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

KAUST Repository

Adhikari, Aniruddha

2016-12-15

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

Ultrafast electron microscopy in materials science, biology, and chemistry

International Nuclear Information System (INIS)

King, Wayne E.; Campbell, Geoffrey H.; Frank, Alan; Reed, Bryan; Schmerge, John F.; Siwick, Bradley J.; Stuart, Brent C.; Weber, Peter M.

2005-01-01

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

Ultrafast dynamics of correlated electrons

International Nuclear Information System (INIS)

Rettig, Laurenz

2012-01-01

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

Ultrafast Plasmonic Electron Emission from Ag Nanolayers with Different Roughness

Czech Academy of Sciences Publication Activity Database

Márton, I.; Ayadi, V.; Rácz, P.; Stefaniuk, T.; Wróbel, Piotr; Földi, P.; Dombi, P.

2016-01-01

Roč. 11, č. 3 (2016), s. 811-816 ISSN 1557-1955 Institutional support: RVO:67985882 Keywords : Nanoparticles * Ultrafast phenomena * Electron emission Subject RIV: JA - Electronics ; Optoelectronics, Electrical Engineering Impact factor: 2.139, year: 2016

Ultrafast transient-absorption of the solvated electron in water

International Nuclear Information System (INIS)

Kimura, Y.; Alfano, J.C.; Walhout, P.K.; Barbara, P.F.

1994-01-01

Ultrafast near infrared (NIR)-pump/variable wavelength probe transient-absorption spectroscopy has been performed on the aqueous solvated electron. The photodynamics of the solvated electron excited to its p-state are qualitatively similar to previous measurements of the dynamics of photoinjected electrons at high energy. This result confirms the previous interpretation of photoinjected electron dynamics as having a rate-limiting bottleneck at low energies presumably involving the p-state

Ultrafast dynamics of correlated electrons

Energy Technology Data Exchange (ETDEWEB)

Rettig, Laurenz

2012-07-09

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

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

International Nuclear Information System (INIS)

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

2015-01-01

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

Analytic model of electron pulse propagation in ultrafast electron diffraction experiments

International Nuclear Information System (INIS)

Michalik, A.M.; Sipe, J.E.

2006-01-01

We present a mean-field analytic model to study the propagation of electron pulses used in ultrafast electron diffraction experiments (UED). We assume a Gaussian form to characterize the electron pulse, and derive a system of ordinary differential equations that are solved quickly and easily to give the pulse dynamics. We compare our model to an N-body numerical simulation and are able to show excellent agreement between the two result sets. This model is a convenient alternative to time consuming and computationally intense N-body simulations in exploring the dynamics of UED electron pulses, and as a tool for refining UED experimental designs

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

KAUST Repository

Aly, Shawkat Mohammede

2014-10-02

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

Hot-electrons-induced ultrafast demagnitization in Co/Pt multilayers

NARCIS (Netherlands)

Bergeard, N.; Hehn, M.; Mangin, S.; Lengaigne, G.; Montaigne, F.; Lalieu, M. L. M.; Koopmans, B.; Malinowski, G.

2016-01-01

Using specially engineered structures to tailor the optical absorption in a metallic multilayer, we analyze the magnetization dynamics of a Co/Pt multilayer buried below a thick Cu layer. We demonstrate that hot electrons alone can very efficiently induce ultrafast demagnetization. Simulations based

Overview of interatomic potentials

International Nuclear Information System (INIS)

Bonny, G.; Malerba, L.

2005-12-01

In this report an overview on interatomic potentials is given. This overview is by no means complete and it has merely the intention to give the reader an idea of where interatomic potentials come from, as well as to provide the basic ideas behind some commonly used methods for deriving interatomic potentials for molecular dynamics applications. We start by giving a short introduction about the concept of interatomic potential in the framework of quantum mechanics, followed by a short description of commonly used methods for deriving semi-empirical interatomic potentials. After some short theoretical notions on each method, some practical parameterizations of commonly used potentials are given, including very recent ones. An effort has been made to classify existing approaches within a rational and consequent scheme, which is believed to be of use for a thorough comprehension of the topic. Although these approaches can be used in a variety of different materials, we will only discuss the practical cases of metals. Following this, some widespread ad hoc modification of the general methods are discussed. The report is concluded by a generalization of the methods to multi-component materials, in particular metallic alloys. (author)

Interatomic inelastic current

DEFF Research Database (Denmark)

Hansen, Tim; Solomon, Gemma C.; Hansen, Thorsten

2017-01-01

In order to identify the location of an inelastic event and to distinguish between situations that are before or after this event, we derive equations for the interatomic inelastic transmission as a perturbation series in the electron-phonon interaction. This series contains both even and odd...... to second order and the 1st order correction represents the lowest order term of this new family of terms. We apply this to three model systems and are able to distinguish between situations before and after the inelastic event as steps in the 2nd order transmission. We also see that when the transmission...

[Non-empirical interatomic potentials for transition metals

International Nuclear Information System (INIS)

1993-01-01

The report is divided into the following sections: potential-energy functions for d-band metals, potential-energy functions for aluminides and quasicrystals, electronic structure of complex structures and quasicrystals, potential-energy functions in transition-metal oxides, applications to defect structure and mechanical properties, and basic theory of interatomic potentials

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

KAUST Repository

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

2016-01-01

Four-dimensional ultrafast electron microscopy (4D-UEM) is a novel analytical technique that aims to fulfill the long-held dream of researchers to investigate materials at extremely short spatial and temporal resolutions by integrating the excellent

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

International Nuclear Information System (INIS)

Carpene, E; Mancini, E; Dallera, C; Schwen, D; Ronning, C; Silvestri, S De

2007-01-01

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

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

Energy Technology Data Exchange (ETDEWEB)

Qiu Weihong; Li Tanping; Zhang Luyuan; Yang Yi; Kao Yating; Wang Lijuan [Department of Physics, Chemistry, and Biochemistry, Program of Biophysics, Chemical Physics, and Biochemistry, Ohio State University, Columbus, OH 43210 (United States); Zhong Dongping [Department of Physics, Chemistry, and Biochemistry, Program of Biophysics, Chemical Physics, and Biochemistry, Ohio State University, Columbus, OH 43210 (United States)], E-mail: dongping@mps.ohio-state.edu

2008-06-23

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.

Ultrafast electron microscopy integrated with a direct electron detection camera.

Science.gov (United States)

Lee, Young Min; Kim, Young Jae; Kim, Ye-Jin; Kwon, Oh-Hoon

2017-07-01

In the past decade, we have witnessed the rapid growth of the field of ultrafast electron microscopy (UEM), which provides intuitive means to watch atomic and molecular motions of matter. Yet, because of the limited current of the pulsed electron beam resulting from space-charge effects, observations have been mainly made to periodic motions of the crystalline structure of hundreds of nanometers or higher by stroboscopic imaging at high repetition rates. Here, we develop an advanced UEM with robust capabilities for circumventing the present limitations by integrating a direct electron detection camera for the first time which allows for imaging at low repetition rates. This approach is expected to promote UEM to a more powerful platform to visualize molecular and collective motions and dissect fundamental physical, chemical, and materials phenomena in space and time.

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

DEFF Research Database (Denmark)

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

2013-01-01

photo-initiated interfacial electron transfer. This approach enables time-resolved study of the fate and mobility of electrons within the solid phase. However, complete analysis of the ultrafast processes following dye photoexcitation of the sensitized iron(iii) oxide nanoparticles has not been reported....... We addressed this topic by performing femtosecond transient absorption (TA) measurements of aqueous suspensions of uncoated and DCF-sensitized iron oxide and oxyhydroxide nanoparticles, and an aqueous iron(iii)–dye complex. Following light absorption, excited state relaxation times of the dye of 115...... a four-state model of the dye-sensitized system, finding electron and energy transfer to occur on the same ultrafast timescale. The interfacial electron transfer rates for iron oxides are very close to those previously reported for DCF-sensitized titanium dioxide (for which dye–oxide energy transfer...

Concept and design of a beam blanker with integrated photoconductive switch for ultrafast electron microscopy.

Science.gov (United States)

Weppelman, I G C; Moerland, R J; Hoogenboom, J P; Kruit, P

2018-01-01

We present a new method to create ultrashort electron pulses by integrating a photoconductive switch with an electrostatic deflector. This paper discusses the feasibility of such a system by analytical and numerical calculations. We argue that ultrafast electron pulses can be achieved for micrometer scale dimensions of the blanker, which are feasible with MEMS-based fabrication technology. According to basic models, the design presented in this paper is capable of generating 100 fs electron pulses with spatial resolutions of less than 10 nm. Our concept for an ultrafast beam blanker (UFB) may provide an attractive alternative to perform ultrafast electron microscopy, as it does not require modification of the microscope nor realignment between DC and pulsed mode of operation. Moreover, only low laser pulse energies are required. Due to its small dimensions the UFB can be inserted in the beam line of a commercial microscope via standard entry ports for blankers or variable apertures. The use of a photoconductive switch ensures minimal jitter between laser and electron pulses. Copyright © 2017 Elsevier B.V. All rights reserved.

Design and commissioning of an aberration-corrected ultrafast spin-polarized low energy electron microscope with multiple electron sources.

Science.gov (United States)

Wan, Weishi; Yu, Lei; Zhu, Lin; Yang, Xiaodong; Wei, Zheng; Liu, Jefferson Zhe; Feng, Jun; Kunze, Kai; Schaff, Oliver; Tromp, Ruud; Tang, Wen-Xin

2017-03-01

We describe the design and commissioning of a novel aberration-corrected low energy electron microscope (AC-LEEM). A third magnetic prism array (MPA) is added to the standard AC-LEEM with two prism arrays, allowing the incorporation of an ultrafast spin-polarized electron source alongside the standard cold field emission electron source, without degrading spatial resolution. The high degree of symmetries of the AC-LEEM are utilized while we design the electron optics of the ultrafast spin-polarized electron source, so as to minimize the deleterious effect of time broadening, while maintaining full control of electron spin. A spatial resolution of 2nm and temporal resolution of 10ps (ps) are expected in the future time resolved aberration-corrected spin-polarized LEEM (TR-AC-SPLEEM). The commissioning of the three-prism AC-LEEM has been successfully finished with the cold field emission source, with a spatial resolution below 2nm. Copyright © 2017 Elsevier B.V. All rights reserved.

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

Energy Technology Data Exchange (ETDEWEB)

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

2015-12-07

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

Ultrafast electron microscopy integrated with a direct electron detection camera

Directory of Open Access Journals (Sweden)

Young Min Lee

2017-07-01

Full Text Available In the past decade, we have witnessed the rapid growth of the field of ultrafast electron microscopy (UEM, which provides intuitive means to watch atomic and molecular motions of matter. Yet, because of the limited current of the pulsed electron beam resulting from space-charge effects, observations have been mainly made to periodic motions of the crystalline structure of hundreds of nanometers or higher by stroboscopic imaging at high repetition rates. Here, we develop an advanced UEM with robust capabilities for circumventing the present limitations by integrating a direct electron detection camera for the first time which allows for imaging at low repetition rates. This approach is expected to promote UEM to a more powerful platform to visualize molecular and collective motions and dissect fundamental physical, chemical, and materials phenomena in space and time.

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

NARCIS (Netherlands)

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

2000-01-01

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

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

Science.gov (United States)

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.

Ultrafast electron microscopy: Instrument response from the single-electron to high bunch-charge regimes

Science.gov (United States)

Plemmons, Dayne A.; Flannigan, David J.

2017-09-01

We determine the instrument response of an ultrafast electron microscope equipped with a conventional thermionic electron gun and absent modifications beyond the optical ports. Using flat, graphite-encircled LaB6 cathodes, we image space-charge effects as a function of photoelectron-packet population and find that an applied Wehnelt bias has a negligible effect on the threshold levels (>103 electrons per pulse) but does appear to suppress blurring at the upper limits (∼105 electrons). Using plasma lensing, we determine the instrument-response time for 700-fs laser pulses and find that single-electron packets are laser limited (1 ps), while broadening occurs well below the space-charge limit.

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

Science.gov (United States)

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

2015-07-21

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 (k(e)∼ 5 × 10(14) 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.

Attractive short-range interatomic potential in the lattice dynamics of niobium and tantalum

International Nuclear Information System (INIS)

Onwuagba, B.N.; Pal, S.

1987-01-01

It is shown in the framework of the pseudopotential approach that there is a sizable attractive short-range component of the interatomic potential due to the s-d interaction which has the same functional form in real space as the Born-Mayer repulsion due to the overlap of core electron wave functions centred on neighbouring ions. The magnitude of this attractive component is such as to completely cancel the conventional Born-Mayer repulsion, making the resultant short-range interatomic potential attractive rather than repulsive. Numerical calculations show that the attractive interatomics potential, which represents the local-field correction, leads to a better understanding of the occurrence of the soft modes in the phonon dispersion curves of niobium and tantalum

INTERATOM experience of cleaning sodium-wetted components

International Nuclear Information System (INIS)

Haubold, W.

1978-01-01

INTERATOM has been concerned since 1967 with the development, testing, and application of methods to clean sodium wetted components by moist nitrogen, vacuum distillation or alcohol. The activities of INTERATOM in this area have been reported at the IAEA Specialists Meeting on 'Decontamination of Plant Components from Sodium and Radioactivity' in Dounreay, April 9-12, 1973. The three cleaning methods mentioned above are practised at present, too - with minor modifications - by INTERATOM and in the facilities of the SNR project. This note summarizes the experiences of INTERATOM with methods of sodium removal since 1973

Temperature dependence in interatomic potentials and an improved potential for Ti

International Nuclear Information System (INIS)

Ackland, G J

2012-01-01

The process of deriving an interatomic potentials represents an attempt to integrate out the electronic degrees of freedom from the full quantum description of a condensed matter system. In practice it is the derivatives of the interatomic potentials which are used in molecular dynamics, as a model for the forces on a system. These forces should be the derivative of the free energy of the electronic system, which includes contributions from the entropy of the electronic states. This free energy is weakly temperature dependent, and although this can be safely neglected in many cases there are some systems where the electronic entropy plays a significant role. Here a method is proposed to incorporate electronic entropy in the Sommerfeld approximation into empirical potentials. The method is applied as a correction to an existing potential for titanium. Thermal properties of the new model are calculated, and a simple method for fixing the melting point and solid-solid phase transition temperature for existing models fitted to zero temperature data is presented.

The screening length of interatomic potential in atomic collisions

International Nuclear Information System (INIS)

Yamamura, Y.; Takeuchi, W.; Kawamura, T.

1998-03-01

In computer studies on the interaction of charged particle with solids, many authors treat the nuclear collision by the Thomas-Fermi screened Coulomb potential. For better agreement with experiment, the screening length is modified sometimes. We investigate the theoretical background for the correction factor of the screening length in the interatomic potential which can be deduced from two steps. The first step is to select the correction factor of an isolated atom so as to match the average radius of the Thomas-Fermi electron distribution with that of the Hartree-Fock electron distribution, where we use the Clementi and Roetti's table. The second step is to determine the correction factor of the screening length of the interatomic potential by using a combination rule. The correction factors obtained for the screening length are in good agreement with those determined by the computer analysis of the Impact Collision Ion Scattering Spectroscopy (ICISS) data. (author)

Ultrafast Electron Dynamics in Solar Energy Conversion.

Science.gov (United States)

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

2017-08-23

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

Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

Energy Technology Data Exchange (ETDEWEB)

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

2015-01-01

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

A novel proof of the DFT formula for the interatomic force field of Molecular Dynamics

International Nuclear Information System (INIS)

Morante, S.; Rossi, G.C.

2017-01-01

We give a novel and simple proof of the DFT expression for the interatomic force field that drives the motion of atoms in classical Molecular Dynamics, based on the observation that the ground state electronic energy, seen as a functional of the external potential, is the Legendre transform of the Hohenberg–Kohn functional, which in turn is a functional of the electronic density. We show in this way that the so-called Hellmann–Feynman analytical formula, currently used in numerical simulations, actually provides the exact expression of the interatomic force.

A novel proof of the DFT formula for the interatomic force field of Molecular Dynamics

Energy Technology Data Exchange (ETDEWEB)

Morante, S., E-mail: morante@roma2.infn.it [Dipartimento di Fisica, Università di Roma, “ Tor Vergata ”, INFN, Sezione di Roma 2, Via della Ricerca Scientifica - 00133 Roma (Italy); Rossi, G.C., E-mail: rossig@roma2.infn.it [Dipartimento di Fisica, Università di Roma, “ Tor Vergata ”, INFN, Sezione di Roma 2, Via della Ricerca Scientifica - 00133 Roma (Italy); Centro Fermi-Museo Storico della Fisica e Centro Studi e Ricerche E. Fermi, Compendio del Viminale, Piazza del Viminale 1, I-00184 Rome (Italy)

2017-02-15

We give a novel and simple proof of the DFT expression for the interatomic force field that drives the motion of atoms in classical Molecular Dynamics, based on the observation that the ground state electronic energy, seen as a functional of the external potential, is the Legendre transform of the Hohenberg–Kohn functional, which in turn is a functional of the electronic density. We show in this way that the so-called Hellmann–Feynman analytical formula, currently used in numerical simulations, actually provides the exact expression of the interatomic force.

Interatomic decay of inner-valence ionized states in ArXe clusters: Relativistic approach

International Nuclear Information System (INIS)

Fasshauer, Elke; Pernpointner, Markus; Gokhberg, Kirill

2013-01-01

In this work we investigate interatomic electronic decay processes taking place in mixed argon-xenon clusters upon the inner-valence ionization of an argon center. We demonstrate that both interatomic Coulombic decay and electron-transfer mediated decay (ETMD) are important in larger rare gas clusters as opposed to dimers. Calculated secondary electron spectra are shown to depend strongly on the spin-orbit coupling in the final states of the decay as well as the presence of polarizable environment. It follows from our calculations that ETMD is a pure interface process taking place between the argon-xenon layers. The interplay of all these effects is investigated in order to arrive at a suitable physical model for the decay of inner-valence vacancies taking place in mixed ArXe clusters.

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

KAUST Repository

Masih, Dilshad

2015-02-25

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

Bunch evolution study in optimization of MeV ultrafast electron diffraction

International Nuclear Information System (INIS)

Lu Xianhai; Du Yingchao; Huang Wenhui; Tang Chuanxiang

2014-01-01

transverse 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. (authors)

Bunch evolution study in optimization of MeV ultrafast electron diffraction

Science.gov (United States)

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

2014-12-01

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

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

DEFF Research Database (Denmark)

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

2015-01-01

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

Interatom results for stage 2

International Nuclear Information System (INIS)

Coors, D.

1990-01-01

This report contains the Interatom results for Stage 2 of the ''IWGFR Programme on Intercomparison of LMFBR Core Mechanics Codes'' which was agreed upon on a Consultants Meeting in Vienna, 8-10 December, 1987. The calculations were performed with the 3D core mechanics code system DDT developed at Interatom and with the 2D core mechanics code FIAT. (author). 5 refs, 11 figs, 8 tabs

Ultrafast Photoinduced Electron Transfer in Bimolecular Donor-Acceptor Systems

KAUST Repository

Alsulami, Qana A.

2016-11-30

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

Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source.

Science.gov (United States)

Houdellier, F; Caruso, G M; Weber, S; Kociak, M; Arbouet, A

2018-03-01

We report on the development of an ultrafast Transmission Electron Microscope based on a cold field emission source which can operate in either DC or ultrafast mode. Electron emission from a tungsten nanotip is triggered by femtosecond laser pulses which are tightly focused by optical components integrated inside a cold field emission source close to the cathode. The properties of the electron probe (brightness, angular current density, stability) are quantitatively determined. The measured brightness is the largest reported so far for UTEMs. Examples of imaging, diffraction and spectroscopy using ultrashort electron pulses are given. Finally, the potential of this instrument is illustrated by performing electron holography in the off-axis configuration using ultrashort electron pulses. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrafast Gap Dynamics and Electronic Interactions in a Photoexcited Cuprate Superconductor

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S. Parham

2017-10-01

Full Text Available We perform time- and angle-resolved photoemission spectroscopy (trARPES on optimally doped Bi_{2}Sr_{2}CaCu_{2}O_{8+δ} (BSCCO-2212 using sufficient energy resolution (9 meV to resolve the k-dependent near-nodal gap structure on time scales where the concept of an electronic pseudotemperature is a useful quantity, i.e., after electronic thermalization has occurred. We study the ultrafast evolution of this gap structure, uncovering a very rich landscape of decay rates as a function of angle, temperature, and energy. We explicitly focus on the quasiparticle states at the gap edge as well as on the spectral weight inside the gap that “fills” the gap—understood as an interaction, or self-energy effect—and we also make high resolution measurements of the nodal states, enabling a direct and accurate measurement of the electronic temperature (or pseudotemperature of the electrons in the system. Rather than the standard method of interpreting these results using individual quasiparticle scattering rates that vary significantly as a function of angle, temperature, and energy, we show that the entire landscape of relaxations can be understood by modeling the system as following a nonequilibrium, electronic pseudotemperature that controls all electrons in the zone. Furthermore, this model has zero free parameters, as we obtain the crucial information of the SC gap Δ and the gap-filling strength Γ_{TDoS} by connecting to static ARPES measurements. The quantitative and qualitative agreement between data and model suggests that the critical parameters and interactions of the system, including the pairing interactions, follow parametrically from the electronic pseudotemperature. We expect that this concept will be relevant for understanding the ultrafast response of a great variety of electronic materials, even though the electronic pseudotemperature may not be directly measurable.

Mapping momentum-dependent electron-phonon coupling and nonequilibrium phonon dynamics with ultrafast electron diffuse scattering

Science.gov (United States)

Stern, Mark J.; René de Cotret, Laurent P.; Otto, Martin R.; Chatelain, Robert P.; Boisvert, Jean-Philippe; Sutton, Mark; Siwick, Bradley J.

2018-04-01

Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone has remained elusive. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map the relative EPC and PPC strength through their profound sensitivity to photoinduced changes in phonon populations. We measure strong EPC to the K -point TO phonon of A1' symmetry (K -A1' ) and along the entire TO branch between Γ -K , not only to the Γ -E2 g phonon. We also determine that the subsequent phonon relaxation of these strongly coupled optical phonons involve three stages: decay via several identifiable channels to TA and LA phonons (1 -2 ps), intraband thermalization of the non-equilibrium TA/LA phonon populations (30 -40 ps) and interband relaxation of the TA/LA modes (115 ps). Combining UEDS with ultrafast angle-resolved photoelectron spectroscopy will yield a complete picture of the dynamics within and between electron and phonon subsystems, helping to unravel complex phases in which the intertwined nature of these systems has a strong influence on emergent properties.

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

Science.gov (United States)

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

2013-02-01

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

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

Energy Technology Data Exchange (ETDEWEB)

He, Z.-H.; Thomas, A. G. R.; Nees, J. A.; Hou, B.; Krushelnick, K. [Center for Ultrafast Optical Science, University of Michigan, Ann Arbor, Michigan 48106-2099 (United States); Beaurepaire, B.; Malka, V.; Faure, J. [Laboratoire d' Optique Appliquee, ENSTA-CNRS-Ecole Polytechnique, UMR 7639, 91761 Palaiseau (France)

2013-02-11

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.

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

International Nuclear Information System (INIS)

Shafizadeh, Niloufar; Poisson, Lionel; Soep, Benoit

2008-01-01

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

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

Science.gov (United States)

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

2014-09-01

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

Diffraction contrast as a sensitive indicator of femtosecond sub-nanoscale motion in ultrafast transmission electron microscopy

Science.gov (United States)

Cremons, Daniel R.; Schliep, Karl B.; Flannigan, David J.

2013-09-01

With ultrafast transmission electron microscopy (UTEM), access can be gained to the spatiotemporal scales required to directly visualize rapid, non-equilibrium structural dynamics of materials. This is achieved by operating a transmission electron microscope (TEM) in a stroboscopic pump-probe fashion by photoelectrically generating coherent, well-timed electron packets in the gun region of the TEM. These probe photoelectrons are accelerated down the TEM column where they travel through the specimen before reaching a standard, commercially-available CCD detector. A second laser pulse is used to excite (pump) the specimen in situ. Structural changes are visualized by varying the arrival time of the pump laser pulse relative to the probe electron packet at the specimen. Here, we discuss how ultrafast nanoscale motions of crystalline materials can be visualized and precisely quantified using diffraction contrast in UTEM. Because diffraction contrast sensitively depends upon both crystal lattice orientation as well as incoming electron wavevector, minor spatial/directional variations in either will produce dynamic and often complex patterns in real-space images. This is because sections of the crystalline material that satisfy the Laue conditions may be heterogeneously distributed such that electron scattering vectors vary over nanoscale regions. Thus, minor changes in either crystal grain orientation, as occurs during specimen tilting, warping, or anisotropic expansion, or in the electron wavevector result in dramatic changes in the observed diffraction contrast. In this way, dynamic contrast patterns observed in UTEM images can be used as sensitive indicators of ultrafast specimen motion. Further, these motions can be spatiotemporally mapped such that direction and amplitude can be determined.

Probing Ultrafast Electron Dynamics at Surfaces Using Soft X-Ray Transient Reflectivity Spectroscopy

Science.gov (United States)

Baker, L. Robert; Husek, Jakub; Biswas, Somnath; Cirri, Anthony

The ability to probe electron dynamics with surface sensitivity on the ultrafast time scale is critical for understanding processes such as charge separation, injection, and surface trapping that mediate efficiency in catalytic and energy conversion materials. Toward this goal, we have developed a high harmonic generation (HHG) light source for femtosecond soft x-ray reflectivity. Using this light source we investigated the ultrafast carrier dynamics at the surface of single crystalline α-Fe2O3, polycrystalline α-Fe2O3, and the mixed metal oxide, CuFeO2. We have recently demonstrated that CuFeO2 in particular is a selective catalyst for photo-electrochemical CO2 reduction to acetate; however, the role of electronic structure and charge carrier dynamics in mediating catalytic selectivity has not been well understood. Soft x-ray reflectivity measurements probe the M2,3, edges of the 3d transition metals, which provide oxidation and spin state resolution with element specificity. In addition to chemical state specificity, these measurements are also surface sensitive, and by independently simulating the contributions of the real and imaginary components of the complex refractive index, we can differentiate between surface and sub-surface contributions to the excited state spectrum. Accordingly, this work demonstrates the ability to probe ultrafast carrier dynamics in catalytic materials with element and chemical state specificity and with surface sensitivity.

High peak power THz source for ultrafast electron diffraction

Directory of Open Access Journals (Sweden)

Shengguang Liu

2018-01-01

Full Text Available Terahertz (THz science and technology have already become the research highlight at present. In this paper, we put forward a device setup to carry out ultrafast fundamental research. A photocathode RF gun generates electron bunches with ∼MeV energy, ∼ps bunch width and about 25pC charge. The electron bunches inject the designed wiggler, the coherent radiation at THz spectrum emits from these bunches and increases rapidly until the saturation at ∼MW within a short wiggler. THz pulses can be used as pump to stimulate an ultra-short excitation in some kind of sample. Those electron bunches out of wiggler can be handled into bunches with ∼1pC change, small beam spot and energy spread to be probe. Because the pump and probe comes from the same electron source, synchronization between pump and probe is inherent. The whole facility can be compacted on a tabletop.

Orientational anharmonicity of interatomic interaction in cubic monocrystals

International Nuclear Information System (INIS)

Belomestnykh, Vladimir N.; Tesleva, Elena P.

2010-01-01

Anharmonicity of interatomic interaction from a position of physical acoustics under the standard conditions is investigated. It is shown that the measure of anharmonicity of interatomic interaction (Grilneisen parameter) is explicitly expressed through velocities of sound. Calculation results of orientation anharmonicity are shown on the example of 116 cubic monocrystals with different lattice structural type and type of chemical bond. Two types of anharmonicity interatomic interaction anisotropy are determined. Keywords: acoustics, orientational anharmonicity, Gruneisen parameter, velocity of sound

Ultrafast molecular dynamics illuminated with synchrotron radiation

International Nuclear Information System (INIS)

Bozek, John D.; Miron, Catalin

2015-01-01

Highlights: • Ultrafast molecular dynamics probed with synchrotron radiation. • Core-excitation as probe of ultrafast dynamics through core-hole lifetime. • Review of experimental and theoretical methods in ultrafast dynamics using core-level excitation. - Abstract: Synchrotron radiation is a powerful tool for studying molecular dynamics in small molecules in spite of the absence of natural matching between the X-ray pulse duration and the time scale of nuclear motion. Promoting core level electrons to unoccupied molecular orbitals simultaneously initiates two ultrafast processes, nuclear dynamics on the potential energy surfaces of the highly excited neutral intermediate state of the molecule on the one hand and an ultrafast electronic decay of the intermediate excited state to a cationic final state, characterized by a core hole lifetime. The similar time scales of these processes enable core excited pump-probe-type experiments to be performed with long duration X-ray pulses from a synchrotron source. Recent results obtained at the PLIEADES beamline concerning ultrafast dissociation of core excited states and molecular potential energy curve mapping facilitated by changes in the geometry of the short-lived intermediate core excited state are reviewed. High brightness X-ray beams combined with state-of-the art electron and ion-electron coincidence spectrometers and highly sophisticated theoretical methods are required to conduct these experiments and to achieve a full understanding of the experimental results.

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

KAUST Repository

Aly, Shawkat Mohammede

2015-03-05

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

The Investigation of New Magnetic Materials and Their Phenomena Using Ultrafast Fresnel Transmission Electron Microscopy

Science.gov (United States)

Schliep, Karl B.

State-of-the-art technology drives scientific progress, pushing the boundaries of our current understanding of fundamental processes and mechanisms. Our continual scientific advancement is hindered only by what we can observe and experimentally verify; thus, it is reasonable to assert that instrument development and improvement is the cornerstone for technological and intellectual growth. For example, the invention of transmission electron microscopy (TEM) allowed us to observe nanoscale phenomena for the first time in the 1930s and even now it is invaluable in the development of smaller, faster electronics. As we uncover more about the fundamentals of nanoscale phenomena, we have realized that images alone reveal only a snapshot of the story; to continue progressing we need a way to observe the entire scene unfold (e.g. how defects affect the flow of current across a transistor or how thermal energy propagates in nanoscale systems like graphene). Recently, by combining the spatial resolution of a TEM with the temporal resolution of ultrafast lasers, ultrafast electron microscopy ? or microscope ? (UEM) has allowed us to simultaneously observe transient nanoscale phenomena at ultrafast timescales. Ultrafast characterization techniques allow for the investigation of a new realm of previously unseen phenomenon inherent to the transient electronic, magnetic, and structural properties of materials. However, despite the progress made in ultrafast techniques, capturing the nanoscale spatial sub-ns temporal mechanisms and phenomenon at play in magnetic materials (especially during the operation of magnetic devices) has only recently become possible using UEM. With only a handful of instruments available, magnetic characterization using UEM is far from commonplace and any advances made are sparsely reported, and further, specific to the individual instrument. In this dissertation, I outline the development of novel magnetic materials and the establishment of a UEM lab at

Structural dynamics of surfaces by ultrafast electron crystallography: experimental and multiple scattering theory.

Science.gov (United States)

Schäfer, Sascha; Liang, Wenxi; Zewail, Ahmed H

2011-12-07

Recent studies in ultrafast electron crystallography (UEC) using a reflection diffraction geometry have enabled the investigation of a wide range of phenomena on the femtosecond and picosecond time scales. In all these studies, the analysis of the diffraction patterns and their temporal change after excitation was performed within the kinematical scattering theory. In this contribution, we address the question, to what extent dynamical scattering effects have to be included in order to obtain quantitative information about structural dynamics. We discuss different scattering regimes and provide diffraction maps that describe all essential features of scatterings and observables. The effects are quantified by dynamical scattering simulations and examined by direct comparison to the results of ultrafast electron diffraction experiments on an in situ prepared Ni(100) surface, for which structural dynamics can be well described by a two-temperature model. We also report calculations for graphite surfaces. The theoretical framework provided here allows for further UEC studies of surfaces especially at larger penetration depths and for those of heavy-atom materials. © 2011 American Institute of Physics

Electro-optic sampling for time resolving relativistic ultrafast electron diffraction

International Nuclear Information System (INIS)

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

2009-01-01

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.

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

Directory of Open Access Journals (Sweden)

Erik Kieft

2015-09-01

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

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

KAUST Repository

Aly, Shawkat Mohammede; Parida, Manas R.; Alarousu, Erkki; Mohammed, Omar F.

2014-01-01

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

Electronic and structural response of nanomaterials to ultrafast and ultraintense laser pulses.

Science.gov (United States)

Jiang, Chen-Wei; Zhou, Xiang; Lin, Zhibin; Xie, Rui-Hua; Li, Fu-Li; Allen, Roland E

2014-02-01

The interaction of materials with ultrafast and ultraintense laser pulses is a current frontier of science both experimentally and theoretically. In this review, we briefly discuss some recent theoretical studies by the present authors with our method of semiclassical electron-radiation-ion dynamics (SERID). In particular, Zhou et al. and Jiang et al. respectively, determined the optimal duration and optimal timing for a series of femtosecond scale laser pulses to excite a specific vibrational mode in a general chemical system. A set of such modes can be used as a "fingerprint" for characterizing a particular molecule or a complex in a solid. One can therefore envision many applications, ranging from fundamental studies to detection of chemical or biological agents. Allen et al. proved that dimers are preferentially emitted during photofragmentation of C60 under an ultrafast and ultraintense laser pulse. For interactions between laser pulses and semiconductors, e.g., GaAs, Si and InSb, besides experimentally accessible optical properties--epsilon(omega) and chi(2)-Allen et al. offered many other indicators to confirm the nonthermal nature of structural changes driven by electronic excitations and occurring during the first few hundred femtoseconds. Lin et al. found that, after the application of a femtosecond laser pulse, excited electrons in materials automatically equilibrate to a Fermi-Dirac distribution within roughly 100 fs, solely because of their coupling to the nuclear motion, even though the resulting electronic temperature is one to two orders of magnitude higher than the kinetic temperature defined by the nuclear motion.

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

Directory of Open Access Journals (Sweden)

Colwyn Gulliford

2016-09-01

Full Text Available We present the results of multiobjective genetic algorithm optimizations of a single-shot ultrafast electron diffraction beam line utilizing a 225 kV dc gun with a novel cryocooled photocathode system and buncher cavity. Optimizations of the transverse projected emittance as a function of bunch charge are presented and discussed in terms of the scaling laws derived in the charge saturation limit. Additionally, optimization of the transverse coherence length as a function of final rms bunch length at the sample location have been performed for three different sample radii: 50, 100, and 200  μm, for two final bunch charges: 10^{5} electrons (16 fC and 10^{6} electrons (160 fC. Example optimal solutions are analyzed, and the effects of disordered induced heating estimated. In particular, a relative coherence length of L_{c,x}/σ_{x}=0.27  nm/μm was obtained for a final bunch charge of 10^{5} electrons and final bunch length of σ_{t}≈100  fs. For a final charge of 10^{6} electrons the cryogun produces L_{c,x}/σ_{x}≈0.1  nm/μm for σ_{t}≈100–200  fs and σ_{x}≥50  μm. These results demonstrate the viability of using genetic algorithms in the design and operation of ultrafast electron diffraction beam lines.

Picosecond phase-velocity dispersion of hypersonic phonons imaged with ultrafast electron microscopy

International Nuclear Information System (INIS)

Cremons, Daniel R.; Du, Daniel X.; Flannigan, David J.

2017-01-01

We describe the direct imaging—with four-dimensional ultrafast electron microscopy—of the emergence, evolution, dispersion, and decay of photoexcited, hypersonic coherent acoustic phonons in nanoscale germanium wedges. Coherent strain waves generated via ultrafast in situ photoexcitation were imaged propagating with initial phase velocities of up to 35 km/s across discrete micrometer-scale crystal regions. We then observe that, while each wave front travels at a constant velocity, the entire wave train evolves with a time-varying phase-velocity dispersion, displaying a single-exponential decay to the longitudinal speed of sound (5 km/s) and with a mean lifetime of 280 ps. We also find that the wave trains propagate along a single in-plane direction oriented parallel to striations introduced during specimen preparation, independent of crystallographic direction. Elastic-plate modeling indicates the dynamics arise from excitation of a single, symmetric (dilatational) guided acoustic mode. Further, by precisely determining the experiment time-zero position with a plasma-lensing method, we find that wave-front emergence occurs approximately 100 ps after femtosecond photoexcitation, which matches well with Auger recombination times in germanium. We conclude by discussing the similarities between the imaged hypersonic strain-wave dynamics and electron/hole plasma-wave dynamics in strongly photoexcited semiconductors.

Picosecond phase-velocity dispersion of hypersonic phonons imaged with ultrafast electron microscopy

Science.gov (United States)

Cremons, Daniel R.; Du, Daniel X.; Flannigan, David J.

2017-12-01

Here, we describe the direct imaging—with four-dimensional ultrafast electron microscopy—of the emergence, evolution, dispersion, and decay of photoexcited, hypersonic coherent acoustic phonons in nanoscale germanium wedges. Coherent strain waves generated via ultrafast in situ photoexcitation were imaged propagating with initial phase velocities of up to 35 km/s across discrete micrometer-scale crystal regions. We observe that, while each wave front travels at a constant velocity, the entire wave train evolves with a time-varying phase-velocity dispersion, displaying a single-exponential decay to the longitudinal speed of sound (5 km/s) and with a mean lifetime of 280 ps. We also find that the wave trains propagate along a single in-plane direction oriented parallel to striations introduced during specimen preparation, independent of crystallographic direction. Elastic-plate modeling indicates the dynamics arise from excitation of a single, symmetric (dilatational) guided acoustic mode. Further, by precisely determining the experiment time-zero position with a plasma-lensing method, we find that wave-front emergence occurs approximately 100 ps after femtosecond photoexcitation, which matches well with Auger recombination times in germanium. We conclude by discussing the similarities between the imaged hypersonic strain-wave dynamics and electron/hole plasma-wave dynamics in strongly photoexcited semiconductors.

Theoretical Study of Ultrafast Electron Injection into a Dye/TiO2 System in Dye-Sensitized Solar Cells

Science.gov (United States)

Lin, Chundan; Xia, Qide; Li, Kuan; Li, Juan; Yang, Zhenqing

2018-06-01

The ultrafast injection of excited electrons in dye/TiO2 system plays a critical role, which determines the device's efficiency in large part. In this work, we studied the geometrical structures and electronic properties of a dye/TiO2 composite system for dye-sensitized solar cells (DSSCs) by using density functional theory, and we analyzed the mechanism of ultrafast electron injection with emphasis on the power conversion efficiency. The results show that the dye SPL103/TiO2 (101) surface is more stable than dye SPL101. The electron injection driving force of SPL103/TiO2 (101) is 3.55 times that of SPL101, indicating that SPL103/TiO2 (101) has a strong ability to transfer electrons. SPL103 and SPL101/TiO2 (101) both have fast electron transfer processes, and especially the electron injection time of SPL103/TiO2 (101) is only 1.875 fs. The results of this work are expected to provide a new understanding of the mechanism of electron injection in dyes/TiO2 systems for use in highly effective DSSCs.

Distinctive Spectral Features of Exciton and Excimer States in the Ultrafast Electronic Deactivation of the Adenine Dinucleotide

Science.gov (United States)

Stuhldreier, Mayra C.; Röttger, Katharina; Temps, Friedrich

We report the observation by transient absorption spectroscopy of distinctive spectro-temporal signatures of delocalized exciton versus relaxed, weakly bound excimer states in the ultrafast electronic deactivation after UV photoexcitation of the adenine dinucleotide.

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

International Nuclear Information System (INIS)

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

2006-01-01

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

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

International Nuclear Information System (INIS)

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

2013-01-01

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

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

International Nuclear Information System (INIS)

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

2008-01-01

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 (τ 1 ) is the measure of the fastest ET rate (τ 1 =τ 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 τ 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 ∼0.4 for aromatic amines and ∼0.8 for aliphatic amines. Beyond these dilutions in the two respective cases of the amine systems, the τ 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 (π-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 π-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 ultrafast ET reaction. In contrary, the

Ultra-fast framing camera tube

Science.gov (United States)

Kalibjian, Ralph

1981-01-01

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

Ultrafast THz Saturable Absorption in Doped Semiconductors

DEFF Research Database (Denmark)

Turchinovich, Dmitry; Hoffmann, Matthias C.

2011-01-01

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

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

KAUST Repository

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

2015-01-01

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

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

KAUST Repository

Aly, Shawkat Mohammede

2015-10-29

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

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

Energy Technology Data Exchange (ETDEWEB)

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

2016-01-25

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

Static and Dynamic Electron Microscopy Investigations at the Atomic and Ultrafast Scales

Science.gov (United States)

Suri, Pranav Kumar

Advancements in the electron microscopy capabilities - aberration-corrected imaging, monochromatic spectroscopy, direct-electron detectors - have enabled routine visualization of atomic-scale processes with millisecond temporal resolutions in this decade. This, combined with progress in the transmission electron microscopy (TEM) specimen holder technology and nanofabrication techniques, allows comprehensive experiments on a wide range of materials in various phases via in situ methods. The development of ultrafast (sub-nanosecond) time-resolved TEM with ultrafast electron microscopy (UEM) has further pushed the envelope of in situ TEM to sub-nanosecond temporal resolution while maintaining sub-nanometer spatial resolution. A plethora of materials phenomena - including electron-phonon coupling, phonon transport, first-order phase transitions, bond rotation, plasmon dynamics, melting, and dopant atoms arrangement - are not yet clearly understood and could be benefitted with the current in situ TEM capabilities having atomic-level and ultrafast precision. Better understanding of these phenomena and intrinsic material dynamics (e.g. how phonons propagate in a material, what time-scales are involved in a first-order phase transition, how fast a material melts, where dopant atoms sit in a crystal) in new-generation and technologically important materials (e.g. two-dimensional layered materials, semiconductor and magnetic devices, rare-earth-element-free permanent magnets, unconventional superconductors) could bring a paradigm shift in their electronic, structural, magnetic, thermal and optical applications. Present research efforts, employing cutting-edge static and dynamic in situ electron microscopy resources at the University of Minnesota, are directed towards understanding the atomic-scale crystallographic structural transition and phonon transport in an iron-pnictide parent compound LaFeAsO, studying the mechanical stability of fast moving hard-drive heads in heat

Novel radio-frequency gun structures for ultrafast relativistic electron diffraction.

Science.gov (United States)

Musumeci, P; Faillace, L; Fukasawa, A; Moody, J T; O'Shea, B; Rosenzweig, J B; Scoby, C M

2009-08-01

Radio-frequency (RF) photoinjector-based relativistic ultrafast electron diffraction (UED) is a promising new technique that has the potential to probe structural changes at the atomic scale with sub-100 fs temporal resolution in a single shot. We analyze the limitations on the temporal and spatial resolution of this technique considering the operating parameters of a standard 1.6 cell RF gun (which is the RF photoinjector used for the first experimental tests of relativistic UED at Stanford Linear Accelerator Center; University of California, Los Angeles; Brookhaven National Laboratory), and study the possibility of employing novel RF structures to circumvent some of these limits.

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

OpenAIRE

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

2014-01-01

We present feasibility study of an accelerator-based ultrafast transmission electron microscope (u-TEM) capable of producing a full field image in a single-shot with simultaneous picosecond temporal resolution and nanometer spatial resolution. We study key physics related to performance of u-TEMs, and discuss major challenges as well as possible solutions for practical realization of u-TEMs. The feasibility of u-TEMs is confirmed through simulations using realistic electron beam parameters. W...

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

Energy Technology Data Exchange (ETDEWEB)

Slavov, Chavdar Lyubomirov

2009-07-09

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

A new coupling mechanism between two graphene electron waveguides for ultrafast switching

Science.gov (United States)

Huang, Wei; Liang, Shi-Jun; Kyoseva, Elica; Ang, Lay Kee

2018-03-01

In this paper, we report a novel coupling between two graphene electron waveguides, in analogy the optical waveguides. The design is based on the coherent quantum mechanical tunneling of Rabi oscillation between the two graphene electron waveguides. Based on this coupling mechanism, we propose that it can be used as an ultrafast electronic switching device. Based on a modified coupled mode theory, we construct a theoretical model to analyze the device characteristics, and predict that the switching speed is faster than 1 ps and the on-off ratio exceeds 106. Due to the long mean free path of electrons in graphene at room temperature, the proposed design avoids the limitation of low temperature operation required in the traditional design by using semiconductor quantum-well structure. The layout of our design is similar to that of a standard complementary metal-oxide-semiconductor transistor that should be readily fabricated with current state-of-art nanotechnology.

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

International Nuclear Information System (INIS)

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

2015-01-01

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

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

KAUST Repository

Sun, Jingya; Melnikov, Vasily; Khan, Jafar Iqbal; Mohammed, Omar F.

2015-01-01

, 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

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

KAUST Repository

Alsulami, Qana

2015-06-25

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

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

KAUST Repository

Alsulami, Qana; Aly, Shawkat Mohammede; Goswami, Subhadip; Alarousu, Erkki; Usman, Anwar; Schanze, Kirk S.; Mohammed, Omar F.

2015-01-01

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

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

Energy Technology Data Exchange (ETDEWEB)

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

2012-07-25

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

Imaging nanoscale spatial modulation of a relativistic electron beam with a MeV ultrafast electron microscope

Science.gov (United States)

Lu, Chao; Jiang, Tao; Liu, Shengguang; Wang, Rui; Zhao, Lingrong; Zhu, Pengfei; Liu, Yaqi; Xu, Jun; Yu, Dapeng; Wan, Weishi; Zhu, Yimei; Xiang, Dao; Zhang, Jie

2018-03-01

An accelerator-based MeV ultrafast electron microscope (MUEM) has been proposed as a promising tool to the study structural dynamics at the nanometer spatial scale and the picosecond temporal scale. Here, we report experimental tests of a prototype MUEM where high quality images with nanoscale fine structures were recorded with a pulsed ˜3 MeV picosecond electron beam. The temporal and spatial resolutions of the MUEM operating in the single-shot mode are about 4 ps (FWHM) and 100 nm (FWHM), corresponding to a temporal-spatial resolution of 4 × 10-19 s m, about 2 orders of magnitude higher than that achieved with state-of-the-art single-shot keV UEM. Using this instrument, we offer the demonstration of visualizing the nanoscale periodic spatial modulation of an electron beam, which may be converted into longitudinal density modulation through emittance exchange to enable production of high-power coherent radiation at short wavelengths. Our results mark a great step towards single-shot nanometer-resolution MUEMs and compact intense x-ray sources that may have widespread applications in many areas of science.

Quantum modeling of ultrafast photoinduced charge separation

Science.gov (United States)

Rozzi, Carlo Andrea; Troiani, Filippo; Tavernelli, Ivano

2018-01-01

Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the separation of photogenerated charges is a crucial prerequisite in many applicative contexts, including quantum electronics, photo-electrochemical water splitting, photocatalytic dye degradation, and energy conversion. In particular, photoinduced charge separation is the pivotal step driving the storage of sun light into electrical or chemical energy. If properly mastered, these processes may also allow us to achieve a better command of information storage at the nanoscale, as required for the development of molecular electronics, optical switching, or quantum technologies, amongst others. In this Topical Review we survey recent progress in the understanding of ultrafast charge separation from photoexcited states. We report the state-of-the-art of the observation and theoretical description of charge separation phenomena in the ultrafast regime mainly focusing on molecular- and nano-sized solar energy conversion systems. In particular, we examine different proposed mechanisms driving ultrafast charge dynamics, with particular regard to the role of quantum coherence and electron-nuclear coupling, and link experimental observations to theoretical approaches based either on model Hamiltonians or on first principles simulations.

Charge dynamics in aluminum oxide thin film studied by ultrafast scanning electron microscopy.

Science.gov (United States)

Zani, Maurizio; Sala, Vittorio; Irde, Gabriele; Pietralunga, Silvia Maria; Manzoni, Cristian; Cerullo, Giulio; Lanzani, Guglielmo; Tagliaferri, Alberto

2018-04-01

The excitation dynamics of defects in insulators plays a central role in a variety of fields from Electronics and Photonics to Quantum computing. We report here a time-resolved measurement of electron dynamics in 100 nm film of aluminum oxide on silicon by Ultrafast Scanning Electron Microscopy (USEM). In our pump-probe setup, an UV femtosecond laser excitation pulse and a delayed picosecond electron probe pulse are spatially overlapped on the sample, triggering Secondary Electrons (SE) emission to the detector. The zero of the pump-probe delay and the time resolution were determined by measuring the dynamics of laser-induced SE contrast on silicon. We observed fast dynamics with components ranging from tens of picoseconds to few nanoseconds, that fits within the timescales typical of the UV color center evolution. The surface sensitivity of SE detection gives to the USEM the potential of applying pump-probe investigations to charge dynamics at surfaces and interfaces of current nano-devices. The present work demonstrates this approach on large gap insulator surfaces. Copyright © 2018 Elsevier B.V. All rights reserved.

Intra- and inter-atomic optical transitions of Fe, Co, and Ni ferrocyanides studied using first-principles many-electron calculations

Energy Technology Data Exchange (ETDEWEB)

Watanabe, Shinta, E-mail: s-watanabe@nucl.nagoya-u.ac.jp, E-mail: j-onoe@nucl.nagoya-u.ac.jp; Sawada, Yuki; Nakaya, Masato; Yoshino, Masahito; Nagasaki, Takanori; Onoe, Jun, E-mail: s-watanabe@nucl.nagoya-u.ac.jp, E-mail: j-onoe@nucl.nagoya-u.ac.jp [Department of Materials, Physics and Energy Engineering, Graduated School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8603 (Japan); Kameyama, Tatsuya; Torimoto, Tsukasa [Department of Crystalline Materials Science, Graduated School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8603 (Japan); Inaba, Yusuke; Takahashi, Hideharu; Takeshita, Kenji [Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology, 2-12-1-N1-16 O-okayama, Meguro-ku, Tokyo 152-8550 (Japan)

2016-06-21

We have investigated the electronic structures and optical properties of Fe, Co, and Ni ferrocyanide nanoparticles using first-principles relativistic many-electron calculations. The overall features of the theoretical absorption spectra for Fe, Ni, and Co ferrocyanides calculated using a first-principles many-electron method well reproduced the experimental one. The origins of the experimental absorption spectra were clarified by performing a configuration analysis based on the many-electron wave functions. For Fe ferrocyanide, the experimental absorption peaks originated from not only the charge-transfer transitions from Fe{sup 2+} to Fe{sup 3+} but also the 3d-3d intra-transitions of Fe{sup 3+} ions. In addition, the spin crossover transition of Fe{sup 3+} predicted by the many-electron calculations was about 0.24 eV. For Co ferrocyanide, the experimental absorption peaks were mainly attributed to the 3d-3d intra-transitions of Fe{sup 2+} ions. In contrast to the Fe and Co ferrocyanides, Ni ferrocyanide showed that the absorption peaks originated from the 3d-3d intra-transitions of Ni{sup 3+} ions in a low-energy region, while from both the 3d-3d intra-transitions of Fe{sup 2+} ions and the charge-transfer transitions from Fe{sup 2+} to Ni{sup 3+} in a high-energy region. These results were quite different from those of density-functional theory (DFT) calculations. The discrepancy between the results of DFT calculations and those of many-electron calculations suggested that the intra- and inter-atomic transitions of transition metal ions are significantly affected by the many-body effects of strongly correlated 3d electrons.

Perspective: Ultrafast magnetism and THz spintronics

Energy Technology Data Exchange (ETDEWEB)

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

2016-10-14

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

Perspective: Ultrafast magnetism and THz spintronics

International Nuclear Information System (INIS)

Walowski, Jakob; Münzenberg, Markus

2016-01-01

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

Ultrafast Processes in Atoms and Molecules: Integrated treatment of electronic and nuclear motion in ultrashort XUV pulses

Energy Technology Data Exchange (ETDEWEB)

McCurdy, C. William [Univ. of California, Davis, CA (United States). Dept. of

2017-12-14

This project made use of Multiconfiguration Time-Dependent Hartree-Fock method developed earlier in the McCurdy group in a series of novel applications of the method to ultrafast spectroscopic processes. MCTDHF treats the dynamics of a molecule or atom under the influence of an external field in manner that has all electrons active. That property distinguishes this method from the more popular (and much less computationally demanding) approaches for treating the electron dynamics of atoms and molecules in fields, such as the time-dependent “Configuration Interaction Singles” approximation or approaches that limit the treatment to either one or two-electron models.

Sub-nanometre resolution of atomic motion during electronic excitation in phase-change materials.

Science.gov (United States)

Mitrofanov, Kirill V; Fons, Paul; Makino, Kotaro; Terashima, Ryo; Shimada, Toru; Kolobov, Alexander V; Tominaga, Junji; Bragaglia, Valeria; Giussani, Alessandro; Calarco, Raffaella; Riechert, Henning; Sato, Takahiro; Katayama, Tetsuo; Ogawa, Kanade; Togashi, Tadashi; Yabashi, Makina; Wall, Simon; Brewe, Dale; Hase, Muneaki

2016-02-12

Phase-change materials based on Ge-Sb-Te alloys are widely used in industrial applications such as nonvolatile memories, but reaction pathways for crystalline-to-amorphous phase-change on picosecond timescales remain unknown. Femtosecond laser excitation and an ultrashort x-ray probe is used to show the temporal separation of electronic and thermal effects in a long-lived (>100 ps) transient metastable state of Ge2Sb2Te5 with muted interatomic interaction induced by a weakening of resonant bonding. Due to a specific electronic state, the lattice undergoes a reversible nondestructive modification over a nanoscale region, remaining cold for 4 ps. An independent time-resolved x-ray absorption fine structure experiment confirms the existence of an intermediate state with disordered bonds. This newly unveiled effect allows the utilization of non-thermal ultra-fast pathways enabling artificial manipulation of the switching process, ultimately leading to a redefined speed limit, and improved energy efficiency and reliability of phase-change memory technologies.

Interatomic spacing distribution in multicomponent alloys

International Nuclear Information System (INIS)

Toda-Caraballo, I.; Wróbel, J.S.; Dudarev, S.L.; Nguyen-Manh, D.; Rivera-Díaz-del-Castillo, P.E.J.

2015-01-01

A methodology to compute the distribution of interatomic distances in highly concentrated multicomponent alloys is proposed. By using the unit cell parameter and bulk modulus of the elements involved, the method accurately describes the distortion in the lattice produced by the interaction of the different atomic species. To prove this, density functional theory calculations have been used to provide the description of the lattice in a monophasic BCC MoNbTaVW high entropy alloy and its five sub-quaternary systems at different temperatures. Short-range order is also well described by the new methodology, where the mean error in the predicted atomic coordinates in comparison with the atomistic simulations is in the order of 1–2 pm over all the compositions and temperatures considered. The new method can be applied to tailor solid solution hardening, highly dependent on the distribution of interatomic distances, and guide the design of new high entropy alloys with enhanced properties

Ultrafast electron-optical phonon scattering and quasiparticle lifetime in CVD-grown graphene.

Science.gov (United States)

Shang, Jingzhi; Yu, Ting; Lin, Jianyi; Gurzadyan, Gagik G

2011-04-26

Ultrafast quasiparticle dynamics in graphene grown by chemical vapor deposition (CVD) has been studied by UV pump/white-light probe spectroscopy. Transient differential transmission spectra of monolayer graphene are observed in the visible probe range (400-650 nm). Kinetics of the quasiparticle (i.e., low-energy single-particle excitation with renormalized energy due to electron-electron Coulomb, electron-optical phonon (e-op), and optical phonon-acoustic phonon (op-ap) interactions) was monitored with 50 fs resolution. Extending the probe range to near-infrared, we find the evolution of quasiparticle relaxation channels from monoexponential e-op scattering to double exponential decay due to e-op and op-ap scattering. Moreover, quasiparticle lifetimes of mono- and randomly stacked graphene films are obtained for the probe photon energies continuously from 1.9 to 2.3 eV. Dependence of quasiparticle decay rate on the probe energy is linear for 10-layer stacked graphene films. This is due to the dominant e-op intervalley scattering and the linear density of states in the probed electronic band. A dimensionless coupling constant W is derived, which characterizes the scattering strength of quasiparticles by lattice points in graphene.

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

KAUST Repository

Sun, Jingya

2015-09-14

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

Interatomic methods for the dispersion energy derived from the adiabatic connection fluctuation-dissipation theorem

Science.gov (United States)

Tkatchenko, Alexandre; Ambrosetti, Alberto; DiStasio, Robert A.

2013-02-01

Interatomic pairwise methods are currently among the most popular and accurate ways to include dispersion energy in density functional theory calculations. However, when applied to more than two atoms, these methods are still frequently perceived to be based on ad hoc assumptions, rather than a rigorous derivation from quantum mechanics. Starting from the adiabatic connection fluctuation-dissipation (ACFD) theorem, an exact expression for the electronic exchange-correlation energy, we demonstrate that the pairwise interatomic dispersion energy for an arbitrary collection of isotropic polarizable dipoles emerges from the second-order expansion of the ACFD formula upon invoking the random-phase approximation (RPA) or the full-potential approximation. Moreover, for a system of quantum harmonic oscillators coupled through a dipole-dipole potential, we prove the equivalence between the full interaction energy obtained from the Hamiltonian diagonalization and the ACFD-RPA correlation energy. This property makes the Hamiltonian diagonalization an efficient method for the calculation of the many-body dispersion energy. In addition, we show that the switching function used to damp the dispersion interaction at short distances arises from a short-range screened Coulomb potential, whose role is to account for the spatial spread of the individual atomic dipole moments. By using the ACFD formula, we gain a deeper understanding of the approximations made in the interatomic pairwise approaches, providing a powerful formalism for further development of accurate and efficient methods for the calculation of the dispersion energy.

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI.

Science.gov (United States)

Gutt, C; Sant, T; Ksenzov, D; Capotondi, F; Pedersoli, E; Raimondi, L; Nikolov, I P; Kiskinova, M; Jaiswal, S; Jakob, G; Kläui, M; Zabel, H; Pietsch, U

2017-09-01

We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M 2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q -resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Q z , we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Influence of cathode geometry on electron dynamics in an ultrafast electron microscope

Directory of Open Access Journals (Sweden)

Shaozheng Ji

2017-09-01

Full Text Available Efforts to understand matter at ever-increasing spatial and temporal resolutions have led to the development of instruments such as the ultrafast transmission electron microscope (UEM that can capture transient processes with combined nanometer and picosecond resolutions. However, analysis by UEM is often associated with extended acquisition times, mainly due to the limitations of the electron gun. Improvements are hampered by tradeoffs in realizing combinations of the conflicting objectives for source size, emittance, and energy and temporal dispersion. Fundamentally, the performance of the gun is a function of the cathode material, the gun and cathode geometry, and the local fields. Especially shank emission from a truncated tip cathode results in severe broadening effects and therefore such electrons must be filtered by applying a Wehnelt bias. Here we study the influence of the cathode geometry and the Wehnelt bias on the performance of a photoelectron gun in a thermionic configuration. We combine experimental analysis with finite element simulations tracing the paths of individual photoelectrons in the relevant 3D geometry. Specifically, we compare the performance of guard ring cathodes with no shank emission to conventional truncated tip geometries. We find that a guard ring cathode allows operation at minimum Wehnelt bias and improve the temporal resolution under realistic operation conditions in an UEM. At low bias, the Wehnelt exhibits stronger focus for guard ring than truncated tip cathodes. The increase in temporal spread with bias is mainly a result from a decrease in the accelerating field near the cathode surface. Furthermore, simulations reveal that the temporal dispersion is also influenced by the intrinsic angular distribution in the photoemission process and the initial energy spread. However, a smaller emission spot on the cathode is not a dominant driver for enhancing time resolution. Space charge induced temporal broadening

Influence of cathode geometry on electron dynamics in an ultrafast electron microscope.

Science.gov (United States)

Ji, Shaozheng; Piazza, Luca; Cao, Gaolong; Park, Sang Tae; Reed, Bryan W; Masiel, Daniel J; Weissenrieder, Jonas

2017-09-01

Efforts to understand matter at ever-increasing spatial and temporal resolutions have led to the development of instruments such as the ultrafast transmission electron microscope (UEM) that can capture transient processes with combined nanometer and picosecond resolutions. However, analysis by UEM is often associated with extended acquisition times, mainly due to the limitations of the electron gun. Improvements are hampered by tradeoffs in realizing combinations of the conflicting objectives for source size, emittance, and energy and temporal dispersion. Fundamentally, the performance of the gun is a function of the cathode material, the gun and cathode geometry, and the local fields. Especially shank emission from a truncated tip cathode results in severe broadening effects and therefore such electrons must be filtered by applying a Wehnelt bias. Here we study the influence of the cathode geometry and the Wehnelt bias on the performance of a photoelectron gun in a thermionic configuration. We combine experimental analysis with finite element simulations tracing the paths of individual photoelectrons in the relevant 3D geometry. Specifically, we compare the performance of guard ring cathodes with no shank emission to conventional truncated tip geometries. We find that a guard ring cathode allows operation at minimum Wehnelt bias and improve the temporal resolution under realistic operation conditions in an UEM. At low bias, the Wehnelt exhibits stronger focus for guard ring than truncated tip cathodes. The increase in temporal spread with bias is mainly a result from a decrease in the accelerating field near the cathode surface. Furthermore, simulations reveal that the temporal dispersion is also influenced by the intrinsic angular distribution in the photoemission process and the initial energy spread. However, a smaller emission spot on the cathode is not a dominant driver for enhancing time resolution. Space charge induced temporal broadening shows a close to

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

KAUST Repository

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

2016-01-01

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

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

KAUST Repository

Sun, Jingya

2016-02-25

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

Ultrafast spectroscopy of biological photoreceptors

NARCIS (Netherlands)

Kennis, J.T.M.; Groot, M.L.

2007-01-01

We review recent new insights on reaction dynamics of photoreceptors proteins gained from ultrafast spectroscopy. In Blue Light sensing Using FAD (BLUF) domains, a hydrogen-bond rearrangement around the flavin chromophore proceeds through a radical-pair mechanism, by which light-induced electron and

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

International Nuclear Information System (INIS)

Deleuze, Michael S; Hajgato, Balazs; Morini, Filippo

2009-01-01

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

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI

Directory of Open Access Journals (Sweden)

C. Gutt

2017-09-01

Full Text Available We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q-resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Qz, we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Ultrafast exciton decay in PbS quantum dots through simultaneous electron and hole recombination with a surface-localized ion pair

Energy Technology Data Exchange (ETDEWEB)

Edme, Kedy; Bettis Homan, Stephanie; Nepomnyashchii, Alexander B.; Weiss, Emily A., E-mail: e-weiss@northwestern.edu

2016-06-01

Highlights: • We synthesize complexes of PbS quantum dots (QDs) and tetracyanoquinodimethane (TCNQ). Each PbS QD spontaneously reduces up to 17 TCNQ molecules. • The photoluminescence of the PbS QDs is quenched in the presence of the reduced TCNQ species through ultrafast non-radiative, simultaneous decay of the electron and hole. • We assign this decay to a four-carrier, concerted charge recombination mechanism with the surface localized sulfur–TCNQ{sup x−} ion pair. - Abstract: This paper describes the ultrafast decay of the band-edge exciton in PbS quantum dots (QDs) through simultaneous recombination of the excitonic hole and electron with the surface localized ion pair formed upon adsorption of tetracyanoquinodimethane (TCNQ). Each PbS QD (R = 1.8 nm) spontaneously reduces up to 17 TCNQ molecules upon adsorption of the TCNQ molecule to a sulfur on the QD surface. The photoluminescence of the PbS QDs is quenched in the presence of the reduced TCNQ species through ultrafast (⩽15-ps) non-radiative decay of the exciton; the rate constant for the decay process increases approximately linearly with the number of adsorbed, reduced TCNQ molecules. Near-infrared and mid-infrared transient absorption show that this decay occurs through simultaneous transfer of the excitonic electron and hole, and is assigned to a four-carrier, concerted charge recombination mechanism based on the observations that (i) the PL of the QDs recovers when spontaneously reduced TCNQ{sup 1−} desorbs from the QD surface upon addition of salt, and (ii) the PL of the QDs is preserved when another spontaneous oxidant, ferrocinium, which cannot participate in charge transfer in its reduced state, is substituted for TCNQ.

The role of tungsten in the change of interatomic bond in Nb-W alloy

International Nuclear Information System (INIS)

Arkharov, V.I.; Samojlenko, Z.A.; Darovskikh, E.G.

1982-01-01

To study the chemical inhomogeneity and the peculiarities in electronic structure of solid solutions in fracture region, the X-ray spectral studies of niobium-tungsten alloys with 0.5; 1.0; 12.0; 13.6; 23.g mass % W have been carried out. The W concentration changes on the fracture and the difference in the electron energy distribution in the 4d-band in comparison between the fracture and mocrosection are determined. The niobium doping with tungsten is shown to be accompanied by the increase in the fraction of locally bound electrons as compared to the collectivized one. Alloys with 12-13% W are the most homogeneous in composition and electrons energy state. This state is characterized by features the increased number of electrons with noncompensated spins in intercrystalline boundaries as compared to a crystallite thickness. These alloys have homogeneous properties in sample microvolumes and large interatomic binding force

OSA Trends in Optics and Photonics Series. Volume 13: Ultrafast Electronics and Optoelectronics

Science.gov (United States)

1997-01-01

tomography. Many materials such as plastics, cardboard, wood and rubber have good transparency in the terahertz frequency range. Hence, this new...Ultrafast processes in semiconductors. Introduction Nonlinear Bragg reflector ( NBR ) consists of periodically distributed optical nonlinearity coexisting...with multiple reflection and group-delay dispersion. Recent theoretical analyses showed the potential of NBR in ultrafast optoelectronics such as all

On macromolecular refinement at subatomic resolution with interatomic scatterers

Energy Technology Data Exchange (ETDEWEB)

Afonine, Pavel V., E-mail: pafonine@lbl.gov; Grosse-Kunstleve, Ralf W.; Adams, Paul D. [Lawrence Berkeley National Laboratory, One Cyclotron Road, BLDG 64R0121, Berkeley, CA 94720 (United States); Lunin, Vladimir Y. [Institute of Mathematical Problems of Biology, Russian Academy of Sciences, Pushchino 142290 (Russian Federation); Urzhumtsev, Alexandre [IGMBC, 1 Rue L. Fries, 67404 Illkirch and IBMC, 15 Rue R. Descartes, 67084 Strasbourg (France); Faculty of Sciences, Nancy University, 54506 Vandoeuvre-lès-Nancy (France); Lawrence Berkeley National Laboratory, One Cyclotron Road, BLDG 64R0121, Berkeley, CA 94720 (United States)

2007-11-01

Modelling deformation electron density using interatomic scatters is simpler than multipolar methods, produces comparable results at subatomic resolution and can easily be applied to macromolecules. A study of the accurate electron-density distribution in molecular crystals at subatomic resolution (better than ∼1.0 Å) requires more detailed models than those based on independent spherical atoms. A tool that is conventionally used in small-molecule crystallography is the multipolar model. Even at upper resolution limits of 0.8–1.0 Å, the number of experimental data is insufficient for full multipolar model refinement. As an alternative, a simpler model composed of conventional independent spherical atoms augmented by additional scatterers to model bonding effects has been proposed. Refinement of these mixed models for several benchmark data sets gave results that were comparable in quality with the results of multipolar refinement and superior to those for conventional models. Applications to several data sets of both small molecules and macromolecules are shown. These refinements were performed using the general-purpose macromolecular refinement module phenix.refine of the PHENIX package.

Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

Science.gov (United States)

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.

Handbook of interatomic potentials

International Nuclear Information System (INIS)

Stoneham, A.M.; Taylor, R.

1981-08-01

This Handbook collects together interatomic potentials for a large number of metals. Most of the potentials describe the interactions of host metal atoms with each other, and these, in some cases, may be applied to solid and liquid metals. In addition, there are potentials (a) for a metallic impurity alloyed with the host, (b) for a small number of chemical impurities in the metal (eg H, O), and (c) for rare-gas impurities, notably He. The Handbook is intended to be a convenient source of potentials for bulk, surface and defect calculations, both static and dynamic. (author)

Ultrafast X-Ray Spectroscopy of Conical Intersections

Science.gov (United States)

Neville, Simon P.; Chergui, Majed; Stolow, Albert; Schuurman, Michael S.

2018-06-01

Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S2(π π*) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections.

Ultrafast chemical interface scattering as an additional decay channel for nascent nonthermal electrons in small metal nanoparticles.

Science.gov (United States)

Bauer, Christophe; Abid, Jean-Pierre; Fermin, David; Girault, Hubert H

2004-05-15

The use of 4.2 nm gold nanoparticles wrapped in an adsorbates shell and embedded in a TiO2 metal oxide matrix gives the opportunity to investigate ultrafast electron-electron scattering dynamics in combination with electronic surface phenomena via the surface plasmon lifetimes. These gold nanoparticles (NPs) exhibit a large nonclassical broadening of the surface plasmon band, which is attributed to a chemical interface damping. The acceleration of the loss of surface plasmon phase coherence indicates that the energy and the momentum of the collective electrons can be dissipated into electronic affinity levels of adsorbates. As a result of the preparation process, gold NPs are wrapped in a shell of sulfate compounds that gives rise to a large density of interfacial molecules confined between Au and TiO2, as revealed by Fourier-transform-infrared spectroscopy. A detailed analysis of the transient absorption spectra obtained by broadband femtosecond transient absorption spectroscopy allows separating electron-electron and electron-phonon interaction. Internal thermalization times (electron-electron scattering) are determined by probing the decay of nascent nonthermal electrons (NNEs) and the build-up of the Fermi-Dirac electron distribution, giving time constants of 540 to 760 fs at 0.42 and 0.34 eV from the Fermi level, respectively. Comparison with literature data reveals that lifetimes of NNEs measured for these small gold NPs are more than four times longer than for silver NPs with similar sizes. The surprisingly long internal thermalization time is attributed to an additional decay mechanism (besides the classical e-e scattering) for the energy loss of NNEs, identified as the ultrafast chemical interface scattering process. NNEs experience an inelastic resonant scattering process into unoccupied electronic states of adsorbates, that directly act as an efficient heat bath, via the excitation of molecular vibrational modes. The two-temperature model is no longer

Photoelectron diffraction from single oriented molecules: Towards ultrafast structure determination of molecules using x-ray free-electron lasers

Science.gov (United States)

Kazama, Misato; Fujikawa, Takashi; Kishimoto, Naoki; Mizuno, Tomoya; Adachi, Jun-ichi; Yagishita, Akira

2013-06-01

We provide a molecular structure determination method, based on multiple-scattering x-ray photoelectron diffraction (XPD) calculations. This method is applied to our XPD data on several molecules having different equilibrium geometries. Then it is confirmed that, by our method, bond lengths and bond angles can be determined with a resolution of less than 0.1 Å and 10∘, respectively. Differently from any other scenario of ultrafast structure determination, we measure the two- or three-dimensional XPD of aligned or oriented molecules in the energy range from 100 to 200 eV with a 4π detection velocity map imaging spectrometer. Thanks to the intense and ultrashort pulse properties of x-ray free-electron lasers, our approach exhibits the most probable method for obtaining ultrafast real-time structural information on small to medium-sized molecules consisting of light elements, i.e., a “molecular movie.”

A W−Ne interatomic potential for simulation of neon implantation in tungsten

Energy Technology Data Exchange (ETDEWEB)

Backman, Marie; Juslin, Niklas; Huang, Guiyang [Department of Nuclear Engineering, University of Tennessee, Knoxville, TN 37996-2300 (United States); Wirth, Brian D., E-mail: bdwirth@utk.edu [Department of Nuclear Engineering, University of Tennessee, Knoxville, TN 37996-2300 (United States); P.O. Box 2008, MS-6003, Oak Ridge National Laboratory, Oak Ridge, TN 37831 (United States)

2016-08-15

An interatomic pair potential for W−Ne is developed for atomistic molecular dynamics simulations of neon implantation in tungsten. The new potential predicts point defect energies and binding energies of small clusters that are in good agreement with electronic structure calculations. Molecular dynamics simulations of small neon clusters in tungsten show that trap mutation, in which an interstitial neon cluster displaces a tungsten atom from its lattice site, occurs for clusters of three or more neon atoms. However, near a free surface, trap mutation can occur at smaller sizes, including even a single neon interstitial in close proximity to a (100) or (110) surface.

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

Science.gov (United States)

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

2010-08-01

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

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

Energy Technology Data Exchange (ETDEWEB)

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

2016-11-15

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

Evidence of interatomic Coulombic decay in ArKr after Ar 2p Auger decay

International Nuclear Information System (INIS)

Morishita, Y; Saito, N; Suzuki, I H; Fukuzawa, H; Liu, X-J; Sakai, K; Pruemper, G; Ueda, K; Iwayama, H; Nagaya, K; Yao, M; Kreidi, K; Schoeffler, M; Jahnke, T; Schoessler, S; Doerner, R; Weber, T; Harries, J; Tamenori, Y

2008-01-01

We have identified interatomic Coulombic decay (ICD) processes in the ArKr dimer following Ar 2p Auger decay, using momentum-resolved electron-ion-ion coincidence spectroscopy and simultaneously determining the kinetic energy of the ICD electron and the KER between Ar 2+ and Kr + . We find that the spin-conserved ICD processes in which Ar 2+ (3p -3 3d) 1 P and 3 P decay to Ar 2+ (3p -2 ) 1 D and 3 P, respectively, ionizing the Kr atom, are significantly stronger than the spin-flip ICD processes in which Ar 2+ (3p -3 3d) 1 P and 3 P decay to Ar 2+ (3p -2 ) 3 P and 1 D, respectively

Ultrafast quantum control of ionization dynamics in krypton.

Science.gov (United States)

Hütten, Konrad; Mittermair, Michael; Stock, Sebastian O; Beerwerth, Randolf; Shirvanyan, Vahe; Riemensberger, Johann; Duensing, Andreas; Heider, Rupert; Wagner, Martin S; Guggenmos, Alexander; Fritzsche, Stephan; Kabachnik, Nikolay M; Kienberger, Reinhard; Bernhardt, Birgitta

2018-02-19

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.

Interatomic potentials and the simulation of lattice defects in metals

International Nuclear Information System (INIS)

Heugten, W.F.W.M. van.

1979-01-01

The computer simulation technique is applied to investigate the properties of point defects and line defects in metals. For that purpose crystallites are constructed in which these defects are simulated. In the case of line defects (dislocations) the initial positions of the atoms, surrounding the dislocations, are determined using the elastic theory of anisotropic media. Hereafter the atoms in such crystallites are allowed to relax to there minimum potential energy positions under the influence of the interatomic forces. These forces are derived from interatomic interaction potentials. These potentials are together with the boundary conditions of the simulated crystallite the main input data in these computer simulation models. The metals considered include molybdenum, tungsten and tantalum. (Auth.)

Ultrafast photoelectron spectroscopy of small molecule organic films

Science.gov (United States)

Read, Kendall Laine

As research in the field of ultrafast optics has produced shorter and shorter pulses, at an ever-widening range of frequencies, ultrafast spectroscopy has grown correspondingly. In particular, ultrafast photoelectron spectroscopy allows direct observation of electrons in transient or excited states, regardless of the eventual relaxation mechanisms. High-harmonic conversion of 800nm, femtosecond, Ti:sapphire laser pulses allows excite/probe spectroscopy down into atomic core level states. To this end, an ultrafast, X-UV photoelectron spectroscopic system is described, including design considerations for the high-harmonic generation line, the time of flight detector, and the subsequent data collection electronics. Using a similar experimental setup, I have performed several ultrafast, photoelectron excited state decay studies at the IBM, T. J. Watson Research Center. All of the observed materials were electroluminescent thin film organics, which have applications as the emitter layer in organic light emitting devices. The specific materials discussed are: Alq, BAlq, DPVBi, and Alq doped with DCM or DMQA. Alq:DCM is also known to lase at low photoexcitation thresholds. A detailed understanding of the involved relaxation mechanisms is beneficial to both applications. Using 3.14 eV excite, and 26.7 eV probe, 90 fs laser pulses, we have observed the lowest unoccupied molecular orbital (LUMO) decay rate over the first 200 picoseconds. During this time, diffusion is insignificant, and all dynamics occur in the absence of electron transport. With excitation intensities in the range of 100μJ/cm2, we have modeled the Alq, BAlq, and DPVBi decays via bimolecular singlet-singlet annihilation. At similar excitations, we have modeled the Alq:DCM decay via Förster transfer, stimulated emission, and excimeric formation. Furthermore, the Alq:DCM occupied to unoccupied molecular orbital energy gap was seen to shrink as a function of excite-to-probe delay, in accordance with the

Ultrafast electron-lattice coupling dynamics in VO2 and V2O3 thin films

Science.gov (United States)

Abreu, Elsa; Gilbert Corder, Stephanie N.; Yun, Sun Jin; Wang, Siming; Ramírez, Juan Gabriel; West, Kevin; Zhang, Jingdi; Kittiwatanakul, Salinporn; Schuller, Ivan K.; Lu, Jiwei; Wolf, Stuart A.; Kim, Hyun-Tak; Liu, Mengkun; Averitt, Richard D.

2017-09-01

Ultrafast optical pump-optical probe and optical pump-terahertz probe spectroscopy were performed on vanadium dioxide (VO2) and vanadium sesquioxide (V2O3 ) thin films over a wide temperature range. A comparison of the experimental data from these two different techniques and two different vanadium oxides, in particular a comparison of the spectral weight oscillations generated by the photoinduced longitudinal acoustic modulation, reveals the strong electron-phonon coupling that exists in both materials. The low-energy Drude response of V2O3 appears more amenable than VO2 to ultrafast strain control. Additionally, our results provide a measurement of the temperature dependence of the sound velocity in both systems, revealing a four- to fivefold increase in VO2 and a three- to fivefold increase in V2O3 across the insulator-to-metal phase transition. Our data also confirm observations of strong damping and phonon anharmonicity in the metallic phase of VO2, and suggest that a similar phenomenon might be at play in the metallic phase of V2O3 . More generally, our simple table-top approach provides relevant and detailed information about dynamical lattice properties of vanadium oxides, paving the way to similar studies in other complex materials.

Short-Range Electron Transfer in Reduced Flavodoxin: Ultrafast Nonequilibrium Dynamics Coupled with Protein Fluctuations.

Science.gov (United States)

Kundu, Mainak; He, Ting-Fang; Lu, Yangyi; Wang, Lijuan; Zhong, Dongping

2018-05-03

Short-range electron transfer (ET) in proteins is an ultrafast process on the similar timescales as local protein-solvent fluctuations thus the two dynamics are coupled. Here, we use semiquinone flavodoxin and systematically characterized the photoinduced redox cycle with eleven mutations of different aromatic electron donors (tryptophan and tyrosine) and local residues to change redox properties. We observed the forward and backward ET dynamics in a few picoseconds, strongly following a stretched behavior resulting from a coupling between local environment relaxations and these ET processes. We further observed the hot vibrational-state formation through charge recombination and the subsequent cooling dynamics also in a few picoseconds. Combined with the ET studies in oxidized flavodoxin, these results coherently reveal the evolution of the ET dynamics from single to stretched exponential behaviors and thus elucidate critical timescales for the coupling. The observed hot vibration-state formation is robust and should be considered in all photoinduced back ET processes in flavoproteins.

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

Directory of Open Access Journals (Sweden)

Francesco Pennacchio

2017-07-01

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

Ultrafast dynamics of electronically excited molecules and clusters

International Nuclear Information System (INIS)

Lietard, Aude

2014-01-01

This PhD thesis investigated the ultrafast dynamics of photo-chromic molecules and argon clusters in the gas phase at the femtosecond timescale. Pump-probe experiments are performed in a set-up which associates a versatile pulsed molecular beam coupled to a photoelectron/photoion velocity map imager (VMI) and a time-of-flight mass spectrometer (TOF-MS). Theses pump-probe experiments provides the temporal evolution of the electronic distribution for each system of interest. Besides, a modelization has been performed in order to characterize the density and the velocity distribution in the pulsed beam. Regarding the photo-chromic di-thienyl-ethene molecules, parallel electronic relaxation pathways were observed. This contrasts with the observation of sequential relaxation processes in most molecules studied so far. In the present case, the initial wave packet splits in two parts. One part is driven to the ground state at the femtosecond time scale through a conical intersection, and the second part remains for ps in the excited state and experiences oscillations in a suspended well. This study has shed light into the intrinsic dynamics of the molecules under study and a general relaxation mechanism has been proposed, which applies to the whole family of di-thienyl-ethene molecules whatever the state of matter (gas phase or solution) in which they have been investigated. Concerning argon clusters excited at about 14 eV, two behaviors of different time scale have been observed at different time scales. The first one occurs in the first picoseconds of the dynamics. It corresponds to the electronic relaxation of an excitonic state at a rate of 1 eV.ps -1 . The second phenomenon corresponds to the localization of the exciton on the excimer Ar 2 *. This phenomenon is observed 4-5 ps after the excitation. In this study, we also observed the ejection of excited argon atoms, addressing the lifetime of the delocalized excitonic state. This work provide additional informations

Generation of attosecond electron packets via conical surface plasmon electron acceleration

Science.gov (United States)

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. PMID:26764129

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

KAUST Repository

Aly, Shawkat Mohammede; Goswami, Subhadip; Alsulami, Qana; Schanze, Kirk S.; Mohammed, Omar F.

2014-01-01

Controlling charge transfer (CT), charge separation (CS), and charge recombination (CR) at the donor-acceptor interface is extremely important to optimize the conversion efficiency in solar cell devices. In general, ultrafast CT and slow CR

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

DEFF Research Database (Denmark)

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

2016-01-01

This report will describe our recent studies of transition metal complex structural dynamics on the fs and ps time scales using an X-ray free electron laser source, Linac Coherent Light Source (LCLS). Ultrafast XANES spectra at the Ni K-edge of nickel(ii) tetramesitylporphyrin (NiTMP) were measured...... on the low-energy shoulder of the edge, which is aided by the computation of X-ray transitions for postulated excited electronic states. The observed and computed inner shell to valence orbital transition energies demonstrate and quantify the influence of the electronic configuration on specific metal...

Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules

Energy Technology Data Exchange (ETDEWEB)

Yang, Jie; Guehr, Markus; Shen, Xiaozhe; Li, Renkai; Vecchione, Theodore; Coffee, Ryan; Corbett, Jeff; Fry, Alan; Hartmann, Nick; Hast, Carsten; Hegazy, Kareem; Jobe, Keith; Makasyuk, Igor; Robinson, Joseph; Robinson, Matthew S.; Vetter, Sharon; Weathersby, Stephen; Yoneda, Charles; Wang, Xijie; Centurion, Martin

2016-10-03

Observing the motion of the nuclear wave packets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wave packet in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 Å and temporal resolution of 230 fs full width at half maximum. The method is not only sensitive to the position but also the shape of the nuclear wave packet.

Tracking the ultrafast motion of a single molecule by femtosecond orbital imaging

Science.gov (United States)

Cocker, Tyler L.; Peller, Dominik; Yu, Ping; Repp, Jascha; Huber, Rupert

2016-11-01

Watching a single molecule move on its intrinsic timescale has been one of the central goals of modern nanoscience, and calls for measurements that combine ultrafast temporal resolution with atomic spatial resolution. Steady-state experiments access the requisite spatial scales, as illustrated by direct imaging of individual molecular orbitals using scanning tunnelling microscopy or the acquisition of tip-enhanced Raman and luminescence spectra with sub-molecular resolution. But tracking the intrinsic dynamics of a single molecule directly in the time domain faces the challenge that interactions with the molecule must be confined to a femtosecond time window. For individual nanoparticles, such ultrafast temporal confinement has been demonstrated by combining scanning tunnelling microscopy with so-called lightwave electronics, which uses the oscillating carrier wave of tailored light pulses to directly manipulate electronic motion on timescales faster even than a single cycle of light. Here we build on ultrafast terahertz scanning tunnelling microscopy to access a state-selective tunnelling regime, where the peak of a terahertz electric-field waveform transiently opens an otherwise forbidden tunnelling channel through a single molecular state. It thereby removes a single electron from an individual pentacene molecule’s highest occupied molecular orbital within a time window shorter than one oscillation cycle of the terahertz wave. We exploit this effect to record approximately 100-femtosecond snapshot images of the orbital structure with sub-ångström spatial resolution, and to reveal, through pump/probe measurements, coherent molecular vibrations at terahertz frequencies directly in the time domain. We anticipate that the combination of lightwave electronics and the atomic resolution of our approach will open the door to visualizing ultrafast photochemistry and the operation of molecular electronics on the single-orbital scale.

Ultrafast collinear scattering and carrier multiplication in graphene.

Science.gov (United States)

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

2013-01-01

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

Delayed electron relaxation in CdTe nanorods studied by spectral analysis of the ultrafast transient absorption

International Nuclear Information System (INIS)

Kriegel, I.; Scotognella, F.; Soavi, G.; Brescia, R.; Rodríguez-Fernández, J.; Feldmann, J.; Lanzani, G.; Tassone, F.

2016-01-01

Highlights: • We study the photophysics of CdTe nanorods by ultrafast absorption spectroscopy. • We fit photobleaching and photoinduced absorption features at all time delays. • Dynamics are extracted from superpositions of bleaches (Gaussians) and derivatives. • Fast non-radiative recombination and slower hole trapping processes are extracted. • A potential approach to unveil ultrafast non-radiative recombination processes. - Abstract: In transient absorption (TA) spectra, the bleach features originating from state filling are overlapped by their energy-shifted derivatives, arising from excited state energy level shifts. This makes the direct extraction of carrier dynamics from a single-wavelength time-trace misleading. Fitting TA spectra in time, as Gaussian functions and their derivative-like shifted Gaussians, allows to individually extract the real dynamics of both photobleached transitions, and their energy shifts. In CdTe nanorods (NRs) we found a delayed heating of holes due to the release of the large excess energy in the electron relaxation process. The slow hole-trapping process is consistent with a high number of surface trap states in these model NRs. Our results show that only a correct disentanglement of bleaching and energy shift contributions provides a reliable framework to extract the underlying carrier relaxation dynamics, including trapping, non-radiative recombination, and eventually carrier multiplication.

Delayed electron relaxation in CdTe nanorods studied by spectral analysis of the ultrafast transient absorption

Energy Technology Data Exchange (ETDEWEB)

Kriegel, I., E-mail: ilka.kriegel@iit.it [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Scotognella, F. [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); CNST of IIT@POLIMI, Via Pascoli 70/3, 20133 Milano (Italy); Soavi, G. [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Brescia, R. [Department of Nanochemistry, Istituto Italiano di Tecnologia (IIT), via Morego 30, 16163 Genova (Italy); Rodríguez-Fernández, J.; Feldmann, J. [Photonics and Optoelectronics Group, Department of Physics and CeNS, Ludwig-Maximilians-Universität München, Amalienstr. 54, 80799 Munich (Germany); Nanosystems Initiative Munich (NIM), Schellingstr. 4, 80799 Munich (Germany); Lanzani, G., E-mail: guglielmo.lanzani@iit.it [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); CNST of IIT@POLIMI, Via Pascoli 70/3, 20133 Milano (Italy); Tassone, F. [CNST of IIT@POLIMI, Via Pascoli 70/3, 20133 Milano (Italy)

2016-06-01

Highlights: • We study the photophysics of CdTe nanorods by ultrafast absorption spectroscopy. • We fit photobleaching and photoinduced absorption features at all time delays. • Dynamics are extracted from superpositions of bleaches (Gaussians) and derivatives. • Fast non-radiative recombination and slower hole trapping processes are extracted. • A potential approach to unveil ultrafast non-radiative recombination processes. - Abstract: In transient absorption (TA) spectra, the bleach features originating from state filling are overlapped by their energy-shifted derivatives, arising from excited state energy level shifts. This makes the direct extraction of carrier dynamics from a single-wavelength time-trace misleading. Fitting TA spectra in time, as Gaussian functions and their derivative-like shifted Gaussians, allows to individually extract the real dynamics of both photobleached transitions, and their energy shifts. In CdTe nanorods (NRs) we found a delayed heating of holes due to the release of the large excess energy in the electron relaxation process. The slow hole-trapping process is consistent with a high number of surface trap states in these model NRs. Our results show that only a correct disentanglement of bleaching and energy shift contributions provides a reliable framework to extract the underlying carrier relaxation dynamics, including trapping, non-radiative recombination, and eventually carrier multiplication.

Interatomic interaction of additive elements and their influence on the processes in the double metal solutions

Directory of Open Access Journals (Sweden)

Марина Анатоліівна Рябікіна

2016-07-01

Full Text Available Modern industry uses a lot of elements as additives to improve the service characteristics of metal products that are to be used for various purposes. These elements can be divided into two groups: the first group includes the elements interacting with iron and improving its characteristics (alloying elements, and the second group includes the elements, that modify the characteristics of the structure and properties in an undesirable direction. These are trace elements: S, P, O, As, and others in steel. The negative impact of these elements shows itself as banding, the formation of non-metallic inclusions, flakes, grain boundary segregations et al. The influence of the elements of the both groups on the properties of steel depends on the nature and level of interatomic interaction in the alloy. Computational and analytical study of the major impurity elements in steel impact on the interatomic bond strength and the probability of forming complexes, clusters, and chemical compounds with the basic alloying elements in the steel has been carried out in the work. The theoretical parameter which defines the strength of the ion-covalent bond of two atoms: non-metallic – metallic is the electronegativity of elements. The electronegativity difference of the metal and non-metallic elements increasing, the ionic bonding and thermodynamic stability of these compounds  increase. On the other hand, concentration of valent electrons is a universal characteristic of an atomic element which determines many of its properties, and especially the energy of interatomic interaction. Energy calculations of pairwise interatomic impurity elements: H, C, N, S, P, As interaction with Fe and major alloying elements in steel: Mn, Cr, Si, V, Al, Ti, W, Cu, Mo, Nb were made. It has been stated that all the impurity elements except phosphorus, hydrogen and arsenic have sufficient high adhesion with the majority of the metal elements in the modern steels. Phosphorus does

Propagation of complex shaped ultrafast pulses in highly optically dense samples

International Nuclear Information System (INIS)

Davis, J. C.; Fetterman, M. R.; Warren, W. S.; Goswami, D.

2008-01-01

We examine the propagation of shaped (amplitude- and frequency-modulated) ultrafast laser pulses through optically dense rubidium vapor. Pulse reshaping, stimulated emission dynamics, and residual electronic excitation all strongly depend on the laser pulse shape. For example, frequency swept pulses, which produce adiabatic passage in the optically thin limit (independent of the sign of the frequency sweep), behave unexpectedly in optically dense samples. Paraxial Maxwell optical Bloch equations can model our ultrafast pulse propagation results well and provide insight

Interatomic potentials for materials of nuclear interest

International Nuclear Information System (INIS)

Fernandez, Julian R.; Monti, Ana M.; Pasianot, Roberto C.; Simonelli, G.

2007-01-01

Procedures to develop embedded atom method (EAM) interatomic potentials are described, with foreseeable applications in nuclear materials. Their reliability is shown by evaluating relevant properties. The studied materials are Nb, Zr and U. The first two were then used to develop an inter species potential for the Zr-Nb binary system. In this sense, the Fe-Cu system was also studied starting from Fe and Cu potentials extracted from the literature. (author) [es

Ultrafast and ultrasensitive dielectric liquids/mixtures: Basic measurements and applications

International Nuclear Information System (INIS)

Christophorou, L.G.; Faidas, H.; McCorkle, D.L.; Tennessee Univ., Knoxville, TN

1989-01-01

Basic properties of cryogenic and room temperature dielectric liquids/mixtures with high electron yields (under irradiation by ionizing particles) and high excess electron drift velocities are discussed. A number of ultrafast and ultrasensitive liquid media -- appropriate for possible use in liquid-filled radiation detectors and other applications -- are identified. 44 refs., 12 figs

A Recirculating Linac-Based Facility for Ultrafast X-Ray Science

International Nuclear Information System (INIS)

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

2003-01-01

We present an updated design for a proposed source of ultra-fast synchrotron radiation pulses based on a recirculating superconducting linac [1,2], in particular the incorporation of EUV and soft x-ray production. The project has been named LUX--Linac-based Ultrafast X-ray facility. The source produces intense x-ray pulses with duration of 10-100 fs at a 10 kHz repetition rate, with synchronization of 10's fs, optimized for the study of ultra-fast dynamics. The photon range covers the EUV to hard x-ray spectrum by use of seeded harmonic generation in undulators, and a specialized technique for ultra-short pulse photon production in the 1-10 keV range. High brightness rf photocathodes produce electron bunches which are optimized either for coherent emission in free electron lasers, or to provide a large x/y emittance ration and small vertical emittance which allows for manipulation to produce short-pulse hard x-rays. An injector linac accelerates the beam to 120 MeV, and is followed by f our passes through a 600-720 MeV recirculating linac. We outline the major technical components of the proposed facility

Development of an inter-atomic potential for the Pd-H binary system.

Energy Technology Data Exchange (ETDEWEB)

Zimmerman, Jonathan A.; Hoyt, Jeffrey John (McMaster University, Hamilton, Ontario, Canada); Leonard, Francois Leonard; Griffin, Joshua D.; Zhou, Xiao Wang

2007-09-01

Ongoing research at Sandia National Laboratories has been in the area of developing models and simulation methods that can be used to uncover and illuminate the material defects created during He bubble growth in aging bulk metal tritides. Previous efforts have used molecular dynamics calculations to examine the physical mechanisms by which growing He bubbles in a Pd metal lattice create material defects. However, these efforts focused only on the growth of He bubbles in pure Pd and not on bubble growth in the material of interest, palladium tritide (PdT), or its non-radioactive isotope palladium hydride (PdH). The reason for this is that existing inter-atomic potentials do not adequately describe the thermodynamics of the Pd-H system, which includes a miscibility gap that leads to phase separation of the dilute (alpha) and concentrated (beta) alloys of H in Pd at room temperature. This document will report the results of research to either find or develop inter-atomic potentials for the Pd-H and Pd-T systems, including our efforts to use experimental data and density functional theory calculations to create an inter-atomic potential for this unique metal alloy system.

Fourteenth International Conference on Ultrafast Phenomena

CERN Document Server

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

2005-01-01

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

Sixteenth International Conference on Ultrafast Phenomena

CERN Document Server

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

2009-01-01

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

New Aspects of Photocurrent Generation at Graphene pn Junctions Revealed by Ultrafast Optical Measurements

Science.gov (United States)

Aivazian, Grant; Sun, Dong; Jones, Aaron; Ross, Jason; Yao, Wang; Cobden, David; Xu, Xiaodong

2012-02-01

The remarkable electrical and optical properties of graphene make it a promising material for new optoelectronic applications. However, one important, but so far unexplored, property is the role of hot carriers in charge and energy transport at graphene interfaces. Here we investigate the photocurrent (PC) dynamics at a tunable graphene pn junction using ultrafast scanning PC microscopy. Pump-probe measurements show a temperature dependent relaxation time of photogenerated carriers that increases from 1.5ps at 290K to 4ps at 20K; while the amplitude of the PC is independent of the lattice temperature. These observations imply that it is hot carriers, not phonons, which dominate ultrafast energy transport. Gate dependent measurements show many interesting features such as pump induced saturation, enhancement, and sign reversal of probe generated PC. These observations reveal that the underlying PC mechanism is a combination of the thermoelectric and built-in electric field effects. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (˜500 GHz) for graphene-based photodetectors.

High-speed ultrafast laser machining with tertiary beam positioning (Conference Presentation)

Science.gov (United States)

Yang, Chuan; Zhang, Haibin

2017-03-01

For an industrial laser application, high process throughput and low average cost of ownership are critical to commercial success. Benefiting from high peak power, nonlinear absorption and small-achievable spot size, ultrafast lasers offer advantages of minimal heat affected zone, great taper and sidewall quality, and small via capability that exceeds the limits of their predecessors in via drilling for electronic packaging. In the past decade, ultrafast lasers have both grown in power and reduced in cost. For example, recently, disk and fiber technology have both shown stable operation in the 50W to 200W range, mostly at high repetition rate (beyond 500 kHz) that helps avoid detrimental nonlinear effects. However, to effectively and efficiently scale the throughput with the fast-growing power capability of the ultrafast lasers while keeping the beneficial laser-material interactions is very challenging, mainly because of the bottleneck imposed by the inertia-related acceleration limit and servo gain bandwidth when only stages and galvanometers are being used. On the other side, inertia-free scanning solutions like acoustic optics and electronic optical deflectors have small scan field, and therefore not suitable for large-panel processing. Our recent system developments combine stages, galvanometers, and AODs into a coordinated tertiary architecture for high bandwidth and meanwhile large field beam positioning. Synchronized three-level movements allow extremely fast local speed and continuous motion over the whole stage travel range. We present the via drilling results from such ultrafast system with up to 3MHz pulse to pulse random access, enabling high quality low cost ultrafast machining with emerging high average power laser sources.

Extended two-temperature model for ultrafast thermal response of band gap materials upon impulsive optical excitation

Energy Technology Data Exchange (ETDEWEB)

Shin, Taeho [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States); Samsung Advanced Institute of Technology, Suwon 443-803 (Korea, Republic of); Teitelbaum, Samuel W.; Wolfson, Johanna; Nelson, Keith A., E-mail: kanelson@mit.edu [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States); Kandyla, Maria [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States); Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, Athens 116-35 (Greece)

2015-11-21

Thermal modeling and numerical simulations have been performed to describe the ultrafast thermal response of band gap materials upon optical excitation. A model was established by extending the conventional two-temperature model that is adequate for metals, but not for semiconductors. It considers the time- and space-dependent density of electrons photoexcited to the conduction band and accordingly allows a more accurate description of the transient thermal equilibration between the hot electrons and lattice. Ultrafast thermal behaviors of bismuth, as a model system, were demonstrated using the extended two-temperature model with a view to elucidating the thermal effects of excitation laser pulse fluence, electron diffusivity, electron-hole recombination kinetics, and electron-phonon interactions, focusing on high-density excitation.

Interatomic potentials for fusion reactor material simulations

International Nuclear Information System (INIS)

Bjoerkas, C.

2009-01-01

In this thesis, the behaviour of a material situated in a fusion reactor was studied using molecular dynamics simulations. Simulations of processes in the next generation fusion reactor ITER include the reactor materials beryllium, carbon and tungsten as well as the plasma hydrogen isotopes. This means that interaction models, i.e. interatomic potentials, for this complicated quaternary system are needed. The task of finding such potentials is nonetheless nearly at its end, since models for the beryllium-carbon-hydrogen interactions were constructed in this thesis and as a continuation of that work, a beryllium-tungsten model is under development. These potentials are combinable with the earlier tungsten-carbon-hydrogen ones. The potentials were used to explain the chemical sputtering of beryllium due to deuterium plasma exposure. During experiments, a large fraction of the sputtered beryllium atoms were observed to be released as BeD molecules, and the simulations identified the swift chemical sputtering mechanism, previously not believed to be important in metals, as the underlying mechanism. Radiation damage in the reactor structural materials vanadium, iron and iron chromium, as well as in the wall material tungsten and the mixed alloy tungsten carbide, was also studied in this thesis. Interatomic potentials for vanadium, tungsten and iron were modified to be better suited for simulating collision cascades that are formed during particle irradiation, and the potential features affecting the resulting primary damage were identified. Including the often neglected electronic effects in the simulations was also shown to have an impact on the damage. With proper tuning of the electronphonon interaction strength, experimentally measured quantities related to ion-beam mixing in iron could be reproduced. The damage in tungsten carbide alloys showed elemental asymmetry, as the major part of the damage consisted of carbon defects. On the other hand, modelling the damage

A comparison of interatomic potentials for modeling tungsten nanocluster structures

Energy Technology Data Exchange (ETDEWEB)

Hao, Jiannan; Shu, Xiaolin, E-mail: shuxlin@buaa.edu.cn; Jin, Shuo; Zhang, Xuesong; Zhang, Ying; Lu, Guang-Hong

2017-02-15

Molecular dynamic simulation is utilized to study the nanocluster and the fuzz structure on the PFM surface of tungsten. The polyhedral and linear cluster structures based on the icosahedron, cuboctahedron and rhombic dodecahedron are built up. Three interatomic potentials are used in calculating the relationship between the cluster energy and the number of atoms. The results are compared with first-principles calculation to show each potential’s best application scale. Furthermore, the transition between the icosahedral and the cuboctahedral clusters is observed in molecular dynamic simulation at different temperatures, which follows a critical curve for different numbers of atoms. The linear structures are proved to be stable at experimental temperatures by thermodynamics. The work presents a selection of interatomic potentials in simulating tungsten cluster systems and helps researchers understand the growth and evolution laws of clusters and the fuzz-like structure formation process in fusion devices.

A comparison of interatomic potentials for modeling tungsten nanocluster structures

International Nuclear Information System (INIS)

Hao, Jiannan; Shu, Xiaolin; Jin, Shuo; Zhang, Xuesong; Zhang, Ying; Lu, Guang-Hong

2017-01-01

Molecular dynamic simulation is utilized to study the nanocluster and the fuzz structure on the PFM surface of tungsten. The polyhedral and linear cluster structures based on the icosahedron, cuboctahedron and rhombic dodecahedron are built up. Three interatomic potentials are used in calculating the relationship between the cluster energy and the number of atoms. The results are compared with first-principles calculation to show each potential’s best application scale. Furthermore, the transition between the icosahedral and the cuboctahedral clusters is observed in molecular dynamic simulation at different temperatures, which follows a critical curve for different numbers of atoms. The linear structures are proved to be stable at experimental temperatures by thermodynamics. The work presents a selection of interatomic potentials in simulating tungsten cluster systems and helps researchers understand the growth and evolution laws of clusters and the fuzz-like structure formation process in fusion devices.

9th International Symposium on Ultrafast Processes in Spectroscopy

CERN Document Server

Silvestri, S; Denardo, G

1996-01-01

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

Density-functional formulation of the generalized pseudopotential theory. III. Transition-metal interatomic potentials

Science.gov (United States)

Moriarty, John A.

1988-08-01

The first-principles, density-functional version of the generalized pseudopotential theory (GPT) developed in papers I and II of this series [Phys. Rev. B 16, 2537 (1977); 26, 1754 (1982)] for empty- and filled-d-band metals is here extended to pure transition metals with partially filled d bands. The present focus is on a rigorous, real-space expansion of the bulk total energy in terms of widely transferable, structure-independent interatomic potentials, including both central-force pair interactions and angular-force triplet and quadruplet interactions. To accomplish this expansion, a specialized set of starting equations is derived from the basic local-density formalism for a pure metal, including refined expansions for the exchange-correlation terms and a simplified yet accurate representation of the cohesive energy. The parent pseudo-Green's-function formalism of the GPT is then used to develop these equations in a plane-wave, localized-d-state basis. In this basis, the cohesive energy divides quite naturally into a large volume component and a smaller structural component. The volume component,which includes all one-ion intra-atomic energy contributions, already gives a good description of the cohesion in lowest order. The structural component is expanded in terms of weak interatomic matrix elements and gives rise to a multi-ion series which establishes the interatomic potentials. Special attention is focused on the dominant d-electron contributions to this series and complete formal results for the two-ion, three-ion, and four-ion d-state potentials (vd2, vd3, and vd4) are derived. In addition, a simplified model is used to demonstrate that while vd3 can be of comparable importance to vd2, vd4 is inherently small and the series is rapidly convergent beyond three-ion interactions. Analytic model forms are also derived for vd2 and vd3 in the case of canonical d bands. In this limit, vd2 is purely attractive and varies with interatomic distance as r-10, while

Ultrafast Non-thermal Response of Plasmonic Resonance in Gold Nanoantennas

Science.gov (United States)

Soavi, Giancarlo; Valle, Giuseppe Della; Biagioni, Paolo; Cattoni, Andrea; Longhi, Stefano; Cerullo, Giulio; Brida, Daniele

Ultrafast thermalization of electrons in metal nanostructures is studied by means of pump-probe spectroscopy. We track in real-time the plasmon resonance evolution, providing a tool for understanding and controlling gold nanoantennas non-linear optical response.

First-principles assessment of potential ultrafast laser-induced structural transition in Ni

Energy Technology Data Exchange (ETDEWEB)

Bévillon, E.; Colombier, J.P., E-mail: jean.philippe.colombier@univ-st-etienne.fr; Stoian, R.

2016-06-30

Highlights: • First-principles theory calculations in nonequilibrium conditions. • Electronic temperatures fully and consistently taken into account. • Evaluation of an ultrafast laser-induced solid-to-solid transition in Ni. • Relative energies, phonon spectra and energy path are evaluated. • Discussion on the generation of non-thermal forces in metals. - Abstract: The possibility to trigger ultrafast solid-to-solid transitions in transition metals under femtosecond laser irradiation is investigated by means of first-principles calculations. Electronic heating can drastically modify screening, charge distribution and atomic binding features, potentially determining new structural relaxation paths in the solid phase, before thermodynamic solid-to-liquid transformations set in. Consequently, we evaluate here the effect of electronic excitation on structural stability and conditions for structural transitions. Ni is chosen as a case study for the probability of a solid transition, and the stability of its FCC phase is compared to the non-standard HCP structure while accounting for the heating of the electronic subsystem. From a phonon spectra analysis, we show that the thermodynamic stability order reverses at an electronic temperature of around 10{sup 4} K. Both structures exhibit a dynamic stability, indicating they present a metastability depending on the heating. However, the general hardening of phonon modes with the increase of the electronic temperature points out that no transformation will occur, as confirmed by the study of a typical FCC to HCP diffusionless transformation path, showing an increasing energy barrier. Finally, based on electronic density of states interpretation, the tendency of different metal categories to undergo or not an ultrafast laser-induced structural transition is discussed.

Ultrafast demagnetization enhancement in CoFeB/MgO/CoFeB magnetic tunneling junction driven by spin tunneling current.

Science.gov (United States)

He, Wei; Zhu, Tao; Zhang, Xiang-Qun; Yang, Hai-Tao; Cheng, Zhao-Hua

2013-10-07

The laser-induced ultrafast demagnetization of CoFeB/MgO/CoFeB magnetic tunneling junction is exploited by time-resolved magneto-optical Kerr effect (TRMOKE) 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 electrons tunneling current. It opens the door to manipulate the ultrafast spin current in magnetic tunneling junctions.

Case study on the dynamics of ultrafast laser heating and ablation of gold thin films by ultrafast pump-probe reflectometry and ellipsometry

Science.gov (United States)

Pflug, T.; Wang, J.; Olbrich, M.; Frank, M.; Horn, A.

2018-02-01

To increase the comprehension of ultrafast laser ablation, the ablation process has to be portrayed with sufficient temporal resolution. For example, the temporal modification of the complex refractive index {\\tilde{n}} and the relative reflectance of a sample material after irradiation with ultrafast single-pulsed laser radiation can be measured with a pump-probe setup. This work describes the construction and validation of a pump-probe setup enabling spatially, temporally, and spectroscopically resolved Brewster angle microscopy, reflectometry, ellipsometry, and shadow photography. First pump-probe reflectometry and ellipsometry measurements are performed on gold at λ _{probe}= 440 nm and three fluences of the single-pulsed pump radiation at λ _{pump}= 800 nm generating no, gentle, and strong ablation. The relative reflectance overall increases at no and gentle ablation. At strong ablation, the relative reflectance locally decreases, presumable caused by emitted thermal electrons, ballistic electrons, and ablating material. The refractive index n is slightly decreasing after excitation, while the extinction coefficient k is increasing.

Ultrafast, 2 min synthesis of monolayer-protected gold nanoclusters (d < 2 nm)

Science.gov (United States)

Martin, Matthew N.; Li, Dawei; Dass, Amala; Eah, Sang-Kee

2012-06-01

An ultrafast synthesis method is presented for hexanethiolate-coated gold nanoclusters (d gold nanoclusters are separated from the reaction byproducts fast and easily without any need for post-synthesis cleaning.An ultrafast synthesis method is presented for hexanethiolate-coated gold nanoclusters (d gold nanoclusters are separated from the reaction byproducts fast and easily without any need for post-synthesis cleaning. Electronic supplementary information (ESI) available: Experimental details of gold nanocluster synthesis and mass-spectrometry. See DOI: 10.1039/c2nr30890h

Theory of pump–probe ultrafast photoemission and X-ray absorption spectra

Energy Technology Data Exchange (ETDEWEB)

Fujikawa, Takashi, E-mail: tfujikawa@faculty.chiba-u.jp; Niki, Kaori

2016-01-15

Highlights: • Pump–probe ultrafast XAFS and XPS spectra are theoretically studied. • Keldysh Green's function theory is applied. • Important many-body effects are explicitly included. - Abstract: Keldysh Green's function approach is extensively used in order to derive practical formulas to analyze pump–probe ultrafast photoemission and X-ray absorption spectra. Here the pump pulse is strong enough whereas the probe X-ray pulse can be treated by use of a perturbation theory. We expand full Green's function in terms of renormalized Green's function without the interaction between electrons and probe pulse. The present theoretical formulas allow us to handle the intrinsic and extrinsic losses, and furthermore resonant effects in X-ray Absorption Fine Structures (XAFS). To understand the radiation field screening in XPS spectra, we have to use more sophisticated theoretical approach. In the ultrafast XPS and XAFS analyses the intrinsic and extrinsic loss effects can interfere as well. In the XAFS studies careful analyses are necessary to handle extrinsic losses in terms of damped photoelectron propagation. The nonequilibrium dynamics after the pump pulse irradiation is well described by use of the time-dependent Dyson orbitals. Well above the edge threshold, ultrafast photoelectron diffraction and extended X-ray absorption fine structure (EXAFS) provide us with transient structural change after the laser pump excitations. In addition to these slow processes, the rapid oscillation in time plays an important role related to pump electronic excitations. Near threshold detailed information could be obtained for the combined electronic and structural dynamics. In particular high-energy photoemission and EXAFS are not so influenced by the details of excited states by pump pulse. Random-Phase Approximation (RPA)-boson approach is introduced to derive some practical formulas for time-dependent intrinsic amplitudes.

Exciplex formation in bimolecular photoinduced electron-transfer investigated by ultrafast time-resolved infrared spectroscopy.

Science.gov (United States)

Koch, Marius; Letrun, Romain; Vauthey, Eric

2014-03-12

The dynamics of bimolecular photoinduced electron-transfer reactions has been investigated with three donor/acceptor (D/A) pairs in tetrahydrofuran (THF) and acetonitrile (ACN) using a combination of ultrafast spectroscopic techniques, including time-resolved infrared absorption. For the D/A pairs with the highest driving force of electron transfer, all transient spectroscopic features can be unambiguously assigned to the excited reactant and the ionic products. For the pair with the lowest driving force, three additional transient infrared bands, more intense in THF than in ACN, with a time dependence that differs from those of the other bands are observed. From their frequency and solvent dependence, these bands can be assigned to an exciplex. Moreover, polarization-resolved measurements point to a relatively well-defined mutual orientation of the constituents and to a slower reorientational time compared to those of the individual reactants. Thanks to the minimal overlap of the infrared signature of all transient species in THF, a detailed reaction scheme including the relevant kinetic and thermodynamic parameters could be deduced for this pair. This analysis reveals that the formation and recombination of the ion pair occur almost exclusively via the exciplex.

Ultrafast dissociation: An unexpected tool for probing molecular dynamics

International Nuclear Information System (INIS)

Morin, Paul; Miron, Catalin

2012-01-01

Highlights: ► Ultrafast dissociation has been investigated by means of XPS and mass spectrometry. ► The interplay between electron relaxation and molecular dynamics is evidenced. ► Extension toward polyatomics, clusters, adsorbed molecules is considered. ► Quantum effects (spectral hole, angular effects) evidence the molecular field anisotropy. -- Abstract: Ultrafast dissociation following core–shell excitation into an antibonding orbital led to the early observation in HBr of atomic Auger lines associated to the decay of dissociated excited atoms. The purpose of this article is to review the very large variety of systems where such a situation has been encountered, extending from simple diatomic molecules toward more complex systems like polyatomics, clusters, or adsorbed molecules. Interestingly, this phenomenon has revealed an extremely rich and powerful tool for probing nuclear dynamics and its subtle interplay with electron relaxation occurring on a comparable time scale. Consequently this review covers a surprisingly large period, starting in 1986 and still ongoing.

A general transformation to canonical form for potentials in pairwise interatomic interactions.

Science.gov (United States)

Walton, Jay R; Rivera-Rivera, Luis A; Lucchese, Robert R; Bevan, John W

2015-06-14

A generalized formulation of explicit force-based transformations is introduced to investigate the concept of a canonical potential in both fundamental chemical and intermolecular bonding. Different classes of representative ground electronic state pairwise interatomic interactions are referenced to a chosen canonical potential illustrating application of such transformations. Specifically, accurately determined potentials of the diatomic molecules H2, H2(+), HF, LiH, argon dimer, and one-dimensional dissociative coordinates in Ar-HBr, OC-HF, and OC-Cl2 are investigated throughout their bound potentials. Advantages of the current formulation for accurately evaluating equilibrium dissociation energies and a fundamentally different unified perspective on nature of intermolecular interactions will be emphasized. In particular, this canonical approach has significance to previous assertions that there is no very fundamental distinction between van der Waals bonding and covalent bonding or for that matter hydrogen and halogen bonds.

Phonon optimized interatomic potential for aluminum

Directory of Open Access Journals (Sweden)

Murali Gopal Muraleedharan

2017-12-01

Full Text Available We address the problem of generating a phonon optimized interatomic potential (POP for aluminum. The POP methodology, which has already been shown to work for semiconductors such as silicon and germanium, uses an evolutionary strategy based on a genetic algorithm (GA to optimize the free parameters in an empirical interatomic potential (EIP. For aluminum, we used the Vashishta functional form. The training data set was generated ab initio, consisting of forces, energy vs. volume, stresses, and harmonic and cubic force constants obtained from density functional theory (DFT calculations. Existing potentials for aluminum, such as the embedded atom method (EAM and charge-optimized many-body (COMB3 potential, show larger errors when the EIP forces are compared with those predicted by DFT, and thus they are not particularly well suited for reproducing phonon properties. Using a comprehensive Vashishta functional form, which involves short and long-ranged interactions, as well as three-body terms, we were able to better capture interactions that reproduce phonon properties accurately. Furthermore, the Vashishta potential is flexible enough to be extended to Al2O3 and the interface between Al-Al2O3, which is technologically important for combustion of solid Al nano powders. The POP developed here is tested for accuracy by comparing phonon thermal conductivity accumulation plots, density of states, and dispersion relations with DFT results. It is shown to perform well in molecular dynamics (MD simulations as well, where the phonon thermal conductivity is calculated via the Green-Kubo relation. The results are within 10% of the values obtained by solving the Boltzmann transport equation (BTE, employing Fermi’s Golden Rule to predict the phonon-phonon relaxation times.

Phonon optimized interatomic potential for aluminum

Science.gov (United States)

Muraleedharan, Murali Gopal; Rohskopf, Andrew; Yang, Vigor; Henry, Asegun

2017-12-01

We address the problem of generating a phonon optimized interatomic potential (POP) for aluminum. The POP methodology, which has already been shown to work for semiconductors such as silicon and germanium, uses an evolutionary strategy based on a genetic algorithm (GA) to optimize the free parameters in an empirical interatomic potential (EIP). For aluminum, we used the Vashishta functional form. The training data set was generated ab initio, consisting of forces, energy vs. volume, stresses, and harmonic and cubic force constants obtained from density functional theory (DFT) calculations. Existing potentials for aluminum, such as the embedded atom method (EAM) and charge-optimized many-body (COMB3) potential, show larger errors when the EIP forces are compared with those predicted by DFT, and thus they are not particularly well suited for reproducing phonon properties. Using a comprehensive Vashishta functional form, which involves short and long-ranged interactions, as well as three-body terms, we were able to better capture interactions that reproduce phonon properties accurately. Furthermore, the Vashishta potential is flexible enough to be extended to Al2O3 and the interface between Al-Al2O3, which is technologically important for combustion of solid Al nano powders. The POP developed here is tested for accuracy by comparing phonon thermal conductivity accumulation plots, density of states, and dispersion relations with DFT results. It is shown to perform well in molecular dynamics (MD) simulations as well, where the phonon thermal conductivity is calculated via the Green-Kubo relation. The results are within 10% of the values obtained by solving the Boltzmann transport equation (BTE), employing Fermi's Golden Rule to predict the phonon-phonon relaxation times.

A gradient approximation for calculating Debye temperatures from pairwise interatomic potentials

International Nuclear Information System (INIS)

Jackson, D.P.

1975-09-01

A simple gradient approximation is given for calculating the effective Debye temperature of a cubic crystal from central pairwise interatomic potentials. For examples of the Morse potential applied to cubic metals the results are in generally good agreement with experiment. (author)

Accurate Ne-heavier rare gas interatomic potentials

International Nuclear Information System (INIS)

Candori, R.; Pirani, F.; Vecchiocattivi, F.

1983-01-01

Accurate interatomic potential curves for Ne-heavier rare gas systems are obtained by a multiproperty analysis. The curves are given via a parametric function which consists of a modified Dunham expansion connected at long range with the van der Waals expansion. The experimental properties considered in the analysis are the differential scattering cross sections at two different collision energies, the integral cross sections in the glory energy range and the second virial coefficients. The transport properties are considered indirectly by using the potential energy values recently obtained by inversion of the transport coefficients. (author)

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

Energy Technology Data Exchange (ETDEWEB)

Rittman, Dylan R. [Department of Nuclear Engineering and Radiological Sciences, University of Michigan, Ann Arbor, Michigan 48109 (United States); Department of Geological Sciences, Stanford University, Stanford, California 94305 (United States); Tracy, Cameron L.; Cusick, Alex B.; Abere, Michael J.; Yalisove, Steven M. [Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109 (United States); Torralva, Ben [Department of Atmospheric, Oceanic and Space Sciences, University of Michigan, Ann Arbor, Michigan 48109 (United States); Ewing, Rodney C. [Department of Geological Sciences, Stanford University, Stanford, California 94305 (United States)

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.

Robust Stacking-Independent Ultrafast Charge Transfer in MoS2/WS2 Bilayers.

Science.gov (United States)

Ji, Ziheng; Hong, Hao; Zhang, Jin; Zhang, Qi; Huang, Wei; Cao, Ting; Qiao, Ruixi; Liu, Can; Liang, Jing; Jin, Chuanhong; Jiao, Liying; Shi, Kebin; Meng, Sheng; Liu, Kaihui

2017-12-26

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS 2 /WS 2 bilayer with various stacking configurations, by optical two-color ultrafast pump-probe spectroscopy. Surprisingly, we found that the charge transfer is robust against varying interlayer twist angles and interlayer coupling strength, in time scale of ∼90 fs. Our observation, together with atomic-resolved transmission electron characterization and time-dependent density functional theory simulations, reveals that the robust ultrafast charge transfer is attributed to the heterogeneous interlayer stretching/sliding, which provides additional channels for efficient charge transfer previously unknown. Our results elucidate the origin of transfer rate robustness against interlayer stacking configurations in optical devices based on 2D heterostructures, facilitating their applications in ultrafast and high-efficient optoelectronic and photovoltaic devices in the near future.

Interatomic Coulombic decay following the Auger decay: Experimental evidence in rare-gas dimers

International Nuclear Information System (INIS)

Ueda, K.; Fukuzawa, H.; Liu, X.-J.; Sakai, K.; Pruemper, G.; Morishita, Y.; Saito, N.; Suzuki, I.H.; Nagaya, K.; Iwayama, H.; Yao, M.; Kreidi, K.; Schoeffler, M.; Jahnke, T.; Schoessler, S.; Doerner, R.; Weber, Th.; Harries, J.; Tamenori, Y.

2008-01-01

Interatomic Coulombic decay (ICD) in Ar 2 , ArKr and Kr 2 following Ar 2p or Kr 3d Auger decay has been investigated by means of momentum-resolved electron-ion-ion coincidence spectroscopy. This sequential decay leads to Coulombic dissociation into dication and monocation. Simultaneously determining the kinetic energy of the ICD electron and the kinetic energy release between the two atomic ions, we have been able to unambiguously identify the ICD channels. We find that, in general, spin-conserved ICD, in which the singlet (triplet) dicationic state produced via the atomic Auger decay preferentially decays to the singlet (triplet) state, transferring the energy to the other atom, is faster than spin-flip ICD, in which the Auger final singlet (triplet) dicationic state decays to the triplet (singlet) state. However, spin-flip ICD may take place when spin-conserved ICD becomes energetically forbidden. Dipole-forbidden ICDs from Kr 2+ (4s -21 S)-B (B = Ar or Kr) to Kr 2+ (4p -21 D, 3 P)-B + are also observed

Is there a contraction of the interatomic distance in small metal particles?

DEFF Research Database (Denmark)

Hansen, Lars Bruno; Stoltze, Per; Nørskov, Jens Kehlet

1990-01-01

A theoretical analysis is made of the bond lengths of small (100–1000 atoms) Cu particles at various temperatures. The interatomic interactions are calculated using the effective-medium theory and the finite-temperature properties obtained from a molecular-dynamics simulation. We find only very s...... small changes in bond length with particle size, but the motion in the small particles is very anharmonic. We use this observation to resolve the current experimental controversy about the existence of bond contraction for small metal particles.......A theoretical analysis is made of the bond lengths of small (100–1000 atoms) Cu particles at various temperatures. The interatomic interactions are calculated using the effective-medium theory and the finite-temperature properties obtained from a molecular-dynamics simulation. We find only very...

Imaging the Ultrafast Photoelectron Transfer Process in Alizarin-TiO2

Directory of Open Access Journals (Sweden)

Tatiana Gomez

2015-07-01

Full Text Available In this work, we adopt a quantum mechanical approach based on time-dependent density functional theory (TDDFT to study the optical and electronic properties of alizarin supported on TiO2 nano-crystallites, as a prototypical dye-sensitized solar cell. To ensure proper alignment of the donor (alizarin and acceptor (TiO2 nano-crystallite levels, static optical excitation spectra are simulated using time-dependent density functional theory in response. The ultrafast photoelectron transfer from the dye to the cluster is simulated using an explicitly time-dependent, one-electron TDDFT ansatz. The model considers the δ-pulse excitation of a single active electron localized in the dye to the complete set of energetically accessible, delocalized molecular orbitals of the dye/nano-crystallite complex. A set of quantum mechanical tools derived from the transition electronic flux density is introduced to visualize and analyze the process in real time. The evolution of the created wave packet subject to absorbing boundary conditions at the borders of the cluster reveal that, while the electrons of the aromatic rings of alizarin are heavily involved in an ultrafast charge redistribution between the carbonyl groups of the dye molecule, they do not contribute positively to the electron injection and, overall, they delay the process.

Ultrafast MR Imaging in Pediatric Neuroradiology

International Nuclear Information System (INIS)

Singh, R.K.; Smith, J.T.; Wilkinson, I.D.; Griffiths, P.D.

2003-01-01

Purpose: To compare the diagnostic information obtained from ultrafast MR imaging with standard MR imaging techniques in pediatric neuroradiology. The goal was to judge whether ultrafast methods can be used to replace standard methods and reduce the need for sedation or general anesthesia as a result of the considerably shorter scan times. Material and Methods: Our prospective study involved 125 patients. Routine clinical imaging was performed along with two ultrafast methods. Single shot fast spin echo (SSFSE) was used to give T2-weighted images and an echo planar imaging (EPI) sequence to provide a T1-weighted images. The ultrafast images were presented to an experienced neuro radiologist who was also given the information present on the initial referral card. These reports based on the ultrafast images were then compared with the formal radiologic report made solely on the basis of the standard imaging. Results: The overall sensitivity and specificity for ultrafast imaging when compared to the reference standard were 78% and 98% with positive and negative predictive values of 98% and 76%. Pathologies characterized by small areas of subtle T2 prolongation were difficult or impossible to see on the ultrafast images but otherwise they provided reliable information. Conclusions: This paper demonstrates that ultrafast MR imaging can diagnose many pediatric intracranial abnormalities as well as standard methods. Anatomic resolution limits its capacity to define subtle developmental anomalies and contrast resolution limitations of the ultrafast methods reduce the detection of pathology characterized by subtle T2 prolongation

Electro-optic sampling at 90 degree interaction geometry for time-of-arrival stamping of ultrafast relativistic electron diffraction

Directory of Open Access Journals (Sweden)

C. M. Scoby

2010-02-01

Full Text Available In this paper we study a new geometry setup for electro-optic sampling (EOS where the electron beam runs parallel to the ⟨110⟩ face of a ZnTe crystal and the probe laser is perpendicular to it and to the beam path. The simple setup is used to encode the time-of-arrival information of a 3.5  MeV<10  pC electron bunch on the spatial profile of the laser pulse. The electric field lines inside the dielectric bend at an angle due to a relatively large (n∼3 index of refraction of the ZnTe crystal. We found theoretically and experimentally that the EOS signal can be maximized with a proper choice of incoming laser polarization angle. We achieved single-shot nondestructive measurement of the relative time of arrival between the pump and the probe beams thus improving the temporal resolution of ultrafast relativistic electron diffraction experiments.

Ultrafast optical pump terahertz-probe spectroscopy of strongly correlated electron materials

International Nuclear Information System (INIS)

Averitt, R.D.; Taylor, Antoinette J.; Thorsmolle, V.K.; Jia, Quanxi; Lobad, A.I.; Trugman, S.A.

2001-01-01

We have used optical-pump far-infrared probe spectroscopy to probe the low energy electron dynamics of high temperature superconductors and colossal magnetoresistance manganites. For the superconductor YBa2Cu3O7, picosecond conductivity measurements probe the interplay between Cooper-pairs and quasiparticles. In optimally doped films, the recovery time for long-range phase-coherent pairing increases from ∼1.5 ps at 4K to ∼3.5 ps near Tc, consistent with the closing of the superconducting gap. For underdoped films, the measured recovery time is temperature independent (3.5 ps) in accordance with the presence of a pseudogap. Ultrafast picosecond measurements of optically induced changes in the absolute conductivity of La0:7M0:3MnO3 thin films (M = Ca, Sr) from 10K to ∼0.9Tc reveal a two-component relaxation. A fast, ∼2 ps, conductivity decrease arises from optically induced modification of the effective phonon temperature. The slower component, related to spin-lattice relaxation, has a lifetime that increases upon approaching Tc from below in accordance with an increasing spin specific heat. Our results indicate that for T<< Tc, the conductivity is determined by incoherent phonons while spin fluctuations dominate near Tc.

Study of the ultrafast polarization dynamics in lithium borohydride by means of femtosecond X-ray diffraction

International Nuclear Information System (INIS)

Stingl, Johannes

2013-01-01

In this thesis the ultrafast electronic polarisation in the crystalline material lithium borohydride (LiBH 4 ) is examined. The material is excited by a femtosecond long optical pulse and scanned by a likewise short X-ray pulse. Using X-ray scattering the optically induced spatial rearrangement of electronic charge can be directly mapped with atomic spatial resolution. Copper K-alpha X-rays for the experiment are produced in a laboratory table-top laserplasma source with 1 kHz repetition rate. This radiation is then focused on a powdered sample. Debye-Scherrer rings produced from powder diffraction are collected on a large area detector and processed to yield intensity profiles. Using pump-probe technique the change in diffracted intensity, triggered by excitation with a femtosecond optical pulse is examined. The temporal resolution is given by the delay between pump and probe pulse. This way insight is gained into the dynamic electronic evolution of the system. Intensity changes can be correlated to changes in charge density in the relevant material to elucidate structural dynamics on the femtosecond time scale. Lithium borohydride was chosen since it displays necessary characteristics for the exploration of ultrafast electronic polarisation. Up to date there has been no spatially resolved research in the femtosecond regime elucidating this electronic phenomenon. This work presents the ultrafast resonse in Lithiumborhydrid (LiBH 4 ) to strong electronic fields with optical frequencies, which leads to charge relocation accompanied by electronic polarisation.

Ultrafast surface carrier dynamics in the topological insulator Bi₂Te₃.

Science.gov (United States)

Hajlaoui, M; Papalazarou, E; Mauchain, J; Lantz, G; Moisan, N; Boschetto, D; Jiang, Z; Miotkowski, I; Chen, Y P; Taleb-Ibrahimi, A; Perfetti, L; Marsi, M

2012-07-11

We discuss the ultrafast evolution of the surface electronic structure of the topological insulator Bi(2)Te(3) following a femtosecond laser excitation. Using time and angle-resolved photoelectron spectroscopy, we provide a direct real-time visualization of the transient carrier population of both the surface states and the bulk conduction band. We find that the thermalization of the surface states is initially determined by interband scattering from the bulk conduction band, lasting for about 0.5 ps; subsequently, few picoseconds are necessary for the Dirac cone nonequilibrium electrons to recover a Fermi-Dirac distribution, while their relaxation extends over more than 10 ps. The surface sensitivity of our measurements makes it possible to estimate the range of the bulk-surface interband scattering channel, indicating that the process is effective over a distance of 5 nm or less. This establishes a correlation between the nanoscale thickness of the bulk charge reservoir and the evolution of the ultrafast carrier dynamics in the surface Dirac cone.

Intensified CCD for ultrafast diagnostics

International Nuclear Information System (INIS)

Cheng, J.; Tripp, G.; Coleman, L.

1978-01-01

Many of the present laser fusion diagnostics are recorded on either ultrafast streak cameras or on oscilloscopes. For those experiments in which a large volume of data is accumulated, direct computer processing of the information becomes important. We describe an approach which uses a RCA 52501 back-thinned CCD sensor to obtain direct electron readouts for both the streak camera and the CRT. Performance of the 100 GHz streak camera and the 4 GHz CRT are presented. Design parameters and computer interfacing for both systems are described in detail

An electronically tunable ultrafast laser source applied to fluorescence imaging and fluorescence lifetime imaging microscopy

International Nuclear Information System (INIS)

Dunsby, C; Lanigan, P M P; McGinty, J; Elson, D S; Requejo-Isidro, J; Munro, I; Galletly, N; McCann, F; Treanor, B; Oenfelt, B; Davis, D M; Neil, M A A; French, P M W

2004-01-01

Fluorescence imaging is used widely in microscopy and macroscopic imaging applications for fields ranging from biomedicine to materials science. A critical component for any fluorescence imaging system is the excitation source. Traditionally, wide-field systems use filtered thermal or arc-generated white light sources, while point scanning confocal microscope systems require spatially coherent (point-like) laser sources. Unfortunately, the limited range of visible wavelengths available from conventional laser sources constrains the design and usefulness of fluorescent probes in confocal microscopy. A 'hands-off' laser-like source, electronically tunable across the visible spectrum, would be invaluable for fluorescence imaging and provide new opportunities, e.g. automated excitation fingerprinting and in situ measurement of excitation cross-sections. Yet more information can be obtained using fluorescence lifetime imaging (FLIM), which requires that the light source be pulsed or rapidly modulated. We show how a white light continuum, generated by injecting femtosecond optical radiation into a micro-structured optical fibre, coupled with a simple prism-based tunable filter arrangement, can fulfil all these roles as a continuously electronically tunable (435-1150 nm) visible ultrafast light source in confocal, wide-field and FLIM systems

Linear and ultrafast nonlinear plasmonics of single nano-objects

Science.gov (United States)

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

2017-03-01

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

Ultrafast Graphene Photonics and Optoelectronics

Science.gov (United States)

2017-04-14

AFRL-AFOSR-JP-TR-2017-0032 Ultrafast Graphene Photonics and Optoelectronics Kuang-Hsiung Wu National Chiao Tung University Final Report 04/14/2017...DATES COVERED (From - To) 18 Apr 2013 to 17 Apr 2016 4. TITLE AND SUBTITLE Ultrafast Graphene Photonics and Optoelectronics 5a.  CONTRACT NUMBER 5b...Prescribed by ANSI Std. Z39.18 Final Report for AOARD Grant FA2386-13-1-4022 “Ultrafast Graphene Photonics and Optoelectronics” Date May 23th, 2016

Multipole expansion of the retarded interatomic dispersion energy: derivation from quantum electrodynamics

NARCIS (Netherlands)

Michels, M.A.J.; Suttorp, L.G.

1972-01-01

The multipole expansion of the retarded dispersion energy of two atoms in nondegenerate ground states is derived. The result shows that multipoles of different order may give rise to dispersion energies varying in the same way for large interatomic separations.

Ultrafast laser and swift heavy ion irradiation: Response of Gd ₂ O ₃ and ZrO ₂ to intense electronic excitation

Energy Technology Data Exchange (ETDEWEB)

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

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 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$\\bar{2}$), (003), (310), and (112$\\bar{2}$) 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.

Advanced Instrumentation for Ultrafast Science at the LCLS

Energy Technology Data Exchange (ETDEWEB)

Berrah, Nora [Univ. of Connecticut, Storrs, CT (United States)

2015-10-13

This grant supported a Single Investigator and Small Group Research (SISGR) application to enable multi-user research in Ultrafast Science using the Linac Coherent Light Source (LCLS), the world’s first hard x-ray free electron laser (FEL) which lased for the first time at 1.5 Å on April 20, 2009. The goal of our proposal was to enable a New Era of Science by requesting funds to purchase and build Advanced Instrumentation for Ultrafast Science (AIUS), to utilize the intense, short x-ray pulses produced by the LCLS. The proposed instrumentation will allow peer review selected users to probe the ultrasmall and capture the ultrafast. These tools will expand on the investment already made in the construction of the light source and its instrumentation in both the LCLS and LUSI projects. The AIUS will provide researchers in the AMO, Chemical, Biological and Condensed Matter communities with greater flexibility in defining their scientific agenda at the LCLS. The proposed instrumentation will complement and significantly augment the present AMO instrument (funded through the LCLS project) through detectors and capabilities not included in the initial suite of instrumentation at the facility. We have built all of the instrumentations and they have been utilized by scientists. Please see report attached.

Development of an interatomic EAM type potential for Zr

International Nuclear Information System (INIS)

Pasianot, R.C.; Monti, A.M.

1996-01-01

In the present work are developed interatomic potentials of the embedded atom type (EAM) adequate for computer simulation of microstructural defects in the Zr lattice. It is observed that the less repulsive potential agrees better with the experimental data of the self-interstitial relaxation volume and predicts the basal crowdion as the stable configuration, the basal dumbbell having a formation energy slightly higher (0.01 eV). (author). 9 refs., 1 fig., 3 tabs

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

Science.gov (United States)

Tang, Jau

2008-04-28

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

Study of local response effects in interatomic collisions with two active electrons in the framework of time-dependent density functional theory; Untersuchung lokaler Responseffekte in interatomaren Stoessen mit zwei aktiven Elektronen im Rahmen zeitabhaengiger Dichtefunktionaltheorie

Energy Technology Data Exchange (ETDEWEB)

Keim, M.

2005-07-01

In the present thesis response effects in interatomic collisions with two active electrons are studied in the range of non-relativistic collision energies. The starting point is the mapping of the time-dependent interacting many-electron sytem on an effective one-particle picture on the base of the time-dependent density functional theory (TDDFT). By means of the basis generator method the one-particle equations aring in the framework of the TDDFT concept are solved in a finite-dimensional model space. In the study of ionization cross section in the collisional systeem anti p+He it is shown that by response effects an essential diminuishing of the cross sections in comparison to the no-response case is reached. Analoguously the ionization cross sections for the collisional systems p-He, He{sup 2+}-He, Li{sup 3+}-He and p-Li{sup +} behave.

Ultrafast Hierarchical OTDM/WDM Network

Directory of Open Access Journals (Sweden)

Hideyuki Sotobayashi

2003-12-01

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

Electron-mediated relaxation following ultrafast pumping of strongly correlated materials: model evidence of a correlation-tuned crossover between thermal and nonthermal states.

Science.gov (United States)

Moritz, B; Kemper, A F; Sentef, M; Devereaux, T P; Freericks, J K

2013-08-16

We examine electron-electron mediated relaxation following ultrafast electric field pump excitation of the fermionic degrees of freedom in the Falicov-Kimball model for correlated electrons. The results reveal a dichotomy in the temporal evolution of the system as one tunes through the Mott metal-to-insulator transition: in the metallic regime relaxation can be characterized by evolution toward a steady state well described by Fermi-Dirac statistics with an increased effective temperature; however, in the insulating regime this quasithermal paradigm breaks down with relaxation toward a nonthermal state with a complicated electronic distribution as a function of momentum. We characterize the behavior by studying changes in the energy, photoemission response, and electronic distribution as functions of time. This relaxation may be observable qualitatively on short enough time scales that the electrons behave like an isolated system not in contact with additional degrees of freedom which would act as a thermal bath, especially when using strong driving fields and studying materials whose physics may manifest the effects of correlations.

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

Science.gov (United States)

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

2016-08-01

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

Influence of the interatomic potentials on molecular dynamics simulations of displacement cascades

CERN Document Server

Becquart, C S; Legris, A; Van Duysen, J C

2000-01-01

Molecular dynamics (MD) is a powerful tool to study the displacement cascades initiated by the neutrons when they interact with matter. Key components of this technique are the interatomic potentials which model the binding of the different constitutive atoms. There exist many interatomic potentials dedicated to alpha-Fe and we have tested three of them for the study of radiation damage. We have found that the primary damage is potential sensitive. From our study, it appears that some characteristics of the potentials, not always considered, can be correlated to the type of damage produced by displacement cascades. The repulsive part of the potential has a strong influence on the cascade morphology. Moreover, equilibrium properties such as the atoms mean square displacements, the vacancy migration and vacancy-vacancy binding energies also appear to have some influence and should be investigated carefully when simulating radiation damage. It is therefore very important to use extreme care when trying to obtain...

Avant-Garde Ultrafast Laser Writing

Directory of Open Access Journals (Sweden)

Kazansky P. G.

2013-11-01

Full Text Available Ultrafast laser processing of transparent materials reveals new phenomena. Reviewed, are recent demonstrations of 5D optical memory, vortex polarization and Airy beam converters employing self-assembled nanostructuring, ultrafast laser calligraphy and polarization writing control using pulses with tilted front.

Ultrafast nonlinear optics

CERN Document Server

Leburn, Christopher; Reid, Derryck

2013-01-01

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

Nonponderomotive electron acceleration in ultrashort surface-plasmon fields

Energy Technology Data Exchange (ETDEWEB)

Racz, Peter; Dombi, Peter [Wigner Research Centre for Physics, Konkoly-Thege M. ut 29-33, H-1121 Budapest (Hungary)

2011-12-15

We investigate the nonponderomotive nature of ultrafast plasmonic electron acceleration in strongly decaying electromagnetic fields generated by few-cycle and single-cycle femtosecond laser pulses. We clearly identify the conditions contributing to nonponderomotive acceleration and establish fundamental scaling laws and carrier-envelope phase effects. These all-optically accelerated compact, femtosecond electron sources can be utilized in contemporary ultrafast methods.

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

Energy Technology Data Exchange (ETDEWEB)

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

2013-08-15

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

Quantum Hooke's Law to Classify Pulse Laser Induced Ultrafast Melting

Science.gov (United States)

Hu, Hao; Ding, Hepeng; Liu, Feng

2015-02-01

Ultrafast crystal-to-liquid phase transition induced by femtosecond pulse laser excitation is an interesting material's behavior manifesting the complexity of light-matter interaction. There exist two types of such phase transitions: one occurs at a time scale shorter than a picosecond via a nonthermal process mediated by electron-hole plasma formation; the other at a longer time scale via a thermal melting process mediated by electron-phonon interaction. However, it remains unclear what material would undergo which process and why? Here, by exploiting the property of quantum electronic stress (QES) governed by quantum Hooke's law, we classify the transitions by two distinct classes of materials: the faster nonthermal process can only occur in materials like ice having an anomalous phase diagram characterized with dTm/dP < 0, where Tm is the melting temperature and P is pressure, above a high threshold laser fluence; while the slower thermal process may occur in all materials. Especially, the nonthermal transition is shown to be induced by the QES, acting like a negative internal pressure, which drives the crystal into a ``super pressing'' state to spontaneously transform into a higher-density liquid phase. Our findings significantly advance fundamental understanding of ultrafast crystal-to-liquid phase transitions, enabling quantitative a priori predictions.

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

Directory of Open Access Journals (Sweden)

T. Frigge

2015-05-01

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

FAST TRACK COMMUNICATION: A Be-W interatomic potential

Science.gov (United States)

Björkas, C.; Henriksson, K. O. E.; Probst, M.; Nordlund, K.

2010-09-01

In this work, an interatomic potential for the beryllium-tungsten system is derived. It is the final piece of a potential puzzle, now containing all possible interactions between the fusion reactor materials beryllium, tungsten and carbon as well as the plasma hydrogen isotopes. The potential is suitable for plasma-wall interaction simulations and can describe the intermetallic Be2W and Be12W phases. The interaction energy between a Be surface and a W atom, and vice versa, agrees qualitatively with ab initio calculations. The potential can also reasonably describe BexWy molecules with x, y = 1, 2, 3, 4.

Ultrafast optical switching in three-dimensional photonic crystals

OpenAIRE

Mazurenko, D.A.

2004-01-01

The rapidly expanding research on photonic crystals is driven by potential applications in all-optical switches, optical computers, low-threshold lasers, and holographic data storage. The performance of such devices might surpass the speed of traditional electronics by several orders of magnitude and may result in a true revolution in nanotechnology. The heart of such devices would likely be an optical switching element. This thesis analyzes different regimes of ultrafast all-optical switchin...

A simple electron multiplexer

International Nuclear Information System (INIS)

Dobrzynski, L; Akjouj, A; Djafari-Rouhani, B; Al-Wahsh, H; Zielinski, P

2003-01-01

We present a simple multiplexing device made of two atomic chains coupled by two other transition metal atoms. We show that this simple atomic device can transfer electrons at a given energy from one wire to the other, leaving all other electron states unaffected. Closed-form relations between the transmission coefficients and the inter-atomic distances are given to optimize the desired directional electron ejection. Such devices can be adsorbed on insulating substrates and characterized by current surface technologies. (letter to the editor)

Low damage electrical modification of 4H-SiC via ultrafast laser irradiation

Science.gov (United States)

Ahn, Minhyung; Cahyadi, Rico; Wendorf, Joseph; Bowen, Willie; Torralva, Ben; Yalisove, Steven; Phillips, Jamie

2018-04-01

The electrical properties of 4H-SiC under ultrafast laser irradiation in the low fluence regime (engineering spatially localized structural and electronic modification of wide bandgap materials such as 4H-SiC with relatively low surface damage via low temperature processing.

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

Energy Technology Data Exchange (ETDEWEB)

Wang, Xianjie; Zhao, Xiaofeng; Hu, Chang; Zhang, Yang; Song, Bingqian; Zhang, Lingli; Liu, Weilong; Lv, Zhe; Zhang, Yu; Sui, Yu, E-mail: suiyu@hit.edu.cn [Department of Physics, Harbin Institute of Technology, Harbin 150001 (China); Tang, Jinke [Department of Physics and Astronomy, University of Wyoming, Laramie, Wyoming 82071 (United States); Song, Bo, E-mail: songbo@hit.edu.cn [Department of Physics, Harbin Institute of Technology, Harbin 150001 (China); Academy of Fundamental and Interdisciplinary Sciences, Harbin Institute of Technology, Harbin 150001 (China)

2016-07-11

In this paper, we report a large lateral photovoltaic effect (LPE) with ultrafast relaxation time in SnSe/p-Si junctions. The LPE shows a linear dependence on the position of the laser spot, and the position sensitivity is as high as 250 mV mm{sup −1}. The optical response time and the relaxation time of the LPE are about 100 ns and 2 μs, respectively. The current-voltage curve on the surface of the SnSe film indicates the formation of an inversion layer at the SnSe/p-Si interface. Our results clearly suggest that most of the excited-electrons diffuse laterally in the inversion layer at the SnSe/p-Si interface, which results in a large LPE with ultrafast relaxation time. The high positional sensitivity and ultrafast relaxation time of the LPE make the SnSe/p-Si junction a promising candidate for a wide range of optoelectronic applications.

A spectroelectrochemical cell for ultrafast two-dimensional infrared spectroscopy

Energy Technology Data Exchange (ETDEWEB)

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

2015-08-15

A spectroelectrochemical cell has been designed to combine electrochemistry and ultrafast two-dimensional infrared (2D-IR) spectroscopy, which is a powerful tool to extract structure and dynamics information on the femtosecond to picosecond time scale. Our design is based on a gold mirror with the dual role of performing electrochemistry and reflecting IR light. To provide the high optical surface quality required for laser spectroscopy, the gold surface is made by electron beam evaporation on a glass substrate. Electrochemical cycling facilitates in situ collection of ultrafast dynamics of redox-active molecules by means of 2D-IR. The IR beams are operated in reflection mode so that they travel twice through the sample, i.e., the signal size is doubled. This methodology is optimal for small sample volumes and successfully tested with the ferricyanide/ferrocyanide redox system of which the corresponding electrochemically induced 2D-IR difference spectrum is reported.

A spectroelectrochemical cell for ultrafast two-dimensional infrared spectroscopy

International Nuclear Information System (INIS)

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

2015-01-01

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

Femtosecond laser studies of ultrafast intramolecular processes

Energy Technology Data Exchange (ETDEWEB)

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

1993-12-01

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

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

KAUST Repository

Eita, Mohamed Samir

2014-08-28

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

Ultrafast THz saturable absorption in doped semiconductors at room temperature

DEFF Research Database (Denmark)

Turchinovich, Dmitry; Hoffmann, M. V.

2011-01-01

Ultrafast Phenomena XVII presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultraf...

Facilitating the selection and creation of accurate interatomic potentials with robust tools and characterization

Science.gov (United States)

Trautt, Zachary T.; Tavazza, Francesca; Becker, Chandler A.

2015-10-01

The Materials Genome Initiative seeks to significantly decrease the cost and time of development and integration of new materials. Within the domain of atomistic simulations, several roadblocks stand in the way of reaching this goal. While the NIST Interatomic Potentials Repository hosts numerous interatomic potentials (force fields), researchers cannot immediately determine the best choice(s) for their use case. Researchers developing new potentials, specifically those in restricted environments, lack a comprehensive portfolio of efficient tools capable of calculating and archiving the properties of their potentials. This paper elucidates one solution to these problems, which uses Python-based scripts that are suitable for rapid property evaluation and human knowledge transfer. Calculation results are visible on the repository website, which reduces the time required to select an interatomic potential for a specific use case. Furthermore, property evaluation scripts are being integrated with modern platforms to improve discoverability and access of materials property data. To demonstrate these scripts and features, we will discuss the automation of stacking fault energy calculations and their application to additional elements. While the calculation methodology was developed previously, we are using it here as a case study in simulation automation and property calculations. We demonstrate how the use of Python scripts allows for rapid calculation in a more easily managed way where the calculations can be modified, and the results presented in user-friendly and concise ways. Additionally, the methods can be incorporated into other efforts, such as openKIM.

Facilitating the selection and creation of accurate interatomic potentials with robust tools and characterization

International Nuclear Information System (INIS)

Trautt, Zachary T; Tavazza, Francesca; Becker, Chandler A

2015-01-01

The Materials Genome Initiative seeks to significantly decrease the cost and time of development and integration of new materials. Within the domain of atomistic simulations, several roadblocks stand in the way of reaching this goal. While the NIST Interatomic Potentials Repository hosts numerous interatomic potentials (force fields), researchers cannot immediately determine the best choice(s) for their use case. Researchers developing new potentials, specifically those in restricted environments, lack a comprehensive portfolio of efficient tools capable of calculating and archiving the properties of their potentials. This paper elucidates one solution to these problems, which uses Python-based scripts that are suitable for rapid property evaluation and human knowledge transfer. Calculation results are visible on the repository website, which reduces the time required to select an interatomic potential for a specific use case. Furthermore, property evaluation scripts are being integrated with modern platforms to improve discoverability and access of materials property data. To demonstrate these scripts and features, we will discuss the automation of stacking fault energy calculations and their application to additional elements. While the calculation methodology was developed previously, we are using it here as a case study in simulation automation and property calculations. We demonstrate how the use of Python scripts allows for rapid calculation in a more easily managed way where the calculations can be modified, and the results presented in user-friendly and concise ways. Additionally, the methods can be incorporated into other efforts, such as openKIM. (paper)

Bayesian ensemble approach to error estimation of interatomic potentials

DEFF Research Database (Denmark)

Frederiksen, Søren Lund; Jacobsen, Karsten Wedel; Brown, K.S.

2004-01-01

Using a Bayesian approach a general method is developed to assess error bars on predictions made by models fitted to data. The error bars are estimated from fluctuations in ensembles of models sampling the model-parameter space with a probability density set by the minimum cost. The method...... is applied to the development of interatomic potentials for molybdenum using various potential forms and databases based on atomic forces. The calculated error bars on elastic constants, gamma-surface energies, structural energies, and dislocation properties are shown to provide realistic estimates...

Xenon Defects in Uranium Dioxide From First Principles and Interatomic Potentials

Science.gov (United States)

Thompson, Alexander

In this thesis, we examine the defect energetics and migration energies of xenon atoms in uranium dioxide (UO2) from first principles and interatomic potentials. We also parameterize new, accurate interatomic potentials for xenon and uranium dioxide. To achieve accurate energetics and provide a foundation for subsequent calculations, we address difficulties in finding consistent energetics within Hubbard U corrected density functional theory (DFT+U). We propose a method of slowly ramping the U parameter in order to guide the calculation into low energy orbital occupations. We find that this method is successful for a variety of materials. We then examine the defect energetics of several noble gas atoms in UO2 for several different defect sites. We show that the energy to incorporate large noble gas atoms into interstitial sites is so large that it is energetically favorable for a Schottky defect cluster to be created to relieve the strain. We find that, thermodynamically, xenon will rarely ever be in the interstitial site of UO2. To study larger defects associated with the migration of xenon in UO 2, we turn to interatomic potentials. We benchmark several previously published potentials against DFT+U defect energetics and migration barriers. Using a combination of molecular dynamics and nudged elastic band calculations, we find a new, low energy migration pathway for xenon in UO2. We create a new potential for xenon that yields accurate defect energetics. We fit this new potential with a method we call Iterative Potential Refinement that parameterizes potentials to first principles data via a genetic algorithm. The potential finds accurate energetics for defects with relatively low amounts of strain (xenon in defect clusters). It is important to find accurate energetics for these sorts of low-strain defects because they essentially represent small xenon bubbles. Finally, we parameterize a new UO2 potential that simultaneously yields accurate vibrational properties

Ultrafast characterization of optoelectronic devices and systems

Science.gov (United States)

Zheng, Xuemei

The recent fast growth in high-speed electronics and optoelectronics has placed demanding requirements on testing tools. Electro-optic (EO) sampling is a well-established technique for characterization of high-speed electronic and optoelectronic devices and circuits. However, with the progress in device miniaturization, lower power consumption (smaller signal), and higher throughput (higher clock rate), EO sampling also needs to be updated, accordingly, towards better signal-to-noise ratio (SNR) and sensitivity, without speed sacrifice. In this thesis, a novel EO sampler with a single-crystal organic 4-dimethylamino-N-methy-4-stilbazolium tosylate (DAST) as the EO sensor is developed. The system exhibits sub-picosecond temporal resolution, sub-millivolt sensitivity, and a 10-fold improvement on SNR, compared with its LiTaO3 counterpart. The success is attributed to the very high EO coefficient, the very low dielectric constant, and the fast response, coming from the major contribution of the pi-electrons in DAST. With the advance of ultrafast laser technology, low-noise and compact femtosecond fiber lasers have come to maturation and become light-source options for ultrafast metrology systems. We have successfully integrated a femtosecond erbium-doped-fiber laser into an EO sampler, making the system compact and very reliable. The fact that EO sampling is essentially an impulse-response measurement process, requires integration of ultrashort (sub-picosecond) impulse generation network with the device under test. We have implemented a reliable lift-off and transfer technique in order to obtain epitaxial-quality freestanding low-temperature-grown GaAs (LT-GaAs) thin-film photo-switches, which can be integrated with many substrates. The photoresponse of our freestanding LT-GaAs devices was thoroughly characterized with the help of our EO sampler. As fast as 360 fs full-width-at-half-maximum (FWHM) and >1 V electrical pulses were obtained, with quantum efficiency

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

Directory of Open Access Journals (Sweden)

Laurent P. René de Cotret

2017-07-01

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

Role of interatomic bonding in the mechanical anisotropy and interlayer cohesion of CSH crystals

Energy Technology Data Exchange (ETDEWEB)

Dharmawardhana, C.C. [Department of Physics and Astronomy, University of Missouri—Kansas City, Kansas City, MO 64110 (United States); Misra, A. [Department of Civil, Environmental, and Architectural Engineering, University of Kansas, Lawrence, KS 66045 (United States); Aryal, S.; Rulis, P. [Department of Physics and Astronomy, University of Missouri—Kansas City, Kansas City, MO 64110 (United States); Ching, W.Y., E-mail: ccdxz8@mail.umkc.edu [Department of Physics and Astronomy, University of Missouri—Kansas City, Kansas City, MO 64110 (United States)

2013-10-15

Atomic scale properties of calcium silicate hydrate (CSH), the main binding phase of hardened Portland cement, are not well understood. Over a century of intense research has identified almost 50 different crystalline CSH minerals which are mainly categorized by their Ca/Si ratio. The electronic structure and interatomic bonding in four major CSH crystalline phases with structures close to those found in hardened cement are investigated via ab initio methods. Our result reveals the critical role of hydrogen bonding and importance of specifying precise locations for water molecules. Quantitative analysis of contributions from different bond types to the overall cohesion shows that while the Si-O covalent bonds dominate, the hydrogen bonding and Ca-O bonding are also very significant. Calculated results reveal the correlation between bond topology and interlayer cohesion. The overall bond order density (BOD) is found to be a more critical measure than the Ca/Si ratio in classifying different CSH crystals.

PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

Science.gov (United States)

Kono, Junichiro

2013-02-01

Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton-phonon and exciton-plasmon interactions; exciton-exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz-Keldysh effects; and non-perturbative light-mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section, and the

Ultrafast laser spectroscopy in complex solid state materials

Energy Technology Data Exchange (ETDEWEB)

Li, Tianqi [Iowa State Univ., Ames, IA (United States)

2014-12-01

This thesis summarizes my work on applying the ultrafast laser spectroscopy to the complex solid state materials. It shows that the ultrafast laser pulse can coherently control the material properties in the femtosecond time scale. And the ultrafast laser spectroscopy can be employed as a dynamical method for revealing the fundamental physical problems in the complex material systems.

Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

Energy Technology Data Exchange (ETDEWEB)

Perlík, Václav; Seibt, Joachim; Šanda, František; Mančal, Tomáš [Institute of Physics, Faculty of Mathematics and Physics, Charles University in Prague, Ke Karlovu 5, Prague 121 16 (Czech Republic); Cranston, Laura J.; Cogdell, Richard J. [Institute of Molecular Cell and System Biology, College of Medical, Veterinary and Life Sciences, University of Glasgow, Glasgow Biomedical Research Centre, 120 University Place, Glasgow G12 8TA, Scotland (United Kingdom); Lincoln, Craig N.; Hauer, Jürgen, E-mail: juergen.hauer@tuwien.ac.at [Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, 1040 Vienna (Austria); Savolainen, Janne [Department of Physical Chemistry II, Ruhr-University Bochum, 44780 Bochum (Germany)

2015-06-07

The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system’s Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems.

Vibronic coupling explains the ultrafast carotenoid-to-bacteriochlorophyll energy transfer in natural and artificial light harvesters

International Nuclear Information System (INIS)

Perlík, Václav; Seibt, Joachim; Šanda, František; Mančal, Tomáš; Cranston, Laura J.; Cogdell, Richard J.; Lincoln, Craig N.; Hauer, Jürgen; Savolainen, Janne

2015-01-01

The initial energy transfer steps in photosynthesis occur on ultrafast timescales. We analyze the carotenoid to bacteriochlorophyll energy transfer in LH2 Marichromatium purpuratum as well as in an artificial light-harvesting dyad system by using transient grating and two-dimensional electronic spectroscopy with 10 fs time resolution. We find that Förster-type models reproduce the experimentally observed 60 fs transfer times, but overestimate coupling constants, which lead to a disagreement with both linear absorption and electronic 2D-spectra. We show that a vibronic model, which treats carotenoid vibrations on both electronic ground and excited states as part of the system’s Hamiltonian, reproduces all measured quantities. Importantly, the vibronic model presented here can explain the fast energy transfer rates with only moderate coupling constants, which are in agreement with structure based calculations. Counterintuitively, the vibrational levels on the carotenoid electronic ground state play the central role in the excited state population transfer to bacteriochlorophyll; resonance between the donor-acceptor energy gap and the vibrational ground state energies is the physical basis of the ultrafast energy transfer rates in these systems

Temporal behavior of hydrated electron studied up to 400 deg. C by ultrafast pulse radiolysis and Monte Carlo calculation

International Nuclear Information System (INIS)

Katsumura, Yosuke; Muroya, Yusa; Lin, Mingzhang; Yu, Yan; Mehran, Mostafavi; Sanguanmith, Sunuchakan; Meesungnoen, Jintana; Jay-Gerin, Jean-Paul

2012-09-01

Pulse radiolysis is a very powerful and unique method to observe the transient species and to determine their yields and has been widely used up to now. Since the radiation-induced reactions at elevated temperatures are accelerated, precise measurement becomes difficult by the conventional pulse radiolysis systems. Then, a higher time resolved pulse radiolysis system is highly expected. Recently, an ultrafast pulse radiolysis system has been developed in the University of Tokyo and applied to water radiolysis at elevated temperatures [1]. Temporal behavior of the hydrated electron at elevated temperatures up to 400 deg C has been detected. The time dependent behavior of hydrated electron at elevated temperatures were detected and the latest version of the Monte Carlo simulation code developed at University of Sherbrooke was applied to reproduce the experimental results. From the simulation, it was made clear that the thermalization distance becomes smaller with increasing temperature. In addition, in supercritical water, the initial yield is significantly dependent on density (pressure), which is consistent with our previous evaluation. (authors)

Development of an empirical interatomic potential for the Ag–Ti system

Energy Technology Data Exchange (ETDEWEB)

Zhou, Ying, E-mail: y.zhou3@lboro.ac.uk [Department of Mathematical Sciences, Loughborough University, Leicestershire LE11 3TU (United Kingdom); Smith, Roger [Department of Mathematical Sciences, Loughborough University, Leicestershire LE11 3TU (United Kingdom); Kenny, Steven D. [Department of Materials, Loughborough University, Leicestershire LE11 3TU (United Kingdom); Lloyd, Adam L. [Department of Mathematical Sciences, Loughborough University, Leicestershire LE11 3TU (United Kingdom)

2017-02-15

Highlights: • A new modified embedded-atom method interatomic potential for Ag and Ti was developed. • Binding energies for various configurations were calculated using SIESTA and were used as the fitting target. • Two mixing rules for the embedded-atom method based on the same elemental potentials were also investigated. • The results showed that the MEAM with the optimised parameters gives the best agreement to the DFT results. - Abstract: Two interatomic potential mixing rules for the Ti–Ag system were investigated based on the embedded-atom method (EAM) elemental potentials. First principles calculations were performed using SIESTA for various configurations of the Ti–Ag system to see which model best fitted the ab initio results. The results showed that the surface energies, especially that of Ti, were not well fitted by either model and the surface binding energies differed from the ab initio calculations. As a result, the modified embedded-atom method (MEAM) was investigated. In contrast to the other models, surface energies for pure Ti calculated by MEAM were in good agreement with the experimental data and the ab initio results. The MEAM mixing rule was used to investigate Ag ad-atoms on Ti and Ti ad-atoms on Ag. The results showed good agreement with SIESTA after parameter optimisation.

Earle K. Plyler Prize Lecture: The Three Pillars of Ultrafast Molecular Science - Time, Phase, Intensity

Science.gov (United States)

Stolow, Albert

We discuss the probing and control of molecular wavepacket dynamics in the context of three main `pillars' of light-matter interaction: time, phase, intensity. Time: Using short, coherent laser pulses and perturbative matter-field interactions, we study molecular wavepackets with a focus on the ultrafast non-Born-Oppenheimer dynamics, that is, the coupling of electronic and nuclear motions. Time-Resolved Photoelectron Spectroscopy (TRPES) is a powerful ultrafast probe of these processes in polyatomic molecules because it is sensitive both electronic and vibrational dynamics. Ideally, one would like to observe these ultrafast processes from the molecule's point of view - the Molecular Frame - thereby avoiding loss of information due to orientational averaging. This can be achieved by Time-Resolved Coincidence Imaging Spectroscopy (TRCIS) which images 3D recoil vectors of both photofragments and photoelectrons, in coincidence and as a function of time, permitting direct Molecular Frame imaging of valence electronic dynamics during a molecular dynamics. Phase: Using intermediate strength non-perturbative interactions, we apply the second order (polarizability) Non-Resonant Dynamic Stark Effect (NRDSE) to control molecular dynamics without any net absorption of light. NRDSE is also the interaction underlying molecular alignment and applies to field-free 1D of linear molecules and field-free 3D alignment of general (asymmetric) molecules. Using laser alignment, we can transiently fix a molecule in space, yielding a more general approach to direct Molecular Frame imaging of valence electronic dynamics during a chemical reaction. Intensity: In strong (ionizing) laser fields, a new laser-matter physics emerges for polyatomic systems wherein both the single active electron picture and the adiabatic electron response, both implicit in the standard 3-step models, can fail dramatically. This has important consequences for all attosecond strong field spectroscopies of

Free-electron laser driven by the LBNL laser-plasma accelerator

International Nuclear Information System (INIS)

Schroeder, C.B.; Fawley, W.M.; Gruner, F.; Bakeman, M.; Nakamura, K.; Robinson, K.E.; Toth, Cs.; Esarey, E.; Leemans, W.P.

2008-01-01

A design of a compact free-electron laser (FEL), generating ultra-fast, high-peak flux, XUV pulses is presented. The FEL is driven by ahigh-current, 0.5 GeV electron beam from the Lawrence Berkeley National Laboratory (LBNL) laser-plasma accelerator, whose active acceleration length is only a few centimeters. The proposed ultra-fast source (∼10 fs) would be intrinsically temporally synchronized to the drive laser pulse, enabling pump-probe studies in ultra-fast science. Owing to the high current (>10 kA) of the laser-plasma-accelerated electron beams, saturated output fluxes are potentially greater than 10 13 photons/pulse. Devices based both on self-amplified spontaneous emission and high-harmonic generated input seeds, to reduce undulator length and fluctuations, are considered.

Structural Transformation of LiFePO4 during Ultrafast Delithiation.

Science.gov (United States)

Kuss, Christian; Trinh, Ngoc Duc; Andjelic, Stefan; Saulnier, Mathieu; Dufresne, Eric M; Liang, Guoxian; Schougaard, Steen B

2017-12-21

The prolific lithium battery electrode material lithium iron phosphate (LiFePO 4 ) stores and releases lithium ions by undergoing a crystallographic phase change. Nevertheless, it performs unexpectedly well at high rate and exhibits good cycling stability. We investigate here the ultrafast charging reaction to resolve the underlying mechanism while avoiding the limitations of prevailing electrochemical methods by using a gaseous oxidant to deintercalate lithium from the LiFePO 4 structure. Oxidizing LiFePO 4 with nitrogen dioxide gas reveals structural changes through in situ synchrotron X-ray diffraction and electronic changes through in situ UV/vis reflectance spectroscopy. This study clearly shows that ultrahigh rates reaching 100% state of charge in 10 s does not lead to a particle-wide union of the olivine and heterosite structures. An extensive solid solution phase is therefore not a prerequisite for ultrafast charge/discharge.

On the doubly ionized states of Ar2 and their intra- and interatomic decay to Ar23+

International Nuclear Information System (INIS)

Stoychev, Spas D.; Kuleff, Alexander I.; Tarantelli, Francesco; Cederbaum, Lorenz S.

2008-01-01

Potential energy curves of the Auger state Ar + (2p -1 )-Ar, the different one- and two-site dicationic states Ar 2 ++ (with energies in the range of 32-77 eV), and the lowest two-site tricationic states Ar ++ -Ar + (with energies in the range of 64-76 eV) computed using elaborated ab initio methods are reported. The accessible relaxation channels of the electronic states of Ar ++ -Ar populated by Auger decay are studied. In particular, we study in detail the interatomic Coulombic decay following the population of one-site satellite states of Ar ++ (3s -1 3p -1 )-Ar recently observed experimentally. Other relaxation pathways of Ar ++ -Ar, including radiative charge transfer, nuclear dynamics through curve crossing, and intra-atomic decay processes are also investigated

Ultrafast lattice dynamics in photoexcited nanostructures. Femtosecond X-ray diffraction with optimized evaluation schemes

International Nuclear Information System (INIS)

Schick, Daniel

2013-01-01

Within the course of this thesis, I have investigated the complex interplay between electron and lattice dynamics in nanostructures of perovskite oxides. Femtosecond hard X-ray pulses were utilized to probe the evolution of atomic rearrangement directly, which is driven by ultrafast optical excitation of electrons. The physics of complex materials with a large number of degrees of freedom can be interpreted once the exact fingerprint of ultrafast lattice dynamics in time-resolved X-ray diffraction experiments for a simple model system is well known. The motion of atoms in a crystal can be probed directly and in real-time by femtosecond pulses of hard X-ray radiation in a pump-probe scheme. In order to provide such ultrashort X-ray pulses, I have built up a laser-driven plasma X-ray source. The setup was extended by a stable goniometer, a two-dimensional X-ray detector and a cryogen-free cryostat. The data acquisition routines of the diffractometer for these ultrafast X-ray diffraction experiments were further improved in terms of signal-to-noise ratio and angular resolution. The implementation of a high-speed reciprocal-space mapping technique allowed for a two-dimensional structural analysis with femtosecond temporal resolution. I have studied the ultrafast lattice dynamics, namely the excitation and propagation of coherent phonons, in photoexcited thin films and superlattice structures of the metallic perovskite SrRuO 3 . Due to the quasi-instantaneous coupling of the lattice to the optically excited electrons in this material a spatially and temporally well-defined thermal stress profile is generated in SrRuO 3 . This enables understanding the effect of the resulting coherent lattice dynamics in time-resolved X-ray diffraction data in great detail, e.g. the appearance of a transient Bragg peak splitting in both thin films and superlattice structures of SrRuO 3 . In addition, a comprehensive simulation toolbox to calculate the ultrafast lattice dynamics and the

Parameterization of interatomic potential by genetic algorithms: A case study

Energy Technology Data Exchange (ETDEWEB)

Ghosh, Partha S., E-mail: psghosh@barc.gov.in; Arya, A.; Dey, G. K. [Materials Science Division, Bhabha Atomic Research Centre, Mumbai-400085 (India); Ranawat, Y. S. [Department of Ceramic Engineering, Indian Institute of Technology (BHU), Varanasi-221005 (India)

2015-06-24

A framework for Genetic Algorithm based methodology is developed to systematically obtain and optimize parameters for interatomic force field functions for MD simulations by fitting to a reference data base. This methodology is applied to the fitting of ThO{sub 2} (CaF{sub 2} prototype) – a representative of ceramic based potential fuel for nuclear applications. The resulting GA optimized parameterization of ThO{sub 2} is able to capture basic structural, mechanical, thermo-physical properties and also describes defect structures within the permissible range.

Ultrafast magnon generation in an Fe film on Cu(100).

Science.gov (United States)

Schmidt, A B; Pickel, M; Donath, M; Buczek, P; Ernst, A; Zhukov, V P; Echenique, P M; Sandratskii, L M; Chulkov, E V; Weinelt, M

2010-11-05

We report on a combined experimental and theoretical study of the spin-dependent relaxation processes in the electron system of an iron film on Cu(100). Spin-, time-, energy- and angle-resolved two-photon photoemission shows a strong characteristic dependence of the lifetime of photoexcited electrons on their spin and energy. Ab initio calculations as well as a many-body treatment corroborate that the observed properties are determined by relaxation processes involving magnon emission. Thereby we demonstrate that magnon emission by hot electrons occurs on the femtosecond time scale and thus provides a significant source of ultrafast spin-flip processes. Furthermore, engineering of the magnon spectrum paves the way for tuning the dynamic properties of magnetic materials.

Ultrafast photoconductor detector-laser-diode transmitter

International Nuclear Information System (INIS)

Wang, C.L.; Davis, B.A.; Davies, T.J.; Nelson, M.A.; Thomas, M.C.; Zagarino, P.A.

1987-01-01

We report the results of an experiment in which we used an ultrafast, photoconductive, radiation detector to drive a fast laser-diode transmitter. When we irradiated the neutron-damaged Cr-doped GaAs detector with 17-MeV electron beams, the temporal response was measured to be less than 30 ps. The pulses from this detector modulated a fast GaAlAs laser diode to transmit the laser output through 30- and 1100-m optical fibers. Preliminary results indicate that 50- and 80-ps time resolutions, respectively, are obtainable with these fibers. We are now working to integrate the photoconductive detector and the laser diode transmitter into a single chip

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

International Nuclear Information System (INIS)

Gu Zhiguo; Yang Shuping; Li Zaijun; Sun Xiulan; Wang Guangli; Fang Yinjun; Liu Junkang

2011-01-01

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

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

Energy Technology Data Exchange (ETDEWEB)

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

2011-10-30

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

Low-order moment expansions to tight binding for interatomic potentials: Successes and failures

International Nuclear Information System (INIS)

Kress, J.D.; Voter, A.F.

1995-01-01

We discuss the use of moment-based approximations to tight binding. Using a maximum entropy form for the electronic density of states, we show that a general interatomic potential can be defined that is suitable for molecular-dynamics simulations and has several other desirable features. For covalent materials (C and Si), properties where the atoms are in equivalent environments are well converged at low-order moments. For defect environments, which offer a more critical (and relevant) test, the method is found to give less satisfactory results. For example, the vacancy formation energy for Si is too low by ∼2 eV at 10 moments relative to exact tight binding. Attempts to improve the accuracy were unsuccessful, leading to the conclusion that potentials based on this approach are inadequate for covalent materials. We speculate that this may be a deficiency of low-order moment methods in general. For metals, in contrast to the covalent systems, we find that the low-order moment approach is better behaved. This finding is consistent with the success of existing empirical fourth-moment potentials for metals

Ultrafast strain engineering in complex oxide heterostructures

Energy Technology Data Exchange (ETDEWEB)

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

2012-07-01

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

Ultrafast dynamics during the photoinduced phase transition in VO2

Science.gov (United States)

Wegkamp, Daniel; Stähler, Julia

2015-12-01

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

Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements.

Science.gov (United States)

Heilpern, Tal; Manjare, Manoj; Govorov, Alexander O; Wiederrecht, Gary P; Gray, Stephen K; Harutyunyan, Hayk

2018-05-10

Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions about the functional form of the initial energy distribution or using indirect sensors like localized plasmon frequency shifts. Here we directly determine non-thermal and thermal distributions and dynamics in thin films by applying a double inversion procedure to optical pump-probe data that relates the reflectivity changes around Fermi energy to the changes in the dielectric function and in the single-electron energy band occupancies. When applied to normal incidence measurements our method uncovers the ultrafast excitation of a non-Fermi-Dirac distribution and its subsequent thermalization dynamics. Furthermore, when applied to the Kretschmann configuration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.

First principles calculations of structural, electronic and thermal ...

Indian Academy of Sciences (India)

Administrator

2013-07-28

Jul 28, 2013 ... The structural, electronic and thermal properties of lead chalcogenides PbS, PbSe and BeTe using .... results for all the systems are presented in table 1, along ... as interatomic bonding, equations of state and phonon spectra.

Ultrafast Time-Resolved Photoluminescence Studies of Gallium-Arsenide

Science.gov (United States)

Johnson, Matthew Bruce

This thesis concerns the study of ultrafast phenomena in GaAs using time-resolved photoluminescence (PL). The thesis consists of five chapters. Chapter one is an introduction, which discusses the study of ultrafast phenomena in semiconductors. Chapter two is a description of the colliding-pulse mode-locked (CPM) ring dye laser, which is at the heart of the experimental apparatus used in this thesis. Chapter three presents a detailed experimental and theoretical investigation of photoluminescence excitation correlation spectroscopy (PECS), the novel technique which is used to time-resolve ultrafast PL phenomena. Chapters 4 and 5 discuss two applications of the PECS technique. In Chapter 4 the variation of PL intensity in In-alloyed GaAs substrate material is studied, while Chapter 5 discusses the variation of carrier lifetimes in ion-damaged GaAs used in photo-conductive circuit elements (PCEs). PECS is a pulse-probe technique that measures the cross correlation of photo-excited carrier populations. The theoretical model employed in this thesis is based upon the rate equation for a simple three-level system consisting of valence and conduction bands and a single trap level. In the limit of radiative band-to-band dominated recombination, no PECS signal should be observed; while in the capture -dominated recombination limit, the PECS signal from the band-to-band PL measures the cross correlation of the excited electron and hole populations and thus, the electron and hole lifetimes. PECS is experimentally investigated using a case study of PL in semi-insulating (SI) GaAs and In -alloyed GaAs. At 77 K, the PECS signal is characteristic of a capture-dominated system, yielding an electron-hole lifetime of about 200 ps. However, at 5 K the behavior is more complicated and shows saturation effects due to the C acceptor level, which is un-ionized at 5 K. As a first application, PECS is used to investigate the large band-to-band PL contrast observed near dislocations in In

Ultrafast stimulated Raman spectroscopy in the near-infrared region

International Nuclear Information System (INIS)

Takaya, Tomohisa

2016-01-01

A number of electronic transitions in the near-infrared wavelength region are associated with migration or delocalization of electrons in large molecules or molecular systems. Time-resolved near-infrared Raman spectroscopy will be a powerful tool for investigating the structural dynamic of samples with delocalized electrons. However, the sensitivity of near-infrared spontaneous Raman spectrometers is significantly low due to an extremely small probability of Raman scattering and a low sensitivity of near-infrared detectors. Nonlinear Raman spectroscopy is one of the techniques that can overcome the sensitivity problems and enable us to obtain time-resolved Raman spectra in resonance with near-IR transitions. In this article, the author introduces recent progress of ultrafast time-resolved near-infrared stimulated Raman spectroscopy. Optical setup, spectral and temporal resolution, and applications of the spectrometer are described. (author)

Scattering of thermal He beams by crossed atomic and molecular beams. I. Sensitivity of the elastic differential cross section to the interatomic potential

International Nuclear Information System (INIS)

Keil, M.; Kuppermann, A.

1978-01-01

The ability of diffraction oscillations in atomic beam scattering experiments to uniquely determine interatomic potentials for highly quantal systems is examined. Assumed but realistic potentials are used to generate, by scattering calculations and incorporation of random errors, differential cross sections which are then treated as if they were ''experimental'' data. From these, attempts are made to recover the initial potential by varying the parameters of assumed mathematical forms different from the original one, until a best fit to the ''experimental'' results is obtained. It is found that the region of the interaction potential around the van der Waals minimum is accurately determined by the ''measured'' differential cross sections over a range of interatomic separations significantly wider than would be expected classically. It is also found, for collision energies at which the weakly repulsive wall is appreciably sampled, that the SPF--Dunham and double Morse--van der Waals types of potentials lead to accurate determinations of the interatomic potential, whereas many other mathematical forms do not. Analytical parameterizations most appropriate for obtaining accurate interatomic potentials from thermal DCS experiments, for a given highly quantal system, may depend on the collision energy used

Eutectic composite NiAl-Cr properties modeling based on interatomic interaction forces

Science.gov (United States)

Badamshin, I. Kh

2018-03-01

For new materials, information on the elasticity and strength characteristics necessary for calculating the stress-strain state of the turbine blades is limited. In these conditions, there is a need for theoretical methods for calculating the elastic and strength characteristics. The proposed theoretical methods are based on forces of interatomic interaction calculation. The classical methods based on the hypothesis of continuity do not allow calculating the material strength and thermophysical properties.

Ultrafast atomic-scale visualization of acoustic phonons generated by optically excited quantum dots

Directory of Open Access Journals (Sweden)

Giovanni M. Vanacore

2017-07-01

Full Text Available Understanding the dynamics of atomic vibrations confined in quasi-zero dimensional systems is crucial from both a fundamental point-of-view and a technological perspective. Using ultrafast electron diffraction, we monitored the lattice dynamics of GaAs quantum dots—grown by Droplet Epitaxy on AlGaAs—with sub-picosecond and sub-picometer resolutions. An ultrafast laser pulse nearly resonantly excites a confined exciton, which efficiently couples to high-energy acoustic phonons through the deformation potential mechanism. The transient behavior of the measured diffraction pattern reveals the nonequilibrium phonon dynamics both within the dots and in the region surrounding them. The experimental results are interpreted within the theoretical framework of a non-Markovian decoherence, according to which the optical excitation creates a localized polaron within the dot and a travelling phonon wavepacket that leaves the dot at the speed of sound. These findings indicate that integration of a phononic emitter in opto-electronic devices based on quantum dots for controlled communication processes can be fundamentally feasible.

Laser selective cutting of biological tissues by impulsive heat deposition through ultrafast vibrational excitations.

Science.gov (United States)

Franjic, Kresimir; Cowan, Michael L; Kraemer, Darren; Miller, R J Dwayne

2009-12-07

Mechanical and thermodynamic responses of biomaterials after impulsive heat deposition through vibrational excitations (IHDVE) are investigated and discussed. Specifically, we demonstrate highly efficient ablation of healthy tooth enamel using 55 ps infrared laser pulses tuned to the vibrational transition of interstitial water and hydroxyapatite around 2.95 microm. The peak intensity at 13 GW/cm(2) was well below the plasma generation threshold and the applied fluence 0.75 J/cm(2) was significantly smaller than the typical ablation thresholds observed with nanosecond and microsecond pulses from Er:YAG lasers operating at the same wavelength. The ablation was performed without adding any superficial water layer at the enamel surface. The total energy deposited per ablated volume was several times smaller than previously reported for non-resonant ultrafast plasma driven ablation with similar pulse durations. No micro-cracking of the ablated surface was observed with a scanning electron microscope. The highly efficient ablation is attributed to an enhanced photomechanical effect due to ultrafast vibrational relaxation into heat and the scattering of powerful ultrafast acoustic transients with random phases off the mesoscopic heterogeneous tissue structures.

Ultrafast probing of core hole localization in N2.

Science.gov (United States)

Schöffler, M S; Titze, J; Petridis, N; Jahnke, T; Cole, K; Schmidt, L Ph H; Czasch, A; Akoury, D; Jagutzki, O; Williams, J B; Cherepkov, N A; Semenov, S K; McCurdy, C W; Rescigno, T N; Cocke, C L; Osipov, T; Lee, S; Prior, M H; Belkacem, A; Landers, A L; Schmidt-Böcking, H; Weber, Th; Dörner, R

2008-05-16

Although valence electrons are clearly delocalized in molecular bonding frameworks, chemists and physicists have long debated the question of whether the core vacancy created in a homonuclear diatomic molecule by absorption of a single x-ray photon is localized on one atom or delocalized over both. We have been able to clarify this question with an experiment that uses Auger electron angular emission patterns from molecular nitrogen after inner-shell ionization as an ultrafast probe of hole localization. The experiment, along with the accompanying theory, shows that observation of symmetry breaking (localization) or preservation (delocalization) depends on how the quantum entangled Bell state created by Auger decay is detected by the measurement.

Coulomb-Driven Relativistic Electron Beam Compression.

Science.gov (United States)

Lu, Chao; Jiang, Tao; Liu, Shengguang; Wang, Rui; Zhao, Lingrong; Zhu, Pengfei; Xiang, Dao; Zhang, Jie

2018-01-26

Coulomb interaction between charged particles is a well-known phenomenon in many areas of research. In general, the Coulomb repulsion force broadens the pulse width of an electron bunch and limits the temporal resolution of many scientific facilities such as ultrafast electron diffraction and x-ray free-electron lasers. Here we demonstrate a scheme that actually makes use of the Coulomb force to compress a relativistic electron beam. Furthermore, we show that the Coulomb-driven bunch compression process does not introduce additional timing jitter, which is in sharp contrast to the conventional radio-frequency buncher technique. Our work not only leads to enhanced temporal resolution in electron-beam-based ultrafast instruments that may provide new opportunities in probing material systems far from equilibrium, but also opens a promising direction for advanced beam manipulation through self-field interactions.

Coulomb-Driven Relativistic Electron Beam Compression

Science.gov (United States)

Lu, Chao; Jiang, Tao; Liu, Shengguang; Wang, Rui; Zhao, Lingrong; Zhu, Pengfei; Xiang, Dao; Zhang, Jie

2018-01-01

Coulomb interaction between charged particles is a well-known phenomenon in many areas of research. In general, the Coulomb repulsion force broadens the pulse width of an electron bunch and limits the temporal resolution of many scientific facilities such as ultrafast electron diffraction and x-ray free-electron lasers. Here we demonstrate a scheme that actually makes use of the Coulomb force to compress a relativistic electron beam. Furthermore, we show that the Coulomb-driven bunch compression process does not introduce additional timing jitter, which is in sharp contrast to the conventional radio-frequency buncher technique. Our work not only leads to enhanced temporal resolution in electron-beam-based ultrafast instruments that may provide new opportunities in probing material systems far from equilibrium, but also opens a promising direction for advanced beam manipulation through self-field interactions.

Ultrafast photoconductive detector-laser-diode transmitter

International Nuclear Information System (INIS)

Wang, C.L.; Davies, T.J.; Nelson, M.A.; Thomas, M.C.; Zagarino, P.A.; Davis, B.A.

1987-01-01

The authors report the results of an experiment in which they used an ultrafast, photoconductive, radiation detector to drive a fast laser-diode transmitter. When they irradiated the neutron-damaged Cr-doped Ga/As detector with 17-MeV electron beams, the temporal response of was measured to be less than 30 ps. The pulses from this detector modulated a fast GaAlAs laser diode to transmit the laser output through 30- and 1100-m optical fibers. Preliminary results indicate that 50- and 80-ps time resolutions, respectively, are obtainable with these fibers. They are now working to integrate the photoconductive detector and the laser diode transmitter into a single chip

Ultrafast generation of pseudo-magnetic field for valley excitons in WSe2 monolayers

KAUST Repository

Kim, J.

2014-12-04

The valley pseudospin is a degree of freedom that emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2). The capability to manipulate it, in analogy to the control of spin in spintronics, can open up exciting opportunities. Here, we demonstrate that an ultrafast and ultrahigh valley pseudo-magnetic field can be generated by using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Using ultrafast pump-probe spectroscopy, we observed a pure and valley-selective optical Stark effect in WSe2 monolayers from the nonresonant pump, resulting in an energy splitting of more than 10 milli-electron volts between the K and K′ valley exciton transitions. Our study opens up the possibility to coherently manipulate the valley polarization for quantum information applications.

Ultrafast generation of pseudo-magnetic field for valley excitons in WSe2 monolayers

KAUST Repository

Kim, J.; Hong, X.; Jin, C.; Shi, S.-F.; Chang, C.-Y. S.; Chiu, Ming-Hui; Li, Lain-Jong; Wang, F.

2014-01-01

The valley pseudospin is a degree of freedom that emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2). The capability to manipulate it, in analogy to the control of spin in spintronics, can open up exciting opportunities. Here, we demonstrate that an ultrafast and ultrahigh valley pseudo-magnetic field can be generated by using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Using ultrafast pump-probe spectroscopy, we observed a pure and valley-selective optical Stark effect in WSe2 monolayers from the nonresonant pump, resulting in an energy splitting of more than 10 milli-electron volts between the K and K′ valley exciton transitions. Our study opens up the possibility to coherently manipulate the valley polarization for quantum information applications.

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

International Nuclear Information System (INIS)

Fotakis, C; Zorba, V; Stratakis, E; Athanassiou, A; Tzanetakis, P; Zergioti, I; Papagoglou, D G; Sambani, K; Filippidis, G; Farsari, M; Pouli, V; Bounos, G; Georgiou, S

2007-01-01

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

Interatomic forces and bonding mechanisms in MgO clusters

International Nuclear Information System (INIS)

Wright, N.F.; Painter, G.S.

1990-01-01

We report results from a first-principles local spin density quantum mechanical study of the energetics and elastic properties of a series of magnesium-oxygen clusters of various morphologies. The role of quantum effects, e.g. covalency, in the bonding character of diatomic MgO is determined by comparison of classical and quantum restoring force curves. The dependence of binding properties on geometry and metal to oxygen ratio is determined by comparison of binding energy curves for a series of clusters. Results show that while gross features of the binding curves may be represented by simple interatomic potentials, details require the many body corrections of a full quantum treatment. 6 refs., 5 figs

Impact of local order and stoichiometry on the ultrafast magnetization dynamics of Heusler compounds

International Nuclear Information System (INIS)

Steil, Daniel; Schmitt, Oliver; Fetzer, Roman; Aeschlimann, Martin; Cinchetti, Mirko; Kubota, Takahide; Naganuma, Hiroshi; Oogane, Mikihiko; Ando, Yasuo; Rodan, Steven; Blum, Christian G F; Wurmehl, Sabine; Balke, Benjamin

2015-01-01

Nowadays, a wealth of information on ultrafast magnetization dynamics of thin ferromagnetic films exists in the literature. Information is, however, scarce on bulk single crystals, which may be especially important for the case of multi-sublattice systems. In Heusler compounds, representing prominent examples for such multi-sublattice systems, off-stoichiometry and degree of order can significantly change the magnetic properties of thin films, while bulk single crystals may be generally produced with a much more well-defined stoichiometry and a higher degree of ordering. A careful characterization of the local structure of thin films versus bulk single crystals combined with ultrafast demagnetization studies can, thus, help to understand the impact of stoichiometry and order on ultrafast spin dynamics.Here, we present a comparative study of the structural ordering and magnetization dynamics for thin films and bulk single crystals of the family of Heusler alloys with composition Co 2 Fe 1 − x Mn x Si. The local ordering is studied by 59 Co nuclear magnetic resonance (NMR) spectroscopy, while the time-resolved magneto-optical Kerr effect gives access to the ultrafast magnetization dynamics. In the NMR studies we find significant differences between bulk single crystals and thin films, both regarding local ordering and stoichiometry. The ultrafast magnetization dynamics, on the other hand, turns out to be mostly unaffected by the observed structural differences, especially on the time scale of some hundreds of femtoseconds. These results confirm hole-mediated spin-flip processes as the main mechanism for ultrafast demagnetization and the robustness of this demagnetization channel against defect states in the minority band gap as well as against the energetic position of the band gap with respect to the Fermi energy. The very small differences observed in the magnetization dynamics on the picosecond time-scale, on the other hand, can be explained by considering the

Characterization of Nanostructured Semiconductors by Ultrafast Luminescence Imaging

Science.gov (United States)

Blake, Jolie

Single nanostructures are predicted to be the building blocks of next generation devices and have already been incorporated into prototypes for solar cells, biomedical devices and lasers. Their role in such applications requires a fundamental understanding of their opto-electronic properties and in particular the charge carrier dynamics occurring on an ultrafast timescale. Luminescence detection is a common approach used to investigate electronic properties of nanostructures because of the contact-less nature of these methods. They are, however, often not equipped to efficiently measure multiple single nanostructures nor do they have the temporal resolution necessary for observing femtosecond dynamics. This dissertation intends to address this paucity of techniques available for the contact-less measurement of single nanostructures through the development of an ultrafast wide-field Kerr-gated microscope system and measurement technique. The setup, operational in both the steady state and transient mode and capable of microscopic and spectroscopic measurements, was developed to measure the transient luminescence of single semiconductor nanostructures. With sub micron spatial resolution and the potential to achieve a temporal resolution greater than 90 fs, the system was used to probe the charge carrier dynamics at multiple discrete locations on single nanowires exhibiting amplified spontaneous emission. Using a rate model for amplified spontaneous emission, the transient emission data was fitted to extract the values of the competing Shockley-Read-Hall, non-geminate and Auger recombination constants. The capabilities of the setup were first demonstrated in the visible detection range, where single nanowires of the ternary alloy CdS x Se1-x were measured. The temporal emission dynamics at two separate locations were compared and calculation of the Langevin mobility revealed that the large carrier densities generated in the nanowire allows access to non

Progress in ultrafast laser processing and future prospects

Science.gov (United States)

Sugioka, Koji

2017-03-01

The unique characteristics of ultrafast lasers have rapidly revolutionized materials processing after their first demonstration in 1987. The ultrashort pulse width of the laser suppresses heat diffusion to the surroundings of the processed region, which minimizes the formation of a heat-affected zone and thereby enables ultrahigh precision micro- and nanofabrication of various materials. In addition, the extremely high peak intensity can induce nonlinear multiphoton absorption, which extends the diversity of materials that can be processed to transparent materials such as glass. Nonlinear multiphoton absorption enables three-dimensional (3D) micro- and nanofabrication by irradiation with tightly focused femtosecond laser pulses inside transparent materials. Thus, ultrafast lasers are currently widely used for both fundamental research and practical applications. This review presents progress in ultrafast laser processing, including micromachining, surface micro- and nanostructuring, nanoablation, and 3D and volume processing. Advanced technologies that promise to enhance the performance of ultrafast laser processing, such as hybrid additive and subtractive processing, and shaped beam processing are discussed. Commercial and industrial applications of ultrafast laser processing are also introduced. Finally, future prospects of the technology are given with a summary.

Design of a free-electron laser driven by the LBNL laser-plasma-accelerator

International Nuclear Information System (INIS)

Schroeder, C.B.; Fawley, W.M.; Montgomery, A.L.; Robinson, K.E.; Gruner, F.; Bakeman, M.; Leemans, W.P.

2007-01-01

We discuss the design and current status of a compact free-electron laser (FEL), generating ultra-fast, high-peak flux, VUV pulses driven by a high-current, GeV electron beam from the existing Lawrence Berkeley National Laboratory (LBNL) laser-plasma accelerator, whose active acceleration length is only a few cm. The proposed ultra-fast source would be intrinsically temporally synchronized to the drive laser pulse, enabling pump-probe studies in ultra-fast science with pulse lengths of tens of fs. Owing to the high current ( and 10 kA) of the laser-plasma-accelerated electron beams, saturated output fluxes are potentially greater than 1013 photons/pulse. Devices based both on SASE and high-harmonic generated input seeds, to reduce undulator length and fluctuations, are considered

Ultrafast secondary emission x-ray imaging detectors

International Nuclear Information System (INIS)

Akkerman, A.; Gibrekhterman, A.; Majewski, S.

1991-07-01

Fast high accuracy, x-ray imaging at high photon flux can be achieved when coupling thin solid convertors to gaseous electron multipliers, operating at low gas pressures. Secondary electron emitted from the convertor foil are multiplied in several successive amplification elements. The obvious advantage of solid x-ray detectors, as compared to gaseous conversion, are the production of parallax-free images and the fast (subnanoseconds) response. These x-ray detectors have many potential applications in basic and applied research. Of particular interest is the possibility of an efficient and ultrafast high resolution imaging of transition radiation,with a reduced dE/dx background. We present experimental results on the operation of the secondary emission x-ray (SEX) detectors, their detection efficiency, localization and time resolution. The experimental work is accompanied by mathematical modelling and computer simulation of transition radiation detectors based on CsI transition radiation convertors. (author)

Modified embedded-atom method interatomic potential for the Fe-Al system

International Nuclear Information System (INIS)

Lee, Eunkoo; Lee, Byeong-Joo

2010-01-01

An interatomic potential for the Fe-Al binary system has been developed based on the modified embedded-atom method (MEAM) potential formalism. The potential can describe various fundamental physical properties of Fe-Al binary alloys-structural, elastic and thermodynamic properties, defect formation behavior and interactions between defects-in reasonable agreement with experimental data or higher-level calculations. The applicability of the potential to atomistic investigations of various defect formation behaviors and their effects on the mechanical properties of high aluminum steels as well as Fe-Al binary alloys is demonstrated.

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

KAUST Repository

Kar, Prasenjit; Sardar, Samim; Alarousu, Erkki; Sun, Jingya; Seddigi, Zaki Shakir Abdullah; Ahmed, Saleh Abdel Mgeed; Danish, Ekram Yousif; Mohammed, Omar F.; Pal, Samir Kumar

2014-01-01

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

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

KAUST Repository

Kar, Prasenjit

2014-07-10

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

High Harmonic Generation XUV Spectroscopy for Studying Ultrafast Photophysics of Coordination Complexes

Science.gov (United States)

Ryland, Elizabeth S.; Lin, Ming-Fu; Benke, Kristin; Verkamp, Max A.; Zhang, Kaili; Vura-Weis, Josh

2017-06-01

Extreme ultraviolet (XUV) spectroscopy is an inner shell technique that probes the M_{2,3}-edge excitation of atoms. Absorption of the XUV photon causes a 3p→3d transition, the energy and shape of which is directly related to the element and ligand environment. This technique is thus element-, oxidation state-, spin state-, and ligand field specific. A process called high-harmonic generation (HHG) enables the production of ultrashort (˜20fs) pulses of collimated XUV photons in a tabletop instrument. This allows transient XUV spectroscopy to be conducted as an in-lab experiment, where it was previously only possible at accelerator-based light sources. Additionally, ultrashort pulses provide the capability for unprecedented time resolution (˜50fs IRF). This technique has the capacity to serve a pivotal role in the study of electron and energy transfer processes in materials and chemical biology. I will present the XUV transient absorption instrument we have built, along with ultrafast transient M_{2,3}-edge absorption data of a series of small inorganic molecules in order to demonstrate the high specificity and time resolution of this tabletop technique as well as how our group is applying it to the study of ultrafast electronic dynamics of coordination complexes.

Roadmap of ultrafast x-ray atomic and molecular physics

Science.gov (United States)

Young, Linda; Ueda, Kiyoshi; Gühr, Markus; Bucksbaum, Philip H.; Simon, Marc; Mukamel, Shaul; Rohringer, Nina; Prince, Kevin C.; Masciovecchio, Claudio; Meyer, Michael; Rudenko, Artem; Rolles, Daniel; Bostedt, Christoph; Fuchs, Matthias; Reis, David A.; Santra, Robin; Kapteyn, Henry; Murnane, Margaret; Ibrahim, Heide; Légaré, François; Vrakking, Marc; Isinger, Marcus; Kroon, David; Gisselbrecht, Mathieu; L'Huillier, Anne; Wörner, Hans Jakob; Leone, Stephen R.

2018-02-01

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ˜1 Ångstrom, and HHG provides unprecedented time resolution (˜50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ˜280 eV (44 Ångstroms) and the bond length in methane of ˜1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since

VoroMQA: Assessment of protein structure quality using interatomic contact areas.

Science.gov (United States)

Olechnovič, Kliment; Venclovas, Česlovas

2017-06-01

In the absence of experimentally determined protein structure many biological questions can be addressed using computational structural models. However, the utility of protein structural models depends on their quality. Therefore, the estimation of the quality of predicted structures is an important problem. One of the approaches to this problem is the use of knowledge-based statistical potentials. Such methods typically rely on the statistics of distances and angles of residue-residue or atom-atom interactions collected from experimentally determined structures. Here, we present VoroMQA (Voronoi tessellation-based Model Quality Assessment), a new method for the estimation of protein structure quality. Our method combines the idea of statistical potentials with the use of interatomic contact areas instead of distances. Contact areas, derived using Voronoi tessellation of protein structure, are used to describe and seamlessly integrate both explicit interactions between protein atoms and implicit interactions of protein atoms with solvent. VoroMQA produces scores at atomic, residue, and global levels, all in the fixed range from 0 to 1. The method was tested on the CASP data and compared to several other single-model quality assessment methods. VoroMQA showed strong performance in the recognition of the native structure and in the structural model selection tests, thus demonstrating the efficacy of interatomic contact areas in estimating protein structure quality. The software implementation of VoroMQA is freely available as a standalone application and as a web server at http://bioinformatics.lt/software/voromqa. Proteins 2017; 85:1131-1145. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Ultrafast Synaptic Events in a Chalcogenide Memristor

Science.gov (United States)

Li, Yi; Zhong, Yingpeng; Xu, Lei; Zhang, Jinjian; Xu, Xiaohua; Sun, Huajun; Miao, Xiangshui

2013-04-01

Compact and power-efficient plastic electronic synapses are of fundamental importance to overcoming the bottlenecks of developing a neuromorphic chip. Memristor is a strong contender among the various electronic synapses in existence today. However, the speeds of synaptic events are relatively slow in most attempts at emulating synapses due to the material-related mechanism. Here we revealed the intrinsic memristance of stoichiometric crystalline Ge2Sb2Te5 that originates from the charge trapping and releasing by the defects. The device resistance states, representing synaptic weights, were precisely modulated by 30 ns potentiating/depressing electrical pulses. We demonstrated four spike-timing-dependent plasticity (STDP) forms by applying programmed pre- and postsynaptic spiking pulse pairs in different time windows ranging from 50 ms down to 500 ns, the latter of which is 105 times faster than the speed of STDP in human brain. This study provides new opportunities for building ultrafast neuromorphic computing systems and surpassing Von Neumann architecture.

Zeroth-order exchange energy as a criterion for optimized atomic basis sets in interatomic force calculations

International Nuclear Information System (INIS)

Varandas, A.J.C.

1980-01-01

A suggestion is made for using the zeroth-order exchange term, at the one-exchange level, in the perturbation development of the interaction energy as a criterion for optmizing the atomic basis sets in interatomic force calculations. The approach is illustrated for the case of two helium atoms. (orig.)

Ultra-fast dynamics in the nonlinear optical response of silver nanoprism ordered arrays.

Science.gov (United States)

Sánchez-Esquivel, Héctor; Raygoza-Sanchez, Karen Y; Rangel-Rojo, Raúl; Kalinic, Boris; Michieli, Niccolò; Cesca, Tiziana; Mattei, Giovanni

2018-03-15

In this work we present the study of the ultra-fast dynamics of the nonlinear optical response of a honeycomb array of silver triangular nanoprisms, performed using a femtosecond pulsed laser tuned with the dipolar surface plasmon resonance of the nanoarray. Nonlinear absorption and refraction, and their time-dependence, were explored using the z-scan and time-resolved excite-probe techniques. Nonlinear absorption is shown to change sign with the input irradiance and the behavior was explained on the basis of a three-level model. The response time was determined to be in the picosecond regime. A technique based on a variable frequency chopper was also used in order to discriminate the thermal and electronic contributions to the nonlinearity, which were found to have opposite signs. All these findings propel the investigated nanoprism arrays as good candidates for applications in advanced ultra-fast nonlinear nanophotonic devices.

Time resolved 3D momentum imaging of ultrafast dynamics by coherent VUV-XUV radiation

Energy Technology Data Exchange (ETDEWEB)

Sturm, F. P., E-mail: fpsturm@lbl.gov [Ultrafast X-Ray Science Lab, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); Institut für Kernphysik, Universität Frankfurt, Max-von-Laue Str. 1, D-60438 Frankfurt (Germany); Wright, T. W.; Ray, D.; Zalyubovskaya, I.; Shivaram, N.; Slaughter, D. S.; Belkacem, A.; Weber, Th. [Ultrafast X-Ray Science Lab, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); Ranitovic, P. [Ultrafast X-Ray Science Lab, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); ELI-ALPS, ELI-Hu Nkft, Dugonics ter 13, Szeged H6720 (Hungary)

2016-06-15

We present a new experimental setup for measuring ultrafast nuclear and electron dynamics of molecules after photo-excitation and ionization. We combine a high flux femtosecond vacuum ultraviolet (VUV) and extreme ultraviolet (XUV) source with an internally cold molecular beam and a 3D momentum imaging particle spectrometer to measure electrons and ions in coincidence. We describe a variety of tools developed to perform pump-probe studies in the VUV-XUV spectrum and to modify and characterize the photon beam. First benchmark experiments are presented to demonstrate the capabilities of the system.

An ultrafast angle-resolved photoemission apparatus for measuring complex materials

Science.gov (United States)

Smallwood, Christopher L.; Jozwiak, Christopher; Zhang, Wentao; Lanzara, Alessandra

2012-12-01

We present technical specifications for a high resolution time- and angle-resolved photoemission spectroscopy setup based on a hemispherical electron analyzer and cavity-dumped solid state Ti:sapphire laser used to generate pump and probe beams, respectively, at 1.48 and 5.93 eV. The pulse repetition rate can be tuned from 209 Hz to 54.3 MHz. Under typical operating settings the system has an overall energy resolution of 23 meV, an overall momentum resolution of 0.003 Å-1, and an overall time resolution of 310 fs. We illustrate the system capabilities with representative data on the cuprate superconductor Bi2Sr2CaCu2O8+δ. The descriptions and analyses presented here will inform new developments in ultrafast electron spectroscopy.

Ultrafast photoinduced structure phase transition in antimony single crystals

NARCIS (Netherlands)

Fausti, Daniele; Misochko, Oleg V.; van Loosdrecht, Paul H. M.

2009-01-01

Picosecond Raman scattering is used to study the photoinduced ultrafast dynamics in Peierls distorted antimony. We find evidence for an ultrafast nonthermal reversible structural phase transition. Most surprisingly, we find evidence that this transition evolves toward a lower symmetry in contrast to

Few-cycle surface plasmon enhanced electron acceleration

International Nuclear Information System (INIS)

Racz, P.; Lenner, M.; Kroo, N.; Farkas, Gy.; Dombi, P.; Takao Fuji; Krausz, F.; Irvine, S.E.; Elezzabi, A.Y.

2010-01-01

Complete text of publication follows. It is possible to generate high-quality ultrafast electron beams with keV energy based on surface plasmon-enhanced electron acceleration. The beam generated this way can be also used to investigate ultrafast phenomena in the plasmon field. For the better understanding of the temporal behavior of these ultrafast surface processes we carried out time-resolved experiments with 5.5 fs laser pulses for the first time. In this experiment, we executed an autocorrelation measurement with an ultra-broadband interferometer. By generating surface plasmons at the output of the interferometer, we measured the plasmonic photocurrent as a function of the delay between the interferometer arms. Figure (a) shows a typical measured result, and figure (b) shows the fourth order calculated autocorrelation function of the 5.5 fs long laser pulse, corresponding to the fourth order nonlinearity of the electron emission process. According to the correspondence of these two curves, we can also state that the length of the generated surface plasmon pulse is only 2-3 optical cycles. As a further experiment, we executed spectrally resolved measurements of the electron beam at higher intensities. According to these results, it is possible to reach electron beams with keV energy in the few-cycle regime too. It was found that the field strength of the surface plasmons is x 7 to x 30 higher than that of the focused laser pulse.

Direct Characterization of Ultrafast Energy-Time Entangled Photon Pairs.

Science.gov (United States)

MacLean, Jean-Philippe W; Donohue, John M; Resch, Kevin J

2018-02-02

Energy-time entangled photons are critical in many quantum optical phenomena and have emerged as important elements in quantum information protocols. Entanglement in this degree of freedom often manifests itself on ultrafast time scales, making it very difficult to detect, whether one employs direct or interferometric techniques, as photon-counting detectors have insufficient time resolution. Here, we implement ultrafast photon counters based on nonlinear interactions and strong femtosecond laser pulses to probe energy-time entanglement in this important regime. Using this technique and single-photon spectrometers, we characterize all the spectral and temporal correlations of two entangled photons with femtosecond resolution. This enables the witnessing of energy-time entanglement using uncertainty relations and the direct observation of nonlocal dispersion cancellation on ultrafast time scales. These techniques are essential to understand and control the energy-time degree of freedom of light for ultrafast quantum optics.

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

Science.gov (United States)

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

2017-02-08

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

Progress in ultrafast intense laser science

CERN Document Server

Yamanouchi, Kaoru; Mathur, Deepak

2014-01-01

The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance

Ultrafast Ultrasound Imaging With Cascaded Dual-Polarity Waves.

Science.gov (United States)

Zhang, Yang; Guo, Yuexin; Lee, Wei-Ning

2018-04-01

Ultrafast ultrasound imaging using plane or diverging waves, instead of focused beams, has advanced greatly the development of novel ultrasound imaging methods for evaluating tissue functions beyond anatomical information. However, the sonographic signal-to-noise ratio (SNR) of ultrafast imaging remains limited due to the lack of transmission focusing, and thus insufficient acoustic energy delivery. We hereby propose a new ultrafast ultrasound imaging methodology with cascaded dual-polarity waves (CDWs), which consists of a pulse train with positive and negative polarities. A new coding scheme and a corresponding linear decoding process were thereby designed to obtain the recovered signals with increased amplitude, thus increasing the SNR without sacrificing the frame rate. The newly designed CDW ultrafast ultrasound imaging technique achieved higher quality B-mode images than coherent plane-wave compounding (CPWC) and multiplane wave (MW) imaging in a calibration phantom, ex vivo pork belly, and in vivo human back muscle. CDW imaging shows a significant improvement in the SNR (10.71 dB versus CPWC and 7.62 dB versus MW), penetration depth (36.94% versus CPWC and 35.14% versus MW), and contrast ratio in deep regions (5.97 dB versus CPWC and 5.05 dB versus MW) without compromising other image quality metrics, such as spatial resolution and frame rate. The enhanced image qualities and ultrafast frame rates offered by CDW imaging beget great potential for various novel imaging applications.

Ultrafast Dynamic Pressure Sensors Based on Graphene Hybrid Structure.

Science.gov (United States)

Liu, Shanbiao; Wu, Xing; Zhang, Dongdong; Guo, Congwei; Wang, Peng; Hu, Weida; Li, Xinming; Zhou, Xiaofeng; Xu, Hejun; Luo, Chen; Zhang, Jian; Chu, Junhao

2017-07-19

Mechanical flexible electronic skin has been focused on sensing various physical parameters, such as pressure and temperature. The studies of material design and array-accessible devices are the building blocks of strain sensors for subtle pressure sensing. Here, we report a new and facile preparation of a graphene hybrid structure with an ultrafast dynamic pressure response. Graphene oxide nanosheets are used as a surfactant to prevent graphene restacking in aqueous solution. This graphene hybrid structure exhibits a frequency-independent pressure resistive sensing property. Exceeding natural skin, such pressure sensors, can provide transient responses from static up to 10 000 Hz dynamic frequencies. Integrated by the controlling system, the array-accessible sensors can manipulate a robot arm and self-rectify the temperature of a heating blanket. This may pave a path toward the future application of graphene-based wearable electronics.

Nitrogen-Doped Holey Graphene Film-Based Ultrafast Electrochemical Capacitors.

Science.gov (United States)

Zhou, Qinqin; Zhang, Miao; Chen, Ji; Hong, Jong-Dal; Shi, Gaoquan

2016-08-17

The commercialized aluminum electrolytic capacitors (AECs) currently used for alternating current (AC) line-filtering are usually the largest components in the electronic circuits because of their low specific capacitances and bulky sizes. Herein, nitrogen-doped holey graphene (NHG) films were prepared by thermal annealing the composite films of polyvinylpyrrolidone (PVP), graphene oxide (GO), and ferric oxide (Fe2O3) nanorods followed by chemical etching with hydrochloride acid. The typical electrochemical capacitor with NHG electrodes exhibited high areal and volumetric specific capacitances of 478 μF cm(-2) and 1.2 F cm(-3) at 120 Hz, ultrafast frequency response with a phase angle of -81.2° and a resistor-capacitor time constant of 203 μs at 120 Hz, as well as excellent cycling stability. Thus, it is promising to replace conventional AEC for AC line-filtering in miniaturized electronics.

Quantum dynamics of a BEC interacting with a single-mode quantized field in the presence of interatom collisions

Energy Technology Data Exchange (ETDEWEB)

Ghasemian, E. [Atomic and Molecular Group, Faculty of Physics, Yazd University, Yazd (Iran, Islamic Republic of); Tavassoly, M.K., E-mail: mktavassoly@yazd.ac.ir [Atomic and Molecular Group, Faculty of Physics, Yazd University, Yazd (Iran, Islamic Republic of); Photonics Research Group, Engineering Research Center, Yazd University, Yazd (Iran, Islamic Republic of); The Laboratory of Quantum Information Processing, Yazd University, Yazd (Iran, Islamic Republic of)

2016-09-23

In this paper, we consider a model in which N two-level atoms in a Bose–Einstein condensate (BEC) interact with a single-mode quantized laser field. Our goal is to investigate the quantum dynamics of atoms in the BEC in the presence of interatom interactions. To achieve the purpose, at first, using the collective angular momentum operators, we try to reduce the dynamical Hamiltonian of the system to a well-known Jaynes–Cummings like model (JCM). We also use the Dicke model to construct the state of atomic subsystem, by which the analytical solution of the system may be obtained. Then, we analyze the atomic population inversion, the degree of entanglement between the “atoms in BEC” and the “field” as well as the Mandel parameter. Numerical results show that, the atomic population inversion, atom-field entanglement and quantum statistics of photons are very sensitive to the evolved parameters in the model (and so can be well-adjusted), such as the number of atoms in BEC, the intensity of initial field, the interatom coupling constant and detuning. To investigate the entanglement properties, we pay attention to the entropy and linear entropy. It is shown that, oscillations in the two entropy criteria may be seen, with some maxima of entanglement at some moments of time. Finally, looking for the quantum statistics, we evaluate the Mandel parameter, by which we demonstrate the sub-Poissonian statistics and so the nonclassical characteristics of the field state of system. Collapse-revival phenomenon, which is a distinguishable nonclassical characteristic of the system, can be apparently observed in the atomic population inversion and the Mandel parameter. - Highlights: • N two-level atoms in a BEC interacting with a laser field in the presence of interatom interactions is considered. • The atomic population inversion, degree of entanglement between the “atoms in BEC” and the “field” and the Mandel parameter are investigated. • Collapse

Generation of ultrafast pulse via combined effects of stimulated

Indian Academy of Sciences (India)

A project of ultrafast pulse generation has been presented and demonstrated by utilizing the combined nonlinear effects of stimulated Raman scattering (SRS) and non-degenerate two-photon absorption (TPA) based on silicon nanophotonic chip, in which a continuous wave (CW) and an ultrafast dark pulse are ...

Design and implementation of a fs-resolved transmission electron microscope based on thermionic gun technology

Energy Technology Data Exchange (ETDEWEB)

Piazza, L., E-mail: luca.piazza@epfl.ch [Laboratory for Ultrafast Microscopy and Electron Scattering (LUMES), ICMP, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne (Switzerland); Masiel, D.J. [Integrated Dynamic Electron Solutions, Inc., 455 Bolero Drive, Danville, CA 94526 (United States); LaGrange, T.; Reed, B.W. [Condensed Matter and Materials Division Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States); Barwick, B. [Department of Physics, Trinity College, 300 Summit St., Hartford, CT 06106 (United States); Carbone, Fabrizio [Laboratory for Ultrafast Microscopy and Electron Scattering (LUMES), ICMP, Ecole Polytechnique Fédérale de Lausanne, CH-1015 Lausanne (Switzerland)

2013-09-23

Highlights: • We present the implementation of a femtosecond-resolved ultrafast TEM. • This is the first ultrafast TEM based on a thermionic gun geometry. • An additional condenser lens has been used to maximize the electron count. • We achieved a time resolution of about 300 fs and an energy resolution of 1 eV. - Abstract: In this paper, the design and implementation of a femtosecond-resolved ultrafast transmission electron microscope is presented, based on a thermionic gun geometry. Utilizing an additional magnetic lens between the electron acceleration and the nominal condenser lens system, a larger percentage of the electrons created at the cathode are delivered to the specimen without degrading temporal, spatial and energy resolution significantly, while at the same time maintaining the femtosecond temporal resolution. Using the photon-induced near field electron microscopy effect (PINEM) on silver nanowires the cross-correlation between the light and electron pulses was measured, showing the impact of the gun settings and initiating laser pulse duration on the electron bunch properties. Tuneable electron pulses between 300 fs and several ps can be obtained, and an overall energy resolution around 1 eV was achieved.

Visualizing a protein quake with time-resolved X-ray scattering at a free-electron laser

DEFF Research Database (Denmark)

Arnlund, David; Johansson, Linda C.; Wickstrand, Cecilia

2014-01-01

We describe a method to measure ultrafast protein structural changes using time-resolved wide-angle X-ray scattering at an X-ray free-electron laser. We demonstrated this approach using multiphoton excitation of the Blastochloris viridis photosynthetic reaction center, observing an ultrafast glob...

Locking Lasers to RF in an Ultrafast FEL

International Nuclear Information System (INIS)

Wilcox, R.; Huang, G.; Doolittle, L.; White, W.; Frisch, J.; Coffee, R.

2010-01-01

Using a novel, phase-stabilized RF-over-fiber scheme, they transmit 3GHz over 300m with 27fs RMS error in 250kHz bandwidth over 12 hours, and phase lock a laser to enable ultrafast pump-probe experiments. Free-electron lasers (FELs) are capable of producing short-duration (< 10fs), high-energy X-ray pulses for a range of scientific applications. The recently activated Linac Coherent Light Source (LCLS) FEL facility at SLAC will support experiments which require synchronized light pulses for pump-probe schemes. They developed and operated a fiber optic RF transmission system to synchronize lasers to the emitted X-ray pulses, which was used to enable the first pump-probe experiments at the LCLS.

An ultrafast angle-resolved photoemission apparatus for measuring complex materials

International Nuclear Information System (INIS)

Smallwood, Christopher L.; Lanzara, Alessandra; Jozwiak, Christopher; Zhang Wentao

2012-01-01

We present technical specifications for a high resolution time- and angle-resolved photoemission spectroscopy setup based on a hemispherical electron analyzer and cavity-dumped solid state Ti:sapphire laser used to generate pump and probe beams, respectively, at 1.48 and 5.93 eV. The pulse repetition rate can be tuned from 209 Hz to 54.3 MHz. Under typical operating settings the system has an overall energy resolution of 23 meV, an overall momentum resolution of 0.003 Å −1 , and an overall time resolution of 310 fs. We illustrate the system capabilities with representative data on the cuprate superconductor Bi 2 Sr 2 CaCu 2 O 8+δ . The descriptions and analyses presented here will inform new developments in ultrafast electron spectroscopy.

Photoelectron and ICD electron angular distributions from fixed-in-space neon dimers

International Nuclear Information System (INIS)

Jahnke, T; Czasch, A; Schoeffler, M; Schoessler, S; Kaesz, M; Titze, J; Kreidi, K; Grisenti, R E; Staudte, A; Jagutzki, O; Schmidt, L Ph H; Semenov, S K; Cherepkov, N A; Schmidt-Boecking, H; Doerner, R

2007-01-01

We report on molecular frame angular distributions of 2s photoelectrons and electrons emitted by interatomic Coulombic decay from neon dimers. We found that the measured angular distribution of the photoelectron strongly depends on the environment of the cluster. The experimental results are in excellent agreement with frozen core Hartree-Fock calculations. The ICD electrons show slight variations in their angular distribution for different kinetic energies

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

KAUST Repository

Shaheen, Basamat; Sun, Jingya; Yang, Ding-Shyue; Mohammed, Omar F.

2017-01-01

information can be obtained using the one-of-a-kind methodology of scanning ultrafast electron microscopy (S-UEM). Here, we address the fundamental issue of how the thickness of the absorber layer may significantly affect the charge carrier dynamics

Feed-forward motor control of ultrafast, ballistic movements.

Science.gov (United States)

Kagaya, K; Patek, S N

2016-02-01

To circumvent the limits of muscle, ultrafast movements achieve high power through the use of springs and latches. The time scale of these movements is too short for control through typical neuromuscular mechanisms, thus ultrafast movements are either invariant or controlled prior to movement. We tested whether mantis shrimp (Stomatopoda: Neogonodactylus bredini) vary their ultrafast smashing strikes and, if so, how this control is achieved prior to movement. We collected high-speed images of strike mechanics and electromyograms of the extensor and flexor muscles that control spring compression and latch release. During spring compression, lateral extensor and flexor units were co-activated. The strike initiated several milliseconds after the flexor units ceased, suggesting that flexor activity prevents spring release and determines the timing of strike initiation. We used linear mixed models and Akaike's information criterion to serially evaluate multiple hypotheses for control mechanisms. We found that variation in spring compression and strike angular velocity were statistically explained by spike activity of the extensor muscle. The results show that mantis shrimp can generate kinematically variable strikes and that their kinematics can be changed through adjustments to motor activity prior to the movement, thus supporting an upstream, central-nervous-system-based control of ultrafast movement. Based on these and other findings, we present a shishiodoshi model that illustrates alternative models of control in biological ballistic systems. The discovery of feed-forward control in mantis shrimp sets the stage for the assessment of targets, strategic variation in kinematics and the role of learning in ultrafast animals. © 2016. Published by The Company of Biologists Ltd.

Ultrafast Nonlinear Signal Processing in Silicon Waveguides

DEFF Research Database (Denmark)

Oxenløwe, Leif Katsuo; Mulvad, Hans Christian Hansen; Hu, Hao

2012-01-01

We describe recent demonstrations of exploiting highly nonlinear silicon waveguides for ultrafast optical signal processing. We describe wavelength conversion and serial-to-parallel conversion of 640 Gbit/s data signals and 1.28 Tbit/s demultiplexing and all-optical sampling.......We describe recent demonstrations of exploiting highly nonlinear silicon waveguides for ultrafast optical signal processing. We describe wavelength conversion and serial-to-parallel conversion of 640 Gbit/s data signals and 1.28 Tbit/s demultiplexing and all-optical sampling....

Optimization and practical implementation of ultrafast 2D NMR experiments

Energy Technology Data Exchange (ETDEWEB)

Queiroz Junior, Luiz H. K., E-mail: professorkeng@gmail.com [Universidade Federal de Sao Carlos (UFSC), SP (Brazil). Departamento de Quimica; Universidade Federal de Goias (UFGO), Goiania, GO (Brazil). Inst. de Quimica; Ferreira, Antonio G. [Universidade Federal de Sao Carlos (UFSC), SP (Brazil). Departamento de Quimica; Giraudeau, Patrick [Universite de Nantes (France). CNRS, Chimie et Interdisciplinarite: Synthese, Analyse, Modelisation

2013-09-01

Ultrafast 2D NMR is a powerful methodology that allows recording of a 2D NMR spectrum in a fraction of second. However, due to the numerous non-conventional parameters involved in this methodology its implementation is no trivial task. Here, an optimized experimental protocol is carefully described to ensure efficient implementation of ultrafast NMR. The ultrafast spectra resulting from this implementation are presented based on the example of two widely used 2D NMR experiments, COSY and HSQC, obtained in 0.2 s and 41 s, respectively. (author)

All-optical temporal integration of ultrafast pulse waveforms.

Science.gov (United States)

Park, Yongwoo; Ahn, Tae-Jung; Dai, Yitang; Yao, Jianping; Azaña, José

2008-10-27

An ultrafast all-optical temporal integrator is experimentally demonstrated. The demonstrated integrator is based on a very simple and practical solution only requiring the use of a widely available all-fiber passive component, namely a reflection uniform fiber Bragg grating (FBG). This design allows overcoming the severe speed (bandwidth) limitations of the previously demonstrated photonic integrator designs. We demonstrate temporal integration of a variety of ultrafast optical waveforms, including Gaussian, odd-symmetry Hermite Gaussian, and (odd-)symmetry double pulses, with temporal features as fast as ~6-ps, which is about one order of magnitude faster than in previous photonic integration demonstrations. The developed device is potentially interesting for a multitude of applications in all-optical computing and information processing, ultrahigh-speed optical communications, ultrafast pulse (de-)coding, shaping and metrology.

Concerning the theory of radiation cascades of atomic collisions in a solid with an arbitrary interatomic interaction potential

International Nuclear Information System (INIS)

Ryazanov, A.I.; Metelkin, E.V.

1980-01-01

Cascades of atomic collisions created by high energy particles as a result of irradiation of solids by them are considered. The solution of the problem is based on the investigation of the Boltzmann stationary kinetic equation for moving atoms. For this equation a model scattering indicatrix is constructed with an arbitrary form of the potential of interaction of moving atoms with lattice atoms. The choice of the model scattering indicatrix of atoms is determined by the normalization, the average energy loss in a single collision and by the deviation of the energy losses really occurring in the collision from the mean value, as well as by the initial kinetic equation for moving atoms. The energy distribution of moving atoms for arbitrary interatomic interaction potentials has been obtained using the constructed model scattering indicatrix. On the basis of the theory constructed a cascade is calculated with an interatomic interaction potential in the form of the Thomas-Fermi potential and the power potential. (author)

Ultrafast dynamics of electrons at interfaces

Energy Technology Data Exchange (ETDEWEB)

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

1999-05-03

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

Ultrafast re-structuring of the electronic landscape of transparent dielectrics: new material states (Die-Met)

Science.gov (United States)

Gamaly, E. G.; Rode, A. V.

2018-03-01

Swift excitation of transparent dielectrics by ultrashort and highly intense laser pulse leads to ultra-fast re-structuring of the electronic landscape and generates many transient material states, which are continuously reshaped in accord with the changing pulse intensity. These unconventional transient material states, which exhibit simultaneously both dielectric and metallic properties, we termed here as the `Die-Met' states. The excited material is transparent and conductive at the same time. The real part of permittivity of the excited material changes from positive to negative values with the increase of excitation, which affects strongly the interaction process during the laser pulse. When the incident field has a component along the permittivity gradient, the amplitude of the field increases resonantly near the point of zero permittivity, which dramatically changes the interaction mode and increases absorption in a way that is similar to the resonant absorption in plasma. The complex 3D structure of the permittivity makes a transparent part of the excited dielectric (at ɛ 0 > ɛ re > 0) optically active. The electro-magnetic wave gets a twisted trajectory and accrues the geometric phase while passing through such a medium. Both the phase and the rotation of the polarisation plane depend on the 3D permittivity structure. Measuring the transmission, polarisation and the phase of the probe beam allows one to quantitatively identify these new transient states. We discuss the revelations of this effect in different experimental situations and their possible applications.

Unlocking the Constraints of Cyanobacterial Productivity: Acclimations Enabling Ultrafast Growth

Energy Technology Data Exchange (ETDEWEB)

Bernstein, Hans C.; McClure, Ryan S.; Hill, Eric A.; Markillie, Lye Meng; Chrisler, William B.; Romine, Margie F.; McDermott, Jason E.; Posewitz, Matthew C.; Bryant, Donald A.; Konopka, Allan E.; Fredrickson, James K.; Beliaev, Alexander S.

2016-07-26

Harnessing the metabolic potential of photosynthetic microbes for next-generation biotechnology objectives requires detailed scientific understanding of the physiological constraints and regulatory controls affecting carbon partitioning between biomass, metabolite storage pools, and bioproduct synthesis. We dissected the cellular mechanisms underlying the remarkable physiological robustness of the euryhaline unicellular cyanobacteriumSynechococcussp. strain PCC 7002 (Synechococcus7002) and identify key mechanisms that allow cyanobacteria to achieve unprecedented photoautotrophic productivities (~2.5-h doubling time). Ultrafast growth ofSynechococcus7002 was supported by high rates of photosynthetic electron transfer and linked to significantly elevated transcription of precursor biosynthesis and protein translation machinery. Notably, no growth or photosynthesis inhibition signatures were observed under any of the tested experimental conditions. Finally, the ultrafast growth inSynechococcus7002 was also linked to a 300% expansion of average cell volume. We hypothesize that this cellular adaptation is required at high irradiances to support higher cell division rates and reduce deleterious effects, corresponding to high light, through increased carbon and reductant sequestration.

IMPORTANCEEfficient coupling between photosynthesis and productivity is central to the development of biotechnology based on solar energy. Therefore, understanding the factors constraining maximum rates of carbon processing is necessary to identify regulatory mechanisms and devise strategies to overcome productivity constraints. Here, we interrogate the molecular mechanisms that operate at a systems level to allow cyanobacteria to achieve ultrafast growth. This was done by considering growth and photosynthetic kinetics with global transcription patterns. We have delineated

Study of interatomic potential and thermal structural properties of β-Zn4Sb3

International Nuclear Information System (INIS)

Li, Guodong; Li, Yao; Liu, Lisheng; Zhang, Qingjie; Zhai, Pengcheng

2012-01-01

Highlights: ► The multi-body interatomic potentials of various models of β-Zn 4 Sb 3 have been developed to describe atomic interactions. ► The radial distribution function shows that the 10% vacancy of Zn site leads to the disorder of β-Zn 4 Sb 3 . ► The 10% vacancy of Zn site is the main cause of the exceptional low thermal conductivity. -- Abstract: Previous experimental research shows that the disordered Zn atoms in β-Zn 4 Sb 3 may have an important influence on its exceptionally low thermal conductivity and easily occurred phase transition. So the present work aims to study the influence of disordered Zn atoms on thermodynamics properties of β-Zn 4 Sb 3 by using molecular dynamics (MD) method. Firstly, based on first principles calculation and experimental results, the interatomic potentials of β-Zn 4 Sb 3 and MD analysis method are established, and the feasibility is verified. Then, the influence of disordered Zn atoms on thermal conductivity of β-Zn 4 Sb 3 is studied in detail. The simulation results indicate that the 10% vacant Zn atoms is the main reason for the exceptionally low thermal conductivity of β-Zn 4 Sb 3 , and it seems that the interstitial Zn atoms have little effect on its thermal conductivity.

First-principles interatomic potentials for transition-metal aluminides. III. Extension to ternary phase diagrams

Science.gov (United States)

Widom, Mike; Al-Lehyani, Ibrahim; Moriarty, John A.

2000-08-01

Modeling structural and mechanical properties of intermetallic compounds and alloys requires detailed knowledge of their interatomic interactions. The first two papers of this series [Phys. Rev. B 56, 7905 (1997); 58, 8967 (1998)] derived first-principles interatomic potentials for transition-metal (TM) aluminides using generalized pseudopotential theory (GPT). Those papers focused on binary alloys of aluminum with first-row transition metals and assessed the ability of GPT potentials to reproduce and elucidate the alloy phase diagrams of Al-Co and Al-Ni. This paper addresses the phase diagrams of the binary alloy Al-Cu and the ternary systems Al-Co-Cu and Al-Co-Ni, using GPT pair potentials calculated in the limit of vanishing transition-metal concentration. Despite this highly simplifying approximation, we find rough agreement with the known low-temperature phase diagrams, up to 50% total TM concentration provided the Co fraction is below 25%. Full composition-dependent potentials and many-body interactions would be required to correct deficiencies at higher Co concentration. Outside this troublesome region, the experimentally determined stable and metastable phases all lie on or near the convex hull of a scatter plot of energy versus composition. We verify, qualitatively, reported solubility ranges extending binary alloys into the ternary diagram in both Al-Co-Cu and Al-Co-Ni. Finally, we reproduce previously conjectured transition-metal positions in the decagonal quasicrystal phase.

Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering

Science.gov (United States)

Walt, Samuel G.; Bhargava Ram, Niraghatam; Atala, Marcos; Shvetsov-Shilovski, Nikolay I; von Conta, Aaron; Baykusheva, Denitsa; Lein, Manfred; Wörner, Hans Jakob

2017-01-01

Strong-field photoelectron holography and laser-induced electron diffraction (LIED) are two powerful emerging methods for probing the ultrafast dynamics of molecules. However, both of them have remained restricted to static systems and to nuclear dynamics induced by strong-field ionization. Here we extend these promising methods to image purely electronic valence-shell dynamics in molecules using photoelectron holography. In the same experiment, we use LIED and photoelectron holography simultaneously, to observe coupled electronic-rotational dynamics taking place on similar timescales. These results offer perspectives for imaging ultrafast dynamics of molecules on femtosecond to attosecond timescales. PMID:28643771

An interatomic potential for studying CuZr bulk metallic glasses

International Nuclear Information System (INIS)

Paduraru, A.; Kenoufi, A.; Bailey, N.P.; Schioetz, J.

2007-01-01

Glass forming ability has been found in only a small number of binary alloys, one being CuZr. In order to simulate this glass, we fitted an interatomic potential within Effective Medium Theory (EMT). For this purpose we use basic properties of the B2 crystal structure as calculated from Density Functional Theory (DFT) or obtained from experiments. We then performed Molecular Dynamics (MD) simulations of the cooling process and studied the thermodynamics and structure of CuZr glass. We find that the potential gives a good description of the CuZr glass, with a glass transition temperature and elastic constants close to the experimental values. The local atomic order, as witnessed by the radial distribution function, is also consistent with similar experimental data. (Abstract Copyright [2007], Wiley Periodicals, Inc.)

Radio frequency acceleration and manipulation of ultra-cold electron bunches

NARCIS (Netherlands)

Franssen, J.G.H.; Vredenbregt, E.J.D.; Luiten, O.J.

2016-01-01

We are developing an ultra-fast and ultra-cold electron source based on a grating magneto optical trap, RF acceleration and RF (de-) compression techniques. The electrons will be created by near-threshold, femtosecond photoionization of a laser-cooled and trapped gas. The electron cloud is extracted

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy.

Science.gov (United States)

Hayes, Dugan; Kohler, Lars; Hadt, Ryan G; Zhang, Xiaoyi; Liu, Cunming; Mulfort, Karen L; Chen, Lin X

2018-01-28

The kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(i) bis(phenanthroline)/ruthenium(ii) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(i)-Ru(ii) analogs of the homodinuclear Cu(i)-Cu(i) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These results suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.

Progress in ultrafast intense laser science XI

CERN Document Server

Yamanouchi, Kaoru; Martin, Philippe

2014-01-01

The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance

Progress in Ultrafast Intense Laser Science II

CERN Document Server

Yamanouchi, Kaoru; Agostini, Pierre; Ferrante, Gaetano

2007-01-01

This book series addresses a newly emerging interdisciplinary research field, Ultrafast Intense Laser Science, spanning atomic and molecular physics, molecular science, and optical science. Its progress is being stimulated by the recent development of ultrafast laser technologies. Highlights of this second volume include Coulomb explosion and fragmentation of molecules, control of chemical dynamics, high-order harmonic generation, propagation and filamentation, and laser-plasma interaction. All chapters are authored by foremost experts in their fields and the texts are written at a level accessible to newcomers and graduate students, each chapter beginning with an introductory overview.

Emerging Low-Dimensional Materials for Nonlinear Optics and Ultrafast Photonics.

Science.gov (United States)

Liu, Xiaofeng; Guo, Qiangbing; Qiu, Jianrong

2017-04-01

Low-dimensional (LD) materials demonstrate intriguing optical properties, which lead to applications in diverse fields, such as photonics, biomedicine and energy. Due to modulation of electronic structure by the reduced structural dimensionality, LD versions of metal, semiconductor and topological insulators (TIs) at the same time bear distinct nonlinear optical (NLO) properties as compared with their bulk counterparts. Their interaction with short pulse laser excitation exhibits a strong nonlinear character manifested by NLO absorption, giving rise to optical limiting or saturated absorption associated with excited state absorption and Pauli blocking in different materials. In particular, the saturable absorption of these emerging LD materials including two-dimensional semiconductors as well as colloidal TI nanoparticles has recently been utilized for Q-switching and mode-locking ultra-short pulse generation across the visible, near infrared and middle infrared wavelength regions. Beside the large operation bandwidth, these ultrafast photonics applications are especially benefit from the high recovery rate as well as the facile processibility of these LD materials. The prominent NLO response of these LD materials have also provided new avenues for the development of novel NLO and photonics devices for all-optical control as well as optical circuits beyond ultrafast lasers. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics

Directory of Open Access Journals (Sweden)

Mizuho Fushitani

2016-11-01

Full Text Available We present applications of extreme ultraviolet (XUV single-order laser harmonics to gas-phase ultrafast photoelectron spectroscopy. Ultrashort XUV pulses at 80 nm are obtained as the 5th order harmonics of the fundamental laser at 400 nm by using Xe or Kr as the nonlinear medium and separated from other harmonic orders by using an indium foil. The single-order laser harmonics is applied for real-time probing of vibrational wavepacket dynamics of I2 molecules in the bound and dissociating low-lying electronic states and electronic-vibrational wavepacket dynamics of highly excited Rydberg N2 molecules.

Single-order laser high harmonics in XUV for ultrafast photoelectron spectroscopy of molecular wavepacket dynamics.

Science.gov (United States)

Fushitani, Mizuho; Hishikawa, Akiyoshi

2016-11-01

We present applications of extreme ultraviolet (XUV) single-order laser harmonics to gas-phase ultrafast photoelectron spectroscopy. Ultrashort XUV pulses at 80 nm are obtained as the 5th order harmonics of the fundamental laser at 400 nm by using Xe or Kr as the nonlinear medium and separated from other harmonic orders by using an indium foil. The single-order laser harmonics is applied for real-time probing of vibrational wavepacket dynamics of I 2 molecules in the bound and dissociating low-lying electronic states and electronic-vibrational wavepacket dynamics of highly excited Rydberg N 2 molecules.

Ultrafast dynamics of colloidal semiconductor nanocrystals relevant to solar fuels production

Science.gov (United States)

Cogan, Nicole M. B.; Liu, Cunming; Qiu, Fen; Burke, Rebeckah; Krauss, Todd D.

2017-05-01

Artificial conversion of sunlight to chemical fuels has attracted attention for several decades as a potential source of clean, renewable energy. We recently found that CdSe quantum dots (QDs) and simple aqueous Ni2+ salts in the presence of a sacrificial electron donor form a highly efficient, active, and robust system for photochemical reduction of protons to molecular hydrogen. Ultrafast transient absorption spectroscopy studies of electron transfer (ET) processes from the QDs to the Ni catalysts reveal extremely fast ET, and provide a fundamental explanation for the exceptional photocatalytic H2 activity. Additionally, by studying H2 production of the Ni catalyst with CdSe/CdS nanoparticles of various structures, it was determined that surface charge density plays an important role in charge transfer and ultimately H2 production activity.

Ab initio study of lattice instabilities of zinc chalcogenides ZnX (X=O, S, Se, Te induced by ultrafast intense laser irradiation

Directory of Open Access Journals (Sweden)

Dahua Ren

2017-09-01

Full Text Available Ab initio calculations of lattice constants, lattice stabilities of ZnX (X=O, S, Se, Te at different electronic temperatures (Te have been performed using generalized gradient approximation (GGA pseudopotential method within the density functional theory (DFT. The calculated phonon frequencies of ZnX at Te = 0 eV accord well with the experimental and other theoretical values. Firstly, it is indicated that the lattice constants of ZnX increase and all the phonon frequencies reduce as Te increases. Additionally, the transverse-acoustic phonon frequencies of ZnX are imaginary with the elevation of Te, namely the lattices of ZnX become unstable under ultrafast intense laser irradiation. Moreover, the transverse optical mode-longitudinal optical mode (LO-TO splitting degree of ZnX (X=S, Se, Te gradually decreases as the electronic temperature increases, mainly due to the reason that the electronic excitation weakens the strength ionicity of ionic crystal ZnX under intense laser irradiation. However, the LO-TO splitting degree of ZnO firstly increases and then decreases with the increase of electronic temperature. After that, it can be helpful for understanding the mechanism of ultrafast intense laser induced semiconductors damage.

Carrier dynamics in graphene. Ultrafast many-particle phenomena

Energy Technology Data Exchange (ETDEWEB)

Malic, E.; Brem, S.; Jago, R. [Department of Physics, Chalmers University of Technology, Goeteborg (Sweden); Winzer, T.; Wendler, F.; Knorr, A. [Institut fuer Theoretische Physik, Technische Universitaet Berlin (Germany); Mittendorff, M.; Koenig-Otto, J.C.; Schneider, H.; Helm, M.; Winnerl, S. [Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany); Ploetzing, T.; Neumaier, D. [Advanced Microelectronic Center Aachen, AMO GmbH, Aachen (Germany)

2017-11-15

Graphene is an ideal material to study fundamental Coulomb- and phonon-induced carrier scattering processes. Its remarkable gapless and linear band structure opens up new carrier relaxation channels. In particular, Auger scattering bridging the valence and the conduction band changes the number of charge carriers and gives rise to a significant carrier multiplication - an ultrafast many-particle phenomenon that is promising for the design of highly efficient photodetectors. Furthermore, the vanishing density of states at the Dirac point combined with ultrafast phonon-induced intraband scattering results in an accumulation of carriers and a population inversion suggesting the design of graphene-based terahertz lasers. Here, we review our work on the ultrafast carrier dynamics in graphene and Landau-quantized graphene is presented providing a microscopic view on the appearance of carrier multiplication and population inversion. (copyright 2017 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

WE-B-210-02: The Advent of Ultrafast Imaging in Biomedical Ultrasound

International Nuclear Information System (INIS)

Tanter, M.

2015-01-01

In the last fifteen years, the introduction of plane or diverging wave transmissions rather than line by line scanning focused beams has broken the conventional barriers of ultrasound imaging. By using such large field of view transmissions, the frame rate reaches the theoretical limit of physics dictated by the ultrasound speed and an ultrasonic map can be provided typically in tens of micro-seconds (several thousands of frames per second). Interestingly, this leap in frame rate is not only a technological breakthrough but it permits the advent of completely new ultrasound imaging modes, including shear wave elastography, electromechanical wave imaging, ultrafast doppler, ultrafast contrast imaging, and even functional ultrasound imaging of brain activity (fUltrasound) introducing Ultrasound as an emerging full-fledged neuroimaging modality. At ultrafast frame rates, it becomes possible to track in real time the transient vibrations – known as shear waves – propagating through organs. Such “human body seismology” provides quantitative maps of local tissue stiffness whose added value for diagnosis has been recently demonstrated in many fields of radiology (breast, prostate and liver cancer, cardiovascular imaging, …). Today, Supersonic Imagine company is commercializing the first clinical ultrafast ultrasound scanner, Aixplorer with real time Shear Wave Elastography. This is the first example of an ultrafast Ultrasound approach surpassing the research phase and now widely spread in the clinical medical ultrasound community with an installed base of more than 1000 Aixplorer systems in 54 countries worldwide. For blood flow imaging, ultrafast Doppler permits high-precision characterization of complex vascular and cardiac flows. It also gives ultrasound the ability to detect very subtle blood flow in very small vessels. In the brain, such ultrasensitive Doppler paves the way for fUltrasound (functional ultrasound imaging) of brain activity with unprecedented

WE-B-210-02: The Advent of Ultrafast Imaging in Biomedical Ultrasound

Energy Technology Data Exchange (ETDEWEB)

Tanter, M. [Laboratoire Ondes et Acoustique (France)

2015-06-15

In the last fifteen years, the introduction of plane or diverging wave transmissions rather than line by line scanning focused beams has broken the conventional barriers of ultrasound imaging. By using such large field of view transmissions, the frame rate reaches the theoretical limit of physics dictated by the ultrasound speed and an ultrasonic map can be provided typically in tens of micro-seconds (several thousands of frames per second). Interestingly, this leap in frame rate is not only a technological breakthrough but it permits the advent of completely new ultrasound imaging modes, including shear wave elastography, electromechanical wave imaging, ultrafast doppler, ultrafast contrast imaging, and even functional ultrasound imaging of brain activity (fUltrasound) introducing Ultrasound as an emerging full-fledged neuroimaging modality. At ultrafast frame rates, it becomes possible to track in real time the transient vibrations – known as shear waves – propagating through organs. Such “human body seismology” provides quantitative maps of local tissue stiffness whose added value for diagnosis has been recently demonstrated in many fields of radiology (breast, prostate and liver cancer, cardiovascular imaging, …). Today, Supersonic Imagine company is commercializing the first clinical ultrafast ultrasound scanner, Aixplorer with real time Shear Wave Elastography. This is the first example of an ultrafast Ultrasound approach surpassing the research phase and now widely spread in the clinical medical ultrasound community with an installed base of more than 1000 Aixplorer systems in 54 countries worldwide. For blood flow imaging, ultrafast Doppler permits high-precision characterization of complex vascular and cardiac flows. It also gives ultrasound the ability to detect very subtle blood flow in very small vessels. In the brain, such ultrasensitive Doppler paves the way for fUltrasound (functional ultrasound imaging) of brain activity with unprecedented

FPS-vidicon television camras for ultrafast-scan data acquisition

International Nuclear Information System (INIS)

Noel, B.W.; Yates, G.J.

1980-06-01

Two ultrafast-scan ( 500 TV lines per picture height with a corresponding dynamic range (to light input) of more than 100. The cameras use the unique properties of FPS vidicons and specially designed electronics to achieve their performance levels and versatility. The advantages and disadvantages of FPS vidicons and of antimony trisulfide and silicon target materials in such applications are discussed in detail. All of the electronics circuits are discussed. The sweep generator designs are treated at length because they are the key to the cameras' versatility. Emphasis is placed on remotely controllable analog and digital sweep generators. The latter is a complete CAMAC-compatible subsystem containing a 16-function master arithmetic logic unit. Pulsed and cw methods of obtaining transfer characteristics are described and compared. The effects of generation rates, tube types, and target types on the resolution, determined from contrast-transfer-function curves, are discussed. Several applications are described, including neutron TV pinhole, TREAT, and barium-release experiments

Extending the accuracy of the SNAP interatomic potential form

Science.gov (United States)

Wood, Mitchell A.; Thompson, Aidan P.

2018-06-01

The Spectral Neighbor Analysis Potential (SNAP) is a classical interatomic potential that expresses the energy of each atom as a linear function of selected bispectrum components of the neighbor atoms. An extension of the SNAP form is proposed that includes quadratic terms in the bispectrum components. The extension is shown to provide a large increase in accuracy relative to the linear form, while incurring only a modest increase in computational cost. The mathematical structure of the quadratic SNAP form is similar to the embedded atom method (EAM), with the SNAP bispectrum components serving as counterparts to the two-body density functions in EAM. The effectiveness of the new form is demonstrated using an extensive set of training data for tantalum structures. Similar to artificial neural network potentials, the quadratic SNAP form requires substantially more training data in order to prevent overfitting. The quality of this new potential form is measured through a robust cross-validation analysis.

Coherent combination of ultrafast fiber amplifiers

International Nuclear Information System (INIS)

Hanna, Marc; Guichard, Florent; Druon, Frédéric; Georges, Patrick; Zaouter, Yoann; Papadopoulos, Dimitris N

2016-01-01

We review recent progress in coherent combining of femtosecond pulses amplified in optical fibers as a way to scale the peak and average power of ultrafast sources. Different methods of achieving coherent pulse addition in space (beam combining) and time (divided pulse amplification) domains are described. These architectures can be widely classified into active methods, where the relative phases between pulses are subject to a servomechanism, and passive methods, where phase matching is inherent to the geometry. Other experiments that combine pulses with different spectral contents, pulses that have been nonlinearly broadened or successive pulses from a mode-locked laser oscillator, are then presented. All these techniques allow access to unprecedented parameter range for fiber ultrafast sources. (topical review)

Hot electron dynamics at semiconductor surfaces: Implications for quantum dot photovoltaics

Science.gov (United States)

Tisdale, William A., III

Finding a viable supply of clean, renewable energy is one of the most daunting challenges facing the world today. Solar cells have had limited impact in meeting this challenge because of their high cost and low power conversion efficiencies. Semiconductor nanocrystals, or quantum dots, are promising materials for use in novel solar cells because they can be processed with potentially inexpensive solution-based techniques and because they are predicted to have novel optoelectronic properties that could enable the realization of ultra-efficient solar power converters. However, there is a lack of fundamental understanding regarding the behavior of highly-excited, or "hot," charge carriers near quantum-dot and semiconductor interfaces, which is of paramount importance to the rational design of high-efficiency devices. The elucidation of these ultrafast hot electron dynamics is the central aim of this Dissertation. I present a theoretical framework for treating the electronic interactions between quantum dots and bulk semiconductor surfaces and propose a novel experimental technique, time-resolved surface second harmonic generation (TR-SHG), for probing these interactions. I then describe a series of experimental investigations into hot electron dynamics in specific quantum-dot/semiconductor systems. A two-photon photoelectron spectroscopy (2PPE) study of the technologically-relevant ZnO(1010) surface reveals ultrafast (sub-30fs) cooling of hot electrons in the bulk conduction band, which is due to strong electron-phonon coupling in this highly polar material. The presence of a continuum of defect states near the conduction band edge results in Fermi-level pinning and upward (n-type) band-bending at the (1010) surface and provides an alternate route for electronic relaxation. In monolayer films of colloidal PbSe quantum dots, chemical treatment with either hydrazine or 1,2-ethanedithiol results in strong and tunable electronic coupling between neighboring quantum dots

Synchronous Measurement of Ultrafast Anisotropy Decay of the B850 in Bacterial LH2 Complex

International Nuclear Information System (INIS)

Wang Yun-Peng; Du Lu-Chao; Zhu Gang-Bei; Wang Zhuan; Weng Yu-Xiang

2015-01-01

Ultrafast anisotropic decay is a prominent parameter revealing ultrafast energy and electron transfer; however, it is difficult to be determined reliably owing to the requirement of a simultaneous availability of the parallel and perpendicular polarized decay kinetics. Nowadays, any measurement of anisotropic decay is a kind of approach to the exact simultaneity. Here we report a novel method for a synchronous ultrafast anisotropy decay measurement, which can well determine the anisotropy, even at a very early time, as the rising phase of the excitation laser pulse. The anisotropic decay of the B850 in bacterial light harvesting antenna complex LH2 of Rhodobacter sphaeroides in solution at room temperature with coherent excitation is detected by this method, which shows a polarization response time of 30 fs, and the energy transfer from the initial excitation to the bacteriochlorophylls in B850 ring takes about 70 fs. The anisotropic decay that is probed at the red side of the absorption spectrum, such as 880 nm, has an initial value of 0.4, corresponding to simulated emission, while the blue side with an anisotropy of 0.1 contributes to the ground-state bleaching. Our results show that the coherent excitation covering the whole ring might not be realized owing to the symmetry breaking of LH2: from C_9 symmetry in membrane to C_2 symmetry in solution. (atomic and molecular physics)

Synchronous Measurement of Ultrafast Anisotropy Decay of the B850 in Bacterial LH2 Complex

Science.gov (United States)

Wang, Yun-Peng; Du, Lu-Chao; Zhu, Gang-Bei; Wang, Zhuan; Weng, Yu-Xiang

2015-02-01

Ultrafast anisotropic decay is a prominent parameter revealing ultrafast energy and electron transfer; however, it is difficult to be determined reliably owing to the requirement of a simultaneous availability of the parallel and perpendicular polarized decay kinetics. Nowadays, any measurement of anisotropic decay is a kind of approach to the exact simultaneity. Here we report a novel method for a synchronous ultrafast anisotropy decay measurement, which can well determine the anisotropy, even at a very early time, as the rising phase of the excitation laser pulse. The anisotropic decay of the B850 in bacterial light harvesting antenna complex LH2 of Rhodobacter sphaeroides in solution at room temperature with coherent excitation is detected by this method, which shows a polarization response time of 30 fs, and the energy transfer from the initial excitation to the bacteriochlorophylls in B850 ring takes about 70 fs. The anisotropic decay that is probed at the red side of the absorption spectrum, such as 880 nm, has an initial value of 0.4, corresponding to simulated emission, while the blue side with an anisotropy of 0.1 contributes to the ground-state bleaching. Our results show that the coherent excitation covering the whole ring might not be realized owing to the symmetry breaking of LH2: from C9 symmetry in membrane to C2 symmetry in solution.

Controlling competing electronic orders via non-equilibrium acoustic phonons

Science.gov (United States)

Schuett, Michael; Orth, Peter; Levchenko, Alex; Fernandes, Rafael

The interplay between multiple electronic orders is a hallmark of strongly correlated systems displaying unconventional superconductivity. While doping, pressure, and magnetic field are the standard knobs employed to assess these different phases, ultrafast pump-and-probe techniques opened a new window to probe these systems. Recent examples include the ultrafast excitation of coherent optical phonons coupling to electronic states in cuprates and iron pnictides. In this work, we demonstrate theoretically that non-equilibrium acoustic phonons provide a promising framework to manipulate competing electronic phases and favor unconventional superconductivity over other states. In particular, we show that electrons coupled to out-of-equilibrium anisotropic acoustic phonons enter a steady state in which the effective electronic temperature varies around the Fermi surface. Such a momentum-dependent temperature can then be used to selectively heat electronic states that contribute primarily to density-wave instabilities, reducing their competition with superconductivity. We illustrate this phenomenon by computing the microscopic steady-state phase diagram of the iron pnictides, showing that superconductivity is enhanced with respect to the competing antiferromagnetic phase.

Probing ultrafast carrier tunneling dynamics in individual quantum dots and molecules

Energy Technology Data Exchange (ETDEWEB)

Mueller, Kai; Bechtold, Alexander; Kaldewey, Timo; Zecherle, Markus; Wildmann, Johannes S.; Bichler, Max; Abstreiter, Gerhard; Finley, Jonathan J. [Walter Schottky Institut and Physik-Department, Technische Universitaet Muenchen, Am Coulombwall 4, 85748, Garching (Germany); Ruppert, Claudia; Betz, Markus [Experimentelle Physik 2, TU Dortmund, 44221, Dortmund (Germany); Krenner, Hubert J. [Lehrstuhl fuer Experimentalphysik 1 and Augsburg Centre for Innovative Technologies (ACIT), Universitaet Augsburg, Universitaetsstr 1, 86159, Augsburg (Germany); Villas-Boas, Jose M. [Instituto de Fisica, Universidade Federal de Uberlandia, 38400-902, Uberlandia, MG (Brazil)

2013-02-15

Ultrafast pump-probe spectroscopy is employed to directly monitor the tunneling of charge carriers from single and vertically coupled quantum dots and probe intra-molecular dynamics. Immediately after resonant optical excitation, several peaks are observed in the pump-probe spectrum arising from Coulomb interactions between the photogenerated charge carriers. The influence of few-Fermion interactions in the photoexcited system and the temporal evolution of the optical response is directly probed in the time domain. In addition, the tunneling times for electrons and holes from the QD nanostructure are independently determined. In polarization resolved measurements, near perfect Pauli-spin blockade is observed in the spin-selective absorption spectrum as well as stimulated emission. While electron and hole tunneling from single quantum dots is shown to be well explained by the WKB formalism, for coupled quantum dots pronounced resonances in the electron tunneling rate are observed arising from elastic and inelastic electron tunneling between the different dots. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Ultrafast optical signal processing using semiconductor quantum dot amplifiers

DEFF Research Database (Denmark)

Berg, Tommy Winther; Mørk, Jesper

2002-01-01

The linear and nonlinear properties of quantum dot amplifiers are discussed on the basis of an extensive theoretical model. These devices show great potential for linear amplification as well as ultrafast signal processing.......The linear and nonlinear properties of quantum dot amplifiers are discussed on the basis of an extensive theoretical model. These devices show great potential for linear amplification as well as ultrafast signal processing....

Ultrafast Thermal Transport at Interfaces

Energy Technology Data Exchange (ETDEWEB)

Cahill, David [Univ. of Illinois, Champaign, IL (United States); Murphy, Catherine [Univ. of Illinois, Champaign, IL (United States); Martin, Lane [Univ. of Illinois, Champaign, IL (United States)

2014-10-21

Our research program on Ultrafast Thermal Transport at Interfaces advanced understanding of the mesoscale science of heat conduction. At the length and time scales of atoms and atomic motions, energy is transported by interactions between single-particle and collective excitations. At macroscopic scales, entropy, temperature, and heat are the governing concepts. Key gaps in fundamental knowledge appear at the transitions between these two regimes. The transport of thermal energy at interfaces plays a pivotal role in these scientific issues. Measurements of heat transport with ultrafast time resolution are needed because picoseconds are the fundamental scales where the lack of equilibrium between various thermal excitations becomes a important factor in the transport physics. A critical aspect of our work has been the development of experimental methods and model systems that enabled more precise and sensitive investigations of nanoscale thermal transport.

Investigation on properties of ultrafast switching in a bulk gallium arsenide avalanche semiconductor switch

International Nuclear Information System (INIS)

Hu, Long; Su, Jiancang; Ding, Zhenjie; Hao, Qingsong; Yuan, Xuelin

2014-01-01

Properties of ultrafast switching in a bulk gallium arsenide (GaAs) avalanche semiconductor switch based on semi-insulating wafer, triggered by an optical pulse, were analyzed using physics-based numerical simulations. It has been demonstrated that when a voltage with amplitude of 5.2 kV is applied, after an exciting optical pulse with energy of 1 μJ arrival, the structure with thickness of 650 μm reaches a high conductivity state within 110 ps. Carriers are created due to photons absorption, and electrons and holes drift to anode and cathode terminals, respectively. Static ionizing domains appear both at anode and cathode terminals, and create impact-generated carriers which contribute to the formation of electron-hole plasma along entire channel. When the electric field in plasma region increases above the critical value (∼4 kV/cm) at which the electrons drift velocity peaks, a domain comes into being. An increase in carrier concentration due to avalanche multiplication in the domains reduces the domain width and results in the formation of an additional domain as soon as the field outside the domains increases above ∼4 kV/cm. The formation and evolution of multiple powerfully avalanching domains observed in the simulations are the physical reasons of ultrafast switching. The switch exhibits delayed breakdown with the characteristics affected by biased electric field, current density, and optical pulse energy. The dependence of threshold energy of the exciting optical pulse on the biased electric field is discussed

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

Directory of Open Access Journals (Sweden)

Yulu Huang

2016-08-01

Full Text Available 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 (150  mA-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 repetition 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. Off-axis injection and extraction issues and beam optics using a multicavity kick-drift scheme will also be discussed.

First-principles interatomic potentials for transition-metal aluminides. III. Extension to ternary phase diagrams

International Nuclear Information System (INIS)

Widom, Mike; Al-Lehyani, Ibrahim; Moriarty, John A.

2000-01-01

Modeling structural and mechanical properties of intermetallic compounds and alloys requires detailed knowledge of their interatomic interactions. The first two papers of this series [Phys. Rev. B 56, 7905 (1997); 58, 8967 (1998)] derived first-principles interatomic potentials for transition-metal (TM) aluminides using generalized pseudopotential theory (GPT). Those papers focused on binary alloys of aluminum with first-row transition metals and assessed the ability of GPT potentials to reproduce and elucidate the alloy phase diagrams of Al-Co and Al-Ni. This paper addresses the phase diagrams of the binary alloy Al-Cu and the ternary systems Al-Co-Cu and Al-Co-Ni, using GPT pair potentials calculated in the limit of vanishing transition-metal concentration. Despite this highly simplifying approximation, we find rough agreement with the known low-temperature phase diagrams, up to 50% total TM concentration provided the Co fraction is below 25%. Full composition-dependent potentials and many-body interactions would be required to correct deficiencies at higher Co concentration. Outside this troublesome region, the experimentally determined stable and metastable phases all lie on or near the convex hull of a scatter plot of energy versus composition. We verify, qualitatively, reported solubility ranges extending binary alloys into the ternary diagram in both Al-Co-Cu and Al-Co-Ni. Finally, we reproduce previously conjectured transition-metal positions in the decagonal quasicrystal phase. (c) 2000 The American Physical Society

Changes in the vibrational energies and interatomic spacings upon the formation of vacancies in the volume and in the cores of crystallite conjugation regions of polycrystalline transition metals with cubic lattices

International Nuclear Information System (INIS)

Klotsman, S.M.; Timofeev, A.N.

2008-01-01

Measured changes (ε vac ) i,j of vibrational energy on vacancies formation in i-fields (in volumes and nuclei of crystallite conjugation regions of polycrystalline metals (CCR-PM)): Cr, Mo, Ta, W, Cu, Ir are presented. Changes ε vol of vibrational energy of vacancy nearest environment formed in the metal volume, changes ε FCC of vibrational energy when vacancies formation in CCR nuclei of BCC- and FCC lattices transition metals are discussed. Measured changes ε FCC of vibrational energy, u FCC potential energy and determined sign of interatomic distances changes Δa FCC when formation of split vacancy in the FCC-lattice CCR-PM, changes ε BCC of vibrational energy, u BCC potential energy and determined sign of Δa BCC changes of interatomic distances when vacancies formation in the BCC-lattice CCR-PM are demonstrated. It is noted that the increase of interatomic distances when vacancies formation in the BCC-lattice CCR nucleus of transition metals is conditioned by the the appearance of vacancies alternative structure. Properties of CCR-PM nuclei are more sensitive to interatomic distances changes in the vacancies environment, than to changes of its nearest neighbours numbers [ru

Ultrafast vibrations of gold nanorings

DEFF Research Database (Denmark)

Kelf, T; Tanaka, Y; Matsuda, O

2011-01-01

We investigate the vibrational modes of gold nanorings on a silica substrate with an ultrafast optical technique. By comparison with numerical simulations, we identify several resonances in the gigahertz range associated with axially symmetric deformations of the nanoring and substrate. We...

Ultrafast Spectroscopy of Semiconductor Devices

DEFF Research Database (Denmark)

Borri, Paola; Langbein, Wolfgang; Hvam, Jørn Marcher

1999-01-01

In this work we present an experimental technique for investigating ultrafast carrier dynamics in semiconductor optical amplifiers at room temperature. These dynamics, influenced by carrier heating, spectral hole-burning and two-photon absorption, are very important for device applications in inf...

Ultrafast Mid-Infrared Intra-Excitonic Response of Individualized Single-Walled Carbon Nanotubes

International Nuclear Information System (INIS)

Wang, Jigang; Graham, Matt W.; Ma, Yingzhong; Fleming, Graham R.; Kaindl, Robert A.

2009-01-01

The quasi-1D confinement and reduced screening of photoexcited charges in single-walled carbon nanotubes (SWNTs) entails strongly-enhanced Coulomb interactions and exciton binding energies. Such amplified electron-hole (e-h) correlations have important implications for both fundamental physics and optoelectronic applications of nanotubes. The availability of 'individualized' SWNT ensembles with bright and structured luminescence has rendered specific tube chiralities experimentally accessible. In these samples, evidence for excitonic behavior was found in absorption-luminescence maps, two-photon excited luminescence, or ultrafast carrier dynamics. Here, we report ultrafast mid-infrared (mid-IR) studies of individualized SWNTs, evidencing strong photoinduced absorption around 200 meV in semiconducting tubes of (6,5) and (7,5) chiralities. This manifests the observation of quasi-1D intra-excitonic transitions between different relative-momentum states, in agreement with the binding energy and calculated oscillator strength. Our measurements further reveal a saturation of the photoinduced absorption with increasing phase-space filling of the correlated e-h pairs. The transient mid-IR response represents a new tool, unhindered by restrictions of momentum or interband dipole moment, to investigate the density and dynamics of SWNT excitons.

Ultrafast control and monitoring of material properties using terahertz pulses

Energy Technology Data Exchange (ETDEWEB)

Bowlan, Pamela Renee [Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Lab. for Ultrafast Materials Optical Science (LUMOS)

2016-05-02

These are a set of slides on ultrafast control and monitoring of material properties using terahertz pulses. A few of the topics covered in these slides are: How fast is a femtosecond (fs), Different frequencies probe different properties of molecules or solids, What can a THz pulse do to a material, Ultrafast spectroscopy, Generating and measuring ultrashort THz pulses, Tracking ultrafast spin dynamics in antiferromagnets through spin wave resonances, Coherent two-dimensional THz spectroscopy, and Probing vibrational dynamics at a surface. Conclusions are: Coherent two-dimensional THz spectroscopy: a powerful approach for studying coherence and dynamics of low energy resonances. Applying this to graphene we investigated the very strong THz light mater interaction which dominates over scattering. Useful for studying coupled excitations in multiferroics and monitoring chemical reactions. Also, THz-pump, SHG-probe spectoscopy: an ultrafast, surface sensitive probe of atomic-scale symmetry changes and nonlinear phonon dymanics. We are using this in Bi₂Se₃ to investigate the nonlinear surface phonon dynamics. This is potentially very useful for studying catalysis.

Electrically-driven GHz range ultrafast graphene light emitter (Conference Presentation)

Science.gov (United States)

Kim, Youngduck; Gao, Yuanda; Shiue, Ren-Jye; Wang, Lei; Aslan, Ozgur Burak; Kim, Hyungsik; Nemilentsau, Andrei M.; Low, Tony; Taniguchi, Takashi; Watanabe, Kenji; Bae, Myung-Ho; Heinz, Tony F.; Englund, Dirk R.; Hone, James

2017-02-01

Ultrafast electrically driven light emitter is a critical component in the development of the high bandwidth free-space and on-chip optical communications. Traditional semiconductor based light sources for integration to photonic platform have therefore been heavily studied over the past decades. However, there are still challenges such as absence of monolithic on-chip light sources with high bandwidth density, large-scale integration, low-cost, small foot print, and complementary metal-oxide-semiconductor (CMOS) technology compatibility. Here, we demonstrate the first electrically driven ultrafast graphene light emitter that operate up to 10 GHz bandwidth and broadband range (400 1600 nm), which are possible due to the strong coupling of charge carriers in graphene and surface optical phonons in hBN allow the ultrafast energy and heat transfer. In addition, incorporation of atomically thin hexagonal boron nitride (hBN) encapsulation layers enable the stable and practical high performance even under the ambient condition. Therefore, electrically driven ultrafast graphene light emitters paves the way towards the realization of ultrahigh bandwidth density photonic integrated circuits and efficient optical communications networks.

Bosonic excitations and electron pairing in an electron-doped cuprate superconductor

Science.gov (United States)

Wang, M. C.; Yu, H. S.; Xiong, J.; Yang, Y.-F.; Luo, S. N.; Jin, K.; Qi, J.

2018-04-01

By applying ultrafast optical spectroscopy to electron-doped La1.9Ce0.1CuO4 ±δ , we discern a bosonic mode of electronic origin and provide the evolution of its coupling with the charge carriers as a function of temperature. Our results show that it has the strongest coupling strength near Tc and can fully account for the superconducting pairing. This mode can be associated with the two-dimensional antiferromagnetic spin correlations emerging below a critical temperature T† larger than Tc. Our work may help to establish a quantitative relation between bosonic excitations and superconducting pairing in electron-doped cuprates.

Ultrafast demagnetisation dependence on film thickness: A TDDFT calculation

Science.gov (United States)

Singh, N.; Sharma, S.

2018-04-01

Ferromagnetic materials when subjected to intense laser pulses leads to reduction of their magnetisation on an ultrafast scale. Here, we perform an ab-initio calculation to study the behavior of ultrafast demagnetisation as a function of film thickness for Nickel as compared to the bulk of the material. In thin films surface formation results in amplification of demagnetisation with the percentage of demagnetisation depending upon the film thickness.

Polarization-dependent force driving the Eg mode in bismuth under optical excitation: comparison of first-principles theory with ultra-fast x-ray experiments

Science.gov (United States)

Fahy, Stephen; Murray, Eamonn

2015-03-01

Using first principles electronic structure methods, we calculate the induced force on the Eg (zone centre transverse optical) phonon mode in bismuth immediately after absorption of a ultrafast pulse of polarized light. To compare the results with recent ultra-fast, time-resolved x-ray diffraction experiments, we include the decay of the force due to carrier scattering, as measured in optical Raman scattering experiments, and simulate the optical absorption process, depth-dependent atomic driving forces, and x-ray diffraction in the experimental geometry. We find excellent agreement between the theoretical predictions and the observed oscillations of the x-ray diffraction signal, indicating that first-principles theory of optical absorption is well suited to the calculation of initial atomic driving forces in photo-excited materials following ultrafast excitation. This work is supported by Science Foundation Ireland (Grant No. 12/IA/1601) and EU Commission under the Marie Curie Incoming International Fellowships (Grant No. PIIF-GA-2012-329695).

Electrons from fixed in space molecules and clusters

International Nuclear Information System (INIS)

Doerner, R.; Jahnke, T.; Czasch, A.; Jagutzki, O.; Schmidt-Boecking; Kreidi, K.; Knapp, A.; Schmidt, L.; Schoeffler, M.; Foucar, L.; Cocke, C.L.; Osipov, T.; Alnaser, A.

2004-01-01

Full text: We use modern multi particle momentum imaging techniques (COLTRIMS) to measure the vector momenta of all charged fragments, ions, photoelectrons and Auger electrons for small molecules excited by synchrotron radiation. These complete images of the fragmentation give an umprecedented detailed insight in the molecular photoionization and Auger process. Also latest results on molecular double ionisation and on cluster fragmentation unveiling interatomic coulomb decay will be presented

Femtochemistry and femtobiology ultrafast dynamics in molecular science

CERN Document Server

Douhal, Abderrazzak

2002-01-01

This book contains important contributions from top international scientists on the-state-of-the-art of femtochemistry and femtobiology at the beginning of the new millennium. It consists of reviews and papers on ultrafast dynamics in molecular science.The coverage of topics highlights several important features of molecular science from the viewpoint of structure (space domain) and dynamics (time domain). First of all, the book presents the latest developments, such as experimental techniques for understanding ultrafast processes in gas, condensed and complex systems, including biological mol

An injector for the proposed Berkeley Ultrafast X-Ray Light Source

International Nuclear Information System (INIS)

Lidia, Steven; Corlett, John; Pusina, Jan; Staples, John; Zholents, Alexander

2003-01-01

Berkeley Lab has proposed to build a recirculating linac based X-ray source for ultra-fast dynamic studies [1]. This machine requires a flat electron beam with a small vertical emittance and large x/y emittance ratio to allow for compression of spontaneous undulator emission of soft and hard x-ray pulses, and a low-emittance, round electron beam for coherent emission of soft x-rays via the FEL process based on cascaded harmonic generation [2]. We propose an injector system consisting of two high gradient high repetition rate photo cathode guns [3] (one for each application), an ∼120 MeV super conducting linear accelerator, a 3rd harmonic cavity for linearization of the longitudinal phase space, and a bunch compressor. We present details of the design and the results of particle tracking studies using several computer codes

Ultrafast vibrations of gold nanorings

DEFF Research Database (Denmark)

Kelf, T; Tanaka, Y; Matsuda, O

2011-01-01

We investigate the vibrational modes of gold nanorings on a silica substrate with an ultrafast optical technique. By comparison with numerical simulations, we identify several resonances in the gigahertz range associated with axially symmetric deformations of the nanoring and substrate. We elucid...

Atomistic simulations of TeO₂-based glasses: interatomic potentials and molecular dynamics.

Science.gov (United States)

Gulenko, Anastasia; Masson, Olivier; Berghout, Abid; Hamani, David; Thomas, Philippe

2014-07-21

In this work we present for the first time empirical interatomic potentials that are able to reproduce TeO2-based systems. Using these potentials in classical molecular dynamics simulations, we obtained first results for the pure TeO2 glass structure model. The calculated pair distribution function is in good agreement with the experimental one, which indicates a realistic glass structure model. We investigated the short- and medium-range TeO2 glass structures. The local environment of the Te atom strongly varies, so that the glass structure model has a broad Q polyhedral distribution. The glass network is described as weakly connected with a large number of terminal oxygen atoms.

Ultrafast surface-enhanced Raman spectroscopy.

Science.gov (United States)

Keller, Emily L; Brandt, Nathaniel C; Cassabaum, Alyssa A; Frontiera, Renee R

2015-08-07

Ultrafast surface-enhanced Raman spectroscopy (SERS) with pico- and femtosecond time resolution has the ability to elucidate the mechanisms by which plasmons mediate chemical reactions. Here we review three important technological advances in these new methodologies, and discuss their prospects for applications in areas including plasmon-induced chemistry and sensing at very low limits of detection. Surface enhancement, arising from plasmonic materials, has been successfully incorporated with stimulated Raman techniques such as femtosecond stimulated Raman spectroscopy (FSRS) and coherent anti-Stokes Raman spectroscopy (CARS). These techniques are capable of time-resolved measurement on the femtosecond and picosecond time scale and can be used to follow the dynamics of molecules reacting near plasmonic surfaces. We discuss the potential application of ultrafast SERS techniques to probe plasmon-mediated processes, such as H2 dissociation and solar steam production. Additionally, we discuss the possibilities for high sensitivity SERS sensing using these stimulated Raman spectroscopies.

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

International Nuclear Information System (INIS)

Thompson, A.P.; Swiler, L.P.; Trott, C.R.; Foiles, S.M.; Tucker, G.J.

2015-01-01

We present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

Energy Technology Data Exchange (ETDEWEB)

Thompson, Aidan P. [Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States). Multiscale Science Dept.; Swiler, Laura P. [Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States). Optimization and Uncertainty Quantification Dept.; Trott, Christian R. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Scalable Algorithms Dept.; Foiles, Stephen M. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Computational Materials and Data Science Dept.; Tucker, Garritt J. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Computational Materials and Data Science Dept.; Drexel Univ., Philadelphia, PA (United States). Dept. of Materials Science and Engineering

2015-03-15

Here, we present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

Energy Technology Data Exchange (ETDEWEB)

Thompson, A.P., E-mail: athomps@sandia.gov [Multiscale Science Department, Sandia National Laboratories, PO Box 5800, MS 1322, Albuquerque, NM 87185 (United States); Swiler, L.P., E-mail: lpswile@sandia.gov [Optimization and Uncertainty Quantification Department, Sandia National Laboratories, PO Box 5800, MS 1318, Albuquerque, NM 87185 (United States); Trott, C.R., E-mail: crtrott@sandia.gov [Scalable Algorithms Department, Sandia National Laboratories, PO Box 5800, MS 1322, Albuquerque, NM 87185 (United States); Foiles, S.M., E-mail: foiles@sandia.gov [Computational Materials and Data Science Department, Sandia National Laboratories, PO Box 5800, MS 1411, Albuquerque, NM 87185 (United States); Tucker, G.J., E-mail: gtucker@coe.drexel.edu [Computational Materials and Data Science Department, Sandia National Laboratories, PO Box 5800, MS 1411, Albuquerque, NM 87185 (United States); Department of Materials Science and Engineering, Drexel University, Philadelphia, PA 19104 (United States)

2015-03-15

We present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.

Role of coherence and delocalization in photo-induced electron transfer at organic interfaces

Science.gov (United States)

Abramavicius, V.; Pranculis, V.; Melianas, A.; Inganäs, O.; Gulbinas, V.; Abramavicius, D.

2016-09-01

Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fullerene derivative PCBM using the stochastic Schrödinger equation (SSE) and reveal the complex time evolution of electron transfer, mediated by electronic coherence and delocalization. By fitting the model to ultrafast charge separation experiments, we estimate the extent of electron delocalization and establish the transition from coherent electron propagation to incoherent hopping. Our results indicate that even a relatively weak coupling between PCBM molecules is sufficient to facilitate electron delocalization and efficient charge separation at organic interfaces.

Ultra-fast movies of thin-film laser ablation

Science.gov (United States)

Domke, Matthias; Rapp, Stephan; Schmidt, Michael; Huber, Heinz P.

2012-11-01

Ultra-short-pulse laser irradiation of thin molybdenum films from the glass substrate side initiates an intact Mo disk lift off free from thermal effects. For the investigation of the underlying physical effects, ultra-fast pump-probe microscopy is used to produce stop-motion movies of the single-pulse ablation process, initiated by a 660-fs laser pulse. The ultra-fast dynamics in the femtosecond and picosecond ranges are captured by stroboscopic illumination of the sample with an optically delayed probe pulse of 510-fs duration. The nanosecond and microsecond delay ranges of the probe pulse are covered by an electronically triggered 600-ps laser. Thus, the setup enables an observation of general laser ablation processes from the femtosecond delay range up to the final state. A comparison of time- and space-resolved observations of film and glass substrate side irradiation of a 470-nm molybdenum layer reveals the driving mechanisms of the Mo disk lift off initiated by glass-side irradiation. Observations suggest that a phase explosion generates a liquid-gas mixture in the molybdenum/glass interface about 10 ps after the impact of the pump laser pulse. Then, a shock wave and gas expansion cause the molybdenum layer to bulge, while the enclosed liquid-gas mixture cools and condenses at delay times in the 100-ps range. The bulging continues for approximately 20 ns, when an intact Mo disk shears and lifts off at a velocity of above 70 m/s. As a result, the remaining hole is free from thermal effects.

Ultrafast gas switching experiments

International Nuclear Information System (INIS)

Frost, C.A.; Martin, T.H.; Patterson, P.E.; Rinehart, L.F.; Rohwein, G.J.; Roose, L.D.; Aurand, J.F.; Buttram, M.T.

1993-01-01

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 Khz at > 100 kV/m E field

Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

Science.gov (United States)

Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

2015-10-01

Optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recovery time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.

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

Science.gov (United States)

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.

Ultrafast magnetization dynamics

OpenAIRE

Woodford, Simon

2008-01-01

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

An atomic string model for a screw dislocation in iron: Implications for the development of interatomic potentials

International Nuclear Information System (INIS)

Gilbert, M.R.; Dudarev, S.L.; Chiesa, S.; Derlet, P.M.

2009-01-01

Thermally activated motion of screw dislocations is the rate-determining mechanism for plastic deformation and fracture of body centred cubic (bcc) metals and alloys. Recent experimental observations by S.G. Roberts' group at Oxford showed that ductile-brittle behaviour of bcc vanadium, tungsten, pure iron, and iron-chromium alloys is controlled by an Arrhenius process in which the energy for thermal activation is proportional to the formation energy for a double kink on a b= 1/2 screw dislocation, where b is the Burgers vector of the dislocation. Interpreting these experimental observations and extending the analysis to the case of irradiated materials requires developing a full quantitative treatment for perfect and kinked screw dislocations. Modelling screw dislocations also presents a challenge for the development of interatomic potentials. Recent density functional theory (DFT) calculations have revealed that the ground-state structure of the core of screw dislocations in all the bcc transition metals is non-degenerate and symmetric, whereas inter-atomic potentials used in molecular dynamics simulations for these metals often predict a degenerate, symmetry-broken core-structure. In this work we show how, by treating the structure of a screw dislocation within a multistring Frenkel-Kontorova model, we can develop a criterion that guarantees the correct symmetric core of the dislocation. Extending this treatment, we find a systematic recipe for constructing Finnis-Sinclair-type potentials that are able, as a matter of routine, produce non-degenerate core structures of 1/2 screw dislocations. Modelling thermally activated mobility of screw dislocations also requires that the transition pathway between stable core positions of a dislocation is accurately reproduced. DFT data indicates that the shape of the 'Peierls energy barrier' is a single-hump curve, including transitional configurations close to the so-called 'hard' structure. Interatomic potentials have, up

Theoretical study of the elasticity, mechanical behavior, electronic structure, interatomic bonding, and dielectric function of an intergranular glassy film model in prismatic β-Si3N4

International Nuclear Information System (INIS)

Ching, W. Y.; Rulis, Paul; Aryal, Sitaram; Ouyang, Lizhi; Misra, Anil

2010-01-01

Microstructures such as intergranular glassy films (IGFs) are ubiquitous in many structural ceramics. They control many of the important physical properties of polycrystalline ceramics and can be influenced during processing to modify the performance of devices that contain them. In recent years, there has been intense research, both experimentally and computationally, on the structure and properties of IGFs. Unlike grain boundaries or dislocations with well-defined crystalline planes, the atomic scale structure of IGFs, their fundamental electronic interactions, and their bonding characteristics are far more complicated and not well known. In this paper, we present the results of theoretical simulations using ab initio methods on an IGF model in β-Si 3 N 4 with prismatic crystalline planes. The 907-atom model has a dimension of 14.533 A x 15.225 A x 47.420 A . The IGF layer is perpendicular to the z axis, 16.4 A wide, and contains 72 Si, 32 N, and 124 O atoms. Based on this model, the mechanical and elastic properties, the electronic structure, the interatomic bonding, the localization of defective states, the distribution of electrostatic potential, and the optical dielectric function are evaluated and compared with crystalline β-Si 3 N 4 . We have also performed a theoretical tensile experiment on this model by incrementally extending the structure in the direction perpendicular to the IGF plane until the model fully separated. It is shown that fracture occurs at a strain of 9.42% with a maximum stress of 13.9 GPa. The fractured segments show plastic behavior and the formation of surfacial films on the β-Si 3 N 4 . These results are very different from those of a previously studied basal plane model [J. Chen et al., Phys. Rev. Lett. 95, 256103 (2005)] and add insights to the structure and behavior of IGFs in polycrystalline ceramics. The implications of these results and the need for further investigations are discussed.

Tissue strain rate estimator using ultrafast IQ complex data

OpenAIRE

TERNIFI , Redouane; Elkateb Hachemi , Melouka; Remenieras , Jean-Pierre

2012-01-01

International audience; Pulsatile motion of brain parenchyma results from cardiac and breathing cycles. In this study, transient motion of brain tissue was estimated using an Aixplorer® imaging system allowing an ultrafast 2D acquisition mode. The strain was computed directly from the ultrafast IQ complex data using the extended autocorrelation strain estimator (EASE), which provides great SNRs regardless of depth. The EASE first evaluates the autocorrelation function at each depth over a set...

Interatomic Potential to Simulate Radiation Damage in Fe-Cr Alloys

International Nuclear Information System (INIS)

Bonny, G.; Pasianot, R.; Terentyev, D.; Malerba, L.

2011-01-01

The report presents an Fe-Cr interatomic potential to model high-Cr ferritic alloys. The potential is fitted to thermodynamic and point-defect properties obtained from density functional theory (DFT) calculations and experiments. The developed potential is also benchmarked against other potentials available in literature. It shows particularly good agreement with the DFT obtained mixing enthalpy of the random alloy, the formation energy of intermetallics and experimental excess vibrational entropy and phase diagram. In addition, DFT calculated point-defect properties, both interstitial and substitutional, are well reproduced, as is the screw dislocation core structure. As a first validation of the potential, we study the precipitation hardening of Fe-Cr alloys via static simulations of the interaction between Cr precipitates and screw dislocations. It is concluded that the description of the dislocation core modification near a precipitate might have a significant influence on the interaction mechanisms observed in dynamic simulations.

Interatomic Potential to Simulate Radiation Damage in Fe-Cr Alloys

Energy Technology Data Exchange (ETDEWEB)

Bonny, G.; Pasianot, R.; Terentyev, D.; Malerba, L.

2011-03-15

The report presents an Fe-Cr interatomic potential to model high-Cr ferritic alloys. The potential is fitted to thermodynamic and point-defect properties obtained from density functional theory (DFT) calculations and experiments. The developed potential is also benchmarked against other potentials available in literature. It shows particularly good agreement with the DFT obtained mixing enthalpy of the random alloy, the formation energy of intermetallics and experimental excess vibrational entropy and phase diagram. In addition, DFT calculated point-defect properties, both interstitial and substitutional, are well reproduced, as is the screw dislocation core structure. As a first validation of the potential, we study the precipitation hardening of Fe-Cr alloys via static simulations of the interaction between Cr precipitates and screw dislocations. It is concluded that the description of the dislocation core modification near a precipitate might have a significant influence on the interaction mechanisms observed in dynamic simulations.

Observing Structure and Motion in Molecules with Ultrafast Strong Field and Short Wavelength Laser Radiation

Energy Technology Data Exchange (ETDEWEB)

Bucksbaum, Philip H

2011-04-13

The term "molecular movie" has come to describe efforts to track and record Angstrom-scale coherent atomic and electronic motion in a molecule. The relevant time scales for this range cover several orders of magnitude, from sub-femtosecond motion associated with electron-electron correlations, to 100-fs internal vibrations, to multi-picosecond motion associated with the dispersion and quantum revivals of molecular reorientation. Conventional methods of cinematography do not work well in this ultrafast and ultrasmall regime, but stroboscopic "pump and probe" techniques can reveal this motion with high fidelity. This talk will describe some of the methods and recent progress in exciting and controlling this motion, using both laboratory lasers and the SLAC Linac Coherent Light Source x-ray free electron laser, and will further try to relate the date to the goal of molecular movies.

Patellofemoral joint motion: Evaluation by ultrafast computed tomography

International Nuclear Information System (INIS)

Stanford, W.; Phelan, J.; Kathol, M.H.; Rooholamini, S.A.; El-Khoury, G.Y.; Palutsis, G.R.; Albright, J.P.

1988-01-01

Patellofemoral maltracking is a recognized cause of peripatellar pain. Clinicians currently rely on observation, palpation, and static radiographic images to evaluate the symptomatic patient. Ultrafast computed tomography (ultrafast CT) offers objective observations of the dynamic influences of muscle contraction on the patellofemoral joint as the knee is actively moved through a range of motion from 90 0 C flexion of full extension. This study reports our initial observations and establishes a range of normal values so that patients with a clinical suspicion of patellar maltracking may be evaluated. (orig./GDG)

Patellofemoral joint motion: Evaluation by ultrafast computed tomography

Energy Technology Data Exchange (ETDEWEB)

Stanford, W.; Phelan, J.; Kathol, M.H.; Rooholamini, S.A.; El-Khoury, G.Y.; Palutsis, G.R.; Albright, J.P.

1988-10-01

Patellofemoral maltracking is a recognized cause of peripatellar pain. Clinicians currently rely on observation, palpation, and static radiographic images to evaluate the symptomatic patient. Ultrafast computed tomography (ultrafast CT) offers objective observations of the dynamic influences of muscle contraction on the patellofemoral joint as the knee is actively moved through a range of motion from 90/sup 0/C flexion of full extension. This study reports our initial observations and establishes a range of normal values so that patients with a clinical suspicion of patellar maltracking may be evaluated. (orig./GDG).

Femtosecond Soft X-ray Spectroscopy of Solvated Transition-Metal Complexes: Deciphering the Interplay of Electronic and Structural Dynamics

Energy Technology Data Exchange (ETDEWEB)

Huse, Nils; Cho, Hana; Hong, Kiryong; Jamula, Lindsey; de Groot, Frank M. F.; Kim, Tae Kyu; McCusker, James K.; Schoenlein, Robert W.

2011-04-21

We present the first implementation of femtosecond soft X-ray spectroscopy as an ultrafast direct probe of the excited-state valence orbitals in solution-phase molecules. This method is applied to photoinduced spin crossover of [Fe(tren(py)3)]2+, where the ultrafast spinstate conversion of the metal ion, initiated by metal-to-ligand charge-transfer excitation, is directly measured using the intrinsic spin-state selectivity of the soft X-ray L-edge transitions. Our results provide important experimental data concerning the mechanism of ultrafast spin-state conversion and subsequent electronic and structural dynamics, highlighting the potential of this technique to study ultrafast phenomena in the solution phase.

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

Directory of Open Access Journals (Sweden)

Jérémy R. Rouxel

2017-07-01

Full Text Available Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. We present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O provide different local windows onto the parity breaking geometry change thus revealing the enantiomer asymmetry.

Silicon based ultrafast optical waveform sampling

DEFF Research Database (Denmark)

Ji, Hua; Galili, Michael; Pu, Minhao

2010-01-01

A 300 nmx450 nmx5 mm silicon nanowire is designed and fabricated for a four wave mixing based non-linear optical gate. Based on this silicon nanowire, an ultra-fast optical sampling system is successfully demonstrated using a free-running fiber laser with a carbon nanotube-based mode-locker as th......A 300 nmx450 nmx5 mm silicon nanowire is designed and fabricated for a four wave mixing based non-linear optical gate. Based on this silicon nanowire, an ultra-fast optical sampling system is successfully demonstrated using a free-running fiber laser with a carbon nanotube-based mode......-locker as the sampling source. A clear eye-diagram of a 320 Gbit/s data signal is obtained. The temporal resolution of the sampling system is estimated to 360 fs....

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.

Science.gov (United States)

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

2013-12-01

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.

A tungsten-rhenium interatomic potential for point defect studies

Science.gov (United States)

Setyawan, Wahyu; Gao, Ning; Kurtz, Richard J.

2018-05-01

A tungsten-rhenium (W-Re) classical interatomic potential is developed within the embedded atom method interaction framework. A force-matching method is employed to fit the potential to ab initio forces, energies, and stresses. Simulated annealing is combined with the conjugate gradient technique to search for an optimum potential from over 1000 initial trial sets. The potential is designed for studying point defects in W-Re systems. It gives good predictions of the formation energies of Re defects in W and the binding energies of W self-interstitial clusters with Re. The potential is further evaluated for describing the formation energy of structures in the σ and χ intermetallic phases. The predicted convex-hulls of formation energy are in excellent agreement with ab initio data. In pure Re, the potential can reproduce the formation energies of vacancies and self-interstitial defects sufficiently accurately and gives the correct ground state self-interstitial configuration. Furthermore, by including liquid structures in the fit, the potential yields a Re melting temperature (3130 K) that is close to the experimental value (3459 K).

Ultrafast light matter interaction in CdSe/ZnS core-shell quantum dots

Science.gov (United States)

Yadav, Rajesh Kumar; Sharma, Rituraj; Mondal, Anirban; Adarsh, K. V.

2018-04-01

Core-shell quantum dot are imperative for carrier (electron and holes) confinement in core/shell, which provides a stage to explore the linear and nonlinear optical phenomena at the nanoscalelimit. Here we present a comprehensive study of ultrafast excitation dynamics and nonlinear optical absorption of CdSe/ZnS core shell quantum dot with the help of ultrafast spectroscopy. Pump-probe and time-resolved measurements revealed the drop of trapping at CdSe surface due to the presence of the ZnS shell, which makes more efficient photoluminescence. We have carried out femtosecond transient absorption studies of the CdSe/ZnS core-shell quantum dot by irradiation with 400 nm laser light, monitoring the transients in the visible region. The optical nonlinearity of the core-shell quantum dot studied by using the Z-scan technique with 120 fs pulses at the wavelengths of 800 nm. The value of two photon absorption coefficients (β) of core-shell QDs extracted as80cm/GW, and it shows excellent benchmark for the optical limiting onset of 2.5GW/cm2 with the low limiting differential transmittance of 0.10, that is an order of magnitude better than graphene based materials.

Transient state of electron transport in semiconductors: over velocity and ballistic effect

International Nuclear Information System (INIS)

Laval, S.

1984-01-01

As the dimensions of the active regions of electronic components are reduced, transient effects must be considered when electrons encounter a high electric field gradient. The electron velocity can overshoot its stationary value over a few tenths of a micron and during about one picosecond. This has been observed experimentally and permits to forecast new ultrafast electronic devices [fr

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

KAUST Repository

Mohammed, Omar F.

2014-05-01

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

Real-time control of ultrafast laser micromachining by laser-induced breakdown spectroscopy

International Nuclear Information System (INIS)

Tong Tao; Li Jinggao; Longtin, Jon P.

2004-01-01

Ultrafast laser micromachining provides many advantages for precision micromachining. One challenging problem, however, particularly for multilayer and heterogeneous materials, is how to prevent a given material from being ablated, as ultrafast laser micromachining is generally material insensitive. We present a real-time feedback control system for an ultrafast laser micromachining system based on laser-induced breakdown spectroscopy (LIBS). The characteristics of ultrafast LIBS are reviewed and discussed so as to demonstrate the feasibility of the technique. Comparison methods to identify the material emission patterns are developed, and several of the resulting algorithms were implemented into a real-time computer control system. LIBS-controlled micromachining is demonstrated for the fabrication of microheater structures on thermal sprayed materials. Compared with a strictly passive machining process without any such feedback control, the LIBS-based system provides several advantages including less damage to the substrate layer, reduced machining time, and more-uniform machining features

Spin-controlled ultrafast vertical-cavity surface-emitting lasers

Science.gov (United States)

Höpfner, Henning; Lindemann, Markus; Gerhardt, Nils C.; Hofmann, Martin R.

2014-05-01

Spin-controlled semiconductor lasers are highly attractive spintronic devices providing characteristics superior to their conventional purely charge-based counterparts. In particular, spin-controlled vertical-cavity surface emitting lasers (spin-VCSELs) promise to offer lower thresholds, enhanced emission intensity, spin amplification, full polarization control, chirp control and ultrafast dynamics. Most important, the ability to control and modulate the polarization state of the laser emission with extraordinarily high frequencies is very attractive for many applications like broadband optical communication and ultrafast optical switches. We present a novel concept for ultrafast spin-VCSELs which has the potential to overcome the conventional speed limitation for directly modulated lasers by the relaxation oscillation frequency and to reach modulation frequencies significantly above 100 GHz. The concept is based on the coupled spin-photon dynamics in birefringent micro-cavity lasers. By injecting spin-polarized carriers in the VCSEL, oscillations of the coupled spin-photon system can by induced which lead to oscillations of the polarization state of the laser emission. These oscillations are decoupled from conventional relaxation oscillations of the carrier-photon system and can be much faster than these. Utilizing these polarization oscillations is thus a very promising approach to develop ultrafast spin-VCSELs for high speed optical data communication in the near future. Different aspects of the spin and polarization dynamics, its connection to birefringence and bistability in the cavity, controlled switching of the oscillations, and the limitations of this novel approach will be analysed theoretically and experimentally for spin-polarized VCSELs at room temperature.

Ultrafast Terahertz Conductivity of Photoexcited Nanocrystalline Silicon

DEFF Research Database (Denmark)

Cooke, David; MacDonald, A. Nicole; Hryciw, Aaron

2007-01-01

The ultrafast transient ac conductivity of nanocrystalline silicon films is investigated using time-resolved terahertz spectroscopy. While epitaxial silicon on sapphire exhibits a free carrier Drude response, silicon nanocrystals embedded in glass show a response that is best described by a class...... in the silicon nanocrystal films is dominated by trapping at the Si/SiO2 interface states, occurring on a 1–100 ps time scale depending on particle size and hydrogen passivation......The ultrafast transient ac conductivity of nanocrystalline silicon films is investigated using time-resolved terahertz spectroscopy. While epitaxial silicon on sapphire exhibits a free carrier Drude response, silicon nanocrystals embedded in glass show a response that is best described...

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

KAUST Repository

Alsulami, Qana

2016-04-10

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

Development of functional materials by using ultrafast laser pulses

Science.gov (United States)

Shimotsuma, Y.; Sakakura, M.; Miura, K.

2018-01-01

The polarization-dependent periodic nanostructures inside various materials are successfully induced by ultrafast laser pulses. The periodic nanostructures in various materials can be empirically classified into the following three types: (1) structural deficiency, (2) expanded structure, (3) partial phase separation. Such periodic nanostructures exhibited not only optical anisotropy but also intriguing electric, thermal, and magnetic properties. The formation mechanisms of the periodic nanostructure was interpreted in terms of the interaction between incident light field and the generated electron plasma. Furthermore, the fact that the periodic nanostructures in semiconductors could be formed empirically only if it is indirect bandgap semiconductor materials indicates the stress-dependence of bandgap structure and/or the recombination of the excited electrons are also involved to the nanostructure formation. More recently we have also confirmed that the periodic nanostructures in glass are related to whether a large amount of non-bridged oxygen is present. In the presentation, we demonstrate new possibilities for functionalization of common materials ranging from an eternal 5D optical storage, a polarization imaging, to a thermoelectric conversion, based on the indicated phenomena.

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

Science.gov (United States)

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-05-08

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification

Chirped pulse digital holography for measuring the sequence of ultrafast optical wavefronts

Science.gov (United States)

Karasawa, Naoki

2018-04-01

Optical setups for measuring the sequence of ultrafast optical wavefronts using a chirped pulse as a reference wave in digital holography are proposed and analyzed. In this method, multiple ultrafast object pulses are used to probe the temporal evolution of ultrafast phenomena and they are interfered with a chirped reference wave to record a digital hologram. Wavefronts at different times can be reconstructed separately from the recorded hologram when the reference pulse can be treated as a quasi-monochromatic wave during the pulse width of each object pulse. The feasibility of this method is demonstrated by numerical simulation.

Elastic, electronic properties and intra-atomic bonding in orthorhombic and tetragonal polymorphs of BaZn2As2 from first-principles calculations

International Nuclear Information System (INIS)

Shein, I.R.; Ivanovskii, A.L.

2014-01-01

Highlights: • α and β polymorphs of BaZn 2 As 2 as a parent phase of the new DMSs are examined. • Structural, elastic, electronic properties are evaluated from first principles. • Inter-atomic bonding picture is discussed. -- Abstract: Very recently, on the example of hole- and spin-doped BaZn 2 As 2 , quite an unexpected area of potential applications of 122-like phases was proposed as a promising platform for searching the new diluted magnetic semiconductors (DMSs) (2013; K. Zhao, et al, Nature Commun. 4:1442). Herein, by means of the first-principles calculations, we have examined in detail the basic structural, elastic, electronic properties and the peculiarities of the inter-atomic bonding in α and β polymorphs of 122-like BaZn 2 As 2 – a parent phase of the new DMSs. Our characterization of these materials covers the optimized structural parameters, the main elastic parameters (elastic constants, bulk, shear, and Young’s moduli, Poisson’s ratio, anisotropy indexes, and Pugh’s criterion), as well as electronic bands and densities of electronic states

Ultrafast laser-semiconductor interactions

International Nuclear Information System (INIS)

Schile, L.A.

1996-01-01

Studies of the ultrafast (< 100 fs) interactions of infrared, sub-100 fs laser pulses with IR, photosensitive semiconductor materials InGaAs, InSb, and HgCdTe are reported. Both the carrier dynamics and the associated Terahertz radiation from these materials are discussed. The most recent developments of femtosecond (< 100 fs) Optical Parametric Oscillators (OPO) has extended the wavelength range from the visible to 5.2 μm. The photogenerated semiconductor free carrier dynamics are determined in the 77 to 300 degrees K temperature range using the Transmission Correlation Peak (TCP) method. The electron-phonon scattering times are typically 200 - 600 fs. Depending upon the material composition and substrate on which the IR crystalline materials are deposited, the nonlinear TCP absorption gives recombination rates as fast as 10's of picoseconds. For the HgCdTe, there exists a 400 fs electron-phonon scattering process along with a much longer 3600 fs loss process. Studies of the interactions of these ultrashort laser pulses with semiconductors produce Terahertz (Thz) radiative pulses. With undoped InSb, there is a substantial change in the spectral content of this THz radiation between 80 - 260 degrees K while the spectrum of Te-doped InSb remains nearly unchanged, an effect attributed to its mobility being dominated by impurity scattering. At 80 degrees K, the terahertz radiation from undoped InSb is dependent on wavelength, with both a higher frequency spectrum and much larger amplitudes generated at longer wavelengths. No such effect is observed at 260 degrees K. Finally, new results on the dependence of the emitted THz radiation on the InSb crystal's orientation is presented

Ultrafast Spectroscopic Noninvasive Probe of Vertical Carrier Transport in Heterostructure Devices

Science.gov (United States)

2016-03-01

ARL-TR-7618 ● MAR 2016 US Army Research Laboratory Ultrafast Spectroscopic Noninvasive Probe of Vertical Carrier Transport in...US Army Research Laboratory Ultrafast Spectroscopic Noninvasive Probe of Vertical Carrier Transport in Heterostructure Devices by Blair C...Spectroscopic Noninvasive Probe of Vertical Carrier Transport in Heterostructure Devices 5a. CONTRACT NUMBER 5b. GRANT NUMBER 5c. PROGRAM ELEMENT

Progress in Ultrafast Intense Laser Science

CERN Document Server

Yamanouchi, Kaoru; Li, Ruxin; Chin, See Leang

2009-01-01

The PUILS series presents Progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science. PUILS has been stimulated by the recent development of ultrafast laser technologies. Each volume contains approximately 15 chapters, authored by researchers at the forefront. Each chapter opens with an overview of the topics to be discussed, so that researchers, who are not experts in the specific topics, as well as graduate students can grasp the importance and attractions of this sub-field of research, and these are followed by reports of cutting-edge discoveries. This fourth volume covers a broad range of topics from this interdisciplinary research field, focusing on strong field ionization of atoms; excitation, ionization and fragmentation of molecules; nonlinear intense optical phenomena and attosecond pulses; and laser - solid interactions and photoemission.

Ultrafast dynamic optical prop erties of graphene%石墨烯超快动态光学性质∗

Institute of Scientific and Technical Information of China (English)

金芹; 董海明; 韩奎; 王雪峰

2015-01-01

Graphene exhibits excellent ultrafast optical properties due to its unique electronic structure. In this paper we investigate theoretically the ultrafast dynamic optical properties of graphene based on the Bloch-equations, and introduce the theoretical model of graphene. First, we give the energy which has a linear relationship with the wave vector k. The behavior of electrons in the vicinity of the two Dirac points can be described by the massless Dirac-equation, thus we have the Dirac equation of graphene. Second, we discuss the interaction between graphene and light field. The Bloch-equations of graphene are obtained through the Heisenberg equation and then we discuss the photon carriers ,electric polarization and optical current change over time by analyzing the Bloch-equations. It is found that the nonequilibrium carriers in graphene induced by a terahertz field can be built in 20–200 fs due to the Pauli blocking and the conservation of energy principle. The photon carrier density will increase with the frequency of enhanced light field. Thus an optical current can be created rapidly within 1 ps. A graphene system responds linearly to the external optical field for √2evFE0t≪~ω, while the graphene systems respond nonlinearly to the external optical field, where E0 andωare respectively the intensity and the frequency of the light, t is the time and vF the Dirac velocity in graphene. The electric polarization and optical current increase with increasing photon energies. These theoretical results are in agreement with recent experimental findings and indicate that graphene exhibits important features and has practical applications in the ultrafast optic filed, especially in terahertz field.

Electronic structure and interatomic bonding in Al10V

International Nuclear Information System (INIS)

Jahnatek, M; Krajci, M; Hafner, J

2003-01-01

On the basis of ab initio calculations we analysed the electron density distribution in the elementary cell of the compound Al 10 V. We found covalent bonding between certain atoms. The Al-V bonds of enhanced covalency are linked into -Al-V-Al-V- chains that extend over the whole crystal. The chains intersect at each V site and together form a Kagome network of corner-sharing tetrahedra. The large voids of this network are filled by Z 16 Friauf polyhedra consisting of Al atoms only. The skeleton of the Friauf polyhedron has the form of a truncated tetrahedron and consists of 12 strongly bonded Al atoms. These Al-Al bonds also have covalent character. The bonding is dominated by sp 2 hybridization. The centre of the Friauf polyhedron may be empty or occupied by an Al atom. The thermodynamic stability of the phase is investigated. The Al 21 V 2 phase with occupied voids is at low temperatures less stable than Al 10 V. The Al 10 V structure can be considered as a special case of the Al 18 Cr 2 Mg 3 structural class. We have found the same picture of bonding as we report here for Al 10 V for several other aluminium-rich alloys belonging to the Al 18 Cr 2 Mg 3 structural class also

Ultrafast Optical Modulation of Second- and Third-Harmonic Generation from Cut-Disk-Based Metasurfaces

KAUST Repository

Sartorello, Giovanni

2016-06-06

We design and fabricate a metasurface composed of gold cut-disk resonators that exhibits a strong coherent nonlinear response. We experimentally demonstrate all-optical modulation of both second- and third-harmonic signals on a subpicosecond time scale. Pump-probe experiments and numerical models show that the observed effects are due to the ultrafast response of the electronic excitations in the metal under external illumination. These effects pave the way for the development of novel active nonlinear metasurfaces with controllable and switchable coherent nonlinear response. © 2016 American Chemical Society.

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

International Nuclear Information System (INIS)

Beni, A; Bogani, L; Bussotti, L; Dei, A; Gentili, P L; Righini, R

2005-01-01

The valence tautomerism of low-spin Co III (Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin Co II (Cat-N-BQ) 2 that, secondly, reaches the chemical equilibrium with the reactant species

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

Science.gov (United States)

Beni, A.; Bogani, L.; Bussotti, L.; Dei, A.; Gentili, P. L.; Righini, R.

2005-01-01

The valence tautomerism of low-spin CoIII(Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin CoII(Cat-N-BQ)2 that, secondly, reaches the chemical equilibrium with the reactant species.

Pump polarization insensitive and efficient laser-diode pumped Yb:KYW ultrafast oscillator.

Science.gov (United States)

Wang, Sha; Wang, Yan-Biao; Feng, Guo-Ying; Zhou, Shou-Huan

2016-02-01

We theoretically and experimentally report and evaluate a novel split laser-diode (LD) double-end pumped Yb:KYW ultrafast oscillator aimed at improving the performance of an ultrafast laser. Compared to a conventional unpolarized single-LD end-pumped ultrafast laser system, we improve the laser performance such as absorption efficiency, slope efficiency, cw mode-locking threshold, and output power by this new structure LD-pumped Yb:KYW ultrafast laser. Experiments were carried out with a 1 W output fiber-coupled LD. Experimental results show that the absorption increases from 38.7% to 48.4%, laser slope efficiency increases from 18.3% to 24.2%, cw mode-locking threshold decreases 12.7% from 630 to 550 mW in cw mode-locking threshold, and maximum output-power increases 28.5% from 158.4 to 221.5 mW when we switch the pump scheme from an unpolarized single-end pumping structure to a split LD double-end pumping structure.

Probing Photoinduced Structural Phase Transitions by Fast or Ultra-Fast Time-Resolved X-Ray Diffraction

Science.gov (United States)

Cailleau, Hervé Collet, Eric; Buron-Le Cointe, Marylise; Lemée-Cailleau, Marie-Hélène Koshihara, Shin-Ya

A new frontier in the field of structural science is the emergence of the fast and ultra-fast X-ray science. Recent developments in time-resolved X-ray diffraction promise direct access to the dynamics of electronic, atomic and molecular motions in condensed matter triggered by a pulsed laser irradiation, i.e. to record "molecular movies" during the transformation of matter initiated by light pulse. These laser pump and X-ray probe techniques now provide an outstanding opportunity for the direct observation of a photoinduced structural phase transition as it takes place. The use of X-ray short-pulse of about 100ps around third-generation synchrotron sources allows structural investigations of fast photoinduced processes. Other new X-ray sources, such as laser-produced plasma ones, generate ultra-short pulses down to 100 fs. This opens the way to femtosecond X-ray crystallography, but with rather low X-ray intensities and more limited experimental possibilities at present. However this new ultra-fast science rapidly progresses around these sources and new large-scale projects exist. It is the aim of this contribution to overview the state of art and the perspectives of fast and ultra-fast X-ray scattering techniques to study photoinduced phase transitions (here, the word ultra-fast is used for sub-picosecond time resolution). In particular we would like to largely present the contribution of crystallographic methods in comparison with optical methods, such as pump-probe reflectivity measurements, the reader being not necessary familiar with X-ray scattering. Thus we want to present which type of physical information can be obtained from the positions of the Bragg peaks, their intensity and their shape, as well as from the diffuse scattering beyond Bragg peaks. An important physical feature is to take into consideration the difference in nature between a photoinduced phase transition and conventional homogeneous photoinduced chemical or biochemical processes where

Multiplane wave imaging increases signal-to-noise ratio in ultrafast ultrasound imaging

International Nuclear Information System (INIS)

Tiran, Elodie; Deffieux, Thomas; Correia, Mafalda; Maresca, David; Osmanski, Bruno-Felix; Pernot, Mathieu; Tanter, Mickael; Sieu, Lim-Anna; Bergel, Antoine; Cohen, Ivan

2015-01-01

Ultrafast imaging using plane or diverging waves has recently enabled new ultrasound imaging modes with improved sensitivity and very high frame rates. Some of these new imaging modalities include shear wave elastography, ultrafast Doppler, ultrafast contrast-enhanced imaging and functional ultrasound imaging. Even though ultrafast imaging already encounters clinical success, increasing even more its penetration depth and signal-to-noise ratio for dedicated applications would be valuable.Ultrafast imaging relies on the coherent compounding of backscattered echoes resulting from successive tilted plane waves emissions; this produces high-resolution ultrasound images with a trade-off between final frame rate, contrast and resolution. In this work, we introduce multiplane wave imaging, a new method that strongly improves ultrafast images signal-to-noise ratio by virtually increasing the emission signal amplitude without compromising the frame rate. This method relies on the successive transmissions of multiple plane waves with differently coded amplitudes and emission angles in a single transmit event. Data from each single plane wave of increased amplitude can then be obtained, by recombining the received data of successive events with the proper coefficients.The benefits of multiplane wave for B-mode, shear wave elastography and ultrafast Doppler imaging are experimentally demonstrated. Multiplane wave with 4 plane waves emissions yields a 5.8  ±  0.5 dB increase in signal-to-noise ratio and approximately 10 mm in penetration in a calibrated ultrasound phantom (0.7 d MHz −1 cm −1 ). In shear wave elastography, the same multiplane wave configuration yields a 2.07  ±  0.05 fold reduction of the particle velocity standard deviation and a two-fold reduction of the shear wave velocity maps standard deviation. In functional ultrasound imaging, the mapping of cerebral blood volume results in a 3 to 6 dB increase of the contrast-to-noise ratio in

Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

International Nuclear Information System (INIS)

Liu, Yuzhu; Knopp, Gregor; Qin, Chaochao; Gerber, Thomas

2015-01-01

Graphical abstract: - Highlights: • Relaxation dynamics of furan are tracked by femtosecond photoelectron imaging. • The mechanism for ultrafast formation of α-carbene and β-carbene is proposed. • Ultrafast internal conversion from S 2 to S 1 is observed. • The transient characteristics of the fragment ions are obtained. • Single-color multi-photon ionization dynamics at 800 nm are also studied. - Abstract: Ultrafast internal conversion dynamics of furan has been studied by femtosecond photoelectron imaging (PEI) coupled with photofragmentation (PF) spectroscopy. Photoelectron imaging of single-color multi-photon ionization and two-color pump–probe ionization are obtained and analyzed. Photoelectron bands are assigned to the related states. The time evolution of the photoelectron signal by pump–probe ionization can be well described by a biexponential decay: two rapid relaxation pathways with time constants of ∼15 fs and 85 (±11) fs. The rapid relaxation is ascribed to the ultrafast internal conversion (IC) from the S 2 state to the vibrationally hot S 1 state. The second relaxation process is attributed to the redistributions and depopulation of secondarily populated high vibronic S 1 state and the formation of α-carbene and β-carbene by H immigration. Additionally, the transient characteristics of the fragment ions are also measured and discussed as a complementary understanding

Ultrafast equilibration of excited electrons in dynamical simulations.

Science.gov (United States)

Lin, Zhibin; Allen, Roland E

2009-12-02

In our density-functional-based simulations of materials responding to femtosecond-scale laser pulses, we have observed a potentially useful phenomenon: the excited electrons automatically equilibrate to a Fermi-Dirac distribution within ∼100 fs, solely because of their coupling to the nuclear motion, even though the resulting electronic temperature is one to two orders of magnitude higher than the kinetic temperature defined by the nuclear motion. Microscopic simulations like these can then provide the separate electronic and kinetic temperatures, chemical potentials, pressures, and nonhydrostatic stresses as input for studies on larger lengths and timescales.

Fast MR imaging and ultrafast MR imaging of fetal central nervous system abnormalities

Energy Technology Data Exchange (ETDEWEB)

Shakudo, Miyuki; Manabe, Takao; Murata, Katsuko; Matsuo, Ryoichi; Oda, Junro [Osaka City General Hospital (Japan); Inoue, Yuichi; Mochizuki, Kunizo; Yamada, Ryusaku

2001-12-01

The aims of this study were two: to compare the efficacy of fast MRI (breath-hold fast spin-echo T2-weighted and fast gradient-echo T1-weighted sequence) and ultrafast MRI (half-Fourier acquisition single-shot turbo spin-echo sequence) in evaluation of fetal central nervous system (CNS) abnormalities at late gestational age, and to compare the capability of fast MRI and ultrafast MRI to assess fetal CNS abnormalities with that of prenatal ultrasonography (US). Forty-nine women with fetuses at gestational ages of 26-39 weeks underwent fast MRI (29 patients) or ultrafast MRI (20 patients). In detection of motion artifact, visualization of the lateral and 4th ventricles, and differentiation between gray and white matter in cerebral hemispheres, ultrafast MRI was significantly superior to fast MRI (p<0.0001, Mann-Whitney U test). In 25 of 43 cases, US and MR diagnoses were the same and consistent with postnatal diagnosis. In 10 of 43 cases, MRI demonstrated findings additional to or different from those of US, and MR findings were confirmed postnatally. MRI, particularly ultrafast MRI, is useful for demonstrating CNS abnormalities in situations in which US is suggestive but not definitive. (author)

Ultrafast electron diffraction using an ultracold source

Directory of Open Access Journals (Sweden)

M. W. van Mourik

2014-05-01

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

Ultrafast biophotonics

CERN Document Server

Vasa, P

2016-01-01

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

Ultrafast Holographic Image Recording by Single Shot Femtosecond Spectral Hole Burning

National Research Council Canada - National Science Library

Rebane, Aleksander

2001-01-01

.... This allowed us to record image holograms with 150-fs duration pulses without need to accumulate the SHB effect from many exposures. Results of this research show that it is possible to perform optical recording of data in frequency-domain on ultrafast time scale. These results can be used also as a new diagnostic tool for femtosecond dynamics in various ultrafast optical interactions.

Ultra-fast ipsilateral DPOAE adaptation not modulated by attention?

Science.gov (United States)

Dalhoff, Ernst; Zelle, Dennis; Gummer, Anthony W.

2018-05-01

Efferent stimulation of outer hair cells is supposed to attenuate cochlear amplification of sound waves and is accompanied by reduced DPOAE amplitudes. Recently, a method using two subsequent f2 pulses during presentation of a longer f1 pulse was introduced to measure fast ipsilateral adaptation effects on separated DPOAE components. Compensating primary-tone onsets for their latencies at the f2-tonotopic place, the average adaptation measured in four normal-hearing subjects was 5.0 dB with a time constant below 5 ms. In the present study, two experiments were performed to determine the origin of this ultra-fast ipsilateral adaptation effect. The first experiment measured ultra-fast ipsilateral adaptation using a two-pulse paradigm at three frequencies in the four subjects, while controlling for visual attention of the subjects. The other experiment also controlled for visual attention, but utilized a sequence of f2 short pulses in the presence of a continuous f1 tone to sample ipsilateral adaptation effects with longer time constants in eight subjects. In the first experiment, no significant change in the ultra-fast adaptation between non-directed attention and visual attention could be detected. In contrast, the second experiment revealed significant changes in the magnitude of the slower ipsilateral adaptation in the visual-attention condition. In conclusion, the lack of an attentional influence indicates that the ultra-fast ipsilateral DPOAE adaptation is not solely mediated by the medial olivocochlear reflex.

Interplay of intra-atomic and interatomic effects: An investigation of the 2p core level spectra of atomic Fe and molecular FeCl2

International Nuclear Information System (INIS)

Richter, T.; Wolff, T.; Zimmermann, P.; Godehusen, K.; Martins, M.

2004-01-01

The 2p photoabsorption and photoelectron spectra of atomic Fe and molecular FeCl 2 were studied by photoion and photoelectron spectroscopy using monochromatized synchrotron radiation and atomic or molecular beam technique. The atomic spectra were analyzed with configuration interaction calculations yielding excellent agreement between experiment and theory. For the analysis of the molecular photoelectron spectrum which shows pronounced interatomic effects, a charge transfer model was used, introducing an additional 3d 7 configuration. The resulting good agreement between the experimental and theoretical spectrum and the remarkable similarity of the molecular with the corresponding spectrum in the solid phase opens a way to a better understanding of the interplay of the interatomic and intra-atomic interactions in the 2p core level spectra of the 3d metal compounds

Advanced ultrafast fiber laser sources enabled by fiber nonlinearities

International Nuclear Information System (INIS)

Liu, Wei

2017-05-01

Development of high power/energy ultrafast fiber lasers for scientific research and industrial applications is one of the most exciting fields in ultrafast optics. This thesis demonstrated new means to improve two essential properties - which are indispensable for novel applications such as high-harmonic generation (HHG) and multiphoton microscopy (MPM) - of an ultrafast fiber laser system: energy scaling capability and wavelength tunability. High photon-flux extreme ultraviolet sources enabled by HHG desire high power (>100 W), high repetition-rate (>1 MHz) ultrafast driving laser sources. We have constructed from scratch a high-power Yb-fiber laser system using the well-known chirped-pulse amplification (CPA) technique. Such a CPA system capable of producing ∝200-W average power consists of a monolithic Yb-fiber oscillator, an all-fiber stretcher, a pre-amplifier chain, a main amplifier constructed from rode-type large pitch fiber, and a diffraction-grating based compressor. To increase the HHG efficiency, ultrafast pulses with duration 130-W average power. The amplified pulses are compressed to 60-fs pulses with 100-W average power, constituting a suitable HHG driving source. MPM is a powerful biomedical imaging tool, featuring larger penetration depth while providing the capability of optical sectioning. Although femtosecond solid-state lasers have been widely accepted as the standard option as MPM driving sources, fiber-based sources have received growing research efforts due to their superior performance. In the second part of this thesis, we both theoretically and experimentally demonstrated a new method of producing wavelength widely tunable femtosecond pulses for driving MPM. We employed self-phase modulation to broaden a narrowband spectrum followed by bandpass filters to select the rightmost/leftmost spectral lobes. Widely tunable in 820-1225 nm, the resulting sources generated nearly transform-limited, ∝100 fs pulses. Using short fibers with large

2008 Electron Donor Acceptor Interactions Gordon Research Conference-August 3-8, 2009

Energy Technology Data Exchange (ETDEWEB)

Forbes, Malcolm [Univ. of North Carolina, Chapel Hill, NC (United States); Gray, Nancy Ryan [Gordon Research Conferences, West Kingston, RI (United States)

2009-09-19

The conference presents and advances the current frontiers in experimental and theoretical studies of Electron Transfer and Transport in Molecular and Nano-scale Systems. The program includes sessions on coupled electron transfers, molecular solar energy conversion, biological and biomimetic systems, spin effects, ultrafast reactions and technical frontiers as well as electron transport in single molecules and devices.

Octave-Spanning Mid-IR Supercontinuum Generation with Ultrafast Cascaded Nonlinearities

DEFF Research Database (Denmark)

Zhou, Binbin; Guo, Hairun; Liu, Xing

2014-01-01

An octave-spanning mid-IR supercontinuum is observed experimentally using ultrafast cascaded nonlinearities in an LiInS2 quadratic nonlinear crystal pumped with 70 fs energetic mid-IR pulses and cut for strongly phase-mismatched second-harmonic generation.......An octave-spanning mid-IR supercontinuum is observed experimentally using ultrafast cascaded nonlinearities in an LiInS2 quadratic nonlinear crystal pumped with 70 fs energetic mid-IR pulses and cut for strongly phase-mismatched second-harmonic generation....

Investigation of an Ultrafast Harmonic Resonant RF Kicker

Energy Technology Data Exchange (ETDEWEB)

Huang, Yulu [Univ. of Chinese Academy of Sciences (CAS), Beijing (China)

2016-10-01

An Energy Recovery Linac (ERL) based multi-turn electron Circulator Cooler Ring (CCR) is envisaged in the proposed Jefferson Lab Electron Ion Collider (JLEIC) to cool the ion bunches with high energy (55 MeV), high current (1.5 A), high repetition frequency (476.3 MHz), high quality magnetized electron bunches. A critical component in this scheme is a pair of ultrafast kickers for the exchange of electron bunches between the ERL and the CCR. The ultrafast kicker should operate with the rise and fall time in less than 2.1 ns, at the repetition rate of ~10s MHz, and should be able to run continuously during the whole period of cooling. These -and-fall time being combined together, are well beyond the state-of-art of traditional pulsed power supplies and magnet kickers. To solve this technical challenge, an alternative method is to generate this high repetition rate, fast rise-and-fall time short pulse continuous waveform by summing several finite number of (co)sine waves at harmonic frequencies of the kicking repetition frequency, and these harmonic modes can be generated by the Quarter Wave Resonater (QWR) based multifrequency cavities. Assuming the recirculator factor is 10, 10 harmonic modes (from 47.63 MHz to 476.3 MHz) with proper amplitudes and phases, plus a DC offset are combined together, a continuous short pulse waveform with the rise-and-fall time in less than 2.1 ns, repetition rate of 47.63 MHz waveform can be generated. With the compact and matured technology of QWR cavities, the total cost of both hardware development and operation can be reduced to a modest level. Focuse on the technical scheme, three main topics will be discussed in this thesis: the synthetization of the kicking pulse, the design and optimization of the deflecting QWR multi-integer harmonic frequency resonator and the fabrication and bench measurements of a half scale copper prototype. In the kicking pulse synthetization part, we begin with the Fourier Series expansion of an ideal

Atomistic simulation of tantalum nanoindentation: Effects of indenter diameter, penetration velocity, and interatomic potentials on defect mechanisms and evolution

International Nuclear Information System (INIS)

Ruestes, C.J.; Stukowski, A.; Tang, Y.; Tramontina, D.R.; Erhart, P.; Remington, B.A.; Urbassek, H.M.; Meyers, M.A.; Bringa, E.M.

2014-01-01

Nanoindentation simulations are a helpful complement to experiments. There is a dearth of nanoindentation simulations for bcc metals, partly due to the lack of computationally efficient and reliable interatomic potentials at large strains. We carry out indentation simulations for bcc tantalum using three different interatomic potentials and present the defect mechanisms responsible for the creation and expansion of the plastic deformation zone: twins are initially formed, giving rise to shear loop expansion and the formation of sequential prismatic loops. The calculated elastic constants as function of pressure as well as stacking fault energy surfaces explain the significant differences found in the defect structures generated for the three potentials investigated in this study. The simulations enable the quantification of total dislocation length and twinning fraction. The indenter velocity is varied and, as expected, the penetration depth for the first pop-in (defect emission) event shows a strain rate sensitivity m in the range of 0.037–0.055. The effect of indenter diameter on the first pop-in is discussed. A new intrinsic length-scale model is presented based on the profile of the residual indentation and geometrically necessary dislocation theory

Atomistic simulation of tantalum nanoindentation: Effects of indenter diameter, penetration velocity, and interatomic potentials on defect mechanisms and evolution

Energy Technology Data Exchange (ETDEWEB)

Ruestes, C.J., E-mail: cjruestes@hotmail.com [Department of Mechanical and Aerospace Engineering, University of California, San Diego, La Jolla, CA 92093 (United States); Facultad de Ciencias Exactas y Naturales, Univ. Nac. de Cuyo, Mendoza 5500 (Argentina); CONICET, Mendoza 5500 (Argentina); Stukowski, A. [Technische Universität Darmstadt, Darmstadt 64287 (Germany); Tang, Y. [Shanghai Institute of Applied Mathematics and Mechanics, Shanghai University, Shanghai 200072 (China); Tramontina, D.R. [Facultad de Ciencias Exactas y Naturales, Univ. Nac. de Cuyo, Mendoza 5500 (Argentina); Erhart, P. [Chalmers University of Technology, Department of Applied Physics, Gothenburg 41296 (Sweden); Remington, B.A. [Lawrence Livermore National Lab, Livermore, CA 94550 (United States); Urbassek, H.M. [Physics Department and Research Center OPTIMAS, University of Kaiserslautern, Kaiserslautern 67663 (Germany); Meyers, M.A. [Department of Mechanical and Aerospace Engineering, University of California, San Diego, La Jolla, CA 92093 (United States); Bringa, E.M. [Facultad de Ciencias Exactas y Naturales, Univ. Nac. de Cuyo, Mendoza 5500 (Argentina); CONICET, Mendoza 5500 (Argentina)

2014-09-08

Nanoindentation simulations are a helpful complement to experiments. There is a dearth of nanoindentation simulations for bcc metals, partly due to the lack of computationally efficient and reliable interatomic potentials at large strains. We carry out indentation simulations for bcc tantalum using three different interatomic potentials and present the defect mechanisms responsible for the creation and expansion of the plastic deformation zone: twins are initially formed, giving rise to shear loop expansion and the formation of sequential prismatic loops. The calculated elastic constants as function of pressure as well as stacking fault energy surfaces explain the significant differences found in the defect structures generated for the three potentials investigated in this study. The simulations enable the quantification of total dislocation length and twinning fraction. The indenter velocity is varied and, as expected, the penetration depth for the first pop-in (defect emission) event shows a strain rate sensitivity m in the range of 0.037–0.055. The effect of indenter diameter on the first pop-in is discussed. A new intrinsic length-scale model is presented based on the profile of the residual indentation and geometrically necessary dislocation theory.

Photonic-assisted ultrafast THz wireless access

DEFF Research Database (Denmark)

Yu, Xianbin; Chen, Ying; Galili, Michael

THz technology has been considered feasible for ultrafast wireless data communi- cation, to meet the increasing demand on next-generation fast wireless access, e.g., huge data file transferring and fast mobile data stream access. This talk reviews recent progress in high-speed THz wireless...

Discrete decoding based ultrafast multidimensional nuclear magnetic resonance spectroscopy

International Nuclear Information System (INIS)

Wei, Zhiliang; Lin, Liangjie; Ye, Qimiao; Li, Jing; Cai, Shuhui; Chen, Zhong

2015-01-01

The three-dimensional (3D) nuclear magnetic resonance (NMR) spectroscopy constitutes an important and powerful tool in analyzing chemical and biological systems. However, the abundant 3D information arrives at the expense of long acquisition times lasting hours or even days. Therefore, there has been a continuous interest in developing techniques to accelerate recordings of 3D NMR spectra, among which the ultrafast spatiotemporal encoding technique supplies impressive acquisition speed by compressing a multidimensional spectrum in a single scan. However, it tends to suffer from tradeoffs among spectral widths in different dimensions, which deteriorates in cases of NMR spectroscopy with more dimensions. In this study, the discrete decoding is proposed to liberate the ultrafast technique from tradeoffs among spectral widths in different dimensions by focusing decoding on signal-bearing sites. For verifying its feasibility and effectiveness, we utilized the method to generate two different types of 3D spectra. The proposed method is also applicable to cases with more than three dimensions, which, based on the experimental results, may widen applications of the ultrafast technique

Discrete decoding based ultrafast multidimensional nuclear magnetic resonance spectroscopy

Science.gov (United States)

Wei, Zhiliang; Lin, Liangjie; Ye, Qimiao; Li, Jing; Cai, Shuhui; Chen, Zhong

2015-07-01

The three-dimensional (3D) nuclear magnetic resonance (NMR) spectroscopy constitutes an important and powerful tool in analyzing chemical and biological systems. However, the abundant 3D information arrives at the expense of long acquisition times lasting hours or even days. Therefore, there has been a continuous interest in developing techniques to accelerate recordings of 3D NMR spectra, among which the ultrafast spatiotemporal encoding technique supplies impressive acquisition speed by compressing a multidimensional spectrum in a single scan. However, it tends to suffer from tradeoffs among spectral widths in different dimensions, which deteriorates in cases of NMR spectroscopy with more dimensions. In this study, the discrete decoding is proposed to liberate the ultrafast technique from tradeoffs among spectral widths in different dimensions by focusing decoding on signal-bearing sites. For verifying its feasibility and effectiveness, we utilized the method to generate two different types of 3D spectra. The proposed method is also applicable to cases with more than three dimensions, which, based on the experimental results, may widen applications of the ultrafast technique.

Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

Energy Technology Data Exchange (ETDEWEB)

Liu, Yuzhu, E-mail: yuzhu.liu@gmail.com [School of Physics and Optoelectronic Engineering, Nanjing University of Information Science and Technology, Nanjing 210044 (China); Knopp, Gregor [Paul Scherrer Institute, Villigen 5232 (Switzerland); Qin, Chaochao [Department of Physics, Henan Normal University, Xinxiang 453007 (China); Gerber, Thomas [Paul Scherrer Institute, Villigen 5232 (Switzerland)

2015-01-13

Graphical abstract: - Highlights: • Relaxation dynamics of furan are tracked by femtosecond photoelectron imaging. • The mechanism for ultrafast formation of α-carbene and β-carbene is proposed. • Ultrafast internal conversion from S{sub 2} to S{sub 1} is observed. • The transient characteristics of the fragment ions are obtained. • Single-color multi-photon ionization dynamics at 800 nm are also studied. - Abstract: Ultrafast internal conversion dynamics of furan has been studied by femtosecond photoelectron imaging (PEI) coupled with photofragmentation (PF) spectroscopy. Photoelectron imaging of single-color multi-photon ionization and two-color pump–probe ionization are obtained and analyzed. Photoelectron bands are assigned to the related states. The time evolution of the photoelectron signal by pump–probe ionization can be well described by a biexponential decay: two rapid relaxation pathways with time constants of ∼15 fs and 85 (±11) fs. The rapid relaxation is ascribed to the ultrafast internal conversion (IC) from the S{sub 2} state to the vibrationally hot S{sub 1} state. The second relaxation process is attributed to the redistributions and depopulation of secondarily populated high vibronic S{sub 1} state and the formation of α-carbene and β-carbene by H immigration. Additionally, the transient characteristics of the fragment ions are also measured and discussed as a complementary understanding.

Sputtering of octatetraene by 15 keV C{sub 60} projectiles: Comparison of reactive interatomic potentials

Energy Technology Data Exchange (ETDEWEB)

Kanski, Michal; Maciazek, Dawid; Golunski, Mikolaj; Postawa, Zbigniew, E-mail: zbigniew.postawa@uj.edu.pl

2017-02-15

Highlights: • Probing the effect of interatomic potentials on sputtering of an octatetraene sample. • Problems with charge calculations are observed during cluster impact for ReaxFF. • COMB3 leads to a very low sputtering yield due to abrupt energy dissipation. • AIREBO is computationally the most efficient, while ReaxFF is more accurate. - Abstract: Molecular dynamics computer simulations have been used to probe the effect of the AIREBO, ReaxFF and COMB3 interatomic potentials on sputtering of an organic sample composed of octatetraene molecules. The system is bombarded by a 15 keV C{sub 60} projectile at normal incidence. The effect of the applied force fields on the total time of simulation, the calculated sputtering yield and the angular distribution of sputtered particles is investigated and discussed. It has been found that caution should be taken when simulating particles ejection from nonhomogeneous systems that undergo significant fragmentation described by the ReaxFF. In this case, the charge state of many particles is improper due to an inadequacy of a procedure used for calculating partial charges on atoms in molecules for conditions present during sputtering. A two-step simulation procedure is proposed to minimize the effect of this deficiency. There is also a possible problem with the COMB3 potential, at least at conditions present during cluster impact, as its results are very different from AIREBO or ReaxFF.

Ultrafast photocurrents in monolayer MoS2

Science.gov (United States)

Parzinger, Eric; Wurstbauer, Ursula; Holleitner, Alexander W.

Two-dimensional transition metal dichalcogenides such as MoS2 have emerged as interesting materials for optoelectronic devices. In particular, the ultrafast dynamics and lifetimes of photoexcited charge carriers have attracted great interest during the last years. We investigate the photocurrent response of monolayer MoS2 on a picosecond time scale utilizing a recently developed pump-probe spectroscopy technique based on coplanar striplines. We discuss the ultrafast dynamics within MoS2 including photo-thermoelectric currents and the impact of built-in fields due to Schottky barriers as well as the Fermi level pinning at the contact region. We acknowledge support by the ERC via Project 'NanoREAL', the DFG via excellence cluster 'Nanosystems Initiative Munich' (NIM), and through the TUM International Graduate School of Science and Engineering (IGSSE) and BaCaTeC.

Measurements of ionic structure in shock compressed lithium hydride from ultrafast x-ray Thomson scattering.

Science.gov (United States)

Kritcher, A L; Neumayer, P; Brown, C R D; Davis, P; Döppner, T; Falcone, R W; Gericke, D O; Gregori, G; Holst, B; Landen, O L; Lee, H J; Morse, E C; Pelka, A; Redmer, R; Roth, M; Vorberger, J; Wünsch, K; Glenzer, S H

2009-12-11

We present the first ultrafast temporally, spectrally, and angularly resolved x-ray scattering measurements from shock-compressed matter. The experimental spectra yield the absolute elastic and inelastic scattering intensities from the measured density of free electrons. Laser-compressed lithium-hydride samples are well characterized by inelastic Compton and plasmon scattering of a K-alpha x-ray probe providing independent measurements of temperature and density. The data show excellent agreement with the total intensity and structure when using the two-species form factor and accounting for the screening of ion-ion interactions.

Ultrafast dynamic ellipsometry and spectroscopy of laser shocked materials

Energy Technology Data Exchange (ETDEWEB)

Mcgrane, Shawn David [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Bolme, Cindy B [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Whitley, Von H [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Moore, David S [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2010-01-01

Shock waves create extreme states of matter with very high pressures, temperatures, and volumetric compressions, at an exceedingly rapid rate of change. We review how to use a beamsplitter and a note card to turn a typical chirp pulse amplified femtosecond laser system into an ultrafast shock dynamics machine. Open scientific questions that can be addressed with such an apparatus are described. We report on the development of several single shot time resolved diagnostics needed to answer these questions. These single shot diagnostics are expected to be broadly applicable to other types of laser ablation experiments. Experimental results measured from shocked material dynamics of several systems are detailed. Finally, we report on progress towards using transient absorption as a measure of electronic excitation and coherent Raman as a picosecond probe of temperature in shock compressed condensed matter.

MoS2-modified ZnO quantum dots nanocomposite: Synthesis and ultrafast humidity response

International Nuclear Information System (INIS)

Ze, Lu; Yueqiu, Gong; Xujun, Li; Yong, Zhang

2017-01-01

Highlights: • MoS 2 @ZnO QDs composite structure was synthesized by two-steps methods. • Ultrafast humidity sensing response is achieved by MoS 2 @ZnO QDs humidity sensor. • Sensor performs excellent cycle stability from 11% to 95% RH. • Humidity sensor could detect wide humidity range (11–95%). - Abstract: In this work, ZnO quantum dots (QDs), layered MoS 2 and MoS 2 -modified ZnO QDs (MoS 2 @ZnO QDs) nanocomposite were synthesized and then applied as humidity sensor. The crystal structure, morphology and element distribution of ZnO QDs, MoS 2 and MoS 2 @ZnO QDs were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and energy dispersive X-ray spectrometry, respectively. The humidity sensing characteristics of the MoS 2 and MoS 2 @ZnO QDs against various relative humidity were measured at room temperature. The results show that the MoS 2 @ZnO QDs sensor exhibits high sensitivity with an impedance variation of three or four orders of magnitude to relative humidity range of 11–95% and it exhibits a short response-recovery time (1 s for adsorption and 20 s for desorption) and excellent repeatability. The mechanisms of the excellent performance for humidity sensing of MoS 2 @ZnO QDs sensor were discussed based on its impedance properties. Our work could offer guidelines to design higher performance especially ultrafast humidity response sensor utilizing the nanocomposite structure with two dimensional material and QDs.

Ultrafast spectroscopy of model biological membranes

NARCIS (Netherlands)

Ghosh, Avishek

2009-01-01

In this PhD thesis, I have described the novel time-resolved sum-frequency generation (TR-SFG) spectroscopic technique that I developed during the course of my PhD research and used it study the ultrafast vibrational, structural and orientational dynamics of water molecules at model biological

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

Directory of Open Access Journals (Sweden)

Emrah Turgut

2013-09-01

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

Retrieval of interatomic separations of molecules from laser-induced high-order harmonic spectra

International Nuclear Information System (INIS)

Le, Van-Hoang; Nguyen, Ngoc-Ty; Jin, C; Le, Anh-Thu; Lin, C D

2008-01-01

We illustrate an iterative method for retrieving the internuclear separations of N 2 , O 2 and CO 2 molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is preferable to retrieve the interatomic separation iteratively by fitting the extracted dipole moment. Our results show that time-resolved chemical imaging of molecules using infrared laser pulses with femtosecond temporal resolutions is possible

Development of Ultrafast Laser Flash Methods for Measuring Thermophysical Properties of Thin Films and Boundary Thermal Resistances

Science.gov (United States)

Baba, Tetsuya; Taketoshi, Naoyuki; Yagi, Takashi

2011-11-01

Reliable thermophysical property values of thin films are important to develop advanced industrial technologies such as highly integrated electronic devices, phase-change memories, magneto-optical disks, light-emitting diodes (LEDs), organic light-emitting diodes (OLEDs), semiconductor lasers (LDs), flat-panel displays, and power electronic devices. In order to meet these requirements, the National Metrology Institute of Japan of the National Institute of Advanced Industrial Science and Technology (NMIJ/AIST) has developed ultrafast laser flash methods heated by picosecond pulse or nanosecond pulse with the same geometrical configuration as the laser flash method, which is the standard method to measure the thermal diffusivity of bulk materials. Since these pulsed light heating methods induce one-dimensional heat diffusion across a well-defined length of the specimen thickness, the absolute value of thermal diffusivity across thin films can be measured reliably. Using these ultrafast laser flash methods, the thermal diffusivity of each layer of multilayered thin films and the boundary thermal resistance between the layers can be determined from the observed transient temperature curves based on the response function method. The thermophysical properties of various thin films important for modern industries such as the transparent conductive films used for flat-panel displays, hard coating films, and multilayered films of next-generation phase-change optical disks have been measured by these methods.

Nonadiabatic effects in electronic and nuclear dynamics

Directory of Open Access Journals (Sweden)

Martin P. Bircher

2017-11-01

Full Text Available Due to their very nature, ultrafast phenomena are often accompanied by the occurrence of nonadiabatic effects. From a theoretical perspective, the treatment of nonadiabatic processes makes it necessary to go beyond the (quasi static picture provided by the time-independent Schrödinger equation within the Born-Oppenheimer approximation and to find ways to tackle instead the full time-dependent electronic and nuclear quantum problem. In this review, we give an overview of different nonadiabatic processes that manifest themselves in electronic and nuclear dynamics ranging from the nonadiabatic phenomena taking place during tunnel ionization of atoms in strong laser fields to the radiationless relaxation through conical intersections and the nonadiabatic coupling of vibrational modes and discuss the computational approaches that have been developed to describe such phenomena. These methods range from the full solution of the combined nuclear-electronic quantum problem to a hierarchy of semiclassical approaches and even purely classical frameworks. The power of these simulation tools is illustrated by representative applications and the direct confrontation with experimental measurements performed in the National Centre of Competence for Molecular Ultrafast Science and Technology.

Cutting-Edge High-Power Ultrafast Thin Disk Oscillators

Directory of Open Access Journals (Sweden)

Thomas Südmeyer

2013-04-01

Full Text Available A growing number of applications in science and industry are currently pushing the development of ultrafast laser technologies that enable high average powers. SESAM modelocked thin disk lasers (TDLs currently achieve higher pulse energies and average powers than any other ultrafast oscillator technology, making them excellent candidates in this goal. Recently, 275 W of average power with a pulse duration of 583 fs were demonstrated, which represents the highest average power so far demonstrated from an ultrafast oscillator. In terms of pulse energy, TDLs reach more than 40 μJ pulses directly from the oscillator. In addition, another major milestone was recently achieved, with the demonstration of a TDL with nearly bandwidth-limited 96-fs long pulses. The progress achieved in terms of pulse duration of such sources enabled the first measurement of the carrier-envelope offset frequency of a modelocked TDL, which is the first key step towards full stabilization of such a source. We will present the key elements that enabled these latest results, as well as an outlook towards the next scaling steps in average power, pulse energy and pulse duration of such sources. These cutting-edge sources will enable exciting new applications, and open the door to further extending the current performance milestones.

Feasibility of UltraFast Doppler in Post-operative Evaluation of Hepatic Artery in Recipients following Liver Transplantation.

Science.gov (United States)

Kim, Se-Young; Kim, Kyoung Won; Choi, Sang Hyun; Kwon, Jae Hyun; Song, Gi-Won; Kwon, Heon-Ju; Yun, Young Ju; Lee, Jeongjin; Lee, Sung-Gyu

2017-11-01

To determine the feasibility of using UltraFast Doppler in post-operative evaluation of the hepatic artery (HA) after liver transplantation (LT), we evaluated 283 simultaneous conventional and UltraFast Doppler sessions in 126 recipients over a 2-mo period after LT, using an Aixplorer scanner The Doppler indexes of the HA (peak systolic velocity [PSV], end-diastolic velocity [EDV], resistive index [RI] and systolic acceleration time [SAT]) by retrospective analysis of retrieved waves from UltraFast Doppler clips were compared with those obtained by conventional spectral Doppler. Correlation, performance in diagnosing the pathologic wave, examination time and reproducibility were evaluated. The PSV, EDV, RI and SAT of spectral and UltraFast Doppler measurements exhibited excellent correlation with favorable diagnostic performance. During the bedside examination, the mean time spent for UltraFast clip storing was significantly shorter than that for conventional Doppler US measurements. Both conventional and UltraFast Doppler exhibited good to excellent inter-analysis consistency. In conclusion, compared with conventional spectral Doppler, UltraFast Doppler values correlated excellently and yielded acceptable pathologic wave diagnostic performance with reduced examination time at the bedside and excellent reproducibility. Copyright © 2017 World Federation for Ultrasound in Medicine & Biology. Published by Elsevier Inc. All rights reserved.

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Beni, A [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy); Bogani, L [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy); Bussotti, L [LENS, Universita di Firenze, Via Nello Carrara 1, 50019 Sesto Fiorentino, Florence (Italy); Dei, A [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy); Gentili, P L [LENS, Universita di Firenze, Via Nello Carrara 1, 50019 Sesto Fiorentino, Florence (Italy); Righini, R [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy)

2005-01-01

The valence tautomerism of low-spin Co{sup III}(Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin Co{sup II}(Cat-N-BQ){sub 2} that, secondly, reaches the chemical equilibrium with the reactant species.

Ultrafast transient absorption revisited: Phase-flips, spectral fingers, and other dynamical features

Energy Technology Data Exchange (ETDEWEB)

Cina, Jeffrey A., E-mail: cina@uoregon.edu; Kovac, Philip A. [Department of Chemistry and Biochemistry, and Oregon Center for Optical, Molecular, and Quantum Science, University of Oregon, Eugene, Oregon 97403 (United States); Jumper, Chanelle C. [Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6 (Canada); Dean, Jacob C.; Scholes, Gregory D., E-mail: gscholes@princeton.edu [Department of Chemistry, Princeton University, Princeton, New Jersey 08544 (United States)

2016-05-07

We rebuild the theory of ultrafast transient-absorption/transmission spectroscopy starting from the optical response of an individual molecule to incident femtosecond pump and probe pulses. The resulting description makes use of pulse propagators and free molecular evolution operators to arrive at compact expressions for the several contributions to a transient-absorption signal. In this alternative description, which is physically equivalent to the conventional response-function formalism, these signal contributions are conveniently expressed as quantum mechanical overlaps between nuclear wave packets that have undergone different sequences of pulse-driven optical transitions and time-evolution on different electronic potential-energy surfaces. Using this setup in application to a simple, multimode model of the light-harvesting chromophores of PC577, we develop wave-packet pictures of certain generic features of ultrafast transient-absorption signals related to the probed-frequency dependence of vibrational quantum beats. These include a Stokes-shifting node at the time-evolving peak emission frequency, antiphasing between vibrational oscillations on opposite sides (i.e., to the red or blue) of this node, and spectral fingering due to vibrational overtones and combinations. Our calculations make a vibrationally abrupt approximation for the incident pump and probe pulses, but properly account for temporal pulse overlap and signal turn-on, rather than neglecting pulse overlap or assuming delta-function excitations, as are sometimes done.

Non-equilibrium lattice dynamics of one-dimensional In chains on Si(111 upon ultrafast optical excitation

Directory of Open Access Journals (Sweden)

T. Frigge

2018-03-01

Full Text Available The photoinduced structural dynamics of the atomic wire system on the Si(111-In surface has been studied by ultrafast electron diffraction in reflection geometry. Upon intense fs-laser excitation, this system can be driven in around 1 ps from the insulating (8×2 reconstructed low temperature phase to a metastable metallic (4×1 reconstructed high temperature phase. Subsequent to the structural transition, the surface heats up on a 6 times slower timescale as determined from a transient Debye-Waller analysis of the diffraction spots. From a comparison with the structural response of the high temperature (4×1 phase, we conclude that electron-phonon coupling is responsible for the slow energy transfer from the excited electron system to the lattice. The significant difference in timescales is evidence that the photoinduced structural transition is non-thermally driven.

Current-limiting and ultrafast system for the characterization of resistive random access memories.

Science.gov (United States)

Diaz-Fortuny, J; Maestro, M; Martin-Martinez, J; Crespo-Yepes, A; Rodriguez, R; Nafria, M; Aymerich, X

2016-06-01

A new system for the ultrafast characterization of resistive switching phenomenon is developed to acquire the current during the Set and Reset process in a microsecond time scale. A new electronic circuit has been developed as a part of the main setup system, which is capable of (i) applying a hardware current limit ranging from nanoampers up to miliampers and (ii) converting the Set and Reset exponential gate current range into an equivalent linear voltage. The complete system setup allows measuring with a microsecond resolution. Some examples demonstrate that, with the developed setup, an in-depth analysis of resistive switching phenomenon and random telegraph noise can be made.

Ultrafast terahertz-induced response of GeSbTe phase-change materials

Energy Technology Data Exchange (ETDEWEB)

Shu, Michael J. [Department of Applied Physics, Stanford University, Stanford, California 94305 (United States); Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Zalden, Peter [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Chen, Frank [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Department of Electrical Engineering, Stanford University, Stanford, California 94305 (United States); Weems, Ben [Department of Materials Science and Engineering, Stanford University, Stanford, California 94305 (United States); Chatzakis, Ioannis [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Xiong, Feng; Jeyasingh, Rakesh; Pop, Eric; Philip Wong, H.-S. [Department of Electrical Engineering, Stanford University, Stanford, California 94305 (United States); Hoffmann, Matthias C. [SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Wuttig, Matthias [I. Physikalisches Institut, RWTH Aachen University, 52056 Aachen (Germany); JARA–Fundamentals of Information Technology, RWTH Aachen University, 52056 Aachen (Germany); Lindenberg, Aaron M., E-mail: aaronl@stanford.edu [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Department of Materials Science and Engineering, Stanford University, Stanford, California 94305 (United States)

2014-06-23

The time-resolved ultrafast electric field-driven response of crystalline and amorphous GeSbTe films has been measured all-optically, pumping with single-cycle terahertz pulses as a means of biasing phase-change materials on a sub-picosecond time-scale. Utilizing the near-band-gap transmission as a probe of the electronic and structural response below the switching threshold, we observe a field-induced heating of the carrier system and resolve the picosecond-time-scale energy relaxation processes and their dependence on the sample annealing condition in the crystalline phase. In the amorphous phase, an instantaneous electroabsorption response is observed, quadratic in the terahertz field, followed by field-driven lattice heating, with Ohmic behavior up to 200 kV/cm.

Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective

Directory of Open Access Journals (Sweden)

Daria Popova-Gorelova

2018-02-01

Full Text Available A wide range of ultrafast phenomena in various atomic, molecular and condense matter systems is governed by electron dynamics. Therefore, the ability to image electronic motion in real space and real time would provide a deeper understanding of such processes and guide developments of tools to control them. Ultrashort light pulses, which can provide unprecedented time resolution approaching subfemtosecond time scale, are perspective to achieve real-time imaging of electron dynamics. This task is challenging not only from an experimental view, but also from a theory perspective, since standard theories describing light-matter interaction in a stationary regime can provide erroneous results in an ultrafast case as demonstrated by several theoretical studies. We review the theoretical framework based on quantum electrodynamics, which has been shown to be necessary for an accurate description of time-resolved imaging of electron dynamics with ultrashort light pulses. We compare the results of theoretical studies of time-resolved nonresonant and resonant X-ray scattering, and time- and angle-resolved photoelectron spectroscopy and show that the corresponding time-resolved signals encode analogous information about electron dynamics. Thereby, the information about an electronic system provided by these time-resolved techniques is different from the information provided by their time-independent analogues.

On the relation between Marcus theory and ultrafast spectroscopy of solvation kinetics

Science.gov (United States)

Roy, Santanu; Galib, Mirza; Schenter, Gregory K.; Mundy, Christopher J.

2018-01-01

The phenomena of solvent exchange control the process of solvating ions, protons, and charged molecules. Building upon our extension of Marcus' philosophy of electron transfer, we provide a new perspective of ultrafast solvent exchange mechanism around ions measurable by two-dimensional infrared (2DIR) spectroscopy. In this theory, solvent rearrangement drives an ion-bound water to an activated state of higher coordination number, triggering ion-water separation that leads to the solvent-bound state of the water molecule. This ion-bound to solvent-bound transition rate for a BF4--water system is computed using ab initio molecular dynamics and Marcus theory, and is found to be in excellent agreement with the 2DIR measurement.

Progress in ultrafast intense laser science XIII

CERN Document Server

III, Wendell; Paulus, Gerhard

2017-01-01

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

Progress in ultrafast intense laser science XII

CERN Document Server

Roso, Luis; Li, Ruxin; Mathur, Deepak; Normand, Didier

2015-01-01

This  volume covers a broad range of topics focusing on atoms, molecules, and clusters interacting in intense laser field, laser induced filamentation, and laser plasma interaction and application. The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance and attractions of the research topic at hand; these are followed by reports of cutting-edge discoveries. .

Hypothetical planar and nanotubular crystalline structures with five interatomic bonds of Kepler nets type

Directory of Open Access Journals (Sweden)

Aleksey I. Kochaev

2017-02-01

Full Text Available The possibility of metastable existence of planar and non-chiral nanotubular crystalline lattices in the form of Kepler nets of 34324, 3342, and 346 types (the notations are given in Schläfly symbols, using ab initio calculations, has researched. Atoms of P, As, Sb, Bi from 15th group and atoms of S, Se, Te from 16th group of the periodic table were taken into consideration. The lengths of interatomic bonds corresponding to the steadiest states for such were determined. We found that among these new composed structures crystals encountered strong elastic properties. Besides, some of them can possess pyroelectric and piezoelectric properties. Our results can be used for nanoelectronics and nanoelectromechanical devices designing.

Directing the path of light-induced electron transfer at a molecular fork using vibrational excitation

Science.gov (United States)

Delor, Milan; Archer, Stuart A.; Keane, Theo; Meijer, Anthony J. H. M.; Sazanovich, Igor V.; Greetham, Gregory M.; Towrie, Michael; Weinstein, Julia A.

2017-11-01

Ultrafast electron transfer in condensed-phase molecular systems is often strongly coupled to intramolecular vibrations that can promote, suppress and direct electronic processes. Recent experiments exploring this phenomenon proved that light-induced electron transfer can be strongly modulated by vibrational excitation, suggesting a new avenue for active control over molecular function. Here, we achieve the first example of such explicit vibrational control through judicious design of a Pt(II)-acetylide charge-transfer donor-bridge-acceptor-bridge-donor 'fork' system: asymmetric 13C isotopic labelling of one of the two -C≡C- bridges makes the two parallel and otherwise identical donor→acceptor electron-transfer pathways structurally distinct, enabling independent vibrational perturbation of either. Applying an ultrafast UVpump(excitation)-IRpump(perturbation)-IRprobe(monitoring) pulse sequence, we show that the pathway that is vibrationally perturbed during UV-induced electron transfer is dramatically slowed down compared to its unperturbed counterpart. One can thus choose the dominant electron transfer pathway. The findings deliver a new opportunity for precise perturbative control of electronic energy propagation in molecular devices.

Probing electron correlation and nuclear dynamics in Momentum Space

International Nuclear Information System (INIS)

Deleuze, M S; Hajgato, B; Morini, F; Knippenberg, S

2010-01-01

Orbital imaging experiments employing Electron Momentum Spectroscopy are subject to many complications, such as distorted wave effects, conformational mobility in the electronic ground state, ultra-fast nuclear dynamics in the final state, or a dispersion of the ionization intensity over electronically excited (shake-up) configurations of the cation. The purpose of the present contribution is to illustrate how a proper treatment of these complications enables us to probe in momentum space the consequences of electron correlation and nuclear dynamics in neutral and cationic states.

Ultrafast time-resolved spectroscopy of xanthophylls at low temperature.

Science.gov (United States)

Cong, Hong; Niedzwiedzki, Dariusz M; Gibson, George N; Frank, Harry A

2008-03-20

Many of the spectroscopic features and photophysical properties of xanthophylls and their role in energy transfer to chlorophyll can be accounted for on the basis of a three-state model. The characteristically strong visible absorption of xanthophylls is associated with a transition from the ground state S0 (1(1)Ag-) to the S2 (1(1)Bu+) excited state. The lowest lying singlet state denoted S1 (2(1)Ag-), is a state into which absorption from the ground state is symmetry forbidden. Ultrafast optical spectroscopic studies and quantum computations have suggested the presence of additional excited singlet states in the vicinity of S1 (2(1)Ag-) and S2 (1(1)Bu+). One of these is denoted S* and has been suggested in previous work to be associated with a twisted molecular conformation of the molecule in the S1 (2(1)Ag-) state. In this work, we present the results of a spectroscopic investigation of three major xanthophylls from higher plants: violaxanthin, lutein, and zeaxanthin. These molecules have systematically increasing extents of pi-electron conjugation from nine to eleven conjugated carbon-carbon double bonds. All-trans isomers of the molecules were purified by high-performance liquid chromatography (HPLC) and studied by steady-state and ultrafast time-resolved optical spectroscopy at 77 K. Analysis of the data using global fitting techniques has revealed the inherent spectral properties and ultrafast dynamics of the excited singlet states of each of the molecules. Five different global fitting models were tested, and it was found that the data are best explained using a kinetic model whereby photoexcitation results in the promotion of the molecule into the S2 (1(1)Bu+) state that subsequently undergoes decay to a vibrationally hot S1 (1(1)Ag-) state and with the exception of violaxanthin also to the S* state. The vibrationally hot S1 (1(1)Ag-) state then cools to a vibrationally relaxed S1 (2(1)Ag-) state in less than a picosecond. It was also found that a portion

Advanced ultrafast fiber laser sources enabled by fiber nonlinearities

Energy Technology Data Exchange (ETDEWEB)

Liu, Wei

2017-05-15

Development of high power/energy ultrafast fiber lasers for scientific research and industrial applications is one of the most exciting fields in ultrafast optics. This thesis demonstrated new means to improve two essential properties - which are indispensable for novel applications such as high-harmonic generation (HHG) and multiphoton microscopy (MPM) - of an ultrafast fiber laser system: energy scaling capability and wavelength tunability. High photon-flux extreme ultraviolet sources enabled by HHG desire high power (>100 W), high repetition-rate (>1 MHz) ultrafast driving laser sources. We have constructed from scratch a high-power Yb-fiber laser system using the well-known chirped-pulse amplification (CPA) technique. Such a CPA system capable of producing ∝200-W average power consists of a monolithic Yb-fiber oscillator, an all-fiber stretcher, a pre-amplifier chain, a main amplifier constructed from rode-type large pitch fiber, and a diffraction-grating based compressor. To increase the HHG efficiency, ultrafast pulses with duration <60 fs are highly desired. We proposed and demonstrated a novel amplification technique, named as pre-chirp managed amplification (PCMA). We successfully constructed an Yb-fiber based PCMA system that outputs 75-MHz spectrally broadened pulses with >130-W average power. The amplified pulses are compressed to 60-fs pulses with 100-W average power, constituting a suitable HHG driving source. MPM is a powerful biomedical imaging tool, featuring larger penetration depth while providing the capability of optical sectioning. Although femtosecond solid-state lasers have been widely accepted as the standard option as MPM driving sources, fiber-based sources have received growing research efforts due to their superior performance. In the second part of this thesis, we both theoretically and experimentally demonstrated a new method of producing wavelength widely tunable femtosecond pulses for driving MPM. We employed self-phase modulation

Ultrafast Photoinduced Electron Transfer in Bimolecular Donor-Acceptor Systems

KAUST Repository

Alsulami, Qana

2016-01-01

, electronic properties and chemical structure. Interestingly, clear correlations among the steady-state measurements, time-resolved spectroscopy results, grain alignment of the electron transporting layer (ETL), carrier mobility, and device performance

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

Science.gov (United States)

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

2017-03-01

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

Ultrashort and coherent single-electron pulses for diffraction at ultimate resolutions

International Nuclear Information System (INIS)

Kirchner, Friedrich Oscar

2013-01-01

Ultrafast electron diffraction is a powerful tool for studying structural dynamics with femtosecond temporal and sub-aangstroem spatial resolutions. It benefits from the high scattering cross-sections of electrons compared X-rays and allows the examination of thin samples, surfaces and gases. One of the main challenges in ultrafast electron diffraction is the generation of electron pulses with a short duration and a large transverse coherence. The former limits the temporal resolution of the experiment while the latter determines the maximum size of the scattering structures that can be studied. In this work, we strive to push the limits of electron diffraction towards higher temporal and spatial resolutions. The decisive step in our approach is to eliminate all detrimental effects caused by Coulomb repulsion between the electrons by reducing the number of electrons per pulse to one. In this situation, the electrons' longitudinal and transverse velocity distributions are determined solely by the photoemission process. By reducing the electron source size on the photocathode, we make use of the small transverse velocity spread to produce electron pulses with a transverse coherence length of 20 nm, which is about an order of magnitude larger than the reported values for comparable experiments. The energy distribution of an ensemble of single-electron pulses from a photoemission source is directly linked to the mismatch between the photon energy and the cathode's work function. This excess energy can be reduced by using a photon energy close to the material's work function. Using a tunable source of ultraviolet pulses, we demonstrate the reduction of the velocity spread of the electrons, resulting in a shorter duration of the electron pulses. The reduced electron pulse durations achieved by a tunable excitation or by other approaches require new characterization techniques for electron pulses. We developed a novel method for the characterization of electron pulses at

Fast and ultrafast MR-imaging of the heart

International Nuclear Information System (INIS)

Schulthess, G.K. von; Davis, C.P.; Debatin, J.F.; McKinnon, G.C.

1995-01-01

MRI has been hampered by long image acquisition times. This combined with its non-realtime nature and the limited spatial resolution has made it difficult to extend MRT to the study of small cardiac structures. Recent technical improvements have made breath-held or realtime MRI feasible and thus laid the foundations for further applications in the field of cardiovascular imaging, notably MR coronary angiography, imaging of cardiac valve leaflets, as well as firstpass perfusion studies. Moreover ultrafast MR techniques may eventually replace conventional data acquisition strategies and thus drastically increase patient throughput by shortening acquisition time. This article provides an overview of the technical advances in MRI and their application to the cardiovascular system and discusses possibilities of combined ultrafast and interventional strategies. (orig.) [de

Quantum Computation with Ultrafast Laser Pulse Shaping

Indian Academy of Sciences (India)

Home; Journals; Resonance – Journal of Science Education; Volume 10; Issue 6. Quantum Computation with Ultrafast Laser Pulse Shaping. Debabrata Goswami. General Article Volume 10 Issue 6 June 2005 pp 8-14. Fulltext. Click here to view fulltext PDF. Permanent link:

Detection of coronary calcification in ultrafast CT compared to coronary angiography

International Nuclear Information System (INIS)

Koesling, S.; Hoffmann, U.; Rother, T.; Lieberenz, S.; Heywang-Koebrunner, S.H.; Schulz, H.G.

1994-01-01

The angiographical findings of 24 patients with coronary artery disease were compared with qualitative and quantitative detection of coronary calcification by ultrafast CT. Doubts concerning the capabilities of the ultrafast CT for a screening of coronary artery disease arise when the results of one third false positive and fase negative findings are considered. Variations in the quantification of coronary calcification were too great to allow a realistic assessment of the degree of stenosis of the coronary arteries. (orig.) [de

Spin squeezing of atomic ensembles via nuclear-electronic spin entanglement

DEFF Research Database (Denmark)

Fernholz, Thomas; Krauter, Hanna; Jensen, Kasper

2008-01-01

quantum limit for quantum memory experiments and applications in quantum metrology and is thus a complementary alternative to spin squeezing obtained via inter-atom entanglement. Squeezing of the collective spin is verified by quantum state tomography.......We demonstrate spin squeezing in a room temperature ensemble of 1012 Cesium atoms using their internal structure, where the necessary entanglement is created between nuclear and electronic spins of each individual atom. This state provides improvement in measurement sensitivity beyond the standard...

Nitrogen plasma formation through terahertz-induced ultrafast electron field emission

DEFF Research Database (Denmark)

Iwaszczuk, Krzysztof; Zalkovskij, Maksim; Strikwerda, Andrew

2015-01-01

Electron microscopy and electron diffraction techniques rely on electron sources. Those sources require strong electric fields to extract electrons from metals, either by the photoelectric effect, driven by multiphoton absorption of strong laser fields, or in the static field emission regime....... Terahertz (THz) radiation, commonly understood to be nonionizing due to its low photon energy, is here shown to produce electron field emission. We demonstrate that a carrier-envelope phase-stable single-cycle optical field at THz frequencies interacting with a metallic microantenna can generate...... and accelerate ultrashort and ultrabright electron bunches into free space, and we use these electrons to excite and ionize ambient nitrogen molecules near the antenna. The associated UV emission from the gas forms a novel THz wave detector, which, in contrast with conventional photon-counting or heat...

Retrieval of interatomic separations of molecules from laser-induced high-order harmonic spectra

Energy Technology Data Exchange (ETDEWEB)

Le, Van-Hoang; Nguyen, Ngoc-Ty [Department of Physics, University of Pedagogy, 280 An Duong Vuong, Ward 5, Ho Chi Minh City (Viet Nam); Jin, C; Le, Anh-Thu; Lin, C D [J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS 66506 (United States)

2008-04-28

We illustrate an iterative method for retrieving the internuclear separations of N{sub 2}, O{sub 2} and CO{sub 2} molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is preferable to retrieve the interatomic separation iteratively by fitting the extracted dipole moment. Our results show that time-resolved chemical imaging of molecules using infrared laser pulses with femtosecond temporal resolutions is possible.

Highly sensitive and ultrafast response surface acoustic wave humidity sensor based on electrospun polyaniline/poly(vinyl butyral) nanofibers

International Nuclear Information System (INIS)

Lin Qianqian; Li Yang; Yang Mujie

2012-01-01

Highlights: ► Polyanline/poly(vinyl butyral) nanofibers are prepared by electrospinning. ► Nanofiber-based SAW humidity sensor show high sensitivity and ultrafast response. ► The SAW sensor can detect very low humidity. - Abstract: Polyaniline (PANi) composite nanofibers were deposited on surface acoustic wave (SAW) resonator with a central frequency of 433 MHz to construct humidity sensors. Electrospun nanofibers of poly(methyl methacrylate), poly(vinyl pyrrolidone), poly(ethylene oxide), poly(vinylidene fluoride), poly(vinyl butyral) (PVB) were characterized by scanning electron microscopy, and humidity response of corresponding SAW humidity sensors were investigated. The results indicated that PVB was suitable as a matrix to form nanofibers with PANi by electrospinning (ES). Electrospun PANi/PVB nanofibers exhibited a core–sheath structure as revealed by transmittance electron microscopy. Effects of ES collection time on humidity response of SAW sensor based on PANi/PVB nanofibers were examined at room temperature. The composite nanofiber sensor exhibited very high sensitivity of ∼75 kHz/%RH from 20 to 90%RH, ultrafast response (1 s and 2 s for humidification and desiccation, respectively) and good sensing linearity. Furthermore, the sensor could detect humidity as low as 0.5%RH, suggesting its potentials for low humidity detection. Attempts were done to explain the attractive humidity sensing performance of the sensor by considering conductivity, hydrophilicity, viscoelasticity and morphology of the polymer composite nanofibers.

Complete elimination of nonlinear light-matter interactions with broadband ultrafast laser pulses

DEFF Research Database (Denmark)

Shu, Chuan-Cun; Dong, Daoyi; Petersen, Ian R.

2017-01-01

optical effects, however, the probability of pure single-photon absorption is usually very low, which is particularly pertinent in the case of strong ultrafast laser pulses with broad bandwidth. Here we demonstrate theoretically a counterintuitive coherent single-photon absorption scheme by eliminating...... nonlinear interactions of ultrafast laser pulses with quantum systems. That is, a completely linear response of the system with respect to the spectral energy density of the incident light at the transition frequency can be obtained for all transition probabilities between 0 and 100% in multilevel quantum...... systems. To that end, a multiobjective optimization algorithm is developed to find an optimal spectral phase of an ultrafast laser pulse, which is capable of eliminating all possible nonlinear optical responses while maximizing the probability of single-photon absorption between quantum states. This work...

Progress in Ultrafast Intense Laser Science III

CERN Document Server

Yamanouchi, Kaoru; Agostini, Pierre; Ferrante, Gaetano

2008-01-01

The PUILS series presents Progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science. PUILS has been stimulated by the recent development of ultrafast laser technologies. Each volume contains approximately 15 chapters, authored by researchers at the forefront. Each chapter opens with an overview of the topics to be discussed, so that researchers, who are not experts in the specific topics, as well as graduate students can grasp the importance and attractions of this sub-field of research, and these are followed by reports of cutting-edge discoveries. This third volume covers a diverse range of disciplines, focusing on such topics as strong field ionization of atoms, ionization and fragmentation of molecules and clusters, generation of high-order harmonics and attosecond pulses, filamentation and laser plasma interaction, and the development of ultrashort and ultrahigh-intensity light sources.

Progress in Ultrafast Intense Laser Science VIII

CERN Document Server

Nisoli, Mauro; Hill, Wendell; III, III

2012-01-01

The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science and optical science which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield as well as graduate students can grasp the importance and attractions of the research topic at hand. These are followed by reports of cutting-edge discoveries. This eighth volume covers a broad range of topics from this interdisciplinary research field, focusing on molecules interacting with ultrashort and intense laser fields, advanced technologies for the characterization of ultrashort laser pulses and their applications, laser plasma formation and laser acceleration.

Progress in Ultrafast Intense Laser Science VI

CERN Document Server

Yamanouchi, Kaoru; Bandrauk, André D

2010-01-01

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

Development of an interatomic EAM type potential for Zr; Desarrollo de un potencial interatomico del tipo EAM para Zr

Energy Technology Data Exchange (ETDEWEB)

Pasianot, R C; Monti, A M [Comision Nacional de Energia Atomica, San Martin (Argentina). Unidad de Actividad Materiales

1997-12-31

In the present work are developed interatomic potentials of the embedded atom type (EAM) adequate for computer simulation of microstructural defects in the Zr lattice. It is observed that the less repulsive potential agrees better with the experimental data of the self-interstitial relaxation volume and predicts the basal crowdion as the stable configuration, the basal dumbbell having a formation energy slightly higher (0.01 eV). (author). 9 refs., 1 fig., 3 tabs.

Thermal conductance of suspended nanoribbons: interplay between strain and interatomic potential nonlinearity

Science.gov (United States)

Barreto, Roberto; Florencia Carusela, M.; Monastra, Alejandro G.

2017-10-01

We investigate the role that nonlinearity in the interatomic potential has on the thermal conductance of a suspended nanoribbon when it is subjected to a longitudinal strain. To focus on the first cubic and quartic nonlinear terms of a general potential, we propose an atomic system based on an α-β Fermi-Pasta-Ulam nearest neighbor interaction. We perform classical molecular dynamics simulations to investigate the contribution of longitudinal, transversal and flexural modes to the thermal conductance as a function of the α-β parameters and the applied strain. We compare the cases where atoms are allowed to vibrate only in plane (2D) with the case of vibrations in and out of plane (3D). We find that the dependence of conductance on α and β relies on a crossover phenomenon between linear/nonlinear delocalized/localized flexural and transversal modes, driven by an on/off switch of the strain.

Simple and robust generation of ultrafast laser pulse trains using polarization-independent parallel-aligned thin films

Science.gov (United States)

Wang, Andong; Jiang, Lan; Li, Xiaowei; Wang, Zhi; Du, Kun; Lu, Yongfeng

2018-05-01

Ultrafast laser pulse temporal shaping has been widely applied in various important applications such as laser materials processing, coherent control of chemical reactions, and ultrafast imaging. However, temporal pulse shaping has been limited to only-in-lab technique due to the high cost, low damage threshold, and polarization dependence. Herein we propose a novel design of ultrafast laser pulse train generation device, which consists of multiple polarization-independent parallel-aligned thin films. Various pulse trains with controllable temporal profile can be generated flexibly by multi-reflections within the splitting films. Compared with other pulse train generation techniques, this method has advantages of compact structure, low cost, high damage threshold and polarization independence. These advantages endow it with high potential for broad utilization in ultrafast applications.

Ultrafast carrier dynamics in a GaN/Al 0.18Ga0.82N superlattice

Science.gov (United States)

Mahler, Felix; Tomm, Jens W.; Reimann, Klaus; Woerner, Michael; Elsaesser, Thomas; Flytzanis, Christos; Hoffmann, Veit; Weyers, Markus

2018-04-01

Relaxation processes of photoexcited carriers in a GaN /Al0.18Ga0.82N superlattice are studied in femtosecond spectrally resolved reflectivity measurements at ambient temperature. The transient reflectivity reveals electron trapping into defect states close to the conduction-band minimum with a 150-200 fs time constant, followed by few-picosecond carrier cooling. A second slower trapping process into a different manifold of defect states is observed on a time scale of approximately 10 ps. Our results establish the prominent role of structural defects and disorder for ultrafast carrier dynamics in nitride semiconductor structures.

Synchronization of x-ray pulses to the pump laser in an ultrafast x-ray facility

International Nuclear Information System (INIS)

Corlett, J.N.; Barry, W.; Byrd, J.M.; Schoenlein, R.; Zholents, A.

2002-01-01

Accurate timing of ultrafast x-ray probe pulses emitted from a synchrotron radiation source with respect to a pump laser exciting processes in the sample under study is critical for the investigation of structural dynamics in the femtosecond regime. We describe a scheme for synchronizing femtosecond x-ray pulses relative to a pump laser. X-ray pulses of <100 fs duration are generated from a proposed source based on a recirculating superconducting linac [1,2,3]. Short x-ray pulses are obtained by a process of electron pulse compression, followed by transverse temporal correlation of the electrons, and ultimately x-ray pulse compression. Timing of the arrival of the x-ray pulse with respect to the pump laser is found to be dominated by the operation of the deflecting cavities which provide the transverse temporal correlation of the electrons. The deflecting cavities are driven from a highly stable RF signal derived from a modelocked laser oscillator which is also the origin of the pump l aser pulses

Ultrafast comparison of personal genomes

OpenAIRE

Mauldin, Denise; Hood, Leroy; Robinson, Max; Glusman, Gustavo

2017-01-01

We present an ultra-fast method for comparing personal genomes. We transform the standard genome representation (lists of variants relative to a reference) into 'genome fingerprints' that can be readily compared across sequencing technologies and reference versions. Because of their reduced size, computation on the genome fingerprints is fast and requires little memory. This enables scaling up a variety of important genome analyses, including quantifying relatedness, recognizing duplicative s...

Parametric spectro-temporal analyzer (PASTA) for ultrafast optical performance monitoring

Science.gov (United States)

Zhang, Chi; Wong, Kenneth K. Y.

2013-12-01

Ultrafast optical spectrum monitoring is one of the most challenging tasks in observing ultrafast phenomena, such as the spectroscopy, dynamic observation of the laser cavity, and spectral encoded imaging systems. However, conventional method such as optical spectrum analyzer (OSA) spatially disperses the spectrum, but the space-to-time mapping is realized by mechanical rotation of a grating, so are incapable of operating at high speed. Besides the spatial dispersion, temporal dispersion provided by dispersive fiber can also stretches the spectrum in time domain in an ultrafast manner, but is primarily confined in measuring short pulses. In view of these constraints, here we present a real-time spectrum analyzer called parametric spectro-temporal analyzer (PASTA), which is based on the time-lens focusing mechanism. It achieves a 100-MHz frame rate and can measure arbitrary waveforms. For the first time, we observe the dynamic spectrum of an ultrafast swept-source: Fourier domain mode-locked (FDML) laser, and the spectrum evolution of a laser cavity during its stabilizing process. In addition to the basic single-lens structure, the multi-lens configurations (e.g. telescope or wide-angle scope) will provide a versatile operating condition, which can zoom in to achieve 0.05-nm resolution and zoom out to achieve 10-nm observation range, namely 17 times zoom in/out ratio. In view of the goal of achieving spectrum analysis with fine accuracy, PASTA provides a promising path to study the real-time spectrum of some dynamic phenomena and non-repetitive events, with orders of magnitude enhancement in the frame rate over conventional OSAs.

All-optical devices for ultrafast packet switching

DEFF Research Database (Denmark)

Dorren, H.J.S.; HerreraDorren, J.; Raz, O.

2007-01-01

We discuss integrated devices for all-optical packet switching. We focus on monolithically integrated all-optical flip-flops, ultra-fast semiconductor based wavelength converters and explain the operation principles. Finally, a 160 Gb/s all-optical packet switching experiment over 110 km of field...

Silicon as a virtual plasmonic material: Acquisition of its transient optical constants and the ultrafast surface plasmon-polariton excitation

Energy Technology Data Exchange (ETDEWEB)

Danilov, P. A.; Ionin, A. A.; Kudryashov, S. I., E-mail: sikudr@sci.lebedev.ru; Makarov, S. V.; Rudenko, A. A. [Lebedev Physical Institute (Russian Federation); Saltuganov, P. N. [Moscow Institute of Physics and Technology (State University) (Russian Federation); Seleznev, L. V.; Yurovskikh, V. I.; Zayarny, D. A. [Lebedev Physical Institute (Russian Federation); Apostolova, T. [Bulgarian Academy of Sciences, Institute for Nuclear Research and Nuclear Energetics (Bulgaria)

2015-06-15

Ultrafast intense photoexcitation of a silicon surface is complementarily studied experimentally and theoretically, with its prompt optical dielectric function obtained by means of time-resolved optical reflection microscopy and the underlying electron-hole plasma dynamics modeled numerically, using a quantum kinetic approach. The corresponding transient surface plasmon-polariton (SPP) dispersion curves of the photo-excited material were simulated as a function of the electron-hole plasma density, using the derived optical dielectric function model, and directly mapped at several laser photon energies, measuring spatial periods of the corresponding SPP-mediated surface relief nanogratings. The unusual spectral dynamics of the surface plasmon resonance, initially increasing with the increase in the electron-hole plasma density but damped at high interband absorption losses induced by the high-density electron-hole plasma through instantaneous bandgap renormalization, was envisioned through the multi-color mapping.

Ultrafast Control of Magnetism in Ferromagnetic Semiconductors via Photoexcited Transient Carriers

Energy Technology Data Exchange (ETDEWEB)

Cotoros, Ingrid A. [Univ. of California, Berkeley, CA (United States)

2008-12-01

The field of spintronics offers perspectives for seamless integration of coupled and inter-tunable electrical and magnetic properties in a single device. For integration of the spin degree of freedom with current electronic technology, new semiconductors are needed that show electrically-tunable magnetic properties at room temperature and above. Dilute magnetic semiconductors derived from III-V compounds, like GaMnAs and InMnAs, show coupled and tunable magnetic, transport, and optical properties, due to the fact that their ferromagnetism is hole-mediated. These unconventional materials are ideal systems for manipulating the magnetic order by changing the carrier polarization, population density, and energy band distribution of the complementary subsystem of holes. This is the main theme we cover in this thesis. In particular, we develop a unique setup by use of ultraviolet pump, near-infrared probe femtosecond laser pulses, that allows for magneto-optical Kerr effect (MOKE) spectroscopy experiments. We photo-excite transient carriers in our samples, and measure the induced transient magnetization dynamics. One set of experiments performed allowed us to observe for the first time enhancement of the ferromagnetic order in GaMnAs, on an ultrafast time scale of hundreds of picoseconds. The corresponding transient increase of Curie temperature (Tc, the temperature above which a ferromagnetic material loses its permanent magnetism) of about 1 K for our experimental conditions is a very promising result for potential spintronics applications, especially since it is seconded by observation of an ultrafast ferromagnetic to paramagnetic phase transition above Tc. In a different set of experiments, we "write" the magnetization in a particular orientation in the sample plane. Using an ultrafast scheme, we alter the distribution of holes in the system and detect signatures of the particular memory state in the subsequent magnetization dynamics, with unprecedented hundreds of

Ultrafast Carrier Trapping of a Metal-Doped Titanium Dioxide Semiconductor Revealed by Femtosecond Transient Absorption Spectroscopy

KAUST Repository

Sun, Jingya; Yang, Yang; Khan, Jafar I.; Alarousu, Erkki; Guo, Zaibing; Zhang, Xixiang; Zhang, Qiang; Mohammed, Omar F.

2014-01-01

We explored for the first time the ultrafast carrier trapping of a metal-doped titanium dioxide (TiO2) semiconductor using broad-band transient absorption (TA) spectroscopy with 120 fs temporal resolution. Titanium dioxide was successfully doped layer-by-layer with two metal ions, namely tungsten and cobalt. The time-resolved data demonstrate clearly that the carrier trapping time decreases progressively as the doping concentration increases. A global-fitting procedure for the carrier trapping suggests the appearance of two time components: a fast one that is directly associated with carrier trapping to the defect state in the vicinity of the conduction band and a slow one that is attributed to carrier trapping to the deep-level state from the conduction band. With a relatively long doping deposition time on the order of 30 s, a carrier lifetime of about 1 ps is obtained. To confirm that the measured ultrafast carrier dynamics are associated with electron trapping by metal doping, we explored the carrier dynamics of undoped TiO2. The findings reported here may be useful for the implementation of high-speed optoelectronic applications and fast switching devices.

Ultrafast Carrier Trapping of a Metal-Doped Titanium Dioxide Semiconductor Revealed by Femtosecond Transient Absorption Spectroscopy

KAUST Repository

Sun, Jingya

2014-06-11

We explored for the first time the ultrafast carrier trapping of a metal-doped titanium dioxide (TiO2) semiconductor using broad-band transient absorption (TA) spectroscopy with 120 fs temporal resolution. Titanium dioxide was successfully doped layer-by-layer with two metal ions, namely tungsten and cobalt. The time-resolved data demonstrate clearly that the carrier trapping time decreases progressively as the doping concentration increases. A global-fitting procedure for the carrier trapping suggests the appearance of two time components: a fast one that is directly associated with carrier trapping to the defect state in the vicinity of the conduction band and a slow one that is attributed to carrier trapping to the deep-level state from the conduction band. With a relatively long doping deposition time on the order of 30 s, a carrier lifetime of about 1 ps is obtained. To confirm that the measured ultrafast carrier dynamics are associated with electron trapping by metal doping, we explored the carrier dynamics of undoped TiO2. The findings reported here may be useful for the implementation of high-speed optoelectronic applications and fast switching devices.

Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

Directory of Open Access Journals (Sweden)

Pramod Kumar Verma

2016-03-01

Full Text Available We employ transient absorption from the deep-UV to the visible region and fluorescence upconversion to investigate the photoinduced excited-state intramolecular proton-transfer dynamics in a biologically relevant drug molecule, 2-acetylindan-1,3-dione. The molecule is a ß-diketone which in the electronic ground state exists as exocyclic enol with an intramolecular H-bond. Upon electronic excitation at 300 nm, the first excited state of the exocyclic enol is initially populated, followed by ultrafast proton transfer (≈160 fs to form the vibrationally hot endocyclic enol. Subsequently, solvent-induced vibrational relaxation takes place (≈10 ps followed by decay (≈390 ps to the corresponding ground state.

Real-time visualization of soliton molecules with evolving behavior in an ultrafast fiber laser

Science.gov (United States)

Liu, Meng; Li, Heng; Luo, Ai-Ping; Cui, Hu; Xu, Wen-Cheng; Luo, Zhi-Chao

2018-03-01

Ultrafast fiber lasers have been demonstrated to be great platforms for the investigation of soliton dynamics. The soliton molecules, as one of the most fascinating nonlinear phenomena, have been a hot topic in the field of nonlinear optics in recent years. Herein, we experimentally observed the real-time evolving behavior of soliton molecule in an ultrafast fiber laser by using the dispersive Fourier transformation technology. Several types of evolving soliton molecules were obtained in our experiments, such as soliton molecules with monotonically or chaotically evolving phase, flipping and hopping phase. These results would be helpful to the communities interested in soliton nonlinear dynamics as well as ultrafast laser technologies.

Atomic and electronic structure transformations of silver nanoparticles under rapid cooling conditions

OpenAIRE

Lobato, I.; Rojas, J.; Landauro, C. V.; Torres, J.

2008-01-01

The structural evolution and dynamics of silver nanodrops Ag${}_{2896}$ (4.4 nm in diameter) during rapid cooling conditions has been studied by means of molecular dynamics simulations and electronic density of state calculations. The interaction of silver atoms is modeled by a tight-binding semiempirical interatomic potential proposed by Cleri and Rosato. The pair correlation functions and the pair analysis technique is applied to reveal the structural transition in the process of solidifica...

Interest in broadband dielectric spectroscopy to study the electronic transport in materials for lithium batteries

Energy Technology Data Exchange (ETDEWEB)

Badot, Jean-Claude, E-mail: jc.badot@chimie-paristech.fr [Institut de Recherche de Chimie Paris, UMR CNRS 8247, Réseau sur le Stockage Electrochimique de l' Energie (RS2E), Chimie Paris Tech, PSL*, 11 rue P. et M. Curie, 75231 Cedex 05 Paris (France); Lestriez, Bernard [Institut des Matériaux Jean Rouxel, UMR CNRS 6502, Université de Nantes, 2 rue de la Houssinière, BP32229, 44322 Nantes (France); Dubrunfaut, Olivier [GeePs | Group of electrical engineering – Paris, UMR CNRS 8507, CentraleSupélec, Univ. Paris-Sud, Université Paris-Saclay, Sorbonne Universités, UPMC Univ Paris 06, 3 & 11 rue Joliot-Curie, Plateau de Moulon, 91192 Gif-sur-Yvette CEDEX, Paris (France)

2016-11-15

Highlights: • Broadband dielectric spectroscopy measures the multiscale electronic conductivity from macroscopic to interatomic sizes. • There is an influence of the surface states on the electronic transfer of powdered materials (e.g. thin insulating layer of Li{sub 2}CO{sub 3} on LiNiO{sub 2} and carbon coating on LiFePO{sub 4}). • Electrical relaxations resulting from the interfacial polarizations at the different scales of the carbon black network are evidenced. - Abstract: Broadband dielectric spectroscopy (BDS) is used to measure complex permittivity and conductivity of conducting materials for lithium batteries at frequencies from a few Hz to several GHz with network and impedance analysers. Under the influence of an electric field, there will be charge density fluctuations in the conductor mainly due to electronic transfer. These fluctuations result in dielectric relaxations for frequencies below 100 GHz. The materials are compacted powders in which each element (particles, agglomerates of particles) can have different sizes and morphologies. In the present review, studies are reported on the influence of surface states in LiNiO{sub 2} (ageing and degradation in air) and LiFePO{sub 4} (carbon coating thin layer), and on a composite electrode based on the lithium trivanadate (Li{sub 1.1}V{sub 3}O{sub 8}) active material. The results have shown that the BDS technique is very sensitive to the different scales of materials architectures involved in electronic transport, from interatomic distances to macroscopic sizes.

Interest in broadband dielectric spectroscopy to study the electronic transport in materials for lithium batteries

International Nuclear Information System (INIS)

Badot, Jean-Claude; Lestriez, Bernard; Dubrunfaut, Olivier

2016-01-01

Highlights: • Broadband dielectric spectroscopy measures the multiscale electronic conductivity from macroscopic to interatomic sizes. • There is an influence of the surface states on the electronic transfer of powdered materials (e.g. thin insulating layer of Li_2CO_3 on LiNiO_2 and carbon coating on LiFePO_4). • Electrical relaxations resulting from the interfacial polarizations at the different scales of the carbon black network are evidenced. - Abstract: Broadband dielectric spectroscopy (BDS) is used to measure complex permittivity and conductivity of conducting materials for lithium batteries at frequencies from a few Hz to several GHz with network and impedance analysers. Under the influence of an electric field, there will be charge density fluctuations in the conductor mainly due to electronic transfer. These fluctuations result in dielectric relaxations for frequencies below 100 GHz. The materials are compacted powders in which each element (particles, agglomerates of particles) can have different sizes and morphologies. In the present review, studies are reported on the influence of surface states in LiNiO_2 (ageing and degradation in air) and LiFePO_4 (carbon coating thin layer), and on a composite electrode based on the lithium trivanadate (Li_1_._1V_3O_8) active material. The results have shown that the BDS technique is very sensitive to the different scales of materials architectures involved in electronic transport, from interatomic distances to macroscopic sizes.

Electronic self-organization in layered transition metal dichalcogenides

Energy Technology Data Exchange (ETDEWEB)

Ritschel, Tobias

2015-10-30

The interplay between different self-organized electronically ordered states and their relation to unconventional electronic properties like superconductivity constitutes one of the most exciting challenges of modern condensed matter physics. In the present thesis this issue is thoroughly investigated for the prototypical layered material 1T-TaS{sub 2} both experimentally and theoretically. At first the static charge density wave order in 1T-TaS{sub 2} is investigated as a function of pressure and temperature by means of X-ray diffraction. These data indeed reveal that the superconductivity in this material coexists with an inhomogeneous charge density wave on a macroscopic scale in real space. This result is fundamentally different from a previously proposed separation of superconducting and insulating regions in real space. Furthermore, the X-ray diffraction data uncover the important role of interlayer correlations in 1T-TaS{sub 2}. Based on the detailed insights into the charge density wave structure obtained by the X-ray diffraction experiments, density functional theory models are deduced in order to describe the electronic structure of 1T-TaS{sub 2} in the second part of this thesis. As opposed to most previous studies, these calculations take the three-dimensional character of the charge density wave into account. Indeed the electronic structure calculations uncover complex orbital textures, which are interwoven with the charge density wave order and cause dramatic differences in the electronic structure depending on the alignment of the orbitals between neighboring layers. Furthermore, it is demonstrated that these orbital-mediated effects provide a route to drive semiconductor-to-metal transitions with technologically pertinent gaps and on ultrafast timescales. These results are particularly relevant for the ongoing development of novel, miniaturized and ultrafast devices based on layered transition metal dichalcogenides. The discovery of orbital textures

Tracking Ultrafast Carrier Dynamics in Single Semiconductor Nanowire Heterostructures

Directory of Open Access Journals (Sweden)

Taylor A.J.

2013-03-01

Full Text Available An understanding of non-equilibrium carrier dynamics in silicon (Si nanowires (NWs and NW heterostructures is very important due to their many nanophotonic and nanoelectronics applications. Here, we describe the first measurements of ultrafast carrier dynamics and diffusion in single heterostructured Si nanowires, obtained using ultrafast optical microscopy. By isolating individual nanowires, we avoid complications resulting from the broad size and alignment distribution in nanowire ensembles, allowing us to directly probe ultrafast carrier dynamics in these quasi-one-dimensional systems. Spatially-resolved pump-probe spectroscopy demonstrates the influence of surface-mediated mechanisms on carrier dynamics in a single NW, while polarization-resolved femtosecond pump-probe spectroscopy reveals a clear anisotropy in carrier lifetimes measured parallel and perpendicular to the NW axis, due to density-dependent Auger recombination. Furthermore, separating the pump and probe spots along the NW axis enabled us to track space and time dependent carrier diffusion in radial and axial NW heterostructures. These results enable us to reveal the influence of radial and axial interfaces on carrier dynamics and charge transport in these quasi-one-dimensional nanosystems, which can then be used to tailor carrier relaxation in a single nanowire heterostructure for a given application.

Ultra-fast secure communication with complex systems in classical channels (Conference Presentation)

KAUST Repository

Mazzone, Valerio

2017-04-28

Developing secure communications is a research area of growing interest. During the past years, several cryptographic schemes have been developed, with Quantum cryptography being a promising scheme due to the use of quantum effects, which make very difficult for an eavesdropper to intercept the communication. However, practical quantum key distribution methods have encountered several limitations; current experimental realizations, in fact, fail to scale up on long distances, as well as in providing unconditional security and speed comparable to classical optical communications channels. Here we propose a new, low cost and ultra-fast cryptographic system based on a fully classical optical channel. Our cryptographic scheme exploits the complex synchronization of two different random systems (one on the side of the sender and another on the side of the receiver) to realize a “physical” one paid system. The random medium is created by an optical chip fabricated through electron beam lithography on a Silicon On Insulator (SOI) substrate. We present experiments with ps lasers and commercial fibers, showing the ultrafast distribution of a random key between two users (Alice and Bob), with absolute no possibility for a passive/active eavesdropper to intercept the communication. Remarkably, this system enables the same security of quantum cryptography, but with the use of a classical communication channel. Our system exploits a unique synchronization that exists between two different random systems, and at such is extremely versatile and can enable safe communications among different users in standards telecommunications channels.

The Ultrafast Wolff Rearrangement in the Gas Phase

Science.gov (United States)

Steinbacher, Andreas; Roeding, Sebastian; Brixner, Tobias; Nuernberger, Patrick

The Wolff rearrangement of gas-phase 5-diazo Meldrum's acid is disclosed with femtosecond ion spectroscopy. Distinct differences are found for 267 nm and 200 nm excitation, the latter leading to even two ultrafast rearrangement reactions.

Proposal to DOE Basic Energy Sciences Ultrafast X-ray science facility at the Advanced Light Source

CERN Document Server

Schönlein, R W; Alivisatos, A P; Belkacem, A; Berrah, N; Bozek, J; Bressler, C; Cavalleri, A; Chang, Z; Chergui, M; Falcone, R W; Glover, T E; Heimann, P A; Hepburn, J; Larsson, J; Lee, R W; McCusker, J; Padmore, H A; Pattison, P; Pratt, S T; Robin, D W; Schlüter, Ross D; Shank, C V; Wark, J; Zholents, A A; Zolotorev, M S

2001-01-01

We propose to develop a true user facility for ultrafast x-ray science at the Advanced Light Source. This facility will be unique in the world, and will fill a critical need for the growing ultrafast x-ray research community. The development of this facility builds upon the expertise from long-standing research efforts in ultrafast x-ray spectroscopy and the development of femtosecond x-ray sources and techniques at both the Lawrence Berkeley National Laboratory and at U.C. Berkeley. In particular, the technical feasibility of a femtosecond x-ray beamline at the ALS has already been demonstrated, and existing ultrafast laser technology will enable such a beamline to operate near the practical limit for femtosecond x-ray flux and brightness from a 3rd generation synchrotron.

Proposal to DOE Basic Energy Sciences: Ultrafast X-ray science facility at the Advanced Light Source

Energy Technology Data Exchange (ETDEWEB)

Schoenlein, Robert W.; Falcone, Roger W.; Abela, R.; Alivisatos, A.P.; Belkacem, A.; Berrah, N.; Bozek, J.; Bressler, C.; Cavalleri, A.; Chergui, M.; Glover, T.E.; Heimann, P.A.; Hepburn, J.; Larsson, J.; Lee, R.W.; McCusker, J.; Padmore, H.A.; Pattison, P.; Pratt, S.T.; Shank, C.V.; Wark, J.; Chang, Z.; Robin, D.W.; Schlueter, R.D.; Zholents, A.A.; Zolotorev, M.S.

2001-12-12

We propose to develop a true user facility for ultrafast x-ray science at the Advanced Light Source. This facility will be unique in the world, and will fill a critical need for the growing ultrafast x-ray research community. The development of this facility builds upon the expertise from long-standing research efforts in ultrafast x-ray spectroscopy and the development of femtosecond x-ray sources and techniques at both the Lawrence Berkeley National Laboratory and at U.C. Berkeley. In particular, the technical feasibility of a femtosecond x-ray beamline at the ALS has already been demonstrated, and existing ultrafast laser technology will enable such a beamline to operate near the practical limit for femtosecond x-ray flux and brightness from a 3rd generation synchrotron.

Proposal to DOE Basic Energy Sciences: Ultrafast X-ray science facility at the Advanced Light Source

International Nuclear Information System (INIS)

Schoenlein, Robert W.; Falcone, Roger W.; Abela, R.; Alivisatos, A.P.; Belkacem, A.; Berrah, N.; Bozek, J.; Bressler, C.; Cavalleri, A.; Chergui, M.; Glover, T.E.; Heimann, P.A.; Hepburn, J.; Larsson, J.; Lee, R.W.; McCusker, J.; Padmore, H.A.; Pattison, P.; Pratt, S.T.; Shank, C.V.; Wark, J.; Chang, Z.; Robin, D.W.; Schlueter, R.D.; Zholents, A.A.; Zolotorev, M.S.

2001-01-01

We propose to develop a true user facility for ultrafast x-ray science at the Advanced Light Source. This facility will be unique in the world, and will fill a critical need for the growing ultrafast x-ray research community. The development of this facility builds upon the expertise from long-standing research efforts in ultrafast x-ray spectroscopy and the development of femtosecond x-ray sources and techniques at both the Lawrence Berkeley National Laboratory and at U.C. Berkeley. In particular, the technical feasibility of a femtosecond x-ray beamline at the ALS has already been demonstrated, and existing ultrafast laser technology will enable such a beamline to operate near the practical limit for femtosecond x-ray flux and brightness from a 3rd generation synchrotron

Nanoscale electron manipulation in metals with intense THz electric fields

Science.gov (United States)

Takeda, Jun; Yoshioka, Katsumasa; Minami, Yasuo; Katayama, Ikufumi

2018-03-01

Improved control over the electromagnetic properties of metals on a nanoscale is crucial for the development of next-generation nanoelectronics and plasmonic devices. Harnessing the terahertz (THz)-electric-field-induced nonlinearity for the motion of electrons is a promising method of manipulating the local electromagnetic properties of metals, while avoiding undesirable thermal effects and electronic transitions. In this review, we demonstrate the manipulation of electron delocalization in ultrathin gold (Au) films with nanostructures, by intense THz electric-field transients. On increasing the electric-field strength of the THz pulses, the transmittance in the THz-frequency region abruptly decreases around the percolation threshold. The observed THz-electric-field-induced nonlinearity is analysed, based on the Drude-Smith model. The results suggest that ultrafast electron delocalization occurs by electron tunnelling across the narrow insulating bridge between the Au nanostructures, without material breakdown. In order to quantitatively discuss the tunnelling process, we perform scanning tunnelling microscopy with carrier-envelope phase (CEP)-controlled single-cycle THz electric fields. By applying CEP-controlled THz electric fields to the 1 nm nanogap between a metal nanotip and graphite sample, many electrons could be coherently driven through the quantum tunnelling process, either from the nanotip to the sample or vice versa. The presented concept, namely, electron tunnelling mediated by CEP-controlled single-cycle THz electric fields, can facilitate the development of nanoscale electron manipulation, applicable to next-generation ultrafast nanoelectronics and plasmonic devices.

Intramolecular photoinduced electron-transfer in azobenzene-perylene diimide

International Nuclear Information System (INIS)

Feng Wen-Ke; Wang Shu-Feng; Gong Qi-Huang; Feng Yi-Yu; Feng Wei; Yi Wen-Hui

2010-01-01

This paper studies the intramolecular photoinduced electron-transfer (PET) of covalent bonded azobenzene-perylene diimide (AZO-PDI) in solvents by using steady-state and time-resolved fluorescence spectroscopy together with ultrafast transient absorption spectroscopic techniques. Fast fluorescence quenching is observed when AZO-PDI is excited at characteristic wavelengths of AZO and perylene moieties. Reductive electron-transfer with transfer rate faster than 10 11 s −1 is found. This PET process is also consolidated by femtosecond transient absorption spectra

Ultra-fast X-ray absorption spectroscopy for the study of matter in transient regime; Spectroscopie d'absorption ultra-rapide de rayonnement X pour l'etude de la matiere en regime transitoire

Energy Technology Data Exchange (ETDEWEB)

Lecherbourg, L

2007-12-15

In this work, we study the physics of dense matter, plasmas or solids, using X-ray absorption spectroscopy. Through the use of sources produced by laser-matter interaction, we have measured the absorption spectra of aluminum and bromine plasmas, as well as those of vanadium dioxide (VO{sub 2}). The measurement of absorption coefficients allows us to probe the dense matter and to study its properties. The experiments are carried out following the same principle: they use the same experimental set-up, called pump-probe. When the matter is dense, the absorption properties of an atom are modified by the surrounding environment. In a plasma, it is mainly the bound- bound transitions which are altered: the shapes of those spectral rays are modified. In a solid, the position of the neighbouring atoms in relation to the absorbing atom modify the structure of absorption levels (bound-free transition). The study of this structure allows us to measure the parameters of the material, and provides information such as the state of the electronic band or the interatomic gaps. The experiments carried out at the LULI have allowed us to probe plasmas in the relatively unknown regime of the Warm Dense Matter. One of the key parameters is that the plasma is characterised independently (FDI diagnostic). It allows for a better comparison of the measured absorption against a calculation made with the numerical model OPA-S. The experiments carried out at INRS have led to the realisation of an experimental system having the characteristics which allow the study of the dynamics of solids showing ultra-fast phase transition. For those experiments, we have used vanadium dioxide as a model system allowing us to test the feasibility of the method. (author)

A PSF-shape-based beamforming strategy for robust 2D motion estimation in ultrafast data

NARCIS (Netherlands)

Saris, Anne E.C.M.; Fekkes, Stein; Nillesen, Maartje; Hansen, Hendrik H.G.; de Korte, Chris L.

2018-01-01

This paper presents a framework for motion estimation in ultrafast ultrasound data. It describes a novel approach for determining the sampling grid for ultrafast data based on the system's point-spread-function (PSF). As a consequence, the cross-correlation functions (CCF) used in the speckle

Use of interfacial layers to prolong hole lifetimes in hematite probed by ultrafast transient absorption spectroscopy

Science.gov (United States)

Paradzah, Alexander T.; Diale, Mmantsae; Maabong, Kelebogile; Krüger, Tjaart P. J.

2018-04-01

Hematite is a widely investigated material for applications in solar water oxidation due primarily to its small bandgap. However, full realization of the material continues to be hampered by fast electron-hole recombination rates among other weaknesses such as low hole mobility, short hole diffusion length and low conductivity. To address the problem of fast electron-hole recombination, researchers have resorted to growth of nano-structured hematite, doping and use of under-layers. Under-layer materials enhance the photo-current by minimising electron-hole recombination through suppressing of back electron flow from the substrate, such as fluorine-doped tin oxide (FTO), to hematite. We have carried out ultrafast transient absorption spectroscopy on hematite in which Nb2O5 and SnO2 materials were used as interfacial layers to enhance hole lifetimes. The transient absorption data was fit with four different lifetimes ranging from a few hundred femtoseconds to a few nanoseconds. We show that the electron-hole recombination is slower in samples where interfacial layers are used than in pristine hematite. We also develop a model through target analysis to illustrate the effect of under-layers on electron-hole recombination rates in hematite thin films.

Ultrafast dynamics in CeTe{sub 3} near the pressure-induced charge-density-wave transition

Energy Technology Data Exchange (ETDEWEB)

Tauch, Jonas; Obergfell, Manuel [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Schaefer, Hanjo [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Institute of Physics, Ilmenau University of Technology (Germany); Demsar, Jure [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Institute of Physics, Ilmenau University of Technology (Germany); Institute of Physics, Johannes Gutenberg-University Mainz (Germany); Giraldo, Paula; Fisher, Ian R. [Geballe Laboratory for Advanced Materials and Department of Applied Physics, Stanford University (United States); Pashkin, Alexej [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Helmholtz-Zentrum Dresden-Rossendorf (Germany)

2015-07-01

Femtosecond pump-probe spectroscopy is an efficient tool for studying ultrafast dynamics in strongly correlated electronic systems, in particular, compounds with a charge-density-wave (CDW) order. Application of external pressure often leads to a suppression of a CDW state due to an impairment of the Fermi surface nesting. We combine time-resolved optical spectroscopy and diamond anvil cell technology to study electron and lattice dynamics in tri-telluride compound CeTe{sub 3}. Around pressures of 4 GPa we observe a gradual vanishing of the relaxation process related to the recombination of the photoexcited quasiparticles. The coherent oscillations of the phonon modes coupled to the CDW order parameter demonstrate even more dramatic suppression with increasing pressure. These observations clearly indicate a transition into the metallic state of CeTe{sub 3} induced by the external pressure.

Ultrafast pre-breakdown dynamics in Al₂O₃SiO₂ reflector by femtosecond UV laser spectroscopy.

Science.gov (United States)

Du, Juan; Li, Zehan; Xue, Bing; Kobayashi, Takayoshi; Han, Dongjia; Zhao, Yuanan; Leng, Yuxin

2015-06-29

Ultrafast carrier dynamics in Al2O3/SiO2 high reflectors has been investigated by UV femtosecond laser. It is identified by laser spectroscopy that, the carrier dynamics contributed from the front few layers of Al2O3 play a dominating role in the initial laser-induced damage of the UV reflector. Time-resolved reflection decrease after the UV excitation is observed, and conduction electrons is found to relaxed to a mid-gap defect state locating about one photon below the conduction band . To interpret the laser induced carrier dynamics further, a theoretical model including electrons relaxation to a mid-gap state is built, and agrees very well with the experimental results.. To the best of our knowledge, this is the first study on the pre-damage dynamics in UV high reflector induced by femtosecond UV laser.

Calculation of electron spectra of stoichiometric and nitrogen-deficient zirconium nitrides

International Nuclear Information System (INIS)

Ivashchenko, V.I.; Lisenko, A.A.; Zhurakovskij, E.A.; Bekenev, V.L.

1984-01-01

English structure using the method of associated plane waves - linear combinations of atom orbitals - coherent potential (APW-LCAO-CP) are given. The calculation results for ZrN electron spectrum indicate availability of a Zr-N binding and a Zr-N antibonding bands. The Fermi level lies in the antibonding metal band. While deffecting from the stoichiometric content the Fermi level simultaneously with filling the metal band shifts towards the Variation of the main kinetic parameters with increasing defectiveness in nitrogen is explained by increasing the number of antibonding collectivized electrons. Application of the combined method of APW-LCAO-CP gives a rather realistic picture of interatomic interaction in ZrNsub(x)

Fusion of Ultraviolet-Visible and Infrared Transient Absorption Spectroscopy Data to Model Ultrafast Photoisomerization.

Science.gov (United States)

Debus, Bruno; Orio, Maylis; Rehault, Julien; Burdzinski, Gotard; Ruckebusch, Cyril; Sliwa, Michel

2017-08-03

Ultrafast photoisomerization reactions generally start at a higher excited state with excess of internal vibrational energy and occur via conical intersections. This leads to ultrafast dynamics which are difficult to investigate with a single transient absorption spectroscopy technique, be it in the ultraviolet-visible (UV-vis) or infrared (IR) domain. On one hand, the information available in the UV-vis domain is limited as only slight spectral changes are observed for different isomers. On the other hand, the interpretation of vibrational spectra is strongly hindered by intramolecular relaxation and vibrational cooling. These limitations can be circumvented by fusing UV-vis and IR transient absorption spectroscopy data in a multiset multivariate curve resolution analysis. We apply this approach to describe the spectrodynamics of the ultrafast cis-trans photoisomerization around the C-N double bond observed for aromatic Schiff bases. Twisted intermediate states could be elucidated, and isomerization was shown to occur through a continuous complete rotation. More broadly, data fusion can be used to rationalize a vast range of ultrafast photoisomerization processes of interest in photochemistry.

High speed fluorescence imaging with compressed ultrafast photography

Science.gov (United States)

Thompson, J. V.; Mason, J. D.; Beier, H. T.; Bixler, J. N.

2017-02-01

Fluorescent lifetime imaging is an optical technique that facilitates imaging molecular interactions and cellular functions. Because the excited lifetime of a fluorophore is sensitive to its local microenvironment,1, 2 measurement of fluorescent lifetimes can be used to accurately detect regional changes in temperature, pH, and ion concentration. However, typical state of the art fluorescent lifetime methods are severely limited when it comes to acquisition time (on the order of seconds to minutes) and video rate imaging. Here we show that compressed ultrafast photography (CUP) can be used in conjunction with fluorescent lifetime imaging to overcome these acquisition rate limitations. Frame rates up to one hundred billion frames per second have been demonstrated with compressed ultrafast photography using a streak camera.3 These rates are achieved by encoding time in the spatial direction with a pseudo-random binary pattern. The time domain information is then reconstructed using a compressed sensing algorithm, resulting in a cube of data (x,y,t) for each readout image. Thus, application of compressed ultrafast photography will allow us to acquire an entire fluorescent lifetime image with a single laser pulse. Using a streak camera with a high-speed CMOS camera, acquisition rates of 100 frames per second can be achieved, which will significantly enhance our ability to quantitatively measure complex biological events with high spatial and temporal resolution. In particular, we will demonstrate the ability of this technique to do single-shot fluorescent lifetime imaging of cells and microspheres.

Novel phenomena in clusters irradiated by short-wavelength free-electron lasers

International Nuclear Information System (INIS)

Fukuzawa, Hironobu; Ueda, Kiyoshi

2017-01-01

By electron spectroscopy, we investigated various phenomena that are caused by the irradiation of extreme ultraviolet (EUV) and X-ray free-electron laser (FEL) pulses on rare-gas clusters. The results for the Ne clusters, which were irradiated by EUVFEL pulses at a photon energy of 20.3 eV below the ionization threshold, illustrate that novel interatomic processes yield low-energy electrons. The results for the Xe clusters, irradiated by EUVFEL pulses at a photon energy of 24.3 eV above the threshold, illustrate that nanoplasma is formed as a result of trapping the photoelectrons and consequently emits low-energy thermal electrons. The results for the Ar clusters irradiated by 5 keV XFEL pulses illustrate that nanoplasma is formed by trapping low-energy Auger electrons and secondary electrons in the tens of fs range, and continuous thermal emission from the plasma occurs in the ps range. (author)

Demonstration of Ultra-Fast Switching in Nano metallic Resistive Switching Memory Devices

International Nuclear Information System (INIS)

Yang, Y.

2016-01-01

Interdependency of switching voltage and time creates a dilemma/obstacle for most resistive switching memories, which indicates low switching voltage and ultra-fast switching time cannot be simultaneously achieved. In this paper, an ultra-fast (sub-100 ns) yet low switching voltage resistive switching memory device (“nano metallic ReRAM”) was demonstrated. Experimental switching voltage is found independent of pulse width (intrinsic device property) when the pulse is long but shows abrupt time dependence (“cliff”) as pulse width approaches characteristic RC time of memory device (extrinsic device property). Both experiment and simulation show that the onset of cliff behavior is dependent on physical device size and parasitic resistance, which is expected to diminish as technology nodes shrink down. We believe this study provides solid evidence that nano metallic resistive switching memory can be reliably operated at low voltage and ultra-fast regime, thus beneficial to future memory technology.

Resolving molecular vibronic structure using high-sensitivity two-dimensional electronic spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Bizimana, Laurie A.; Brazard, Johanna; Carbery, William P.; Gellen, Tobias; Turner, Daniel B., E-mail: dturner@nyu.edu [Department of Chemistry, New York University, 100 Washington Square East, New York, New York 10003 (United States)

2015-10-28

Coherent multidimensional optical spectroscopy is an emerging technique for resolving structure and ultrafast dynamics of molecules, proteins, semiconductors, and other materials. A current challenge is the quality of kinetics that are examined as a function of waiting time. Inspired by noise-suppression methods of transient absorption, here we incorporate shot-by-shot acquisitions and balanced detection into coherent multidimensional optical spectroscopy. We demonstrate that implementing noise-suppression methods in two-dimensional electronic spectroscopy not only improves the quality of features in individual spectra but also increases the sensitivity to ultrafast time-dependent changes in the spectral features. Measurements on cresyl violet perchlorate are consistent with the vibronic pattern predicted by theoretical models of a highly displaced harmonic oscillator. The noise-suppression methods should benefit research into coherent electronic dynamics, and they can be adapted to multidimensional spectroscopies across the infrared and ultraviolet frequency ranges.

Microwave-controlled ultrafast synthesis of uniform silver nanocubes and nanowires

Science.gov (United States)

Zhao, Tian; Fan, Jun-Bing; Cui, Jing; Liu, Jin-Hua; Xu, Xiao-Bo; Zhu, Ming-Qiang

2011-01-01

Synthesis of well-defined silver nanostructure in terms of size and shape has been strongly motivated by the requirements to their size- and shape-dependent optical properties which achieve their practical applications ranging from biosensing to catalysis and optics. In this Letter, an ultrafast synthetic process for the well-defined Ag nanocubes and nanowires have been developed, which simply involve the microwave-mediated polyol reduction of silver nitrate in ethylene glycol by adding different amount sodium sulfide (Na2S) into the solution. The possible growth and evolution process of the Ag nanocubes and nanowires involves the microwave ultrafast nucleation and growth followed by oxidative etching of Ag nanocrystals.

Real-Time Observation of Ultrafast Intraband Relaxation and Exciton Multiplication in PbS Quantum Dots

KAUST Repository

El-Ballouli, Ala’a O.

2014-03-19

We examine ultrafast intraconduction band relaxation and multiple-exciton generation (MEG) in PbS quantum dots (QDs) using transient absorption spectroscopy with 120 fs temporal resolution. The intraconduction band relaxation can be directly and excellently resolved spectrally and temporally by applying broadband pump-probe spectroscopy to excite and detect the wavelengths around the exciton absorption peak, which is located in the near-infrared region. The time-resolved data unambiguously demonstrate that the intraband relaxation time progressively increases as the pump-photon energy increases. Moreover, the relaxation time becomes much shorter as the size of the QDs decreases, indicating the crucial role of spatial confinement in the intraband relaxation process. Additionally, our results reveal the systematic scaling of the intraband relaxation time with both excess energy above the effective energy band gap and QD size. We also assess MEG in different sizes of the QDs. Under the condition of high-energy photon excitation, which is well above the MEG energy threshold, ultrafast bleach recovery due to the nonradiative Auger recombination of the multiple electron-hole pairs provides conclusive experimental evidence for the presence of MEG. For instance, we achieved quantum efficiencies of 159, 129 and 106% per single-absorbed photon at pump photoexcition of three times the band gap for QDs with band gaps of 880 nm (1.41 eV), 1000 nm (1.24 eV) and 1210 nm (1.0 eV), respectively. These findings demonstrate clearly that the efficiency of transferring excess photon energy to carrier multiplication is significantly increased in smaller QDs compared with larger ones. Finally, we discuss the Auger recombination dynamics of the multiple electron-hole pairs as a function of QD size.

MoS{sub 2}-modified ZnO quantum dots nanocomposite: Synthesis and ultrafast humidity response

Energy Technology Data Exchange (ETDEWEB)

Ze, Lu [School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105 (China); Yueqiu, Gong, E-mail: yqgong@xtu.edu.cn [School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105 (China); Xujun, Li; Yong, Zhang [School of Physics and Optoelectronics, Xiangtan University, Xiangtan 411105 (China)

2017-03-31

Highlights: • MoS{sub 2}@ZnO QDs composite structure was synthesized by two-steps methods. • Ultrafast humidity sensing response is achieved by MoS{sub 2}@ZnO QDs humidity sensor. • Sensor performs excellent cycle stability from 11% to 95% RH. • Humidity sensor could detect wide humidity range (11–95%). - Abstract: In this work, ZnO quantum dots (QDs), layered MoS{sub 2} and MoS{sub 2}-modified ZnO QDs (MoS{sub 2}@ZnO QDs) nanocomposite were synthesized and then applied as humidity sensor. The crystal structure, morphology and element distribution of ZnO QDs, MoS{sub 2} and MoS{sub 2}@ZnO QDs were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and energy dispersive X-ray spectrometry, respectively. The humidity sensing characteristics of the MoS{sub 2} and MoS{sub 2}@ZnO QDs against various relative humidity were measured at room temperature. The results show that the MoS{sub 2}@ZnO QDs sensor exhibits high sensitivity with an impedance variation of three or four orders of magnitude to relative humidity range of 11–95% and it exhibits a short response-recovery time (1 s for adsorption and 20 s for desorption) and excellent repeatability. The mechanisms of the excellent performance for humidity sensing of MoS{sub 2}@ZnO QDs sensor were discussed based on its impedance properties. Our work could offer guidelines to design higher performance especially ultrafast humidity response sensor utilizing the nanocomposite structure with two dimensional material and QDs.