 nm (NOPA#1 output) and 1600 nm (DFG output) we illuminate the apex of a sharply etched gold tip. Varying the delay we observe an exponential decay of photoemitted electrons with a distinctly asymmetric decay length on both sides, indicating the population of different states. Superimposed on the decay is a clearly discernible quantum beat pattern with a period of <50 fs, which arises from the motion of Rydberg photoelectrons bound within their own image potential. These results therefore constitute a step towards controlling single electron wavepackets released from a gold tip opening up fascinating perspectives for applications in ultrafast electron microscopy [3]. [1] Hofer, U. et al. Science 277, 1480 (1997) [2] Vogelsang, J., Robin J. et al. Opt. Express 22, 25295 (2014) [3] Petek, H. et al. ACS Nano 8, 5 (2014)

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

    PubMed

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

    2016-05-19

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

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

    PubMed

    Gessner, Oliver; Gühr, Markus

    2016-01-19

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

  1. Synthesis and Properties of Bis(2,5-dimethylpyrrolo[3,4-d])tetrathiafulvalenes, a Class of Annelated Tetrathiafulvalene Derivatives with Excellent Electron Donor Properties.

    PubMed

    Zong, Kyukwan; Chen, Wha; Cava, Michael P.; Rogers, Robin D.

    1996-11-15

    The synthesis of the first derivatives of bis(pyrrolo[3,4-d])tetrathiafulvalene has been studied in detail. Starting from the readily available 2,5-dimethylpyrrole (11) and N-phenyl-2,5-dimethylpyrrole, bis(2,5-dimethylpyrrolo[3,4-d])tetrathiafulvalene (8) and the N,N'-disubstituted derivatives 6, 7, 9, and 10 were prepared in good yields by practical procedures. In contrast to the other types of aromatic annelated tetrathiafulvalenes (TTFs), which have appreciably higher oxidation potentials than TTF, the redox behavior of the pyrrolo tetrathiafulvalenes (TTFs) is very close to that of TTF itself. The potential of pyrrolotetrathiafulvalenes as a new series of organic metal building blocks is shown by the two-probe conductivities of the tetracyanoquinodimethane (TCNQ) complexes of the N-phenyl compound 7 and the N-methyl compound 9, which give higher values than TTF-TCNQ under similar conditions. PMID:11667799

  2. Tuning of Magnetic Optical Response in a Dielectric Nanoparticle by Ultrafast Photoexcitation of Dense Electron-Hole Plasma.

    PubMed

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

    2015-09-01

    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 photoinjection of dense (>10(20) cm(-3)) electron-hole plasma within such nanoparticle, drastically changing its transient dielectric permittivity. This allows manipulation 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 a single-particle nanodevice enables designing of fast and ultracompact optical switchers and modulators. PMID:26259100

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

    NASA Astrophysics Data System (ADS)

    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.

  4. Study of beam loading and its compensation in the Compact Ultrafast Terahertz Free-Electron Laser injector linac

    SciTech Connect

    Lal, Shankar Pant, K. K.

    2014-12-15

    The RF properties of an accelerating structure, and the pulse structure and charge per bunch in the electron beam propagating through it are important parameters that determine the impact of beam loading in the structure. The injector linac of the Compact Ultrafast Terahertz Free-Electron Laser (CUTE-FEL) has been operated with two different pulse structures during initial commissioning experiments and the effect of beam loading on the accelerated electron beam parameters has been studied analytically for these two pulse structures. This paper discusses the analytical study of beam loading in a Standing Wave, Plane Wave Transformer linac employed in the CUTE-FEL setup, and a possible technique for its compensation for the electron beam parameters of the CUTE-FEL. A parametric study has been performed to study beam loading for different beam currents and to optimize injection time of the electron beam to compensate beam loading. Results from the parametric study have also been used to explain previously observed results from acceleration experiments in the CUTE-FEL setup.

  5. Soft Route to 4D Tomography

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  6. Protein-cofactor binding and ultrafast electron transfer in riboflavin binding protein under the spatial confinement of nanoscopic reverse micelles.

    PubMed

    Saha, Ranajay; Rakshit, Surajit; Verma, Pramod Kumar; Mitra, Rajib Kumar; Pal, Samir Kumar

    2013-02-01

    In this contribution, we study the effect of confinement on the ultrafast electron transfer (ET) dynamics of riboflavin binding protein (RBP) to the bound cofactor riboflavin (Rf, vitamin B2), an important metabolic process, in anionic sodium bis(2-ethylhexyl) sulfosuccinate reverse micelles (AOT-RMs) of various hydration levels. Notably, in addition to excluded volume effect, various nonspecific interactions like ionic charge of the confining surface can influence the biochemical reactions in the confined environment of the cell. To this end, we have also studied the ET dynamics of RBP-Rf complex under the confinement of a cationic hexadecyltrimethylammonium bromide (CTAB) RMs with similar water pool size to the anionic AOT-RMs towards simulating equal restricted volume effect. It has been found that the spatial confinement of RBP in the AOT-RM of w(0) = 10 leads to the loss of its tertiary structure and hence vitamin binding capacity. Although, RBP regains its binding capacity and tertiary structure in AOT-RMs of w(0) ≥ 20 due to its complete hydration, the ultrafast ET from RBP to Rf merely occurs in such systems. However, to our surprise, the ET process is found to occur in cationic CTAB-RMs of similar volume restriction. It is found that under the spatial confinement of anionic AOT-RM, the isoalloxazine ring of Rf is improperly placed in the protein nanospace so that ET between RBP and Rf is not permitted. This anomaly in the binding behaviour of Rf to RBP in AOT-RMs is believed to be the influence of repulsive potential of the anionic AOT-RM surface to the protein. Our finding thus suggests that under similar size restriction, both the hydration and surface charge of the confining volume could have major implication in the intraprotein ET dynamics in real cellular environments. PMID:23334913

  7. Ultrafast saturation of electronic-resonance-enhanced coherent anti-Stokes Raman scattering and comparison for pulse durations in the nanosecond to femtosecond regime

    NASA Astrophysics Data System (ADS)

    Patnaik, Anil K.; Roy, Sukesh; Gord, James R.

    2016-02-01

    The saturation threshold of a probe pulse in an ultrafast electronic-resonance-enhanced (ERE) coherent anti-Stokes Raman spectroscopy (CARS) configuration is calculated. We demonstrate that while the underdamping condition is a sufficient condition for saturation of ERE-CARS with the long-pulse excitations, a transient gain must be achieved to saturate the ERE-CARS signal for the ultrafast probe regime. We identify that the area under the probe pulse can be used as a definitive parameter to determine the criterion for a saturation threshold for ultrafast ERE-CARS. From a simplified analytical solution and a detailed numerical calculation based on density-matrix equations, the saturation threshold of ERE-CARS is compared for a wide range of probe-pulse durations from the 10-ns to the 10-fs regime. The theory explains both qualitatively and quantitatively the saturation thresholds of resonant transitions and also gives a predictive capability for other pulse duration regimes. The presented criterion for the saturation threshold will be useful in establishing the design parameters for ultrafast ERE-CARS.

  8. Ultrafast laser and swift heavy ion irradiation: Response of Gd2O3 and ZrO2 to intense electronic excitation

    NASA Astrophysics Data System (ADS)

    Rittman, Dylan R.; Tracy, Cameron L.; Cusick, Alex B.; Abere, Michael J.; Torralva, Ben; Ewing, Rodney C.; Yalisove, Steven M.

    2015-04-01

    In order to investigate the response of materials to extreme conditions, there are several approaches to depositing extremely high concentrations of energy into very small volumes of material, including ultrafast laser and swift heavy ion (SHI) irradiation. In this study, crystalline-to-crystalline phase transformations in cubic Gd2O3 and monoclinic ZrO2 have been investigated using ultrafast laser irradiation. The phases produced by the extreme conditions of irradiation were characterized by grazing incidence x-ray diffraction (GIXRD) and Raman spectroscopy. Gd2O3 exhibited a cubic-to-monoclinic phase transformation, as evidenced by the appearance of the monoclinic (40 2 ¯ ), (003), (310), and (11 2 ¯ ) peaks in the GIXRD pattern and of four Ag and three Bg Raman modes. ZrO2 underwent a monoclinic-to-tetragonal phase transformation, as evidenced by the emergence of the tetragonal (101) peak in the GIXRD pattern and of Eg and A1g Raman modes. The new phases formed by ultrafast laser irradiation are high temperature polymorphs of the two materials. No evidence of amorphization was seen in the GIXRD data, though Raman spectroscopy indicated point defect accumulation. These results are identical to those produced by irradiation with SHIs, which also deposit energy in materials primarily through electronic excitation. The similarity in damage process and material response between ultrafast laser and SHI irradiation suggests a fundamental relationship between these two techniques.

  9. Imaging Acoustic Phonon Dynamics on the Nanometer-Femtosecond Spatiotemporal Length-Scale with Ultrafast Electron Microscopy

    NASA Astrophysics Data System (ADS)

    Plemmons, Dayne; Flannigan, David

    Coherent collective lattice oscillations known as phonons dictate a broad range of physical observables in condensed matter and act as primary energy carriers across a wide range of material systems. Despite this omnipresence, analysis of phonon dynamics on their ultrashort native spatiotemporal length scale - that is, the combined nanometer (nm), spatial and femtosecond (fs), temporal length-scales - has largely remained experimentally inaccessible. Here, we employ ultrafast electron microscopy (UEM) to directly image discrete acoustic phonons in real-space with combined nm-fs resolution. By directly probing electron scattering in the image plane (as opposed to the diffraction plane), we retain phase information critical for following the evolution, propagation, scattering, and decay of phonons in relation to morphological features of the specimen (i.e. interfaces, grain boundaries, voids, ripples, etc.). We extract a variety of morphologically-specific quantitative information from the UEM videos including phonon frequencies, phase velocities, and decays times. We expect these direct manifestations of local elastic properties in the vicinity of material defects and interfaces will aide in the understanding and application of phonon-mediated phenomena in nanostructures. Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, MN, 55455, USA.

  10. Ultrafast harmonic rf kicker design and beam dynamics analysis for an energy recovery linac based electron circulator cooler ring

    DOE PAGESBeta

    Huang, Yulu; Wang, Haipeng; Rimmer, Robert A.; Wang, Shaoheng; Guo, Jiquan

    2016-08-01

    An ultrafast kicker system is being developed for the energy recovery linac (ERL) based electron circulator cooler ring (CCR) in the proposed Jefferson Lab Electron Ion Collider (JLEIC, previously named MEIC). In the CCR, the injected electron bunches can be recirculated while performing ion cooling for 10–30 turns before the extraction, thus reducing the recirculation beam current in the ERL to 1/10–1/30 (150mA–50 mA) of the cooling beam current (up to 1.5 A). Assuming a bunch repetition rate of 476.3 MHz and a recirculating factor of 10 in the CCR, the kicker is required to operate at a pulse repetitionmore » rate of 47.63 MHz with pulse width of around 2 ns, so that only every 10th bunch in the CCR will experience a transverse kick while the rest of the bunches will not be disturbed. Such a kicker pulse can be synthesized by ten harmonic modes of the 47.63 MHz kicker pulse repetition frequency, using up to four quarter wavelength resonator (QWR) based deflecting cavities. In this paper, several methods to synthesize such a kicker waveform will be discussed and a comparison of their beam dynamics performance is made using ELEGANT. Four QWR cavities are envisaged with high transverse shunt impedance requiring less than 100 W of total rf power for a Flat-Top kick pulse. Multipole fields due to the asymmetry of this type of cavity are analyzed. The transverse emittance growth due to the sextupole component is simulated in ELEGANT. In conclusion, off-axis injection and extraction issues and beam optics using a multicavity kick-drift scheme will also be discussed.« less

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

    SciTech Connect

    Arrell, C. A. Ojeda, J.; Mourik, F. van; Chergui, M.; Sabbar, M.; Gallmann, L.; Keller, U.; Okell, W. A.; Witting, T.; Siegel, T.; Diveki, Z.; Hutchinson, S.; Tisch, J. W.G.; Marangos, J. P.; Chapman, R. T.; Cacho, C.; Rodrigues, N.; Turcu, I. C.E.; Springate, E.

    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.

  12. Nanoscale heat transport from Ge hut, dome, and relaxed clusters on Si(001) measured by ultrafast electron diffraction

    SciTech Connect

    Frigge, T. Hafke, B.; Tinnemann, V.; Krenzer, B.; Horn-von Hoegen, M.

    2015-02-02

    The thermal transport properties of crystalline nanostructures on Si were studied by ultra-fast surface sensitive time-resolved electron diffraction. Self-organized growth of epitaxial Ge hut, dome, and relaxed clusters was achieved by in-situ deposition of 8 monolayers of Ge on Si(001) at 550 °C under UHV conditions. The thermal response of the three different cluster types subsequent to impulsive heating by fs laser pulses was determined through the Debye-Waller effect. Time resolved spot profile analysis and life-time mapping was employed to distinguish between the thermal response of the different cluster types. While dome clusters are cooling with a time constant of τ = 150 ps, which agrees well with numerical simulations, the smaller hut clusters with a height of 2.3 nm exhibit a cooling time constant of τ = 50 ps, which is a factor of 1.4 slower than expected.

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

    PubMed

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

    2016-08-18

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

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

    NASA Astrophysics Data System (ADS)

    Arrell, C. A.; Ojeda, J.; Sabbar, M.; Okell, W. A.; Witting, T.; Siegel, T.; Diveki, Z.; Hutchinson, S.; Gallmann, L.; Keller, U.; van Mourik, F.; Chapman, R. T.; Cacho, C.; Rodrigues, N.; Turcu, I. C. E.; Tisch, J. W. G.; Springate, E.; Marangos, J. P.; Chergui, M.

    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.

  15. Comparing ultrafast surface and bulk heating using time-resolved electron diffraction

    SciTech Connect

    Streubühr, C.; Kalus, A.; Zhou, P. Kammler, M.; Linde, D. von der; Ligges, M.; Hanisch-Blicharski, A.; Bovensiepen, U.; Horn-von Hoegen, M.

    2014-04-21

    From measurements of the transient Debye-Waller effect in Bismuth, we determine the buildup time of the random atomic motion resulting from the electronic relaxation after short pulse laser excitation. The surface sensitive reflection high energy electron diffraction and transmission electron diffraction yield a time constant of about 12 ps and 3 ps, respectively. The different energy transfer rates indicate relatively weak coupling between bulk and surface vibrational modes.

  16. Contribution of electronic excitation to the structural evolution of ultrafast laser-irradiated tungsten nanofilms

    NASA Astrophysics Data System (ADS)

    Murphy, Samuel T.; Giret, Yvelin; Daraszewicz, Szymon L.; Lim, Anthony C.; Shluger, Alexander L.; Tanimura, Katsumi; Duffy, Dorothy M.

    2016-03-01

    The redistribution of the electron density in a material during laser irradiation can have a significant impact on its structural dynamics. This electronic excitation can be incorporated into two temperature molecular dynamics (2T-MD) simulations through the use of electronic temperature dependent potentials. Here, we study the structural dynamics of laser irradiated tungsten nanofilms using 2T-MD simulations with an electronic temperature dependent potential and compare the results to equivalent simulations that employ a ground-state interatomic potential. Electronic excitation leads to an expansion of the crystal and a decrease in the melting point of tungsten. During laser irradiation these factors ensure that the threshold fluences to the different melting regimes are reduced. Furthermore, both heterogenous and homogeneous melting are predicted to occur more rapidly due to excitation and oscillations in the film thickness will be accentuated.

  17. Monitoring the Coherent Vibrational Control of Electronic Excitation Transfer Using Ultrafast Pump-Probe Polarization Spectroscopy

    NASA Astrophysics Data System (ADS)

    Biggs, Jason; Cina, Jeffrey

    2010-03-01

    The interplay between nuclear and electronic degrees of freedom in molecular energy-transfer complexes is a subject of current interest. We have proposed a method to use coherent nuclear motion to control the transfer of electronic excitation energy between donor and acceptor moieties in electronically coupled dimers. The underlying electronic and nuclear motion at the level of quantum mechanical amplitudes can be observed using nonlinear wave-packet interferometry(nl-WPI), a form of fluorescence-detected multidimensional electronic spectroscopy. In our control scheme, coherent nuclear motion is induced in the acceptor chromophore prior to direct electronic excitation of the donor. This nuclear motion affects the instantaneous resonance conditions between donor and acceptor moieties and thus affects subsequent energy transfer dynamics. We have developed the framework to simulate four-pulse nl-WPI experiments, and the pump-probe limit thereof, on energy-transfer systems after interaction with a control pulse that induces nuclear motion. We present simulations in the pump-probe limit from model energy-transfer systems subjected to prior impulsive vibrational excitation, and show how pulse polarization can be used to infer electronic dynamics from isotropically oriented dimers.

  18. An ultrafast spectroscopic and quantum mechanical investigation of multiple emissions in push-pull pyridinium derivatives bearing different electron donors.

    PubMed

    Carlotti, B; Benassi, E; Cesaretti, A; Fortuna, C G; Spalletti, A; Barone, V; Elisei, F

    2015-08-28

    A joint experimental and theoretical approach, involving state-of-the-art femtosecond fluorescence up-conversion measurements and quantum mechanical computations including vibronic effects, was employed to get a deep insight into the excited state dynamics of two cationic dipolar chromophores (Donor-π-Acceptor(+)) where the electron deficient portion is a N-methyl pyridinium and the electron donor a trimethoxyphenyl or a pyrene, respectively. The ultrafast spectroscopic investigation, and the time resolved area normalised emission spectra in particular, revealed a peculiar multiple emissive behaviour and allowed the distinct emitting states to be remarkably distinguished from solvation dynamics, occurring in water in a similar timescale. The two and three emissions experimentally detected for the trimethoxyphenyl and pyrene derivatives, respectively, were associated with specific local emissive minima in the potential energy surface of S1 on the ground of quantum-mechanical calculations. A low polar and planar Locally Excited (LE) state together with a highly polar and Twisted Intramolecular Charge Transfer (TICT) state is identified to be responsible for the dual emission of the trimethoxyphenyl compound. Interestingly, the more complex photobehaviour of the pyrenyl derivative was explained considering the contribution to the fluorescence coming not only from the LE and TICT states but also from a nearly Planar Intramolecular Charge Transfer (PICT) state, with both the TICT and the PICT generated from LE by progressive torsion around the quasi-single bond between the methylpyridinium and the ethene bridge. These findings point to an interconversion between rotamers for the pyrene compound taking place in its excited state against the Non-equilibrated Excited Rotamers (NEER) principle. PMID:26213993

  19. Ultrafast electron transfer in the recognition of different DNA sequences by a DNA-binding protein with different dynamical conformations.

    PubMed

    Mondol, Tanumoy; Batabyal, Subrata; Pal, Samir Kumar

    2012-01-01

    Ultrafast electron transfer (ET) phenomenon in protein and protein-DNA complex is very much crucial and often leads to the regulation of various kinds of redox reactions in biological system. Although, the conformation of the protein in protein-DNA complex is concluded to play the key role in the ET process, till date very little evidences exist in the literature. λ-repressor-operator DNA interaction, particularly O(R)1 and O(R)2, is a key component of the λ-genetic switch and is a model system for understanding the chemical principles of the conformation-dependent ET reaction, governed by differential protein dynamics upon binding with different DNA target sequences. Here, we have explored the photoinduced electron transfer from the tryptophan moieties of the protein λ-repressor to two operators DNA of different sequences (O(R)1 and O(R)2) using picosecond-resolved fluorescence spectroscopy. The enhanced flexibility and different conformation of the C-terminal domain of the repressor upon complexation with O(R)1 DNA compared to O(R)2 DNA are found to have pronounced effect on the rate of ET. We have also observed the ET phenomenon from a dansyl chromophore, bound to the lysine residue, distal from the DNA-binding domain of the protein to the operator DNA with a specific excitation at 299 nm wavelength. The altered ET dynamics as a consequence of differential protein conformation upon specific DNA sequence recognition may have tremendous biological implications. PMID:22686485

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

    NASA Astrophysics Data System (ADS)

    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.

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

    SciTech Connect

    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.

  2. Ultrafast Electron Dynamics in Gold in the Presence of Laser Excited Surface Plasma Waves

    SciTech Connect

    Raynaud, M.

    2010-02-02

    Surface plasmon excitation with ultrashort intense laser pulses enhances efficiently laser absorption in metals and creates local high fields and non-equilibrium hot electrons population that have attractivity for numerous applications such as the development of intense sources of high-energy particles or photons and in the fast ignitor scheme in the framework of inertial fusion. In this context, the knowledge of the dynamics of relaxation of the collective electrons behavior is of importance. Using gold grating, we have investigated electrons relaxation in the presence of laser excited surface plasmon waves using a multiple-wavelengh femtosecond pump-probe technique. The results yield evidence of longer relaxation time in the presence of the collective excitation than that of individual electronic states.

  3. Roadmap on ultrafast optics

    NASA Astrophysics Data System (ADS)

    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.

  4. Nonlinear Ultrafast Spectroscopy of Electron and Energy Transfer in Molecule Complexes

    SciTech Connect

    Mukamel, Shaul

    2006-02-09

    The proposed research program will focus on the development of a unified dynamical theoretical framework for calculating the optical response of molecular assemblies and applying it towards studying the interplay of energy and charge transfer in artificial chromophore-aggregate complexes. Applications will be made to poly (p phenylene vinylene), (PPV) oligomers, several families of stilbenoid aggregates with stacking through a cyclophane group, coupled porphyrin arrays, and energy funneling in phenylacetylene dendrimers. The approach is based on formulating the problem using the density- matrix and developing Liouville-space techniques which provide physical insight and are particularly suitable for computing both coherent and incoherent transport. A physical picture based on collective electronic normal modes which represent the dynamics of the optically-driven reduced single electron density matrix will be established. Femtosecond signals and optical properties will be directly related to the motions of electron-hole pairs in real space, completely avoiding the calculation of many-electron excited-state wavefunctions, thus, considerably reducing computational effort. Vibrational and solvent effects will be incorporated. Guidelines for the synthesis of new donor/bridge/acceptor molecules with desired properties such as carrier transport, optical response time scales and fluorescence quantum yields will be developed. The analogy with Thz emission spectroscopy which probes charge carrier dynamic is in semiconductor superlattices will be explored. A systematic procedure for identifying the electronic coherence sizes which control the transport and optical properties will be developed. Localization of electronic transition density matrices of large molecules will be used to break the description of their optical response into coupled chromophores. The proposal is divided into four parts: (i) Collective-Oscillator Representation of Electronic Excitations in Molecular

  5. X-Ray Imaging of Ultrafast Magnetic Reconnection Driven by Relativistic Electrons

    NASA Astrophysics Data System (ADS)

    Raymond, Anthony; McKelvey, Andrew; Zulick, Calvin; Maksimchuk, Anatoly; Thomas, Alexander; Willingale, Louise; Chvykov, Vladimir; Yanovsky, Victor; Krushelnick, Karl

    2014-10-01

    Magnetic reconnection events driven by relativistic electrons are observed between two high intensity laser/plasma interaction sites. The two laser focuses were on average 20 μm FWHM containing 50 TW of power each, delivered with a split f/3 paraboloid onto copper foil targets at a focused intensity of 4×1018 W/cm2. A spherically bent k-alpha X-ray Bragg crystal was utilized to image the interactions, and by motorizing one half of the paraboloid vertically the focal separation was varied between 0-200 μm. While these k-alpha images demonstrated a ring structure surrounding a single focus (due to electrons returning from vacuum to the rear of the target surface), splitting the focuses revealed the rings of either spot interacting and enhancing between the focuses, evidencing magnetic reconnection driven by the relativistic electron currents. Imaging the transversely propagating electrons with a filtered LANEX screen demonstrated relativistic currents with spatial nonuniformities potentially directly originating from reconnection events, and varying target geometries were used to investigate the resulting effects on the spatial electron profiles. At present PIC simulations are being conducted to better understand and attempt to reproduce the measured electron outflow dynamics. Currently at: ELI Attosecond Light Pulse Source.

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

    NASA Astrophysics Data System (ADS)

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

    2005-10-01

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

  7. Ultrafast spectroscopy of electron transfer dynamics in liquids; excitation transfer studies of phase transitions

    NASA Astrophysics Data System (ADS)

    Goun, Alexei A.

    The transfer of an electron from a donor to an acceptor is the fundamental step in a wide range of chemical and biological processes. As a result, electron-transfer reactions have been the focus of numerous theoretical and experimental efforts aimed at understanding the kinetics and mechanism of the transfer event. Liquid solvents are an important medium for electron-transfer processes. The influences of the distance dependence, diffusion, the radial distribution function, and the hydrodynamic effect have been incorporated into the theory of electron transfer in solution, as well as into the theory of electron transfer between donors and acceptors in the head group regions of micelles. The development of new laser system with a pulse duration of tens of femtoseconds, with tunable wavelength allowed us to study these processes on a considerably shorter time scale than previous studies. This allowed us to observe not only the diffusion controlled but also the kinetics of electron transfer for donor/acceptor pairs that are in close proximity. In one set of experiments we have studied the kinetics of electron transfer in electron accepting molecule (rhodamine 3B) dissolved in electron donating solvent (N,N-dimethylaniline). The data for the forward electron transfer and geminate recombination are approximated by the statistical theory of the electron transfer. Optical anisotropy observed in the experiment demonstrates the orientation dependence of the electron transfer rate. In further experiments we investigated the electron transfer in non-hydrogen bonding liquids of increasing viscosity. The effective value of the donor/acceptor electronic coupling was found to decrease with viscosity. Electron transfer experiments were also carried out on the surface of micelles. The systems studied are the hole donor octadecyl-rhodamine B (ODRB) and the hole acceptor N,N-dimethyl-aniline (DMA) in micelles made of dodecyltrimethylammonium bromide (DTAB) and

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

    PubMed

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

    2016-06-23

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-05-01

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

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

    SciTech Connect

    Rasmussen, Andrew M. Ramakrishna, S.; Weiss, Emily A.; Seideman, Tamar

    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.

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

    NASA Astrophysics Data System (ADS)

    Smith, Brian Ampere

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

  12. Probing Ultrafast Nuclear Dynamics in Halomethanes by Time-Resolved Electron and Ion Imaging

    NASA Astrophysics Data System (ADS)

    Ziaee, F.; Rudenko, A.; Rolles, D.; Savelyev, E.; Bomme, C.; Boll, R.; Manschwetus, B.; Erk, B.; Trippel, S.; Wiese, J.; Kuepper, J.; Amini, K.; Lee, J.; Brouard, M.; Brausse, F.; Rouzee, A.; Olshin, P.; Mereshchenko, A.; Lahl, J.; Johnsson, P.; Simon, M.; Marchenko, T.; Holland, D.; Underwood, J.

    2016-05-01

    Femtosecond pump-probe experiments provide opportunities to investigate photochemical reaction dynamics and the resulting changes in molecular structure in detail. Here, we present a study of the UV-induced photodissociation of gas-phase halomethane molecules (CH3 I, CH2 IBr, ...) in a pump-probe arrangement using two complementary probe schemes, either using a femtosecond near-infrared laser or the FLASH free-electron laser. We measured electrons and ions produced during the interaction using a double-sided velocity map imaging spectrometer equipped with a CCD camera for electron detection and with the Pixel Imaging Mass Spectrometry (PImMS) camera for ions, which can record the arrival time for up to four ions per pixel. This project is supported by the DOE, Office of Science, BES, Division of Chemical, Geological, and Biological Sciences.

  13. Theory of ultrafast photoinduced heterogeneous electron transfer: Decay of vibrational coherence into a finite electronic-vibrational quasicontinuum

    NASA Astrophysics Data System (ADS)

    Ramakrishna, S.; Willig, F.; May, V.

    2001-08-01

    Photo-induced electron transfer from a surface attached dye molecule to the band levels of a semiconductor is modeled via an electronic-vibronic quasicontinuum. The description enables one to obtain a fairly accurate expression for the decay of the excited molecular state, including initial vibronic coherences. The model accounts for (a) the effect of a finite band width, (b) variations in reorganization energy and electronic coupling, (c) various energetic positions for the injecting level, (d) different initial vibrational wave packets in the excited state, and (e) two vibrational modes participating in the electron transfer process. Most cases are studied numerically and can be reasonably well understood from the obtained decay expression.

  14. Ultrafast laser and swift heavy ion irradiation: Response of Gd{sub 2}O{sub 3} and ZrO{sub 2} to intense electronic excitation

    SciTech Connect

    Rittman, Dylan R.; Tracy, Cameron L.; Cusick, Alex B.; Abere, Michael J.; Yalisove, Steven M.; Torralva, Ben; Ewing, Rodney C.

    2015-04-27

    In order to investigate the response of materials to extreme conditions, there are several approaches to depositing extremely high concentrations of energy into very small volumes of material, including ultrafast laser and swift heavy ion (SHI) irradiation. In this study, crystalline-to-crystalline phase transformations in cubic Gd{sub 2}O{sub 3} and monoclinic ZrO{sub 2} have been investigated using ultrafast laser irradiation. The phases produced by the extreme conditions of irradiation were characterized by grazing incidence x-ray diffraction (GIXRD) and Raman spectroscopy. Gd{sub 2}O{sub 3} exhibited a cubic-to-monoclinic phase transformation, as evidenced by the appearance of the monoclinic (402{sup ¯}), (003), (310), and (112{sup ¯}) peaks in the GIXRD pattern and of four A{sub g} and three B{sub g} Raman modes. ZrO{sub 2} underwent a monoclinic-to-tetragonal phase transformation, as evidenced by the emergence of the tetragonal (101) peak in the GIXRD pattern and of E{sub g} and A{sub 1g} Raman modes. The new phases formed by ultrafast laser irradiation are high temperature polymorphs of the two materials. No evidence of amorphization was seen in the GIXRD data, though Raman spectroscopy indicated point defect accumulation. These results are identical to those produced by irradiation with SHIs, which also deposit energy in materials primarily through electronic excitation. The similarity in damage process and material response between ultrafast laser and SHI irradiation suggests a fundamental relationship between these two techniques.

  15. Ultrafast laser and amplifier sources

    NASA Astrophysics Data System (ADS)

    Rundquist, A.; Durfee, C.; Chang, Z.; Taft, G.; Zeek, E.; Backus, S.; Murnane, M. M.; Kapteyn, H. C.; Christov, I.; Stoev, V.

    1997-08-01

    There has been remarkable progress in the development of high peak-power ultrafast lasers in recent years. Lasers capable of generating terawatt peak powers with unprecedented short pulse durations can now be built on a single optical table in a small laboratory. The rapid technological progress has made possible a host of new scientific advances in high-field science, such as the generation of coherent femtosecond X-ray pulses, and the generation of MeV-energy electron beams and high-energy ions. In this paper, we review progress in the development and design of ultrafast high-power lasers based on Ti:sapphire, including the ultrafast laser oscillators that are a very important enabling technology for high-power ultrafast systems, and ultrafast amplified laser systems that generate 20 fs duration pulses with several watts average power at kilohertz repetition-rates. Ultrafast waveform measurements of these pulses demonstrate that such short pulses can be generated with high fidelity. Finally, we discuss applications of ultrafast high-power pulses, including the generation of femtosecond to attosecond X-ray pulses.

  16. Ultrafast electron transfer at organic semiconductor interfaces: Importance of molecular orientation

    DOE PAGESBeta

    Ayzner, Alexander L.; Nordlund, Dennis; Kim, Do -Hwan; Bao, Zhenan; Toney, Michael F.

    2014-12-04

    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 approximatelymore » 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.« less

  17. Ultrafast electron transfer at organic semiconductor interfaces: Importance of molecular orientation

    SciTech Connect

    Ayzner, Alexander L.; Nordlund, Dennis; Kim, Do -Hwan; Bao, Zhenan; Toney, Michael F.

    2014-12-04

    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.

  18. Theory of ultrafast heterogeneous electron transfer: Contributions of direct charge transfer excitations to the absorbance

    NASA Astrophysics Data System (ADS)

    Wang, Luxia; Willig, Frank; May, Volkhard

    2007-04-01

    Absorption spectra related to heterogeneous electron transfer are analyzed with the focus on direct charge transfer transition from the surface attached molecule into the semiconductor band states. The computations are based on a model of reduced dimensionality with a single intramolecular vibrational coordinate but a complete account for the continuum of conduction band states. The applicability of this model to perylene on TiO2 has been demonstrated in a series of earlier papers. Here, based on a time-dependent formulation, the absorbance is calculated with the inclusion of charge transfer excitations. A broad parameter set inspired by the perylene TiO2 systems is considered. In particular, the description generalizes the Fano effect to heterogeneous electron transfer reactions. Preliminary simulations of measured spectra are presented for perylene-catechol attached to TiO2.

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

    PubMed

    Ayzner, Alexander L; Nordlund, Dennis; Kim, Do-Hwan; Bao, Zhenan; Toney, Michael F

    2015-01-01

    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. PMID:26263084

  20. Ultrafast Heme Dynamics of Ferric Cytochrome c in Different Environments: Electronic, Vibrational, and Conformational Relaxation.

    PubMed

    Karunakaran, Venugopal

    2015-12-21

    The excited-state dynamics of ferric cytochrome c (Cyt c), an important electron-transfer heme protein, in acidic to alkaline medium and in its unfolded form are investigated by using femtosecond pump-probe spectroscopy, exciting the heme and Tryptophan (Trp) to understand the electronic, vibrational, and conformational relaxation of the heme. At 390 nm excitation, the electronic relaxation of heme is found to be ≈150 fs at different pH values, increasing to 480 fs in the unfolded form. Multistep vibrational relaxation dynamics of the heme, including fast and slow processes, are observed at pH 7. However, in the unfolded form and at pH 2 and 11, fast phases of vibrational relaxation dominate, revealing the energy dissipation occurring through the covalent bond interaction between the heme and the nearest amino acids. A significant shortening of the excited-state lifetime of Trp is observed at various pH values at 280 nm excitation due to resonance energy transfer to the heme. The longer time constant (25 ps) observed in the unfolded form is attributed to a complete global conformational relaxation of Cyt c. PMID:26416435

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

    SciTech Connect

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

    2012-06-22

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

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

    NASA Astrophysics Data System (ADS)

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

    2002-01-01

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

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

    PubMed

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

    2016-07-01

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

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

    PubMed Central

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

    2016-01-01

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

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

    PubMed

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

    2013-01-01

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

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

    PubMed Central

    Yang, Ding-Shyue; Baum, Peter; Zewail, Ahmed H.

    2016-01-01

    Time-resolved electron diffraction with atomic-scale spatial and temporal resolution was used to unravel the transformation pathway in the photoinduced structural phase transition of vanadium dioxide. Results from bulk crystals and single-crystalline thin-films reveal a common, stepwise mechanism: First, there is a femtosecond V−V bond dilation within 300 fs, second, an intracell adjustment in picoseconds and, third, a nanoscale shear motion within tens of picoseconds. Experiments at different ambient temperatures and pump laser fluences reveal a temperature-dependent excitation threshold required to trigger the transitional reaction path of the atomic motions. PMID:27376103

  7. Ultrafast electron radiography of magnetic fields in high-intensity laser-solid interactions.

    PubMed

    Schumaker, W; Nakanii, N; McGuffey, C; Zulick, C; Chyvkov, V; Dollar, F; Habara, H; Kalintchenko, G; Maksimchuk, A; Tanaka, K A; Thomas, A G R; Yanovsky, V; Krushelnick, K

    2013-01-01

    Using electron bunches generated by laser wakefield acceleration as a probe, the temporal evolution of magnetic fields generated by a 4 × 10(19) W/cm(2) ultrashort (30 fs) laser pulse focused on solid density targets is studied experimentally. Magnetic field strengths of order B(0) ~ 10(4) T are observed expanding at close to the speed of light from the interaction point of a high-contrast laser pulse with a 10-μm-thick aluminum foil to a maximum diameter of ~1 mm. The field dynamics are shown to agree with particle-in-cell simulations. PMID:23383801

  8. Ultrafast electron diffraction pattern simulations using GPU technology. Applications to lattice vibrations.

    PubMed

    Eggeman, A S; London, A; Midgley, P A

    2013-11-01

    Graphical processing units (GPUs) offer a cost-effective and powerful means to enhance the processing power of computers. Here we show how GPUs can greatly increase the speed of electron diffraction pattern simulations by the implementation of a novel method to generate the phase grating used in multislice calculations. The increase in speed is especially apparent when using large supercell arrays and we illustrate the benefits of fast encoding the transmission function representing the atomic potentials through the simulation of thermal diffuse scattering in silicon brought about by specific vibrational modes. PMID:23770032

  9. Ultrafast electron dynamics in rare gas clusters under X-FEL light

    NASA Astrophysics Data System (ADS)

    Rost, Jan Michael; Gnodtke, Christian; Saalmann, Ulf

    2009-05-01

    Time resolved imaging with Angstrom resolution is one of the prime goals to use XFEL light for. Here we investigate in detail the dynamics of electrons and ions of a cluster exposed to a realistic X-FEL pulse. We focus on electron migration phenomena and investigate their role under the aspect of harm and benefit for imaging the cluster structure. Field ionization processes turn out to play an important role where the electric field is generated by quickly formed ions [1]. We also propose an experiment with double pulse of 1 fs duration each, separated by 10-100 fs which can be realized at LCLS in Stanford. With this pump-probe scenario, the dynamics of Auger processes in rare gas clusters (here Ne) can be studied which promises to be interesting since it differs from the isolated atom due to the neighboring ions/atoms [2]. [4pt] [1] Ch. Gnodtke, U. Saalmann, Jan M. Rost, submitted (2009).[0pt] [2] Ulf Saalmann and Jan M. Rost, Phys. Rev. Lett. 89, 143401 (2002).

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

    PubMed Central

    Frigge, T.; Hafke, B.; Tinnemann, V.; Witte, T.; Horn-von Hoegen, M.

    2015-01-01

    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. PMID:26798797

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

    NASA Astrophysics Data System (ADS)

    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

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

    PubMed

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

    2016-04-14

    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. PMID:26984120

  13. Direct observation of ultrafast surface transport of laser-driven fast electrons in a solid target

    NASA Astrophysics Data System (ADS)

    Singh, Prashant Kumar; Cui, Y. Q.; Chatterjee, Gourab; Adak, Amitava; Wang, W. M.; Ahmed, Saima; Lad, Amit D.; Sheng, Z. M.; Ravindra Kumar, G.

    2013-11-01

    We demonstrate rapid spread of surface ionization on a glass target excited by an intense, ultrashort laser pulse at an intensity of 3 × 1017 W cm-2. Time- and space-resolved reflectivity of the target surface indicates that the initial plasma region created by the pump pulse expands at c/7. The measured quasi-static megagauss magnetic field is found to expand in a manner very similar to that of surface ionization. Two-dimensional particle-in-cell simulations reproduce measurements of surface ionization and magnetic fields. Both the experiment and simulation convincingly demonstrate the role of self-induced electric and magnetic fields in confining fast electrons along the target-vacuum interface.

  14. Direct observation of ultrafast surface transport of laser-driven fast electrons in a solid target

    SciTech Connect

    Singh, Prashant Kumar; Chatterjee, Gourab; Adak, Amitava; Ahmed, Saima; Lad, Amit D.; Ravindra Kumar, G.; Cui, Y. Q.; Wang, W. M.; Sheng, Z. M.

    2013-11-15

    We demonstrate rapid spread of surface ionization on a glass target excited by an intense, ultrashort laser pulse at an intensity of 3 × 10{sup 17} W cm{sup −2}. Time- and space-resolved reflectivity of the target surface indicates that the initial plasma region created by the pump pulse expands at c/7. The measured quasi-static megagauss magnetic field is found to expand in a manner very similar to that of surface ionization. Two-dimensional particle-in-cell simulations reproduce measurements of surface ionization and magnetic fields. Both the experiment and simulation convincingly demonstrate the role of self-induced electric and magnetic fields in confining fast electrons along the target-vacuum interface.

  15. R4D on Ramp

    NASA Technical Reports Server (NTRS)

    1956-01-01

    This Photograph taken in 1956 shows the first of three R4D Skytrain aircraft on the ramp behind the NACA High-Speed Flight Station. Note the designation 'United States NACA' on the side of the aircraft. NACA stood for the National Advisory Committee for Aeronautics, which evolved into the National Aeronautics and Space Administration (NASA) in 1958. The R4D Skytrain was one of the early workhorses for NACA and NASA at Edwards Air Force Base, California, from 1952 to 1984. Designated the R4D by the U.S. Navy, the aircraft was called the C-47 by the U.S. Army and U.S. Air Force and the DC-3 by its builder, Douglas Aircraft. Nearly everyone called it the 'Gooney Bird.' In 1962, Congress consolidated the military-service designations and called all of them the C-47. After that date, the R4D at NASA's Flight Research Center (itself redesignated the Dryden Flight Research Center in 1976) was properly called a C-47. Over the 32 years it was used at Edwards, three different R4D/C-47s were used to shuttle personnel and equipment between NACA/NASA Centers and test locations throughout the country and for other purposes. One purpose was landing on 'dry' lakebeds used as alternate landing sites for the X-15, to determine whether their surfaces were hard (dry) enough for the X-15 to land on in case an emergency occurred after its launch and before it could reach Rogers Dry Lake at Edwards Air Force Base. The R4D/C-47 served a variety of needs, including serving as the first air-tow vehicle for the M2-F1 lifting body (which was built of mahogany plywood). The C-47 (as it was then called) was used for 77 tows before the M2-F1 was retired for more advanced lifting bodies that were dropped from the NASA B-52 'Mothership.' The R4D also served as a research aircraft. It was used to conduct early research on wing-tip-vortex flow visualization as well as checking out the NASA Uplink Control System. The first Gooney Bird was at the NACA High-Speed Flight Research Station (now the Dryden

  16. Ultrafast Electronic Energy Transfer Beyond the Weak Coupling Limit in a Proximal but Orthogonal Molecular Dyad.

    PubMed

    Hedley, Gordon J; Ruseckas, Arvydas; Benniston, Andrew C; Harriman, Anthony; Samuel, Ifor D W

    2015-12-24

    Electronic energy transfer (EET) from a donor to an acceptor is an important mechanism that controls the light harvesting efficiency in a wide variety of systems, including artificial and natural photosynthesis and contemporary photovoltaic technologies. The detailed mechanism of EET at short distances or large angles between the donor and acceptor is poorly understood. Here the influence of the orientation between the donor and acceptor on EET is explored using a molecule with two nearly perpendicular chromophores. Very fast EET with a time constant of 120 fs is observed, which is at least 40 times faster than the time predicted by Coulombic coupling calculations. Depolarization of the emission signal indicates that the transition dipole rotates through ca. 64°, indicating the near orthogonal nature of the EET event. The rate of EET is found to be similar to structural relaxation rates in the photoexcited oligothiophene donor alone, which suggests that this initial relaxation brings the dyad to a conical intersection where the excitation jumps to the acceptor. PMID:26617059

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

    SciTech Connect

    Zastrau, U.; Sperling, P.; Fortmann-Grote, C.; Bornath, T.; Bredow, R.; Doppner, T.; Fennel, T.; Fletcher, L. B.; Forster, E.; Gode, 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.; Tiggesbaumker, J.; Toleikis, S.; White, T. G.; Glenzer, S. H.; Redmer, R.; Tschentscher, T.

    2015-09-25

    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 $40\\;\\mathrm{eV}$ for simulated delay times up to $+70\\;\\mathrm{fs}$ 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. In conclusion, we resolved the time-scale for laser-heating of hydrogen, and PIC results for laser–matter interaction were successfully tested against the experiment data.

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

    DOE PAGESBeta

    Zastrau, U.; Sperling, P.; Fortmann-Grote, C.; Becker, A.; Bornath, T.; Bredow, R.; Doppner, T.; Fennel, T.; Fletcher, L. B.; Forster, E.; et al

    2015-09-25

    Dense cryogenic hydrogen is heated by intense femtosecond infrared laser pulses at intensities ofmore » $${10}^{15}-{10}^{16}\\;$$ 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 $$40\\;\\mathrm{eV}$$ for simulated delay times up to $$+70\\;\\mathrm{fs}$$ 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. In conclusion, we resolved the time-scale for laser-heating of hydrogen, and PIC results for laser–matter interaction were successfully tested against the experiment data.« less

  19. Ab initio nonadiabatic molecular dynamics of the ultrafast electron injection from a PbSe quantum dot into the TiO2 surface.

    PubMed

    Long, Run; Prezhdo, Oleg V

    2011-11-30

    Following recent experiments [Science 2010, 328, 1543; PNAS 2011, 108, 965], we report an ab initio nonadiabatic molecular dynamics (NAMD) simulation of the ultrafast photoinduced electron transfer (ET) from a PbSe quantum dot (QD) into the rutile TiO(2) (110) surface. The system forms the basis for QD-sensitized semiconductor solar cells and demonstrates that ultrafast interfacial ET is instrumental for achieving high efficiencies in solar-to-electrical energy conversion. The simulation supports the observation that the ET successfully competes with energy losses due to electron-phonon relaxation. The ET proceeds by the adiabatic mechanism because of strong donor-acceptor coupling. High frequency polar vibrations of both QD and TiO(2) promote the ET, since these modes can rapidly influence the donor-acceptor state energies and coupling. Low frequency vibrations generate a distribution of initial conditions for ET, which shows a broad variety of scenarios at the single-molecule level. Compared to the molecule-TiO(2) interfaces, the QD-TiO(2) system exhibits pronounced differences that arise due to the larger size and higher rigidity of QDs relative to molecules. Both donor and acceptor states are more delocalized in the QD system, and the ET is promoted by optical phonons, which have relatively low frequencies in the QD materials composed of heavy elements. In contrast, in molecular systems, optical phonons are not thermally accessible under ambient conditions. Meanwhile, TiO(2) acceptor states resemble surface impurities due to the local influence of molecular chromophores. At the same time, the photoinduced ET at both QD-TiO(2) and molecule-TiO(2) interfaces is ultrafast and occurs by the adiabatic mechanism, as a result of strong donor-acceptor coupling. The reported state-of-the-art simulation generates a detailed time-domain atomistic description of the interfacial ET process that is fundamental to a wide variety of applications. PMID:22007727

  20. Nondipole Effects in Xe 4d Photoemission

    SciTech Connect

    Hemmers, O; Guillemin, R; Wolska, A; Lindle, D W; Rolles, D; Cheng, K T; Johnson, W R; Zhou, H L; Manson, S T

    2004-07-14

    We measured the nondipole parameters for the spin-orbit doublets Xe 4d{sub 5/2} and Xe 4d{sub 3/2} over a photon-energy range from 100 eV to 250 eV at beamline 8.0.1.3 of the Advanced Light Source at the Lawrence Berkeley National Laboratory. Significant nondipole effects are found at relatively low energies as a result of Cooper minima in dipole channels and interchannel coupling in quadrupole channels. Most importantly, sharp disagreement between experiment and theory, when otherwise excellent agreement was expected, has provided the first evidence of satellite two-electron quadrupole photoionization transitions, along with their crucial importance for a quantitatively accurate theory.

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

    SciTech Connect

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

    2013-10-07

    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 O{sub 2}{sup −} 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

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

    NASA Astrophysics Data System (ADS)

    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

  3. Plasmonic enhanced ultrafast switch.

    SciTech Connect

    Subramania,Ganapathi Subramanian; Reno, John Louis; Passmore, Brandon Scott; Harris, Tom.; Shaner, Eric Arthur; Barrick, Todd A.

    2009-09-01

    Ultrafast electronic switches fabricated from defective material have been used for several decades in order to produce picosecond electrical transients and TeraHertz radiation. Due to the ultrashort recombination time in the photoconductor materials used, these switches are inefficient and are ultimately limited by the amount of optical power that can be applied to the switch before self-destruction. The goal of this work is to create ultrafast (sub-picosecond response) photoconductive switches on GaAs that are enhanced through plasmonic coupling structures. Here, the plasmonic coupler primarily plays the role of being a radiation condenser which will cause carriers to be generated adjacent to metallic electrodes where they can more efficiently be collected.

  4. PREFACE: Ultrafast biophotonics Ultrafast biophotonics

    NASA Astrophysics Data System (ADS)

    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

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

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

    PubMed

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

    2016-08-21

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

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

    PubMed

    Eita, Mohamed; Usman, Anwar; El-Ballouli, Ala'a O; Alarousu, Erkki; Bakr, Osman M; Mohammed, Omar F

    2015-01-01

    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. PMID:25163799

  8. Electron-phonon interactions in MoS{sub 2} probed with ultrafast two-dimensional visible/far-infrared spectroscopy

    SciTech Connect

    Guo, Xunmin; Chen, Hailong; Wen, Xiewen; Zheng, Junrong

    2015-06-07

    An ultrafast two-dimensional visible/far-IR spectroscopy based on the IR/THz air biased coherent detection method and scanning the excitation frequencies is developed. The method allows the responses in the far-IR region caused by various electronic excitations in molecular or material systems to be observed in real time. Using the technique, the relaxation dynamics of the photo-excited carriers and electron/phonon coupling in bulk MoS{sub 2} are investigated. It is found that the photo-generation of excited carriers occurs within two hundred fs and the relaxation of the carriers is tens of ps. The electron-phonon coupling between the excitations of electrons and the phonon mode E{sub 1u} of MoS{sub 2} is also directly observed. The electron excitation shifts the frequency of the phonon mode 9 cm{sup −1} higher, resulting in an absorption peak at 391 cm{sup −1} and a bleaching peak at 382 cm{sup −1}. The frequency shift diminishes with the relaxation of the carriers.

  9. Effect of high-optical excitation on the ultrafast electron dynamics in stacked-monolayer graphene samples

    NASA Astrophysics Data System (ADS)

    Castañeda, Juan A.; Guimarães Rosa, Henrique; Gomes, José C. V.; Thoroh de Souza, Eunezio A.; de Brito-Cruz, Carlos H.; Fragnito, Hugo L.; Padilha, Lázaro A.

    2016-05-01

    We report on transient absorption experiments performed at high optical excitation fluences and used to study the ultrafast dynamics in graphene. We employed a degenerated scheme of pump and probe at 800 nm (1.55 eV). The time resolution of our measurements was limited by the pulse duration ~ 100 fs. The samples were prepared by chemical vapor deposition (CVD) as single-layers on silica and, then staked layer-by-layer in order to make a stack of up to 5 graphene monolayers. We observed saturable absorption (SA) and fluence-dependent relaxation times. We see that the ultrafast carrier dynamics is composed by two decay mechanisms, one with response time of about 200 fs and a slower process of about 1 ps. The fast decay, due to both carrier-carrier and carrier-optical phonon scattering, becomes slower when the density of excited carrier was increased. We implemented a theoretical model and found that both the optical phonon rate emission and the optical phonon lifetime are affect by the pump fluence.

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

    PubMed

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

    2016-03-01

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

  11. Ultrafast Electronic and Vibrational Dynamics of Stabilized A State Mutants of the Green Fluorescent Protein (GFP): Snipping the Proton Wire

    PubMed Central

    Stoner-Ma, Deborah; Jaye, Andrew A.; Ronayne, Kate L.; Nappa, Jerome; Tonge, Peter J.; Meech, Stephen R.

    2008-01-01

    Two blue absorbing and emitting mutants (S65G/T203V/E222Q and S65T at pH 5.5) of the green fluorescent protein (GFP) have been investigated through ultrafast time resolved infra-red (TRIR) and fluorescence spectroscopy. In these mutants, in which the excited state proton transfer reaction observed in wild type GFP has been blocked, the photophysics are dominated by the neutral A state. It was found that the A* excited state lifetime is short, indicating that it is relatively less stabilised in the protein matrix than the anionic form. However, the lifetime of the A* state can be increased through modifications to the protein structure. The TRIR spectra show that a large shifts in protein vibrational modes on excitation of the A* state occurs in both these GFP mutants. This is ascribed to a change in H-bonding interactions between the protein matrix and the excited state. PMID:19554079

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

    PubMed

    Mohammed, Omar F; Xiao, Dequan; Batista, Victor S; Nibbering, Erik T J

    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 S2 electronic excited state is initially populated, followed by a rapid equilibration within 150 fs through population transfer to the S1 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. PMID:24684387

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

    NASA Astrophysics Data System (ADS)

    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

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

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

    PubMed

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

    2014-08-11

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

  16. 4-D OCT in Developmental Cardiology

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed

    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. PMID:27439363

  18. Ultrafast and steady-state laser heating effects on electron relaxation and phonon coupling mechanisms in thin gold films

    SciTech Connect

    Hopkins, Patrick E.; Duda, John C.; Kaehr, Bryan; Wang Zhou, Xiao; Peter Yang, C.-Y.; Jones, Reese E.

    2013-11-18

    We study the scattering mechanisms driving electron-phonon relaxation in thin gold films via pump-probe time-domain thermoreflectance. Electron-electron scattering can enhance the effective rate of electron-phonon relaxation when the electrons are out of equilibrium with the phonons. In order to correctly and consistently infer electron-phonon coupling factors in films on different substrates, we must account for the increase in steady-state lattice temperature due to laser heating. Our data provide evidence that a thermalized electron population will not directly exchange energy with the substrate during electron-phonon relaxation, whereas this pathway can exist between a non-equilibrium distribution of electrons and a non-metallic substrate.

  19. EDITORIAL: Ultrafast magnetization processes

    NASA Astrophysics Data System (ADS)

    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. 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

    PubMed Central

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

    2016-01-01

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

  1. Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5.

    PubMed

    Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G

    2015-01-01

    Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization. PMID:26314613

  2. Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5

    NASA Astrophysics Data System (ADS)

    Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G.

    2015-08-01

    Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization.

  3. Ultrafast time-resolved electron diffraction revealing the nonthermal dynamics of near-UV photoexcitation-induced amorphization in Ge2Sb2Te5

    PubMed Central

    Hada, Masaki; Oba, Wataru; Kuwahara, Masashi; Katayama, Ikufumi; Saiki, Toshiharu; Takeda, Jun; Nakamura, Kazutaka G.

    2015-01-01

    Because of their robust switching capability, chalcogenide glass materials have been used for a wide range of applications, including optical storages devices. These phase transitions are achieved by laser irradiation via thermal processes. Recent studies have suggested the potential of nonthermal phase transitions in the chalcogenide glass material Ge2Sb2Te5 triggered by ultrashort optical pulses; however, a detailed understanding of the amorphization and damage mechanisms governed by nonthermal processes is still lacking. Here we performed ultrafast time-resolved electron diffraction and single-shot optical pump-probe measurements followed by femtosecond near-ultraviolet pulse irradiation to study the structural dynamics of polycrystalline Ge2Sb2Te5. The experimental results present a nonthermal crystal-to-amorphous phase transition of Ge2Sb2Te5 initiated by the displacements of Ge atoms. Above the fluence threshold, we found that the permanent amorphization caused by multi-displacement effects is accompanied by a partial hexagonal crystallization. PMID:26314613

  4. 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.

    PubMed

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

    2016-01-01

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

  5. Partially coherent ultrafast spectrography

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

  6. Partially coherent ultrafast spectrography

    PubMed Central

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

    2015-01-01

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

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

    NASA Astrophysics Data System (ADS)

    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.

  8. Ultrafast electronic response of Ag(111) and Cu(111) surfaces: From early excitonic transients to saturated image potential

    NASA Astrophysics Data System (ADS)

    Silkin, V. M.; Lazić, P.; Došlić, N.; Petek, H.; Gumhalter, B.

    2015-10-01

    We investigate the evolution of attosecond to femtosecond screening and emergent potentials that govern the dynamics and energetics of electrons and holes excited in the various stages of multiphoton photoemission processes and control the photoelectron yield in recently reported experiments [X. Cui, C. Wang, A. Argondizzo, S. Garrett-Roe, B. Gumhalter, and H. Petek, Nat. Phys. 10, 505 (2014), 10.1038/nphys2981]. The study is focused on the dynamical screening of holes created in preexistent quasi-two-dimensional Shockley state bands on Ag(111) and Cu(111) surfaces and of electrons excited to the intermediate and emerging screened states. Using the formalism of self-consistent electronic response, we analyze first the effects of screening on the dynamics of photoexcited electrons and holes and then of the Coulomb correlated photoexcited pair. Special attention is paid to the correlated primary electron-hole states, which commence as transient surface excitons and develop in the course of screening into uncorrelated electrons and holes propagating in the image potential and surface state bands, respectively. The obtained results enable to establish a consistent picture of transient electron dynamics at Ag(111) and Cu(111) surfaces that are becoming accessible by the time-, energy-, and momentum-resolved pump-probe multiphoton photoelectron spectroscopies.

  9. Multielectron Spectroscopy: The Xenon 4d Hole Double Auger Decay

    SciTech Connect

    Penent, F.; Palaudoux, J.; Lablanquie, P.; Andric, L.; Feifel, R.; Eland, J.H.D.

    2005-08-19

    A magnetic bottle spectrometer of the type recently developed by Eland et al. [Phys. Rev. Lett. 90, 053003 (2003).] has been implemented for use with synchrotron radiation, allowing multidimensional electron spectroscopy. Its application to the Xe 4d double Auger decay reveals all the energy pathways involved. The dominant path is a cascade process with a rapid (6 fs) ejection of a first Auger electron followed by the slower (>23 fs) emission of a second Auger electron. Weaker processes implying 3 electron processes are also revealed, namely, direct double Auger and associated Rydberg series.

  10. Los Alamos National Laboratory 4D Database

    SciTech Connect

    Atencio, Julian J.

    2014-05-02

    4D is an integrated development platform - a single product comprised of the components you need to create and distribute professional applications. You get a graphical design environment, SQL database, a programming language, integrated PHP execution, HTTP server, application server, executable generator, and much more. 4D offers multi-platform development and deployment, meaning whatever you create on a Mac can be used on Windows, and vice-versa. Beyond productive development, 4D is renowned for its great flexibility in maintenance and modification of existing applications, and its extreme ease of implementation in its numerous deployment options. Your professional application can be put into production more quickly, at a lower cost, and will always be instantly scalable. 4D makes it easy, whether you're looking to create a classic desktop application, a client-server system, a distributed solution for Web or mobile clients - or all of the above!

  11. Computing Myocardial Motion in 4D Echocardiography

    PubMed Central

    Mukherjee, Ryan; Sprouse, Chad; Pinheiro, Aurélio; Abraham, Theodore; Burlina, Philippe

    2012-01-01

    4D (3D spatial+time) echocardiography is gaining widespread acceptance at clinical institutions for its high temporal resolution and relatively low cost. We describe a novel method for computing dense 3D myocardial motion with high accuracy. The method is based on a classical variational optical flow technique, but exploits modern developments in optical flow research to utilize the full capabilities of 4D echocardiography. Using a variety of metrics, we present an in-depth performance evaluation of the method on synthetic, phantom, and intraoperative 4D Transesophageal Echocardiographic (TEE) data. When compared with state-of-the-art optical flow and speckle tracking techniques currently found in 4D echocardiography, the method we present shows notable improvements in error. We believe the performance improvements shown can have a positive impact when the method is used as input for various applications, such as strain computation, biomechanical modeling, or automated diagnostics. PMID:22677256

  12. Indirect excitation of ultrafast demagnetization

    DOE PAGESBeta

    Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; Delaunay, Renaud; Müller, Leonard; Berntsen, Magnus H.; Grübel, Gerhard; Malinowski, Grégory; Weier, Christian; Gautier, Julien; et al

    2016-01-06

    Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset andmore » at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. As a result, our data thus confirm recent theoretical predictions.« less

  13. Indirect excitation of ultrafast demagnetization

    PubMed Central

    Vodungbo, Boris; Tudu, Bahrati; Perron, Jonathan; Delaunay, Renaud; Müller, Leonard; Berntsen, Magnus H.; Grübel, Gerhard; Malinowski, Grégory; Weier, Christian; Gautier, Julien; Lambert, Guillaume; Zeitoun, Philippe; Gutt, Christian; Jal, Emmanuelle; Reid, Alexander H.; Granitzka, Patrick W.; Jaouen, Nicolas; Dakovski, Georgi L.; Moeller, Stefan; Minitti, Michael P.; Mitra, Ankush; Carron, Sebastian; Pfau, Bastian; von Korff Schmising, Clemens; Schneider, Michael; Eisebitt, Stefan; Lüning, Jan

    2016-01-01

    Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. PMID:26733106

  14. Indirect excitation of ultrafast demagnetization.

    PubMed

    Vodungbo, Boris; Tudu, Bharati; Tudu, Bahrati; Perron, Jonathan; Delaunay, Renaud; Müller, Leonard; Berntsen, Magnus H; Grübel, Gerhard; Malinowski, Grégory; Weier, Christian; Gautier, Julien; Lambert, Guillaume; Zeitoun, Philippe; Gutt, Christian; Jal, Emmanuelle; Reid, Alexander H; Granitzka, Patrick W; Jaouen, Nicolas; Dakovski, Georgi L; Moeller, Stefan; Minitti, Michael P; Mitra, Ankush; Carron, Sebastian; Pfau, Bastian; von Korff Schmising, Clemens; Schneider, Michael; Eisebitt, Stefan; Lüning, Jan

    2016-01-01

    Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions. PMID:26733106

  15. On "new massive" 4D gravity

    NASA Astrophysics Data System (ADS)

    Bergshoeff, Eric A.; Fernández-Melgarejo, J. J.; Rosseel, Jan; Townsend, Paul K.

    2012-04-01

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

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

    PubMed

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

    2016-03-01

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

  17. Helical 4D CT and Comparison with Cine 4D CT

    NASA Astrophysics Data System (ADS)

    Pan, Tinsu

    4D CT was one of the most important developments in radiation oncology in the last decade. Its early development in single slice CT and commercialization in multi-slice CT has radically changed our practice in radiation treatment of lung cancer, and has enabled the stereotactic radiosurgery of early stage lung cancer. In this chapter, we will document the history of 4D CT development, detail the data sufficiency condition governing the 4D CT data collection; present the design of the commercial helical 4D CTs from Philips and Siemens; compare the differences between the helical 4D CT and the GE cine 4D CT in data acquisition, slice thickness, acquisition time and work flow; review the respiratory monitoring devices; and understand the causes of image artifacts in 4D CT.

  18. Two-photon photoemission spectra related to an ultrafast heterogeneous electron transfer from perylene to TiO2

    NASA Astrophysics Data System (ADS)

    Tsivlin, Dmitry V.; Willig, Frank; May, Volkhard

    2008-01-01

    Two-photon photoemission (2PPE) spectra related to sub- 100-fs heterogeneous electron transfer from perylene to TiO2 are calculated. The approach accounts for the dominant intramolecular vibration of perylene as well as for the band structure of TiO2 described in a tight-binding model. The focus is on the influence of the pump and probe laser pulse duration, with the pump laser originating charge injection and the probe laser causing the photoemission process. The latter may proceed directly from the photoexcited molecule or, after charge injection, from the TiO2 conduction band. The time-dependent Schrödinger equation which describes charge injection and accounts for the pump pulse is solved exactly within a time interval of about 250fs . The action of the probe pulse is considered in linear response theory. While the vibrational structure in the 2PPE spectra broadens with decreasing pump pulse length, it is found that this structure is largely preserved when varying the probe pulse duration. In order to estimate dephasing caused by intramolecular vibrational energy redistribution in perylene and electron phonon coupling in TiO2 , a density matrix scheme is also introduced describing heterogeneous electron transfer and the photoelectron emission processes. A finite escape depth for electrons at the TiO2 surface is finally taken into account to evaluate its influence on the spectra.

  19. Excitation laser energy dependence of surface-enhanced fluorescence showing plasmon-induced ultrafast electronic dynamics in dye molecules

    NASA Astrophysics Data System (ADS)

    Itoh, Tamitake; Yamamoto, Yuko S.; Tamaru, Hiroharu; Biju, Vasudevanpillai; Murase, Norio; Ozaki, Yukihiro

    2013-06-01

    We find unique properties accompanying surface-enhanced fluorescence (SEF) from dye molecules adsorbed on Ag nanoparticle aggregates, which generate surface-enhanced Raman scattering. The properties are observed in excitation laser energy dependence of SEF after excluding plasmonic spectral modulation in SEF. The unique properties are large blue shifts of fluorescence spectra, deviation of ratios between anti-Stokes SEF intensity and Stokes from those of normal fluorescence, super-broadening of Stokes spectra, and returning to original fluorescence by lower energy excitation. We elucidate that these properties are induced by electromagnetic enhancement of radiative decay rates exceeding the vibrational relaxation rates within an electronic excited state, which suggests that molecular electronic dynamics in strong plasmonic fields can be largely deviated from that in free space.

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

    PubMed

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

    2014-08-01

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

  1. Ultrafast Two-Electron Transfer in a CdS Quantum Dot-Extended-Viologen Cyclophane Complex.

    PubMed

    Young, Ryan M; Jensen, Stephen C; Edme, Kedy; Wu, Yilei; Krzyaniak, Matthew D; Vermeulen, Nicolaas A; Dale, Edward J; Stoddart, J Fraser; Weiss, Emily A; Wasielewski, Michael R; Co, Dick T

    2016-05-18

    Time-resolved optical spectroscopies reveal multielectron transfer from the biexcitonic state of a CdS quantum dot to an adsorbed tetracationic compound cyclobis(4,4'-(1,4-phenylene) bipyridin-1-ium-1,4-phenylene-bis(methylene)) (ExBox(4+)) to form both the ExBox(3+•) and the doubly reduced ExBox(2(+•)) states from a single laser pulse. Electron transfer in the single-exciton regime occurs in 1 ps. At higher excitation powers the second electron transfer takes ∼5 ps, which leads to a mixture of redox states of the acceptor ligand. The doubly reduced ExBox(2(+•)) state has a lifetime of ∼10 ns, while CdS(+•):ExBox(3+•) recombines with multiple time constants, the longest of which is ∼300 μs. The long-lived charge separation and ability to accumulate multiple charges on ExBox(4+) demonstrate the potential of the CdS:ExBox(4+) complex to serve as a platform for two-electron photocatalysis. PMID:27111529

  2. Thermodynamic picture of ultrafast charge transport in graphene

    NASA Astrophysics Data System (ADS)

    Mics, Zoltán; Tielrooij, Klaas-Jan; Parvez, Khaled; Jensen, Søren A.; Ivanov, Ivan; Feng, Xinliang; Müllen, Klaus; Bonn, Mischa; Turchinovich, Dmitry

    2015-07-01

    The outstanding charge transport properties of graphene enable numerous electronic applications of this remarkable material, many of which are expected to operate at ultrahigh speeds. In the regime of ultrafast, sub-picosecond electric fields, however, the very high conduction properties of graphene are not necessarily preserved, with the physical picture explaining this behaviour remaining unclear. Here we show that in graphene, the charge transport on an ultrafast timescale is determined by a simple thermodynamic balance maintained within the graphene electronic system acting as a thermalized electron gas. The energy of ultrafast electric fields applied to graphene is converted into the thermal energy of its entire charge carrier population, near-instantaneously raising the electronic temperature. The dynamic interplay between heating and cooling of the electron gas ultimately defines the ultrafast conductivity of graphene, which in a highly nonlinear manner depends on the dynamics and the strength of the applied electric fields.

  3. Ultra-fast framing camera tube

    DOEpatents

    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.

  4. Development and testing of gallium arsenide photoconductive detectors for ultra-fast, high dose rate electron and photon radiation measurements

    NASA Astrophysics Data System (ADS)

    Kharashvili, George

    Real time radiation dose measurements often present a challenge in high dose rate environments, like those needed for testing survivability of electronic devices or biological agents. Dosimetry needs at particle accelerator facilities require development of devices with fast (tens of picoseconds or less) response to pulsed radiation, linear response over a wide range of dose rates (up to 1011 Gy/s), high resistance to radiation damage, and successful operation in mixed gamma and neutron environments. Gallium arsenide photoconductive detectors (GaAs PCDs) have been shown to exhibit many of these desirable characteristics, especially the fast time response, when neutron irradiation is used to introduce displacement damage in the crystalline lattice of GaAs, hence improving the time response characteristics of the devices at the expense of their sensitivity. The objective of this project was to develop and test GaAs PCDs for ultra fast, high dose rate electron and bremsstrahlung radiation measurements. Effects of neutron pre-irradiation and detector size on the PCD properties were also investigated. GaAs PCDs with three different neutron irradiation levels (0, ˜1014, and 5 x 1015 n/cm 2 (1-MeV equivalent in GaAs) were fabricated. The devices were tested with 7, 20 and 38-MeV electron pulses produced by linear accelerators operating at the L-band frequency of 1.3-GHz and the S-band frequency of 2.8-GHz. In addition, detector responses at high dose rates were tested with 33-ns wide, 7-MeV maximum energy bremsstrahlung pulses produced by a pulse-power accelerator. The time response characteristics and the dose-rate ranges of application of the GaAs PCDs were determined. Several operational issues were identified. Recommendations on how to improve the PCD fabrication procedure and diagnostic capabilities for the high intensity radiation research are also discussed.

  5. 4D Bioprinting for Biomedical Applications.

    PubMed

    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. PMID:27056447

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

    ScienceCinema

    Margaret, Murnane [University of Colorado, Boulder and NIST

    2010-09-01

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

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

    SciTech Connect

    Margaret, Murnane

    2010-03-31

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

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

    SciTech Connect

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

    2010-03-15

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

  9. Ultrafast photodriven intramolecular electron transfer from an iridium-based water-oxidation catalyst to perylene diimide derivatives

    PubMed Central

    Vagnini, Michael T.; Smeigh, Amanda L.; Blakemore, James D.; Eaton, Samuel W.; Schley, Nathan D.; D’Souza, Francis; Crabtree, Robert H.; Brudvig, Gary W.; Co, Dick T.; Wasielewski, Michael R.

    2012-01-01

    Photodriving the activity of water-oxidation catalysts is a critical step toward generating fuel from sunlight. The design of a system with optimal energetics and kinetics requires a mechanistic understanding of the single-electron transfer events in catalyst activation. To this end, we report here the synthesis and photophysical characterization of two covalently bound chromophore-catalyst electron transfer dyads, in which the dyes are derivatives of the strong photooxidant perylene-3,4:9,10-bis(dicarboximide) (PDI) and the molecular catalyst is the Cp∗Ir(ppy)Cl metal complex, where ppy = 2-phenylpyridine. Photoexcitation of the PDI in each dyad results in reduction of the chromophore to PDI•- in less than 10 ps, a process that outcompetes any generation of 3∗PDI by spin-orbit-induced intersystem crossing. Biexponential charge recombination largely to the PDI-Ir(III) ground state is suggestive of multiple populations of the PDI•--Ir(IV) ion-pair, whose relative abundance varies with solvent polarity. Electrochemical studies of the dyads show strong irreversible oxidation current similar to that seen for model catalysts, indicating that the catalytic integrity of the metal complex is maintained upon attachment to the high molecular weight photosensitizer. PMID:22586073

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

    PubMed Central

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

    2015-01-01

    Aims To establish a framework to implement the 4D integrated extended cardiac torso (XCAT) digital phantom for 4D radiotherapy (RT) research. Materials and Methods A computer program was developed to facilitate the characterization and implementation of the 4D XCAT phantom. The program can (1) generate 4D XCAT images with customized parameter files; (2) review 4D XCAT images; (3) generate composite images from 4D XCAT images; (4) track motion of selected region-of-interested (ROI); (5) convert XCAT raw binary images into DICOM format; (6) analyse clinically acquired 4DCT images and real-time position management (RPM) respiratory signal. Motion tracking algorithm was validated by comparing with manual method. Major characteristics of the 4D XCAT phantom were studied. Results The comparison between motion tracking and manual measurements of lesion motion trajectory showed a small difference between them (mean difference in motion amplitude: 1.2 mm). The maximum lesion motion decreased nearly linearly (R2 = 0.97) as its distance to the diaphragm (DD) increased. At any given DD, lesion motion amplitude increased nearly linearly (R 2 range: 0.89 to 0.95) as the inputted diaphragm motion increased. For a given diaphragm motion, the lesion motion is independent of the lesion size at any given DD. The 4D XCAT phantom can closely reproduce irregular breathing profile. The end-to-end test showed that clinically comparable treatment plans can be generated successfully based on 4D XCAT images. 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. PMID:23361276

  11. Ultrafast soft x-ray two-dimensional plasma imaging system based on gas electron multiplier detector with pixel readout

    NASA Astrophysics Data System (ADS)

    Pacella, D.; Pizzicaroli, G.; Gabellieri, L.; Leigheb, M.; Bellazzini, R.; Brez, A.; Gariano, G.; Latronico, L.; Lumb, N.; Spandre, G.; Massai, M. M.; Reale, S.

    2001-02-01

    In the present article a new diagnostic device in the soft x-ray range, for magnetic fusion plasmas, is proposed based on a gas electron multiplier detector with 2.5×2.5 cm active area, equipped with a true two-dimensional readout system. The readout printed circuit board, designed for these experiments, has 128 pads. Each pad is 2 mm square and covers a roughly circular area. The operational conditions of the detector are settled to work in the x-ray range 3-15 keV at very high counting rates, with a linear response up to 2 MHz/pixel. This limitation is due to the electronic dead time. Images of a wrench and two pinholes were done at rates of 2.5 MHz/pixel with a powerful x-ray laboratory source showing an excellent imaging capability. Finally preliminary measurements of x-ray emission from a magnetic fusion plasma were performed on the Frascati tokamak upgrade experiment. The system was able to image the plasma with a wide dynamic range (more than a factor of 100), with a sampling frequency of 20 kHz and with counting rates up to 4 MHz/pixel, following the changes of the x-ray plasma emissivity due to additional radio frequency heating. The spatial resolution and imaging properties of this detector have been studied in this work for conditions of high counting rates and high gain, with the detector fully illuminated by very intense x-ray sources (laboratory tube and tokamak plasma).

  12. An Exact Formulation of Laser Assisted Electron Emission on a Biased Metal Surface

    NASA Astrophysics Data System (ADS)

    Zhang, Peng; Lau, Y. Y.; Ang, L. K.; Shiffler, D.; Jensen, K. L.; Gilgenbach, R. M.

    2015-11-01

    Laser-driven ultrafast electron emission is important to free electron lasers (FELs), laser acceleration of relativistic electrons, and ultrafast electron diffraction. It would enable exciting technological development on four-dimensional (4D) time-resolved electron microscopy. We constructed an analytic solution for the highly nonlinear electron emission from a metal surface that is exposed to both a dc biased electric field and a single frequency laser field. The solution is valid for arbitrary combinations of dc electric field, laser electric field, laser frequency, metal work function and Fermi level. Various emission mechanisms, such as multiphoton absorption or emission, optical or dc field emission, are all included in this single formulation. The time-dependent emission current reveals that intense current modulation may be possible even with a low intensity laser, by merely increasing the applied dc bias. This work was supported by AFOSR Grant No. FA9550-14-1-0309.

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

    NASA Technical Reports Server (NTRS)

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

    2008-01-01

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

  14. Order/Disorder Dynamics in a Dodecanethiol-Capped Gold Nanoparticles Supracrystal by Small-Angle Ultrafast Electron Diffraction.

    PubMed

    Mancini, Giulia Fulvia; Latychevskaia, Tatiana; Pennacchio, Francesco; Reguera, Javier; Stellacci, Francesco; Carbone, Fabrizio

    2016-04-13

    The design and the characterization of functionalized gold nanoparticles supracrystals require atomically resolved information on both the metallic core and the external organic ligand shell. At present, there is no known approach to characterize simultaneously the static local order of the ligands and of the nanoparticles, nor their dynamical evolution. In this work, we apply femtosecond small-angle electron diffraction combined with angular cross-correlation analysis, to retrieve the local arrangement from nanometer to interatomic scales in glassy aggregates. With this technique we study a two-dimensional distribution of functionalized gold nanoparticles deposited on amorphous carbon. We show that the dodecanethiol ligand chains, coating the gold cores, order in a preferential orientation on the nanoparticle surface and throughout the supracrystal. Furthermore, we retrieve the dynamics of the supracrystal upon excitation with light and show that the positional disorder is induced by light pulses, while its overall homogeneity is surprisingly found to transiently increase. This new technique will enable the systematic investigation of the static and dynamical structural properties of nanoassembled materials containing light elements, relevant for several applications including signal processing and biology. PMID:26918756

  15. 4D-Var Developement at GMAO

    NASA Technical Reports Server (NTRS)

    Pelc, Joanna S.; Todling, Ricardo; Akkraoui, Amal El

    2014-01-01

    The Global Modeling and Assimilation Offce (GMAO) is currently using an IAU-based 3D-Var data assimilation system. GMAO has been experimenting with a 3D-Var-hybrid version of its data assimilation system (DAS) for over a year now, which will soon become operational and it will rapidly progress toward a 4D-EnVar. Concurrently, the machinery to exercise traditional 4DVar is in place and it is desirable to have a comparison of the traditional 4D approach with the other available options, and evaluate their performance in the Goddard Earth Observing System (GEOS) DAS. This work will also explore the possibility for constructing a reduced order model (ROM) to make traditional 4D-Var computationally attractive for increasing model resolutions. Part of the research on ROM will be to search for a suitably acceptable space to carry on the corresponding reduction. This poster illustrates how the IAU-based 4D-Var assimilation compares with our currently used IAU-based 3D-Var.

  16. Constrained reconstructions for 4D intervention guidance

    NASA Astrophysics Data System (ADS)

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

    2013-05-01

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

  17. The structure of the inhibitory complex of alloxanthine (1H-pyrazolo[3,4-d]pyrimidine-4,6-diol) with the molybdenum centre of xanthine oxidase from electron-paramagnetic-resonance spectroscopy.

    PubMed Central

    Hawkes, T R; George, G N; Bray, R C

    1984-01-01

    Studies were carried out on the inhibitory complex of alloxanthine (1H-pyrazolo[3,4-d]pyrimidine-4,5-diol) with xanthine oxidase, in extension of the work of Williams & Bray [Biochem. J. (1981) 195, 753-760]. By suitable regulation of the reaction conditions, up to 10% of the functional enzyme could be converted into the complex in the Mo(V) oxidation state. The e.p.r. spectrum of the complex was investigated in detail with the help of computer simulation and substitution with stable isotopes. Close structural analogy of the signal-giving species to that of the Very Rapid intermediate in enzyme turnover is shown by g-values (2.0279, 1.9593 and 1.9442) and by coupling to 33S in the cyanide-labile site of the enzyme [A(33S) 0.30, 3.10 and 0.70mT]. However, whereas in the Very Rapid signal there is strong coupling to 17O [Gutteridge & Bray, Biochem. J. (1980) 189, 615-623], instead, in the Alloxanthine signal there is strong coupling to a single nitrogen atom [A(14N) 0.35, 0.35, 0.32 mT]. This is presumed to originate from the 2-position of the heterocyclic ring system. From this work and from earlier kinetic studies it is concluded that alloxanthine, after being bound reversibly at the active centre, reacts slowly with it, in a specific manner, distinct from that in the normal catalytic reaction with substrates. This reaction involves elimination of an oxygen ligand of molybdenum and co-ordination, in this site, of alloxanthine via the N-2 nitrogen atom, to give a complex that is structurally but not chemically closely analogous to that of the Very Rapid species. PMID:6326752

  18. Dual-tip-enhanced ultrafast CARS nanoscopy

    NASA Astrophysics Data System (ADS)

    Ballmann, Charles W.; Cao, Bin; Sinyukov, Alexander M.; Sokolov, Alexei V.; Voronine, Dmitri V.

    2014-08-01

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

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

    SciTech Connect

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

    2013-12-15

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

  20. R4D Parked on Ramp

    NASA Technical Reports Server (NTRS)

    1956-01-01

    This Photograph taken in 1956 shows the first of three R4D Skytrain aircraft on the ramp behind the NACA High-Speed Flight Station. NACA stood for the National Advisory Committee for Aeronautics, which evolved into the National Aeronautics and Space Administration (NASA) in 1958. The R4D Skytrain was one of the early workhorses for NACA and NASA at Edwards Air Force Base, California, from 1952 to 1984. Designated the R4D by the U.S. Navy, the aircraft was called the C-47 by the U.S. Army and U.S. Air Force and the DC-3 by its builder, Douglas Aircraft. Nearly everyone called it the 'Gooney Bird.' In 1962, Congress consolidated the military-service designations and called all of them the C-47. After that date, the R4D at NASA's Flight Research Center (itself redesignated the Dryden Flight Research Center in 1976) was properly called a C-47. Over the 32 years it was used at Edwards, three different R4D/C-47s were used to shuttle personnel and equipment between NACA/NASA Centers and test locations throughout the country and for other purposes. One purpose was landing on 'dry' lakebeds used as alternate landing sites for the X-15, to determine whether their surfaces were hard (dry) enough for the X-15 to land on in case an emergency occurred after its launch and before it could reach Rogers Dry Lake at Edwards Air Force Base. The R4D/C-47 served a variety of needs, including serving as the first air-tow vehicle for the M2-F1 lifting body (which was built of mahogany plywood). The C-47 (as it was then called) was used for 77 tows before the M2-F1 was retired for more advanced lifting bodies that were dropped from the NASA B-52 'Mothership.' The R4D also served as a research aircraft. It was used to conduct early research on wing-tip-vortex flow visualization as well as checking out the NASA Uplink Control System. The first Gooney Bird was at the NACA High-Speed Flight Research Station (now the Dryden Flight Research Center) from 1952 to 1956 and flew at least one cross

  1. Ultrafast laser IR countermeasures

    NASA Astrophysics Data System (ADS)

    Rafailov, Michael K.

    2009-05-01

    Directional Infrared Countermeasures (DIRCM) is an effective technique to defeat heat-seeking missiles. The major problem of existing DIRCM is that it may work like a beacon for threats that are not susceptible to the jamming code implemented: attracting a missile instead of re-directing it away from the aircraft. Ultra-fast laser pulse technology is discussed as an alternative to a conventional laser DIRCM. An ultra-fast laser is capable of providing a different type of countermeasure which is compatible with existing laser based DIRCM pointing systems as it requires much less peak power than damage inducing systems. A foundation of ultra-fast technology is its unique ability to alter the intrinsic characteristics of the semiconductor. In this paper, we will only consider the effects of a mild lattice disturbance caused by relatively low energy ultra-fast (femto-second) and, to some extent, fast (pico-second) laser pulses.

  2. Interactive animation of 4D performance capture.

    PubMed

    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. PMID:23492379

  3. Ultrafast scanning probe microscopy

    SciTech Connect

    Botkin, D.; Weiss, S.; Ogletree, D.F.; Salmeron, M.; Chemla, D.S.

    1994-01-01

    The authors have developed a general technique which combines the temporal resolution of ultrafast laser spectroscopy with the spatial resolution of scanned probe microscopy (SPM). Using this technique with scanning tunneling microscopy (STM), they have obtained simultaneous 2 ps time resolution and 50 {angstrom} spatial resolution. This improves the time resolution currently attainable with STM by nine orders of magnitude. The potential of this powerful technique for studying ultrafast dynamical phenomena on surfaces with atomic resolution is discussed.

  4. 4D image reconstruction for emission tomography

    NASA Astrophysics Data System (ADS)

    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

  5. Crystal growth and electronic phase diagram of 4 d -doped Na1 -δFe1 -xRhxAs in comparison to 3 d -dopedNa1 -δFe1 -xCoxAs

    NASA Astrophysics Data System (ADS)

    Steckel, Frank; Roslova, Maria; Beck, Robert; Morozov, Igor; Aswartham, Saicharan; Evtushinsky, Daniil; Blum, Christian G. F.; Abdel-Hafiez, Mahmoud; Bombor, Dirk; Maletz, Janek; Borisenko, Sergey; Shevelkov, Andrei V.; Wolter, Anja U. B.; Hess, Christian; Wurmehl, Sabine; Büchner, Bernd

    2015-05-01

    Single crystals of Na1 -δFe1 -xTxAs with T = Co, Rh have been grown using a self-flux technique. The crystals were thoroughly characterized by powder x-ray diffraction, magnetic susceptibility, and electronic transport with particular focus on the Rh-doped samples. Measurements of the specific heat and ARPES were conducted exemplarily for the optimally doped compositions. The spin-density wave transition (SDW) observed for samples with low Rh concentration (0 ≤x ≤0.013 ) is fully suppressed in the optimally doped sample. The superconducting transition temperature (Tc) is enhanced from 10 K in Na1 -δFeAs to 21 K in the optimally doped sample (x =0.019 ) of the Na1 -δFe1 -xRhxAs series and decreases for the overdoped compounds, revealing a typical shape for the superconducting part of the electronic phase diagram. Remarkably, the phase diagram is almost identical to that of Co-doped Na1 -δFeAs , suggesting a generic phase diagram for both dopants.

  6. Abdominal and pancreatic motion correlation using 4D CT, 4D transponders, and a gating belt.

    PubMed

    Betancourt, Ricardo; Zou, Wei; Plastaras, John P; Metz, James M; Teo, Boon-Keng; Kassaee, Alireza

    2013-01-01

    The correlation between the pancreatic and external abdominal motion due to respiration was investigated on two patients. These studies utilized four dimensional computer tomography (4D CT), a four dimensional (4D) electromagnetic transponder system, and a gating belt system. One 4D CT study was performed during simulation to quantify the pancreatic motion using computer tomography images at eight breathing phases. The motion under free breathing and breath-hold were analyzed for the 4D electromagnetic transponder system and the gating belt system during treatment. A linear curve was fitted for all data sets and correlation factors were evaluated between the 4D electromagnetic transponder system and the gating belt system data. The 4D CT study demonstrated a modest correlation between the external marker and the pancreatic motion with R-square values larger than 0.8 for the inferior-superior (inf-sup). Then, the relative pressure from the belt gating system correlated well with the 4D electromagnetic transponder system's motion in the anterior-posterior (ant-post) and the inf-post directions. These directions have a correlation value of -0.93 and 0.76, while the lateral only had a 0.03 correlation coefficient. Based on our limited study, external surrogates can be used as predictors of the pancreatic motion in the inf-sup and the ant-post directions. Although there is a low correlation on the lateral direction, its motion is significantly shorter. In conclusion, an appropriate treatment delivery can be used for pancreatic cancer when an internal tracking system, such as the 4D electromagnetic transponder system, is unavailable. PMID:23652242

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

    SciTech Connect

    Liu, Y; Yin, F; Cai, J

    2014-06-01

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

  8. Oblique sounding using the DPS-4D stations in Europe

    NASA Astrophysics Data System (ADS)

    Mosna, Zbysek; Kouba, Daniel; Koucka Knizova, Petra; Arikan, Feza; Arikan, Orhan; Gok, Gokhan; Rejfek, Lubos

    2016-07-01

    The DPS-4D Digisondes are capable of detection of echoes from neighbouring European stations. Currently, a campaign with high-temporal resolution of 5 min is being run. Further, ionograms from regular vertical sounding with 15 min resolution provide us with oblique reflections together with vertical reflections. We analyzed profiles of electron concentration and basic ionospheric parameters derived from the ionograms. We compared results derived from reflections from the ionosphere above the stations (vertical sounding) with information derived from oblique reflections between the stations. This study is supported by the Joint TUBITAK 114E092 and AS CR 14/001 projects.

  9. Active origami by 4D printing

    NASA Astrophysics Data System (ADS)

    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.

  10. Ultrafast infrared spectroscopy in photosynthesis.

    PubMed

    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. PMID:24973600

  11. Ultrafast studies of solution dynamics

    SciTech Connect

    Woodruff, W.H.; Dyer, R.B.; Callender, R.H.

    1997-10-01

    This is the final report of a one-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). Fast chemical dynamics generally must be initiated photochemically. This limits the applicability of modern laser methods for following the structural changes that occur during chemical and biological reactions to those systems that have an electronic chromophore that has a significant yield of photoproduct when excited. This project has developed a new and entirely general approach to ultrafast initiation of reactions in solution: laser-induced temperature jump (T-jump). The results open entire new fields of study of ultrafast molecular dynamics in solution. The authors have demonstrated the T-jump technique on time scales of 50 ps and longer, and have applied it to study of the fast events in protein folding. They find that a general lifetime of alpha-helix formation is ca 100 ns, and that tertiary folds (in apomyoglobin) form in ca 100 {mu}s.

  12. ICT4D: A Computer Science Perspective

    NASA Astrophysics Data System (ADS)

    Sutinen, Erkki; Tedre, Matti

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

  13. Controlled Source 4D Seismic Imaging

    NASA Astrophysics Data System (ADS)

    Luo, Y.; Morency, C.; Tromp, J.

    2009-12-01

    Earth's material properties may change after significant tectonic events, e.g., volcanic eruptions, earthquake ruptures, landslides, and hydrocarbon migration. While many studies focus on how to interpret observations in terms of changes in wavespeeds and attenuation, the oil industry is more interested in how we can identify and locate such temporal changes using seismic waves generated by controlled sources. 4D seismic analysis is indeed an important tool to monitor fluid movement in hydrocarbon reservoirs during production, improving fields management. Classic 4D seismic imaging involves comparing images obtained from two subsequent seismic surveys. Differences between the two images tell us where temporal changes occurred. However, when the temporal changes are small, it may be quite hard to reliably identify and characterize the differences between the two images. We propose to back-project residual seismograms between two subsequent surveys using adjoint methods, which results in images highlighting temporal changes. We use the SEG/EAGE salt dome model to illustrate our approach. In two subsequent surveys, the wavespeeds and density within a target region are changed, mimicking possible fluid migration. Due to changes in material properties induced by fluid migration, seismograms recorded in the two surveys differ. By back propagating these residuals, the adjoint images identify the location of the affected region. An important issue involves the nature of model. For instance, are we characterizing only changes in wavespeed, or do we also consider density and attenuation? How many model parameters characterize the model, e.g., is our model isotropic or anisotropic? Is acoustic wave propagation accurate enough or do we need to consider elastic or poroelastic effects? We will investigate how imaging strategies based upon acoustic, elastic and poroelastic simulations affect our imaging capabilities.

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

    ERIC Educational Resources Information Center

    Park, Sung Jin

    2013-01-01

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

  15. Distributed ultrafast fibre laser

    PubMed Central

    Liu, Xueming; Cui, Yudong; Han, Dongdong; Yao, Xiankun; Sun, Zhipei

    2015-01-01

    A traditional ultrafast fibre laser has a constant cavity length that is independent of the pulse wavelength. The investigation of distributed ultrafast (DUF) lasers is conceptually and technically challenging and of great interest because the laser cavity length and fundamental cavity frequency are changeable based on the wavelength. Here, we propose and demonstrate a DUF fibre laser based on a linearly chirped fibre Bragg grating, where the total cavity length is linearly changeable as a function of the pulse wavelength. The spectral sidebands in DUF lasers are enhanced greatly, including the continuous-wave (CW) and pulse components. We observe that all sidebands of the pulse experience the same round-trip time although they have different round-trip distances and refractive indices. The pulse-shaping of the DUF laser is dominated by the dissipative processes in addition to the phase modulations, which makes our ultrafast laser simple and stable. This laser provides a simple, stable, low-cost, ultrafast-pulsed source with controllable and changeable cavity frequency. PMID:25765454

  16. Vertical integration of ultrafast semiconductor lasers

    NASA Astrophysics Data System (ADS)

    Maas, D. J. H. C.; Bellancourt, A.-R.; Rudin, B.; Golling, M.; Unold, H. J.; Südmeyer, T.; Keller, U.

    2007-09-01

    Lasers generating short pulses - referred to as ultrafast lasers - enable many applications in science and technology. Numerous laboratory experiments have confirmed that ultrafast lasers can significantly increase telecommunication data rates [1], improve computer interconnects, and optically clock microprocessors [2, 3]. New applications in metrology [4], supercontinuum generation [5], and life sciences with two-photon microscopy [6] only work with ultrashort pulses but have relied on bulky and complex ultrafast solid-state lasers. Semiconductor lasers are ideally suited for mass production and widespread applications, because they are based on a wafer-scale technology with a high level of integration. Not surprisingly, the first lasers entering virtually every household were semiconductor lasers in compact disk players. Here we introduce a new concept and make the first feasibility demonstration of a new class of ultrafast semiconductor lasers which are power scalable, support both optical and electrical pumping and allow for wafer-scale fabrication. The laser beam propagates vertically (perpendicularly) through the epitaxial layer structure which has both gain and absorber layers integrated. In contrast to edge-emitters, these lasers have semiconductor layers that can be optimized separately by using different growth parameters and with no regrowth. This is especially important to integrate the gain and absorber layers, which require different quantum confinement. A saturable absorber is required for pulse generation and we optimized its parameters with a single self-assembled InAs quantum dot layer at low growth temperatures. We refer to this class of devices as modelocked integrated external-cavity surface emitting lasers (MIXSEL). Vertical integration supports a diffraction-limited circular output beam, transform-limited pulses, lower timing jitter, and synchronization to an external electronic clock. The pulse repetition rate scales from 1-GHz to 100-GHz by

  17. Four-dimensional electron microscopy.

    PubMed

    Zewail, Ahmed H

    2010-04-01

    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. PMID:20378810

  18. Four-Dimensional Electron Microscopy

    NASA Astrophysics Data System (ADS)

    Zewail, Ahmed H.

    2010-04-01

    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.

  19. Time-resolved spectroscopy of CI and CII line emissions from an ultrafast laser induced solid graphite plasma

    SciTech Connect

    N, Smijesh; K, Chandrasekharan; Philip, Reji

    2014-10-15

    We present an experimental characterization of the evolution dynamics of CI and CII lines in an ultrafast laser produced graphite plasma under various ambient conditions. Fast and slow components are observed in the temporal evolution of CI transition at 658.7 nm (3p{sup 1}P - 4d{sup 1}P{sup 0}) and CII transition at 426.7 nm (3d {sup 2}D - 4f {sup 2}F{sup 0}). Fast peak is due to the recombination of fast ions species with electrons, found to have an increase in velocity upon increasing the ambient pressure. Whereas the slow peaks in both cases can be the results of slow ions or slow neutrals in the plume.

  20. Time-resolved spectroscopy of CI and CII line emissions from an ultrafast laser induced solid graphite plasma

    NASA Astrophysics Data System (ADS)

    N, Smijesh; K, Chandrasekharan; Philip, Reji

    2014-10-01

    We present an experimental characterization of the evolution dynamics of CI and CII lines in an ultrafast laser produced graphite plasma under various ambient conditions. Fast and slow components are observed in the temporal evolution of CI transition at 658.7 nm (3p1P - 4d1P0) and CII transition at 426.7 nm (3d 2D - 4f 2F0). Fast peak is due to the recombination of fast ions species with electrons, found to have an increase in velocity upon increasing the ambient pressure. Whereas the slow peaks in both cases can be the results of slow ions or slow neutrals in the plume.

  1. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2013 CFR

    2013-04-01

    ... 17 Commodity and Securities Exchanges 3 2013-04-01 2013-04-01 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)...

  2. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2014 CFR

    2014-04-01

    ... 17 Commodity and Securities Exchanges 4 2014-04-01 2014-04-01 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)...

  3. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2010 CFR

    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)...

  4. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2011 CFR

    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)...

  5. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2014 CFR

    2011-04-01

    ... 17 Commodity and Securities Exchanges 3 2011-04-01 2011-04-01 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)...

  6. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2011 CFR

    2005-04-01

    ... 17 Commodity and Securities Exchanges 3 2005-04-01 2005-04-01 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)...

  7. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2014 CFR

    2000-04-01

    ... 17 Commodity and Securities Exchanges 3 2000-04-01 2000-04-01 false Content. 260.4d-8 Section 260.4d-8 Commodity and Securities Exchanges GENERAL RULES AND REGULATIONS, TRUST INDENTURE ACT OF 1939 Rules Under Section 304 § 260.4d-8 Content. (a) Each application for an order under section 304(d)...

  8. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2010 CFR

    2015-04-01

    ... 17 Commodity and Securities Exchanges 4 2015-04-01 2015-04-01 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)...

  9. Ultrafast opto-magnetism

    NASA Astrophysics Data System (ADS)

    Kalashnikova, A. M.; Kimel, A. V.; Pisarev, R. V.

    2015-10-01

    In the last decade, a new area of research, referred to as femtomagnetism, has developed within the field of magnetism, which studies the excitation and control of magnetic medium dynamics on time scales comparable to or even much shorter than those of spin-lattice, spin-orbit, and exchange interactions. Among the many femtomagnetic processes studied to date, the opto-magnetic interaction of femtosecond laser pulses with media is of particular interest. This interaction is based on nondissipative Raman-type mechanisms and enables coherent spin dynamics to be efficiently and selectively excited and its parameters to be controlled. This review considers the key features of ultrafast opto-magnetic phenomena and how they relate to magneto-optical effects. A number of experimentally observed examples of ultrafast spin dynamics excited via opto-magnetic inverse Faraday and Cotton-Mouton effects are considered, and their microscopical nature is discussed. An experimental example is given demonstrating that combining ultrafast opto-magnetic phenomena with other laser-induced processes allows magnetization to be controlled on a picosecond time scale.

  10. Ultrafast reduction of the total magnetization in iron

    SciTech Connect

    Fognini, A. Michlmayr, T. U.; Salvatella, G.; Vaterlaus, A.; Acremann, Y.; Wetli, C.; Sorgenfrei, F.; Beye, M.; Eschenlohr, A.; Pontius, N.; Föhlisch, A.; Stamm, C.; Hieke, F.; Dell'Angela, M.; Wurth, W.; Jong, S. de; Dürr, H. A.; and others

    2014-01-20

    Surprisingly, if a ferromagnet is exposed to an ultrafast laser pulse, its apparent magnetization is reduced within less than a picosecond. Up to now, the total magnetization, i.e., the average spin polarization of the whole valence band, was not detectable on a sub-picosecond time scale. Here, we present experimental data, confirming the ultrafast reduction of the total magnetization. Soft x-ray pulses from the free electron laser in Hamburg (FLASH) extract polarized cascade photoelectrons from an iron layer excited by a femtosecond laser pulse. The spin polarization of the emitted electrons is detected by a Mott spin polarimeter.

  11. Suppression of the molecular ultra-fast dissociation in bromomethane clusters

    SciTech Connect

    Rander, T.; Lindblad, A.; Bradeanu, I.; Svensson, S.; Björneholm, O.; Öhrwall, G.

    2014-12-14

    We address the influence of clustering on the ultra-fast dissociation of bromomethane. Valence and core photo-electron spectroscopy, partial electron yield absorption, and resonant Auger spectroscopy have been used together with ab initio calculations to investigate the properties of the ultra-fast dissociation. The ratio of ultra-fast dissociation of molecules in clusters as compared to free molecules is determined to be significantly reduced. We propose partial delocalization of the excited electronic state as being responsible for this behavior.

  12. Ultrafast photophysics of transition metal complexes.

    PubMed

    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

  13. Insight into water molecules bonding on 4d metal surfaces

    NASA Astrophysics Data System (ADS)

    Carrasco, Javier; Michaelides, Angelos; Scheffler, Matthias

    2008-03-01

    Water-metal interactions are of capital importance to a wide variety of phenomena in materials science, catalysis, corrosion, electrochemistry, etc. Here we address the nature of the bond between water molecules and metal surfaces through a careful systematic study. Specifically, the bonding of isolated water molecules to a series of close-packed transition metal surfaces - Ru(0001), Rh(111), Pd(111) and Ag(111) - has been examined in detail with density functional theory (DFT). Aiming to understand the origin behind energetic and structural trends along the 4d series we employ a range of analysis tools, such as decomposition of the density of states, electron density differences, electronic reactivity function and inspection of individual Kohn-Sham orbitals. The results obtained allow us to rationalize the bonding between water and transition metal surfaces as a balance of covalent and electrostatic interactions. A frontier orbital scheme based on so-called two-center four-electron interactions between molecular orbitals of water and d band states of the surface proves incisive in understanding these systems.

  14. Ultrafast Time-Resolved Photoelectric Emission.

    PubMed

    Juffmann, Thomas; Klopfer, Brannon B; Skulason, Gunnar E; Kealhofer, Catherine; Xiao, Fan; Foreman, Seth M; Kasevich, Mark A

    2015-12-31

    The emission times of laser-triggered electrons from a sharp tungsten tip are directly characterized under ultrafast, near-infrared laser excitation at Keldysh parameters of 6.6<γ<19.1. Emission delays up to 10 fs are observed, which are inferred from the energy gain of photoelectrons emitted into a synchronously driven microwave cavity. Few femtosecond timing resolution is achieved in a configuration capable of measuring timing shifts up to 55 ps. The technique can also be used to measure the microwave phase inside the cavity with a precision below 70 fs upon the energy resolved detection of a single electron. PMID:26764997

  15. Motion4D-library extended

    NASA Astrophysics Data System (ADS)

    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

  16. 17 CFR 260.4d-8 - Content.

    Code of Federal Regulations, 2011 CFR

    1998-04-01

    ... 17 Commodity and Securities Exchanges 3 1998-04-01 1998-04-01 false Content. 260.4d-8 Section 260.4d-8 GENERAL RULES AND REGULATIONS, TRUST INDENTURE ACT OF 1939 Rules Under Section 304 § 260.4d-8 Content. (a) Each application for an order under section 304(d) of the Act (15 U.S.C. 77ddd(d))...

  17. The 4D-TECS integration for NASA TSRV airplane

    NASA Technical Reports Server (NTRS)

    Kaminer, I.; Oshaughnessy, P. R.

    1989-01-01

    The integration of the Total Energy Control System (TECS) concept with 4D navigation is described. This integration was made to increase the operational capacity of modern aircraft and encourage incorporation of this increased capability with the evolving National Airspace System (NAS). Described herein is: 4D smoothing, the basic concepts of TECS, the spoiler integration concept, an algorithm for nulling out time error, speed and altitude profile modes, manual spoiler implementation, 4D logic, and the results of linear and nonlinear analysis.

  18. Killing Weeds with 2,4-D. Extension Bulletin 389.

    ERIC Educational Resources Information Center

    Lee, Oliver C.

    Discussed is the use of the herbicide 2,4-D. Though written for farmers and agricultural workers, the pamphlet considers turf weed control and use of 2,4-D near ornamental plants. Aspects of the use of this herbicide covered are: (1) the common forms of 2,4-D; (2) plant responses and tolerances to the herbicide; (3) dilution and concentration of…

  19. Pros and cons for C4d as a biomarker.

    PubMed

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

    2012-04-01

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

  20. Ultrafast microchannel plate photomultipliers.

    PubMed

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

    1988-03-15

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

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

    SciTech Connect

    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.

  2. Phosphodiesterase 4D Inhibitors Limit Prostate Cancer Growth Potential

    PubMed Central

    Powers, Ginny L.; Hammer, Kimberly D.P.; Domenech, Maribella; Frantskevich, Katsiaryna; Malinowski, Rita L.; Bushman, Wade; Beebe, David J.; Marker, Paul C.

    2014-01-01

    Phosphodiesterase 4D (PDE4D) has recently been implicated as a proliferation-promoting factor in prostate cancer and is over-expressed in human prostate carcinoma. However, the effects of PDE4D inhibition using pharmacological inhibitors have not been examined in prostate cancer. These studies examined the effects of selective PDE4D inhibitors, NVP-ABE171 and cilomilast, as anti-prostate cancer therapies in both in vitro and in vivo models. The effects of PDE4D inhibitors on pathways that are critical in prostate cancer and/or downstream of cyclic AMP (cAMP) were examined. Both NVP-ABE171 and cilomilast decreased cell growth. In vitro, PDE4D inhibitors lead to decreased signaling of the sonic hedgehog (SHH), Androgen Receptor (AR), and MAPK pathways, but growth inhibition was best correlated to the sonic hedgehog pathway. PDE4D inhibition also reduced proliferation of epithelial cells induced by paracrine signaling from co-cultured stromal cells that had activated hedgehog signaling. In addition, PDE4D inhibitors decreased the weight of the prostate in wild-type mice. Prostate cancer xenografts grown in nude mice that were treated with cilomilast or NVP-ABE171 had decreased wet weight and increased apoptosis compared to vehicle treated controls. These studies suggest the pharmacological inhibition of PDE4D using small molecule inhibitors is an effective option for prostate cancer therapy. Implications PDE4D inhibitors decrease the growth of prostate cancer cells in vivo and in vitro, and PDE4D inhibition has therapeutic potential in prostate cancer. PMID:25149359

  3. Effect of an ultrafast laser induced plasma on a relativistic electron beam to determine temporal overlap in pump-probe experiments.

    PubMed

    Scoby, Cheyne M; Li, R K; Musumeci, P

    2013-04-01

    In this paper we report on a simple and robust method to measure the absolute temporal overlap of the laser and the electron beam at the sample based on the effect of a laser induced plasma on the electron beam transverse distribution, successfully extending a similar method from keV to MeV electron beams. By pumping a standard copper TEM grid to form the plasma, we gain timing information independent of the sample under study. In experiments discussed here the optical delay to achieve temporal overlap between the pump electron beam and probe laser can be determined with ~1 ps precision. PMID:22951263

  4. Ultrafast scanning tunneling microscopy

    SciTech Connect

    Botkin, D.A. |

    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.

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

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed

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

    2016-05-27

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

  7. Fourier information optics for the ultrafast time domain.

    PubMed

    Weiner, Andrew M

    2008-02-01

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

  8. 32 CFR 1645.4 - Exclusion from Class 4-D.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 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...

  9. 32 CFR 1645.4 - Exclusion from Class 4-D.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 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...

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

    Code of Federal Regulations, 2011 CFR

    2011-07-01

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

  11. 32 CFR 1645.4 - Exclusion from Class 4-D.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 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...

  12. 32 CFR 1645.4 - Exclusion from Class 4-D.

    Code of Federal Regulations, 2010 CFR

    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...

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

    PubMed

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

    2006-01-15

    The energy transfer and charge separation kinetics in several core Photosystem I particles of Chlamydomonas reinhardtii with point mutations around the PA and PB reaction center chlorophylls (Chls) have been studied using ultrafast transient absorption spectroscopy in the femtosecond to nanosecond time range to characterize the influence on the early electron transfer processes. The data have been analyzed in terms of kinetic compartment models. The adequate description of the transient absorption kinetics requires three different radical pairs in the time range up to approximately 100 ps. Also a charge recombination process from the first radical pair back to the excited state is present in all the mutants, as already shown previously for the wild-type (Müller, M. G., J. Niklas, W. Lubitz, and A. R. Holzwarth. 2003. Biophys. J. 85:3899-3922; and Holzwarth, A. R., M. G. Müller, J. Niklas, and W. Lubitz. 2005. J. Phys. Chem. B. 109:5903-59115). In all mutants, the primary charge separation occurs with the same effective rate constant within the error limits as in the wild-type (>350 ns(-1)), which implies an intrinsic rate constant of charge separation of <1 ps(-1). The rate constant of the secondary electron transfer process is slowed down by a factor of approximately 2 in the mutant B-H656C, which lacks the ligand to the central metal of Chl PB. For the mutant A-T739V, which breaks the hydrogen bond to the keto carbonyl of Chl PA, only a slight slowing down of the secondary electron transfer is observed. Finally for mutant A-W679A, which has the Trp near the PA Chl replaced, either no pronounced effect or, at best, a slight increase on the secondary electron transfer rate constants is observed. The effective charge recombination rate constant is modified in all mutants to some extent, with the strongest effect observed in mutant B-H656C. Our data strongly suggest that the Chls of the PA and PB pair, constituting what is traditionally called the "primary electron

  14. Spin current generated by thermally driven ultrafast demagnetization.

    PubMed

    Choi, Gyung-Min; Min, Byoung-Chul; Lee, Kyung-Jin; Cahill, David G

    2014-01-01

    Spin current is the key element for nanoscale spintronic devices. For ultrafast operation of such nano-devices, generation of spin current in picoseconds, a timescale that is difficult to achieve using electrical circuits, is highly desired. Here we show thermally driven ultrafast demagnetization of a perpendicular ferromagnet leads to spin accumulation in a normal metal and spin transfer torque in an in-plane ferromagnet. The data are well described by models of spin generation and transport based on differences and gradients of thermodynamic parameters. The temperature difference between electrons and magnons is the driving force for spin current generation by ultrafast demagnetization. On longer timescales, a few picoseconds following laser excitation, we also observe a small contribution to spin current by a temperature gradient and the spin-dependent Seebeck effect. PMID:25007978

  15. Femtosecond laser studies of ultrafast intramolecular processes

    SciTech Connect

    Hayden, C.

    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.

  16. Ultrafast Strain Engineering in Complex Oxide Heterostructures

    NASA Astrophysics Data System (ADS)

    Caviglia, A. D.; Scherwitzl, R.; Popovich, P.; Hu, W.; Bromberger, H.; Singla, R.; Mitrano, M.; Hoffmann, M. C.; Kaiser, S.; Zubko, P.; Gariglio, S.; Triscone, J.-M.; Först, M.; Cavalleri, A.

    2012-03-01

    We report on ultrafast optical experiments in which femtosecond midinfrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO3 epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates.

  17. Ultrafast strain engineering in complex oxide heterostructures.

    PubMed

    Caviglia, A D; Scherwitzl, R; Popovich, P; Hu, W; Bromberger, H; Singla, R; Mitrano, M; Hoffmann, M C; Kaiser, S; Zubko, P; Gariglio, S; Triscone, J-M; Först, M; Cavalleri, A

    2012-03-30

    We report on ultrafast optical experiments in which femtosecond midinfrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO(3) epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates. PMID:22540718

  18. Theoretical studies of the external vibrational control of electronic excitation transfer and its observation using polarization- and optical phase-sensitive ultrafast spectroscopy

    NASA Astrophysics Data System (ADS)

    Biggs, Jason Daniel

    Our theoretical studies involve the control of electronic energy transfer in molecular dimers through the preparation of specific vibrational coherences prior to electronic excitation. Our control strategy is based upon the fact that, following impulsive electronic excitation, nuclear motion acts to change the instantaneous energy difference between site-excited electronic states and thereby influences short-time electronic excitation transfer (EET). By inducing coherent intramolecular vibration in one of the chromophores prior to short-pulse electronic excitation, we exert external control over electronic dynamics. As a means to monitor this coherent control over EET, we propose using multidimensional wave-packet interferometry (md-WPI). Two pairs of polarized phase-related femtosecond pulses following the control pulse would generate superpositions of coherent nuclear wave packets in optically accessible electronic states. Interference contributions to the time- and frequency-integrated fluorescence signal due to overlaps among the superposed wave packets provide amplitude-level information on the nuclear and electronic dynamics. We test both the control strategy and its spectroscopic investigation by calculating pump-probe difference signals for various combinations of pulse polarizations. That signal is the limiting case of the control-influenced md-WPI signal in which the two pulses in the pump pulse-pair coincide, as do the two pulses in the probe pulse-pair. We present calculated pump-probe difference signals for a variety of systems including a simplified model of the covalent dimer dithia-anthracenophane (DTA) in which we treat only the weakly Franck-Condon active nu12 anthracene vibration at 385 cm-1. We further present calculated nl-WPI difference signals for an oriented DTA complex, which reveal amplitude-level dynamical information about the interaction of nuclear motion and electronic energy transfer. We also present pump-probe difference signals from

  19. Rational material design for ultrafast rechargeable lithium-ion batteries.

    PubMed

    Tang, Yuxin; Zhang, Yanyan; Li, Wenlong; Ma, Bing; Chen, Xiaodong

    2015-10-01

    Rechargeable lithium-ion batteries (LIBs) are important electrochemical energy storage devices for consumer electronics and emerging electrical/hybrid vehicles. However, one of the formidable challenges is to develop ultrafast charging LIBs with the rate capability at least one order of magnitude (>10 C) higher than that of the currently commercialized LIBs. This tutorial review presents the state-of-the-art developments in ultrafast charging LIBs by the rational design of materials. First of all, fundamental electrochemistry and related ionic/electronic conduction theories identify that the rate capability of LIBs is kinetically limited by the sluggish solid-state diffusion process in electrode materials. Then, several aspects of the intrinsic materials, materials engineering and processing, and electrode materials architecture design towards maximizing both ionic and electronic conductivity in the electrode with a short diffusion length are deliberated. Finally, the future trends and perspectives for the ultrafast rechargeable LIBs are discussed. Continuous rapid progress in this area is essential and urgent to endow LIBs with ultrafast charging capability to meet huge demands in the near future. PMID:25857819

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

    NASA Astrophysics Data System (ADS)

    Magrakvelidze, Maia; Madjet, Mohamed El-Amine; Chakraborty, Himadri S.

    2016-07-01

    A Kohn-Sham time-dependent local-density-functional scheme is utilized to predict attosecond time delays of xenon 4 d photoionization that involves the 4 d 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), 10.1103/PhysRevA.91.033413]. For the Cooper minimum, a qualitative similarity with a photorecombination experiment near argon 3 p minimum [S. B. Schoun et al., Phys. Rev. Lett. 112, 153001 (2014), 10.1103/PhysRevLett.112.153001] is found. The result should encourage attosecond measurements of Xe 4 d photoemission.

  1. Fast 4D segmentation of large datasets using graph cuts

    NASA Astrophysics Data System (ADS)

    Lombaert, Herve; Sun, Yiyong; Cheriet, Farida

    2011-03-01

    In this paper, we propose to use 4D graph cuts for the segmentation of large spatio-temporal (4D) datasets. Indeed, as 4D datasets grow in popularity in many clinical areas, so will the demand for efficient general segmentation algorithms. The graph cuts method1 has become a leading method for complex 2D and 3D image segmentation in many applications. Despite a few attempts2-5 in 4D, the use of graph cuts on typical medical volume quickly exceeds today's computer capacities. Among all existing graph cuts based methods6-10 the multilevel banded graph cuts9 is the fastest and uses the least amount of memory. Nevertheless, this method has its limitation. Memory becomes an issue when using large 4D volume sequences, and small structures become hardly recoverable when using narrow bands. We thus improve the boundary refinement efficiency by using a 4D competitive region growing. First, we construct a coarse graph at a low resolution with strong temporal links to prevent the shrink bias inherent to the graph cuts method. Second, we use a competitive region growing using a priority queue to capture all fine details. Leaks are prevented by constraining the competitive region growing within a banded region and by adding a viscosity term. This strategy yields results comparable to the multilevel banded graph cuts but is faster and allows its application to large 4D datasets. We applied our method on both cardiac 4D MRI and 4D CT datasets with promising results.

  2. Searching for solvent cavities via electron photodetachment: The ultrafast charge-transfer-to-solvent dynamics of sodide in a series of ether solvents

    SciTech Connect

    Larsen, Molly C.; Schwartz, Benjamin J.

    2009-10-21

    It was recently predicted by simulations and confirmed by neutron diffraction experiments that the structure of liquid tetrahydrofuran (THF) contains cavities. The cavities can be quite large and have a net positive electrostatic potential, so they can serve as pre-existing traps for excess electrons created via photodetachment from various solutes. In this paper, we use electron photodetachment via charge-transfer-to-solvent (CTTS) excitation of sodide (Na{sup -}) to probe for the presence of pre-existing cavities in a series of ether solvents: THF, diethyl ether, 1,2-dimethoxyethane (DME), and diglyme (DG). We find that electrons photodetached from sodide appear after a time delay with their equilibrium spectrum in all of these solvents, suggesting that the entire series of ethers contains pre-existing solvent cavities. We then use the variation in electron recombination dynamics with CTTS excitation wavelength to probe the nature of the cavities in the different ethers. We find that the cavities that form the deepest electron traps turn on at about the same energy in all four ether solvents investigated, but that the density of cavities is lower in DG and DME than in THF. We also examine the dynamics of the neutral sodium species that remains following CTTS photodetachment of an electron from sodide. We find that the reaction of the initially created gas-phase-like Na atom to form a (Na{sup +},e{sup -}) tight-contact pair occurs at essentially the same rate in all four ether solvents, indicating that only local solvent motions and not bulk solvent rearrangements are what is responsible for driving the partial ejection of the remaining Na valence electron.

  3. Quarterly progress report for Q2 FY06 for Complex Transient Events in Materials Studied Using Ultrafast Electron Probes and Terascale Simulation (FWP SCW0289)

    SciTech Connect

    Campbell, G H

    2006-03-29

    In this quarter (Q2 FY06), the DTEM underwent a substantial reconfiguration of its laser systems. The cathode laser system was changed to provide greater numbers of electrons per pulse by lengthening the time duration of the pulse to 30 ns. The greater number of electrons per pulse has allowed us to acquire high quality pulsed images and diffraction patterns. The spatial resolution in the single pulsed image has been measured at better than 20 nm. The diffraction patterns are now more comparable to conventional electron microscope operation. Examples are found in the body of the report. We summarize important achievements in the following list: (1) Instrument performance and design improvements--(A) The laser system was changed for the cathode photoemission system (75 ns at 1053 nm wavelength converted to 30ns at 211 nm wavelength) to give longer electron pulses at the same current to yield more electrons per pulse. (B) New specimen drive laser constructed. (C) New computer monitored and controlled alignment systems installed for both laser systems to facilitate laser alignment through a user friendly computer interface. (2) Experimental Progress--(A) The spatial resolution of pulsed images was tested by imaging a cross-section of multilayer thin foils with 30 nm and 20 nm periods. Single pulse images were observed to have spatial resolution better than 20 nm. This combination of 20 nm spatial and 30 ns temporal resolution is thought to be highest combined spatial and temporal measurement ever made. (B) The quality of single pulse electron diffraction patterns have been improved to the point where differentiating the HCP from BCC patterns in Ti is substantially easier. The spatial coherence of the electron illumination on the specimen was improved to give much smaller diffraction spots in the pattern.

  4. Ultrafast lasers in ophthalmology

    NASA Astrophysics Data System (ADS)

    Lubatschowski, Holger

    Ultrafast laser pulses have become a promising tool for microsurgery of the eye. Due to the low energy threshold, side effects are limited to the micrometer range This precision enables the use of ultrashort laser pulses in a broad field of medical applications. Especially, the interaction process based on nonlinear absorption offers the opportunity to process transparent tissue not only on top of a surface but three dimensionally inside the bulk. This mechanism is used in refractive eye surgery, where fs pulses create flaps into the corneal tissue to remodel the curvature of the eye and to improve visual acuity. Moreover, fs pulses could be used to influence the biomechanics of the crystalline lens of the eye and improve accommodation on eyes who suffer from presbyopia.

  5. C4 Glomerulopathy: A Disease Entity Associated With C4d Deposition.

    PubMed

    Sethi, Sanjeev; Quint, Patrick S; O'Seaghdha, Conall M; Fervenza, Fernando C; Bijol, Vanesa; Dorman, Anthony; Dasari, Surendra; Smith, Richard J H; Kurtin, Paul J; Rennke, Helmut G

    2016-06-01

    Complement-mediated glomerulonephritis, which includes C3 glomerulopathy, is characterized by dominant staining of C3 with minimal or no immunoglobulin deposits on immunofluorescence studies. We describe a new entity of complement-mediated glomerulonephritis that is characterized by bright C4d staining but with no or minimal C3 or immunoglobulin deposits on immunofluorescence studies. We label this entity as C4 glomerulopathy. C4 glomerulopathy includes C4 dense deposit disease and C4 glomerulonephritis. C4 dense deposit disease is characterized by bright C4d staining and dense deposits along glomerular basement membranes. C4 glomerulonephritis is characterized by bright C4d staining and many mesangial electron-dense deposits, with or without rare intramembranous electron-dense deposits. We describe clinical features and kidney biopsy results in a short series of 3 patients to highlight these findings. All 3 patients presented with proteinuria, and 2 patients also had hematuria. Kidney function was preserved in 2 patients, whereas 1 patient presented with declining kidney function. Evaluation for autoimmune disease, infection, and paraprotein yielded negative results in all patients. Complement levels were normal, although 1 patient had borderline low C4 levels. Kidney biopsy showed mesangial proliferative or membranoproliferative glomerulonephritis with bright C4d staining and absent or minimal C1q, C3, and immunoglobulin. Laser microdissection and mass spectrometry of glomeruli in all 3 patients showed large to moderate numbers of spectra matching C4. Furthermore, analysis of amino acid sequences showed that they were localized to the C4d portion of C4, consistent with immunofluorescence findings. Further studies are required to determine the underlying cause. In summary, we describe a novel complement-mediated glomerulonephritis that is characterized by bright glomerular C4d staining with minimal or absent staining for C1q, C3, and immunoglobulin. PMID

  6. AttoPhotoChemistry. Probing ultrafast electron dynamics by the induced nuclear motion: The prompt and delayed predissociation of N2

    NASA Astrophysics Data System (ADS)

    Muskatel, B. H.; Remacle, F.; Levine, R. D.

    2014-05-01

    Quantum mechanical wavepacket dynamics simulation that includes the nuclear motion exhibit a prompt, few fs, dissociation of electronically attosecond excited N2 in addition to the slow dissociation evident from spectral line broadening in well resolved spectra. The simulations show that nuclear motion can probe early times electron dynamics. The separation of time scales is mimicked by a model study fashioned like chemical kinetics of unimolecular dissociation. The physical origin of the separation into prompt and delayed decay is argued to be the same in the vibrational and the present case, namely that there are more bound than dissociative channels.

  7. Real-time measurements of ultrafast electronic dynamics in the disproportionation of [TCNQ]22- using a visible sub-10 fs pulse laser

    NASA Astrophysics Data System (ADS)

    Hashimoto, Sena; Yabushita, Atsushi; Kobayashi, Takayoshi; Iwakura, Izumi

    2016-04-01

    The reduction of 7,7,8,8-tetracyanoquinodimethane (TCNQ) generates a π radical anion, TCNQrad -, that dimerizes in methanol solution. This dimer ([TCNQ]22-) exhibits a charge-transfer absorption peak at 620 nm and will disproportionate to give TCNQ and TCNQ2- in response to excitation within this charge-transfer band. The present study examined the electronic dynamics of [TCNQ]22- disproportionation. The disproportionation was found to proceed in two steps. Electron transfer, representing the first step, occurred within the 10 fs pulse window, followed by the actual dissociation, within 350 fs. The emission lifetime of the singlet excited state of TCNQ2- was estimated to be 900 fs.

  8. 4D-Var or Ensemble Kalman Filter

    NASA Astrophysics Data System (ADS)

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

    2007-05-01

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

  9. Low-power and ultrafast all-optical tunable plasmon-induced transparency in plasmonic nanostructures

    NASA Astrophysics Data System (ADS)

    Chai, Zhen; Hu, Xiaoyong; Zhu, Yu; Zhang, Fan; Yang, Hong; Gong, Qihuang

    2013-05-01

    We report an ultrafast and low-power all-optical tunable plasmon-induced transparency in a plasmonic nanostructure consisting of a gold nanowire grating embedded in a polycrystalline lithium niobate layer, realized based on strong quantum confinement enhancing nonlinearity. The all-optical tunability is realized based on the third-order nonlinear Kerr effect. A shift of 30 nm in the central wavelength of the transparency window is achieved under excitation of a pump light with an intensity as low as 7 MW/cm2. An ultrafast response time of 69 ps is reached because of ultrafast relaxation dynamics of bound electrons in polycrystalline lithium niobate.

  10. Ultrafast X-Ray Coherent Control

    SciTech Connect

    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.

  11. 4-D-Var or ensemble Kalman filter?

    NASA Astrophysics Data System (ADS)

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

    2007-10-01

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

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

    NASA Astrophysics Data System (ADS)

    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

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

    PubMed

    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

  14. Ultrafast and nonlinear optics in carbon nanomaterials.

    PubMed

    Kono, Junichiro

    2013-02-01

    Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton–phonon and exciton–plasmon interactions; exciton–exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz–Keldysh effects; and non-perturbative light–mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section

  15. Plasmonics: An ultrafast plasmonic tuning knob

    NASA Astrophysics Data System (ADS)

    Wagner, Martin; Liu, Mengkun

    2016-04-01

    Near- and mid-infrared plasmonics are exciting research areas with applications in nanoscale energy concentration, sensing or ultrafast switching for telecommunication. Now, a new efficient way to manipulate plasmon resonances in semiconductor nanoarrays at ultrafast timescales has been found.

  16. Ultrafast nonlinear acoustics in crystals and nanostructures

    NASA Astrophysics Data System (ADS)

    van Capel, P. J. S.

    2008-09-01

    This research aims at experimentally monitoring nonlinear generation and propagation of picosecond coherent acoustic strain wave packets in solids. The experiments are performed by ultrafast pump-probe reflectometry and interferometry. At first, nonlinear strain generation in thin nickel and chromium films is characterized. At high pump fluences, the elevated electron and lattice temperatures in the absorption layer significantly modify thermal and mechanical material parameters, thereby increasing the strain amplitude superlinearly. Electron diffusion is suppressed by electron-electron collisions. The results are accurately described by a two-temperature model for fluences up to 80% of the damage threshold, above which nonthermal processes come into play. At room temperature, the high-amplitude strain waves generated in a thin chromium film and launched into the sapphire substrate, transform into an acoustic shock wave within tens of micrometer due to large atomic displacements and the nonparabolic interatomic potential. When lowering the temperature, thermal attenuation gradually decreases and lattice dispersion comes into play. At 20 K, propagation is undamped, thus leading to the formation of acoustic solitons. A maximum number of seven solitons is measured. By performing measurements on different sample thicknesses, the superlinear soliton velocity can be determined. Since the soliton velocity is intimately linked to its spatial width, a soliton width as short as two nanometer can be derived. The measured soliton velocities and volumes are in excellent agreement with numerical simulations of propagation, as well with the exact predictions by the Korteweg - De Vries equation. Following the demonstration of acoustic solitons, an experiment was devised in which these solitons are used to modulate nanostructures on ultrafast timescales. Modulation of exciton states inside a semiconductor within times shorter than the exciton lifetime leads to chirping, i

  17. Manipulating magnetic anisotropy and ultrafast spin dynamics of magnetic nanostructures

    NASA Astrophysics Data System (ADS)

    Cheng, Zhao-Hua; He, Wei; Zhang, Xiang-Qun; Sun, Da-Li; Du, Hai-Feng; Wu, Qiong; Ye, Jun; Fang, Ya-Peng; Liu, Hao-Liang

    2015-07-01

    We present our extensive research into magnetic anisotropy. We tuned the terrace width of Si(111) substrate by a novel method: varying the direction of heating current and consequently manipulating the magnetic anisotropy of magnetic structures on the stepped substrate by decorating its atomic steps. Laser-induced ultrafast demagnetization of a CoFeB/MgO/CoFeB magnetic tunneling junction was explored by the time-resolved magneto-optical Kerr effect (TR-MOKE) for both the parallel state (P state) and the antiparallel state (AP state) of the magnetizations between two magnetic layers. It was observed that the demagnetization time is shorter and the magnitude of demagnetization is larger in the AP state than those in the P state. These behaviors are attributed to the ultrafast spin transfer between two CoFeB layers via the tunneling of hot electrons through the MgO barrier. Our observation indicates that ultrafast demagnetization can be engineered by the hot electron tunneling current. This opens the door to manipulate the ultrafast spin current in magnetic tunneling junctions. Furthermore, an all-optical TR-MOKE technique provides the flexibility for exploring the nonlinear magnetization dynamics in ferromagnetic materials, especially with metallic materials. Project supported by the National Basic Research Program of China (Grant Nos. 2015CB921403, 2011CB921801, and 2012CB933101) and the National Natural Science Foundation of China (Grant Nos. 51427801, 11374350, 51201179, and 11274361).

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

    PubMed

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

    2016-02-10

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

  19. Generation of sub-20 fs Tunable Visible Pulses from a 100 kHz NOPA For Measuring Ultrafast Heterogeneous Electron Transfer

    NASA Astrophysics Data System (ADS)

    Ernstorfer, R.; Gundlach, L.; Zimmermann, C.; Willig, F.; Eichberger, R.; Riedle, E.

    We describe the design and performance of a noncollinear optical parametric amplifier that can be pumped by the output of a commercial 100 kHz Ti:sapphire regenerative amplifier. The output of the NOPA is compressed to sub-20 fs length and tunable from 460 nm to beyond 1 pm. The maximum pulse energy is 750 nJ. The system is used to measure photoinduced electron transfer in a perylene/TiO2 system with unprecedented temporal resolution.

  20. Resolution limits of ultrafast ultrasound localization microscopy.

    PubMed

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

    2015-11-21

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

  1. Soil matrix and macropore biodegradation of 2,4-D

    SciTech Connect

    Pivetz, B.E.; Steenhuis, T.S.

    1995-07-01

    Preferential flow of pesticides in macropores can lead to decreased travel times through the vadose zone and increased groundwater contamination. Macropores, however, may present a favorable environment for biodegradation because of greater oxygen, nutrient, and substrate supply, and higher microbial populations in earthworm burrows, compared to the soil matrix. The biodegradation of 2,4-dichlorophenoxyacetic acid (2,4-D) was measured in macropores and soil matrix of packed soil columns (7.0-cm diam., 10-cm length) and undisturbed cores contained as well-defined artificial macropore and the undisturbed cores contained earthworm-burrow macropores. A 50 {mu}g/L 2,4-D solution was continuously applied to the unsaturated soil surface and breakthrough curves (BTCs) indicating pesticide loss in the effluent were obtained from the soil matrix and macropore flow paths. Biodegradation rates were calculated separately for each flow path by comparing the BTCs to BTCs representing abiotic conditions, and dividing the 2,4-D loss by the travel time through each flow path. The biodegradation rates increased with time in both flow paths, and the final biodegradation rate in the macropore region surpassed that of the matrix, presumably because of increased microbial populations in the macropore. Complete loss of the 2,4-D in both flow paths was observed after continuous application of 2,4-D for 400 h, with maximum column-averaged 2,4-D loss rates of 0.879 {mu}g/(L h) in the matrix and 1.073 {mu}g/(L h) in the macropore. Biodegradation of 2,4-D was also observed in the macropore and matrix regions of the undisturbed soil cores. 19 refs., 7 figs., 2 tabs.

  2. Semaphorin 4D Promotes Skeletal Metastasis in Breast Cancer

    PubMed Central

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

    2016-01-01

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

  3. Plasma Heating and Ultrafast Semiconductor Laser Modulation Through a Terahertz Heating Field

    NASA Technical Reports Server (NTRS)

    Li, Jian-Zhong; Ning, C. Z.

    2000-01-01

    Electron-hole plasma heating and ultrafast modulation in a semiconductor laser under a terahertz electrical field are investigated using a set of hydrodynamic equations derived from the semiconductor Bloch equations. The self-consistent treatment of lasing and heating processes leads to the prediction of a strong saturation and degradation of modulation depth even at moderate terahertz field intensity. This saturation places a severe limit to bandwidth achievable with such scheme in ultrafast modulation. Strategies for increasing modulation depth are discussed.

  4. Vibrational Conical Intersections: Implications for Ultrafast Vibrational Dynamics

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

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

    SciTech Connect

    Murnane, Margaret

    2010-03-31

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

  6. UVA radiation induced ultrafast electron transfer from a food carcinogen benzo[a]pyrene to organic molecules, biological macromolecules, and inorganic nano structures.

    PubMed

    Banerjee, Soma; Sarkar, Soumik; Lakshman, Karthik; Dutta, Joydeep; Pal, Samir Kumar

    2013-04-11

    Reactions involving electron transfer (ET) and reactive oxygen species (ROS) play a pivotal role in carcinogenesis and cancer biochemistry. Our present study emphasizes UVA radiation induced ET reaction as one of the key aspects of a potential carcinogen, benzo[a]pyrene (BP), in the presence of a wide variety of molecules covering organic p-benzoquinone (BQ), biological macromolecules like calf-thymus DNA (CT-DNA), human serum albumin (HSA) protein, and inorganic zinc oxide (ZnO) nanorods (NRs). Steady-state and picosecond-resolved fluorescence spectroscopy have been used to monitor such ET reactions. Physical consequences of BP association with CT-DNA have been investigated through temperature-dependent circular dichroism (CD) spectroscopy. The temperature-dependent steady-state, picosecond-resolved fluorescence lifetime and anisotropy studies reveal the effect of temperature on the perturbation of such ET reactions from BP to biological macromolecules, highlighting their temperature-dependent association. Furthermore, the electron-donating property of BP has been corroborated by measuring wavelength-dependent photocurrent in a BP-anchored ZnO NR-based photodevice, offering new physical insights for the carcinogenic study of BP. PMID:23484622

  7. Ultrafast Thermal Nonlinearity

    PubMed Central

    Khurgin, Jacob B.; Sun, Greg; Chen, Wei Ting; Tsai, Wei-Yi; Tsai, Din Ping

    2015-01-01

    Third order nonlinear optical phenomena explored in the last half century have been predicted to find wide range of applications in many walks of life, such as all-optical switching, routing, and others, yet this promise has not been fulfilled primarily because the strength of nonlinear effects is too low when they are to occur on the picosecond scale required in today’s signal processing applications. The strongest of the third-order nonlinearities, engendered by thermal effects, is considered to be too slow for the above applications. In this work we show that when optical fields are concentrated into the volumes on the scale of few tens of nanometers, the speed of the thermo-optical effects approaches picosecond scale. Such a sub-diffraction limit concentration of field can be accomplished with the use of plasmonic effects in metal nanoparticles impregnating the thermo-optic dielectric (e.g. amorphous Si) and leads to phase shifts sufficient for all optical switching on ultrafast scale. PMID:26644322

  8. Ultrafast scanning probe microscopy

    DOEpatents

    Weiss, Shimon; Chemla, Daniel S.; Ogletree, D. Frank; Botkin, David

    1995-01-01

    An ultrafast scanning probe microscopy method for achieving subpicosecond-temporal resolution and submicron-spatial resolution of an observation sample. In one embodiment of the present claimed invention, a single short optical pulse is generated and is split into first and second pulses. One of the pulses is delayed using variable time delay means. The first pulse is then directed at an observation sample located proximate to the probe of a scanning probe microscope. The scanning probe microscope produces probe-sample signals indicative of the response of the probe to characteristics of the sample. The second pulse is used to modulate the probe of the scanning probe microscope. The time delay between the first and second pulses is then varied. The probe-sample response signal is recorded at each of the various time delays created between the first and second pulses. The probe-sample response signal is then plotted as a function of time delay to produce a cross-correlation of the probe sample response. In so doing, the present invention provides simultaneous subpicosecond-temporal resolution and submicron-spatial resolution of the sample.

  9. Ultrafast gas switching experiments

    SciTech Connect

    Frost, C.A.; Martin, T.H.; Patterson, P.E.; Rinehart, L.F.; Rohwein, G.J.; Roose, L.D.; Aurand, J.F.; Buttram, M.T.

    1996-11-01

    We describe recent experiments which studied the physics of ultrafast gas breakdown under the extreme overvoltages which occur when a high pressure gas switch is pulse charged to hundreds of kV in 1 ns or less. The highly overvolted peaking gaps produce powerful electromagnetic pulses with risetimes < 100 ps which can be used for ultrawideband radar systems, particle accelerators, laser drivers, bioelectromagnetic studies, electromagnetic effects testing, and for basic studies of gas breakdown physics. We have produced and accurately measured pulses with 50 to 100 ps risetimes to peak levels of 75 to 160 kV at pulse repetition frequencies (PRF) to I kHz. A unique gas switch was developed to hold off hundreds of kV with parasitic inductance less than I nH. An advanced diagnostic system using Fourier compensation was developed to measure single-shot risetimes below 35 ps. The complete apparatus is described and wave forms are presented. The measured data are compared with a theoretical model which predicts key features including dependence on gas species and pressure. We have applied this technology to practical systems driving ultrawideband radiating antennas and bounded wave simulators. For example, we have developed a thyristor/pulse transformer based system using a highly overvolted cable switch. This pulser driving a Sandia- designed TEM cell, provides an ultra wideband impulse with < 200 ps risetime to the test object at a PRF > 1 kHz at > 100 kV/m E field.

  10. Ultrafast gas switching experiments

    SciTech Connect

    Frost, C.A.; Martin, T.H.; Patterson, P.E.; Rinehart, L.F.; Rohwein, G.J.; Roose, L.D.; Aurand, J.F.; Buttram, M.T.

    1993-08-01

    We describe recent experiments which studied the physics of ultrafast gas breakdown under the extreme overvoltages which occur when a high pressure gas switch is pulse charged to hundreds of kV in 1 ns or less. The highly overvolted peaking gaps produce powerful electromagnetic pulses with risetimes < 100 ps which can be used for ultrawideband radar systems, particle accelerators, laser drivers, bioelectromagnetic studies, electromagnetic effects testing, and for basic studies of gas breakdown physics. We have produced and accurately measured pulses with 50 to 100 ps risetimes to peak levels of 75 to 160 kV at pulse repetition frequencies (PRF) to 1 kHz. A unique gas switch was developed to hold off hundreds of kV with parasitic inductance less than 1 nH. An advanced diagnostic system using Fourier compensation was developed to measure single-shot risetimes below 35 ps. The complete apparatus is described and waveforms are presented. The measured data are compared with a theoretical model which predicts key features including dependence on gas species and technology to practical systems antennas and bounded wave developed a thyristor/pulse transformer based system using a highly overvolted cable switch. This pulser driving a Sandia-designed TEM cell, provides an ultra wideband impulse with < 200 ps risetime to the test object at a PRF > Khz at > 100 kV/m E field.

  11. Ultrafast Thermal Nonlinearity.

    PubMed

    Khurgin, Jacob B; Sun, Greg; Chen, Wei Ting; Tsai, Wei-Yi; Tsai, Din Ping

    2015-01-01

    Third order nonlinear optical phenomena explored in the last half century have been predicted to find wide range of applications in many walks of life, such as all-optical switching, routing, and others, yet this promise has not been fulfilled primarily because the strength of nonlinear effects is too low when they are to occur on the picosecond scale required in today's signal processing applications. The strongest of the third-order nonlinearities, engendered by thermal effects, is considered to be too slow for the above applications. In this work we show that when optical fields are concentrated into the volumes on the scale of few tens of nanometers, the speed of the thermo-optical effects approaches picosecond scale. Such a sub-diffraction limit concentration of field can be accomplished with the use of plasmonic effects in metal nanoparticles impregnating the thermo-optic dielectric (e.g. amorphous Si) and leads to phase shifts sufficient for all optical switching on ultrafast scale. PMID:26644322

  12. Ultrafast scanning probe microscopy

    DOEpatents

    Weiss, S.; Chemla, D.S.; Ogletree, D.F.; Botkin, D.

    1995-05-16

    An ultrafast scanning probe microscopy method is described for achieving subpicosecond-temporal resolution and submicron-spatial resolution of an observation sample. In one embodiment of the present claimed invention, a single short optical pulse is generated and is split into first and second pulses. One of the pulses is delayed using variable time delay means. The first pulse is then directed at an observation sample located proximate to the probe of a scanning probe microscope. The scanning probe microscope produces probe-sample signals indicative of the response of the probe to characteristics of the sample. The second pulse is used to modulate the probe of the scanning probe microscope. The time delay between the first and second pulses is then varied. The probe-sample response signal is recorded at each of the various time delays created between the first and second pulses. The probe-sample response signal is then plotted as a function of time delay to produce a cross-correlation of the probe sample response. In so doing, the present invention provides simultaneous subpicosecond-temporal resolution and submicron-spatial resolution of the sample. 6 Figs.

  13. Ultrafast Imaging using Spectral Resonance Modulation

    NASA Astrophysics Data System (ADS)

    Huang, Eric; Ma, Qian; Liu, Zhaowei

    2016-04-01

    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 Imaging using Spectral Resonance Modulation.

    PubMed

    Huang, Eric; Ma, Qian; Liu, Zhaowei

    2016-01-01

    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. PMID:27122101

  15. Ultrafast Imaging using Spectral Resonance Modulation

    PubMed Central

    Huang, Eric; Ma, Qian; Liu, Zhaowei

    2016-01-01

    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. PMID:27122101

  16. Ultrafast carriers dynamics in filled-skutterudites

    SciTech Connect

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

    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.

  17. New C4D Sensor with a Simulated Inductor

    PubMed Central

    Lyu, Yingchao; Ji, Haifeng; Yang, Shijie; Huang, Zhiyao; Wang, Baoliang; Li, Haiqing

    2016-01-01

    A new capacitively coupled contactless conductivity detection (C4D) sensor with an improved simulated inductor is developed in this work. The improved simulated inductor is designed on the basis of the Riordan-type floating simulated inductor. With the improved simulated inductor, the negative influence of the coupling capacitances is overcome and the conductivity measurement is implemented by the series resonance principle. The conductivity measurement experiments are carried out in three pipes with different inner diameters of 3.0 mm, 4.6 mm and 6.4 mm, respectively. The experimental results show that the designs of the new C4D sensor and the improved simulated inductor are successful. The maximum relative error of the conductivity measurement is less than 5%. Compared with the C4D sensors using practical inductors, the measurement accuracy of the new C4D sensor is comparable. The research results also indicate that the adjustability of a simulated inductor can reduce the requirement for the AC source and guarantee the interchangeableness. Meanwhile, it is recommended that making the potential of one terminal of a simulated inductor stable is beneficial to the running stability. Furthermore, this work indirectly verifies the possibility and feasibility of the miniaturization of the C4D sensor by using the simulated inductor technique and lays a good foundation for future research work. PMID:26828493

  18. In Vitro Self-Assembly of the Light Harvesting Pigment-Protein LH2 Revealed by Ultrafast Spectroscopy and Electron Microscopy

    PubMed Central

    Schubert, Axel; Stenstam, Anna; Beenken, Wichard J. D.; Herek, Jennifer L.; Cogdell, Richard; Pullerits, Tõnu; Sundström, Villy

    2004-01-01

    Controlled ensemble formation of protein-surfactant systems provides a fundamental concept for the realization of nanoscale devices with self-organizing capability. In this context, spectroscopic monitoring of pigment-containing proteins yields detailed structural information. Here we have studied the association behavior of the bacterial light-harvesting protein LH2 from Rhodobacter spheroides in an n,n-dimethyldodecylamine-n-oxide/water environment. Time-resolved studies of the excitation annihilation yielded information about aggregate sizes and packing of the protein complexes therein. The results are compared to transmission electron microscopy images of instantaneously frozen samples. Our data indicate the manifestation of different phases, which are discussed with respect to the thermodynamic equilibrium in ternary protein-surfactant-water systems. Accordingly, by varying the concentration the formation of different types of aggregates can be controlled. Conditions for the appearance of isolated LH2 complexes are defined. PMID:15041674

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

    NASA Astrophysics Data System (ADS)

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

    2010-03-01

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

  20. Cold atom quantum emulation of ultrafast processes

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

  1. The influence of ultrafast laser pulses on electron transfer in molecular wires studied by a non-Markovian density-matrix approach.

    PubMed

    Welack, Sven; Schreiber, Michael; Kleinekathöfer, Ulrich

    2006-01-28

    New features of molecular wires can be observed when they are irradiated by laser fields. These effects can be achieved by periodically oscillating fields but also by short laser pulses. The theoretical foundation used for these investigations is a density-matrix formalism where the full system is partitioned into a relevant part and a thermal fermionic bath. The derivation of a quantum master equation, either based on a time-convolutionless or time-convolution projection-operator approach, incorporates the interaction with time-dependent laser fields nonperturbatively and is valid at low temperatures for weak system-bath coupling. From the population dynamics the electrical current through the molecular wire is determined. This theory including further extensions is used for the determination of electron transport through molecular wires. As examples, we show computations of coherent destruction of tunneling in asymmetric periodically driven quantum systems, alternating currents and the suppression of the directed current by using a short laser pulse. PMID:16460205

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

    NASA Astrophysics Data System (ADS)

    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.

  3. Assimilation of DMSP/SSUSI UV data into IDA4D

    NASA Astrophysics Data System (ADS)

    Gelinas, L. J.; Bust, G. S.; Brinkman, D. G.; Straus, P. R.; Swartz, R. L.

    2014-12-01

    Ionospheric Data Assimilation Four-Dimensional (IDA4D) is a continuous-time, three-dimensional imaging algorithm that can produce 4D electron density specifications for various science investigations [e.g., Bust et al., 2007]. IDA4D is based on three-dimensional variational (3DVAR) data assimilation [Daley and Barker, 2001]. The algorithm combines various data sources and their associated error covariances with a background model (in this case the IRI) and its covariances to produce an ionospheric specification with formal uncertainties. IDA4D employs a Gauss- Markov Kalman filter technique similar to that used by operational assimilation models. The model can ingest a broad spectrum of data types that are either linearly or non-linearly related to electron density, including ground-based TEC, space-based TEC as measured by GPS occultation sensors and UV emissions associated with nightside recombination of O+. IDA4D has been undergoing testing at The Aerospace Corporation to determine its performance with respect to combinations of input data sets under different conditions (solar minimum, solar maximum, geomagnetic activity). The results presented here summarize the performance of IDA4D when UV data is ingested, both with and without additional TEC measurements. The UV data used in the study summarized here are 135.6 nm emissions measured the SSUSI instruments on F16 and F18 DMSP. We discuss the process by which UV data is ingested into IDA4D, including data binning, error estimation and correction of 135.6 nm contamination from mutual neutralization of O+ and O-. Model performance is then assessed using comparisons to various ground truth data, including ISR data, Jason VTEC, CNOF/S in-situ plasma density and ionosonde-derived NmF2 values. The results of this study show that UV data improves model performance, particularly when TEC data coverage is sparse. Bust, G. S., G. Crowley, T. W. Garner, T. L. Gaussiran II, R. W. Meggs, C. N. Mitchell, P. S. J. Spencer, P

  4. Relative charge transfer cross section from Rb (4d)

    NASA Astrophysics Data System (ADS)

    Shah, M. H.; Camp, H. A.; Trachy, M. L.; Fléchard, X.; Gearba, M. A.; Nguyen, H.; Brédy, R.; Lundeen, S. R.; Depaola, B. D.

    2005-08-01

    Relative charge transfer cross section measurements for the excited state Rb(4d) with 7keV Na+ is reported. The specific channels reported are Na++Rb(4d5/2)→Na(nl)+Rb+ , where the dominant transfer cross sections channels were nl=3d and 4s . Using a combination of a magneto-optical trap and recoil ion momentum spectroscopy (MOTRIMS methodology), the cross sections were measured relative to the previously studied Na++Rb(5s,5p) systems at the same collision energy.

  5. Relative charge transfer cross section from Rb(4d)

    SciTech Connect

    Shah, M.H.; Camp, H.A.; Trachy, M.L.; De Paola, B.D.; Flechard, X.; Gearba, M.A.; Nguyen, H.; Bredy, R.; Lundeen, S.R.

    2005-08-15

    Relative charge transfer cross section measurements for the excited state Rb(4d) with 7 keV Na{sup +} is reported. The specific channels reported are Na{sup +}+Rb(4d{sub 5/2}){yields}Na(nl)+Rb{sup +}, where the dominant transfer cross sections channels were nl=3d and 4s. Using a combination of a magneto-optical trap and recoil ion momentum spectroscopy (MOTRIMS methodology), the cross sections were measured relative to the previously studied Na{sup +}+Rb(5s,5p) systems at the same collision energy.

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

    NASA Technical Reports Server (NTRS)

    Dickmanns, Ernst D.

    1994-01-01

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

  7. Emerging Applications of Abdominal 4D Flow MRI

    PubMed Central

    Roldán-Alzate, Alejandro; Francois, Christopher J.; Wieben, Oliver; Reeder, Scott B.

    2016-01-01

    OBJECTIVE Comprehensive assessment of abdominal hemodynamics is crucial for many clinical diagnoses but is challenged by a tremendous complexity of anatomy, normal physiology, and a wide variety of pathologic abnormalities. This article introduces 4D flow MRI as a powerful technique for noninvasive assessment of the hemodynamics of abdominal vascular territories. CONCLUSION Four-dimensional flow MRI provides clinicians with a more extensive and straightforward approach to evaluate disorders that affect blood flow in the abdomen. This review presents a series of clinical cases to illustrate the utility of 4D flow MRI in the comprehensive assessment of the abdominal circulation. PMID:27187681

  8. Ultrafast fluorescence upconversion technique and its applications to proteins.

    PubMed

    Chosrowjan, Haik; Taniguchi, Seiji; Tanaka, Fumio

    2015-08-01

    The basic principles and main characteristics of the ultrafast time-resolved fluorescence upconversion technique (conventional and space-resolved), including requirements for nonlinear crystals, mixing spectral bandwidth, acceptance angle, etc., are presented. Applications to flavoproteins [wild-type (WT) FMN-binding protein and its W32Y, W32A, E13R, E13K, E13Q and E13T mutants] and photoresponsive proteins [WT photoactive yellow protein and its R52Q mutant in solution and as single crystals] are demonstrated. For flavoproteins, investigations elucidating the effects of ionic charges on ultrafast electron transfer (ET) dynamics are summarized. It is shown that replacement of the ionic amino acid Glu13 and the resulting modification of the electrostatic charge distribution in the protein chromphore-binding pocket substantially alters the ultrafast fluorescence quenching dynamics and ET rate in FMN-binding protein. It is concluded that, together with donor-acceptor distances, electrostatic interactions between ionic photoproducts and other ionic groups in the proteins are important factors influencing the ET rates. In WT photoactive yellow protein and the R52Q mutant, ultrafast photoisomerization dynamics of the chromophore (deprotonated trans-p-coumaric acid) in liquid and crystal phases are investigated. It is shown that the primary dynamics in solution and single-crystal phases are quite similar; hence, the photocycle dynamics and structural differences observed at longer time scales arise mostly from the structural restraints imposed by the crystal lattice rigidity versus the flexibility in solution. PMID:25532707

  9. Ultrafast spectroscopy of novel materials

    NASA Astrophysics Data System (ADS)

    Hardison, Lindsay M.

    My research focused on steady state and time-resolved photophysical characterization of a series of semiconductor nanoparticles and water soluble conjugated polyelectrolytes. Several studies have shown that the electronic structure and relaxation dynamics in CdSe nanocrystals are not only size but are also shape and passivation dependent; however, there is no detailed comparison of the photophysical properties of ZnCdSe particles with different relative amounts of Zn. This dissertation presents data collected for colloidal CdSe, CdSe/ZnSe and ZnCdSe nanoparticles with rod-like architectures synthesized and investigated in our labs to determine how size, shape, passivation and composition affect the quantum confinement and dynamics. In addition, a series of different polymer repeat unit lengths of a linear conjugated polyelectrolyte (CPE) with a carboxylate ionic side chain have been synthesized and their photophysical properties have been explored. Spectral shifts and line broadening exhibited within the Raman spectroscopy, UV-Vis spectroscopy and photoluminescence aided in determining the extent of alloying and compositional disorder created during the alloying process. The photoluminescence quantum yield of ZnCdSe nanorods is higher than that from pristine CdSe nanorods indicating a higher binding energy of the exciton. This effect is speculated to be due to increased localization of the exciton as a result of fluctuations in the composition, ultimately resulting in increases in luminescence efficiencies. Moreover, time-resolved photoluminescence characterized lifetimes of nanoparticles with similar shape but different composition. Emission of an inhomogeneous population distribution (different sizes, shapes or composition) leads to the simultaneous probing of particles with different decaying rates. A stretched exponential function, I(t)= A*exp[-(t/tau) beta], can be used to describe these systems, where beta <1 corresponds to disperse populations. In the

  10. Graphene in Ultrafast and Ultrastrong Laser Pulses

    NASA Astrophysics Data System (ADS)

    Koochakikelardeh, Hamed; Apalkov, Vadym; Stockman, Mark

    2015-03-01

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

  11. 2,4-Dichlorophenoxyacetic acid (2,4-D)

    Integrated Risk Information System (IRIS)

    2,4 - Dichlorophenoxyacetic acid ( 2,4 - D ) ; CASRN 94 - 75 - 7 Human health assessment information on a chemical substance is included in the IRIS database only after a comprehensive review of toxicity data , as outlined in the IRIS assessment development process . Sections I ( Health Hazard Asses

  12. 4D flow mri post-processing strategies for neuropathologies

    NASA Astrophysics Data System (ADS)

    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

  13. Catching Up with Ultrafast Endocytosis.

    PubMed

    Brockmann, Marisa M; Rosenmund, Christian

    2016-05-01

    The mechanism and speed of endocytosis at central synapses after neurotransmitter release is still under debate. In this issue of Neuron,Delvendahl et al. (2016) propose an ultrafast form of endocytosis after single action potentials (APs) at physiological temperature. PMID:27151632

  14. 4D MR imaging using robust internal respiratory signal

    NASA Astrophysics Data System (ADS)

    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.

  15. Ultrafast laser-induced changes in optical properties of semiconductors

    SciTech Connect

    Chirila, C. C.; Lim, Freda C. H.; Gavaza, M. G.

    2012-04-01

    We study the effect of laser radiation on optical properties of semiconductors of industrial interest. The material is pumped with a laser of chosen central frequency, for which the absorption is maximal, thus inducing electron dynamics, which modifies the optical properties. By using an improved theoretical model, we study ultrafast dynamic changes in the refraction index and reflectivity corresponding to a wide frequency-interval of probing radiation and identify that interval where these optical changes are most significant.

  16. Quasimomentum-Space Image for Ultrafast Melting of Silicon

    NASA Astrophysics Data System (ADS)

    Zier, Tobias; Zijlstra, Eeuwe S.; Garcia, Martin E.

    2016-04-01

    By exciting electron-hole pairs that survive for picoseconds strong femtosecond lasers may transiently influence the bonding properties of semiconductors, causing structure changes, in particular, ultrafast melting. In order to determine the energy flow during this process in silicon we performed ab initio molecular dynamics simulations and an analysis in quasimomentum space. We found that energy flows very differently as a function of increasing excitation density, namely, mainly through long wavelength, L -point, or X -point lattice vibrations, respectively.

  17. Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

    PubMed

    Mongin, Denis; Shaviv, Ehud; Maioli, Paolo; Crut, Aurélien; Banin, Uri; Del Fatti, Natalia; Vallée, Fabrice

    2012-08-28

    Hybrid nano-objects formed by two or more disparate materials are among the most promising and versatile nanosystems. A key parameter in their properties is interaction between their components. In this context we have investigated ultrafast charge separation in semiconductor-metal nanohybrids using a model system of gold-tipped CdS nanorods in a matchstick architecture. Experiments are performed using an optical time-resolved pump-probe technique, exciting either the semiconductor or the metal component of the particles, and probing the light-induced change of their optical response. Electron-hole pairs photoexcited in the semiconductor part of the nanohybrids are shown to undergo rapid charge separation with the electron transferred to the metal part on a sub-20 fs time scale. This ultrafast gold charging leads to a transient red-shift and broadening of the metal surface plasmon resonance, in agreement with results for free clusters but in contrast to observation for static charging of gold nanoparticles in liquid environments. Quantitative comparison with a theoretical model is in excellent agreement with the experimental results, confirming photoexcitation of one electron-hole pair per nanohybrid followed by ultrafast charge separation. The results also point to the utilization of such metal-semiconductor nanohybrids in light-harvesting applications and in photocatalysis. PMID:22792998

  18. Ultrafast optical demagnetization manipulates nanoscale spin structure in domain walls

    PubMed Central

    Pfau, B.; Schaffert, S.; Müller, L.; Gutt, C.; Al-Shemmary, A.; Büttner, F.; Delaunay, R.; Düsterer, S.; Flewett, S.; Frömter, R.; Geilhufe, J.; Guehrs, E.; Günther, C.M.; Hawaldar, R.; Hille, M.; Jaouen, N.; Kobs, A.; Li, K.; Mohanty, J.; Redlin, H.; Schlotter, W.F.; Stickler, D.; Treusch, R.; Vodungbo, B.; Kläui, M.; Oepen, H.P.; Lüning, J.; Grübel, G.; Eisebitt, S.

    2012-01-01

    During ultrafast demagnetization of a magnetically ordered solid, angular momentum has to be transferred between the spins, electrons, and phonons in the system on femto- and picosecond timescales. Although the intrinsic spin-transfer mechanisms are intensely debated, additional extrinsic mechanisms arising due to nanoscale heterogeneity have only recently entered the discussion. Here we use femtosecond X-ray pulses from a free-electron laser to study thin film samples with magnetic domain patterns. We observe an infrared-pump-induced change of the spin structure within the domain walls on the sub-picosecond timescale. This domain-topography-dependent contribution connects the intrinsic demagnetization process in each domain with spin-transport processes across the domain walls, demonstrating the importance of spin-dependent electron transport between differently magnetized regions as an ultrafast demagnetization channel. This pathway exists independent from structural inhomogeneities such as chemical interfaces, and gives rise to an ultrafast spatially varying response to optical pump pulses. PMID:23033076

  19. Ultrafast charge localization in a stripe-phase nickelate

    SciTech Connect

    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.

  20. Microscopic model for ultrafast remagnetization dynamics.

    PubMed

    Chimata, Raghuveer; Bergman, Anders; Bergqvist, Lars; Sanyal, Biplab; Eriksson, Olle

    2012-10-12

    In this Letter, we provide a microscopic model for the ultrafast remagnetization of atomic moments already quenched above the Stoner-Curie temperature by a strong laser fluence. Combining first-principles density functional theory, atomistic spin dynamics utilizing the Landau-Lifshitz-Gilbert equation, and a three-temperature model, we analyze the temporal evolution of atomic moments as well as the macroscopic magnetization of bcc Fe and hcp Co covering a broad time scale, ranging from femtoseconds to picoseconds. Our simulations show a variety of complex temporal behavior of the magnetic properties resulting from an interplay between electron, spin, and lattice subsystems, which causes an intricate time evolution of the atomic moment, where longitudinal and transversal fluctuations result in a macrospin moment that evolves highly nonmonotonically. PMID:23102359

  1. An ultrafast silicon nanoplasmonic ballistic triode

    SciTech Connect

    Greig, S. R. Elezzabi, A. Y.

    2014-12-15

    A nanoscale three terminal silicon based nanoplasmonic triode is proposed as a nanometer transistor. The device is suitable for monolithic integration with complementary-metal-oxide-semiconductor technology. Due to the highly spatially inhomogeneous, highly confined nanoplasmonic mode, electrons generated through two-photon absorption in the silicon are ponderomotively accelerated towards the copper anode producing an output current. Application of a negative grid voltage allows for control of the output current. The nanoplasmonic triode is able to achieve output current as high as 628 mA/μm on an ultrafast timescale of 150 fs in a compact footprint of 0.07 μm{sup 2}. Reduction of the plasmonic field strength allows for a CMOS compatible current of 11.7 mA/μm. The results demonstrate the potential for the compact optical control of current useful for applications in high-speed, high current switching, and amplification.

  2. An ultrafast silicon nanoplasmonic ballistic triode

    NASA Astrophysics Data System (ADS)

    Greig, S. R.; Elezzabi, A. Y.

    2014-12-01

    A nanoscale three terminal silicon based nanoplasmonic triode is proposed as a nanometer transistor. The device is suitable for monolithic integration with complementary-metal-oxide-semiconductor technology. Due to the highly spatially inhomogeneous, highly confined nanoplasmonic mode, electrons generated through two-photon absorption in the silicon are ponderomotively accelerated towards the copper anode producing an output current. Application of a negative grid voltage allows for control of the output current. The nanoplasmonic triode is able to achieve output current as high as 628 mA/μm on an ultrafast timescale of 150 fs in a compact footprint of 0.07 μm2. Reduction of the plasmonic field strength allows for a CMOS compatible current of 11.7 mA/μm. The results demonstrate the potential for the compact optical control of current useful for applications in high-speed, high current switching, and amplification.

  3. Ultrafast charge transfer and atomic orbital polarization

    SciTech Connect

    Deppe, M.; Foehlisch, A.; Hennies, F.; Nagasono, M.; Beye, M.; Sanchez-Portal, D.; Echenique, P. M.; Wurth, W.

    2007-11-07

    The role of orbital polarization for ultrafast charge transfer between an atomic adsorbate and a substrate is explored. Core hole clock spectroscopy with linearly polarized x-ray radiation allows to selectively excite adsorbate resonance states with defined spatial orientation relative to the substrate surface. For c(4x2)S/Ru(0001) the charge transfer times between the sulfur 2s{sup -1}3p*{sup +1} antibonding resonance and the ruthenium substrate have been studied, with the 2s electron excited into the 3p{sub perpendicular}* state along the surface normal and the 3p{sub parallel}* state in the surface plane. The charge transfer times are determined as 0.18{+-}0.07 and 0.84{+-}0.23 fs, respectively. This variation is the direct consequence of the different adsorbate-substrate orbital overlap.

  4. Generation of attosecond electron packets via conical surface plasmon electron acceleration

    NASA Astrophysics Data System (ADS)

    Greig, S. R.; Elezzabi, A. Y.

    2016-01-01

    We present a method for the generation of high kinetic energy attosecond electron packets via magnetostatic and aperture filtering of conical surface plasmon (SP) accelerated electrons. The conical SP waves are excited by coupling an ultrafast radially polarized laser beam to a conical silica lens coated with an Ag film. Electromagnetic and particle tracking models are employed to characterize the ultrafast electron packets.

  5. Impact of incorporating visual biofeedback in 4D MRI.

    PubMed

    To, David T; Kim, Joshua P; Price, Ryan G; Chetty, Indrin J; Glide-Hurst, Carri K

    2016-01-01

    Precise radiation therapy (RT) for abdominal lesions is complicated by respiratory motion and suboptimal soft tissue contrast in 4D CT. 4D MRI offers improved con-trast although long scan times and irregular breathing patterns can be limiting. To address this, visual biofeedback (VBF) was introduced into 4D MRI. Ten volunteers were consented to an IRB-approved protocol. Prospective respiratory-triggered, T2-weighted, coronal 4D MRIs were acquired on an open 1.0T MR-SIM. VBF was integrated using an MR-compatible interactive breath-hold control system. Subjects visually monitored their breathing patterns to stay within predetermined tolerances. 4D MRIs were acquired with and without VBF for 2- and 8-phase acquisitions. Normalized respiratory waveforms were evaluated for scan time, duty cycle (programmed/acquisition time), breathing period, and breathing regularity (end-inhale coefficient of variation, EI-COV). Three reviewers performed image quality assessment to compare artifacts with and without VBF. Respiration-induced liver motion was calculated via centroid difference analysis of end-exhale (EE) and EI liver contours. Incorporating VBF reduced 2-phase acquisition time (4.7 ± 1.0 and 5.4 ± 1.5 min with and without VBF, respectively) while reducing EI-COV by 43.8% ± 16.6%. For 8-phase acquisitions, VBF reduced acquisition time by 1.9 ± 1.6 min and EI-COVs by 38.8% ± 25.7% despite breathing rate remaining similar (11.1 ± 3.8 breaths/min with vs. 10.5 ± 2.9 without). Using VBF yielded higher duty cycles than unguided free breathing (34.4% ± 5.8% vs. 28.1% ± 6.6%, respectively). Image grading showed that out of 40 paired evaluations, 20 cases had equivalent and 17 had improved image quality scores with VBF, particularly for mid-exhale and EI. Increased liver excursion was observed with VBF, where superior-inferior, anterior-posterior, and left-right EE-EI displacements were 14.1± 5.8, 4.9 ± 2.1, and 1.5 ± 1.0 mm, respectively, with VBF compared to 11.9

  6. Intelligent Vehicle Systems: A 4D/RCS Approach

    SciTech Connect

    Madhavan, Raj

    2007-04-01

    This book presents new research on autonomous mobility capabilities and shows how technological advances can be anticipated in the coming two decades. An in-depth description is presented on the theoretical foundations and engineering approaches that enable these capabilities. Chapter 1 provides a brief introduction to the 4D/RCS reference model architecture and design methodology that has proven successful in guiding the development of autonomous mobility systems. Chapters 2 through 7 provide more detailed descriptions of research that has been conducted and algorithms that have been developed to implement the various aspects of the 4D/RCS reference model architecture and design methodology. Chapters 8 and 9 discuss applications, performance measures, and standards. Chapter 10 provides a history of Army and DARPA research in autonomous ground mobility. Chapter 11 provides a perspective on the potential future developments in autonomous mobility.

  7. Quantication and analysis of respiratory motion from 4D MRI

    NASA Astrophysics Data System (ADS)

    Aizzuddin Abd Rahni, Ashrani; Lewis, Emma; Wells, Kevin

    2014-11-01

    It is well known that respiratory motion affects image acquisition and also external beam radiotherapy (EBRT) treatment planning and delivery. However often the existing approaches for respiratory motion management are based on a generic view of respiratory motion such as the general movement of organ, tissue or fiducials. This paper thus aims to present a more in depth analysis of respiratory motion based on 4D MRI for further integration into motion correction in image acquisition or image based EBRT. Internal and external motion was first analysed separately, on a per-organ basis for internal motion. Principal component analysis (PCA) was then performed on the internal and external motion vectors separately and the relationship between the two PCA spaces was analysed. The motion extracted from 4D MRI on general was found to be consistent with what has been reported in literature.

  8. Exome sequencing identifies PDE4D mutations in acrodysostosis.

    PubMed

    Lee, Hane; Graham, John M; Rimoin, David L; Lachman, Ralph S; Krejci, Pavel; Tompson, Stuart W; Nelson, Stanley F; Krakow, Deborah; Cohn, Daniel H

    2012-04-01

    Acrodysostosis is a dominantly-inherited, multisystem disorder characterized by skeletal, endocrine, and neurological abnormalities. To identify the molecular basis of acrodysostosis, we performed exome sequencing on five genetically independent cases. Three different missense mutations in PDE4D, which encodes cyclic AMP (cAMP)-specific phosphodiesterase 4D, were found to be heterozygous in three of the cases. Two of the mutations were demonstrated to have occurred de novo, providing strong genetic evidence of causation. Two additional cases were heterozygous for de novo missense mutations in PRKAR1A, which encodes the cAMP-dependent regulatory subunit of protein kinase A and which has been recently reported to be the cause of a form of acrodysostosis resistant to multiple hormones. These findings demonstrate that acrodysostosis is genetically heterogeneous and underscore the exquisite sensitivity of many tissues to alterations in cAMP homeostasis. PMID:22464252

  9. 4D, Script N = 1 supersymmetry genomics (I)

    NASA Astrophysics Data System (ADS)

    Gates, S. James, Jr.; Gonzales, James; MacGregor, Boanne; Parker, James; Polo-Sherk, Ruben; Rodgers, Vincent G. J.; Wassink, Luke

    2009-12-01

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

  10. Brain tissue segmentation in 4D CT using voxel classification

    NASA Astrophysics Data System (ADS)

    van den Boom, R.; Oei, M. T. H.; Lafebre, S.; Oostveen, L. J.; Meijer, F. J. A.; Steens, S. C. A.; Prokop, M.; van Ginneken, B.; Manniesing, R.

    2012-02-01

    A method is proposed to segment anatomical regions of the brain from 4D computer tomography (CT) patient data. The method consists of a three step voxel classification scheme, each step focusing on structures that are increasingly difficult to segment. The first step classifies air and bone, the second step classifies vessels and the third step classifies white matter, gray matter and cerebrospinal fluid. As features the time averaged intensity value and the temporal intensity change value were used. In each step, a k-Nearest-Neighbor classifier was used to classify the voxels. Training data was obtained by placing regions of interest in reconstructed 3D image data. The method has been applied to ten 4D CT cerebral patient data. A leave-one-out experiment showed consistent and accurate segmentation results.

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

    PubMed

    Chien, Chen-Yu; Tai, Shu-Yu; Wang, Ling-Feng; Hsi, Edward; Chang, Ning-Chia; Wang, Hsun-Mo; Wu, Ming-Tsang; Ho, Kuen-Yao

    2016-09-01

    The phosphodiesterase 4D (PDE4D) gene has been reported as a risk gene for ischemic stroke. The vascular factors are between the hypothesized etiologies of sudden sensorineural hearing loss (SSNHL), and this genetic effect might be attributed for its role in SSNHL. We hypothesized that genetic variants of the PDE4D gene are associated with susceptibility to SSNHL. We conducted a case-control study with 362 SSNHL cases and 209 controls. Three single nucleotide polymorphisms (SNPs) were selected. The genotypes were determined using TaqMan technology. Hardy-Weinberg equilibrium (HWE) was tested for each SNP, and genetic effects were evaluated according to three inheritance modes. We carried out sex-specific analysis to analyze the overall data. All three SNPs were in HWE. When subjects were stratified by sex, the genetic effect was only evident in females but not in males. The TT genotype of rs702553 exhibited an adjusted odds ratio (OR) of 3.83 (95 % confidence interval = 1.46-11.18) (p = 0.006) in female SSNHL. The TT genotype of SNP rs702553 was associated with female SSNHL under the recessive model (p = 0.004, OR 3.70). In multivariate logistic regression analysis, TT genotype of rs702553 was significantly associated with female SSNHL (p = 0.0043, OR 3.70). These results suggest that PDE4D gene polymorphisms influence the susceptibility for the development of SSNHL in the southern Taiwanese female population. PMID:26521189

  12. Limits to Electron Beam Emittance from Stochastic Coulomb Interactions

    SciTech Connect

    Coleman-Smith, Christopher; Padmore, Howard A.; Wan, Weishi

    2008-08-22

    Dense electron beams can now be generated on an ultrafast timescale using laser driven photo-cathodes and these are used for a range of applications from ultrafast electron defraction to free electron lasers. Here we determine a lower bound to the emittance of an electron beam limited by fundamental stochastic Coulomb interactions.

  13. Photonic metasurfaces for spatiotemporal and ultrafast light control

    NASA Astrophysics Data System (ADS)

    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.

  14. 4D-Flow validation, numerical and experimental framework

    NASA Astrophysics Data System (ADS)

    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.

  15. 4D remote sensing image coding with JPEG2000

    NASA Astrophysics Data System (ADS)

    Muñoz-Gómez, Juan; Bartrina-Rapesta, Joan; Blanes, Ian; Jiménez-Rodríguez, Leandro; Aulí-Llinàs, Francesc; Serra-Sagristà, Joan

    2010-08-01

    Multicomponent data have become popular in several scientific fields such as forest monitoring, environmental studies, or sea water temperature detection. Nowadays, this multicomponent data can be collected more than one time per year for the same region. This generates different instances in time of multicomponent data, also called 4D-Data (1D Temporal + 1D Spectral + 2D Spatial). For multicomponent data, it is important to take into account inter-band redundancy to produce a more compact representation of the image by packing the energy into fewer number of bands, thus enabling a higher compression performance. The principal decorrelators used to compact the inter-band correlation redundancy are the Karhunen Loeve Transform (KLT) and Discrete Wavelet Transform (DWT). Because of the Temporal Dimension added, the inter-band redundancy among different multicomponent images is increased. In this paper we analyze the influence of the Temporal Dimension (TD) and the Spectral Dimension (SD) in 4D-Data in terms of coding performance for JPEG2000, because it has support to apply different decorrelation stages and transforms to the components through the different dimensions. We evaluate the influence to perform different decorrelators techniques to the different dimensions. Also we will assess the performance of the two main decorrelation techniques, KLT and DWT. Experimental results are provided, showing rate-distortion performances encoding 4D-Data using KLT and WT techniques to the different dimensions TD and SD.

  16. 4D flow imaging: current status to future clinical applications.

    PubMed

    Markl, Michael; Schnell, Susanne; Barker, Alex J

    2014-05-01

    4D flow MRI permits a comprehensive in-vivo assessment of three-directional blood flow within 3-dimensional vascular structures throughout the cardiac cycle. Given the large coverage permitted from a 4D flow acquisition, the distribution of vessel wall and flow parameters along an entire vessel of interest can thus be derived from a single measurement without being dependent on multiple predefined 2D acquisitions. In addition to qualitative 3D visualizations of complex cardiac and vascular flow patterns, quantitative flow analysis can be performed and is complemented by the ability to compute sophisticated hemodynamic parameters, such as wall shear stress or 3D pressure difference maps. These metrics can provide information previously unavailable with conventional modalities regarding the impact of cardiovascular disease or therapy on global and regional changes in hemodynamics. This review provides an introduction to the methodological aspects of 4D flow MRI to assess vascular hemodynamics and describes its potential for the assessment and understanding of altered hemodynamics in the presence of cardiovascular disease. PMID:24700368

  17. A 4D Hyperspherical Interpretation of q-Space

    PubMed Central

    Hosseinbor, A. Pasha; Chung, Moo K.; Wu, Yu-Chien; Bendlin, Barbara B.; Alexander, Andrew L.

    2015-01-01

    3D q-space can be viewed as the surface of a 4D hypersphere. In this paper, we seek to develop a 4D hyperspherical interpretation of q-space by projecting it onto a hypersphere and subsequently modeling the q-space signal via 4D hyperspherical harmonics (HSH). Using this orthonormal basis, we derive several well-established q-space indices and numerically estimate the diffusion orientation distribution function (dODF). We also derive the integral transform describing the relationship between the diffusion signal and propagator on a hypersphere. Most importantly, we will demonstrate that for hybrid diffusion imaging (HYDI) acquisitions low order linear expansion of the HSH basis is sufficient to characterize diffusion in neural tissue. In fact, the HSH basis achieves comparable signal and better dODF reconstructions than other well-established methods, such as Bessel Fourier orientation reconstruction (BFOR), using fewer fitting parameters. All in all, this work provides a new way of looking at q-space. PMID:25624043

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

    NASA Astrophysics Data System (ADS)

    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. Modeling ultrafast exciton deactivation in oligothiophenes via nonadiabatic dynamics.

    PubMed

    Fazzi, Daniele; Barbatti, Mario; Thiel, Walter

    2015-03-28

    Ultrafast excited-state processes play a key role in organic electronics and photovoltaics, governing the way of how excitons can relax and separate. Through the use of nonadiabatic excited-state dynamics, relaxation processes were investigated at the sub-picosecond timescale in thiophene and oligothiophenes (nT, n = 2, 3, 4), prototype oligomers for efficient π-electron conjugated polymers adopted in photovoltaics. For thiophene, TDDFT and TDA nonadiabatic excited-state dynamics revealed ultrafast nonradiative relaxation processes through ring opening and ring puckering, bringing the system to an S1/S0 conical intersection seam. The computed relaxation time is 110 fs, matching well the experimental one (∼105 fs). In oligothiophenes (n = 2-4), high-energy (hot) excitations were considered. Exciton relaxation through the manifold of excited states to the lowest excited state is predicted to occur within ∼150-200 fs, involving bond stretching, ring puckering, and torsional oscillations. For the longer oligomer (4T), the ultrafast relaxation process leads to exciton localization over three thiophene rings in 150 fs. These data agree with the self-localization mechanism (∼100-200 fs) observed for poly(3-hexylthiophene) (P3HT) and shed light on the complex exciton relaxation dynamics occurring in π-conjugated oligomers of potential interest for optoelectronic applications. PMID:25714233

  20. Ultrafast charge localization in a stripe-phase nickelate

    PubMed Central

    Coslovich, G.; Huber, B.; Lee, W. -S.; Chuang, Y. -D.; Zhu, Y.; Sasagawa, T.; Hussain, Z.; Bechtel, H. A.; Martin, M. C.; Shen, Z. -X.; Schoenlein, R. W.; Kaindl, R. A.

    2013-01-01

    Self-organized electronically ordered phases are a recurring feature in correlated materials, resulting in, for example, 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 dynamic 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. PMID:24153394

  1. 2,4-D impact on bacterial communities, and the activity and genetic potential of 2,4-D degrading communities in soil.

    PubMed

    Gonod, Laure Vieublé; Martin-Laurent, Fabrice; Chenu, Claire

    2006-12-01

    The key role of telluric microorganisms in pesticide degradation is well recognized but the possible relationships between the biodiversity of soil microbial communities and their functions still remain poorly documented. If microorganisms influence the fate of pesticides, pesticide application may reciprocally affect soil microorganisms. The objective of our work was to estimate the impact of 2,4-D application on the genetic structure of bacterial communities and the 2,4-D-degrading genetic potential in relation to 2,4-D mineralization. Experiments combined isotope measurements with molecular analyses. The impact of 2,4-D on soil bacterial populations was followed with ribosomal intergenic spacer analysis. The 2,4-D degrading genetic potential was estimated by real-time PCR targeted on tfdA sequences coding an enzyme specifically involved in 2,4-D mineralization. The genetic structure of bacterial communities was significantly modified in response to 2,4-D application, but only during the intense phase of 2,4-D biodegradation. This effect disappeared 7 days after the treatment. The 2,4-D degrading genetic potential increased rapidly following 2,4-D application. There was a concomitant increase between the tfdA copy number and the 14C microbial biomass. The maximum of tfdA sequences corresponded to the maximum rate of 2,4-D mineralization. In this soil, 2,4-D degrading microbial communities seem preferentially to use the tfd pathway to degrade 2,4-D. PMID:17117994

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

    SciTech Connect

    El Khoury, Youssef; Van Wilderen, Luuk J. G. W.; Vogt, Tim; Winter, Ernst; Bredenbeck, Jens E-mail: bredenbeck@biophysik.uni-frankfurt.de

    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.

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

    PubMed

    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. PMID:26329169

  4. Ultrafast hydrolysis of a Lewis photoacid.

    PubMed

    Henrich, Joseph D; Suchyta, Scott; Kohler, Bern

    2015-02-12

    that the strongly oxidizing excited state of MV(2+) triggers the proton-coupled oxidation of a water molecule. The observed kinetic isotope effect of 1.7 seen in D2O vs H2O is of the magnitude expected for an ultrafast concerted proton-electron transfer reaction. The ultrafast hydrolysis seen here may be a general excited-state quenching mechanism for electronically excited Lewis acids and other powerful photooxidants in aqueous solution. PMID:25510461

  5. Uniform distribution of projection data for improved reconstruction quality of 4D EPR imaging

    PubMed Central

    Ahmad, Rizwan; Vikram, Deepti S.; Clymer, Bradley; Potter, Lee C.; Deng, Yuanmu; Srinivasan, Parthasarathy; Zweier, Jay L.; Kuppusamy, Periannan

    2008-01-01

    In continuous wave (CW) electron paramagnetic resonance imaging (EPRI), high quality of reconstruction in a limited acquisition time is a high priority. It has been shown for the case of 3D EPRI, that a uniform distribution of the projection data generally enhances reconstruction quality. In this work, we have suggested two data acquisition techniques for which the gradient orientations are more evenly distributed over the 4D acquisition space as compared to the existing methods. The first sampling technique is based on equal solid angle partitioning of 4D space, while the second technique is based on Fekete points estimation in 4D to generate a more uniform distribution of data. After acquisition, filtered backprojection (FBP) is applied to carryout the reconstruction in a single stage. The single-stage reconstruction improves the spatial resolution by eliminating the necessity of data interpolation in multi-stage reconstructions. For the proposed data distributions, the simulations and experimental results indicate a higher fidelity to the true object configuration. Using the uniform distribution, we expect about 50% reduction in the acquisition time over the traditional method of equal linear angle acquisition. PMID:17562375

  6. Non-spherical particle generation from 4D optofluidic fabrication.

    PubMed

    Paulsen, Kevin S; Chung, Aram J

    2016-08-01

    Particles with non-spherical shapes can exhibit properties which are not available from spherical shaped particles. Complex shaped particles can provide unique benefits for areas such as drug delivery, tissue engineering, structural materials, and self-assembly building blocks. Current methods of creating complex shaped particles such as 3D printing, photolithography, and imprint lithography are limited by either slow speeds, shape limitations, or expensive processes. Previously, we presented a novel microfluidic flow lithography fabrication scheme combined with fluid inertia called optofluidic fabrication for the creation of complex shaped three-dimensional (3D) particles. This process was able to address the aforementioned limits and overcome two-dimensional shape limitations faced by traditional flow lithography methods; however, all of the created 3D particle shapes displayed top-down symmetry. Here, by introducing the time dimension into our existing optofluidic fabrication process, we break this top-down symmetry, generating fully asymmetric 3D particles where we termed the process: four-dimensional (4D) optofluidic fabrication. This 4D optofluidic fabrication is comprised of three sequential procedures. First, density mismatched precursor fluids flow past pillars within fluidic channels to manipulate the flow cross sections via fluid inertia. Next, the time dimension is incorporated by stopping the flow and allowing the denser fluids to settle by gravity to create asymmetric flow cross sections. Finally, the fluids are exposed to patterned ultraviolet (UV) light in order to polymerize fully asymmetric 3D-shaped particles. By varying inertial flow shaping, gravity-induced flow shaping, and UV light patterns, 4D optofluidic fabrication can create an infinite set of complex shaped asymmetric particles. PMID:27092661

  7. 4D Proton treatment planning strategy for mobile lung tumors

    SciTech Connect

    Kang Yixiu; Zhang Xiaodong; Chang, Joe Y.; Wang He; Wei Xiong; Liao Zhongxing; Komaki, Ritsuko; Cox, James D.; Balter, Peter A.; Liu, Helen; Zhu, X. Ronald; Mohan, Radhe; Dong Lei . E-mail: ldong@mdanderson.org

    2007-03-01

    Purpose: To investigate strategies for designing compensator-based 3D proton treatment plans for mobile lung tumors using four-dimensional computed tomography (4DCT) images. Methods and Materials: Four-dimensional CT sets for 10 lung cancer patients were used in this study. The internal gross tumor volume (IGTV) was obtained by combining the tumor volumes at different phases of the respiratory cycle. For each patient, we evaluated four planning strategies based on the following dose calculations: (1) the average (AVE) CT; (2) the free-breathing (FB) CT; (3) the maximum intensity projection (MIP) CT; and (4) the AVE CT in which the CT voxel values inside the IGTV were replaced by a constant density (AVE{sub R}IGTV). For each strategy, the resulting cumulative dose distribution in a respiratory cycle was determined using a deformable image registration method. Results: There were dosimetric differences between the apparent dose distribution, calculated on a single CT dataset, and the motion-corrected 4D dose distribution, calculated by combining dose distributions delivered to each phase of the 4DCT. The AVE{sub R}IGTV plan using a 1-cm smearing parameter had the best overall target coverage and critical structure sparing. The MIP plan approach resulted in an unnecessarily large treatment volume. The AVE and FB plans using 1-cm smearing did not provide adequate 4D target coverage in all patients. By using a larger smearing value, adequate 4D target coverage could be achieved; however, critical organ doses were increased. Conclusion: The AVE{sub R}IGTV approach is an effective strategy for designing proton treatment plans for mobile lung tumors.

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

    PubMed

    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

    2007-06-21

    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 2pi 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 mue+/-sigmae 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. PMID:17664557

  9. Localization of 4D gravity on pure geometrical thick branes

    SciTech Connect

    Barbosa-Cendejas, Nandinii; Herrera-Aguilar, Alfredo

    2006-04-15

    We consider the generation of thick brane configurations in a pure geometric Weyl integrable 5D spacetime which constitutes a non-Riemannian generalization of Kaluza-Klein (KK) theory. In this framework, we show how 4D gravity can be localized on a scalar thick brane which does not necessarily respect reflection symmetry, generalizing in this way several previous models based on the Randall-Sundrum (RS) system and avoiding both, the restriction to orbifold geometries and the introduction of the branes in the action by hand. We first obtain a thick brane solution that preserves 4D Poincare invariance and breaks Z{sub 2}-symmetry along the extra dimension which, indeed, can be either compact or extended, and supplements brane solutions previously found by other authors. In the noncompact case, this field configuration represents a thick brane with positive energy density centered at y=c{sub 2}, whereas pairs of thick branes arise in the compact case. Remarkably, the Weylian scalar curvature is nonsingular along the fifth dimension in the noncompact case, in contraposition to the RS thin brane system. We also recast the wave equations of the transverse traceless modes of the linear fluctuations of the classical background into a Schroedinger's equation form with a volcano potential of finite bottom in both the compact and the extended cases. We solve Schroedinger equation for the massless zero mode m{sup 2}=0 and obtain a single bound wave function which represents a stable 4D graviton. We also get a continuum gapless spectrum of KK states with m{sup 2}>0 that are suppressed at y=c{sub 2} and turn asymptotically into plane waves.

  10. Multicolor 4D Fluorescence Microscopy using Ultrathin Bessel Light Sheets

    PubMed Central

    Zhao, Teng; Lau, Sze Cheung; Wang, Ying; Su, Yumian; Wang, Hao; Cheng, Aifang; Herrup, Karl; Ip, Nancy Y.; Du, Shengwang; Loy, M. M. T.

    2016-01-01

    We demonstrate a simple and efficient method for producing ultrathin Bessel (‘non-diffracting’) light sheets of any color using a line-shaped beam and an annulus filter. With this robust and cost-effective technology, we obtained two-color, 3D images of biological samples with lateral/axial resolution of 250 nm/400 nm, and high-speed, 4D volume imaging of 20 μm sized live sample at 1 Hz temporal resolution. PMID:27189786

  11. All the supersymmetric configurations of N=4, d=4 supergravity

    NASA Astrophysics Data System (ADS)

    Bellorín, Jorge; Ortín, Tomás

    2005-10-01

    All the supersymmetric configurations of pure, ungauged, N=4, d=4 supergravity are classified in a formalism that keeps manifest the S and T dualities of the theory. We also find simple equations that need to be satisfied by the configurations to be classical solutions of the theory. While the solutions associated to null Killing vectors were essentially classified by Tod (a classification that we refine), we find new configurations and solutions associated to timelike Killing vectors that do not satisfy Tod's rigidity hypothesis (hence, they have a nontrivial U(1) connection) and whose supersymmetry projector is associated to 1-dimensional objects (strings), although they have a trivial axion field.

  12. Founding Gravitation in 4D Euclidean Space-Time Geometry

    SciTech Connect

    Winkler, Franz-Guenter

    2010-11-24

    The Euclidean interpretation of special relativity which has been suggested by the author is a formulation of special relativity in ordinary 4D Euclidean space-time geometry. The natural and geometrically intuitive generalization of this view involves variations of the speed of light (depending on location and direction) and a Euclidean principle of general covariance. In this article, a gravitation model by Jan Broekaert, which implements a view of relativity theory in the spirit of Lorentz and Poincare, is reconstructed and shown to fulfill the principles of the Euclidean approach after an appropriate reinterpretation.

  13. Actively triggered 4d cone-beam CT acquisition

    SciTech Connect

    Fast, Martin F.; Wisotzky, Eric; Oelfke, Uwe; Nill, Simeon

    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

  14. 4D micro-CT using fast prospective gating

    NASA Astrophysics Data System (ADS)

    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

  15. Multicolor 4D Fluorescence Microscopy using Ultrathin Bessel Light Sheets.

    PubMed

    Zhao, Teng; Lau, Sze Cheung; Wang, Ying; Su, Yumian; Wang, Hao; Cheng, Aifang; Herrup, Karl; Ip, Nancy Y; Du, Shengwang; Loy, M M T

    2016-01-01

    We demonstrate a simple and efficient method for producing ultrathin Bessel ('non-diffracting') light sheets of any color using a line-shaped beam and an annulus filter. With this robust and cost-effective technology, we obtained two-color, 3D images of biological samples with lateral/axial resolution of 250 nm/400 nm, and high-speed, 4D volume imaging of 20 μm sized live sample at 1 Hz temporal resolution. PMID:27189786

  16. Ultrafast broadband spectroscopy of crystalline bismuth

    SciTech Connect

    Mel'nikov, A A; Misochko, Oleg V; Chekalin, Sergei V

    2013-04-30

    Femtosecond spectroscopy in the wavelength range 0.4 - 2.3 {mu}m has been used to probe ultrafast electronic and lattice processes in bismuth. The photoresponse of a bismuth crystal is shown to comprise components with relaxation times of 1 ps, 7 ps, and {approx}1 ns. The electron-hole and electron-phonon interaction strengths in bismuth are found to depend significantly on the wave vector in the {Gamma}-T direction of the Brillouin zone. Comparison of the spectral dependences of the amplitudes of coherent E{sub g} and A{sub 1g} phonons and the corresponding dependences of the Raman scattering cross sections indicates that these phonon modes differ in generation mechanism. The generation of coherent A{sub 1g} phonons is mainly due to displacement of the equilibrium position of atoms in the crystal lattice in a nonequilibrium state. This process differs fundamentally from resonance Raman scattering responsible for the coherent excitation of low-symmetry phonon modes. (extreme light fields and their applications)

  17. Spin Dynamics during Ultrafast Optical Demagnetization

    NASA Astrophysics Data System (ADS)

    Eisebitt, Stefan

    2015-03-01

    Magnetic order can be influenced on a sub-picosecund time scale via femtosecond optical pulses. In particular, demagnetization and switching can be triggered optically and while the applications e.g. for magnetic data storage are obvious, the underlying mechanisms are still under debate. We have investigated the contribution of electronic transport to optical demagnetization via pump-probe experiments at free-electron x-ray lasers. In ferromagnetic thin film multilayers with perpendicular anisotropy, optically excited electrons can move within a labyrinth domain network. Using x-ray magnetic circular dichroism (XMCD) as a contrast mechanism for small angle x-ray scattering to probe the local magnetization, we observe an ultrafast broadening of the domain walls, consistent with the existence of superdiffusive spin currents. Via pump-probe x-ray holographic imaging we obtain real space images of the local magnetization within the domain structure after pumping the system by a laterally confined excitation generated by an optical standing wave. With a temporal resolution of about 100 fs, we observe the propagation of a demagnetization front in real space, again consistent with the existence of superdiffusive spin currents. Support by BMBF in FSP-301 and 302 via Contracts 05K10KTB, 05K13KT3 and 05K13KT4 is gratefully acknowledged.

  18. Substrate dependent ultrafast dynamics in thin NiFe films

    NASA Astrophysics Data System (ADS)

    Bosco, C. A. C.; Azevedo, A.; Acioli, L. H.

    2003-09-01

    We have studied the ultrafast electronic response of thin NiFe films by femtosecond transient reflectivity measurements. The experiments were performed on films with varying thicknesses, substrates, and pump fluences. It has been observed that for high excitation densities the electron cooling time depends strongly on the nature of the underlying substrate and we attribute our results to transport of hot carriers out of the excited region. In particular, we have observed that for NiFe over NiO, carrier transport should be less important than for NiFe over Si.

  19. 3D and 4D Simulations of the Dynamics of the Radiation Belts using VERB code

    NASA Astrophysics Data System (ADS)

    Shprits, Yuri; Kellerman, Adam; Drozdov, Alexander; Orlova, Ksenia

    2015-04-01

    Modeling and understanding of ring current and higher energy radiation belts has been a grand challenge since the beginning of the space age. In this study we show long term simulations with a 3D VERB code of modeling the radiation belts with boundary conditions derived from observations around geosynchronous orbit. We also present 4D VERB simulations that include convective transport, radial diffusion, pitch angle scattering and local acceleration. We show that while lower energy radial transport is dominated by the convection and higher energy transport is dominated by the diffusive radial transport. We also show there exists an intermediate range of energies for electrons for which both processes work simultaneously.

  20. Energy transport in ultra-fast eated solid targets

    NASA Astrophysics Data System (ADS)

    Sentoku, Yasuhiko; Johzaki, Tomoyuki; Kemp, Andreas

    2008-11-01

    We discuss hot electron generation in ultra intense laser interaction with initially non-ionized matter. Hot electron energy and the transport inside the target are strongly affected by collisional effects and ionization processes, especially in high-Z material. We have introduced an ionization model into our collisional particle-in-cell code, PICLS, to study hot electron transport in ultra-fast heated matter. Our description of collisional ionization is based on the Thomas-Fermi model, where a local average charge state is calculated from the bulk electron temperature and density. Field ionization is taken into account for ionization of low density plasmas. We have studied laser matter interaction under an irradiation of a laser with 10^20W/cm^2. A strong heat inhibition within a micron distance was observed in a gold target because of the large number of lower energy hot electrons produced at the steepened interface by the laser photon pressure. We will discuss the generation of hot electrons and their transport in ultra-fast heated solid targets of various materials.