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Sample records for waveguides ultrafast dynamics

  1. Quantum dot waveguides: ultrafast dynamics and applications

    DEFF Research Database (Denmark)

    Chen, Yaohui; Mørk, Jesper

    2009-01-01

    In this paper we analyze, based on numerical simulations, the dynamics of semiconductor devices incorporating quantum dots (QDs). In particular we emphasize the unique ultrafast carrier dynamics occurring between discrete QD bound states, and its influence on QD semiconductor optical amplifiers...... (SOAs). Also the possibility of realizing an all-optical regenerator by incorporating a QD absorber section in an amplifier structure is discussed....

  2. Microwave signal processing based on ultrafast dynamics in quantum dot waveguides

    DEFF Research Database (Denmark)

    Chen, Yaohui; Mørk, Jesper

    2010-01-01

    In this paper we review theoretical work on slow and fast light effects in quantum dot (QD) semiconductor waveguides and the potential applications in microwave photonics. In particular we emphasize the unique ultrafast carrier dynamics occurring between discrete QD bound states and its influence...... on the dynamic gain grating and cross gain modulation in QD semiconductor optical amplifiers (SOAs). The exploitation of ultrafast carrier dynmaics enables the realization of phase shifters at frequencies in the range of 100 GHz....

  3. Enhancing slow and fast light effects in quantum dot semiconductor waveguides through ultrafast dynamics

    DEFF Research Database (Denmark)

    Chen, Yaohui; Mørk, Jesper

    2010-01-01

    We show that ultrafast carrier dynamics plays an important role on slow and fast light effects based on coherent population oscillations in quantum dot semiconductor waveguides. Fast light in the gain regime and slow light in the absorption regime are found to be enhanced at frequencies beyond th...... the usual limits of the carrier lifetime. The effects are investigated by a comprehensive model and shown to originate from non-equilibrium dynamics within the quantum dot carrier populations....

  4. Enhancing slow- and fast-light effects in quantum dot semiconductor waveguides through ultrafast dynamics

    DEFF Research Database (Denmark)

    Chen, Yaohui; Mørk, Jesper

    2011-01-01

    In this paper we review our theoretical work on slow and fast light effects in quantum dot semiconductor optical amplifiers (QD SOAs), in particular we investigate the carrier dynamical contributions to the dynamic gain grating and cross gain modulation induced by unique ultrafast inter...... in microwave photonics, especially targeting the millimeter wave range, we propose that quantum dot devices might be used to realize an optically fed microwave phase shifter in the frequency range of 100GHz....

  5. 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....

  6. Ultrafast Laser Fabrication of Bragg Waveguides in GLS Chalcogenide Glass

    Directory of Open Access Journals (Sweden)

    McMillen Ben

    2013-11-01

    Full Text Available We present work on the fabrication of Bragg waveguides in gallium-lanthanum-sulfide chalcogenide glass using an ultrafast laser. Waveguides were written with a single pass while modulating the writing beam. The spatial and temporal profile of the writing beam was ontrolled during waveguide fabrication in order to control the shape and size of the waveguide cross-section.

  7. Ultrafast laser fabrication of Bragg waveguides in chalcogenide glass.

    Science.gov (United States)

    McMillen, Ben; Li, Mingshan; Huang, Sheng; Zhang, Botao; Chen, Kevin P

    2014-06-15

    Bragg waveguides are fundamental components in photonic integrated circuits and are particularly interesting for mid-IR applications in high index, highly nonlinear materials. In this work, we present Bragg waveguides fabricated in bulk chalcogenide glass using an ultrafast laser. Waveguides with near circularly symmetric cross sections and low propagation loss are obtained through spatial and temporal beam shaping. Using a single-pass technique, the waveguide and Bragg structure are formed at the same time. First through sixth order gratings with strengths of up to 25 dB are realized, and performance is evaluated based on the modulation duty cycle of the writing beam.

  8. Ultrafast magnetization dynamics

    OpenAIRE

    Woodford, S.

    2008-01-01

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

  9. Ultrafast Magnetization Dynamics

    OpenAIRE

    Woodford, S.

    2008-01-01

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

  10. Inscription of 3D waveguides in diamond using an ultrafast laser

    CERN Document Server

    Courvoisier, Arnaud; Salter, Patrick S

    2016-01-01

    Three dimensional waveguides within the bulk of diamond are manufactured using ultrafast laser fabrication. High intensities within the focal volume of the laser cause breakdown of the diamond into a graphitic phase leading to a stress induced refractive index change in neighboring regions. Type II waveguiding is thus enabled between two adjacent graphitic tracks, but supporting just a single polarization state. We show that adaptive aberration correction during the laser processing allows the controlled fabrication of more complex structures beneath the surface of the diamond which can be used for 3D waveguide splitters and Type III waveguides which support both polarizations.

  11. Inscription of 3D waveguides in diamond using an ultrafast laser

    Science.gov (United States)

    Courvoisier, Arnaud; Booth, Martin J.; Salter, Patrick S.

    2016-07-01

    Three dimensional waveguides within the bulk of diamond are manufactured using ultrafast laser fabrication. High intensities within the focal volume of the laser cause breakdown of the diamond into a graphitic phase leading to a stress induced refractive index change in neighboring regions. Type II waveguiding is thus enabled between two adjacent graphitic tracks, but supporting just a single polarization state. We show that adaptive aberration correction during the laser processing allows the controlled fabrication of more complex structures beneath the surface of the diamond which can be used for 3D waveguide splitters and Type III waveguides which support both polarizations.

  12. Ultrafast surface plasmon-polariton interference and switching in multiple crossing dielectric waveguides

    Science.gov (United States)

    Birr, Tobias; Zywietz, Urs; Fischer, Tim; Chhantyal, Parva; Evlyukhin, Andrey B.; Chichkov, Boris N.; Reinhardt, Carsten

    2016-06-01

    In this paper, we investigate propagation effects and interference switching of surface plasmon-polaritons (SPPs) in a junction of multiple crossed waveguides. These waveguides are produced on a thin gold layer by a simple photolithographic procedure. The waveguide dimensions are optimized for SPP excitation and propagation along two crossed input waveguides. At the waveguide intersection, different possibilities for SPP propagation into multiple output waveguides are offered. Using leakage radiation microscopy, we find that the SPPs preferably propagate into only one specific direction different from the direction of the input waveguides with avoidance of signal backscattering into the input direction. Furthermore, it is demonstrated that the SPP intensity at the output waveguide can be tuned by interference effects induced by a phase shift of the excitation laser beams. Additionally, we study the influence of different angles between the two input and the one specific output waveguides of the junction structure on the propagation properties of SPP modes in order to demonstrate a highest possible energy flux into the output waveguide. The experimental investigations are supported by finite-difference time-domain simulations. Good agreement between experimental results and numerical simulations is obtained. Applications of this effect are discussed for realization of ultrafast optical/plasmonic switches and optical logic gate structures with potential for integration and cascading.

  13. 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

  14. Ultrafast laser fabrication of low-loss waveguides in chalcogenide glass with 0.65 dB/cm loss.

    Science.gov (United States)

    McMillen, Ben; Zhang, Botao; Chen, Kevin P; Benayas, Antonio; Jaque, Daniel

    2012-05-01

    This Letter reports on the fabrication of low-loss waveguides in gallium-lanthanum-sulfide chalcogenide glasses using an ultrafast laser. Spatial beam shaping and temporal pulse width tuning were used to optimize the guided mode profiles and optical loss of laser-written waveguides. Highly symmetric single-mode waveguides guiding at 1560 nm with a loss of 0.65  dB/cm were fabricated using 1.5 ps laser pulses. This Letter suggests a pathway to produce high quality optical waveguides in substrates with strong nonlinearity using the ultrafast laser direct writing technique.

  15. Ultra-fast pulse propagation in nonlinear graphene/silicon ridge waveguide.

    Science.gov (United States)

    Liu, Ken; Zhang, Jian Fa; Xu, Wei; Zhu, Zhi Hong; Guo, Chu Cai; Li, Xiu Jian; Qin, Shi Qiao

    2015-11-18

    We report the femtosecond laser propagation in a hybrid graphene/silicon ridge waveguide with demonstration of the ultra-large Kerr coefficient of graphene. We also fabricated a slot-like graphene/silicon ridge waveguide which can enhance its effective Kerr coefficient 1.5 times compared with the graphene/silicon ridge waveguide. Both transverse-electric-like (TE-like) mode and transverse-magnetic-like (TM-like) mode are experimentally measured and numerically analyzed. The results show nonlinearity dependence on mode polarization not in graphene/silicon ridge waveguide but in slot-like graphene/silicon ridge waveguide. Great spectral broadening was observed due to self-phase modulation (SPM) after propagation in the hybrid waveguide with length of 2 mm. Power dependence property of the slot-like hybrid waveguide is also measured and numerically analyzed. The results also confirm the effective Kerr coefficient estimation of the hybrid structures. Spectral blue shift of the output pulse was observed in the slot-like graphene/silicon ridge waveguide. One possible explanation is that the blue shift was caused by the ultra-fast free carrier effect with the optical absorption of the doped graphene. This interesting effect can be used for soliton compression in femtosecond region. We also discussed the broadband anomalous dispersion of the Kerr coefficient of graphene.

  16. Heat accumulation during high repetition rate ultrafast laser interaction: Waveguide writing in borosilicate glass

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Haibin; Eaton, Shane M; Li, Jianzhao; Herman, Peter R [The Edward S. Rogers Sr. Department of Electrical and Computer Engineering, University of Toronto, 10 King' s College Road, Toronto, ON, M5S 3G4 (Canada)

    2007-04-15

    During high repetition rate (>200 kHz) ultrafast laser waveguide writing, visible heat modified zones surrounding the formed waveguide occur as a result of heat accumulation. The radii of the heat-modified zones increase with the laser net fluence, and were found to correlate with the formation of low-loss and cylindrically symmetric optical waveguides. A numerical thermal model based on the finite difference method is applied here to account for cumulative heating and diffusion effects. The model successfully shows that heat propagation and accumulation accurately predict the radius of the 'heat modified' zones observed in borosilicate glass waveguides formed across a wide range of laser exposure conditions. Such modelling promises better control of thermal effects for optimizing the fabrication and performance of three-dimensional optical devices in transparent materials.

  17. Dynamic optics for ultrafast laser processing

    Directory of Open Access Journals (Sweden)

    Salter Patrick

    2013-11-01

    Full Text Available We present a range of dynamic optical methods to control focal fields for material processing using ultrafast lasers. Adaptive aberration correction maintains focal quality when focusing deep into materials. Dynamic parallelisation methods permit independent control of hundreds of fabrication spots. New adaptive methods for control of pulse front tilt are also presented.

  18. Ultrafast structural dynamics of perovskite superlattices

    Energy Technology Data Exchange (ETDEWEB)

    Woerner, M.; Korff Schmising, C. von; Zhavoronkov, N.; Elsaesser, T. [Max-Born-Institut fuer Nichtlineare Optik und Kurzzeitspektroskopie, Berlin (Germany); Bargheer, M. [Universitaet Potsdam, Institut fuer Physik und Astronomie, Potsdam (Germany); Vrejoiu, I.; Hesse, D.; Alexe, M. [Max-Planck-Institut fuer Mikrostrukturphysik, Halle (Germany)

    2009-07-15

    Femtosecond X-ray diffraction provides direct insight into the ultrafast reversible lattice dynamics of materials with a perovskite structure. Superlattice (SL) structures consisting of a sequence of nanometer-thick layer pairs allow for optically inducing a tailored stress profile that drives the lattice motions and for limiting the influence of strain propagation on the observed dynamics. We demonstrate this concept in a series of diffraction experiments with femtosecond time resolution, giving detailed information on the ultrafast lattice dynamics of ferroelectric and ferromagnetic superlattices. Anharmonically coupled lattice motions in a SrRuO{sub 3}/PbZr{sub 0.2}Ti{sub 0.8}O{sub 3} (SRO/PZT) SL lead to a switch-off of the electric polarizations on a time scale of the order of 1 ps. Ultrafast magnetostriction of photoexcited SRO layers is demonstrated in a SRO/SrTiO{sub 3} (STO) SL. (orig.)

  19. Propagation of Ultra-fast Femtosecond Pulses in Silicon-on-insulator Optical Waveguides

    Institute of Scientific and Technical Information of China (English)

    WU Jian-wei; LUO Feng-guang; Cristiano de Mello Gallep

    2007-01-01

    A complete theoretical modeling, avoiding any priori-assumption, is deduced and demonstrated for ultra-fast femtosecond optical pulses in silicon-on-insulator optical waveguides which includes the group velocity dispersion, third-order dispersion, self-phase and cross-phase modulations, self-steepening and shock formation, Raman depletion, propagation loss, two-photon absorption, free-carrier absorption, and free-carrier dispersion. Finally, the temporal and spectral characteristics of 100 fs optical pulses at 1.55 μm are numerically observed in 5-mm-long waveguides while considering different initial chirps and incident peak intensity levels.

  20. Ultrafast Dynamics of Energetic Materials

    Science.gov (United States)

    2014-01-23

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

  1. Refractive index and dispersion control of ultrafast laser inscribed waveguides in gallium lanthanum sulphide for near and mid-infrared applications

    DEFF Research Database (Denmark)

    Demetriou, Giorgos; Berube, Jean-Philippe; Vallee, Real

    2016-01-01

    The powerful ultrafast laser inscription technique is used to fabricate optical waveguides in gallium lanthanum sulphide substrates. For the first time the refractive index profile and the dispersion of such ultrafast laser inscribed waveguides are experimentally measured. In addition the Zero Di...... in gallium lanthanum sulphide glasses for near and mid-IR applications. (C) 2016 Optical Society of America...

  2. EO-polymer waveguide based high dynamic range EM wave sensors

    CERN Document Server

    Lin, Che-Yun; Zhang, Xingyu; Lee, Beom Suk; Chen, Ray T

    2014-01-01

    In this paper, we present the design and experimental demonstration of a high dynamic range electric field sensor based on electro-optic (EO) polymer directional coupler waveguides that offers the strong and ultra-fast EO response of EO polymer. As compared to conventional photonic electric field sensors, our directional coupler waveguide design offers several advantages such as bias-free operation, highly linear measurement response up to 70dB, and a wide electric field detection range from 16.7V/m to 750kV/m at a frequency of 1GHz.

  3. Ultrafast Laser Pulses for Structuring Materials at Micro/Nano Scale: From Waveguides to Superhydrophobic Surfaces

    Directory of Open Access Journals (Sweden)

    Daniel S. Correa

    2017-01-01

    Full Text Available The current demand for fabricating optical and photonic devices displaying high performance, using low-cost and time-saving methods, prompts femtosecond (fs-laser processing as a promising methodology. High and low repetition femtosecond lasers enable surface and/or bulk modification of distinct materials, which can be used for applications ranging from optical waveguides to superhydrophobic surfaces. Herein, some fundamental aspects of fs-laser processing of materials, as well as the basics of their most common experimental apparatuses, are introduced. A survey of results on polymer fs-laser processing, resulting in 3D waveguides, electroluminescent structures and active hybrid-microstructures for luminescence or biological microenvironments is presented. Similarly, results of fs-laser processing on glasses, gold and silicon to produce waveguides containing metallic nanoparticles, analytical chemical sensors and surface with modified features, respectively, are also described. The complexity of fs-laser micromachining involves precise control of material properties, pushing ultrafast laser processing as an advanced technique for micro/nano devices.

  4. Ultrafast dynamics in InAs quantum dot and GaInNAs quantum well semiconductor heterostructures

    OpenAIRE

    Malins, David B

    2007-01-01

    The quantum confined Stark effect (QCSE) and ultrafast absorption dynamics near the bandedge have been investigated in p-i-n waveguides comprising quantum confined heterostructures grown on GaAs substrates, for emission at 1.3um. The materials are; isolated InAs/InGaAs dot-in-a-well (DWELL) quantum dots (QD), bilayer InAs quantum dots and GaInNAs multiple quantum wells (MQW). The focus was to investigate these dynamics in a planar waveguide geometry, for the purpose of large scale integ...

  5. Ultrafast carriers dynamics in filled-skutterudites

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-06-08

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

  6. Ultrafast carriers dynamics in filled-skutterudites

    Science.gov (United States)

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

    2015-06-01

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

  7. Ultrafast pulse generation in a mode-locked Erbium chip waveguide laser

    CERN Document Server

    Khurmi, Champak; Zhang, Wen Qi; V., Shahraam Afshar; Chen, George; Genest, Jérôme; Monro, Tanya M; Lancaster, David G

    2016-01-01

    We report mode-locked ~1550 nm output of transform-limited ~180 fs pulses from a large mode-area (diameter ~ 50 {\\mu}m) guided-wave erbium fluorozirconate glass laser. The passively mode-locked oscillator generates pulses with 25 nm bandwidth at 156 MHz repetition rate and peak-power of 260 W. Scalability to higher repetition rate is demonstrated by transform-limited 410 fs pulse output at 1.3 GHz. To understand the origins of the broad spectral output, the laser cavity is simulated by using a numerical solution to the Ginzburg-Landau equation. This paper reports the widest bandwidth and shortest pulses achieved from an ultra-fast laser inscribed waveguide laser.

  8. Ultrafast Laser Inscription of a 121-Waveguide Fan-Out for Astrophotonics

    CERN Document Server

    Thomson, R R; Birks, T A; Brown, G; Allington-Smith, J; Bland-Hawthorn, J

    2012-01-01

    Using ultrafast laser inscription, we report the fabrication of a prototype three-dimensional 121-waveguide fan-out device capable of reformatting the output of a 120 core multicore fiber (MCF) into a one-dimensional linear array. When used in conjunction with an actual MCF, we demonstrate that the reformatting function using this prototype would result in an overall throughput loss of approximately 7.0 dB. However, if perfect coupling from the MCF into the fan-out could be achieved, the reformatting function would result in an overall loss of only approximately 1.7 dB. With adequate development, similar devices could efficiently reformat the output of so-called "photonic lanterns" fabricated using highly multicore fibers.

  9. Ultrafast, low-power, all-optical switching via birefringent phase-matched transverse mode conversion in integrated waveguides

    CERN Document Server

    Hellwig, Tim; Schnack, Martin; Boller, Klaus -J; Fallnich, Carsten

    2015-01-01

    We demonstrate the potential of birefringence-based, all-optical, ultrafast conversion between the transverse modes in integrated optical waveguides by modelling the conversion process by numerically solving the multi-mode coupled nonlinear Schroedinger equations. The observed conversion is induced by a control beam and due to the Kerr effect, resulting in a transient index grating which coherently scatters probe light from one transverse waveguide mode into another. We introduce birefringent phase matching to enable efficient all-optically induced mode conversion at different wavelengths of the control and probe beam. It is shown that tailoring the waveguide geometry can be exploited to explicitly minimize intermodal group delay as well as to maximize the nonlinear coefficient, under the constraint of a phase matching condition. The waveguide geometries investigated here, allow for mode conversion with over two orders of magnitude reduced control pulse energy compared to previous schemes and thereby promise ...

  10. Ultrafast dynamic ellipsometry and spectroscopies of laser shocked materials

    Energy Technology Data Exchange (ETDEWEB)

    Mcgrane, Shawn David [Los Alamos National Laboratory; Bolme, Cindy B [Los Alamos National Laboratory; Whitley, Von H [Los Alamos National Laboratory; Moore, David S [Los Alamos National Laboratory

    2010-01-01

    Ultrafast ellipsometry and transient absorption spectroscopies are used to measure material dynamics under extreme conditions of temperature, pressure, and volumetric compression induced by shock wave loading with a chirped, spectrally clipped shock drive pulse.

  11. Ultrafast laser writing of optical waveguides in ceramic Yb:YAG: a study of thermal and non-thermal regimes

    Energy Technology Data Exchange (ETDEWEB)

    Benayas, A.; Jaque, D. [Universidad Autonoma de Madrid, Departamento de Fisica de Materiales, Madrid (Spain); Silva, W.F.; Jacinto, C. [Universidade Federal de Alagoas, Grupo de Fotonica e Fluidos Complexos, Instituto de Fisica, Maceio, Alagoas (Brazil); Rodenas, A.; Thomsom, R.R.; Psaila, N.D.; Reid, D.T.; Kar, A.K. [Heriot-Watt University, School of Engineering and Physical Sciences, Edinburgh (United Kingdom); Vazquez de Aldana, J. [Universidad de Salamanca, Grupo de Optica, Departamento de Fisica Aplicada, Facultad de Ciencias Fisicas, Salamanca (Spain); Chen, F.; Tan, Y. [Shandong University, School of Physics, Jinan (China); Torchia, G.A. [CONICET-CIC, Centro de Investigaciones Opticas, La Plata (Argentina)

    2011-07-15

    We report the improvement of ultrafast laser written optical waveguides in Yb:YAG ceramics by tailoring the presence of heat accumulation effects. From a combination of ytterbium micro-luminescence and micro-Raman structural analysis, maps of lattice defects and stress fields have been obtained. We show how laser annealing can strongly reduce the concentration of defects and also reduce compressive stress, leading to an effective 50% reduction in the propagation losses and to more extended and symmetric propagation modes. (orig.)

  12. 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.

  13. Ultrafast electron dynamics in gold nanoshells

    Science.gov (United States)

    Westcott, Sarah Linda

    2001-10-01

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

  14. Atom laser dynamics in a tight waveguide

    Energy Technology Data Exchange (ETDEWEB)

    Campo, A del; Lizuain, I; Muga, J G [Departamento de Quimica-Fisica, UPV-EHU, Apartado. 644, Bilbao (Spain); Pons, M [Departamento de Fisica Aplicada I, E.U.I.T. de Minas y Obras Publicas, UPV-EHU, 48901 Barakaldo (Spain); Moshinsky, M [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, Apartado Postal 20-364, 01000 Mexico D.F. (Mexico)], E-mail: adolfo.delcampo@ehu.es

    2008-02-15

    We study the transient dynamics that arise during the formation of an atom laser beam in a tight waveguide. The time dependent density profile develops a series of wiggles which are related to the diffraction in time phenomenon. The apodization of matter waves, which relies on the use of smooth aperture functions, allows to suppress such oscillations in a time interval, after which there is a revival of the diffraction in time. The revival time scale is directly related to the inverse of the harmonic trap frequency for the atom reservoir.

  15. Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses

    Science.gov (United States)

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

    2014-10-01

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

  16. 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

  17. Ultrafast impact dynamics of reactive materials (Dlott)

    Science.gov (United States)

    2013-04-16

    Submitted Patents Awarded Awards Jupiter Laser Facility Program Advisory Committee, Lawrence Livermore National Laboratory, 2008, 2011 Executive...related materials such as B/Teflon) to ultrafast laser flash heating. 36-39 In fact during the project period we wrapped up the flash-heating

  18. Ultrafast Magnetism Dynamics Measure Using Tabletop Ultrafast EUV Sources

    Energy Technology Data Exchange (ETDEWEB)

    Silva, Thomas J. [NIST; Murnane, Margaret [University of Colorado

    2013-08-21

    In our work to date, we made two significant advances. First we demonstrated element-selective demagnetization dynamics for the first time, with a record time resolution for x-ray probing of 55 fs. Second, in new work, we were able to probe the timescale of the exchange interaction in magnetic materials, also for the first time. Our measurements were made using the transverse magneto-optic Kerr effect (T-MOKE) geometry, since the reflectivity of a magnetic material changes with the direction of the magnetization vector of a surface. In our experiment, we periodically reversed the magnetization direction of a grating structure made of Permalloy (Ni80Fe20) using an external magnetic field. To achieve maximum contrast, we used HHG light spanning the M-shell (3p) absorption edges of Fe and Ni. Our characterization of the static magnetization of a Permalloy sample shows high magnetic asymmetry at photon energies just above and below the absorption edges at 55 eV and 65 eV, respectively. This result is in excellent agreement with measurements done on the same using a synchrotron source.

  19. Ultrafast, low-power, all-optical switching via birefringent phase-matched transverse mode conversion in integrated waveguides.

    Science.gov (United States)

    Hellwig, Tim; Epping, Jörn P; Schnack, Martin; Boller, Klaus-J; Fallnich, Carsten

    2015-07-27

    We demonstrate the potential of birefringence-based, all-optical, ultrafast conversion between the transverse modes in integrated optical waveguides by modelling the conversion process by numerically solving the multi-mode coupled nonlinear Schroedinger equations. The observed conversion is induced by a control beam and due to the Kerr effect, resulting in a transient index grating which coherently scatters probe light from one transverse waveguide mode into another. We introduce birefringent phase matching to enable efficient all-optically induced mode conversion at different wavelengths of the control and probe beam. It is shown that tailoring the waveguide geometry can be exploited to explicitly minimize intermodal group delay as well as to maximize the nonlinear coefficient, under the constraint of a phase matching condition. The waveguide geometries investigated here, allow for mode conversion with over two orders of magnitude reduced control pulse energy compared to previous schemes and thereby promise nonlinear mode switching exceeding efficiencies of 90% at switching energies below 1 nJ.

  20. Investigations of ultrafast dynamics in electronically excited alkylbenzenes

    Directory of Open Access Journals (Sweden)

    Maksyutenko P.

    2013-03-01

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

  1. Ultrafast gain and index dynamics in quantum dot amplifiers

    DEFF Research Database (Denmark)

    Borri, Paola; Langbein, Wolfgang; Mørk, Jesper

    1999-01-01

    The ultrafast dynamics of gain and refractive index in an InAs/GaAs quantum dot amplifier are investigated at room temperature. The gain is observed to recover with a 90 fs time constant, ruling out problems of slow carrier capture into the dots, and making this component promising for high...

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

    Directory of Open Access Journals (Sweden)

    Novoselov K.S.

    2013-03-01

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

  3. Structural preablation dynamics of graphite observed by ultrafast electron crystallography

    NARCIS (Netherlands)

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

    2008-01-01

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

  4. Ultrafast Dynamics of Quantum-Dot Semiconductor Optical Amplifiers

    DEFF Research Database (Denmark)

    Poel, Mike van der; Hvam, Jørn Märcher

    2007-01-01

    We report on a series of experiments on the dynamical properties of quantum-dot semiconductor optical amplifiers. We show how the amplifier responds to one or several ultrafast (170 fs) pulses in rapid succession and our results demonstrate applicability and ultimate limitations to application...

  5. 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.

  6. Ultrafast spectroscopy of quasiparticle dynamics in cuprate superconductors

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-02-15

    Ultrafast pump-probe spectroscopy is a powerful tool to study the nonequilibrium dynamics in high-Tc cuprate superconductors. The photo-induced quasiparticle (QP) dynamics revealed by pump-probe spectroscopy are sensitive to the near-Fermi level electronic structures. Here we review several selected examples to illustrate the enduring challenges including pairing glue, phase separation, and phase transitions in cuprate superconductors. We also present the data obtained on thin films of YBa{sub 2}Cu{sub 3}O{sub 7−δ} in connection to these issues. - Highlights: • This paper reviews recent ultrafast spectroscopic study on cuprates. • Dynamics related to pairing glues and phase separations are summarized. • Mid-IR pulses enhance the coherent transport in underdoped cuprates. • Pump-probe data on the quasiparticle dynamics in YBCO films are presented.

  7. 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.

  8. Ultrafast Terahertz Dynamics and Switching in Quantum Dots

    DEFF Research Database (Denmark)

    Turchinovich, Dmitry; Hoffmann, Matthias C.

    2012-01-01

    carrier release from the QDs with (sub-)picosecond time resolution, using optical pump–THz probe measurements. In the second part of this chapter we investigate the direct manipulation of the quantum confinement potential of the QDs by an electric field of a strong THz pulse. The resulting THz......-driven quantum-confined Stark effect leads to a strong modulation of a ground-state optical absorption in the QDs. Dynamically, such a THz-induced electro-absorption modulation in QDs (near-)instantaneously follows the absolute value of the electric field of the THz pulse, providing the capability for Tbit......In this Chapter we describe the experimental studies of ultrafast carrier dynamics and all-optical switching in semiconductor quantum dots (QDs) using ultrafast terahertz (THz) techniques. In the first part of this chapter we describe the studies of carrier capture into the QDs, and thermionic...

  9. Ultrafast dynamics and laser action of organic semiconductors

    CERN Document Server

    Vardeny, Zeev Valy

    2009-01-01

    Spurred on by extensive research in recent years, organic semiconductors are now used in an array of areas, such as organic light emitting diodes (OLEDs), photovoltaics, and other optoelectronics. In all of these novel applications, the photoexcitations in organic semiconductors play a vital role. Exploring the early stages of photoexcitations that follow photon absorption, Ultrafast Dynamics and Laser Action of Organic Semiconductors presents the latest research investigations on photoexcitation ultrafast dynamics and laser action in pi-conjugated polymer films, solutions, and microcavities.In the first few chapters, the book examines the interplay of charge (polarons) and neutral (excitons) photoexcitations in pi-conjugated polymers, oligomers, and molecular crystals in the time domain of 100 fs-2 ns. Summarizing the state of the art in lasing, the final chapters introduce the phenomenon of laser action in organics and cover the latest optoelectronic applications that use lasing based on a variety of caviti...

  10. Ultrafast element-specific decoupling of magnetization dynamics in permalloy

    Energy Technology Data Exchange (ETDEWEB)

    Grychtol, Patrik [Department of Physics, JILA, University of Colorado, Boulder, Colorado 80309-0440 (United States); Institute of Solid State Research, IFF-9, Research Center Juelich, 52425, Juelich (Germany); La-O-Vorakiat, Chan; Siemens, Mark; Kapteyn, Henry; Murnane, Margaret [Department of Physics, JILA, University of Colorado, Boulder, Colorado 80309-0440 (United States); Mathias, Stefan [Department of Physics, JILA, University of Colorado, Boulder, Colorado 80309-0440 (United States); University of Kaiserslautern, Research Center OPTIMAS, 67663, Kaiserslautern (Germany); Shaw, Justin; Nembach, Hans; Silva, Tom [Electromagnetics Division, National Institute of Standards and Technology, Boulder, Colorado 80305-3328 (United States); Adam, Roman; Schneider, Claus M. [Institute of Solid State Research, IFF-9, Research Center Juelich, 52425, Juelich (Germany); Eich, Steffen; Aeschlimann, Martin [University of Kaiserslautern, Research Center OPTIMAS, 67663, Kaiserslautern (Germany)

    2011-07-01

    Elucidating the dynamic behavior of complex magnetic systems far from their thermal equilibrium is a topic of utmost scientific interest. In our work, we employ soft x-ray pulses from high-harmonic-generation to probe the dynamic response of thin permalloy films during an ultrafast optically driven demagnetization process. We find that the demagnetization times for the elements Fe and Ni differ significantly, despite their strong exchange coupling in the thermodynamic equilibrium. We ascribe this difference to a breakdown of exchange interaction on the femtosecond timescale, a process that we further enhance by alloying permalloy with Cu. Our data shows that, in general, a site-specific spin environment must be considered to correctly describe ultrafast magnetization processes in compounds.

  11. Ultrafast nonlinear all-optical processes in silicon-on-insulator waveguides

    NARCIS (Netherlands)

    Dekker, R.; Usechak, N.; Först, M.; Driessen, A.

    2007-01-01

    In this review we present an overview of the progress made in recent years in the field of integrated silicon-on-insulator (SOI) waveguide photonics with a strong emphasis on third-order nonlinear optical processes. Although the focus is on simple waveguide structures the utilization of complex stru

  12. Origin of ultrafast excited state dynamics of 1-nitropyrene.

    Science.gov (United States)

    Murudkar, Sushant; Mora, Aruna K; Singh, Prabhat K; Nath, Sukhendu

    2011-10-01

    Time-resolved emission measurements in subpicosecond time domain have been carried out for 1-nitropyrene in different solvents to understand the mechanism for the observed ultrafast decay of its first excited singlet state. Excited-state dynamics of 1-nitropyrene is found to be independent of the solvent viscosity. This result contradicts the proposition in the literature (J. Phys. Chem. A 2007, 111, 552) that the ultrafast decay in 1-nitropyrene is due to the large amplitude torsional motion of the nitro group around the pyrene moiety. Excited-state dynamics of 1-nitropyrene in solvents with different dielectric constants shows that excited-state lifetime suddenly increases after a certain value of the dielectric constant. Detailed quantum chemical calculations have been carried out to understand the process that is responsible for the observed effect of the dielectric constant on the excited-state dynamics of 1-nitropyrene. It is seen that the excited-state lifetime and the singlet-triplet energy gap follow similar variation with the dielectric constant of the medium. Such a correlation between the excited-state lifetime and the singlet-triplet energy gap supports the fact that the observed ultrafast decay for 1-nitropyrene is due to an efficient intersystem crossing rather than to the torsional motion of the nitro group as proposed in the literature.

  13. Ultrafast, green third-harmonic generation and strong-field phenomena in silicon-on-insulator nanoplasmonic waveguides

    CERN Document Server

    Sederberg, Shawn

    2013-01-01

    The emergence of strong-field nanoplasmonics brings extreme laser field-matter interaction into the realm of nanoscale science, unveiling exciting new physics. Highly nonlinear interaction is enabled by tightly confined electric fields in nanoplasmonic structures, permitting use of optical fields from low-power laser oscillators. Here, we report the first demonstration of visible 517nm third harmonic generation in ultracompact nanoplasmonic waveguides on a silicon-on-insulator platform at an unprecedented conversion efficiency of ~10^{-5}. Exponential growth of broadband white light generation confirms a new strong-field phenomenon of ponderomotive force-driven electron avalanche multiplication. Using time-resolved experiments, we show that the strong nanoplasmonic field confinement allows nonlinear interaction to occur on an ultrafast timescale of 1.98 +/- 0.40 ps, despite the long free-carrier lifetime in silicon. These findings uncover a new strong-field interaction that can be used in sensitive nanoplasmo...

  14. Ultrafast dynamic response of single crystal β-HMX

    Science.gov (United States)

    Zaug, Joseph M.; Armstrong, Michael R.; Crowhurst, Jonathan C.; Radousky, Harry B.; Ferranti, Louis; Swan, Raymond; Gross, Rick; Teslich, Nick E.; Wall, Mark A.; Austin, Ryan A.; Fried, Laurence E.

    2017-01-01

    We report results from ultrafast compression experiments conducted on β-HMX single crystals. Results consist of nominally 12 picosecond time-resolved wave profile data, (ultrafast time domain interferometry -TDI measurements), that were analyzed to determine high-velocity wave speeds as a function of piston velocity. TDI results are used to validate calculations of anisotropic stress-strain behavior of shocked loaded energetic materials. Our previous results derived using a 350 ps duration compression drive revealed anisotropic elastic wave response in single crystal β-HMX from (110) and (010) impact planes. Here we present results using a 1.05 ns duration compression drive with a 950 ps interferometry window to extend knowledge of the anisotropic dynamic response of β-HMX within eight microns of the initial impact plane. We observe two distinct wave profiles from (010) and three wave profiles from (010) impact planes. The (110) impact plane wave speeds typically exceed (010) impact plane wave speeds at the same piston velocities. The development of multiple hydrodynamic wave profiles begins at 20 GPa for the (110) impact plane and 28 GPa for the (10) impact plane. We compare our ultrafast TDI results with previous gun and plate impact results on β-HMX and PBX9501.

  15. Film morphology and ultrafast photoexcitation dynamics in polyfluorene

    Science.gov (United States)

    Korovyanko, O. J.; Vardeny, Z. V.

    2002-04-01

    We study the effect of sample morphology on ultrafast dynamics of photoexcited species in poly(9,9-dioctyl)fluorene (PFO). We show that within 200 fs both excitons and geminate polaron pairs with distinctly different absorption bands in the visible-near infrared spectral range are photogenerated in PFO solutions, pristine films, thermal and vapor treated films. However the branching ratio between the excitons and polaron pairs, as well as the polaron pair recombination kinetics depends on film morphology; polaron pair generation is enhanced and their recombination kinetics is faster in a solid phase, called the β phase, where the polymer chains are more planar.

  16. Ultrafast magnetization dynamics in diluted magnetic semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Morandi, O [INRIA Nancy Grand-Est and Institut de Recherche en Mathematiques Avancees, 7 rue Rene Descartes, F-67084 Strasbourg (France); Hervieux, P-A; Manfredi, G [Institut de Physique et Chimie des Materiaux de Strasbourg, 23 rue du Loess, F-67037 Strasbourg (France)], E-mail: morandi@dipmat.univpm.it

    2009-07-15

    We present a dynamical model that successfully explains the observed time evolution of the magnetization in diluted magnetic semiconductor quantum wells after weak laser excitation. Based on the pseudo-fermion formalism and a second-order many-particle expansion of the exact p-d exchange interaction, our approach goes beyond the usual mean-field approximation. It includes both the sub-picosecond demagnetization dynamics and the slower relaxation processes that restore the initial ferromagnetic order in a nanosecond timescale. In agreement with experimental results, our numerical simulations show that, depending on the value of the initial lattice temperature, a subsequent enhancement of the total magnetization may be observed within the timescale of a few hundred picoseconds.

  17. Ultrafast domain wall dynamics in magnetic nanotubes and nanowires

    Science.gov (United States)

    Hertel, R.

    2016-12-01

    The dynamic properties of magnetic domain walls in nanotubes and in cylindrical nanowires can be significantly different from the well known domain wall dynamics in thin films and in flat thin strips. The main differences are the occurrence of chiral symmetry breaking and, perhaps more importantly, the possibility to obtain magnetic domain walls that are stable against the usual Walker breakdown. This stability enables the magnetic field-driven propagation of the domain walls in nanotubes and nanocylinders at constant velocities which are significantly higher than the usual propagation speeds of the domain walls. Simulations predict that the ultrafast motion of magnetic domain walls at velocities in a range above 1000 m s-1 can lead to the spontaneous excitation of spin waves in a process that is the magnetic analog of the Cherenkov effect. In the case of solid cylindrical wires, the domain wall can contain a micromagnetic point singularity. We discuss the current knowledge on the ultrafast dynamics of such Bloch points, which remains still largely unexplored.

  18. Fusion of Renewable Ring Resonator Lasers and Ultrafast Laser Inscribed Photonic Waveguides

    Science.gov (United States)

    Chandrahalim, Hengky; Rand, Stephen C.; Fan, Xudong

    2016-09-01

    We demonstrated the monolithic integration of reusable and wavelength reconfigurable ring resonator lasers and waveguides of arbitrary shapes to out-couple and guide laser emission on the same fused-silica chip. The ring resonator hosts were patterned by a single-mask standard lithography, whereas the waveguides were inscribed in the proximity of the ring resonator by using 3-dimensional femtosecond laser inscription technology. Reusability of the integrated ring resonator – waveguide system was examined by depositing, removing, and re-depositing dye-doped SU-8 solid polymer, SU-8 liquid polymer, and liquid solvent (toluene). The wavelength reconfigurability was validated by employing Rhodamine 6G (R6G) and 3,3‧-Diethyloxacarbocyanine iodide (CY3) as exemplary gain media. In all above cases, the waveguide was able to couple out and guide the laser emission. This work opens a door to reconfigurable active and passive photonic devices for on-chip coherent light sources, optical signal processing, and the investigation of new optical phenomena.

  19. 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.

  20. Cold atom dynamics in crossed laser beam waveguides

    CERN Document Server

    Torrontegui, E; Ruschhaupt, A; Guéry-Odelin, D; Muga, J G

    2010-01-01

    We study the dynamics of neutral cold atoms in an $L$-shaped crossed-beam optical waveguide formed by two perpendicular red-detuned lasers of different intensities and a blue-detuned laser at the corner. Complemented with a vibrational cooling process this setting works as a one-way device or "atom diode".

  1. Ultrafast, broadband, and configurable midinfrared all-optical switching in nonlinear graphene plasmonic waveguides

    Directory of Open Access Journals (Sweden)

    Kelvin J. A. Ooi

    2016-07-01

    Full Text Available Graphene plasmonics provides a unique and excellent platform for nonlinear all-optical switching, owing to its high nonlinear conductivity and tight optical confinement. In this paper, we show that impressive switching performance on graphene plasmonic waveguides could be obtained for both phase and extinction modulations at sub-MW/cm2 optical pump intensities. Additionally, we find that the large surface-induced nonlinearity enhancement that comes from the tight confinement effect can potentially drive the propagating plasmon pump power down to the pW range. The graphene plasmonic waveguides have highly configurable Fermi-levels through electrostatic-gating, allowing for versatility in device design and a broadband optical response. The high capabilities of nonlinear graphene plasmonics would eventually pave the way for the adoption of the graphene plasmonics platform in future all-optical nanocircuitry.

  2. Multi-gigahertz repetition rate ultrafast waveguide lasers mode-locked with graphene saturable absorbers

    Science.gov (United States)

    Obraztsov, P. A.; Okhrimchuk, A. G.; Rybin, M. G.; Obraztsova, E. D.; Garnov, S. V.

    2016-08-01

    We report the development of an approach to build compact waveguide lasers that operate in the stable fundamental mode-locking regime with multigigahertz repetition rates. The approach is based on the use of depressed cladding multi- or single-mode waveguides fabricated directly in the active laser crystal using the femtosecond laser inscription method and a graphene saturable absorber. Using this approach we achieve the stable self-starting mode-locking operation of a diode-pumped waveguide Nd:YAG laser that delivers picosecond pulses at a repetition rate of up to 11.5 GHz with an average power of 12 mW at a central wavelength of 1064 nm. The saturable absorbers are formed through the chemical vapor deposition of single-layer graphene on the output coupler mirror or directly on the end facet of the laser crystal. The stable self-starting mode-locking operation is achieved by controlling the group delay dispersion in the laser cavity with an intracavity interferometer. The method developed for the creation of compact ultrashort pulse laser generators with gigahertz repetition rates can be extended further and applied for the development of compact high-repetition rate lasers that operate at a wide range of IR wavelengths.

  3. Structural, mechanical and optical studies on ultrafast laser inscribed chalcogenide glass waveguide

    Science.gov (United States)

    Ayiriveetil, Arunbabu; Varma, G. Sreevidya; Chaturvedi, Abhishek; Sabapathy, Tamilarasan; Ramamurty, Upadrasta; Asokan, Sundarrajan

    2017-04-01

    Multi-scan waveguides have been inscribed in GeS2 glass sample with different pulse energies and translation speeds. Mechanical and structural changes on GeS2 binary glass in response to irradiation to 1047 nm femto-second laser pulses have been investigated. The optical characterization of these waveguides has been done at 1550 nm of laser wavelength and the material response to laser exposure is characterized by both nanoindentation studies and micro-Raman spectroscopy. Nanoindentation investigations show a decrease in hardness (H) and elastic modulus (E) upon laser irradiation. The change in E and H are found to be varying with the translational speed, pulse energy and hence the net-fluence at the sample. These changes are correlated with variations in the Raman response of photo-exposed glass which is interpreted in terms of structural modifications made by the laser inscriptions to the glassy network. The mechanical behavior and local structural changes on waveguide writing is found to be dependent on net-fluence and it is correlated with the preparation conditions like melt temperature and cooling rate.

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

    Science.gov (United States)

    Yang, Ding-Shyue; He, Xing

    2017-09-01

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

  5. Optical Nonlinearities and Ultrafast Carrier Dynamics in Semiconductor Quantum Dots

    Energy Technology Data Exchange (ETDEWEB)

    Klimov, V.; McBranch, D.; Schwarz, C.

    1998-08-10

    Low-dimensional semiconductors have attracted great interest due to the potential for tailoring their linear and nonlinear optical properties over a wide-range. Semiconductor nanocrystals (NC's) represent a class of quasi-zero-dimensional objects or quantum dots. Due to quantum cordhement and a large surface-to-volume ratio, the linear and nonlinear optical properties, and the carrier dynamics in NC's are significantly different horn those in bulk materials. napping at surface states can lead to a fast depopulation of quantized states, accompanied by charge separation and generation of local fields which significantly modifies the nonlinear optical response in NC's. 3D carrier confinement also has a drastic effect on the energy relaxation dynamics. In strongly confined NC's, the energy-level spacing can greatly exceed typical phonon energies. This has been expected to significantly inhibit phonon-related mechanisms for energy losses, an effect referred to as a phonon bottleneck. It has been suggested recently that the phonon bottleneck in 3D-confined systems can be removed due to enhanced role of Auger-type interactions. In this paper we report femtosecond (fs) studies of ultrafast optical nonlinearities, and energy relaxation and trap ping dynamics in three types of quantum-dot systems: semiconductor NC/glass composites made by high temperature precipitation, ion-implanted NC's, and colloidal NC'S. Comparison of ultrafast data for different samples allows us to separate effects being intrinsic to quantum dots from those related to lattice imperfections and interface properties.

  6. Efficient Raman generation in a waveguide: A route to ultrafast quantum random number generation

    Science.gov (United States)

    England, D. G.; Bustard, P. J.; Moffatt, D. J.; Nunn, J.; Lausten, R.; Sussman, B. J.

    2014-02-01

    The inherent uncertainty in quantum mechanics offers a source of true randomness which can be used to produce unbreakable cryptographic keys. We discuss the development of a high-speed random number generator based on the quantum phase fluctuations in spontaneously initiated stimulated Raman scattering (SISRS). We utilize the tight confinement and long interaction length available in a Potassium Titanyl Phosphate waveguide to generate highly efficient SISRS using nanojoule pulse energies, reducing the high pump power requirements of the previous approaches. We measure the random phase of the Stokes output using a simple interferometric setup to yield quantum random numbers at 145 Mbps.

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

    Science.gov (United States)

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

    2017-02-01

    Ultrafast pump-probe measurements of plasmonic nanostructures probe the nonequilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions that allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly nonthermal excited carriers and longer-lived thermalizing carriers.

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

    CERN Document Server

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

    2016-01-01

    Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions which allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly non-thermal excited carriers and longer-lived thermalizing carriers.

  9. Perspective: Structure and ultrafast dynamics of biomolecular hydration shells

    Directory of Open Access Journals (Sweden)

    Damien Laage

    2017-07-01

    Full Text Available The structure and function of biomolecules can be strongly influenced by their hydration shells. A key challenge is thus to determine the extent to which these shells differ from bulk water, since the structural fluctuations and molecular excitations of hydrating water molecules within these shells can cover a broad range in both space and time. Recent progress in theory, molecular dynamics simulations, and ultrafast vibrational spectroscopy has led to new and detailed insight into the fluctuations of water structure, elementary water motions, and electric fields at hydrated biointerfaces. Here, we discuss some central aspects of these advances, focusing on elementary molecular mechanisms and processes of hydration on a femto- to picosecond time scale, with some special attention given to several issues subject to debate.

  10. Ultrafast Coercivity Dynamics in GaMnAs

    Science.gov (United States)

    Hall, Kimberley; Zahn, Jeremy; March, Samuel; Liu, Xinyu; Furdyna, Jacek

    2008-03-01

    The hole-mediated ferromagnetism in III-Mn-V diluted magnetic semiconductors opens up a whole host of possibilities for future multifunctional devices. Control over the ferromagnetic properties in these materials through hole density modulation has been demonstrated using electrical gates [1] and CW optical excitation [2], and more recently using femtosecond optical excitation [3,4]. Using time-resolved magneto-optical Kerr Effect spectroscopy, we have measured the magnetization and coercivity dynamics in GaMnAs. Our experiments reveal a subpicosecond ferromagnetic to paramagnetic phase transition followed by coercivity enhancement on longer time scales. Our findings are promising for possible applications in ultrafast, nonthermal magneto-optical recording using diluted magnetic semiconductors. [1] H. Ohno et al., Nature 408, 944 (2000). [2] S. Koshihara et al., Phys. Rev. Lett. 78, 4617 (1997). [3] J. Wang et al., Phys. Rev. Lett. 95, 167401 (2005). [4] J. Wang et al., Phys. Rev. Lett. 98, 217401 (2007).

  11. Ultrashort Dynamics in Quantum Dot Waveguides: Theoretical Analysis and Experimental Investigations

    DEFF Research Database (Denmark)

    Gehrig, E.; Poel, Mike van der; Birkedal, Dan;

    2004-01-01

    Experimental pump-probe measurements and computational modeling on the basis of spatially resolved Quantum Dot Maxwell-Bloch equations allow identification of the processes underlying the ultrafast dot dynamics.......Experimental pump-probe measurements and computational modeling on the basis of spatially resolved Quantum Dot Maxwell-Bloch equations allow identification of the processes underlying the ultrafast dot dynamics....

  12. Ultrafast laser inscribed integrated waveguide components for L-band interferometry

    Science.gov (United States)

    Arriola, A.; Mukherjee, S.; Choudhury, Debaditya; Labadie, L.; Thomson, R. R.

    2014-07-01

    In this paper we report the fabrication and mid-infrared characterization (λ = 3.39 μm) of evanescent field directional couplers. These devices were fabricated using the femtosecond laser direct-writing technique in commercially available Gallium Lanthanum Sulphide (GLS) glass substrates. We demonstrate that the power splitting ratios of the devices can be controlled by adjusting the length of the interaction section between the waveguides, and consequently we demonstrate power splitting ratios of between 8% and 99% for 3.39 μm light. We anticipate that mid-IR beam integrated-optic beam combination instruments based on this technology will be key for future mid-infrared astronomical interferometry, particularly for nulling interferometry and earth-like exoplanet imaging.

  13. Enhancing slow and fast light effects in quantum dot optical amplifiers through ultrafast dynamics

    DEFF Research Database (Denmark)

    Chen, Yaohui; Mørk, Jesper

    2009-01-01

    We numerically demonstrate potential roles of ultrafast carrier dynamics in Quantum dot amplifiers to achieve tunable microwave phase shifting at frequencies beyond the limits of carrier lifetime in coherent population oscillations mechanism.......We numerically demonstrate potential roles of ultrafast carrier dynamics in Quantum dot amplifiers to achieve tunable microwave phase shifting at frequencies beyond the limits of carrier lifetime in coherent population oscillations mechanism....

  14. Ultrafast image-based dynamic light scattering for nanoparticle sizing

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, Wu; Zhang, Jie; Liu, Lili; Cai, Xiaoshu, E-mail: usst-caixs@163.com [Institute of Particle and Two-Phase Flow Measurement, Shanghai Key Laboratory of Multiphase Flow and Heat Transfer in Power Engineering, University of Shanghai for Science and Technology, 516 Jungong Road, Shanghai 200093 (China)

    2015-11-15

    An ultrafast sizing method for nanoparticles is proposed, called as UIDLS (Ultrafast Image-based Dynamic Light Scattering). This method makes use of the intensity fluctuation of scattered light from nanoparticles in Brownian motion, which is similar to the conventional DLS method. The difference in the experimental system is that the scattered light by nanoparticles is received by an image sensor instead of a photomultiplier tube. A novel data processing algorithm is proposed to directly get correlation coefficient between two images at a certain time interval (from microseconds to milliseconds) by employing a two-dimensional image correlation algorithm. This coefficient has been proved to be a monotonic function of the particle diameter. Samples of standard latex particles (79/100/352/482/948 nm) were measured for validation of the proposed method. The measurement accuracy of higher than 90% was found with standard deviations less than 3%. A sample of nanosilver particle with nominal size of 20 ± 2 nm and a sample of polymethyl methacrylate emulsion with unknown size were also tested using UIDLS method. The measured results were 23.2 ± 3.0 nm and 246.1 ± 6.3 nm, respectively, which is substantially consistent with the transmission electron microscope results. Since the time for acquisition of two successive images has been reduced to less than 1 ms and the data processing time in about 10 ms, the total measuring time can be dramatically reduced from hundreds seconds to tens of milliseconds, which provides the potential for real-time and in situ nanoparticle sizing.

  15. Modelling multi-pulse population dynamics from ultrafast spectroscopy.

    Directory of Open Access Journals (Sweden)

    Luuk J G W van Wilderen

    Full Text Available Current advanced laser, optics and electronics technology allows sensitive recording of molecular dynamics, from single resonance to multi-colour and multi-pulse experiments. Extracting the occurring (bio- physical relevant pathways via global analysis of experimental data requires a systematic investigation of connectivity schemes. Here we present a Matlab-based toolbox for this purpose. The toolbox has a graphical user interface which facilitates the application of different reaction models to the data to generate the coupled differential equations. Any time-dependent dataset can be analysed to extract time-independent correlations of the observables by using gradient or direct search methods. Specific capabilities (i.e. chirp and instrument response function for the analysis of ultrafast pump-probe spectroscopic data are included. The inclusion of an extra pulse that interacts with a transient phase can help to disentangle complex interdependent pathways. The modelling of pathways is therefore extended by new theory (which is included in the toolbox that describes the finite bleach (orientation effect of single and multiple intense polarised femtosecond pulses on an ensemble of randomly oriented particles in the presence of population decay. For instance, the generally assumed flat-top multimode beam profile is adapted to a more realistic Gaussian shape, exposing the need for several corrections for accurate anisotropy measurements. In addition, the (selective excitation (photoselection and anisotropy of populations that interact with single or multiple intense polarised laser pulses is demonstrated as function of power density and beam profile. Using example values of real world experiments it is calculated to what extent this effectively orients the ensemble of particles. Finally, the implementation includes the interaction with multiple pulses in addition to depth averaging in optically dense samples. In summary, we show that mathematical

  16. Ultrafast stimulated emission and structural dynamics in nickel porphyrins.

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, X.; Wasinger, E. C.; Muresan, A. Z.; Attenkofer, K.; Jennings, G.; Lindsey, J. S.; Chen, L. X.; North Carolina State U.

    2007-11-22

    The excited-state structural dynamics of nickel(II)tetrakis(2,4,6-trimethylphenyl)porphyrin (NiTMP) and nickel(II)tetrakis(tridec-7-yl)porphyrin (NiSWTP) in a toluene solution were investigated via ultrafast transient optical absorption spectroscopy. An ultrashort stimulated emission between 620 and 670 nm from the S{sub 1} state was observed in both nickel porphyrins only when this state was directly generated via Q-band excitation, whereas such a stimulated emission was absent under B (Soret)-band excitation. Because the stimulated emission in the spectral region occurs only from the S{sub 1} state, this photoexcitation-wavelength-dependent behavior of Ni(II) porphyrins is attributed to a faster intersystem crossing from the S{sub 2} state than the internal conversion S{sub 2} {yields} S{sub 1}. The dynamics of the excited-state pathways involving the ({pi}, {pi}*) and (d, d) states varies with the meso-substituted peripheral groups, which is attributed to the nickel porphyrin macrocycle distortion from a planar configuration. Evidence for intramolecular vibrational relaxation within 2 ps and vibrational cooling in 6-20 ps of a (d, d) excited state has been established for NiTMP and NiSWTP. Finally, the lifetimes of the vibrationally relaxed (d, d) state also depend on the nature of the peripheral groups, decreasing from 200 ps for NiTMP to 100 ps for the bulkier NiSWTP.

  17. Effect of disorder on ultrafast exciton dynamics probed by single molecule spectroscopy

    OpenAIRE

    Hernando Campos, Jordi; van Dijk, Erik M. H. P.; Hoogenboom, Jacob P.; García López, Juan José; Reinhoudt, David N.; Crego Calama, Mercedes; García Parajó, María F.; van Hulst, Niek F.

    2006-01-01

    We present a single-molecule study unraveling the effect of static disorder on the vibrational-assisted ultrafast exciton dynamics in multichromophoric systems. For every single complex, we probe the initial exciton relaxation process by an ultrafast pump-probe approach and the coupling to vibrational modes by emission spectra, while fluorescence lifetime analysis measures the amount of static disorder. Exploiting the wide range of disorder found from complex to complex, we demonstrate that s...

  18. Ultrafast Structural Dynamics in Combustion Relevant Model Systems

    Energy Technology Data Exchange (ETDEWEB)

    Weber, Peter M. [Brown University

    2014-03-31

    The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energy of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of

  19. Dynamics of optical rogue waves in inhomogeneous nonlinear waveguides

    Institute of Scientific and Technical Information of China (English)

    Zhang Jie-Fang; Jin Mei-Zhen; He Ji-Da; Lou Ji-Hui; Dai Chao-Qing

    2013-01-01

    We propose a unified theory to construct exact rogue wave solutions of the (2+1)-dimensional nonlinear Schr(o)dinger equation with varying coefficients.And then the dynamics of the first-and the second-order optical rogues are investigated.Finally,the controllability of the optical rogue propagating in inhomogeneous nonlinear waveguides is discussed.By properly choosing the distributed coefficients,we demonstrate analytically that rogue waves can be restrained or even be annihilated,or emerge periodically and sustain forever.We also figure out the center-of-mass motion of the rogue waves.

  20. Ultrafast magnetization dynamics of lanthanide metals and alloys

    Energy Technology Data Exchange (ETDEWEB)

    Sultan, Muhammad

    2012-05-14

    In this study, the laser-induced magnetization dynamics of the lanthanide ferromagnets Gadolinium (Gd), Terbium (Tb) and their alloys is investigated using femtosecond (fs) time-resolved x-ray magnetic circular dichroism (XMCD), the magneto-optical Kerr effect (MOKE) and magnetic second harmonic generation (MSHG). The magnetization dynamics is analyzed from the time scale of a few fs up to several hundred picoseconds (ps). The contributions of electrons, phonons, spin fluctuations, as well as the temporal regimes corresponding to the spin-orbit and exchange interactions are disentangled. In addition to possible applications in magnetic storage devices, understanding magnetization dynamics in lanthanides is also important because of their different magnetic structure compared to well-studied itinerant ferromagnets. Lanthanides are model Heisenberg-ferromagnets with localized 4f magnetic moments and long range magnetic ordering through indirect exchange interaction. By optical excitation of the conduction electrons, which mediate the exchange interaction, and studying the induced dynamics of the localized 4f and delocalized 5d6s magnetic moments, one can obtain insight into the angular momentum transfer at ultrafast time scales. Moreover, lanthanides offer the possibility to tune spin-lattice coupling via the 4f shell occupation and the concomitant changes in the 4f spin and orbital moments due to Hund's rules. Utilizing this fact, the importance of spin-lattice coupling in laser-induced demagnetization is also analyzed by comparing the magnetization dynamics in Gd and Tb. By investigating the magnetization dynamics of localized 4f moments of Gd and Tb using time-resolved XMCD, it is found that the demagnetization proceeds in both metals in two time scales, following fs laser excitation, which are classified as: (i) non-equilibrium (t > 1 ps), with respect to equilibration of electron and phonon temperatures. The

  1. Ultrafast magnetization dynamics of lanthanide metals and alloys

    Energy Technology Data Exchange (ETDEWEB)

    Sultan, Muhammad

    2012-05-14

    In this study, the laser-induced magnetization dynamics of the lanthanide ferromagnets Gadolinium (Gd), Terbium (Tb) and their alloys is investigated using femtosecond (fs) time-resolved x-ray magnetic circular dichroism (XMCD), the magneto-optical Kerr effect (MOKE) and magnetic second harmonic generation (MSHG). The magnetization dynamics is analyzed from the time scale of a few fs up to several hundred picoseconds (ps). The contributions of electrons, phonons, spin fluctuations, as well as the temporal regimes corresponding to the spin-orbit and exchange interactions are disentangled. In addition to possible applications in magnetic storage devices, understanding magnetization dynamics in lanthanides is also important because of their different magnetic structure compared to well-studied itinerant ferromagnets. Lanthanides are model Heisenberg-ferromagnets with localized 4f magnetic moments and long range magnetic ordering through indirect exchange interaction. By optical excitation of the conduction electrons, which mediate the exchange interaction, and studying the induced dynamics of the localized 4f and delocalized 5d6s magnetic moments, one can obtain insight into the angular momentum transfer at ultrafast time scales. Moreover, lanthanides offer the possibility to tune spin-lattice coupling via the 4f shell occupation and the concomitant changes in the 4f spin and orbital moments due to Hund's rules. Utilizing this fact, the importance of spin-lattice coupling in laser-induced demagnetization is also analyzed by comparing the magnetization dynamics in Gd and Tb. By investigating the magnetization dynamics of localized 4f moments of Gd and Tb using time-resolved XMCD, it is found that the demagnetization proceeds in both metals in two time scales, following fs laser excitation, which are classified as: (i) non-equilibrium (t > 1 ps), with respect to equilibration of electron and phonon temperatures. The

  2. Ultrafast optical control of magnetization dynamics in polycrystalline bismuth doped iron garnet thin films

    Energy Technology Data Exchange (ETDEWEB)

    Deb, Marwan, E-mail: marwan.deb@ipcms.unistra.fr; Vomir, Mircea; Rehspringer, Jean-Luc; Bigot, Jean-Yves [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504, CNRS, Université de Strasbourg, BP 43, 23 rue du Loess, 67034 Strasbourg Cedex 02 (France)

    2015-12-21

    Controlling the magnetization dynamics on the femtosecond timescale is of fundamental importance for integrated opto-spintronic devices. For industrial perspectives, it requires to develop simple growth techniques for obtaining large area magneto-optical materials having a high amplitude ultrafast Faraday or Kerr response. Here we report on optical pump probe studies of light induced spin dynamics in high quality bismuth doped iron garnet polycrystalline film prepared by the spin coating method. We demonstrate an ultrafast non-thermal optical control of the spin dynamics using both circularly and linearly polarized pulses.

  3. Dynamics of single photon transport in a one-dimensional waveguide two-point coupled with a Jaynes-Cummings system

    Science.gov (United States)

    Wang, Yuwen; Zhang, Yongyou; Zhang, Qingyun; Zou, Bingsuo; Schwingenschlogl, Udo

    2016-01-01

    We study the dynamics of an ultrafast single photon pulse in a one-dimensional waveguide two-point coupled with a Jaynes-Cummings system. We find that for any single photon input the transmissivity depends periodically on the separation between the two coupling points. For a pulse containing many plane wave components it is almost impossible to suppress transmission, especially when the width of the pulse is less than 20 times the period. In contrast to plane wave input, the waveform of the pulse can be modified by controlling the coupling between the waveguide and Jaynes-Cummings system. Tailoring of the waveform is important for single photon manipulation in quantum informatics. PMID:27653770

  4. Dynamics of single photon transport in a one-dimensional waveguide two-point coupled with a Jaynes-Cummings system

    KAUST Repository

    Wang, Yuwen

    2016-09-22

    We study the dynamics of an ultrafast single photon pulse in a one-dimensional waveguide two-point coupled with a Jaynes-Cummings system. We find that for any single photon input the transmissivity depends periodically on the separation between the two coupling points. For a pulse containing many plane wave components it is almost impossible to suppress transmission, especially when the width of the pulse is less than 20 times the period. In contrast to plane wave input, the waveform of the pulse can be modified by controlling the coupling between the waveguide and Jaynes-Cummings system. Tailoring of the waveform is important for single photon manipulation in quantum informatics. © The Author(s) 2016.

  5. Femtosecond Carrier Dynamics and Modelocking in Monolithic CPM Lasers. [SB1

    DEFF Research Database (Denmark)

    Brorson, S.D.; Bischoff, Svend; MØrk, J.

    1996-01-01

    Femtosecond pump-probe measurements of the dynamics in both forward- and reverse-biased semiconductor optical waveguides arepresented. Slow (nanosecond) as well as ultrafast (femtosecond) dynamics are observed in both kinds of structures....

  6. Femtosecond Carrier Dynamics and Modelocking in Monolithic CPM Lasers. [SB1

    DEFF Research Database (Denmark)

    Brorson, S.D.; Bischoff, Svend; MØrk, J.;

    1996-01-01

    Femtosecond pump-probe measurements of the dynamics in both forward- and reverse-biased semiconductor optical waveguides arepresented. Slow (nanosecond) as well as ultrafast (femtosecond) dynamics are observed in both kinds of structures....

  7. Ultrafast Laser Dynamics and Interactions in Complex Materials

    Science.gov (United States)

    Patz, Aaron Edward

    The work described in this thesis underscores specific examples of using an ultrafast laser as a materials research tool for studying condensed matter physics in complex materials. The majority of materials studied fall into the iron-pnictide class of unconventional superconductors, which exhibit a multitude of phases that appear to be dependent on each other, or the magnetic semiconductor, GaMnAs. In my work I show various ultrafast laser techniques for studying these complex materials in order to decouple the different properties in the time-domain and gain information about the underlying physics governing the material properties.

  8. Influence of boron concentration on nonlinear absorption and ultrafast dynamics in GaSe crystals

    Science.gov (United States)

    Karatay, Ahmet; Yuksek, Mustafa; Ertap, Hüseyin; Mak, Ali Kemal; Karabulut, Mevlüt; Elmali, Ayhan

    2016-10-01

    The nonlinear absorption properties and ultrafast dynamics of pure and boron doped GaSe crystals have been studied by open aperture Z-scan and ultrafast pump probe spectroscopy techniques. All of the studied crystals showed nonlinear absorption under 100 fs pulse duration and 1200 nm wavelength excitations. Nonlinear absorption coefficients increase with increasing the doping ratio of boron atoms in crystals. These findings indicate that free carrier density increase with boron doping and this behavior leads to excited state absorption. Second harmonic generation signals of crystals were detected with the help of fiber optic spectrometer. The blue shift in the energy of the second harmonic generation signals was observed in boron doped crystals. Ultrafast pump probe experiments indicate that the excited state absorption signal with long lifetime observed for undoped GaSe crystal switches to bleach signal for boron doped GaSe crystals at 625 nm probe wavelength. The effects of increasing doping ratio were observed on ultrafast dynamics as a switching time changes. Our experimental results indicate that it is possible to control nonlinear absorption properties, frequency conversion and ultrafast dynamics of GaSe crystal by changing boron doping ratio.

  9. Ultrafast Structural Dynamics in Combustion Relevant Model Systems

    Energy Technology Data Exchange (ETDEWEB)

    Weber, Peter M. [Brown University

    2014-03-31

    The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energy of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of

  10. Manufacturing of Er:ZBLAN ridge waveguides by pulsed laser deposition and ultrafast laser micromachining for green integrated lasers

    Energy Technology Data Exchange (ETDEWEB)

    Gottmann, Jens [Lehrstuhl fuer Lasertechnik, RWTH Aachen University, Steinbachstr. 15, 52074 Aachen (Germany)], E-mail: jens.gottmann@llt.rwth-aachen.de; Moiseev, Leonid; Vasilief, Ion; Wortmann, Dirk [Lehrstuhl fuer Lasertechnik, RWTH Aachen University, Steinbachstr. 15, 52074 Aachen (Germany)

    2008-01-15

    Laser radiation is used both for the deposition of the laser active thin films and for the microstructuring to define wave guiding structures for the fabrication of waveguide lasers. Thin films of Er:ZBLAN (a fluoride glass consisting of ZrF{sub 4}, BaF{sub 2}, LaF{sub 3}, AlF{sub 3}, NaF, ErF{sub 3}) for green up-conversion lasers (545 nm) are produced by pulsed laser deposition using ArF excimer laser radiation (wavelength 193 nm). Manufacturing of the laser active waveguides by microstructuring is done using fs-laser ablation of the deposited films. The structural and optical properties of the films and the damping losses of the structured waveguides are determined in view of the design and the fabrication of compact and efficient diode pumped waveguide lasers. The resulting waveguides are polished, provided with resonator mirrors, pumped using diode lasers and characterized.

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

    Institute of Scientific and Technical Information of China (English)

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

    2005-01-01

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

  12. Ultra-fast dynamic imaging: an overview of current techniques, their capabilities and future prospects

    Science.gov (United States)

    Altucci, C.; Velotta, R.; Marangos, J. P.

    2010-06-01

    In this review we attempt to sketch an overview of the various methods currently being used or under development to enable ultra-fast dynamic imaging of matter. We concentrate on those techniques which combine atomic scale spatial resolution and femtosecond or even sub-femtosecond temporal resolution. In part this review was inspired and informed by the material presented at the 'Ultrafast Dynamic Imaging II' workshop held in Ischia, Italy in April 2009, but we also have drawn on a wider background of material especially when discussing the emerging laser-based methods.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-05-14

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

  14. Ab initio theory for ultrafast magnetization dynamics with a dynamic band structure

    Science.gov (United States)

    Mueller, B. Y.; Haag, M.; Fähnle, M.

    2016-09-01

    Laser-induced modifications of magnetic materials on very small spatial dimensions and ultrashort timescales are a promising field for novel storage and spintronic devices. Therefore, the contribution of electron-electron spin-flip scattering to the ultrafast demagnetization of ferromagnets after an ultrashort laser excitation is investigated. In this work, the dynamical change of the band structure resulting from the change of the magnetization in time is taken into account on an ab initio level. We find a large influence of the dynamical band structure on the magnetization dynamics and we illustrate the thermalization and relaxation process after laser irradiation. Treating the dynamical band structure yields a demagnetization comparable to the experimental one.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-11-01

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

  16. Toward Ultrafast Spin Dynamics in Low Dimensional Semiconductors

    Science.gov (United States)

    Chiu, Yi-Hsin

    neighboring Fe spins, as well as the resulting exchange-driven electron spin relaxation in GaAs. This lays the groundwork for this dissertation to explore low dimensional systems. Second, we work to facilitate optical studies of spin dynamics in one dimension (1D), which hasnt been possible in the past due to the fundamental challenge of optical polarization anisotropy. We propose a dielectric-matched membrane structure based on GaAs/AlGaAs core-shell nanowires. By simultaneous addressing the optical polarization anisotropy and various technical challenges, this study offers a promising route to optical investigations of 1D spin physics. Third, a novel 2D material, germanane (GeH), is investigated by continuous wave (cw) polarization-resolved photoluminescence (PL) spectroscopy as a first step toward future ultrafast pump-probe study. PL develops a finite degree of circular polarization under circular excitation (optical orientation) or in an applied magnetic field (Zeeman effect), indicating the presence of spin-polarized carriers. This study presents the first magneto-optical investigation in germanane.

  17. Tunable Ultrafast Photon Source and Imaging System for Studying Carrier Dynamics in Graphene Devices

    Science.gov (United States)

    2015-07-23

    Tunable ultrafast photon source and imaging system for studying carrier dynamics in graphene devices This project enabled the acquisition of a...and imaging system for studying carrier dynamics in graphene devices Report Title This project enabled the acquisition of a optical parametric...carrier dynamics in graphene devices As discussed below the focus of this DURIP project was on understanding the interaction between electrons, holes

  18. Ultrafast Gain Dynamics in Quantum Dot Amplifiers: Theoretical Analysis and Experimental Investigations

    DEFF Research Database (Denmark)

    Poel, Mike van der; Gehrig, Edeltraud; Hess, Ortwin;

    2005-01-01

    Ultrafast gain dynamics in an optical amplifier with an active layer of self-organized quantum dots (QDs) emitting near 1.3$muhbox m$is characterized experimentally in a pump-probe experiment and modeled theoretically on the basis of QD Maxwell–Bloch equations. Experiment and theory are in good...

  19. Ultrafast optical dynamics of HITCI in ethylene glycol. A non-Markovian Brownian oscillator description

    NARCIS (Netherlands)

    de Boeij, Wim P; Pshenichnikov, Maxim S.; Duppen, Koos; Wiersma, Douwe A.

    1994-01-01

    Femtosecond photon echo, chirped four-wave mixing and pump-probe experiments are reported, using a 13 fs cavity-dumped Ti: sapphire laser for excitation. It is shown that the optical dynamics of HITCI in ethylene glycol occurs on distinctly different time scales. The ultrafast solvent response is

  20. Terahertz study of ultrafast carrier dynamics in InGa/GaN multiple quantum wells

    DEFF Research Database (Denmark)

    Porte, Henrik; Turchinovich, Dmitry; Cooke, David

    2009-01-01

    Ultrafast carrier dynamics in InGaN/GaN multiple quantum wells is measured by time-resolved terahertz spectroscopy. The built-in piezoelectric field is initially screened by photoexcited, polarized carriers, and is gradullay restored as the carriers recombine. We observe a nonexponential decay...

  1. Ultrafast ring-closing reaction dynamics of a photochromic furan-based difurylethene

    Science.gov (United States)

    Khodko, A.; Khomenko, V.; Shynkarenko, Y.; Mamuta, O.; Kapitanchuk, O.; Sysoiev, D.; Kachalova, N.; Huhn, T.; Snegir, S.

    2017-02-01

    The ultrafast photoinduced ring-closing dynamics of a furan-based difurylethene (YnPhT) has been investigated by femtosecond transient absorption spectroscopy. We performed time-dependent density functional theory (TD-DFT) calculations to explain the experimental results in detail. The sub-picosecond time scale of the ring-closing reaction is comparable with thiophene-based analogues, but oxygen atoms at the photochromic core can avoid adverse interaction between switches and metal contacts in further applications. This observation proves that furan-based diarylethenes are potential optoelectronic elements with an ultrafast optical response.

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

    Science.gov (United States)

    Du, Guangqing; Wu, Yanmin; Uddin, Noor; Yang, Qing; Chen, Feng; Lu, Yu; Bian, Hao; Hou, Xun

    2016-09-01

    The ultrafast thermal dynamics of nano-ripples formation on gold film via ultrafast laser double pulses excitation is theoretically investigated by numerical simulations. The non-equilibrium thermal modulations with respect to the electron and phonon energy transfers within gold film is proposed for predicting the nano-ripples formation. It is revealed that the nano-ripples contrast on gold film surface can be well controlled via tuning the pulse energy ratio, pulse separation and pulse exchange of ultrafast laser double-pulse. It is attributed to the tunable energy transfer routes between the electron thermal diffusion and the electron-phonon coupling via tuning double pulses parameters. The study provides theoretical basis for producing high-contrast ripples for a wide range application in the fields such as high-absorptive solar cells, surface friction devices and super-hydrophobic surface.

  3. Shock induced chemistry in liquids studied with ultrafast dynamic ellipsometry and visible transient absorption spectroscopy.

    Science.gov (United States)

    Dang, N C; Bolme, C A; Moore, D S; McGrane, S D

    2012-10-25

    The response to ultrafast laser shock loading of nine liquids was monitored in an effort to reveal evidence of chemical changes occurring during the first 350 ps following the shock front. In an effort to compare molecular structures possessing a variety of common bonding patterns, data were acquired for the liquids: cyclohexane, cyclohexene, 1,3-cyclohexadiene, benzene, water, acetonitrile, acrylonitrile, tert-butylacetylene, and phenylacetylene. Transient absorption spectra were measured in the spectral region from 440 to 780 nm over shock stress states from 7 to 20 GPa. Ultrafast dynamic ellipsometry was used to measure the shock and particle velocity as well as the shocked refractive index. Significant transient absorption attributed to chemical reaction was observed for shocked phenylacetylene and acrylonitrile. Evidence of volume decreasing chemical reactions was also observed in the ultrafast dynamic ellipsometry data for phenylacetylene and acrylonitrile. The liquid 1,3-cyclohexadiene exhibited volume decreasing reaction in the ultrafast dynamic ellipsometry data but did not exhibit an increase in the transient absorption spectra. There was no evidence of chemical reaction in cyclohexane, cyclohexene, benzene, water, acetonitrile, or tert-butylacetylene in the first 350 ps, despite the application of shock stress that was in many cases well above the reaction threshold observed at microsecond time scales.

  4. Ultrafast nonlinear dynamics of thin gold films due to an intrinsic delayed nonlinearity

    Science.gov (United States)

    Bache, Morten; Lavrinenko, Andrei V.

    2017-09-01

    Using long-range surface plasmon polaritons light can propagate in metal nano-scale waveguides for ultracompact opto-electronic devices. Gold is an important material for plasmonic waveguides, but although its linear optical properties are fairly well understood, the nonlinear response is still under investigation. We consider the propagation of pulses in ultrathin gold strip waveguides, modeled by the nonlinear Schrödinger equation. The nonlinear response of gold is accounted for by the two-temperature model, revealing it as a delayed nonlinearity intrinsic in gold. The consequence is that the measured nonlinearities are strongly dependent on pulse duration. This issue has so far only been addressed phenomenologically, but we provide an accurate estimate of the quantitative connection as well as a phenomenological theory to understand the enhanced nonlinear response as the gold thickness is reduced. In comparison with previous works, the analytical model for the power-loss equation has been improved, and can be applied now to cases with a high laser peak power. We show new fits to experimental data from the literature and provide updated values for the real and imaginary parts of the nonlinear susceptibility of gold for various pulse durations and gold layer thicknesses. Our simulations show that the nonlinear loss is inhibiting efficient nonlinear interaction with low-power laser pulses. We therefore propose to design waveguides suitable for the mid-IR, where the ponderomotive instantaneous nonlinearity can dominate over the delayed hot-electron nonlinearity and provide a suitable plasmonics platform for efficient ultrafast nonlinear optics.

  5. Graphene and carbon nanotubes ultrafast relaxation dynamics and optics

    CERN Document Server

    Malic, Ermin

    2013-01-01

    The book introduces the reader into the ultrafast nanoworld of graphene and carbon nanotubes, including their microscopic tracks and unique optical finger prints. The author reviews the recent progress in this field by combining theoretical and experimental achievements. He offers a clear theoretical foundation by presenting transparently derived equations. Recent experimental breakthroughs are reviewed. By combining both theory and experiment as well as main results and detailed theoretical derivations, the book turns into an inevitable source for a wider audience from graduate students to researchers in physics, materials science, and electrical engineering who work on optoelectronic devices, renewable energies, or in the semiconductor industry.

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

    Science.gov (United States)

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

    2016-11-01

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

  7. Doppler Spectrometry for Ultrafast Temporal Mapping of Density Dynamics in Laser-Induced Plasmas

    Science.gov (United States)

    Mondal, S.; Lad, Amit D.; Ahmed, Saima; Narayanan, V.; Pasley, J.; Rajeev, P. P.; Robinson, A. P. L.; Kumar, G. Ravindra

    2010-09-01

    We present high resolution measurements of the ultrafast temporal dynamics of the critical surface in moderately overdense, hot plasma by using two-color, pump-probe Doppler spectrometry. Our measurements clearly capture the initial inward motion of the plasma inside the critical surface of the pump laser which is followed by outward expansion. The measured instantaneous velocity and acceleration profiles are very well reproduced by a hybrid simulation that uses a 1D electromagnetic particle-in-cell simulation for the initial evolution and a hydrodynamics simulation for the later times. The combination of high temporal resolution and dynamic range in our measurements clearly provides quantitative unraveling of the dynamics in this important region, enabling this as a powerful technique to obtain ultrafast snapshots of plasma density and temperature profiles for providing benchmarks for simulations.

  8. Dynamical light control in longitudinally modulated segmented waveguide arrays

    CERN Document Server

    Kartashov, Yaroslav V

    2011-01-01

    We address light propagation in segmented waveguide arrays where the refractive index is longitudinally modulated with an out-of-phase modulation in adjacent waveguides, so that the coupling strength varies along propagation direction. Thus in resonant segments coupling may be inhibited hence light remains localized, while in detuned segments coupling results in complex switching scenarios that may be controlled by stacking several resonant and nonresonant segments. By tuning the modulation frequency and lengths of waveguide segments one may control the distribution of light among the output guides, including loca-lizing all light in the selected output channel.

  9. Probing Transient Electron Dynamics Using Ultrafast X Rays

    Science.gov (United States)

    Bucksbaum, Philip

    2016-05-01

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

  10. The Anisotropic Dynamic Response of Ultrafast Shocked Single Crystal PETN and Beta-HMX

    Science.gov (United States)

    Zaug, Joseph; Armstrong, Michael; Crowhurst, Jonathan; Austin, Ryan; Ferranti, Louis; Fried, Laurence; Bastea, Sorin

    2015-06-01

    We report results from ultrafast shockwave experiments conducted on single crystal high explosives. Experimental results consist of 12 picosecond time-resolved dynamic response wave profile data, (ultrafast time-domain interferometry-TDI), which are used to validate calculations of anisotropic stress-strain behavior of shocked loaded energetic materials. In addition, here we present unreacted equations of state data from PETN and beta-HMX up to higher pressures than previously reported, which are used to extend the predictive confidence of hydrodynamic simulations. Our previous results derived from a 360 ps drive duration yielded anisotropic elastic wave response in single crystal beta-HMX ((110) and (010) impact planes). Here we provide results using a 3x longer drive duration to probe the plastic response regime of these materials. We compare our ultrafast time domain interferometry (TDI) results with previous gun platform results. Ultrafast time scale resolution TDI measurements further guide the development of continuum models aimed to study pore collapse and energy localization in shock-compressed crystals of beta-HMX. This work was performed under the auspices of the U.S. Department of Energy jointly by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

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

    Science.gov (United States)

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

    2015-06-14

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

  12. Towards Ultrafast Communications: Nonlinear Coupling Dynamics and Light-Semiconductor Interaction

    NARCIS (Netherlands)

    Wang, W.

    2007-01-01

    This thesis deals with some specific problems concerning the processing of ultrashort optical pulses and their interaction with semiconductors. It includes the investigation of the ultrashort optical pulse propagation and coupling dynamics in the nonlinear coupled waveguide, and the coherent and in

  13. Towards Ultrafast Communications: Nonlinear Coupling Dynamics and Light-Semiconductor Interaction

    NARCIS (Netherlands)

    Wang, W.

    2007-01-01

    This thesis deals with some specific problems concerning the processing of ultrashort optical pulses and their interaction with semiconductors. It includes the investigation of the ultrashort optical pulse propagation and coupling dynamics in the nonlinear coupled waveguide, and the coherent and

  14. Ultrafast, green third-harmonic generation and strong-field phenomena in silicon-on-insulator nanoplasmonic waveguides

    OpenAIRE

    Sederberg, Shawn; Elezzabi, Abdulhakem Y.

    2013-01-01

    The emergence of strong-field nanoplasmonics brings extreme laser field-matter interaction into the realm of nanoscale science, unveiling exciting new physics. Highly nonlinear interaction is enabled by tightly confined electric fields in nanoplasmonic structures, permitting use of optical fields from low-power laser oscillators. Here, we report the first demonstration of visible 517nm third harmonic generation in ultracompact nanoplasmonic waveguides on a silicon-on-insulator platform at an ...

  15. Wavelet analysis of molecular dynamics: Efficient extraction of time-frequency information in ultrafast optical processes

    Energy Technology Data Exchange (ETDEWEB)

    Prior, Javier; Castro, Enrique [Departamento de Física Aplicada, Universidad Politécnica de Cartagena, Cartagena 30202 (Spain); Chin, Alex W. [Theory of Condensed Matter Group, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE (United Kingdom); Almeida, Javier; Huelga, Susana F.; Plenio, Martin B. [Institut für Theoretische Physik, Albert-Einstein-Allee 11, Universität Ulm, D-89069 Ulm (Germany)

    2013-12-14

    New experimental techniques based on nonlinear ultrafast spectroscopies have been developed over the last few years, and have been demonstrated to provide powerful probes of quantum dynamics in different types of molecular aggregates, including both natural and artificial light harvesting complexes. Fourier transform-based spectroscopies have been particularly successful, yet “complete” spectral information normally necessitates the loss of all information on the temporal sequence of events in a signal. This information though is particularly important in transient or multi-stage processes, in which the spectral decomposition of the data evolves in time. By going through several examples of ultrafast quantum dynamics, we demonstrate that the use of wavelets provide an efficient and accurate way to simultaneously acquire both temporal and frequency information about a signal, and argue that this greatly aids the elucidation and interpretation of physical process responsible for non-stationary spectroscopic features, such as those encountered in coherent excitonic energy transport.

  16. Wavelet analysis of molecular dynamics: efficient extraction of time-frequency information in ultrafast optical processes.

    Science.gov (United States)

    Prior, Javier; Castro, Enrique; Chin, Alex W; Almeida, Javier; Huelga, Susana F; Plenio, Martin B

    2013-12-14

    New experimental techniques based on nonlinear ultrafast spectroscopies have been developed over the last few years, and have been demonstrated to provide powerful probes of quantum dynamics in different types of molecular aggregates, including both natural and artificial light harvesting complexes. Fourier transform-based spectroscopies have been particularly successful, yet "complete" spectral information normally necessitates the loss of all information on the temporal sequence of events in a signal. This information though is particularly important in transient or multi-stage processes, in which the spectral decomposition of the data evolves in time. By going through several examples of ultrafast quantum dynamics, we demonstrate that the use of wavelets provide an efficient and accurate way to simultaneously acquire both temporal and frequency information about a signal, and argue that this greatly aids the elucidation and interpretation of physical process responsible for non-stationary spectroscopic features, such as those encountered in coherent excitonic energy transport.

  17. Ultrafast carrier dynamics in band edge and broad deep defect emission ZnSe nanowires

    Science.gov (United States)

    Othonos, Andreas; Lioudakis, Emmanouil; Philipose, U.; Ruda, Harry E.

    2007-12-01

    Ultrafast carrier dynamics of ZnSe nanowires grown under different growth conditions have been studied. Transient absorption measurements reveal the dependence of the competing effects of state filling and photoinduced absorption on the probed energy states. The relaxation of the photogenerated carriers occupying defect states in the stoichiometric and Se-rich samples are single exponentials with time constants of 3-4ps. State filling is the main contribution for probe energies below 1.85eV in the Zn-rich grown sample. This ultrafast carrier dynamics study provides an important insight into the role that intrinsic point defects play in the observed photoluminescence from ZnSe nanowires.

  18. Ultrafast gain dynamics in InAs/InGaAs quantum dot amplifiers

    DEFF Research Database (Denmark)

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

    2000-01-01

    The ultrafast dynamics of gain and refractive index in an electrically pumped InAs-InGaAs quantum-dot (QD) optical amplifier are measured at room temperature using differential transmission with femtosecond time resolution. Both absorption and gain regions are investigated. While the absorption...... bleaching recovery occurs on a picosecond time scale, the gain compression recovers with ~100-fs time constant, making devices based on such dots promising for high-speed optical communications....

  19. Predicted Ultrafast Dynamic Metallization of Dielectric Nanofilms by Strong Single-Cycle Optical Fields

    Science.gov (United States)

    Durach, Maxim; Rusina, Anastasia; Kling, Matthias F.; Stockman, Mark I.

    2011-08-01

    We predict a dynamic metallization effect where an ultrafast (single-cycle) optical pulse with a ≲1V/Å field causes plasmonic metal-like behavior of a dielectric film with a few-nm thickness. This manifests itself in plasmonic oscillations of polarization and a significant population of the conduction band evolving on a ˜1fs time scale. These phenomena are due to a combination of both adiabatic (reversible) and diabatic (for practical purposes irreversible) pathways.

  20. Ultrafast solvation dynamics at internal site of staphylococcal nuclease investigated by site-directed mutagenesis

    CERN Document Server

    Guang-yu, Gao; Wei, Wang; Shu-feng, Wang; Zhong, Dongping; Qi-huang, Gong

    2014-01-01

    Solvation is essential for protein activities. To study internal solvation of protein, site-directed mutagenesis is applied. Intrinsic fluorescent probe, tryptophan, is inserted into desired position inside protein molecule for ultrafast spectroscopic study. Here we review this unique method for protein dynamics researches. We introduce the frontiers of protein solvation, site-directed mutagenesis, protein stability and characteristics, and the spectroscopic methods. Then we present time-resolved spectroscopic dynamics of solvation dynamics inside caves of active sites. The studies are carried out on a globular protein, staphylococcal nuclease. The solvation at internal sites of the caves indicate clear characteristics of local environment. These solvation behaviors correlated to the enzyme activity directly.

  1. The study of photo-induced ultrafast dynamics in light-harvesting complex LH2 of purple bacteria

    Institute of Scientific and Technical Information of China (English)

    LIU Wei-min; YAN Yong-li; LIU Kang-jun; XU Chun-he; QIAN Shi-xiong

    2006-01-01

    In this paper,we introduce the photo-induced ultrafast dynamics taking place in the peripheral light harvesting antenna LH2 from purple bacteria Rhodobacter sphaeroides by using absorption,fluorescence emission and ultrafast spectroscopic techniques.Three kinds of LH2 sampies,pH treated LH2 (complete removal of B800 pigments),carotenoid mutated LH2 (GM 309) and electrochemical oxidation treated LH2 were used in comparison with native LH2 to investigate the mechanism of photo-induced ultrafast energy transfer within the LH2 complex.

  2. Ultrafast dynamics of exciton fission in polycrystalline pentacene.

    Science.gov (United States)

    Wilson, Mark W B; Rao, Akshay; Clark, Jenny; Kumar, R Sai Santosh; Brida, Daniele; Cerullo, Giulio; Friend, Richard H

    2011-08-10

    We use ultrafast transient absorption spectroscopy with sub-20 fs time resolution and broad spectral coverage to directly probe the process of exciton fission in polycrystalline thin films of pentacene. We observe that the overwhelming majority of initially photogenerated singlet excitons evolve into triplet excitons on an ∼80 fs time scale independent of the excitation wavelength. This implies that exciton fission occurs at a rate comparable to phonon-mediated exciton localization processes and may proceed directly from the initial, delocalized, state. The singlet population is identified due to the brief presence of stimulated emission, which is emitted at wavelengths which vary with the photon energy of the excitation pulse, a violation of Kasha's Rule that confirms that the lowest-lying singlet state is extremely short-lived. This direct demonstration that triplet generation is both rapid and efficient establishes multiple exciton generation by exciton fission as an attractive route to increased efficiency in organic solar cells. © 2011 American Chemical Society

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

    Science.gov (United States)

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

    2017-07-17

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

  4. The Study of Shock Waves and Laser Excited Lattice Dynamics using Ultrafast X-ray Diffraction

    Science.gov (United States)

    Funk, David J.; Hur, N.; Wark, J.

    2005-07-01

    We have studied the picosecond lattice dynamics of optically pumped hexagonal manganite LuMnO3 using ultrafast x-ray diffraction. The results show a shift and broadening of the diffraction curve due to the stimulated lattice expansion. To understand the transient response of the lattice, the measured time- and angle-resolved diffraction curves are compared with a theoretical calculation based on dynamical diffraction theory modified for the hexagonal crystal structure of LuMnO3. Our simulations reveal that a large coupling coefficient between the a-b plane and the c-axis (c13) is required to the data. We compare this result to our previous coherent phonon studies of LuMnO3 using optical pump-probe spectroscopy. We have also performed preliminary experiments of shock waves traversing thin (approximately one micron) metal single-crystals, characterizing the shock wave using ultrafast spatial interferometry and with ultrafast x-ray diffraction. A summary of our current results will be presented.

  5. Ultrafast nano-imagining of the photoinduced phase transition dynamics in VO2

    Science.gov (United States)

    Doenges, Sven A.; Khatib, Omar; O'Callahan, Brian T.; Atkin, Joanna M.; Park, Jae Hyung; Cobden, David H.; Raschke, Markus B.

    Many quantum phase transitions in correlated matter exhibit spatial inhomogeneities with expected yet unexplored effects on the associated ultrafast dynamics. Here we demonstrate the combination of ultrafast non-degenerate pump-probe spectroscopy with scattering scanning near-field optical microscopy (s-SNOM) for ultrafast nano-imaging. In a femtosecond near-field non-degenerate near-IR (NIR) pump and mid-IR (MIR) probe experiment, we study the photoinduced insulator-to-metal (IMT) transition in nominally homogeneous VO2 micro-crystals using far-from equilibrium excitation. We observe spatial heterogeneity on 50-100 nm length scales in the fluence dependent IMT dynamics, ranging from sub-100 fs to 1 ps. With pump fluences as high as nominally 10 mJ/cm2 we can reach distinct excitation and saturation regimes. These results suggest a large sensitivity of the IMT with respect to local variations in strain, doping, or defects difficult to discern microscopically.

  6. Ultrafast exciton migration in an HJ-aggregate: Potential surfaces and quantum dynamics

    Science.gov (United States)

    Binder, Robert; Polkehn, Matthias; Ma, Tianji; Burghardt, Irene

    2017-01-01

    Quantum dynamical and electronic structure calculations are combined to investigate the mechanism of exciton migration in an oligothiophene HJ aggregate, i.e., a combination of oligomer chains (J-type aggregates) and stacked aggregates of such chains (H-type aggregates). To this end, a Frenkel exciton model is parametrized by a recently introduced procedure [Binder et al., J. Chem. Phys. 141, 014101 (2014)] which uses oligomer excited-state calculations to perform an exact, point-wise mapping of coupled potential energy surfaces to an effective Frenkel model. Based upon this parametrization, the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method is employed to investigate ultrafast dynamics of exciton transfer in a small, asymmetric HJ aggregate model composed of 30 sites and 30 active modes. For a partially delocalized initial condition, it is shown that a torsional defect confines the trapped initial exciton, and planarization induces an ultrafast resonant transition between an HJ-aggregated segment and a covalently bound "dangling chain" end. This model is a minimal realization of experimentally investigated mixed systems exhibiting ultrafast exciton transfer between aggregated, highly planarized chains and neighboring disordered segments.

  7. Ultrafast excited state dynamics of S2 and S1 states of triphenylmethane dyes.

    Science.gov (United States)

    Singhal, Pallavi; Ghosh, Hirendra N

    2014-08-21

    Excited state dynamics of S2 and S1 states for a series of TPM dyes, pyrogallol red (PGR), bromopyrogallol red (Br-PGR) and aurin tricarboxylic acid (ATC), have been monitored by using ultrafast transient absorption and fluorescence up-conversion techniques. Optical absorption studies indicate that all the TPM dyes exist as keto-enol tautomers depending upon the pH of the solution. Interestingly, all the TPM dyes give S2 emission (major emitting state) in addition to weak S1 emission. S2 emission lifetimes as fast as ∼150-300 fs and S1 emission lifetimes of 2-5 ns were observed depending upon the molecular structure of the dyes. Femtosecond transient absorption studies suggest the presence of an ultrafast non-radiative decay channel from the S2 state in addition to S2 luminescence. The vibrational relaxation time from hot S1 state is found to be 2-6 ps. The heavy atom effect has been observed in ultrafast relaxation dynamics of Br-PGR.

  8. 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.

  9. Ultrafast transient lens spectroscopy of photoisomerization dynamics of azocompounds in confined nanospace of cyclodextrins

    Science.gov (United States)

    Yui, Hiroharu; Takei, Masako; Hirose, Yasushi; Sawada, Tsuguo

    2003-01-01

    The ultrafast photoisomerization dynamics of azocompounds encapsulated in the cavity of α-, β-, and γ-cyclodextrin (CD) was investigated by the ultrafast transient lens method regarding effects of special restriction and intermolecular interactions. As expected, the spatial restriction reduced the yield of photoisomerization, but the effect was not so remarkable, indicating that the host and guest were relatively freely bounded. This effect was more prominent in azo: γ-CD=2:2 system, where the two guest molecules were packed in parallel as a dimer. From the viewpoint of the confined nanospace as a new reaction field, we found that the azo: γ-CD=2:2 system induced a specific intermediate having a long lifetime, which was not observed in free solutions. We also found that the formation of hydrogen-bonding between CD and guest remarkably elongated the trans-cis transformation of guest molecules in Orange II/CD systems.

  10. Existence, stability and dynamics of discrete solitary waves in a binary waveguide array

    Science.gov (United States)

    Shen, Y.; Kevrekidis, P. G.; Srinivasan, G.; Aceves, A. B.

    2016-07-01

    Recent work has explored binary waveguide arrays in the long-wavelength, near-continuum limit, here we examine the opposite limit, namely the vicinity of the so-called anti-continuum limit. We provide a systematic discussion of states involving one, two and three excited waveguides, and provide comparisons that illustrate how the stability of these states differ from the monoatomic limit of a single type of waveguide. We do so by developing a general theory which systematically tracks down the key eigenvalues of the linearized system. When we find the states to be unstable, we explore their dynamical evolution through direct numerical simulations. The latter typically illustrate, for the parameter values considered herein, the persistence of localized dynamics and the emergence for the duration of our simulations of robust quasi-periodic states for two excited sites. As the number of excited nodes increases, the unstable dynamics feature less regular oscillations of the solution’s amplitude.

  11. Existence, Stability and Dynamics of Discrete Solitary Waves in a Binary Waveguide Array

    CERN Document Server

    Shen, Y; Srinivasan, G; Aceves, A B

    2015-01-01

    Recent work has explored binary waveguide arrays in the long-wavelength, near-continuum limit, here we examine the opposite limit, namely the vicinity of the so-called anti-continuum limit. We provide a systematic discussion of states involving one, two and three excited waveguides, and provide comparisons that illustrate how the stability of these states differ from the monoatomic limit of a single type of waveguide. We do so by developing a general theory which systematically tracks down the key eigenvalues of the linearized system. When we find the states to be unstable, we explore their dynamical evolution through direct numerical simulations. The latter typically illustrate, for the parameter values considered herein, the persistence of localized dynamics and the emergence for the duration of our simulations of robust quasi-periodic states for two excited sites. As the number of excited nodes increase, the unstable dynamics feature less regular oscillations of the solution's amplitude.

  12. Preface to Special Topic: Invited Papers of the 3rd International Conference on Ultrafast Structural Dynamics.

    Science.gov (United States)

    Johnson, S L

    2016-03-01

    The ability to visualize the real-time dynamics of atomic, magnetic, and electronic structure is widely recognized in many fields as a key element underpinning many important processes in chemistry, materials science, and biology. The need for an improved understanding of such processes becomes acute as energy conversion processes on fast time scales become increasingly relevant to problems in science and technology. This special issue, containing invited papers from participants at the 3rd International Conference on Ultrafast Structural Dynamics held June 10-12, 2015 in Zurich, Switzerland, discusses several recent developments in this area.

  13. Ultrafast low-energy dynamics of graphite studied by nonlinear multi-THz spectroscopy

    Directory of Open Access Journals (Sweden)

    Leitenstorfer A.

    2013-03-01

    Full Text Available Ultraintense few-cycle THz pulses are employed to study the nonlinear response of graphite. A phase sensitive 2D spectroscopy setup is capable of detecting pump-induced transient changes as well as multi-wave mixing processes. The observed strong THz-pump THz-probe signals provide insight into ultrafast dynamics and the spectral response of the low-energy carriers. Here we report the observation of a pump-induced transmission in graphite. The relaxation dynamics shows three distinct time scales, which are assigned to carrier thermalization, phonon emission and a slow cooling down back to equilibrium.

  14. 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.

  15. Ultrafast dynamics of ligand and substrate interaction in endothelial nitric oxide synthase under Soret excitation.

    Science.gov (United States)

    Hung, Chih-Chang; Yabushita, Atsushi; Kobayashi, Takayoshi; Chen, Pei-Feng; Liang, Keng S

    2016-01-01

    Ultrafast transient absorption spectroscopy of endothelial NOS oxygenase domain (eNOS-oxy) was performed to study dynamics of ligand or substrate interaction under Soret band excitation. Photo-excitation dissociates imidazole ligand in 4ps. The eNOS-oxy without additive is partially bound with water molecule, thus its photoexcited dynamics also shows ligand dissociation in <800fs. Then it followed by vibrational cooling coupled with charge transfer in 4.8ps, and recombination of ligand to distal side of heme in 12ps.

  16. Preface to Special Topic: Invited Papers of the 3rd International Conference on Ultrafast Structural Dynamics

    Directory of Open Access Journals (Sweden)

    S. L. Johnson

    2016-03-01

    Full Text Available The ability to visualize the real-time dynamics of atomic, magnetic, and electronic structure is widely recognized in many fields as a key element underpinning many important processes in chemistry, materials science, and biology. The need for an improved understanding of such processes becomes acute as energy conversion processes on fast time scales become increasingly relevant to problems in science and technology. This special issue, containing invited papers from participants at the 3rd International Conference on Ultrafast Structural Dynamics held June 10–12, 2015 in Zurich, Switzerland, discusses several recent developments in this area.

  17. Ultrafast dynamics of o-fluorophenol studied with femtosecond time-resolved photoelectron and photoion spectroscopy

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    The ultrafast dynamics of o-fluorophenol via the excited states has been studied by femtosecond time-resolved photoelectron imaging. The photoion and photoelectron spectra taken with a time delay between 267 nm pump laser and 800 nm probe laser provide a longer-lived S1 electronic state of about ns timescale. In comparison,the spectra obtained by exciting the S2 state with femtosecond laser pulses at 400 nm and ionizing with pulses at 800 nm suggest that the S2 state has an ultrashort lifetime about 102 fs and reflects the internal conversion dynamics of the S2 state to the S1 state.

  18. Robust transmission stabilization and dynamic switching in broadband hybrid waveguide systems with nonlinear gain and loss

    Science.gov (United States)

    Nguyen, Quan M.; Peleg, Avner; Tran, Thinh P.

    2015-01-01

    We develop a method for transmission stabilization and robust dynamic switching for colliding optical soliton sequences in broadband waveguide systems with nonlinear gain and loss. The method is based on employing hybrid waveguides, consisting of spans with linear gain and cubic loss, and spans with linear loss, cubic gain, and quintic loss. We show that the amplitude dynamics is described by a hybrid Lotka-Volterra (LV) model, and use the model to determine the physical parameter values required for enhanced transmission stabilization and switching. Numerical simulations with coupled nonlinear Schrödinger equations confirm the predictions of the LV model, and show complete suppression of radiative instability and pulse distortion. This enables stable transmission over distances larger by an order of magnitude compared with uniform waveguides with linear gain and cubic loss. Moreover, multiple on-off and off-on dynamic switching events are demonstrated over a wide range of soliton amplitudes, showing the superiority of hybrid waveguides compared with static switching in uniform waveguides.

  19. Wave-guided Optical Waveguides tracked and coupled using dynamic diffractive optics

    DEFF Research Database (Denmark)

    Glückstad, Jesper; Villangca, Mark Jayson; Bañas, Andrew Rafael

    With light’s miniscule momentum, shrinking robotics down to the micro- and nano-scale regime creates opportunities for exploiting optical forces and near-field light delivery in advanced actuation and control atthe smallest physical dimensions. Advancing light-driven nano- or micro-actuation requ......With light’s miniscule momentum, shrinking robotics down to the micro- and nano-scale regime creates opportunities for exploiting optical forces and near-field light delivery in advanced actuation and control atthe smallest physical dimensions. Advancing light-driven nano- or micro......-actuation requires the optimization of optical forces and optical torques that, in turn, requires the optimization of the underlying light-matter interaction [1]. We have previously proposed and demonstrated micro-targeted light-delivery and the opto-mechanical capabilities of so-called wave-guided optical...

  20. Ultrafast solvation dynamics explored by nonlinear optical spectroscopy

    NARCIS (Netherlands)

    Boeij, Wilhelmus Petrus de; Wiersma, D. A.

    1997-01-01

    Chemical reaction dynamics and chemical rate processes in the liquid phase are intimately connected to the specific interaction of the solvent on the reaction species. The strong coupling between the dissolved solute and the dynamical solvent causes fluctuations in the solute's energy levels. These

  1. Ultrafast dynamics in unaligned MWCNTs decorated with metal nanoparticles

    DEFF Research Database (Denmark)

    Manzoni, G.; Ponzoni, S.; Galimberti, G.

    2016-01-01

    The relaxation dynamics of unaligned multi-walled carbon nanotubes decorated with metallic nanoparticles have been studied by using transient optical measurements. The fast dynamics due to the short-lived free-charge carriers excited by the pump are not affected by the presence of nanoparticles...

  2. Ultrafast charge generation and relaxation dynamics in methylammonium lead bromide perovskites

    Science.gov (United States)

    Deng, Xiaofan; Wen, Xiaoming; Sheng, Rui; Huang, Shujuan; Harada, Takaaki; Kee, Tak W.; Green, Martin A.; Ho-Baillie, Anita

    2015-12-01

    Methylammonium Lead Bromide (CH3NH3PbBr3) is a promising material for tandem solar cell due to its high band gap. Ultrafast optical techniques on a time scale of femto- and picosecond are used to investigate the carrier dynamics in CH3NH3PbBr3. An ultrafast cooling of hot carriers occurs in sub-picoseconds in CH3NH3PbBr3 by phonon scattering. Two ultrafast relaxation processes are attributed to optical phonon scattering and acoustic phonon scattering. The relaxation processes are evidently slower when CH3NH3PbBr3 is in contact with compact TiO2 (c-TiO2) layer, suggesting better quality CH3NH3PbBr3. when deposited on c-TiO2. The nanosecond decay in CH3NH3PbBr3 film is ascribed to electron-hole recombination. With the presence of c-TiO2 layer, this process is accelerated due to electron transport across the CH3NH3PbBr3/ c-TiO2 interface.

  3. Ultrafast vapourization dynamics of laser-activated polymeric microcapsules

    Science.gov (United States)

    Lajoinie, Guillaume; Gelderblom, Erik; Chlon, Ceciel; Böhmer, Marcel; Steenbergen, Wiendelt; de Jong, Nico; Manohar, Srirang; Versluis, Michel

    2014-04-01

    Precision control of vapourization, both in space and time, has many potential applications; however, the physical mechanisms underlying controlled boiling are not well understood. The reason is the combined microscopic length scales and ultrashort timescales associated with the initiation and subsequent dynamical behaviour of the vapour bubbles formed. Here we study the nanoseconds vapour bubble dynamics of laser-heated single oil-filled microcapsules using coupled optical and acoustic detection. Pulsed laser excitation leads to vapour formation and collapse, and a simple physical model captures the observed radial dynamics and resulting acoustic pressures. Continuous wave laser excitation leads to a sequence of vapourization/condensation cycles, the result of absorbing microcapsule fragments moving in and out of the laser beam. A model incorporating thermal diffusion from the capsule shell into the oil core and surrounding water reveals the mechanisms behind the onset of vapourization. Excellent agreement is observed between the modelled dynamics and experiment.

  4. Ultrafast X-ray Studies of Structural Dynamics at SLAC

    Energy Technology Data Exchange (ETDEWEB)

    Gaffney, K.J.; Lindenberg, A.M.; /SLAC, SSRL; Larsson, J.; /Lund Inst. Tech.; Sokolowski-Tinten, K.; /Jena U. /Duisburg U.; Blome, C.; /DESY; Synnergren, O.; /Lund Inst.; Sheppard, J.; /Oxford U.; Reis, D.A.; /Michigan U.; Hastings, J.B.; /SLAC, SSRL

    2005-09-30

    The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements demonstrate that the initial stage of crystal disordering results from inertial motion on a laser softened potential energy surface. These inertial dynamics dominate for the first half picosecond following laser excitation, indicating that interatomic forces minimally influence atomic excursions from the equilibrium lattice positions, even for motions in excess of an {angstrom}. This also indicates that the atoms disorder initially without losing memory of their lattice reference.

  5. Ultrafast X-ray Studies of Structural Dynamics at SLAC

    Energy Technology Data Exchange (ETDEWEB)

    Gaffney, K.J.; Lindenberg, A.M.; /SLAC, SSRL; Larsson, J.; /Lund Inst. Tech.; Sokolowski-Tinten, K.; /Jena U. /Duisburg U.; Blome, C.; /DESY; Synnergren, O.; /Lund Inst.; Sheppard, J.; /Oxford U.; Reis, D.A.; /Michigan U.; Hastings, J.B.; /SLAC, SSRL

    2005-09-30

    The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements demonstrate that the initial stage of crystal disordering results from inertial motion on a laser softened potential energy surface. These inertial dynamics dominate for the first half picosecond following laser excitation, indicating that interatomic forces minimally influence atomic excursions from the equilibrium lattice positions, even for motions in excess of an {angstrom}. This also indicates that the atoms disorder initially without losing memory of their lattice reference.

  6. Ultrafast Relaxation Dynamics of Photo-excited Dirac Fermion in Three Dimensional Dirac Semimetal Cadmium Arsenide

    CERN Document Server

    Lu, Wei; Liu, Xuefeng; Lu, Hong; Li, Caizhen; Lai, Jiawei; Zhao, Chuan; Tian, Ye; Liao, Zhimin; Jia, Shuang; Sun, Dong

    2016-01-01

    Three dimensional (3D) Dirac semimetal exhibiting ultrahigh mobility has recently attracted enormous research interests as 3D analogues of graphene. From the prospects of future application toward electronic/optoelectronic devices with extreme performance, it is crucial to understand the relaxation dynamics of photo-excited carriers and their coupling with lattice. In this work, we report ultrafast transient reflection measurements of photo-excited carrier dynamics in cadmium arsenide (Cd3As2), which is among the most stable Dirac semimetals that have been confirmed experimentally. With low energy probe photon of 0.3 eV, photo-excited Dirac Fermions dynamics closing to Dirac point are probed. Through transient reflection measurements on bulk and nanoplate samples that have different doping intensities, and systematic probe wavelength, pump power and lattice temperature dependent measurements, the dynamical evolution of carrier distributions can be retrieved qualitatively using a two-temperature model. The pho...

  7. Towards imaging of ultrafast molecular dynamics using FELs

    NARCIS (Netherlands)

    Rouzee, A.; Johnsson, P.; Rading, L.; Siu, W.; Huismans, Y.; Duesterer, S.; Redlin, H.; Tavella, F.; Stojanovic, N.; Al-Shemmary, A.; Lepine, F.; Holland, D. M. P.; Schlathölter, Thomas; Hoekstra, R.; Fukuzawa, H.; Ueda, K.; Vrakking, M. J. J.; Hundertmark, A.

    2013-01-01

    The dissociation dynamics induced by a 100 fs, 400 nm laser pulse in a rotationally cold Br-2 sample was characterized by Coulomb explosion imaging (CEI) using a time-delayed extreme ultra-violet (XUV) FEL pulse, obtained from the Free electron LASer in Hamburg (FLASH). The momentum distribution of

  8. Ultrafast electronic dynamics in laser-excited crystalline bismuth

    Directory of Open Access Journals (Sweden)

    Chekalin S.

    2013-03-01

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

  9. Anharmonic Noninertial Lattice Dynamics during Ultrafast Nonthermal Melting of InSb

    Science.gov (United States)

    Zijlstra, Eeuwe S.; Walkenhorst, Jessica; Garcia, Martin E.

    2008-09-01

    We compute the potential energy surface of femtosecond-laser-excited InSb along the directions in which the crystal becomes soft. Using dynamical simulations the time dependence of the atomic coordinates is obtained. We find that at high excitation densities the anharmonicity of the potential energy surface becomes significant after ˜100fs. On the basis of our results we explain recent time-resolved x-ray diffraction experiments. We point out that an alternative model for ultrafast melting [A. M. Lindenberg , Science 308, 392 (2005)SCIEAS0036-807510.1126/science.1107996] is inconsistent with our calculations.

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

    CERN Document Server

    Li, Mu-Zi; Bian, Xue-Bin

    2016-01-01

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

  11. Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hyunyong; Borondics, Ferenc; Siegel, David A.; Zhou, Shuyun Y.; Martin, Michael C.; Lanzara, Alessandra; Kaindl, Robert A.

    2009-03-26

    We study the broadband optical conductivity and ultrafast carrier dynamics of epitaxial graphene in the few-layer limit. Equilibrium spectra of nominally buffer, monolayer, and multilayer graphene exhibit significant terahertz and near-infrared absorption, consistent with a model of intra- and interband transitions in a dense Dirac electron plasma. Non-equilibrium terahertz transmission changes after photoexcitation are shown to be dominated by excess hole carriers, with a 1.2-ps mono-exponential decay that refects the minority-carrier recombination time.

  12. 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.

  13. Terahertz study of ultrafast carrier dynamics in InGaN/GaN multiple quantum wells

    Science.gov (United States)

    Porte, H. P.; Turchinovich, D.; Cooke, D. G.; Jepsen, P. Uhd

    2009-11-01

    Ultrafast carrier dynamics in InGaN/GaN multiple quantum wells is measured by time-resolved terahertz spectroscopy. The built-in piezoelectric field is initially screened by photoexcited, polarized carriers, and is gradullay restored as the carriers recombine. We observe a nonexponential decay of the carrier density. Time-integrated photoluminescence spectra have shown a complete screening of the built-in piezoelectric field at high excitation fluences. We also observe that the terahertz conductivity spectra differs from simple Drude conductivity, describing the response of free carriers, and are well fitted by the Drude-Smith model.

  14. Terahertz study of ultrafast carrier dynamics in InGaN/GaN multiple quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Porte, H P; Turchinovich, D; Cooke, D G; Jepsen, P Uhd, E-mail: hpor@fotonik.dtu.d [DTU Fotonik, Department of Photonics Engineering, Technical University of Denmark, Oersteds Plads 343, DK 2800 Kongens Lyngby (Denmark)

    2009-11-15

    Ultrafast carrier dynamics in InGaN/GaN multiple quantum wells is measured by time-resolved terahertz spectroscopy. The built-in piezoelectric field is initially screened by photoexcited, polarized carriers, and is gradullay restored as the carriers recombine. We observe a nonexponential decay of the carrier density. Time-integrated photoluminescence spectra have shown a complete screening of the built-in piezoelectric field at high excitation fluences. We also observe that the terahertz conductivity spectra differs from simple Drude conductivity, describing the response of free carriers, and are well fitted by the Drude-Smith model.

  15. Waveguide transition with vacuum window for multiband dynamic nuclear polarization systems

    DEFF Research Database (Denmark)

    Rybalko, Oleksandr; Bowen, Sean; Zhurbenko, Vitaliy

    2016-01-01

    A low loss waveguide transition section and oversized microwave vacuum window covering several frequency bands (94 GHz, 140 GHz, 188 GHz) is presented. The transition is compact and was optimized for multiband Dynamic Nuclear Polarization (DNP) systems in a full-wave simulator. The window is more...

  16. Ultrafast dynamics in DNA base pairs following ultraviolet excitation.

    Science.gov (United States)

    Orr-Ewing, Andrew

    2015-03-01

    Photo-protective mechanisms in DNA are essential to maintain the integrity of the genetic code by preventing damage from absorption of solar ultraviolet (UV) radiation. We have used time-resolved infra-red (TRIR) spectroscopy to observe the dynamics of Watson-Crick nucleobase pairs following absorption of femtosecond UV laser pulses. The base pairs are prepared as nucleosides in solution, and photo-induced dynamics are probed in the carbonyl and N-H bond stretching regions using broadband IR pulses with picosecond time resolution. Results will be presented for the guanine-cytosine (G-C) base pair, contrasting the rapid recovery of ground-state products (the photo-protection pathway) with formation of other photoproducts which might represent photo-damage mechanisms. This work is a collaboration with the group of Prof F. Temps (Christian-Albrechts-Universitat zu Kiel). This research is supported by ERC Advanced Grant 290966 CAPRI.

  17. 4D scanning ultrafast electron microscopy: visualization of materials surface dynamics.

    Science.gov (United States)

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

    2011-05-25

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

  18. Ultrafast dynamics and anionic active states of the flavin cofactor in cryptochrome and photolyase.

    Science.gov (United States)

    Kao, Ya-Ting; Tan, Chuang; Song, Sang-Hun; Oztürk, Nuri; Li, Jiang; Wang, Lijuan; Sancar, Aziz; Zhong, Dongping

    2008-06-18

    We report here our systematic studies of the dynamics of four redox states of the flavin cofactor in both photolyases and insect type 1 cryptochromes. With femtosecond resolution, we observed ultrafast photoreduction of oxidized state flavin adenine dinucleotide (FAD) in subpicosecond and of neutral radical semiquinone (FADH(*)) in tens of picoseconds through intraprotein electron transfer mainly with a neighboring conserved tryptophan triad. Such ultrafast dynamics make these forms of flavin unlikely to be the functional states of the photolyase/cryptochrome family. In contrast, we find that upon excitation the anionic semiquinone (FAD(*-)) and hydroquinone (FADH(-)) have longer lifetimes that are compatible with high-efficiency intermolecular electron transfer reactions. In photolyases, the excited active state (FADH(-)*) has a long (nanosecond) lifetime optimal for DNA-repair function. In insect type 1 cryptochromes known to be blue-light photoreceptors the excited active form (FAD(*-)*) has complex deactivation dynamics on the time scale from a few to hundreds of picoseconds, which is believed to occur through conical intersection(s) with a flexible bending motion to modulate the functional channel. These unique properties of anionic flavins suggest a universal mechanism of electron transfer for the initial functional steps of the photolyase/cryptochrome blue-light photoreceptor family.

  19. Microstructure, morphology, and ultrafast dynamics of a novel edible microemulsion.

    Science.gov (United States)

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

    2012-06-05

    An edible microemulsion (ME) composed of Tween 80/butyl lactate/isopropyl myristate (IPM)/water has been formulated. Pseudoternary phase diagram of the system contains a large single isotropic region. The phase behavior of the system is also studied at low pH (2.6) and in 0.9% NaCl solution. Conductivity, viscosity, ultrasonic velocity, and compressibility studies find consistent results in the structural transition (from water-in-oil (w/o) to bicontinuous, and from bicontinuous to oil-in-water (o/w)) behavior of the ME. Dynamic light scattering studies reveal the size of the MEs. The absorption and steady state emission spectra of 4-(dicyanomethylene)-2-methyl-6-(p-dimethylamino-styryl)-4H-pyran (DCM) successfully probe the polarity of the ME at its solvation shell and shows the efficacy of hosting model drug molecules. The rotational anisotropy of the dye has been studied to ascertain the geometrical restriction of the probe molecule. Picosecond-resolved fluorescence spectroscopy applies well to study the relaxation dynamics of water in the solvation shell of the MEs. The study finds strong correlation in the relaxation dynamics of water with the structure of host assembly and offers an edible ME system which could act as a potential drug delivery system and nontoxic nanotemplate for other applications.

  20. Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+

    DEFF Research Database (Denmark)

    Biasin, Elisa; Brandt van Driel, Tim; Kjær, Kasper Skov;

    2016-01-01

    We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitat......We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows...

  1. Dynamic Tuning of Transmission Wavelength of MEMS-Based Ge Waveguides on a Si Beam

    Directory of Open Access Journals (Sweden)

    Masashi Hirase

    2016-03-01

    Full Text Available Three-dimensional structures of microelectro-mechanical systems (MEMS-based Ge waveguide on a Si beam were fabricated for dynamic tuning of the fundamental absorption edge of Ge by external stressing. The application of various amounts of external forces up to 1 GPa onto the Si beam shows clear red-shifts in the absorption edge of Ge waveguides on the Si beam by ~40 nm. This shift was reproduced by the deformation potential theory, considering that mode of propagation in the Ge waveguide. The wavelength tuning range obtained makes it possible to cover the whole C-band of optical communication, indicating it to be a promising approach to electro-absorption Ge modulators to get them to work with a broader wavelength range than previously reported.

  2. On Ultrafast Photoconductivity Dynamics and Crystallinity of Black Silicon

    DEFF Research Database (Denmark)

    Porte, Hendrik Pieter; Turchinovich, Dmitry; Persheyev, Saydulla;

    2013-01-01

    We investigate the carrier dynamics of thin films of black silicon, amorphous hydrogenated silicon which under laser annealing forms a microstructured surface with extremely high broadband optical absorption. We use Raman spectroscopy to determine the degree of crystallinity of the annealed...... surfaces, and investigate the dependence on crystallinity and fabrication method of the photoconductivity. Time-resolved THz spectroscopy is used to determine the evolution of the carrier scattering time and confinement of carriers on the picosecond time scale. We conclude that a fabrication method...... with high energy leading edge of the annealing laser results in black silicon with the largest photon-to-electron conversion efficiency, largest mobility, and longest carrier lifetime....

  3. Ultrafast Hydration Dynamics Probed by Tryptophan at Protein Surface and Protein-DNA Interface

    Science.gov (United States)

    Qin, Yangzhong

    As we all live in a special water planet Earth, the significance of water to life has been universally recognized. The reason why water is so important to life has intrigued many researchers. This dissertation will focus on the ultrafast dynamics of protein surface water and protein-DNA interfacial water which have direct importance to the protein structure and function. Using tryptophan as an intrinsic fluorescence probe, combined with site-directed mutagenesis and ultrafast fluorescence up-conversion spectroscopy, we can achieve single residue spatial resolution and femtosecond temporal resolution. We can also precisely determine the local hydration water dynamics by monitoring the Stokes shift of tryptophan one at a time. Previously, the protein surface hydration has been extensively studied by our group. In this thesis, we will provide more details on the methods we are using to extract the hydration dynamics, and also validate our methods from both experimental and theoretical perspectives. To further interrogate the interfacial water hydration dynamics relative to the protein surface hydration, we studied two DNA polymerases: DNA Polymerase IV (Dpo4) and DNA Polymerase Beta (Pol beta). Both proteins show typical surface hydration pattern with three distinct time components including: (i) the ultrafast sub-picosecond component reflects the bulk type water motion; (ii) a few picoseconds component shows the inner water relaxation mainly corresponding to the local libration and reorientation; (iii) the tens to hundred picoseconds component represents the water-protein coupled motion involving the whole water network reorganization. Dpo4, a loosely DNA binding protein, exhibits very flexible interfacial water which resembles its surface water yet with a significantly reduced ultrafast component. Such dynamic interfacial water not only maintains interfacial flexibility, but also contributes to the low fidelity of the protein. In contrast to the Dpo4, pol beta

  4. Ultrafast structural dynamics and isomerization in Rydberg-exited Quadricyclane

    Energy Technology Data Exchange (ETDEWEB)

    Rudakov, Fedor M [ORNL

    2012-01-01

    The quadricyclane - norbornadiene system is an important model for the isomerization dynamics between highly strained molecules. In a breakthrough observation for a polyatomic molecular system of that complexity, we follow the photoionization from Rydberg states in the time-domain to derive a measure for the time-dependent structural dynamics and the time-evolving structural dispersion even while the molecule is crossing electronic surfaces. The photoexcitation to the 3s and 3p Rydberg states deposits significant amounts of energy into vibrational motions. We observe the formation and evolution of the vibrational wavepacket on the Rydberg surface and the internal conversion from the 3p Rydberg states to the 3s state. In that state, quadricyclane isomerizes to norbornadiene with a time constant of {tau}{sub 2} = 136(45) fs. The lifetime of the 3p Rydberg state in quadricyclane is {tau}{sub 1} = 320(31) and the lifetime of the 3s Rydberg state in norbornadiene is {tau}{sub 3} = 394(32).

  5. Influence of ultrafast carrier dynamics on semiconductor absorption spectra

    CERN Document Server

    Ouerdane, H

    2001-01-01

    set of coupled rate equations. We obtained a good qualitative agreement with experiments and further insight into the interplay between the various dynamical processes by varying the phenomenological parameters entering the rate equations. In particular we found that the carrier spin-flip occurs on a relatively long time scale (several tens of picoseconds) compared to the carrier distributions relaxation and thermalization (a picosecond or less). We also could monitor the time evolution of the plasma density, energy, temperature and screening. In this thesis, we also studied the photoluminescence in II-VI quantum wells at room temperature. We built a mathematical model to account for Coulomb correlations that are expected to strongly influence the spontaneous emission rate in these materials. We assumed the 1s exciton-free electron scattering to be the main process leading an exciton to the photon line before recombination. The excitonic wavefunctions in a 2D screened Coulomb potential were calculated using t...

  6. Dynamic UltraFast 2D EXchange SpectroscopY (UF-EXSY) of hyperpolarized substrates

    Science.gov (United States)

    Leon Swisher, Christine; Koelsch, Bertram; Sukumar, Subramianam; Sriram, Renuka; Santos, Romelyn Delos; Wang, Zhen Jane; Kurhanewicz, John; Vigneron, Daniel; Larson, Peder

    2015-08-01

    In this work, we present a new ultrafast method for acquiring dynamic 2D EXchange SpectroscopY (EXSY) within a single acquisition. This technique reconstructs two-dimensional EXSY spectra from one-dimensional spectra based on the phase accrual during echo times. The Ultrafast-EXSY acquisition overcomes long acquisition times typically needed to acquire 2D NMR data by utilizing sparsity and phase dependence to dramatically undersample in the indirect time dimension. This allows for the acquisition of the 2D spectrum within a single shot. We have validated this method in simulations and hyperpolarized enzyme assay experiments separating the dehydration of pyruvate and lactate-to-pyruvate conversion. In a renal cell carcinoma cell (RCC) line, bidirectional exchange was observed. This new technique revealed decreased conversion of lactate-to-pyruvate with high expression of monocarboxylate transporter 4 (MCT4), known to correlate with aggressive cancer phenotypes. We also showed feasibility of this technique in vivo in a RCC model where bidirectional exchange was observed for pyruvate-lactate, pyruvate-alanine, and pyruvate-hydrate and were resolved in time. Broadly, the technique is well suited to investigate the dynamics of multiple exchange pathways and applicable to hyperpolarized substrates where chemical exchange has shown great promise across a range of disciplines.

  7. Valley Carrier Dynamics in Monolayer Molybdenum Disulphide from Helicity Resolved Ultrafast Pump-probe Spectroscopy

    CERN Document Server

    Wang, Qinsheng; Li, Xiao; Qiu, Jun; Ji, Yanxin; Feng, Ji; Sun, Dong

    2013-01-01

    We investigate the valley related carrier dynamics in monolayer MoS2 using helicity resolved non-degenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer MoS2 shows remarkable transient reflection signals, in stark contrast to bilayer and bulk MoS2 due to the enhancement of many-body effect at reduced dimensionality. The helicity resolved ultrafast time-resolved result shows that the valley polarization is preserved for only several ps before scattering process makes it undistinguishable. We suggest that the dynamical degradation of valley polarization is attributable primarily to the exciton trapping by defect states in the exfoliated MoS2 samples. Our experiment and a tight-binding model analysis also show that the perfect valley CD selectivity is fairly robust against disorder at the K point, but quickly decays from the high-symmetry point in the momentum space in the presence of disorder.

  8. Ultrafast intramolecular relaxation dynamics of Mg- and Zn-bacteriochlorophyll a

    Energy Technology Data Exchange (ETDEWEB)

    Kosumi, Daisuke [Osaka City University Advanced Research Institute for Natural Science and Technology, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Nakagawa, Katsunori; Sakai, Shunsuke [Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); Nagaoka, Yuya; Maruta, Satoshi; Sugisaki, Mitsuru [CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); Dewa, Takehisa [Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); PRESTO/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Nango, Mamoru [The Osaka City University Advanced Research Institute for Natural Science and Technology, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); Hashimoto, Hideki [The Osaka City University Advanced Research Institute for Natural Science and Technology, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan)

    2013-07-21

    Ultrafast excited-state dynamics of the photosynthetic pigment (Mg-)bacteriochlorophyll a and its Zn-substituted form were investigated by steady-state absorption/fluorescence and femtosecond pump-probe spectroscopic measurements. The obtained steady-state absorption and fluorescence spectra of bacteriochlorophyll a in solution showed that the central metal compound significantly affects the energy of the Q{sub x} state, but has almost no effect on the Q{sub y} state. Photo-induced absorption spectra were recorded upon excitation of Mg- and Zn-bacteriochlorophyll a into either their Q{sub x} or Q{sub y} state. By comparing the kinetic traces of transient absorption, ground-state beaching, and stimulated emission after excitation to the Q{sub x} or Q{sub y} state, we showed that the Q{sub x} state was substantially incorporated in the ultrafast excited-state dynamics of bacteriochlorophyll a. Based on these observations, the lifetime of the Q{sub x} state was determined to be 50 and 70 fs for Mg- and Zn-bacteriochlorophyll a, respectively, indicating that the lifetime was influenced by the central metal atom due to the change of the energy gap between the Q{sub x} and Q{sub y} states.

  9. Ultrafast fluxional exchange dynamics in electrolyte solvation sheath of lithium ion battery

    Science.gov (United States)

    Lee, Kyung-Koo; Park, Kwanghee; Lee, Hochan; Noh, Yohan; Kossowska, Dorota; Kwak, Kyungwon; Cho, Minhaeng

    2017-01-01

    Lithium cation is the charge carrier in lithium-ion battery. Electrolyte solution in lithium-ion battery is usually based on mixed solvents consisting of polar carbonates with different aliphatic chains. Despite various experimental evidences indicating that lithium ion forms a rigid and stable solvation sheath through electrostatic interactions with polar carbonates, both the lithium solvation structure and more importantly fluctuation dynamics and functional role of carbonate solvent molecules have not been fully elucidated yet with femtosecond vibrational spectroscopic methods. Here we investigate the ultrafast carbonate solvent exchange dynamics around lithium ions in electrolyte solutions with coherent two-dimensional infrared spectroscopy and find that the time constants of the formation and dissociation of lithium-ion···carbonate complex in solvation sheaths are on a picosecond timescale. We anticipate that such ultrafast microscopic fluxional processes in lithium-solvent complexes could provide an important clue to understanding macroscopic mobility of lithium cation in lithium-ion battery on a molecular level. PMID:28272396

  10. Applications of time-resolved terahertz spectroscopy in ultrafast carrier dynamics

    Institute of Scientific and Technical Information of China (English)

    Qingli Zhou; Xicheng Zhang

    2011-01-01

    1.Introduction Terahertz time-domain spectroscopy (THz-TDS)[1-3]is a powerful and coherent free-space technique in which nearly single-cycle electromagnetic pulse is generated and detected using femtosecond optical pulses.THz-TDS has been utilized as one of the important methods for material characterization in the past two decades.Because transmission or reflection of THz waves is sensitive to carrier density and mobility,an ultrafast THz-TDS system is required to provide time-resolved capability of material characterization in the THz region[4-6].In the past decade,one of the widely used time-resolved THz spectroscopy methods is optical-pump/THz probe (O/T)spectroscopy[3].%Three time-resolved terahertz (THz) spectroscopy methods (optical-pump/THz-probe spectroscopy, THz-pump/THz-probe spectroscopy, and THz-pump/optical-probe spectroscopy) are reviewed. These are used to characterize ultrafast dynamics in photo- or THz-excited semiconductors, superconductors, nanomateri-als, and other materials. In particular, the optical-pump/THz-probe spectroscopy is utilized to investigate carrier dynamics and the related intervalley scattering phenomena in semiconductors. The recent development of intense pulsed THz sources is expected to affect the research in nonlinear THz responses of various materials.

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

    Directory of Open Access Journals (Sweden)

    Nibbering Erik T. J.

    2013-03-01

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

  12. Ultrafast curve crossing dynamics through conical intersections in methylated cyclopentadienes.

    Science.gov (United States)

    Rudakov, Fedor; Weber, Peter M

    2010-04-08

    We explored the curve crossing dynamics of 1,2,3,4-tetramethyl-cyclopentadiene (TMCPD) and 1,2,3,4,5-pentamethyl-cyclopentadiene (PMCPD) upon pi --> pi* excitation to the 1B(2) state using time-resolved, resonance-enhanced multiphoton ionization mass and photoelectron spectroscopy. Upon excitation with a femtosecond laser pulse at 267 nm, the energy relaxation pathway is observed by a time-delayed probe pulse at 400 nm, which ionizes the molecule through Rydberg states that reveal the momentary state of the molecule in the photoelectron spectra. We observe that the initially populated 1B(2) state decays to the 2A(1) surface in 135 fs in TMCPD and 183 fs in PMCPD, followed by a crossing to the ground state 1A(1) surface on 57 and 60 fs time scales for TMCPD and PMCPD, respectively. The spectroscopic signatures of the 2A(1) states are clearly revealed in the two-photon ionization photoelectron spectra. In both systems we observe that the ground states are recovered completely, indicating that no new molecular structures are created on the time scale of the experiment.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1998-10-01

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

  14. Dynamics of quantum correlation between separated nitrogen-vacancy centers embedded in plasmonic waveguide

    Science.gov (United States)

    Yang, Wan-Li; An, Jun-Hong; Zhang, Cheng-Jie; Chen, Chang-Yong; Oh, C. H.

    2015-10-01

    We investigate the dynamics of quantum correlation between two separated nitrogen vacancy centers (NVCs) placed near a one-dimensional plasmonic waveguide. As a common medium of the radiation field of NVCs propagating, the plasmonic waveguide can dynamically induce quantum correlation between the two NVCs. It is interesting to find that such dynamically induced quantum correlation can be preserved in the long-time steady state by locally applying individual driving on the two NVCs. In particular, we also show that a large degree of quantum correlation can be established by this scheme even when the distance between the NVCs is much larger than their operating wavelength. This feature may open new perspectives for devising active decoherence-immune solid-state optical devices and long-distance NVC-based quantum networks in the context of plasmonic quantum electrodynamics.

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

    CERN Document Server

    Timmers, Henry; Sandhu, Arvinder

    2012-01-01

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

  16. Optically Induced Lattice Dynamics of hexagonal manganite using Ultrafast X-ray Diffraction

    Science.gov (United States)

    Lee, Hae Ja; Workman, J. B.; Hur, N.

    2005-03-01

    We have studied the picosecond lattice dynamics of optically pumped hexagonal manganite LuMnO3 using ultrafast x-ray diffraction. The results show a shift and broadening of the diffraction curve due to the stimulated lattice expansion. To understand the transient response of the lattice, the measured time- and angle-resolved diffraction curves are compared with a theoretical calculation based on dynamical diffraction theory modified for the hexagonal crystal structure of LuMnO3. Our simulations reveal that a large coupling coefficient between the a-b plane and the c-axis (c13) is required to the data. We compare this result to our previous coherent phonon studies of LuMnO3 using optical pump-probe spectroscopy.

  17. Ultrafast dynamics of type-II GaSb/GaAs quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Komolibus, K.; Piwonski, T.; Gradkowski, K. [Centre for Advanced Photonics and Process Analysis, Cork Institute of Technology, Cork (Ireland); Tyndall National Institute, University College Cork, Lee Maltings, Cork (Ireland); Reyner, C. J.; Liang, B.; Huffaker, D. L. [Department of Electrical Engineering and California NanoSystems Institute, University of California - Los Angeles, Los Angeles, California 90095 (United States); Huyet, G. [Centre for Advanced Photonics and Process Analysis, Cork Institute of Technology, Cork (Ireland); Tyndall National Institute, University College Cork, Lee Maltings, Cork (Ireland); National Research University of Information Technologies, Mechanics and Optics, Saint Petersburg (Russian Federation); Houlihan, J. [School of Science, Waterford Institute of Technology, Waterford (Ireland)

    2015-01-19

    In this paper, room temperature two-colour pump-probe spectroscopy is employed to study ultrafast carrier dynamics in type-II GaSb/GaAs quantum dots. Our results demonstrate a strong dependency of carrier capture/escape processes on applied reverse bias voltage, probing wavelength and number of injected carriers. The extracted timescales as a function of both forward and reverse bias may provide important information for the design of efficient solar cells and quantum dot memories based on this material. The first few picoseconds of the dynamics reveal a complex behaviour with an interesting feature, which does not appear in devices based on type-I materials, and hence is linked to the unique carrier capture/escape processes possible in type-II structures.

  18. Ultrafast dynamics in blends of π-conjugated polymers/fullerenes

    Science.gov (United States)

    Singh, Sanjeev; Tong, Minghong; Sheng, Chuanxiang; Vardeny, Zeev

    2008-03-01

    We have studied the ultrafast dynamics of photogenerated charges and excitons in a variety of π-conjugated polymer/fullerene blends using the transient pump-probe photomodulation (PM) spectroscopy with ˜ 100 fs resolution. These composites serve as active layers in organic photovoltaic devices with high power conversion quantum yield, due to the existence of a photoinduced charge transfer (PCT) reaction between the polymer and the fullerene molecules. Our transient PM spectrum spans a broad energy range from 0.1-2.4 eV, and this allows us to monitor the transient behavior of the various photoinduced absorption (PA) bands of polarons and excitons in the PM spectrum; as well as the transient exciton stimulated emission, and photobleaching (PB) of the ground state. The PB dynamics reflect the ground state recovery; hence, it can be used to determine the long-lived polaron photogeneration quantum efficiency in these systems.

  19. Nanoparticle monolayer-based flexible strain gauge with ultrafast dynamic response for acoustic vibration detection

    Institute of Scientific and Technical Information of China (English)

    Lizhi Yi[1; Weihong Jiao[1; Ke Wu[1; Lihua Qian[1; Xunxing Yu[2; Qi Xia[2; Kuanmin Mao[2; Songliu Yuan[1; Shuai Wang[3; Yingtao Jiang[4

    2015-01-01

    The relatively poor dynamic response of current flexible strain gauges has prevented their wide adoption in portable electronics. In this work, we present a greatly improved flexible strain gauge, where one strip of Au nanoparticle (NP) monolayer assembled on a polyethylene terephthalate film is utilized as the active unit. The proposed flexible gauge is capable of responding to applied stimuli without detectable hysteresis via electron tunneling between adjacent nanoparticles within the Au NP monolayer. Based on experimental quantification of the time and frequency domain dependence of the electrical resistance of the proposed strain gauge, acoustic vibrations in the frequency range of 1 to 20,000 Hz could be reliably detected. In addition to being used to measure musical tone, audible speech, and creature vocalization, as demonstrated in this study, the ultrafast dynamic response of this flexible strain gauge can be used in a wide range of applications, including miniaturized vibratory sensors, safe entrance guard management systems, and ultrasensitive pressure sensors.

  20. Real-time ultrafast dynamics of dense, hot matter measured by pump-probe Doppler spectrometry

    Science.gov (United States)

    Lad, Amit D.; Mondal, S.; Narayanan, V.; Ahmed, Saima; Rajeev, P. P.; Robinson, A. P. L.; Pasley, J.; Kumar, G. Ravindra

    2010-08-01

    A detailed understanding of the critical surface motion of high intensity laser produced plasma is very crucial for understanding the interaction. We employ the two colour pump-probe technique to report the first ever femtosecond scale ultrafast dynamics measurement of the critical surface of a solid plasma produced by a relativistically intense, femtosecond pump laser beam (1018 W/cm2, 30 fs, 800 nm) on an aluminium target. We observe the Doppler shift of a time delayed probe laser beam (1012 W/cm2, 80 fs, 400 nm) up to delays of 30 ps. Such unravelling of dynamics has not been possible in earlier measurements, which typically used the self reflection of a powerful pump pulse. We observe time dependent red and blue shifts and measure their magnitudes to infer plasma expansion velocity and acceleration and thereby the plasma profile. Our results are very well reproduced by 1D hydrodynamic simulation (HYADES code).

  1. A Novel Approach to Contrast-Enhanced Breast Magnetic Resonance Imaging for Screening: High-Resolution Ultrafast Dynamic Imaging

    NARCIS (Netherlands)

    Mann, R.M.; Mus, R.D.M.; Zelst, J. van; Geppert, C.; Karssemeijer, N.; Platel, B.

    2014-01-01

    The use of breast magnetic resonance imaging (MRI) as screening tool has been stalled by high examination costs. Scan protocols have lengthened to optimize specificity. Modern view-sharing sequences now enable ultrafast dynamic whole-breast MRI, allowing much shorter and more cost-effective procedur

  2. Ultrafast conductivity dynamics in optically excited InGaN/GaN multiple quantum wells, observed by transient THz spectroscopy

    DEFF Research Database (Denmark)

    Turchinovich, Dmitry; Porte, Henrik; Cooke, David

    2010-01-01

    We investigate ultrafast carrier dynamics in photoexcited InGaN/GaN multiple quantum wells by time-resolved terahertz spectroscopy. The initially very strong built-in piezoelectric field is screened upon photoexcitation by the polarized carriers, and is gradually restored as the carriers recombine...

  3. Ultrafast conductivity dynamics in optically excited InGaN/GaN multiple quantum wells, observed by transient THz spectroscopy

    DEFF Research Database (Denmark)

    Turchinovich, Dmitry; Porte, Henrik; Cooke, David

    2010-01-01

    We investigate ultrafast carrier dynamics in photoexcited InGaN/GaN multiple quantum wells by time-resolved terahertz spectroscopy. The initially very strong built-in piezoelectric field is screened upon photoexcitation by the polarized carriers, and is gradually restored as the carriers recombine...

  4. Ultrafast interfacial charge transfer dynamics in dye-sensitized and quantum dot solar cell

    Science.gov (United States)

    Ghosh, Hirendra N.

    2013-02-01

    Dye sensitized solar cell (DSSC) appeared to be one of the good discovery for the solution of energy problem. We have been involved in studying ultrafast interfacial electron transfer dynamics in DSSC using femtosecond laser spectroscopy. However it has been realized that it is very difficult to design and develop higher efficient one, due to thermodynamic limitation. Again in DSSC most of the absorbed photon energy is lost as heat within the cell, which apart from decreasing the efficiency also destabilizes the device. It has been realized that quantum dot solar cell (QDSC) are the best bet where the sensitizer dye molecules can be replaced by suitable quantum dot (QD) materials in solar cell. The quantum-confinement effect in semiconductors modifies their electronic structure, which is a very important aspect of these materials. For photovoltaic applications, a long-lived charge separation remains one of the most essential criteria. One of the problems in using QDs for photovoltaic applications is their fast charge recombination caused by nonradiative Auger processes, which occur predominantly at lower particle sizes due to an increase in the Coulomb interaction between electrons and holes. Various approaches, such as the use of metal-semiconductor composites, semiconductor-polymer composite, and semiconductor core-shell heterostructures, have been attempted to minimize the fast recombination between electrons and holes. To make higher efficient solar devices it has been realised that it is very important to understand charge carrier and electron transfer dynamics in QD and QD sensitized semiconductor nanostructured materials. In the present talk, we are going to discuss on recent works on ultrafast electron transfer dynamics in dye-sensitized TiO2 nanoparticles/film [1-12] and charge (electron/hole) transfer dynamics in quantum dot core-shell nano-structured materials [13-17].

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

    Science.gov (United States)

    Timmers, Henry Robert

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

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

    Science.gov (United States)

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

    2017-08-24

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

  7. Multidiagnostics analysis of ion dynamics in ultrafast laser ablation of metals over a large fluence range

    Energy Technology Data Exchange (ETDEWEB)

    Anoop, K. K.; Polek, M. P.; Bruzzese, R.; Amoruso, S.; Harilal, Sivanandan S.

    2015-02-28

    The ions dynamics in ultrafast laser ablation of metals is studied over a fluence range spanning from the ablation threshold up to ~75 J/cm2 by means of three established diagnostic techniques. Langmuir probe, Faraday cup and spectrally resolved ICCD imaging simultaneously monitor the laser-produced plasma ions produced during ultrafast laser ablation of a copper target. The fluence dependence of ion yield is analyzed observing the occurrence of three different regimes. Moreover, the specific ion yield shows a maximum at about 4-5 J/cm2, followed by a gradual reduction and a transition to a high-fluence regime above ~50 J/cm2. The fluence variation of the copper ions angular distribution is also analyzed, observing a gradual increase of forward peaking of Cu ions for fluences up to ~10 J/cm2. Then, a broader ion component is observed at larger angles for fluences larger than ~10 J/cm2. Finally, an experimental characterization of the ions angular distribution for several metallic targets (Mg, Al, Cr, Fe, Cu, and W) is carried out at a relatively high fluence of ~66 J/cm2. Interestingly, the ion emission from the volatile metals show a narrow forward peaked distribution and a high peak ion yield compared to the refractory metals. Moreover, the width of ion angular distributions presents a striking correlation with the peak ion yield.

  8. Transmission stability and Raman-induced amplitude dynamics in multichannel soliton-based optical waveguide systems

    Science.gov (United States)

    Peleg, Avner; Nguyen, Quan M.; Tran, Thinh P.

    2016-12-01

    We study transmission stability and dynamics of pulse amplitudes in N-channel soliton-based optical waveguide systems, taking into account second-order dispersion, Kerr nonlinearity, delayed Raman response, and frequency dependent linear gain-loss. We carry out numerical simulations with systems of N coupled nonlinear Schrödinger (NLS) equations and compare the results with the predictions of a simplified predator-prey model for Raman-induced amplitude dynamics. Coupled-NLS simulations for single-fiber transmission with 2 ≤ N ≤ 4 frequency channels show stable oscillatory dynamics of soliton amplitudes at short-to-intermediate distances, in excellent agreement with the predator-prey model's predictions. However, at larger distances, we observe transmission destabilization due to resonant formation of radiative sidebands, which is caused by Kerr nonlinearity. The presence of linear gain-loss in a single fiber leads to a limited increase in transmission stability. Significantly stronger enhancement of transmission stability is achieved in a nonlinear N-waveguide coupler due to efficient suppression of radiative sideband generation by the linear gain-loss. As a result, the distances along which stable Raman-induced dynamics of soliton amplitudes is observed are significantly larger in the waveguide coupler system compared with the single-fiber system.

  9. A Non-Hermitian Approach to Non-Linear Switching Dynamics in Coupled Cavity-Waveguide Systems

    DEFF Research Database (Denmark)

    Heuck, Mikkel; Kristensen, Philip Trøst; Mørk, Jesper

    2012-01-01

    We present a non-Hermitian perturbation theory employing quasi-normal modes to investigate non-linear all-optical switching dynamics in a photonic crystal coupled cavity-waveguide system and compare with finite-difference-time-domain simulations.......We present a non-Hermitian perturbation theory employing quasi-normal modes to investigate non-linear all-optical switching dynamics in a photonic crystal coupled cavity-waveguide system and compare with finite-difference-time-domain simulations....

  10. Short pulse absorption dynamics in a p-i-n InGaAsP MQW waveguide saturable absorber

    DEFF Research Database (Denmark)

    Romstad, Francis Pascal; Öhman, Filip; Mørk, Jesper

    2002-01-01

    The saturation properties and absorption dynamics of an InGaAsP MQW waveguide saturable absorber is measured using short 200-fs and 1-ps pulses. The dependence on the pulse energy and reverse bias is characterized.......The saturation properties and absorption dynamics of an InGaAsP MQW waveguide saturable absorber is measured using short 200-fs and 1-ps pulses. The dependence on the pulse energy and reverse bias is characterized....

  11. Beyond structure: ultrafast X-ray absorption spectroscopy as a probe of non-adiabatic wavepacket dynamics.

    Science.gov (United States)

    Neville, Simon P; Averbukh, Vitali; Patchkovskii, Serguei; Ruberti, Marco; Yun, Renjie; Chergui, Majed; Stolow, Albert; Schuurman, Michael S

    2016-12-16

    The excited state non-adiabatic dynamics of polyatomic molecules, leading to the coupling of structural and electronic dynamics, is a fundamentally important yet challenging problem for both experiment and theory. Ongoing developments in ultrafast extreme vacuum ultraviolet (XUV) and soft X-ray sources present new probes of coupled electronic-structural dynamics because of their novel and desirable characteristics. As one example, inner-shell spectroscopy offers localized, atom-specific probes of evolving electronic structure and bonding (via chemical shifts). In this work, we present the first on-the-fly ultrafast X-ray time-resolved absorption spectrum simulations of excited state wavepacket dynamics: photo-excited ethylene. This was achieved by coupling the ab initio multiple spawning (AIMS) method, employing on-the-fly dynamics simulations, with high-level algebraic diagrammatic construction (ADC) X-ray absorption cross-section calculations. Using the excited state dynamics of ethylene as a test case, we assessed the ability of X-ray absorption spectroscopy to project out the electronic character of complex wavepacket dynamics, and evaluated the sensitivity of the calculated spectra to large amplitude nuclear motion. In particular, we demonstrate the pronounced sensitivity of the pre-edge region of the X-ray absorption spectrum to the electronic and structural evolution of the excited-state wavepacket. We conclude that ultrafast time-resolved X-ray absorption spectroscopy may become a powerful tool in the interrogation of excited state non-adiabatic molecular dynamics.

  12. Water-anion hydrogen bonding dynamics: Ultrafast IR experiments and simulations

    Science.gov (United States)

    Yamada, Steven A.; Thompson, Ward H.; Fayer, Michael D.

    2017-06-01

    Many of water's remarkable properties arise from its tendency to form an intricate and robust hydrogen bond network. Understanding the dynamics that govern this network is fundamental to elucidating the behavior of pure water and water in biological and physical systems. In ultrafast nonlinear infrared experiments, the accessible time scales are limited by water's rapid vibrational relaxation (1.8 ps for dilute HOD in H2O), precluding interrogation of slow hydrogen bond evolution in non-bulk systems. Here, hydrogen bonding dynamics in bulk D2O were studied from the perspective of the much longer lived (36.2 ps) CN stretch mode of selenocyanate (SeCN-) using polarization selective pump-probe (PSPP) experiments, two-dimensional infrared (2D IR) vibrational echo spectroscopy, and molecular dynamics simulations. The simulations make use of the empirical frequency mapping approach, applied to SeCN- for the first time. The PSPP experiments and simulations show that the orientational correlation function decays via fast (2.0 ps) restricted angular diffusion (wobbling-in-a-cone) and complete orientational diffusive randomization (4.5 ps). Spectral diffusion, quantified in terms of the frequency-frequency correlation function, occurs on two time scales. The initial 0.6 ps time scale is attributed to small length and angle fluctuations of the hydrogen bonds between water and SeCN-. The second 1.4 ps measured time scale, identical to that for HOD in bulk D2O, reports on the collective reorganization of the water hydrogen bond network around the anion. The experiments and simulations provide details of the anion-water hydrogen bonding and demonstrate that SeCN- is a reliable vibrational probe of the ultrafast spectroscopy of water.

  13. Theoretical realization of dynamically tunable double plasmonically induced transparency in a graphene-based waveguide structure

    Science.gov (United States)

    Zhang, Zhengren; Fan, Yuancheng; Long, Yang; Yin, Pengfei

    2017-10-01

    A graphene-based waveguide coupled with radiative and subradiant graphene ribbon resonators is proposed to represent the four-level energy diagram in conventional atomic systems and demonstrate a new realization of dynamically tunable double plasmonically induced transparency (DPIT). The radiative resonator is achieved with the help of direct coupling from the graphene waveguide while indirect coupling is relied for the subradiant resonator. By combining the numerical simulation results and the dressed theory, the physical mechanism behind the DPIT is presented in detail. The DPIT phenomenon is derived from the mode splitting caused by the phase-coupled effects. By controlling the Fermi energy level of graphene ribbon, the double transparency windows can be dynamically tuned. The proposed structure may find its application in optical communication or other novel terahertz integrated optical circuits and devices.

  14. Ultrafast vortex core dynamics investigated by finite-element micromagnetic simulations

    Energy Technology Data Exchange (ETDEWEB)

    Gliga, Sebastian

    2010-07-01

    The investigations carried out in this thesis concern the ultrafast dynamics of a fundamental micromagnetic configuration: the vortex. Over the past decade, a detailed understanding of the dynamic and static properties of such magnetic nanostructures has been achieved as a result of close interplay between experiments, theory and numeric simulations. Here, micromagnetic simulations were performed based on the finite-element method. The vortex structure arises in laterally-confined ferromagnets, in particular in thin-film elements, and is characterized by an in-plane curling of the magnetic moments around a very stable and narrow core. In the present study, a novel process in micromagnetism was found: the ultrafast reversal of the vortex core. The possibility of easily switching the core orientation by means of short in-plane field pulses is surprising in view of the very high stability of the core. Moreover, the simulations presented here showed that this reversal process unfolds on a time scale of only a few tens of picoseconds, which leads to the prediction of the fastest and most complex micromagnetic reversal process known to date. Indeed, the vortex core is not merely switched: it is destroyed and recreated in the immediate vicinity with an opposite direction. This is mediated by a rapid sequence of vortex-antivortex pair creation and annihilation subprocesses and results in a sudden burst-like emission of spin waves. Equally fascinating is the ultrafast dynamics of an isolated magnetic antivortex, the topological counterpart of the vortex. The simulations performed here showed that the static complementarity between vortices and antivortices is equally reflected in their ultrafast dynamics, which leads to the reversal of the antivortex core. A promising means for the control of the magnetization on the nanoscale consists in exploiting the spin-transfer torque effect. The study of the current-induced dynamics of vortices showed that the core reversal can be

  15. Femtosecond dynamics of the nonlinear index near the band edge in AlGaAs waveguides

    Science.gov (United States)

    Anderson, K. K.; LaGasse, M. J.; Wang, C. A.; Fujimoto, J. G.; Haus, H. A.

    1990-05-01

    The transient behavior of the nonresonant nonlinear index is investigated in AlGaAs waveguides with femtosecond time resolution. Both the refractive index and the absorption changes are measured by time division interferometry and pump probe techniques. Different mechanisms which contribute to the nonlinear index are distinguished by examining their dynamics, including the optical Stark effect, resonantly excited carriers, and two-photon absorption processes. The relative contribution from each mechanism is a strong function of wavelength near the band edge.

  16. Dynamical manipulation of Cosine-Gauss beams in a graphene plasmonic waveguide.

    Science.gov (United States)

    He, Xueqing; Ning, Tigang; Li, Rujiang; Pei, Li; Zheng, Jingjing; Li, Jing

    2017-06-12

    In this paper, we theoretically propose for the first time that graphene monolayer can be used to manipulate the Cosine-Gauss beams (CGBs). We show that both the transverse oscillation period and propagation length of a CGB can be dynamically manipulated by utilizing the tunability of the graphene's chemical potential. The graphene-based planar plasmonic waveguide provides a good platform to investigate the propagation properties of CGBs, which is potentially compatible to the microelectronic technology.

  17. Orbital-specific mapping of chemical dynamics with ultrafast x-rays

    Science.gov (United States)

    Wernet, Philippe

    Charge and spin density changes at the metal sites of transition-metal complexes and in metalloproteins determine reactivity and selectivity. To understand their function and to optimize complexes for photocatalytic applications the changes of charge and spin densities need to be mapped and ultimately controlled. I will discuss how time-resolved soft x-ray spectroscopy enables a fundamental understanding of local atomic and intermolecular interactions and their dynamics on atomic length and time scales of Ångströms and femtoseconds. The approach consists in using time-resolved, atom- and orbital-specific x-ray spectroscopy and quantum chemical theory to map the frontier-orbital interactions and their evolution in real time of ultrafast chemical transformations. We recently used femtosecond resonant inelastic x-ray scattering (RIXS, the x-ray analog of resonant Raman scattering) at the x-ray free-electron laser LINAC Coherent Light Source (LCLS, Stanford, USA) to probe the reaction dynamics of a transition-metal complex in solution on the femtosecond time scale. Spin crossover and ligation are found to define the excited-state dynamics. It is demonstrated how correlating orbital symmetry and orbital interactions with spin multiplicity allows for determining the reactivity of short-lived reaction intermediates. I will discuss how this complements approaches that probe structural dynamics and how it can be extended to map the local chemical interactions and their dynamical evolution in metalloproteins.

  18. Encrypted Three-dimensional Dynamic Imaging using Snapshot Time-of-flight Compressed Ultrafast Photography.

    Science.gov (United States)

    Liang, Jinyang; Gao, Liang; Hai, Pengfei; Li, Chiye; Wang, Lihong V

    2015-10-27

    Compressed ultrafast photography (CUP), a computational imaging technique, is synchronized with short-pulsed laser illumination to enable dynamic three-dimensional (3D) imaging. By leveraging the time-of-flight (ToF) information of pulsed light backscattered by the object, ToF-CUP can reconstruct a volumetric image from a single camera snapshot. In addition, the approach unites the encryption of depth data with the compressed acquisition of 3D data in a single snapshot measurement, thereby allowing efficient and secure data storage and transmission. We demonstrated high-speed 3D videography of moving objects at up to 75 volumes per second. The ToF-CUP camera was applied to track the 3D position of a live comet goldfish. We have also imaged a moving object obscured by a scattering medium.

  19. Ultrafast dynamics of the lowest-lying neutral states in carbon dioxide

    Science.gov (United States)

    Wright, Travis W.; Champenois, Elio G.; Cryan, James P.; Shivaram, Niranjan; Yang, Chan-Shan; Belkacem, Ali

    2017-02-01

    We present a study of the ultrafast dissociation dynamics of the lowest-lying electronic excited states in CO2 by using ultraviolet (UV) and extreme-ultraviolet (XUV) pulses from high-order harmonic generation. We observe two primary dissociation channels: a direct dissociation channel along the Π1g electronically excited manifold, and a second channel which results from the mixing of electronic states. The direct dissociation channel is found to have a lifetime which is shorter than our experimental resolution, whereas the second channel has a significantly longer lifetime of nearly 200 fs. In this long-lived channel we observe a beating of the vibrational populations with a period of ˜133 fs.

  20. Structural dynamics inside a functionalized metal–organic framework probed by ultrafast 2D IR spectroscopy

    Science.gov (United States)

    Nishida, Jun; Tamimi, Amr; Fei, Honghan; Pullen, Sonja; Ott, Sascha; Cohen, Seth M.; Fayer, Michael D.

    2014-01-01

    The structural elasticity of metal–organic frameworks (MOFs) is a key property for their functionality. Here, we show that 2D IR spectroscopy with pulse-shaping techniques can probe the ultrafast structural fluctuations of MOFs. 2D IR data, obtained from a vibrational probe attached to the linkers of UiO-66 MOF in low concentration, revealed that the structural fluctuations have time constants of 7 and 670 ps with no solvent. Filling the MOF pores with dimethylformamide (DMF) slows the structural fluctuations by reducing the ability of the MOF to undergo deformations, and the dynamics of the DMF molecules are also greatly restricted. Methodology advances were required to remove the severe light scattering caused by the macroscopic-sized MOF particles, eliminate interfering oscillatory components from the 2D IR data, and address Förster vibrational excitation transfer. PMID:25512539

  1. Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface

    Science.gov (United States)

    Caviglia, Andrea

    Static strain in complex oxide heterostructures has been extensively used to engineer electronic and magnetic properties at equilibrium. In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically. Here, by exciting large-amplitude infrared-active vibrations in a LaAlO3 substrate we induce magnetic order melting in a NdNiO3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion. Light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism.

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

    Science.gov (United States)

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

    2016-01-25

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

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

    Science.gov (United States)

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

    2016-08-18

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

  4. BEAM DYNAMICS ANALYSIS FOR THE ULTRA-FAST KICKER IN CIRCULAR COOLER RING OF JLEIC

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Yulu [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Inst. Modern Phys., Chinese Academy of Sciences, Lanzhou, China; Wang, Haipeng [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Rimmer, Robert A. [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Wang, Shaoheng [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States)

    2016-05-01

    An ultra-fast kicker system consisting of four quarter wavelength resonator based deflecting cavities was developed that simultaneously resonates at 10 subharmonic modes of the 476.3MHz bunch repetition frequency. Thus every 10th bunch in the bunch train will experience a transverse kick while all the other bunches are undisturbed. This fast kicker is being developed for the Energy Recovery Linac (ERL) based electron Circular Cooler Ring (CCR) in the proposed Jefferson Lab Electron Ion Collider (JLEIC, previously MEIC). The electron bunches can be reused 10-30 turns thus the beam current in the ERL can be reduced to 1/10 - 1/30 (150mA - 50mA) of the cooling bunch current (1.5A). In this paper, several methods to synthesize such a kicker waveform and the comparison made by the beam dynamics tracking in Elegant will be discussed.

  5. Study on the ultrafast dynamics of o-xylene cation by combined fs-photoelectron imaging-photofragmentation spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Yuzhu, E-mail: yuzhu.liu@psi.ch; Radi, Peter; Gerber, Thomas; Knopp, Gregor, E-mail: gregor.knopp@psi.ch

    2014-10-17

    Highlights: • Photoelectron imaging and photofragment spectroscopy are combined. • Photoelectron imaging has been measured to characterize the prepared cation states. • Ultrafast signal decay with time constant of 734 (±61) fs has been observed. - Abstract: Ultrafast dynamics of o-xylene cation has been studied by time resolved fs-photofragmentation (PF) spectroscopy in combination with photoelectron imaging (PEI). In the experiment, multiphoton ionization is used to prepare the o-xylene cation characterized by PEI. The ultrafast dynamics of o-xylene ions are measured by monitoring the time dependent parent-ion depletion and the fragment-ion formation, simultaneously. An ultrafast relaxation time of the parent ion of 734 (±61) fs has been observed. The PEI-PF measurements support the interpretation of this relaxation channel to a combination of internal conversion between the two ionic states (D{sub 0} and D{sub 1}) and intramolecular vibrational-energy redistribution process within the D{sub 0} state.

  6. A novel approach to contrast-enhanced breast magnetic resonance imaging for screening: high-resolution ultrafast dynamic imaging.

    Science.gov (United States)

    Mann, Ritse M; Mus, Roel D; van Zelst, Jan; Geppert, Christian; Karssemeijer, Nico; Platel, Bram

    2014-09-01

    The use of breast magnetic resonance imaging (MRI) as screening tool has been stalled by high examination costs. Scan protocols have lengthened to optimize specificity. Modern view-sharing sequences now enable ultrafast dynamic whole-breast MRI, allowing much shorter and more cost-effective procedures. This study evaluates whether dynamic information from ultrafast breast MRI can be used to replace standard dynamic information to preserve accuracy. We interleaved 20 ultrafast time-resolved angiography with stochastic trajectory (TWIST) acquisitions (0.9 × 1 × 2.5 mm, temporal resolution, 4.3 seconds) during contrast inflow in a regular high-resolution dynamic MRI protocol. A total of 160 consecutive patients with 199 enhancing abnormalities (95 benign and 104 malignant) were included. The maximum slope of the relative enhancement versus time curve (MS) obtained from the TWIST and curve type obtained from the regular dynamic sequence as defined in the breast imaging reporting and data system (BIRADS) lexicon were recorded. Diagnostic performance was compared using receiver operating characteristic analysis. All lesions were visible on both the TWIST and standard series. Maximum slope allows discrimination between benign and malignant disease with high accuracy (area under the curve, 0.829). Types of MS were defined in analogy to BIRADS curve types: MS type 3 implies a high risk of malignancy (MS >13.3%/s; specificity, 85%), MS type 2 yields intermediate risk (MS 6.4%/s), and MS type 1 implies a low risk (MS BIRADS curve type analysis does (area under the curve, 0.812 vs 0.692; P = 0.0061). Ultrafast dynamic breast MRI allows detection of breast lesions and classification with high accuracy using MS. This allows substantial shortening of scan protocols and hence reduces imaging costs, which is beneficial especially for screening.

  7. Multidiagnostic analysis of ion dynamics in ultrafast laser ablation of metals over a large fluence range

    Energy Technology Data Exchange (ETDEWEB)

    Anoop, K. K., E-mail: anoop.kiliyanamkandy@unina.it; Bruzzese, R.; Amoruso, S. [CNR-SPIN and Dipartimento di Fisica, Universita degli Studi di Napoli Federico II, Complesso Universitario Monte S. Angelo, Via Cintia, Napoli 80126 (Italy); Polek, M. P. [Center for Materials Under Extreme Environment, School of Nuclear Engineering, Purdue University, West Lafayette, Indiana 47907 (United States); Harilal, S. S. [Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352 (United States)

    2015-02-28

    The dynamics of ions in ultrafast laser ablation of metals is studied over fluences ranging from the ablation threshold up to ≈75 J/cm{sup 2} by means of three well-established diagnostic techniques. Langmuir probe, Faraday cup, and spectrally resolved intensified charge coupled device imaging simultaneously monitored the ions produced during ultrafast laser ablation of a pure copper target with 800 nm, ≈50 fs, Ti: Sapphire laser pulses. The fluence dependence of ion yield is analyzed, resulting in the observance of three different regimes. The specific ion yield shows a maximum at about 4–5 J/cm{sup 2}, followed by a gradual reduction and a transition to a high-fluence regime above ≈50 J/cm{sup 2}. The fluence dependence of the copper ions angular distribution is also analyzed, observing a gradual increase in forward-peaking of Cu ions for fluences up to ≈10 J/cm{sup 2}. A broader ion component is observed at larger angles for fluences larger than ≈10 J/cm{sup 2}. Finally, an experimental characterization of the ionic angular distribution for several metallic targets (Mg, Al, Cr, Fe, Cu, and W) is carried out at a relatively high fluence of ≈66 J/cm{sup 2}. Interestingly, the ion emission from the volatile metals shows a narrow, forward-peaked distribution, and a high peak ion yield compared to the refractory metals. Moreover, the width of ionic angular distributions presents a striking correlation with the peak ion yield.

  8. Structure, morphology and ultrafast dynamics of photoexcited states in pi-conjugated polymers

    Science.gov (United States)

    Korovyanko, Oleg J.

    2002-09-01

    Since the discoveries of metallic and super-conductivity, photovoltaic effect and electroluminescence pi-conjugated polymers (PCP) should be regarded as organic semiconductors. However, a typical pristine polymer film has optical properties of a set of disordered organic molecules. Observed optical transitions characterize only discrete portions of polymer chains, called chromophores. The energy transfer to most aligned chromophores takes time of order of a few picoseconds and is similar to that observed in photosynthetic reactions. Therefore, the degree of structural order of PCP is a key parameter governing both photophysics and transport properties. The subject of the present study is the interplay between structure, morphology and ultrafast photophysics in systems of pi-conjugated molecules. Intraband excitons are recognized as the primary optically excited states in all studied polymers and organic crystals. Exciton states follow the symmetry of isolated chains or chain aggregates. Direct band-to-band transitions are of much less importance. In heat- or vapor-treated films a new conformational phase appears. Increased chain planarity results in larger rod-like chromophores. Close contacts between such pi-conjugated chromophores enables geminate polaron pairs generation via exciton dissociation. Polaron pair generation is enhanced in films with increased intrachain order and their diffusion-like recombination kinetics is faster. In films with increased interchain coupling the excitons acquire much larger interchain component. In such films photogenerated geminate polaron pairs with ultrafast dynamics are observed. The recombination rate of polaron pairs permits to estimate the mobilities in self-organized two-dimensional pi-conjugated stacks. Exciton migration plays an important role in the process of laser action in highly luminescent PCPs. While the amplified spontaneous emission is the fastest relaxation process in PCPs with isolated chain morphologies

  9. Size-dependent ultrafast structural dynamics inside phospholipid vesicle bilayers measured with 2D IR vibrational echoes

    Science.gov (United States)

    Kel, Oksana; Tamimi, Amr; Fayer, Michael D.

    2014-01-01

    The ultrafast structural dynamics inside the bilayers of dilauroylphosphatidylcholine (DLPC) and dipalmitoylphosphatidylcholine vesicles with 70, 90, and 125 nm diameters were directly measured with 2D IR vibrational echo spectroscopy. The antisymmetric CO stretch of tungsten hexacarbonyl was used as a vibrational probe and provided information on spectral diffusion (structural dynamics) in the alkyl region of the bilayers. Although the CO stretch absorption spectra remain the same, the interior structural dynamics become faster as the size of the vesicles decrease, with the size dependence greater for dipalmitoylphosphatidylcholine than for DLPC. As DLPC vesicles become larger, the interior dynamics approach those of the planar bilayer. PMID:24395796

  10. Mode specific excited state dynamics study of bis(phenylethynyl)benzene from ultrafast Raman loss spectroscopy

    Science.gov (United States)

    Roy, Khokan; Kayal, Surajit; Ariese, Freek; Beeby, Andrew; Umapathy, Siva

    2017-02-01

    Femtosecond transient absorption (fs-TA) and Ultrafast Raman Loss Spectroscopy (URLS) have been applied to reveal the excited state dynamics of bis(phenylethynyl)benzene (BPEB), a model system for one-dimensional molecular wires that have numerous applications in opto-electronics. It is known from the literature that in the ground state BPEB has a low torsional barrier, resulting in a mixed population of rotamers in solution at room temperature. For the excited state this torsional barrier had been calculated to be much higher. Our femtosecond TA measurements show a multi-exponential behaviour, related to the complex structural dynamics in the excited electronic state. Time-resolved, excited state URLS studies in different solvents reveal mode-dependent kinetics and picosecond vibrational relaxation dynamics of high frequency vibrations. After excitation, a gradual increase in intensity is observed for all Raman bands, which reflects the structural reorganization of Franck-Condon excited, non-planar rotamers to a planar conformation. It is argued that this excited state planarization is also responsible for its high fluorescence quantum yield. The time dependent peak positions of high frequency vibrations provide additional information: a rapid, sub-picosecond decrease in peak frequency, followed by a slower increase, indicates the extent of conjugation during different phases of excited state relaxation. The CC triple (-C≡C-) bond responds somewhat faster to structural reorganization than the CC double (>C=Cwires."

  11. Ultrafast excited-state dynamics at interfaces: fluorescent DNA probes at the dodecane/water interface

    Science.gov (United States)

    Licari, Giuseppe; Vauthey, Eric

    2015-08-01

    Although the interfaces between two isotropic media are of primary importance in many areas of science and technology, their properties are only partially understood. Our strategy to obtain an insight into these properties is to investigate the ultrafast excited-state dynamics of environment-sensitive molecular probes at liquid interfaces using time-resolved surface second harmonic generation, and to compare it with the dynamics of the same molecules in bulk solutions. Additionally, this approach gives rich information on how the chemical reactivity may change when going from the bulk phase to the interface. This is illustrated by an investigation performed with a series of fluorescent DNA probes at the dodecane/water interface without and with the presence of DNA in the aqueous phase. Substantial differences in the conformation of these cyanine dyes (aggregated or not) and in the excited-state dynamics are observed when going from bulk solutions to the interface. Moreover, the presence of double-stranded DNA in the aqueous phase induces some chirality at the interface.

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

    Science.gov (United States)

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

    2014-05-01

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

  13. Theory and Modelling of Ultrafast X-ray Imaging of Dynamical Non-equilibrium Systems

    DEFF Research Database (Denmark)

    Lorenz, Ulf

    , it becomes feasible to exploit this concept for ultrafast processes; in eect, we can study chemical reactions as they occur. This thesis deals with theoretical aspect of ultrafast time-resolved x-ray diraction (TRXD).We derive general formulas for calculating the diraction signal that are closely related...

  14. Probing ultrafast spin dynamics through a magnon resonance in the antiferromagnetic multiferroic HoMnO3

    Science.gov (United States)

    Bowlan, P.; Trugman, S. A.; Bowlan, J.; Zhu, J.-X.; Hur, N. J.; Taylor, A. J.; Yarotski, D. A.; Prasankumar, R. P.

    2016-09-01

    We demonstrate an approach for directly tracking antiferromagnetic (AFM) spin dynamics by measuring ultrafast changes in a magnon resonance. We test this idea on the multiferroic HoMnO3 by optically photoexciting electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced change in the magnon line shape that builds up over 5-12 picoseconds, which we show to be the spin-lattice thermalization time, indicating that electrons heat the spins via phonons. We compare our results to previous studies of spin-lattice thermalization in ferromagnetic manganites, giving insight into fundamental differences between the two systems. Our work sheds light on the microscopic mechanism governing spin-phonon interactions in AFMs and demonstrates a powerful approach for directly monitoring ultrafast spin dynamics.

  15. Coherent helix vacancy phonon and its ultrafast dynamics waning in topological Dirac semimetal C d3A s2

    Science.gov (United States)

    Sun, Fei; Wu, Q.; Wu, Y. L.; Zhao, H.; Yi, C. J.; Tian, Y. C.; Liu, H. W.; Shi, Y. G.; Ding, H.; Dai, X.; Richard, P.; Zhao, Jimin

    2017-06-01

    We report an ultrafast lattice dynamics investigation of the topological Dirac semimetal C d3A s2 . A coherent phonon beating among three evenly spaced A1 g optical phonon modes (of frequencies 1.80, 1.96, and 2.11 THz, respectively) is unambiguously observed. The two side modes originate from the counter helixes composing Cd vacancies. Significantly, such helix vacancy-induced phonon (HVP) modes experience prominent extra waning in their ultrafast dynamics as temperature increases, which is immune to the central mode. Above 200 K, the HVP becomes inactive, which may potentially affect the topological properties. Our results in the lattice degree of freedom suggest the indispensable role of temperature in considering topological properties of such quantum materials.

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

    Directory of Open Access Journals (Sweden)

    Linlin Wei

    2017-07-01

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

  17. Topology Optimization for Photonic Crystal Waveguide Intersection with Wide and Flat Bandwidths in Ultra-Fast All-Optical Switch (PC-SMZ)

    DEFF Research Database (Denmark)

    Sugimoto, Y; Watanabe, Y; Ikeda, N

    2006-01-01

    Numerical and experimental studies on the photonic crystal waveguide intersection based on the topology optimization design method are reported and the effectiveness is shown by achieving high transmission spectra with low crosstalk for the straightforward beam-propagation line....

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

    OpenAIRE

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

    2011-01-01

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

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

    Science.gov (United States)

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

    2014-02-11

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

  20. Ultrafast Molecular Photodissociation Dynamics Studied by Femtosecond Photoelectron-Photoion Coincidence Spectroscopy

    Science.gov (United States)

    Thaler, Bernhard; Heim, Pascal; Ernst, Wolfgang E.; Koch, Markus

    2017-06-01

    To completely characterize photodissociation mechanisms with time-resolved spectroscopy, it is essential to obtain unequivocal experimental information about the fragmentation dynamics induced by the laser pulse. We apply time-resolved photoelectron-photoion coincidence (PEPICO) detection in combination with different excitation schemes to obtain a mechanistic picture of the fragmentation process. For gas phase acetone molecules excited to high lying Rydberg states we are able to disentangle different ionization channels and investigate the fragmentation behavior of each channel separately. In particular, the high differentiability of PEPICO allows to distinguish channels where fragmentation proceeds after ionization from channels with fragmentation in the neutral. We show that excited Rydberg state population undergoes internal conversion due to coupling to valence states, which takes place within (150 ± 30) fs. The corresponding non-adiabatic, ultrafast relaxation dynamics to lower lying states causes conversion of electronic to vibrational energy and is found to play a crucial role in the fragmentation process (see figure 1). By studying the influence of photon energy, pulse duration, chirp and intensity of the laser pulses, we are able to determine the energy-threshold that is required for fragmentation, as well as corresponding fragmentation ratios. Surprisingly, for excitation with pulses possessing a strong negative chirp we observe significantly reduced fragmentation, indicating different internal conversion pathways and the associated intramolecular vibrational redistribution.

  1. Coherent energy scale revealed by ultrafast dynamics of UX3 (X = Al, Sn, Ga) single crystals

    Science.gov (United States)

    Nair, Saritha K.; Zhu, J.-X.; Sarrao, J. L.; Taylor, A. J.; Chia, Elbert E. M.

    2012-09-01

    The temperature dependence of relaxation dynamics of UX3 (X = Al, Ga, Sn) compounds is studied using the time-resolved pump-probe technique in reflectance geometry. For UGa3, our data are consistent with the formation of a spin density wave gap as evidenced from the quasidivergence of the relaxation time τ near the Néel temperature TN. For UAl3 and USn3, the relaxation dynamics shows a change from single-exponential to two-exponential behavior below a particular temperature, suggestive of coherence formation of the 5f electrons with the conduction band electrons. This particular temperature can be attributed to the spin fluctuation temperature Tsf, a measure of the strength of Kondo coherence. Our Tsf is consistent with other data such as resistivity and susceptibility measurements. The temperature dependence of the relaxation amplitude and time of UAl3 and USn3 were also fitted by the Rothwarf-Taylor model. Our results show that ultrafast optical spectroscopy is sensitive to c-f Kondo hybridization in the f-electron systems.

  2. Optically induced lattice dynamics probed with ultrafast x-ray diffraction

    Science.gov (United States)

    Lee, H. J.; Workman, J.; Wark, J. S.; Averitt, R. D.; Taylor, A. J.; Roberts, J.; McCulloch, Q.; Hof, D. E.; Hur, N.; Cheong, S.-W.; Funk, D. J.

    2008-04-01

    We have studied the picosecond lattice dynamics of optically pumped hexagonal LuMnO3 by using ultrafast x-ray diffraction. The results show a shift and broadening of the diffraction curve due to the stimulated lattice expansion. To understand the transient response of the lattice, the measured time- and angle-resolved diffraction curves are compared to a theoretical calculation based on the dynamical diffraction theory of coherent phonon propagation modified for the hexagonal crystal structure of LuMnO3 . Our simulations reveal that a large coupling coefficient (c13) between the a-b plane and the c axis is required to fit the data. Though we interpret the transient response within the framework of thermal coherent phonons, we do not exclude the possibility of strong nonthermal coupling of the electronic excitation to the atomic framework. We compare this result to our previous coherent phonon studies of LuMnO3 in which we used optical pump-probe spectroscopy.

  3. Dynamic Solvent Effect on Ultrafast Charge Recombination Kinetics in Excited Donor-Acceptor Complexes.

    Science.gov (United States)

    Mikhailova, Tatyana V; Mikhailova, Valentina A; Ivanov, Anatoly I

    2016-11-23

    Manifestation of the dynamic solvent effect (DSE) on the charge recombination (CR) kinetics of photoexcited donor-acceptor complexes in polar solvents has been investigated within the framework of the multichannel stochastic model. The model takes into account the reorganization of both the solvent and a number of intramolecular high-frequency vibration modes as well as their relaxation. The non-Markovian solvent dynamics is described in terms of two relaxation modes. The similarities and differences inherent to ultrafast charge transfer reactions occurring in the nonequilibrium and thermal regimes have been identified. The most important differences are as follows: (1) the DSE is strong in the area of weak exergonicity and is weak in the area of strong exergonicity for thermal reactions, whereas for the nonequilibrium reactions, the regions of strong and weak DSEs are reversed; (2) an increase in the electronic coupling value results in a decrease in the magnitude of DSE for nonequilibrium electron transfer and in its increase for the thermal reactions; and (3) the two-staged regime most clearly manifests if the reorganization energy of the relaxation modes noticeably exceeds the CR free-energy gap. With an increase in electronic coupling, the kinetics approaches the exponential regime because in the limit of strong electronic coupling, the reaction includes only single, nonequilibrium, stage.

  4. Synchrotron x-ray ultrafast x-ray imaging on dynamic multiphase flow studies

    Science.gov (United States)

    Wang, Yujie; Fezzaa, Kamel; Wang, Jin; Im, Kyoung-Su

    2007-03-01

    To overcome the long-exposure time of x-ray imaging for liquid systems. In the past year, we have developed the first ultrafast white-beam synchrotron x-ray phase-contrast imaging technique in the world. With its unprecedented temporal (0.5 μs) and spatial resolutions (1 μm), this new technique has already shown great promises in the study of complex fluid mechanical systems. It can probe complex surface morphology and transient dynamics of these interfaces of fluid mechanical systems without the nuisance of multiple scattering. This technique is a big step forward in comparison to millisecond-temporal and micrometer-spatial imaging resolutions normally achieved at various synchrotron sources. With the development of this new technique, we can already carry out research in fluid mechanical systems in competition with world-leading research groups. Our study of the primary breakup process of a coaxial air-assisted liquid jet revealed that the dynamics is dominated by a ``liquid membrane breakup'' process instead of a simple ``ligament mediated breakup'' process owing to our far superior temporal and spatial resolutions. This observation will naturally lead to a cascade idea for the unified treatment of liquid jets, droplets, and liquid membranes breakup mechanism.

  5. Ultrafast pump-probe dynamics of iron oxide based earth pigments for applications to ancient pottery manufacture

    Science.gov (United States)

    Villafana, Tana E.; Brown, William; Warren, Warren S.; Fischer, Martin

    2015-06-01

    We demonstrate that ultrafast pump-probe microscopy provides unique dynamics for natural iron oxide and iron hydroxide earth pigments, despite their chemical similarity. First, we conducted a pump-probe spectroscopy study on heat-treated hematite (the pure red iron oxide mineral) and found the pump-probe dynamics to be temperature dependent. Second, we investigated pottery fired under known conditions and observed firing dependent pump-probe dynamics. Finally, we imaged a New World potshard from the North Carolina Museum of Art. Our results indicate that pump-probe microscopy could be a useful tool in elucidating pottery manufacture.

  6. Dynamics of laser-imploded core plasmas observed by ultrafast two-dimensional x-ray imaging with animation display

    Energy Technology Data Exchange (ETDEWEB)

    Heya, Manabu; Shiraga, Hiroyuki; Shimada, Kyoko; Miyanaga, Noriaki; Takabe, Hideaki; Yamanaka, Tatsuhiko; Mima, Kunioki [Osaka Univ., Inst. of Laser Engineering, Suita, Osaka (Japan)

    1999-05-01

    In order to observe time-resolved, two-dimensional (2D) spatial distribution of x rays emitted from core plasmas at the final stage of the implosion, we have developed a multi-imaging x-ray streak camera (MIXS) and a multi-channel MIXS (McMIXS) methods as new ultrafast 2D x-ray imaging techniques. The observed time-resolved 2D x-ray and electron-temperature images of core plasmas, which are sequentially changing with time, have been displayed by using an animation method. Temporal evolutions of nonuniform structures, including shape, size, and movement of core plasmas can be observed instinctively with the animated display. The ultrafast 2D x-ray imaging with the animation display is a new powerful tool for understanding the dynamics of laser-imploded core plasmas. (author)

  7. Ultrafast chemical reactions in shocked nitromethane probed with dynamic ellipsometry and transient absorption spectroscopy.

    Science.gov (United States)

    Brown, Kathryn E; McGrane, Shawn D; Bolme, Cynthia A; Moore, David S

    2014-04-10

    Initiation of the shock driven chemical reactions and detonation of nitromethane (NM) can be sensitized by the addition of a weak base; however, the chemical mechanism by which sensitization occurs remains unclear. We investigated the shock driven chemical reaction in NM and in NM sensitized with diethylenetriamine (DETA), using a sustained 300 ps shock driven by a chirped Ti:sapphire laser. We measured the solutions' visible transient absorption spectra and measured interface particle and shock velocities of the nitromethane solutions using ultrafast dynamic ellipsometry. We found there to be a volume-increasing reaction that takes place around interface particle velocity up = 2.4 km/s and up = 2.2 km/s for neat NM and NM with 5% DETA, respectively. The rate at which transient absorption increases is similar in all mixtures, but with decreasing induction times for solutions with increasing DETA concentrations. This result supports the hypothesis that the chemical reaction mechanisms for shocked NM and NM with DETA are the same. Data from shocked NM are compared to literature experimental and theoretical data.

  8. Ultrafast dynamics of surface plasmons in InAs by time-resolved infrared nanospectroscopy.

    Science.gov (United States)

    Wagner, Martin; McLeod, Alexander S; Maddox, Scott J; Fei, Zhe; Liu, Mengkun; Averitt, Richard D; Fogler, Michael M; Bank, Seth R; Keilmann, Fritz; Basov, D N

    2014-08-13

    We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump-probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1-2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 μJ/cm(2), much smaller than fluences of ∼ 1-10 mJ/cm(2) previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 μm fiber laser. Thus, InAs--a common semiconductor with favorable plasmonic properties such as a low effective mass--has the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies.

  9. Ultrafast charge- and energy-transfer dynamics in conjugated polymer: cadmium selenide nanocrystal blends.

    Science.gov (United States)

    Morgenstern, Frederik S F; Rao, Akshay; Böhm, Marcus L; Kist, René J P; Vaynzof, Yana; Greenham, Neil C

    2014-02-25

    Hybrid nanocrystal-polymer systems are promising candidates for photovoltaic applications, but the processes controlling charge generation are poorly understood. Here, we disentangle the energy- and charge-transfer processes occurring in a model system based on blends of cadmium selenide nanocrystals (CdSe-NC) with poly[2-methoxy-5-(3',7'-dimethyloctyloxy)-1,4-phenylene vinylene] (MDMO-PPV) using a combination of time-resolved absorption and luminescence measurements. The use of different capping ligands (n-butylamine, oleic acid) as well as thermal annealing allows tuning of the polymer-nanocrystal interaction. We demonstrate that energy transfer from MDMO-PPV to CdSe-NCs is the dominant exciton quenching mechanism in nonannealed blends and occurs on ultrafast time scales (<1 ps). Upon thermal annealing electron transfer becomes competitive with energy transfer, with a transfer rate of 800 fs independent of the choice of the ligand. Interestingly, we find hole transfer to be much less efficient than electron transfer and to extend over several nanoseconds. Our results emphasize the importance of tuning the organic-nanocrystal interaction to achieve efficient charge separation and highlight the unfavorable hole-transfer dynamics in these blends.

  10. The dynamics of azulene in liquids and compressed gases on ultrafast timescales

    Energy Technology Data Exchange (ETDEWEB)

    Schultz, K.E.

    1992-02-01

    The ultrafast dynamics of vibrationally hot ground state azulene molecules have been time resolved by picosecond transient absorption spectroscopy in a variety of solvents including hexane, chloromethanes, methanol, CClF{sub 3}, Xe and Kr. A high pressure optical cell was used to liquify gases for use as solvents and change their density and temperature, independently, over the entire liquid density range. Experimental results indicate the vibrational cooling rate is strongly solvent dependent, with cooling rates of approximately 20 psec in molecular solvents and approximately 150 psec in atomic solvents. Comparison of the rates in Xe and Kr at constant density demonstrates the strong effect of solvent mass on energy transfer. The effect of solvent temperature on vibrational cooling is minimal, as is the effect of solvent density. This latter result is quite surprising in light of earlier experiments on simpler molecular systems, such as I{sub 2} in Xe. This anomalous density effect is examined in light of Isolated Binary Collision (IBC) theory and bulk thermal transport models. Both theories accurately model all experimental results obtained with the exception of the density effort. Possible explanations for the breakdown of the IBC theory in this case are offered along with methods to improve IBC theory for application to complex three dimensional molecular systems.

  11. 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)

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

    Directory of Open Access Journals (Sweden)

    F. Carbone

    2010-01-01

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

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

    CERN Document Server

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

    2016-01-01

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

  14. Ultrafast carrier dynamics and radiative recombination in multiferroic BiFeO3 single crystals and thin films

    Directory of Open Access Journals (Sweden)

    Taylor A. J.

    2013-03-01

    Full Text Available We report a detailed comparison of ultrafast carrier dynamics in single crystals and thin films of multiferroic BiFeO3 (BFO. Using degenerate femtosecond optical pump-probe spectroscopy, we find that the observed dynamics are qualitatively similar in both samples. After photoexcitation, electrons relax to the conduction band minimum through electron-phonon coupling, with subsequent carrier relaxation proceeding via various recombination pathways that extend to a nanosecond timescale. Subtle differences observed in our measurements indicate that BFO films have a higher band gap than single crystals. Overall, our results demonstrate that carrier relaxation in BFO is analogous to that in bulk semiconductors.

  15. Ultrafast phosphate hydration dynamics in bulk H{sub 2}O

    Energy Technology Data Exchange (ETDEWEB)

    Costard, Rene, E-mail: costard@mbi-berlin.de; Tyborski, Tobias; Fingerhut, Benjamin P., E-mail: fingerhut@mbi-berlin.de; Elsaesser, Thomas [Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie, D-12489 Berlin (Germany)

    2015-06-07

    Phosphate vibrations serve as local probes of hydrogen bonding and structural fluctuations of hydration shells around ions. Interactions of H{sub 2}PO{sub 4}{sup −} ions and their aqueous environment are studied combining femtosecond 2D infrared spectroscopy, ab-initio calculations, and hybrid quantum-classical molecular dynamics (MD) simulations. Two-dimensional infrared spectra of the symmetric (ν{sub S}(PO{sub 2}{sup −})) and asymmetric (ν{sub AS}(PO{sub 2}{sup −})) PO{sub 2}{sup −} stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the δ(P-(OH){sub 2}) bending modes. The frequency-time correlation function derived from the 2D spectra consists of a predominant 50 fs decay and a weak constant component accounting for a residual inhomogeneous broadening. MD simulations show that the fluctuating electric field of the aqueous environment induces strong fluctuations of the ν{sub S}(PO{sub 2}{sup −}) and ν{sub AS}(PO{sub 2}{sup −}) transition frequencies with larger frequency excursions for ν{sub AS}(PO{sub 2}{sup −}). The calculated frequency-time correlation function is in good agreement with the experiment. The ν(PO{sub 2}{sup −}) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H{sub 2}PO{sub 4}{sup −}/H{sub 2}O cluster calculations reveal substantial frequency shifts and mode mixing with increasing hydration. Predicted phosphate-water hydrogen bond (HB) lifetimes have values on the order of 10 ps, substantially longer than water-water HB lifetimes. The ultrafast phosphate-water interactions observed here are in marked contrast to hydration dynamics of phospholipids where a quasi-static inhomogeneous broadening of phosphate vibrations suggests minor structural fluctuations of interfacial water.

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

    Science.gov (United States)

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

    2016-12-08

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

  17. Ultrafast excited state dynamics of the green fluorescent protein chromophore and its kindling fluorescent protein analogue.

    Science.gov (United States)

    Addison, Kiri; Heisler, Ismael A; Conyard, Jamie; Dixon, Tara; Page, Philip C Bulman; Meech, Stephen R

    2013-01-01

    Fluorescent proteins exhibit a very diverse range of photochemical behaviour, from efficient fluorescence through photochromism to photochemical reactivity. Remarkably this diverse behaviour arises from chromophores which have very similar structures. Here we describe measurements and modelling of the excited state dynamics in the chromophores of GFP (HBDI) and the kindling fluorescent protein, KFP (FHBMI). The methods are ultrafast fluorescence spectroscopy with sub 50 fs time resolution and the modelling is based on the Smoluchowski equation. The excited state decays of both chromophores are very fast, longer for their anions than for the neutral form and independent of wavelength. Detailed studies show the mean fluorescence wavelength to be independent of time. The excited state decay times are also observed to be a very weak function of solvent polarity and viscosity. These results are modelled utilising recently calculated potential energy surfaces for the ground and excited states as a function of the twist coordinates about the two bridging bonds of the chromophore. For FHBMI and the scarce data on the neutral HBDI the calculations are not successful suggesting the need for refinement of these potential energy surfaces. For HBDI in methanol the simulation is successful provided a strong dependence of the radiationless decay rate on the coordinate is assumed. Such dependence should be included in future calculations of excited state dynamics. When the simulations are extended to more viscous solvents they fail to reproduce the observed weak viscosity dependence. The implications of these results for the nature of the coordinate leading to radiationless decay in the chromophore and for the photodynamics of fluorescent proteins are discussed.

  18. Dynamically encircling exceptional points in a waveguide: asymmetric mode switching from the breakdown of adiabaticity

    CERN Document Server

    Doppler, Jörg; Böhm, Julian; Kuhl, Ulrich; Girschik, Adrian; Libisch, Florian; Milburn, Thomas J; Rabl, Peter; Moiseyev, Nimrod; Rotter, Stefan

    2016-01-01

    Physical systems with loss or gain feature resonant modes that are decaying or growing exponentially with time. Whenever two such modes coalesce both in their resonant frequency and their rate of decay or growth, a so-called "exceptional point" occurs, around which many fascinating phenomena have recently been reported to arise. Particularly intriguing behavior is predicted to appear when encircling an exceptional point sufficiently slowly, like a state-flip or the accumulation of a geometric phase. Experiments dedicated to this issue could already successfully explore the topological structure of exceptional points, but a full dynamical encircling and the breakdown of adiabaticity inevitably associated with it remained out of reach of any measurement so far. Here we demonstrate that a dynamical encircling of an exceptional point can be mapped onto the problem of scattering through a two-mode waveguide, which allows us for the first time to access the elusive effects occurring in this context. Specifically, w...

  19. Ultrafast Dynamics Through Conical Intersections in 2,6-dimethylpyridine Studied with Time-resolved Photoelectron Imaging

    Institute of Scientific and Technical Information of China (English)

    Xue-jun Qiu; Rong-shu Zhu; Yan-qi Xu; Abulimiti Bumaliya; Song Zhang; Bing Zhang

    2011-01-01

    The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy.Upon absorption of 266 nm pump laser,2,6-dimethylpyridine is excited to the S2 state with a ππ* character from So state.The time evolution of the parent ion signals consists of two exponential decays.One is a fast component on a timescale of 635 fs and the other is a slow component with a timescale of 4.37 ps.Time-dependent photoelectron angular distributions and energy-resolved photoelectron spectroscopy are extracted from time-resolved photoelectron imaging and provide the evolutive information of S2 state.In brief,the ultrafast component is a population transfer from S2 to S1 through the S2/S1 conical intersections,the slow component is attributed to simultaneous IC from the S2 state and the higher vibrational levels of S1 state to S0 state,which involves the coupling of S2/S0 and S1/S0 conical intersections.Additionally,the observed ultrafast S2→S1 transition occurs only with an 18% branching ratio.

  20. 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

  1. Infrared studies of impurity states and ultrafast carrier dynamics in semiconductor quantum structures

    Energy Technology Data Exchange (ETDEWEB)

    Stehr, D.

    2007-12-28

    This thesis deals with infrared studies of impurity states, ultrafast carrier dynamics as well as coherent intersubband polarizations in semiconductor quantum structures such as quantum wells and superlattices, based on the GaAs/AlGaAs material system. In the first part it is shown that the 2p{sub z} confined impurity state of a semiconductor quantum well develops into an excited impurity band in the case of a superlattice. This is studied by following theoretically the transition from a single to a multiple quantum well or superlattice by exactly diagonalizing the three-dimensional Hamiltonian for a quantum well system with random impurities. These results also require reinterpretation of previous experimental data. The relaxation dynamics of interminiband transitions in doped GaAs/AlGaAs superlattices in the mid-IR are studied. This involves single-color pump-probe measurements to explore the dynamics at different wavelengths, which is performed with the Rossendorf freeelectron laser (FEL), providing picosecond pulses in a range from 3-200 {mu}m and are used for the first time within this thesis. In these experiments, a fast bleaching of the interminiband transition is observed followed by thermalization and subsequent relaxation, whose time constants are determined to be 1-2 picoseconds. This is followed by an additional component due to carrier cooling in the lower miniband. In the second part, two-color pump-probe measurements are performed, involving the FEL as the pump source and a table-top broad-band tunable THz source for probing the transmission changes. In addition, the dynamics of excited electrons within the minibands is explored and their contribution quantitatively extracted from the measurements. Intersubband absorption experiments of photoexcited carriers in single quantum well structures, measured directly in the time-domain, i.e. probing coherently the polarization between the first and the second subband, are presented. By varying the carrier

  2. Ultrafast dynamics of charge carrier photogeneration and geminate recombination in conjugated polymer:fullerene solar cells

    Science.gov (United States)

    Müller, J. G.; Lupton, J. M.; Feldmann, J.; Lemmer, U.; Scharber, M. C.; Sariciftci, N. S.; Brabec, C. J.; Scherf, U.

    2005-11-01

    We investigate the nature of ultrafast exciton dissociation and carrier generation in acceptor-doped conjugated polymers. Using a combination of two-pulse femtosecond spectroscopy with photocurrent detection, we compare the exciton dissociation and geminate charge recombination dynamics in blends of two conjugated polymers, MeLPPP [methyl-substituted ladder-type poly( p -phenylene)] and MDMO-PPV [poly(2-methoxy,5-(3,7-dimethyloctyloxy)-1,4-phenylenevinylene], with the electron accepting fullerene derivative PCBM [1-(3-methoxycarbonyl)-propyl-1-phenyl- (6,6)C61 ]. This technique allows us to distinguish between free charge carriers and Coulombically bound polaron pairs. Our results highlight the importance of geminate pair recombination in photovoltaic devices, which limits the device performance. The comparison of different materials allows us to address the dependence of geminate recombination on the film morphology directly at the polymer:fullerene interface. We find that in the MeLPPP:PCBM blend exciton dissociation generates Coulombically bound geminate polaron pairs with a high probability for recombination, which explains the low photocurrent yield found in these samples. In contrast, in the highly efficient MDMO-PPV:PCBM blend the electron transfer leads to the formation of free carriers. The anisotropy dynamics of electronic transitions from neutral and charged states indicate that polarons in MDMO-PPV relax to delocalized states in ordered domains within 500fs . The results suggest that this relaxation enlarges the distance of carrier separation within the geminate pair, lowering its binding energy and favoring full dissociation. The difference in geminate pair recombination concurs with distinct dissociation dynamics. The electron transfer is preceded by exciton migration towards the PCBM sites. In MeLPPP:PCBM the exciton migration time decays smoothly with increasing PCBM concentration, indicating a trap-free exciton hopping. In MDMO-PPV:PCBM, however

  3. The dynamics of peptide-water interactions in dialanine: An ultrafast amide I 2D IR and computational spectroscopy study

    Science.gov (United States)

    Feng, Chi-Jui; Tokmakoff, Andrei

    2017-08-01

    We present a joint experimental and computational study of the dynamic interactions of dialanine (Ala-Ala) with water, comparing the results of ultrafast 2D IR and infrared transient absorption spectroscopy of its amide I vibration with spectra modeled from molecular dynamics (MD) simulations. The experimental data are analyzed to describe vibrational frequency fluctuations, vibrational energy relaxation, and chemical exchange processes. The origin of these processes in the same underlying fluctuating forces allows a common description in terms of the fluctuations and conformational dynamics of the peptide and associated solvent. By comparing computational spectroscopy from MD simulations with multiple force fields and water models, we describe how the dynamics of water hydrogen bond fluctuations and switching processes act as a source of friction that governs the dephasing and vibrational relaxation, and provide a description of coupled water and peptide motions that give rise to spectroscopic exchange processes.

  4. 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.

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

    Science.gov (United States)

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

    2015-02-01

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

  6. A Dual-Colour Architecture for Pump-Probe Spectroscopy of Ultrafast Magnetization Dynamics in the Sub-10-femtosecond Range

    Science.gov (United States)

    Gonçalves, C. S.; Silva, A. S.; Navas, D.; Miranda, M.; Silva, F.; Crespo, H.; Schmool, D. S.

    2016-03-01

    Current time-resolution-limited dynamic measurements clearly show the need for improved techniques to access processes on the sub-10-femtosecond timescale. To access this regime, we have designed and constructed a state-of-the-art time-resolved magneto-optic Kerr effect apparatus, based on a new dual-color scheme, for the measurement of ultrafast demagnetization and precessional dynamics in magnetic materials. This system can operate well below the current temporal ranges reported in the literature, which typically lie in the region of around 50 fs and above. We have used a dual-colour scheme, based on ultra broadband hollow-core fibre and chirped mirror pulse compression techniques, to obtain unprecedented sub-8-fs pump and probe pulse durations at the sample plane. To demonstrate the capabilities of this system for ultrafast demagnetization and precessional dynamics studies, we have performed measurements in a ferrimagnetic GdFeCo thin film. Our study has shown that the magnetization shows a sudden drop within the first picosecond after the pump pulse, a fast recovery (remagnetization) within a few picoseconds, followed by a clear oscillation or precession during a slower magnetization recovery. Moreover, we have experimentally confirmed for the first time that a sub-10-fs pulse is able to efficiently excite a magnetic system such as GdFeCo.

  7. Ultrafast Magnetic Light

    CERN Document Server

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

    2015-01-01

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

  8. Studies of solvent effects on reaction dynamics using ultrafast transient absorption spectroscopy

    Science.gov (United States)

    Harris, Don Ahmasi

    Ultrafast transient absorption spectroscopy was used to investigate the solvent dependent reaction dynamics of two prototypical chemical systems: (1) The ring-opening reaction of 1,3-cyclohexadiene, the isolated chromophore in Provitamin D, and (2) The photolysis of various Vitamin B12 cofactors. We investigated the influence of solvent polarity on the ground state conformational relaxation of 1,3,5-cis hexatriene subsequent to the ring opening of 1,3-cyclohexadiene in methanol and 1-propanol solvents. Comparisons to the conformational relaxation in alkane solvents studied earlier demonstrated a surprising influence of solvent polarity on single bond isomerization. Temperature dependent transient absorption measurements were performed on 1,3,5-cis hexatriene in cyclohexane and 1-propanol to determine the effect of solvent polarity on the activation energy barrier for ground state single bond isomerization. These measurements conclude that the polar solvent lowers the energy barrier for single bond isomerization allowing conformational relaxation to proceed faster in alcohol solvents compared to alkane solvents. With no perceived polar transition state for single bond isomerization, this result disagrees with the conventional view of solvation and differentiates the single bond isomerization dynamics of polyenes from alkanes. Transient absorption spectroscopy was also utilized to study the solvent effects in the photolysis of various B12 cofactors in different environments. We investigated the solvent dependent photolysis of adenosylcobalamin, methylcobalamin, and cyanocobalamin in water and ethylene glycol as a function of solvent temperature. In comparing the radical cage escape of adenosylcobalamin and cyanocobalamin, we determined a larger than expected hydrodynamic radii for the diffusing radicals in water compared to ethylene glycol, thus making necessary a revised perspective of solvent interaction with the diffusing radical. In addition, we investigated the

  9. Ultrafast gain and index dynamics of quantum dash structures emitting at 1.55 mu m

    DEFF Research Database (Denmark)

    Poel, Mike van der; Mørk, Jesper; Somers, A.

    2006-01-01

    The authors systematically characterize the ultrafast gain and index recovery of a quantum dash semiconductor optical amplifier after it has amplified a strong femtosecond pulse. The results show a recovery dominated by a fast time constant of 1.4 ps with an ultimate recovery taking place on a 150...

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

    NARCIS (Netherlands)

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

    2016-01-01

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

  11. Interfacial effects revealed by ultrafast relaxation dynamics in BiFeO 3 / YBa 2 Cu 3 O 7 bilayers

    KAUST Repository

    Springer, D.

    2016-02-12

    The temperature dependence of the relaxation dynamics in the bilayer thin film heterostructure composed of multiferroic BiFeO3 (BFO) and superconducting YBa2Cu3O7 (YBCO) grown on a (001) SrTiO3 substrate is studied by a time-resolved pump-probe technique, and compared with that of pure YBCO thin film grown under the same growth conditions. The superconductivity of YBCO is found to be retained in the heterostructure. We observe a speeding up of the YBCO recombination dynamics in the superconducting state of the heterostructure, and attribute it to the presence of weak ferromagnetism at the BFO/YBCO interface as observed in magnetization data. An extension of the Rothwarf-Taylor model is used to fit the ultrafast dynamics of BFO/YBCO, that models an increased quasiparticle occupation of the ferromagnetic interfacial layer in the superconducting state of YBCO.

  12. Optical nonlinearity and-ultrafast dynamics of ion exchanged silver nanoparticles embedded in soda-lime silicate glass

    Institute of Scientific and Technical Information of China (English)

    YANG XiuChun; LI ZhiHui; LI WeiJie; XU JingXian; DONG ZhiWei; QIAN ShiXiong

    2008-01-01

    Ag nanoparticles embedded in soda-lime silicate glass were fabricated by ion-exchange and subsequently annealing method. Z-scan technique, femtosecond time-resolved optical Kerr effect (OKE) technique and femtosecond pump-probe experiment were used to investigate the effects of laser wavelength and laser pulse duration as well as annealing temperature on the third-order optical nonlinearity and ultrafast dynamics of the composites. It was found that the third-order susceptibility of Ag nanoparticles composite glass measured by 400 nm pulse source is larger than that measured by 800 nm pulse source due to an enhancement effect of local field near surface plasmon resonance of Ag nanoparticles in silicate glass. The third-order optical nonlinearity measured by ns laser source is about two orders of magnitude larger than that measured from fs pulse. The annealing temperature has an important effect on the third-order optical nonlinearity and ultrafast dynamics of the composites. Third-order nonlinear susceptibility upto 10-10 esu and fast relaxation process up to 0.2 ps have been obtained in Ag nanoparticles doped glass,

  13. Investigations of ultrafast charge dynamics in laser-irradiated targets by a self probing technique employing laser driven protons

    Energy Technology Data Exchange (ETDEWEB)

    Ahmed, H. [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom); Kar, S., E-mail: s.kar@qub.ac.uk [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom); Cantono, G. [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom); Department of Physics “E. Fermi”, Largo B. Pontecorvo 3, 56127 Pisa (Italy); Consiglio Nazionale delle Ricerche, Istituto Nazionale di Ottica, Research Unit Adriano Gozzini, via G. Moruzzi 1, Pisa 56124 (Italy); Nersisyan, G. [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom); Brauckmann, S. [Institut für Laser-und Plasmaphysik, Heinrich-Heine-Universität, Düsseldorf (Germany); Doria, D.; Gwynne, D. [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom); Macchi, A. [Department of Physics “E. Fermi”, Largo B. Pontecorvo 3, 56127 Pisa (Italy); Consiglio Nazionale delle Ricerche, Istituto Nazionale di Ottica, Research Unit Adriano Gozzini, via G. Moruzzi 1, Pisa 56124 (Italy); Naughton, K. [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom); Willi, O. [Institut für Laser-und Plasmaphysik, Heinrich-Heine-Universität, Düsseldorf (Germany); Lewis, C.L.S.; Borghesi, M. [School of Mathematics and Physics, Queen' s University Belfast, BT7 1NN (United Kingdom)

    2016-09-01

    The divergent and broadband proton beams produced by the target normal sheath acceleration mechanism provide the unique opportunity to probe, in a point-projection imaging scheme, the dynamics of the transient electric and magnetic fields produced during laser-plasma interactions. Commonly such experimental setup entails two intense laser beams, where the interaction produced by one beam is probed with the protons produced by the second. We present here experimental studies of the ultra-fast charge dynamics along a wire connected to laser irradiated target carried out by employing a ‘self’ proton probing arrangement – i.e. by connecting the wire to the target generating the probe protons. The experimental data shows that an electromagnetic pulse carrying a significant amount of charge is launched along the wire, which travels as a unified pulse of 10s of ps duration with a velocity close to speed of light. The experimental capabilities and the analysis procedure of this specific type of proton probing technique are discussed. - Highlights: • Prompt charging of laser irradiated target generates ultra-short EM pulses. • Its ultrafast propagation along a wire was studied by self-proton probing technique. • Self-proton probing technique is the proton probing with one laser pulse. • Pulse temporal profile and speed along the wire were measured with high resolution.

  14. Ultrafast dual photoresponse of isolated biological chromophores: link to the photoinduced mode-specific non-adiabatic dynamics in proteins.

    Science.gov (United States)

    Bochenkova, Anastasia V; Andersen, Lars H

    2013-01-01

    The anionic wild-type Green Fluorescent Protein (GFP) chromophore defines an entire class of naturally occurring chromophores, which are based on the oxydized tyrosine side chain. The GFP chromophore exhibits an enriched photoinduced non-adiabatic dynamics in the multiple excited-state decay channels. Deactivation includes vibrational resonant photodetachment and internal conversion. Here, we provide detailed insight into the efficiency of different vibrational modes in promoting a selective photoresponse in the bare GFP chromophore anion. We introduce a general theoretical model that is capable of accounting for the alternative non-equivalent pathways in internal conversion, and we outline the factors, by which the photo-initiated response may be altered in this channel. The topography around the planar minimum in S1 and the two distinct types of the S1/S0 conical intersections obtained through high-level ab initio calculations provide direct support to the proposed model. There are mode-selective ways to control the photoresponse and to direct it towards a single excited-state decay channel. By tuning the excitation wavelength, the photoresponse may be directed towards the ultrafast non-statistical electron emission coupled with vibrational (de)coherence, whereas a vibrational pre-excitation in the ground state may lead to the ultrafast non-statistical internal conversion through a conical intersection. We also discuss the implication of our results to the photo-initiated non-adiabatic dynamics in the proteins.

  15. Dynamical analysis of a weakly coupled nonlinear dielectric waveguide -- surface-plasmon model as a new type of Josephson Junction

    CERN Document Server

    Ekşioğlu, Yasa; Güven, Kaan

    2011-01-01

    We propose that a weakly-coupled nonlinear dielectric waveguide -- surface-plasmon system can be formulated as a new type of Josephson junction. Such a system can be realized along a metal - dielectric interface where the dielectric medium hosts a nonlinear waveguide (e.g. fiber) for soliton propagation. We demonstrate that the system is in close analogy to the bosonic Josephson-Junction (BJJ) of atomic condensates at very low temperatures, yet exhibits different dynamical features. In particular, the inherently dynamic coupling parameter between soliton and surface-plasmon generates self-trapped oscillatory states at nonzero fractional populations with zero and $\\pi$ time averaged phase difference. The salient features of the dynamics are presented in the phase space.

  16. Dynamics and density distributions in a capillary-discharge waveguide with an embedded supersonic jet

    Energy Technology Data Exchange (ETDEWEB)

    Matlis, N. H., E-mail: nmatlis@gmail.com; Gonsalves, A. J.; Steinke, S.; Tilborg, J. van; Shaw, B.; Mittelberger, D. E.; Geddes, C. G. R. [Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); Matlis, E. H. [Department of Aerospace and Mechanical Engineering, University of Notre Dame, Notre Dame, Indiana 46556 (United States); Leemans, W. P. [Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States); Department of Physics, University of California, Berkeley, California 94720 (United States)

    2015-11-28

    We present an analysis of the gas dynamics and density distributions within a capillary-discharge waveguide with an embedded supersonic jet. This device provides a target for a laser plasma accelerator which uses longitudinal structuring of the gas-density profile to enable control of electron trapping and acceleration. The functionality of the device depends sensitively on the details of the density profile, which are determined by the interaction between the pulsed gas in the jet and the continuously-flowing gas in the capillary. These dynamics are captured by spatially resolving recombination light from several emission lines of the plasma as a function of the delay between the jet and the discharge. We provide a phenomenological description of the gas dynamics as well as a quantitative evaluation of the density evolution. In particular, we show that the pressure difference between the jet and the capillary defines three regimes of operation with qualitatively different longitudinal density profiles and show that jet timing provides a sensitive method for tuning between these regimes.

  17. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-01-01

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

  19. 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.

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

    Science.gov (United States)

    Klamroth, Tillmann

    2006-04-01

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

  1. Revealing the ultrafast charge carrier dynamics in organo metal halide perovskite solar cell materials using time resolved THz spectroscopy.

    Science.gov (United States)

    Ponseca, C S; Sundström, V

    2016-03-28

    Ultrafast charge carrier dynamics in organo metal halide perovskite has been probed using time resolved terahertz (THz) spectroscopy (TRTS). Current literature on its early time characteristics is unanimous: sub-ps charge carrier generation, highly mobile charges and very slow recombination rationalizing the exceptionally high power conversion efficiency for a solution processed solar cell material. Electron injection from MAPbI3 to nanoparticles (NP) of TiO2 is found to be sub-ps while Al2O3 NPs do not alter charge dynamics. Charge transfer to organic electrodes, Spiro-OMeTAD and PCBM, is sub-ps and few hundreds of ps respectively, which is influenced by the alignment of energy bands. It is surmised that minimizing defects/trap states is key in optimizing charge carrier extraction from these materials.

  2. Ultrafast carrier dynamics in type II ZnSe/CdS/ZnSe nanobarbells.

    Science.gov (United States)

    Hewa-Kasakarage, Nishshanka N; El-Khoury, Patrick Z; Tarnovsky, Alexander N; Kirsanova, Maria; Nemitz, Ian; Nemchinov, Alexander; Zamkov, Mikhail

    2010-04-27

    We employ femtosecond transient absorption spectroscopy to get an insight into ultrafast processes occurring at the interface of type II ZnSe/CdS heterostructured nanocrystals fabricated via colloidal routes and comprising a barbell-like arrangement of ZnSe tips and CdS nanorods. Our study shows that resonant excitation of ZnSe tips results in an unprecedently fast transfer of excited electrons into CdS domains of nanobarbells (ZnSe tips (tau(h)= 95 ps). A qualitative thermodynamic description of observed electron processes within the classical limit of Marcus theory was used to identify a specific charge transfer regime associated with the ultrafast electron injection into CdS. Potential photocatalytic applications of the observed fast separation of carriers along the main axis of ZnSe/CdS barbells are discussed.

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

    OpenAIRE

    Park, Hyuk; Zuo, Jian-Min

    2010-01-01

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

  4. Probing ultrafast dynamics of condensed matter with pump and probe experiments with X-rays

    Energy Technology Data Exchange (ETDEWEB)

    Giles, Carlos; Celestre, Rafael; Tasca, Kelin R.; Vescovi, Rafael; Faria, Guilherme; Dias, Carlos S.; Tomm, Natasha; Cordeiro, Cristiano M.B. [Universidade Estadual de Campinas (IFGW/UNICAMP), SP (Brazil). Inst. de Fisica Gleb Wataghin; Silva, Rene Nome [Universidade Estadual de Campinas (IQ/UNICAMP), SP (Brazil). Inst. de Quimica

    2012-07-01

    Full text: In this presentation we will describe recent advances in the route to start ultrafast studies with X-rays in Brazil. From one side pump and probe experiments using synchrotron radiation facilities will be described, showing how the thermal expansion of an invar alloy is not occurring at the picosecond time scales after heating the sample with a femtosecond infrared laser pulse. We will also describe the experimental setup at the LNLS in Campinas were we probe the fast response of a piezoelectric material to a 1 ns electric pulse recorded by a pump and probe X-ray diffraction experiment at the XRD2 LNLS beamline. We will also present the first results of the production of sub-picosecond X-ray pulses using an amplified infrared laser at the Ultrafast Laboratory of DEQ/IFGW. The instrumentation developed at UNICAMP together with the first setup for a pump and probe experiment will be presented. Characteristic radiation of various targets (TiK{alpha}, FeK{alpha}, CuK{alpha}) have been measured at a repetition rate of 1 kHz showing unambiguously our capability of producing a pulsed X-ray source for time resolved x-ray diffraction experiments. Experiments to measure the pulse width of the X-ray radiation are under development and the latest results will be presented. All these efforts open the path to the nucleation of a research group in ultrafast studies using X-rays in Brazil. (author)

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

    Science.gov (United States)

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

    2016-04-01

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

  6. 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.

  7. Ultrafast dynamics of C30 in solution and within CDs and HSA protein.

    Science.gov (United States)

    Martin, Cristina; Cohen, Boiko; Gaamoussi, Issam; Ijjaali, Mustapha; Douhal, Abderrazzak

    2014-05-29

    Steady-state UV-visible absorption and emission together with femto to nanosecond time-resolved emission techniques have been applied to study the dynamics of 3-(2-N-methylbenzimidazolyl)-7-(N,N-diethylamino)coumarin (C30) in neat solvents, as well as in the presence of chemical (β-CD and DM-β-CD) and biological (HSA protein) cavities. The formation of inclusion complexes inside the hydrophobic CDs gives 1:1 and 1:2 guest:host complexes, whereas with the HSA protein, the formed 1:1 inclusion complexes are more robust. The picosecond experiments show the importance of the interactions of C30 with the medium, as well as the intramolecular events in the excited-state relaxation as evidenced by the increase in the global emission lifetime from ∼0.5 ns in MeOH/H2O mixtures to 2.5 ns in THF, and to 1-3 ns when the dye is trapped within CDs and HSA cavities. Time-resolved anisotropy (r(t)) results indicate the involvement of ultrafast depolarization processes, whereas in the MeOH/H2O mixtures r(0) = 0.27, in DM-β-CD, r(0) = 0.35. The rotational time decays clearly show the robustness of the formed complexes with CDs and HSA protein: ∼170 ps in MeOH/H2O solvent mixtures, ∼850 ps due to 1:1 and 1:2 β-CD complexes, and 28 ns for HSA complexes. The femtosecond time-resolved emission experiments reveal the significant changes of the dynamics with the encapsulation of C30 by CDs (from approximately τ1 = 0.3 and τ2 = 2 ps in THF to approximately τ1 = 1.0 and τ2 = 7.5 ps in the MeOH/H2O binary mixture, and to approximately τ1 = 3 and τ2 = 30 ps in the CD complexes). The change is explained in terms of how the water molecules modulate the intramolecular charge transfer (ICT) time (τ1) and how the restriction of the environment modifies the torsional process (τ2). In the case of trapped C30 within the HSA protein the intermolecular interactions with the amino acid residues are revealed, giving rise to a complex photodynamical behavior due to the hydrophobic, H

  8. All-optical thermal microscopy of laser-excited waveguides

    OpenAIRE

    He, R.; De Aldana, J.R.V.; Pedrola, G.L.; Chen, F.; JAQUE, D.

    2016-01-01

    We report on a unique combination of high-resolution confocal microscopy and ratiometric luminescence thermometry to obtain thermal images of 800 nm pumped ultrafast laser-inscribed waveguides in a Nd:YAG crystal. Thermal images evidence a strong localization of thermal load in the waveguide active volume. Comparison between experimental data and numerical simulations reveals that ultrafast laser-inscribed damage tracks in Nd:YAG crystals behave both as low-index and low-thermal conductivity ...

  9. 19th International Conference on Ultrafast Phenomena

    CERN Document Server

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

    2015-01-01

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

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

    Science.gov (United States)

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

    2011-08-04

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

  11. Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+

    CERN Document Server

    Biasin, Elisa; Kjær, Kasper S; Dohn, Asmus O; Christensen, Morten; Harlang, Tobias; Chabera, Pavel; Liu, Yizhu; Uhlig, Jens; Pápai, Mátyás; Németh, Zoltán; Hartsock, Robert; Liang, Winnie; Zhang, Jianxin; Alonso-Mori, Roberto; Chollet, Matthieu; Glownia, James M; Nelson, Silke; Sokaras, Dimosthenis; Assefa, Tadesse A; Britz, Alexander; Galler, Andreas; Gawelda, Wojciech; Bressler, Christian; Gaffney, Kelly J; Lemke, Henrik T; Møller, Klaus B; Nielsen, Martin M; Sundström, Villy; Vankó, György; Wärnmark, Kenneth; Canton, Sophie E; Haldrup, Kristoffer

    2016-01-01

    We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ~ 7 ps.

  12. Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co (terpy)2]2 +

    Science.gov (United States)

    Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S.; Dohn, Asmus O.; Christensen, Morten; Harlang, Tobias; Chabera, Pavel; Liu, Yizhu; Uhlig, Jens; Pápai, Mátyás; Németh, Zoltán; Hartsock, Robert; Liang, Winnie; Zhang, Jianxin; Alonso-Mori, Roberto; Chollet, Matthieu; Glownia, James M.; Nelson, Silke; Sokaras, Dimosthenis; Assefa, Tadesse A.; Britz, Alexander; Galler, Andreas; Gawelda, Wojciech; Bressler, Christian; Gaffney, Kelly J.; Lemke, Henrik T.; Møller, Klaus B.; Nielsen, Martin M.; Sundström, Villy; Vankó, György; Wärnmark, Kenneth; Canton, Sophie E.; Haldrup, Kristoffer

    2016-07-01

    We study the structural dynamics of photoexcited [Co (terpy)2]2 + in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ˜7 ps .

  13. Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)_{2}]^{2+}.

    Science.gov (United States)

    Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S; Dohn, Asmus O; Christensen, Morten; Harlang, Tobias; Chabera, Pavel; Liu, Yizhu; Uhlig, Jens; Pápai, Mátyás; Németh, Zoltán; Hartsock, Robert; Liang, Winnie; Zhang, Jianxin; Alonso-Mori, Roberto; Chollet, Matthieu; Glownia, James M; Nelson, Silke; Sokaras, Dimosthenis; Assefa, Tadesse A; Britz, Alexander; Galler, Andreas; Gawelda, Wojciech; Bressler, Christian; Gaffney, Kelly J; Lemke, Henrik T; Møller, Klaus B; Nielsen, Martin M; Sundström, Villy; Vankó, György; Wärnmark, Kenneth; Canton, Sophie E; Haldrup, Kristoffer

    2016-07-01

    We study the structural dynamics of photoexcited [Co(terpy)_{2}]^{2+} in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ∼7  ps.

  14. 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.

  15. Ultrafast in cellulo photoinduced dynamics processes of the paradigm molecular light switch [Ru(bpy)2dppz](2.).

    Science.gov (United States)

    De la Cadena, Alejandro; Davydova, Dar'ya; Tolstik, Tatiana; Reichardt, Christian; Shukla, Sapna; Akimov, Denis; Heintzmann, Rainer; Popp, Jürgen; Dietzek, Benjamin

    2016-09-20

    An in cellulo study of the ultrafast excited state processes in the paradigm molecular light switch [Ru(bpy)2dppz](2+) by localized pump-probe spectroscopy is reported for the first time. The localization of [Ru(bpy)2dppz](2+) in HepG2 cells is verified by emission microscopy and the characteristic photoinduced picosecond dynamics of the molecular light switch is observed in cellulo. The observation of the typical phosphorescence stemming from a (3)MLCT state suggests that the [Ru(bpy)2dppz](2+) complex intercalates with the DNA in the nucleus. The results presented for this benchmark coordination compound reveal the necessity to study the photoinduced processes in coordination compounds for intracellular use, e.g. as sensors or as photodrugs, in the actual biological target environment in order to derive a detailed molecular mechanistic understanding of the excited-state properties of the systems in the actual biological target environment.

  16. Ultrafast in cellulo photoinduced dynamics processes of the paradigm molecular light switch [Ru(bpy)2dppz]2+

    Science.gov (United States)

    De la Cadena, Alejandro; Davydova, Dar’ya; Tolstik, Tatiana; Reichardt, Christian; Shukla, Sapna; Akimov, Denis; Heintzmann, Rainer; Popp, Jürgen; Dietzek, Benjamin

    2016-01-01

    An in cellulo study of the ultrafast excited state processes in the paradigm molecular light switch [Ru(bpy)2dppz]2+ by localized pump-probe spectroscopy is reported for the first time. The localization of [Ru(bpy)2dppz]2+ in HepG2 cells is verified by emission microscopy and the characteristic photoinduced picosecond dynamics of the molecular light switch is observed in cellulo. The observation of the typical phosphorescence stemming from a 3MLCT state suggests that the [Ru(bpy)2dppz]2+ complex intercalates with the DNA in the nucleus. The results presented for this benchmark coordination compound reveal the necessity to study the photoinduced processes in coordination compounds for intracellular use, e.g. as sensors or as photodrugs, in the actual biological target environment in order to derive a detailed molecular mechanistic understanding of the excited-state properties of the systems in the actual biological target environment. PMID:27644587

  17. Ultrafast in cellulo photoinduced dynamics processes of the paradigm molecular light switch [Ru(bpy)2dppz]2+

    Science.gov (United States)

    de La Cadena, Alejandro; Davydova, Dar'Ya; Tolstik, Tatiana; Reichardt, Christian; Shukla, Sapna; Akimov, Denis; Heintzmann, Rainer; Popp, Jürgen; Dietzek, Benjamin

    2016-09-01

    An in cellulo study of the ultrafast excited state processes in the paradigm molecular light switch [Ru(bpy)2dppz]2+ by localized pump-probe spectroscopy is reported for the first time. The localization of [Ru(bpy)2dppz]2+ in HepG2 cells is verified by emission microscopy and the characteristic photoinduced picosecond dynamics of the molecular light switch is observed in cellulo. The observation of the typical phosphorescence stemming from a 3MLCT state suggests that the [Ru(bpy)2dppz]2+ complex intercalates with the DNA in the nucleus. The results presented for this benchmark coordination compound reveal the necessity to study the photoinduced processes in coordination compounds for intracellular use, e.g. as sensors or as photodrugs, in the actual biological target environment in order to derive a detailed molecular mechanistic understanding of the excited-state properties of the systems in the actual biological target environment.

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

    Science.gov (United States)

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

    2016-05-01

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

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

    Directory of Open Access Journals (Sweden)

    D. S. Badali

    2016-05-01

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

  20. Ultrafast carrier dynamics in purified and as-grown single-walled carbon nanotube films

    Institute of Scientific and Technical Information of China (English)

    Long Yong-Bing; Song Li; Zhang Chun-Yu; Wang Li; Fu Pan-Ming; Zhang Zhi-Guo; Xie Si-Shen; Wang Guo-Ping

    2005-01-01

    Ultrafast time-resolved optical transmissions in purified and as-grown single-walled carbon nanotube films are measured at a temperature of 200K. The signal of the purified sample shows a crossover from photobleaching to photoabsorption. The former and the latter are interpreted as the state filling and the red shift of the π-plasmon,respectively. The signal of the as-grown sample can be perfectly fitted by a single-exponential with a time constant of 232fs. The disappearance of the negative component in the as-grown sample is attributed to the charge transfer between the semiconducting nanotubes and the impurities.

  1. Statistics of decay dynamics of quantum emitters in disordered photonic-crystal waveguides

    DEFF Research Database (Denmark)

    Javadi, Alisa; Garcia-Fernandez, Pedro David; Sapienza, Luca;

    2014-01-01

    We present a statistical analysis of the spontaneous emission of quantum dots coupled to Anderson-localized cavities in disordered photonic-crystal waveguides.We observe an average Purcell factor of ∼ 5 with a maximum value of 24.......We present a statistical analysis of the spontaneous emission of quantum dots coupled to Anderson-localized cavities in disordered photonic-crystal waveguides.We observe an average Purcell factor of ∼ 5 with a maximum value of 24....

  2. Ultrafast relaxation dynamics of photoexcited Dirac fermions in the three-dimensional Dirac semimetal C d3A s2

    Science.gov (United States)

    Lu, Wei; Ge, Shaofeng; Liu, Xuefeng; Lu, Hong; Li, Caizhen; Lai, Jiawei; Zhao, Chuan; Liao, Zhimin; Jia, Shuang; Sun, Dong

    2017-01-01

    Three-dimensional (3D) Dirac semimetals that can be seen as 3D analogues of graphene have attracted enormous interest in research recently. In order to apply these ultra-high-mobility materials in future electronic/optoelectronic devices, it is crucial to understand the relaxation dynamics of photoexcited carriers and their coupling with lattice. In this paper, we report ultrafast transient reflection measurements of the photoexcited carrier dynamics in cadmium arsenide (C d3A s2 ), which is one of the most stable Dirac semimetals that have been confirmed experimentally. By using the low-energy probe photon of 0.3 eV, we probed the dynamics of the photoexcited carriers that are Dirac-Fermi-like approaching the Dirac point. We systematically studied the transient reflection on bulk and nanoplate samples that have different doping intensities by tuning the probe wavelength, pump power, and lattice temperature and find that the dynamical evolution of carrier distributions can be retrieved qualitatively by using a two-temperature model. This result is very similar to that of graphene, but the carrier cooling through the optical phonon couplings is slower and lasts over larger electron temperature range because the optical phonon energies in C d3A s2 are much lower than those in graphene.

  3. Ultra-fast Measurements of Optically Induced Lattice Dynamics in LuMnO3 Using Aluminum K-alpha X-Ray Diffraction.

    Science.gov (United States)

    Workman, J.; Wark, J. S.

    2005-10-01

    An experiment to study the structural dynamics at the ultra-fast time scale in optically-pumped samples is presented. Measurements of lattice dynamics in LuMnO3 are presented and compared to calculations using dynamical diffraction theory modified for hexagonal crystal structure. Ultra-fast x-ray emission is used to measure Bragg peak shifts using diffraction and compared to calculations. Results are presented for optical pump energy densities of 8 and 20-mJ/cm^2. The experiment uses ˜150 mJ of a 100fs Ti:Sapphire laser to excite K-alpha x-ray emission in an aluminum wire with ˜1-2% split off for the material pump. The x-ray emission is relayed using a spherical Quartz crystal to the sample target. Plans for experiments using Cu K-alpha emission to probe Fe samples will also be described.

  4. 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

  5. Ultrafast Excited-State Decays in [Re(CO)3(N,N)(L)](n+): Nonadiabatic Quantum Dynamics.

    Science.gov (United States)

    Fumanal, Maria; Gindensperger, Etienne; Daniel, Chantal

    2017-03-14

    The ultrafast luminescent decay of [Re(CO)3(phen)(im)](+), representative of Re(I) carbonyl α-diimine photosensitizers, is investigated by means of wavepacket propagations based on the multiconfiguration time-dependent Hartree (MCTDH) method. On the basis of electronic structure data obtained at the time-dependent density functional theory (TD-DFT) level, the luminescence decay is simulated by solving a 14 electronic states multimode problem including both vibronic and spin-orbit coupling (SOC) up to 15 vibrational modes. A careful analysis of the results provides the key features of the mechanism of the intersystem crossing (ISC) in this complex. The intermediate state, detected by means of fs - ps time-resolved spectroscopies, is assigned to the T3 state corresponding to the triplet intraligand ((3)IL) transition localized on the phen ligand. By switching off/on SOC and vibronic coupling in the model it is shown that efficient population transfer occurs from the optically active metal-to-ligand-charge-transfer1,3MLCT states to T3 and to the lowest long-lived phosphorescent (3)MLCT (T1) state. The early ultrafast SOC-driven decay followed by a T3/T1 equilibration controlled by vibronic coupling underlies the photoluminescent properties of [Re(CO)3(phen)(im)](+). The impact of the axial and N,N ligands on the photophysics of this class of Re(I) complexes is further rationalized on the basis of their calculated optical properties. The relative position of the (3)IL and upper (3)MLCT states with respect to the optically active singlet state is influenced by the N,N ligand and affects the relaxation dynamics.

  6. Prospect of detection and recognition of single biological molecules using ultrafast coherent dynamics in quantum dot-metallic nanoparticle systems

    Science.gov (United States)

    Sadeghi, S. M.

    2015-08-01

    Conventional plasmonic sensors are based on the intrinsic resonances of metallic nanoparticles. In such sensors wavelength shift of such resonances are used to detect biological molecules. Recently we introduced ultra-sensitive timedomain nanosensors based on the way variations in the environmental conditions influence coherent dynamics of hybrid systems consisting of metallic nanoparticles and quantum dots. Such dynamics are generated via interaction of these systems with a laser field, generating quantum coherence and coherent exciton-plasmon coupling. These sensors are based on impact of variations of the refractive index of the environment on such dynamics, generating time-dependent changes in the emission of the QDs. In this paper we study the impact of material properties of the metallic nanoparticles on this process and demonstrate the key role played by the design of the quantum dots. We show that Ag nanoparticles, even in a simple spherical shape, may allow these sensors to operate at room temperature, owing to the special properties of quantum dot-metallic nanoparticle systems that may allow coherent effects utilized in such sensors happen in the presence of the ultrafast polarization dephasing of quantum dots.

  7. Nonlinear optical localization in embedded chalcogenide waveguide arrays

    Directory of Open Access Journals (Sweden)

    Mingshan Li

    2014-05-01

    Full Text Available We report the nonlinear optical localization in an embedded waveguide array fabricated in chalcogenide glass. The array, which consists of seven waveguides with circularly symmetric cross sections, is realized by ultrafast laser writing. Light propagation in the chalcogenide waveguide array is studied with near infrared laser pulses centered at 1040 nm. The peak intensity required for nonlinear localization for the 1-cm long waveguide array was 35.1 GW/cm2, using 10-nJ pulses with 300-fs pulse width, which is 70 times lower than that reported in fused silica waveguide arrays and with over 7 times shorter interaction distance. Results reported in this paper demonstrated that ultrafast laser writing is a viable tool to produce 3D all-optical switching waveguide circuits in chalcogenide glass.

  8. Ultrafast Structural Dynamics of BlsA, a Photoreceptor from the Pathogenic Bacterium Acinetobacter baumannii

    Science.gov (United States)

    2013-01-01

    Acinetobacter baumannii is an important human pathogen that can form biofilms and persist under harsh environmental conditions. Biofilm formation and virulence are modulated by blue light, which is thought to be regulated by a BLUF protein, BlsA. To understand the molecular mechanism of light sensing, we have used steady-state and ultrafast vibrational spectroscopy to compare the photoactivation mechanism of BlsA to the BLUF photosensor AppA from Rhodobacter sphaeroides. Although similar photocycles are observed, vibrational data together with homology modeling identify significant differences in the β5 strand in BlsA caused by photoactivation, which are proposed to be directly linked to downstream signaling. PMID:24723998

  9. 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.

  10. Dynamic high pressure measurements using a Fiber Bragg Grating probe and an arrayed waveguide grating spectrometer

    Science.gov (United States)

    Barbarin, Y.; Lefrançois, A.; Magne, S.; Woirin, K.; Sinatti, F.; Osmont, A.; Luc, J.

    2016-08-01

    High pressure shock profiles are monitored using a long Fiber Bragg Grating (FBG). Such thin probe, with a diameter of typically 150 μm, can be inserted directly into targets for shock plate experiments. The shocked FBG's portion is stressed under compression, which increases its optical group index and shortens its grating period. Placed along the 2D symmetrical axis of the cylindrical target, the second effect is stronger and the reflected spectrum shifts towards the shorter wavelengths. The dynamic evolution of FBG spectra is recorded with a customized Arrayed Waveguide Grating (AWG) spectrometer covering the C+L band. The AWG provides 40 channels of 200-GHz spacing with a special flattop design. The output channels are fiber-connected to photoreceivers (bandwidth: DC - 400 MHz or 10 kHz - 2 GHz). The experimental setup was a symmetric impact, completed in a 110-mm diameter single-stage gas gun with Aluminum (6061T6) impactors and targets. The FBG's central wavelength was 1605 nm to cover the pressure range of 0 - 8 GPa. The FBG was 50-mm long as well as the target's thickness. The 20-mm thick impactor maintains a shock within the target over a distance of 30 mm. For the impact at 522 m/s, the sustained pressure of 3.6 GPa, which resulted in a Bragg shift of (26.2 +/- 1.5) nm, is measured and retrieved with respectively thin-film gauges and the hydrodynamic code Ouranos. The shock sensitivity of the FBG is about 7 nm/GPa, but it decreases with the pressure level. The overall spectra evolution is in good agreement with the numerical simulations.

  11. Nonlinear Dynamics of Ultrashort Long-Range Surface Plasmon Polariton Pulses in Gold Strip Waveguides

    DEFF Research Database (Denmark)

    Lysenko, Oleg; Bache, Morten; Olivier, Nicolas

    2016-01-01

    We study experimentally and theoretically nonlinear propagation of ultrashort long-range surface plasmon polaritons in gold strip waveguides. The nonlinear absorption of the plasmonic modes in the waveguides is measured with femtosecond pulses revealing a strong dependence of the third......-order nonlinear susceptibility of the gold core on the pulse duration and layer thickness. A comprehensive model for the pulse duration dependence of the third-order nonlinear susceptibility is developed on the basis of the nonlinear Schrödinger equation for plasmonic mode propagation in the waveguides....... The model accounts for the intrinsic delayed (noninstantaneous) nonlinearity of free electrons of gold as well as the thickness of the gold film and is experimentally verified. The obtained results are important for the development of active plasmonic and nanophotonic components....

  12. Ultrafast Transient Absorption Spectroscopy Investigation of Photoinduced Dynamics in Novel Donor-Acceptor Core-Shell Nanostructures for Organic Photovoltaics

    Science.gov (United States)

    Strain, Jacob; Jamhawi, Abdelqader; Abeywickrama, Thulitha M.; Loomis, Wendy; Rathnayake, Hemali; Liu, Jinjun

    2016-06-01

    Novel donor-acceptor nanostructures were synthesized via covalent synthesis and/or UV cross-linking method. Their photoinduced dynamics were investigated with ultrafast transient absorption (TA) spectroscopy. These new nanostructures are made with the strategy in mind to reduce manufacturing steps in the process of fabricating an organic photovoltaic cell. By imitating the heterojunction interface within a fixed particle domain, several fabrication steps can be bypassed reducing cost and giving more applicability to other film deposition methods. Such applications include aerosol deposition and ink-jet printing. The systems that were studied by TA spectroscopy include PDIB core, PDIB-P3HT core-shell, and PDIB-PANT core-shell which range in size from 60 to 130 nm. Within the experimentally accessible spectra range there resides a region of ground state bleaching, stimulated emission, and excited-state absorption of both neutrals and anions. Control experiments have been carried out to assign these features. At high pump fluences the TA spectra of PDIB core alone also indicate an intramolecular charge separation. The TA spectroscopy results thus far suggest that the core-shells resemble the photoinduced dynamics of a standard film although the particles are dispersed in solution, which indicates the desired outcome of the work.

  13. Ultrafast carrier dynamics of CdSe quantum dots prepared by pulse laser deposition for photovoltaic applications

    Science.gov (United States)

    Mahat, Meg; Yakami, Baichhabi; Qilin Dai, Qilin; Tang, Jinke; Pikal, Jon

    2013-03-01

    Quantum-dot sensitized solar cells are a promising alternative to existing photovoltaic technology. Over the last decade solution based colloidal quantum dots (QDs) have been extensively studied. Here we have carried out ultrafast transient absorption measurements on CdSe QDs fabricated using pulse laser deposition (PLD) in order to understand the carrier relaxation dynamics in these nanostructures. The differential transmission measurements show that the PLD QDs have a very fast decay process resulting in a recovery time of less than 10 picoseconds. This is in stark contrast to the colloidal QDs that show a decay process of more than 4 nanoseconds. We also find that the fast decay process observed in the PLD QDs is a function of the carriers density generated in CdSe QDs. To understand these carrier relaxation processes and improve the optical properties of the QDs we perform transient absorption measurements on PLD QDs prepared in different media (e.g. water, methanol, ethanol), under different growth conditions, and with and without ligand. We present a comparison study of the carrier relaxation dynamics in these PLD grown QDs to provide insight into the competing relaxation effects and guide their use in Quantum-dot sensitized solar cells. DOE

  14. Ultrafast Excited-State Dynamics of V3O5 as a Signature of a Photoinduced Insulator-Metal Phase Transition

    Science.gov (United States)

    Kumar, Nardeep; Rúa, Armando; Lu, Junqiang; Fernández, Félix; Lysenko, Sergiy

    2017-08-01

    The ultrafast elastic light scattering technique is applied to reveal the strong nonlinearity of V3O5 associated with a photoinduced insulator-metal phase transition. Observation of time-domain relaxation dynamics suggests several stages of structural transition. We discuss the nonequilibrium processes in V3O5 in terms of photoinduced melting of a polaronic Wigner crystal, coalescence of V-O octahedra, and photogeneration of acoustical phonons in the low-T and high-T phases of V3O5 . A molecular dynamics computation supports experimentally observed stages of V3O5 relaxation dynamics.

  15. Ultrafast excited state dynamics of Pt(II) chromophores bearing multiple infrared absorbers.

    Science.gov (United States)

    Glik, Elena A; Kinayyigit, Solen; Ronayne, Kate L; Towrie, Michael; Sazanovich, Igor V; Weinstein, Julia A; Castellano, Felix N

    2008-08-04

    The paper reports the synthesis, structural characterization, electrochemistry, ultrafast time-resolved infrared (TRIR) and transient absorption (TA) spectroscopy associated with two independent d (8) square planar Pt(II) diimine chromophores, Pt(dnpebpy)Cl 2 ( 1) and Pt(dnpebpy)(C[triple bond]Cnaph) 2 ( 2), where dnpebpy = 4,4'-(CO 2CH 2- (t) Bu) 2-2,2'-bipyridine and CCnaph = naphthylacetylide. The neopentyl ester substitutions provided markedly improved complex solubility relative to the corresponding ethyl ester which facilitates synthetic elaboration as well as spectroscopic investigations. Following 400 nm pulsed laser excitation in CH 2Cl 2, the 23 cm (-1) red shift in the nu C=O vibrations in 1 are representative of a complex displaying a lowest charge-transfer-to-diimine (CT) excited state. The decay kinetics in 1 are composed of two time constants assigned to vibrational cooling of the (3)CT excited-state concomitant with its decay to the ground state (tau = 2.2 +/- 0.4 ps), and to cooling of the formed vibrationally hot ground electronic state (tau = 15.5 +/- 4.0 ps); we note that an assignment of the latter to a ligand field state cannot be excluded. Ultrafast TA data quantitatively support these assignments yielding an excited-state lifetime of 2.7 +/- 0.4 ps for the (3)CT excited-state of 1 and could not detect any longer-lived species. The primary intention of this study was to develop a Pt (II) complex ( 2) bearing dual infrared spectroscopic tags (C[triple bond]C attached to the metal and CO (ester) attached to the diimine ligand) to independently track the movement of charge density in different segments of the molecule following pulsed light excitation. Femtosecond laser excitation of 2 in CH 2Cl 2 at 400 nm simultaneously induces a red-shift in both the nu C=O (-30 cm (-1)) and the nu C[triple bond]C (-61 cm (-1)) vibrations. The TRIR data in 2 are consistent with a charge transfer assignment, and the significant decrease of the energy of the nu

  16. Ultrafast dynamics of a series multi-branched styryl derivatives with reverse conjugated structural configuration

    Science.gov (United States)

    Wang, Yaochuan; Jiang, Yihua; Wang, Yizhuo; Wang, Guiqiu; Liu, Dajun; Hua, Jianli

    2017-07-01

    To study the effect of conjugated structural configurations on the two-photon absorption properties, tri-branched compounds with the same electron-donating and electron-accepting groups connected in a reverse conjugated structural mode, are systematically investigated using steady-state and transient absorption spectroscopies, open-aperture Z-scan, and two-photon fluorescence measurements. The two-photon absorption cross-section of compound R03 with the strong electron donor triphenylamine as the central core of 766 GM is notably large and is approximately 1.7 times larger than that of the tri-branched compound T03-a with a reverse conjugated structural mode and with the 1,3,5-triazine electron acceptor as the central core. This finding indicates that the conjugated mode does have an important effect on the nonlinear optical properties. A two-color pump-probe experiment is used to investigate the ultrafast responses and intra-molecular charge transfer properties of these multi-branched compounds. The formation and relaxation lifetimes of the intra-molecular charge transfer state are determined to be in the ranges of several picoseconds and several hundreds of picoseconds, respectively, for all of the compounds in CHCl3 solutions. An extended π-conjugated system, increased intra-molecular cooperative effect, and effective direction of charge transfer are responsible for the observed large two-photon absorption character.

  17. Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells

    Science.gov (United States)

    Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M.; Vezie, Michelle S.; Few, Sheridan; Bazán, Claudia M.; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R.

    2016-01-01

    All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less. PMID:27412119

  18. Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells

    Science.gov (United States)

    Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M.; Vezie, Michelle S.; Few, Sheridan; Bazán, Claudia M.; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R.

    2016-07-01

    All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less.

  19. On the ultrafast photo-induced dynamics of α-terpinene

    Science.gov (United States)

    Gao, Yan; Pemberton, Christine C.; Zhang, Yao; Weber, Peter M.

    2016-05-01

    The ultrafast relaxation pathway of α-terpinene was studied by photoionization-photoelectron spectroscopy for a range of excitation conditions. Time-resolved spectra were obtained upon optical excitation with ultrashort laser pulses at 5.56 eV, 4.96 eV, 4.76 eV, and 4.56 eV, followed by ionization with 3.06 eV pulses. The experiments yielded spectra of the initially excited state, which decays with a time constant of 66 fs, independent of the excitation wavelength. We also observed a sequential series of Rydberg peaks, including the s, p, and d states with n = 3-6, which capture the travel times on the ensuing reaction path. There is no statistically significant dependence of the travel time on the excitation energy. A comparison of the time-dependent signals with those of the un-substituted parent molecule, 1,3-cyclohexadiene, shows that the substituents on α-terpinene slow the reaction down by a factor of about 2.

  20. Nonlinear Integrated Optical Waveguides in Chalcogenide Glasses

    Institute of Scientific and Technical Information of China (English)

    Yinlan; Ruan; Barry; Luther-Davies; Weitang; Li; Andrei; Rode; Marek; Samoc

    2003-01-01

    This paper reports on the study and measurement of the third order optical nonlinearity in bulk sulfide-based chalcogenide glasses; The fabrication process of the ultrafast laser deposited As-S-(Se)-based chalcogenide films and optical waveguides using two techniques: wet chemistry etching and plasma etching.

  1. Light, Molecules, Action: Using Ultrafast Uv-Visible and X-Ray Spectroscopy to Probe Excited State Dynamics in Photoactive Molecules

    Science.gov (United States)

    Sension, R. J.

    2017-06-01

    Light provides a versatile energy source capable of precise manipulation of material systems on size scales ranging from molecular to macroscopic. Photochemistry provides the means for transforming light energy from photon to process via movement of charge, a change in shape, a change in size, or the cleavage of a bond. Photochemistry produces action. In the work to be presented here ultrafast UV-Visible pump-probe, and pump-repump-probe methods have been used to probe the excited state dynamics of stilbene-based molecular motors, cyclohexadiene-based switches, and polyene-based photoacids. Both ultrafast UV-Visible and X-ray absorption spectroscopies have been applied to the study of cobalamin (vitamin B_{12}) based compounds. Optical measurements provide precise characterization of spectroscopic signatures of the intermediate species on the S_{1} surface, while time-resolved XANES spectra at the Co K-edge probe the structural changes that accompany these transformations.

  2. Dynamic Mass Transfer of Hemoglobin at the Aqueous/Ionic-Liquid Interface Monitored with Liquid Core Optical Waveguide.

    Science.gov (United States)

    Chen, Xuwei; Yang, Xu; Zeng, Wanying; Wang, Jianhua

    2015-08-04

    Protein transfer from aqueous medium into ionic liquid is an important approach for the isolation of proteins of interest from complex biological samples. We hereby report a solid-cladding/liquid-core/liquid-cladding sandwich optical waveguide system for the purpose of monitoring the dynamic mass-transfer behaviors of hemoglobin (Hb) at the aqueous/ionic liquid interface. The optical waveguide system is fabricated by using a hydrophobic IL (1,3-dibutylimidazolium hexafluorophosphate, BBimPF6) as the core, and protein solution as one of the cladding layer. UV-vis spectra are recorded with a CCD spectrophotometer via optical fibers. The recorded spectra suggest that the mass transfer of Hb molecules between the aqueous and ionic liquid media involve accumulation of Hb on the aqueous/IL interface followed by dynamic extraction/transfer of Hb into the ionic liquid phase. A part of Hb molecules remain at the interface even after the accomplishment of the extraction/transfer process. Further investigations indicate that the mass transfer of Hb from aqueous medium into the ionic liquid phase is mainly driven by the coordination interaction between heme group of Hb and the cationic moiety of ionic liquid, for example, imidazolium cation in this particular case. In addition, hydrophobic interactions also contribute to the transfer of Hb.

  3. Ultrafast carrier dynamics and the role of grain boundaries in polycrystalline silicon thin films grown by molecular beam epitaxy

    Science.gov (United States)

    Titova, Lyubov V.; Cocker, Tyler L.; Xu, Sijia; Baribeau, Jean-Marc; Wu, Xiaohua; Lockwood, David J.; Hegmann, Frank A.

    2016-10-01

    We have used time-resolved terahertz spectroscopy to study microscopic photoconductivity and ultrafast photoexcited carrier dynamics in thin, pure, non-hydrogenated silicon films grown by molecular beam epitaxy on quartz substrates at temperatures ranging from 335 °C to 572 °C. By controlling the growth temperature, thin silicon films ranging from completely amorphous to polycrystalline with minimal amorphous phase can be achieved. Film morphology, in turn, determines its photoconductive properties: in the amorphous phase, carriers are trapped in bandtail states on sub-picosecond time scales, while the carriers excited in crystalline grains remain free for tens of picoseconds. We also find that in polycrystalline silicon the photoexcited carrier mobility is carrier-density-dependent, with higher carrier densities mitigating the effects of grain boundaries on inter-grain transport. In a film grown at the highest temperature of 572 °C, the morphology changes along the growth direction from polycrystalline with needles of single crystals in the bulk of the film to small crystallites interspersed with amorphous silicon at the top of the film. Depth profiling using different excitation wavelengths shows corresponding differences in the photoconductivity: the photoexcited carrier lifetime and mobility are higher in the first 100-150 nm from the substrate, suggesting that thinner, low-temperature grown polycrystalline silicon films are preferable for photovoltaic applications.

  4. Resonance effects in thickness-dependent ultrafast carrier and phonon dynamics of topological insulator Bi2Se3

    Science.gov (United States)

    Kim, Sung; Shin, Dong Hee; Kim, Ju Hwan; Jang, Chan Wook; Park, Jun Woo; Lee, Hosun; Choi, Suk-Ho; Kim, Seung Hyun; Yee, Ki-Ju; Bansal, Namrata; Oh, Seongshik

    2016-01-01

    Resonance effects in the thickness-dependent ultrafast carrier and phonon dynamics of topological insulator Bi2Se3 are found irrespective of the kind of substrate by measuring thickness-dependent abrupt changes of pump-probe differential-reflectivity signals (ΔR/R) from Bi2Se3 thin films on four different substrates of poly- and single-crystalline (sc-) ZnO, sc-GaN and SiO2. The absolute peak intensity of the ΔR/R is maximized at ∼t C (6 ∼ 9 quintuple layers), which is not directly related to but is very close to the critical thickness below which the energy gap opens. The intensities of the two phonon modes deduced from the oscillatory behaviors superimposed on the ΔR/R profiles are also peaked at ∼t C for the four kinds of substrates, consistent with the thickness-dependent Raman-scattering behaviors. These resonant effects and others are discussed based on possible physical mechanisms including the effects of three-dimensional carrier depletion and intersurface coupling.

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

    Science.gov (United States)

    Tang, Jau

    2008-04-01

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

  6. Excitation relaxation dynamics and energy transfer in pigment-protein complexes of a dinoflagellate, revealed by ultrafast fluorescence spectroscopy.

    Science.gov (United States)

    Tanaka, Kazunori; Iida, Satoko; Takaichi, Shinichi; Mimuro, Mamoru; Murakami, Akio; Akimoto, Seiji

    2016-12-01

    Photosynthetic light-harvesting complexes, found in aquatic photosynthetic organisms, contain a variety of carotenoids and chlorophylls. Most of the photosynthetic dinoflagellates possess two types of light-harvesting antenna complexes: peridinin (Peri)-chlorophyll (Chl) a/c-protein, as an intrinsic thylakoid membrane complex protein (iPCP), and water-soluble Peri-Chl a-protein, as an extrinsic membrane protein (sPCP) on the inner surface of the thylakoid. Peri is a unique carotenoid that has eight C=C bonds and one C=O bond, which results in a characteristic absorption band in the green wavelength region. In the present study, excitation relaxation dynamics of Peri in solution and excitation energy transfer processes of sPCP and the thylakoid membranes, prepared from the photosynthetic dinoflagellate, Symbiodinium sp., are investigated by ultrafast time-resolved fluorescence spectroscopy. We found that Peri-to-Chl a energy transfer occurs via the Peri S1 state with a time constant of 1.5 ps or 400 fs in sPCP or iPCP, respectively, and that Chl c-to-Chl a energy transfer occurs in the time regions of 350-400 fs and 1.8-2.6 ps.

  7. Ultrafast Dynamics of Hole Injection and Recombination in Organometal Halide Perovskite Using Nickel Oxide as p-Type Contact Electrode.

    Science.gov (United States)

    Corani, Alice; Li, Ming-Hsien; Shen, Po-Shen; Chen, Peter; Guo, Tzung-Fang; El Nahhas, Amal; Zheng, Kaibo; Yartsev, Arkady; Sundström, Villy; Ponseca, Carlito S

    2016-04-01

    There is a mounting effort to use nickel oxide (NiO) as p-type selective electrode for organometal halide perovskite-based solar cells. Recently, an overall power conversion efficiency using this hole acceptor has reached 18%. However, ultrafast spectroscopic investigations on the mechanism of charge injection as well as recombination dynamics have yet to be studied and understood. Using time-resolved terahertz spectroscopy, we show that hole transfer is complete on the subpicosecond time scale, driven by the favorable band alignment between the valence bands of perovskite and NiO nanoparticles (NiO(np)). Recombination time between holes injected into NiO(np) and mobile electrons in the perovskite material is shown to be hundreds of picoseconds to a few nanoseconds. Because of the low conductivity of NiO(np), holes are pinned at the interface, and it is electrons that determine the recombination rate. This recombination competes with charge collection and therefore must be minimized. Doping NiO to promote higher mobility of holes is desirable in order to prevent back recombination.

  8. 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.

  9. 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.

  10. Influence of parameters on light propagation dynamics in optically induced planar waveguide arrays

    Institute of Scientific and Technical Information of China (English)

    2009-01-01

    The diffraction and refraction of light beam in optical periodic structures can be determined by the photonic band-gap structures of spatial frequency.In this paper,by employing the equation governing the nonlinear light propagations in photorefractive crystals,we study the photonic band-gap structures, Bloch modes,and light transmission properties of optically induced planar waveguide arrays.The relationship between the photonic band-gap structures and the light diffraction characteristics is discussed in detail.Then the influence of the parameters of planar waveguide arrays on the band-gaps structures,Bloch modes,and linear light transmissions is analyzed.It is revealed that the linear light transmission properties of waveguide arrays are tightly related to the diffraction relationships determined by band-gap structures.And the Bloch modes corresponding to different transmission bands can be excited by different excitation schemes.Both the increases of the intensity and the period of the array writing beam will lead to the broadening of the forbidden gaps and the concentration of the energy of the Bloch modes to the high-index regions.Furthermore,the broadening of the forbidden gaps will lead to separation and transition between the Bloch modes of neighboring bands around the Bragg angle.Additionally,with the increase of the intensity of the array writing beams,the influences from light intensity will tend to be steady due to the saturation of the photorefractive effect.

  11. Influence of parameters on light propagation dynamics in optically induced planar waveguide arrays

    Institute of Scientific and Technical Information of China (English)

    LIU Sheng; ZHANG Peng; XIAO FaJun; YANG DeXing; ZHAO JianLin

    2009-01-01

    The diffraction and refraction of light beam in optical periodic structures can be determined by the photonic band-gap structures of spatial frequency. In this paper, by employing the equation governing the nonlinear light propagations in photorefractive crystals, we study the photonic band-gap structures,Bloch modes, and light transmission properties of optically induced planar waveguide arrays. The relationship between the photonic band-gap structures and the light diffraction characteristics is discussed in detail. Then the influence of the parameters of planar waveguide arrays on the band-gaps structures, Bloch modes, and linear light transmissions is analyzed. It is revealed that the linear light transmission properties of waveguide arrays are tightly related to the diffraction relationships determined by band-gap structures. And the Bloch modes corresponding to different transmission bands can be excited by different excitation schemes. Both the increases of the intensity and the period of the array writing beam will lead to the broadening of the forbidden gaps and the concentration of the energy of the Bloch modes to the high-index regions. Furthermore, the broadening of the forbidden gaps will lead to separation and transition between the Bloch modes of neighboring bands around the Bragg angle. Additionally, with the increase of the intensity of the array writing beams, the influences from light intensity will tend to be steady due to the saturation of the photorefractive effect.

  12. Investigation of ultrafast photothermal surface expansion and diffusivity in GaAs via laser-induced dynamic gratings

    Energy Technology Data Exchange (ETDEWEB)

    Pennington, D.M.

    1992-04-01

    This thesis details the first direct ultrafast measurements of the dynamic thermal expansion of a surface and the temperature dependent surface thermal diffusivity using a two-color reflection transient grating technique. Studies were performed on p-type, n-type, and undoped GaAs(100) samples over a wide range of temperatures. By utilizing a 90 fs ultraviolet probe with visible excitation beams, the effects of interband saturation and carrier dynamics become negligible; thus lattice expansion due to heating and subsequent contraction caused by cooling provided the dominant influence on the probe. At room temperature a rise due to thermal expansion was observed, corresponding to a maximum net displacement of {approximately} 1 {Angstrom} at 32 ps. The diffracted signal was composed of two components, thermal expansion of the surface and heat flow away from the surface, thus allowing a determination of the rate of expansion as well as the surface thermal diffusivity, D{sub S}. By varying the fringe spacing of the grating, this technique has the potential to separate the signal contributions to the expansion of the lattice in the perpendicular and parallel directions. In the data presented here a large fringe spacing was used, thus the dominant contribution to the rising edge of the signal was expansion perpendicular to the surface. Comparison of he results with a straightforward thermal model yields good agreement over a range of temperatures (20--300{degrees}K). Values for D{sub S} in GaAs were measured and found to be in reasonable agreement with bulk values above 50{degrees}K. Below 50{degrees}K, D{sub S} were determined to be up to an order of magnitude slower than the bulk diffusivity due to increased phonon boundary scattering. The applicability and advantages of the TG technique for studying photothermal and photoacoustic phenomena are discussed.

  13. Investigation of ultrafast photothermal surface expansion and diffusivity in GaAs via laser-induced dynamic gratings

    Energy Technology Data Exchange (ETDEWEB)

    Pennington, Deanna Marie [Univ. of California, Berkeley, CA (United States)

    1992-04-01

    This thesis details the first direct ultrafast measurements of the dynamic thermal expansion of a surface and the temperature dependent surface thermal diffusivity using a two-color reflection transient grating technique. Studies were performed on p-type, n-type, and undoped GaAs(100) samples over a wide range of temperatures. By utilizing a 90 fs ultraviolet probe with visible excitation beams, the effects of interband saturation and carrier dynamics become negligible; thus lattice expansion due to heating and subsequent contraction caused by cooling provided the dominant influence on the probe. At room temperature a rise due to thermal expansion was observed, corresponding to a maximum net displacement of ~ 1 Å at 32 ps. The diffracted signal was composed of two components, thermal expansion of the surface and heat flow away from the surface, thus allowing a determination of the rate of expansion as well as the surface thermal diffusivity, DS. By varying the fringe spacing of the grating, this technique has the potential to separate the signal contributions to the expansion of the lattice in the perpendicular and parallel directions. In the data presented here a large fringe spacing was used, thus the dominant contribution to the rising edge of the signal was expansion perpendicular to the surface. Comparison of he results with a straightforward thermal model yields good agreement over a range of temperatures (20--300°K). Values for DS in GaAs were measured and found to be in reasonable agreement with bulk values above 50°K. Below 50°K, DS were determined to be up to an order of magnitude slower than the bulk diffusivity due to increased phonon boundary scattering. The applicability and advantages of the TG technique for studying photothermal and photoacoustic phenomena are discussed.

  14. Ultrafast Excited State Dynamics in Molecular Motors: Coupling of Motor Length to Medium Viscosity.

    Science.gov (United States)

    Conyard, Jamie; Stacko, Peter; Chen, Jiawen; McDonagh, Sophie; Hall, Christopher R; Laptenok, Sergey P; Browne, Wesley R; Feringa, Ben L; Meech, Stephen R

    2017-03-07

    Photochemically driven molecular motors convert the energy of incident radiation to intramolecular rotational motion. The motor molecules considered here execute four step unidirectional rotational motion. This comprises a pair of successive light induced isomerizations to a metastable state followed by thermal helix inversions. The internal rotation of a large molecular unit required in these steps is expected to be sensitive to both the viscosity of the medium and the volume of the rotating unit. In this work, we describe a study of motor motion in both ground and excited states as a function of the size of the rotating units. The excited state decay is ultrafast, highly non-single exponential, and is best described by a sum of three exponential relaxation components. The average excited state decay time observed for a series of motors with substituents of increasing volume was determined. While substitution does affect the lifetime, the size of the substituent has only a minor effect. The solvent polarity dependence is also slight, but there is a significant solvent viscosity effect. Increasing the viscosity has no effect on the fastest of the three decay components, but it does lengthen the two slower decay times, consistent with them being associated with motion along an intramolecular coordinate displacing a large solvent volume. However, these slower relaxation times are again not a function of the size of the substituent. We conclude that excited state decay arises from motion along a coordinate which does not necessarily require complete rotation of the substituents through the solvent, but is instead more localized in the core structure of the motor. The decay of the metastable state to the ground state through a helix inversion occurs 14 orders of magnitude more slowly than the excited state decay, and was measured as a function of substituent size, solvent viscosity and temperature. In this case neither substituent size nor solvent viscosity influences

  15. Ultrafast and slow charge recombination dynamics of diketopyrrolopyrrole-NiO dye sensitized solar cells.

    Science.gov (United States)

    Zhang, Lei; Favereau, Ludovic; Farré, Yoann; Mijangos, Edgar; Pellegrin, Yann; Blart, Errol; Odobel, Fabrice; Hammarström, Leif

    2016-07-21

    In a photophysical study, two diketopyrrolopyrrole (DPP)-based sensitizers functionalized with 4-thiophenecarboxylic acid as an anchoring group and a bromo (DPPBr) or dicyanovinyl (DPPCN2) group, and a dyad consisting of a DPP unit linked to a naphthalenediimide group (DPP-NDI), were investigated both in solution and grafted on mesoporous NiO films. Femtosecond transient absorption measurements indicate that ultrafast hole injection occurred predominantly on a timescale of ∼200 fs, whereas the subsequent charge recombination occurred on a surprisingly wide range of timescales, from tens of ps to tens of μs; this kinetic heterogeneity is much greater than is typically observed for dye-sensitized TiO2 or ZnO. Also, in contrast to what is typically observed for dye-sensitized TiO2, there was no significant dependence on the excitation power of the recombination kinetics, which can be explained by the hole density being comparatively higher near the valence band of NiO before excitation. The additional acceptor group in DPP-NDI provided a rapid electron shift and stabilized charge separation up to the μs timescale. This enabled efficient (∼95%) regeneration of NDI by a Co(III)(dtb)3 electrolyte (dtb = 4,4'-di-tert-butyl-2,2'-bipyridine), according to transient absorption measurements. The regeneration of DPPBr and DPPCN2 by Co(III)(dtb)3 was instead inefficient, as most recombination for these dyes occurred on the sub-ns timescale. The transient spectroscopy data thus corroborated the trend of the published photovoltaic properties of dye-sensitized solar cells (DSSCs) based on these dyes on mesoporous NiO, and show the potential of a design strategy with a secondary acceptor bound to the dye. The study identifies rapid initial recombination between the dye and NiO as the main obstacle to obtaining high efficiencies in NiO-based DSSCs; these recombination components may be overlooked when studies are conducted using only methods with ns resolution or slower.

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

    Energy Technology Data Exchange (ETDEWEB)

    Radu, I.E.

    2006-03-15

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

  17. Ultrafast coherent dynamics of a photonic crystal all-optical switch

    DEFF Research Database (Denmark)

    Colman, Pierre; Hansen, Per Lunnemann; Yu, Yi

    2016-01-01

    We present pump-probe measurements of an all-optical photonic crystal switch based on a nanocavity, resolving fast coherent temporal dynamics. The measurements demonstrate the importance of coherent effects typically neglected when considering nanocavity dynamics. In particular, we report...

  18. Ultrafast dynamics of solvation and charge transfer in a DNA-based biomaterial.

    Science.gov (United States)

    Choudhury, Susobhan; Batabyal, Subrata; Mondol, Tanumoy; Sao, Dilip; Lemmens, Peter; Pal, Samir Kumar

    2014-05-01

    Charge migration along DNA molecules is a key factor for DNA-based devices in optoelectronics and biotechnology. The association of a significant amount of water molecules in DNA-based materials for the intactness of the DNA structure and their dynamic role in the charge-transfer (CT) dynamics is less documented in contemporary literature. In the present study, we have used a genomic DNA-cetyltrimethyl ammonium chloride (CTMA) complex, a technological important biomaterial, and Hoechest 33258 (H258), a well-known DNA minor groove binder, as fluorogenic probe for the dynamic solvation studies. The CT dynamics of CdSe/ZnS quantum dots (QDs; 5.2 nm) embedded in the as-prepared and swollen biomaterial have also been studied and correlated with that of the timescale of solvation. We have extended our studies on the temperature-dependent CT dynamics of QDs in a nanoenvironment of an anionic, sodium bis(2-ethylhexyl)sulfosuccinate reverse micelle (AOT RMs), whereby the number of water molecules and their dynamics can be tuned in a controlled manner. A direct correlation of the dynamics of solvation and that of the CT in the nanoenvironments clearly suggests that the hydration barrier within the Arrhenius framework essentially dictates the charge-transfer dynamics.

  19. Ultrafast dynamics in semiconductor optical amplifiers and all-optical processing: Bulk versus quantum dot devices

    DEFF Research Database (Denmark)

    Mørk, Jesper; Berg, Tommy Winther; Magnúsdóttir, Ingibjörg

    2003-01-01

    We discuss the dynamical properties of semiconductor optical amplifiers and the importance for all-optical signal processing. In particular, the dynamics of quantum dot amplifiers is considered and it is suggested that these may be operated at very high bit-rates without significant patterning...... effects, as opposed to quantum well or bulk devices....

  20. Ultrafast structural and vibrational dynamics of the hydration shell around DNA

    Directory of Open Access Journals (Sweden)

    Szyc Ł

    2013-03-01

    Full Text Available Two-dimensional infrared spectroscopy in the frequency range of OH- and NH stretch excitations serves for a direct mapping of hydration dynamics around DNA. A moderate slowing down of structural dynamics and resonant OH stretch energy transfer is observed in the DNA water shell compared to bulk water.

  1. Quantum waveguides

    CERN Document Server

    Exner, Pavel

    2015-01-01

    This monograph explains the theory of quantum waveguides, that is, dynamics of quantum particles confined to regions in the form of tubes, layers, networks, etc. The focus is on relations between the confinement geometry on the one hand and the spectral and scattering properties of the corresponding quantum Hamiltonians on the other. Perturbations of such operators, in particular, by external fields are also considered. The volume provides a unique summary of twenty five years of research activity in this area and indicates ways in which the theory can develop further. The book is fairly self-contained. While it requires some broader mathematical physics background, all the basic concepts are properly explained and proofs of most theorems are given in detail, so there is no need for additional sources. Without a parallel in the literature, the monograph by Exner and Kovarik guides the reader through this new and exciting field.

  2. 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...

  3. On the dynamics of persistent states and their secular trends in the waveguides of the Southern Hemisphere troposphere

    Science.gov (United States)

    O'Kane, Terence J.; Risbey, James S.; Monselesan, Didier P.; Horenko, Illia; Franzke, Christian L. E.

    2016-06-01

    We identify the dynamical drivers of systematic changes in persistent quasi-stationary states (regimes) of the Southern Hemisphere troposphere and their secular trends. We apply a purely data-driven approach, whereby a multiscale approximation to nonstationary dynamical processes is achieved through optimal sequences of locally stationary fast vector autoregressive factor processes, to examine a high resolution atmospheric reanalysis over the period encompassing 1958-2013. This approach identifies regimes and their secular trends in terms of the predictability of the flow and is Granger causal. A comprehensive set of diagnostics on both isentropic and isobaric surfaces is employed to examine teleconnections over the full hemisphere and for a set of regional domains. Composite states for the hemisphere obtained from nonstationary nonparametric cluster analysis reveal patterns consistent with a circumglobal wave 3 (polar)-wave 5 (subtropical) pattern, while regional composites reveal the Pacific South American pattern and blocking modes. The respective roles of potential vorticity sources, stationary Rossby waves and baroclinic instability on the dynamics of these circulation modes are shown to be reflected by the seasonal variations of the waveguides, where Rossby wave sources and baroclinic disturbances are largely contained within the waveguides and with little direct evidence of sustained remote tropical influences on persistent synoptic features. Warm surface temperature anomalies are strongly connected with regions of upper level divergence and anticyclonic Rossby wave sources. The persistent states identified reveal significant variability on interannual to decadal time scales with large secular trends identified in all sectors apart from a region close to South America.

  4. Enhanced optical nonlinearities in air-cladding silicon pedestal waveguides

    CERN Document Server

    Zhang, Yaojing; Yao, Yifei; Tsang, Hon Ki

    2016-01-01

    The third-order optical nonlinearity in optical waveguides has found applications in optical switching, optical wavelength conversion, optical frequency comb generation, and ultrafast optical signal processing. The development of an integrated waveguide platform with a high nonlinearity is therefore important for nonlinear integrated photonics. Here, we report the observation of an enhancement in the nonlinearity of an air-cladding silicon pedestal waveguide. We observe enhanced nonlinear spectral broadening compared to a conventional silicon-on-insulator waveguide. At the center wavelength of 1555 nm, the nonlinear-index coefficient of air-cladding silicon pedestal waveguide is measured to be about 5% larger than that of a conventional silicon-on-insulator waveguide. We observe enhanced spectral broadening from self-phase modulation of an optical pulse in the pedestal waveguide. The interaction of light with the confined acoustic phonons in the pedestal structure gives rise to a larger nonlinear-index coeffi...

  5. Ultrafast 2D-IR and simulation investigations of preferential solvation and cosolvent exchange dynamics.

    Science.gov (United States)

    Dunbar, Josef A; Arthur, Evan J; White, Aaron M; Kubarych, Kevin J

    2015-05-21

    Using a derivative of the vitamin biotin labeled with a transition-metal carbonyl vibrational probe in a series of aqueous N,N-dimethylformamide (DMF) solutions, we observe a striking slowdown in spectral diffusion dynamics with decreased DMF concentration. Equilibrium solvation dynamics, measured with the rapidly acquired spectral diffusion (RASD) technique, a variant of heterodyne-detected photon-echo peak shift experiments, range from 1 ps in neat DMF to ∼3 ps in 0.07 mole fraction DMF/water solution. Molecular dynamics simulations of the biotin-metal carbonyl solute in explicit aqueous DMF solutions show marked preferential solvation by DMF, which becomes more pronounced at lower DMF concentrations. The simulations and the experimental data are consistent with an interpretation where the slowdown in spectral diffusion is due to solvent exchange involving distinct cosolvent species. A simple two-component model reproduces the observed spectral dynamics as well as the DMF concentration dependence, enabling the extraction of the solvent exchange time scale of 8 ps. This time scale corresponds to the diffusive motion of a few Å, consistent with a solvent-exchange mechanism. Unlike most previous studies of solvation dynamics in binary mixtures of polar solvents, our work highlights the ability of vibrational probes to sense solvent exchange as a new, slow component in the spectral diffusion dynamics.

  6. Ultrafast Study of Dynamic interfacial Exchange Coupling in Ferromagnet/Oxide/Semiconductor Heterostructures

    Science.gov (United States)

    Ou, Yu-Sheng; Chiu, Yi-Hsin; Harmon, Nicholas; Odenthal, Patrick; Sheffield, Matthew; Chilcote, Michael; Kawakami, Roland; Flatté, Michael; Johnston-Halperin, Ezekiel

    Time-resolved Kerr/Faraday rotation (TRKR/TRFR) is employed to study GaAs spin dynamics in the regime of strong and dynamic exchange coupling to an adjacent MgO/Fe layer. This study reveals a dramatic, resonant suppression in the inhomogeneous spin lifetime (T2*) in the GaAs layer. Further investigation of the magnetization dynamics of the neighboring Fe layer, also using TRKR/TRFR, reveals not only the expected Kittel-dispersion but also additional lower frequency modes with very short lifetime (65 ps) that are not easily observed with conventional ferromagnetic resonance (FMR) techniques. These results suggest the intriguing possibility of resonant dynamic spin transfer between the GaAs and Fe spin systems. We discuss the potential for this work to establish GaAs spin dynamics as an efficient detector of spin dissipation and transport in the regime of dynamically-driven spin injection in ferromagnet/semiconductor heterostructures. Center for Emergent Materials; U.S. Department of Energy.

  7. Experimental investigation of plasmofluidic waveguides

    Energy Technology Data Exchange (ETDEWEB)

    Ku, Bonwoo; Kwon, Min-Suk, E-mail: mskwon@unist.ac.kr [School of Electrical and Computer Engineering, UNIST, 50 UNIST-gil, Eonyang-eup, Ulju-gun, Ulsan 689-798 (Korea, Republic of); Shin, Jin-Soo [Department of Electrical Engineering, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 305-701 (Korea, Republic of)

    2015-11-16

    Plasmofluidic waveguides are based on guiding light which is strongly confined in fluid with the assistance of a surface plasmon polariton. To realize plasmofluidic waveguides, metal-insulator-silicon-insulator-metal (MISIM) waveguides, which are hybrid plasmonic waveguides fabricated using standard complementary metal-oxide-semiconductor technology, are employed. The insulator of the MISIM waveguide is removed to form 30-nm-wide channels, and they are filled with fluid. The plasmofluidic waveguide has a subwavelength-scale mode area since its mode is strongly confined in the fluid. The waveguides are experimentally characterized for different fluids. When the refractive index of the fluid is 1.440, the plasmofluidic waveguide with 190-nm-wide silicon has propagation loss of 0.46 dB/μm; the coupling loss between it and an ordinary silicon photonic waveguide is 1.79 dB. The propagation and coupling losses may be reduced if a few fabrication-induced imperfections are removed. The plasmofluidic waveguide may pave the way to a dynamically phase-tunable ultracompact device.

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

    Energy Technology Data Exchange (ETDEWEB)

    Hau-Riege, S

    2010-10-07

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

  9. Characterization of liquid-core/liquid-cladding optical waveguides of a sodium chloride solution/water system by computational fluid dynamics.

    Science.gov (United States)

    Kamiyama, Junya; Asanuma, Soto; Murata, Hiroyasu; Sugii, Yasuhiko; Hotta, Hiroki; Sato, Kiichi; Tsunoda, Kin-ichi

    2013-12-01

    A stable liquid/liquid optical waveguide (LLW) was formed using a sheath flow, where a 15% sodium chloride (NaCl) solution functioned as the core solution and water functioned as the cladding solution (15% NaCl/water LLW). The LLW was at least 200 mm in length. The concentration distributions of the liquid core and liquid cladding solutions in the LLW system were predicted by computational fluid dynamics (CFD) to validate the characteristics of the waveguide. The broadening of the region of the fluorescence of Rhodamine B excited by the guided light and the increase in the critical angle of the guided light with the increase in the contact time of the core and the cladding solutions were well explained by CFD calculations. However, no substantial leakage of the guided light was observed despite the considerably large change in the refractive index profile of the LLW; thus, a narrower and longer waveguide was realized.

  10. Pump dependence of the dynamics of quantum dot based waveguide absorbers

    Science.gov (United States)

    Viktorov, Evgeny A.; Erneux, Thomas; Piwonski, Tomasz; Pulka, Jaroslaw; Huyet, Guillaume; Houlihan, John

    2012-06-01

    The nonlinear two stage recovery of quantum dot based reverse-biased waveguide absorbers is investigated experimentally and analytically as a function of the initial ground state occupation probability of the dot. The latter is controlled experimentally by the pump pulse power. The slow stage of the recovery is exponential and its basic timescale is independent of pump power. The fast stage of the recovery is a logistic function which we analyze in detail. The relative strength of slow to fast components is highlighted and the importance of higher order absorption processes at the highest pump level is demonstrated.

  11. Non-Markovian reduced dynamics of ultrafast charge transfer at an oligothiophene–fullerene heterojunction

    Energy Technology Data Exchange (ETDEWEB)

    Hughes, Keith H., E-mail: keith.hughes@bangor.ac.uk [School of Chemistry, Bangor University, Bangor, Gwynedd LL57 2UW (United Kingdom); Cahier, Benjamin [School of Chemistry, Bangor University, Bangor, Gwynedd LL57 2UW (United Kingdom); Martinazzo, Rocco [Dipartimento di Chimica Università degli Studi di Milano, v. Golgi 19, 20133 Milano (Italy); Tamura, Hiroyuki [WPI-Advanced Institute for Material Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577 (Japan); Burghardt, Irene [Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt, Max-von-Laue-Str. 7, 60438 Frankfurt/Main (Germany)

    2014-10-17

    Highlights: • Quantum dynamical study of exciton dissociation at a heterojunction interface. • The non-Markovian quantum dynamics involves a highly structured spectral density. • Spectral density is reconstructed from an effective mode transformation of the Hamiltonian. • The dynamics is studied using the hierarchical equations of motion approach. • It was found that the temperature has little effect on the charge transfer. - Abstract: We extend our recent quantum dynamical study of the exciton dissociation and charge transfer at an oligothiophene–fullerene heterojunction interface (Tamura et al., 2012) [6] by investigating the process using the non-perturbative hierarchical equations of motion (HEOM) approach. Based upon an effective mode reconstruction of the spectral density the effect of temperature on the charge transfer is studied using reduced density matrices. It was found that the temperature had little effect on the charge transfer and a coherent dynamics persists over the first few tens of femtoseconds, indicating that the primary charge transfer step proceeds by an activationless pathway.

  12. Strain dependent ultrafast carrier dynamics in EuTiO3 films

    Science.gov (United States)

    Li, Zhong-guo; Zhao, Run; Li, Weiwei; Wang, Haiyan; Yang, Hao; Song, Ying-lin

    2014-10-01

    The photocarrier relaxation dynamics of EuTiO3 films have been investigated using femtosecond transient absorption spectroscopy. Two kinds of EuTiO3 films, with and without strain, have been included. In both films, the decay dynamics of 2p-3dt2g transition has a fast (˜2 ps) and slow (ns) components which are independent of the strain. Remarkably, the transient photobleaching of 4f-3dt2g transition is found to be enhanced considerably in the strained film, accompanied with a subnanosecond carrier lifetime. This behavior can be linked to the strain induced band structure modulation. Our results reveal the dynamical interactions in EuTiO3, identifying the critical roles of strain in photo induced phenomena.

  13. In situ observation of the ultrafast lattice dynamics of graphite under ion irradiation

    Science.gov (United States)

    Ishioka, Kunie; Hase, Muneaki; Kitajima, Masahiro

    2004-05-01

    We develop a pump-probe experiment system, in which vibrational dynamics of a solid sample under ion irradiation can be measured in real time. In situ observation enables us to monitor small changes induced by ion irradiation, without being influenced by the irreproducibility of the sample quality or the experimental configuration. We apply the experimental system to investigate the femtosecond dynamics of the coherent E2 g1 phonon of graphite under 5 keV He + irradiation. A slight decrease in the dephasing rate of the phonon at the initial stage, as well as a downshift followed by an upshift of the phonon frequency, are clearly demonstrated, all of which were ambiguous in the ex situ experiment due to the poor reproducibility of the surface quality. This technique could also be applied to study femtosecond vibrational dynamics in real time during thermal annealing, film deposition with e.g. ablation and sputter, and molecular adsorption on substrates.

  14. Phonon waveguides for electromechanical circuits

    Science.gov (United States)

    Hatanaka, D.; Mahboob, I.; Onomitsu, K.; Yamaguchi, H.

    2014-07-01

    Nanoelectromechanical systems (NEMS), utilizing localized mechanical vibrations, have found application in sensors, signal processors and in the study of macroscopic quantum mechanics. The integration of multiple mechanical elements via electrical or optical means remains a challenge in the realization of NEMS circuits. Here, we develop a phonon waveguide using a one-dimensional array of suspended membranes that offers purely mechanical means to integrate isolated NEMS resonators. We demonstrate that the phonon waveguide can support and guide mechanical vibrations and that the periodic membrane arrangement also creates a phonon bandgap that enables control of the phonon propagation velocity. Furthermore, embedding a phonon cavity into the phonon waveguide allows mobile mechanical vibrations to be dynamically switched or transferred from the waveguide to the cavity, thereby illustrating the viability of waveguide-resonator coupling. These highly functional traits of the phonon waveguide architecture exhibit all the components necessary to permit the realization of all-phononic NEMS circuits.

  15. Ultrafast spin dynamics and switching via spin transfer torque in antiferromagnets with weak ferromagnetism

    Science.gov (United States)

    Kim, Tae Heon; Grünberg, Peter; Han, Song Hee; Cho, Beongki

    2016-10-01

    The spin-torque driven dynamics of antiferromagnets with Dzyaloshinskii-Moriya interaction (DMI) were investigated based on the Landau-Lifshitz-Gilbert-Slonczewski equation with antiferromagnetic and ferromagnetic order parameters (l and m, respectively). We demonstrate that antiferromagnets including DMI can be described by a 2-dimensional pendulum model of l. Because m is coupled with l, together with DMI and exchange energy, close examination of m provides fundamental understanding of its dynamics in linear and nonlinear regimes. Furthermore, we discuss magnetization reversal as a function of DMI and anisotropy energy induced by a spin current pulse.

  16. Ultrafast spin dynamics and switching via spin transfer torque in antiferromagnets with weak ferromagnetism

    Science.gov (United States)

    Kim, Tae Heon; Grünberg, Peter; Han, Song Hee; Cho, Beongki

    2016-01-01

    The spin-torque driven dynamics of antiferromagnets with Dzyaloshinskii-Moriya interaction (DMI) were investigated based on the Landau-Lifshitz-Gilbert-Slonczewski equation with antiferromagnetic and ferromagnetic order parameters (l and m, respectively). We demonstrate that antiferromagnets including DMI can be described by a 2-dimensional pendulum model of l. Because m is coupled with l, together with DMI and exchange energy, close examination of m provides fundamental understanding of its dynamics in linear and nonlinear regimes. Furthermore, we discuss magnetization reversal as a function of DMI and anisotropy energy induced by a spin current pulse. PMID:27713522

  17. Ultrafast coherent dynamics of a photonic crystal all-optical switch

    CERN Document Server

    Colman, Pierre; Yu, Yi; Mørk, Jesper

    2016-01-01

    We present pump-probe measurements of an all-optical photonic crystal switch based on a nanocavity, resolving fast coherent temporal dynamics. The measurements demonstrate the importance of coherent effects typically neglected when considering nanocavity dynamics. In particular, we report the observation of an idler pulse. The measurements are in good agreement with a theoretical model that allows us to ascribe the observation to oscillations of the free carrier population in the nanocavity. The effect opens perspectives for the realization of new all-optical photonic crystal switches with unprecedented switching contrast.

  18. Scattering of two photons on a quantum emitter in a one-dimensional waveguide: exact dynamics and induced correlations

    DEFF Research Database (Denmark)

    Nysteen, Anders; Kristensen, Philip Trøst; McCutcheon, Dara

    2015-01-01

    We develop a wavefunction approach to describe the scattering of two photons on a quantum emitter embedded in a one-dimensional waveguide. Our method allows us to calculate the exact dynamics of the complete system at all times, as well as the transmission properties of the emitter. We show...... that the nonlinearity of the emitter with respect to incoming photons depends strongly on the emitter excitation and the spectral shape of the incoming pulses, resulting in transmission of the photons which depends crucially on their separation and width. In addition, for counter-propagating pulses, we analyze...... the induced level of quantum correlations in the scattered state, and we show that the emitter behaves as a nonlinear beam-splitter when the spectral width of the photon pulses is similar to the emitter decay rate....

  19. Ultrafast dynamics of confined and localised excitons and biexcitons in low-dimensional semiconductors

    DEFF Research Database (Denmark)

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

    1999-01-01

    Coherent optical spectroscopy in the form of nonlinear transient four-wave mixing (TFWM) and linear resonant Rayleigh scattering (RRS) has been applied to investigate the exciton dynamics of low-dimensional semiconductor heterostructures. The dephasing times of excitons are determined from...

  20. An optical and theoretical investigation of the ultrafast dynamics of a bisthienylethene-based photochromic switch

    NARCIS (Netherlands)

    Hania, P.R.; Telesca, R.; Lucas, L.N.; Pugzlys, A; van Esch, J. H; Feringa, B.L.; Snijders, J.G.; Duppen, K.

    2002-01-01

    The switching behavior of 1,2-bis(5-phenyl-2-methylthien-3-yl)cyclopentene is studied by means of polarization selective nonlinear optical spectroscopy and time-dependent density functional theory. The combined information from the observed population and orientational dynamics together with the res

  1. Toward Highlighting the Ultrafast Electron Transfer Dynamics at the Optically Dark Sites of Photocatalysts

    DEFF Research Database (Denmark)

    Canton, Sophie E.; Zhang, Xiaoyi; Zhang, Jianxin

    2013-01-01

    Building a detailed understanding of the structure–function relationship is a crucial step in the optimization of molecular photocatalysts employed in water splitting schemes. The optically dark nature of their active sites usually prevents a complete mapping of the photoinduced dynamics. In this...

  2. Nucleation and ultrafast vaporization dynamics of laser-activated polymeric microcapsules

    Science.gov (United States)

    Lajoinie, Guilaume; Gelderblom, Erik; Chlon, Ceciel; Boehmer, Marcel; Steenbergen, Wiendelt; de Jong, Nico; Manohar, Srirang; Versluis, Michel

    2014-11-01

    Precision control of vaporization, both in space and time, has many potential applications; however, the physical mechanisms underlying controlled boiling are not well understood. The reason is the combined microscopic length scales and ultra-short timescales associated with the initiation and subsequent dynamical behavior of the vapor bubbles formed. Here we study the nanoseconds vapor bubble dynamics of laser-heated single oil-filled microcapsules using coupled optical and acoustic detection. Pulsed laser excitation leads to vapor formation and collapse, and a simple physical model captures the observed radial dynamics and resulting acoustic pressures. Continuous wave laser excitation leads to a sequence of vaporization and condensation cycles, the result of absorbing microcapsule fragments moving in and out of the laser beam. A model incorporating thermal diffusion from the capsule shell into the oil core and surrounding water reveals the mechanisms behind the onset of vaporization. Excellent agreement is observed between the modeled dynamics and experiment. This work is supported by NanoNextNL, a micro and nanotechnology consortium of the Government of the Netherlands and 130 partners.

  3. Model study on the real-time detection of ultrafast nonadiabatic dynamics associated with the Wulf-Chappuis bands of ozone

    Science.gov (United States)

    Stock, Gerhard; Woywod, Clemens; Domcke, Wolfgang

    1992-11-01

    Model calculations on the cw absorption spectrum and femtosecond time-resolved stimulated-emission pump—probe spectra are reported for the Wulf—Chappuis bands of ozone. The model accounts for the three dimensional conical intersection of the 1A 2 and 1B 1 excited states and the associated singular non-Born—Oppenheimer coupling. Effects of dissociation into O+O 2 are modelled phenomenologically. It is demonstrated on the basis of this model that detailed information on the ultrafast nonadiabatic excited-state dynamics can be obtained by pump—probe spectroscopy with ultrashort pulses (pulse duration of the order of 10 fs).

  4. Real-time observation of ultrafast dynamics of individual rotational states in a molecular wavepacket with strong-field-ionization-induced nitrogen lasing

    CERN Document Server

    Zeng, Bin; Li, Guihua; Yao, Jinping; Zhang, Haisu; Ni, Jielei; Jing, Chenrui; Xie, Hongqiang; Cheng, Ya

    2014-01-01

    Molecular rotational spectroscopy based on strong-field-ionization-induced nitrogen laser is employed to investigate the time evolution of the rotational wave packet composed by a coherent superposition of quantum rotational states created in a field-free molecular alignment. We show that this technique uniquely allows real-time observation of the ultrafast dynamics of the individual rotational states in the rotational wavepacket. Our analysis also shows that there exist two channels of generation of the nitrogen laser, shedding new light on the population inversion mechanism behind the air laser generated by intense femtosecond laser pulses.

  5. Ultrafast direct laser writing of cladding waveguides in the 0.8CaSiO{sub 3}-0.2Ca{sub 3}(PO{sub 4}){sub 2} eutectic glass doped with Nd{sup 3+} ions

    Energy Technology Data Exchange (ETDEWEB)

    Martínez de Mendívil, J., E-mail: jon.martinez@uam.es; Lifante, G. [Departamento de Física de Materiales, C-04, Facultad de Ciencias, Universidad Autónoma de Madrid, 28.049 Madrid (Spain); Sola, D.; Peña, J. I. [Departamento de Ciencia y Tecnología de Materiales y Fluidos, Instituto de Ciencia de Materiales de Aragón, Universidad de Zaragoza-CSIC, 50.018 Zaragoza (Spain); Vázquez de Aldana, J. R. [Grupo de Investigación en Microprocesado de Materiales con Láser, Departamento de Física Aplicada, Universidad de Salamanca, 37.008 Salamanca (Spain); Aza, A. H. de; Pena, P. [Instituto de Cerámica y Vidrio-CSIC, 28.049 Madrid (Spain)

    2015-01-28

    We report on tubular cladding optical waveguides fabricated in Neodymium doped Wollastonite-Tricalcium Phosphate glass in the eutectic composition. The glass samples were prepared by melting the eutectic powder mixture in a Pt-Rh crucible at 1600 °C and pouring it in a preheated brass mould. Afterwards, the glass was annealed to relieve the inner stresses. Cladding waveguides were fabricated by focusing beneath the sample surface using a pulsed Ti:sapphire laser with a pulsewidth of 120 fs working at 1 kHz. The optical properties of these waveguides have been assessed in terms of near-field intensity distribution and transmitted power, and these results have been compared to previously reported waveguides with double-line configuration. Optical properties have also been studied as function of the temperature. Heat treatments up to 700 °C were carried out to diminish colour centre losses where waveguide's modes and transmitted power were compared in order to establish the annealing temperature at which the optimal optical properties were reached. Laser experiments are in progress to evaluate the ability of the waveguides for 1064 nm laser light generation under 800 nm optical pumping.

  6. Probing ultrafast carrier dynamics, nonlinear absorption and refraction in core–shell silicon nanowires

    Indian Academy of Sciences (India)

    Sunil Kumar; M Khorasaninejad; M M Adachi; K S Karim; S S Saini; A K Sood

    2012-09-01

    We investigate the relaxation dynamics of photogenerated carriers in silicon nanowires consisting of a crystalline core and a surrounding amorphous shell, using femtosecond time resolved differential reflectivity and transmission spectroscopy at 3.15 eV and 1.57 eV photon energies. The complex behaviour of the differential transmission and reflectivity transients is the mixed contributions from the crystalline core and the amorphous silicon on the nanowire surface and the substrate where competing effects of state-filling and photoinduced absorption govern the carrier dynamics. Faster relaxation rates are observed on increasing the photogenerated carrier density. Independent experimental results on crystalline silicon-on-sapphire (SOS) help us in separating the contributions from the carrier dynamics in crystalline core and the amorphous regions in the nanowire samples. Further, single-beam z-scan nonlinear transmission experiments at 1.57 eV in both open- and close-aperture configurations yield two-photon absorption coefficient (∼3 cm/GW) and nonlinear refraction coefficient (−2.5 × 10−4 cm2 /GW).

  7. Scanning ultrafast electron microscopy.

    Science.gov (United States)

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

    2010-08-24

    Progress has been made in the development of four-dimensional ultrafast electron microscopy, which enables space-time imaging of structural dynamics in the condensed phase. In ultrafast electron microscopy, the electrons are accelerated, typically to 200 keV, and the microscope operates in the transmission mode. Here, we report the development of scanning ultrafast electron microscopy using a field-emission-source configuration. Scanning of pulses is made in the single-electron mode, for which the pulse contains at most one or a few electrons, thus achieving imaging without the space-charge effect between electrons, and still in ten(s) of seconds. For imaging, the secondary electrons from surface structures are detected, as demonstrated here for material surfaces and biological specimens. By recording backscattered electrons, diffraction patterns from single crystals were also obtained. Scanning pulsed-electron microscopy with the acquired spatiotemporal resolutions, and its efficient heat-dissipation feature, is now poised to provide in situ 4D imaging and with environmental capability.

  8. Scanning ultrafast electron microscopy

    Science.gov (United States)

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

    2010-01-01

    Progress has been made in the development of four-dimensional ultrafast electron microscopy, which enables space-time imaging of structural dynamics in the condensed phase. In ultrafast electron microscopy, the electrons are accelerated, typically to 200 keV, and the microscope operates in the transmission mode. Here, we report the development of scanning ultrafast electron microscopy using a field-emission-source configuration. Scanning of pulses is made in the single-electron mode, for which the pulse contains at most one or a few electrons, thus achieving imaging without the space-charge effect between electrons, and still in ten(s) of seconds. For imaging, the secondary electrons from surface structures are detected, as demonstrated here for material surfaces and biological specimens. By recording backscattered electrons, diffraction patterns from single crystals were also obtained. Scanning pulsed-electron microscopy with the acquired spatiotemporal resolutions, and its efficient heat-dissipation feature, is now poised to provide in situ 4D imaging and with environmental capability. PMID:20696933

  9. Ultrafast Dynamics in Low Temperature Saccharide Glasses: A Photon Echo Study

    Science.gov (United States)

    Nagasawa, Yutaka; Nakagawa, Yukako; Mori, Yoshio; Muromoto, Takayuki; Okada, Tadashi

    2004-04-01

    Saccharides are used as protectant by many organisms such as insects and amphibians. The glass transition of the saccharides is considered to be the key factor in the protection of the biological tissue against freezing and dehydration. The molecular dynamics of saccharide glasses were studied by photon echo spectroscopy and it revealed that electronic dephasing time is much longer in saccharide glasses compared to artificial polymer glass, polyvinylalcohol (PVA), at temperature of 10 K. Critically damped oscillation which can be assigned to the phonon mode of the saccharide glass was also observed.

  10. Investigation of ultrafast dynamics of CdTe quantum dots by femtosecond fluorescence up-conversion spectroscopy

    NARCIS (Netherlands)

    Yao, G.-X.; Lü, L.-H.; Gui, M.-F.; Zhang, X.-Y.; Zheng, X.-F.; Ji, X.-H.; Zhang, H.; Cui, Z.-F.

    2012-01-01

    The ultrafast carrier relaxation processes in CdTe quantum dots are investigated by femtosecond fluorescence up-conversion spectroscopy. Photo-excited hole relaxing to the edge of the forbidden gap takes a maximal time of ~ 1.6 ps with exciting at 400 nm, depending on the state of the photo-excited

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

    Directory of Open Access Journals (Sweden)

    T. Stensitzki

    2016-07-01

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

  12. Ultrafast non-equilibrium carrier dynamics in semiconductor laser mode-locking

    Science.gov (United States)

    Hader, J.; Scheller, M.; Laurain, A.; Kilen, I.; Baker, C.; Moloney, J. V.; Koch, S. W.

    2017-01-01

    Experimental and theoretical results on the mode-locking dynamics in vertical-external-cavity surface-emitting lasers with semiconductor and graphene saturable absorber mirrors are reviewed with an emphasis on the role of nonequilibrium carrier effects. The systems are studied theoretically using a fully microscopic many-body model for the carrier distributions and polarizations, coupled to Maxwell’s equations for the field propagation. Pump-probe measurements are performed with (sub-) 100 fs resolution. The analysis shows that the non-equilibrium carrier dynamics in the gain quantum-wells and saturable absorber medium significantly influences the system’s response and the resulting mode-locked pulses. The microscopic model is used to study the pulse build up from spontaneous emission noise and to determine the dependence of achievable pulse lengths and fluences on the amounts of saturable and non-saturable losses and the optical gain. The change of the group delay dispersion (GDD) on the pump level is examined and the dependence of the pulse lengths on the total amount of GDD is demonstrated experimentally. Theory-experiment comparisons are used to demonstrate the highly quantitative accuracy of the fully microscopic modeling.

  13. Ultrafast valley dynamics in atomically thin transition metal dichalcogenides (Conference Presentation)

    Science.gov (United States)

    Bratschitsch, Rudolf

    2016-10-01

    Monolayer transition metal dichalcogenides such as MoS2, WS2, MoSe2, WSe2, and MoTe2 received a lot of attention recently due to their atomic thickness in combination with an optical band gap in the visible or infrared. These properties render them a promising material class for new opto-electronic devices. Strong spin-orbit coupling together with the absence of inversion symmetry leads to an emission of polarized photoluminescence after excitation with circularly polarized light. Therefore, the K and K' valley of the semiconductor can be selectively addressed by left and right handed circularly polarized light, which is interesting for valleytronic applications. To understand the mechanisms governing the creation and destruction of valley polarization, time-resolved experiments are necessary. While stationary photoluminescence experiments show nearly perfect valley polarization, indicating very slow intervalley scattering processes, first valley-selective pump-probe experiments yielded a strong signal immediately after optical excitation in both the pumped and unpumped valley, suggesting a small valley polarization. To understand this behavior, we performed a joint experiment-theory study on the time-resolved valley dynamics in atomically thin WS2. We find strong intervalley Coulomb coupling governing the dynamics in the atomically thin semiconductor. Our results are also applicable to the other transition metal dichalcogenides MoS2, MoSe2, and WSe2, where strong intervalley Coulomb coupling is expected.

  14. The Role of Rydberg-Valence Coupling in the Ultrafast Relaxation Dynamics of Acetone.

    Science.gov (United States)

    Koch, Markus; Thaler, Bernhard; Heim, Pascal; Ernst, Wolfgang E

    2017-08-31

    The electronic structure of excited states of acetone is represented by a Rydberg manifold that is coupled to valence states which provide very fast and efficient relaxation pathways. We observe and characterize the transfer of population from photoexcited Rydberg states (6p, 6d, 7s) to a whole series of lower Rydberg states (3p to 4d) and a simultaneous decay of population from these states. We obtain these results with time-resolved photoelectron-photoion coincidence (PEPICO) detection in combination with the application of Bayesian statistics for data analysis. Despite the expectedly complex relaxation behavior, we find that a simple sequential decay model is able to describe the observed PEPICO transients satisfactorily. We obtain a slower decay (∼320 fs) from photoexcited states compared to a faster decay (∼100 fs) of states that are populated by internal conversion, demonstrating that different relaxation dynamics are active. Within the series of Rydberg states populated by internal conversion, the decay dynamics seem to be similar, and a trend of slower decay from lower states indicates an increasingly higher energy barrier along the decay pathway for lower states. The presented results agree all in all with previous relaxation studies within the Rydberg manifold. The state-resolved observation of transient population ranging from 3p to 4d can serve as reference for time-dependent simulations.

  15. Laser fluence dependence on emission dynamics of ultrafast laser induced copper plasma

    Energy Technology Data Exchange (ETDEWEB)

    Anoop, K. K.; Harilal, S. S.; Philip, Reji; Bruzzese, R.; Amoruso, S.

    2016-11-14

    The characteristic emission features of a laser-produced plasma strongly depend strongly on the laser fluence. We investigated the spatial and temporal dynamics of neutrals and ions in femtosecond laser (800 nm, ≈ 40 fs, Ti:Sapphire) induced copper plasma in vacuum using both optical emission spectroscopy (OES) and spectrally resolved two-dimensional (2D) imaging methods over a wide fluence range of 0.5 J/cm2-77.5 J/cm2. 2D fast gated monochromatic images showed distinct plume splitting between the neutral and ions especially at moderate to higher fluence ranges. OES studies at low to moderate laser fluence regime confirm intense neutral line emission over the ion emission whereas this trend changes at higher laser fluence with dominance of the latter. This evidences a clear change in the physical processes involved in femtosecond laser matter interaction at high input laser intensity. The obtained ion dynamics resulting from the OES, and spectrally resolved 2D imaging are compared with charged particle measurement employing Faraday cup and Langmuir probe and results showed good correlation.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-03-16

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

  17. Ultra-fast charge carrier dynamics across the spectrum of an optical gain media based on InAs/AlGaInAs/InP quantum dots

    Directory of Open Access Journals (Sweden)

    I. Khanonkin

    2017-03-01

    Full Text Available The charge carrier dynamics of improved InP-based InAs/AlGaInAs quantum dot (QD semiconductor optical amplifiers are examined employing the multi-wavelength ultrafast pump-probe measurement technique. The transient transmission response of the continuous wave probe shows interesting dynamical processes during the initial 2-3 ps after the pump pulse, when carriers originating from two photon absorption contribute the least to the recovery. The effects of optical excitations and electrical bias levels on the recovery dynamics of the gain in energetically different QDs are quantified and discussed. The experimental observations are validated qualitatively using a comprehensive finite-difference time-domain model by recording the time evolution of the charge carriers in the QDs ensemble following the pulse.

  18. Silicon waveguide based 320 Gbit/s optical sampling

    DEFF Research Database (Denmark)

    Ji, Hua; Galili, Michael; Pu, Minhao

    2010-01-01

    A silicon waveguide-based 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.......A silicon waveguide-based 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....

  19. Ultrafast photo-induced turning of magnetization and its relaxation dynamics in GaMnAs

    Institute of Scientific and Technical Information of China (English)

    2010-01-01

    We report that,by linearly polarized pumping of different wavelengths,Kerr transients appear at zero magnetic field only in the case when GaMnAs samples are initialized at 3 K by first applying a 0.8 Tesla field and then returning to zero field.We find that,instead of magnetization precession,the near-band gap excitation induces a coherent out-of-plane turning of magnetization,which shows very long relaxation dynamics with no precession.When photon energy increases,the peak value of the Kerr transient increases,but it decays rapidly to the original slow transient seen under the near-band-gap excitation.

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

    Science.gov (United States)

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

    2012-09-10

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

  1. Ultrafast dynamics and fragmentation of C60 in intense laser pulses

    CERN Document Server

    Lin, Zheng-Zhe

    2014-01-01

    The radiation-induced fragmentation of the C60 fullerene was investigated by the tight-binding electron-ion dynamics simulations. In intense laser field, the breathing vibrational mode is much more strongly excited than the pentagonal-pinch mode. The fragmentation effect was found more remarkable at long wavelength lambda>800 nm rather than the resonant wavelengths due to the internal laser-induced dipole force, and the production ratio of C and C2 rapidly grows with increasing wavelength. By such fragmentation law, C atoms, C2 dimers or large Cn fragments could be selectively obtained by changing the laser wavelength. And the fragmentation of C60 by two laser pulses like the multi-step atomic photoionization was investigated.

  2. Dynamics of the higher lying excited states of cyanine dyes. An ultrafast fluorescence study.

    Science.gov (United States)

    Guarin, Cesar A; Villabona-Monsalve, Juan P; López-Arteaga, Rafael; Peon, Jorge

    2013-06-20

    The electronic relaxation dynamics of the second singlet excited states of several cyanine dyes was studied through the femtosecond fluorescence up-conversion technique. Our interest in these molecules comes from the potential applications of systems with upper excited singlet states with a long lifetime, which can include electron and energy transfer from the higher lying singlets after one- or two-photon absorption. We studied three series of cyanines with 4-quinolyl, 2-quinolyl, or benzothiazolyl type end groups, each with varying sp(2) carbon conjugation lengths in the methinic bridge. The dynamics after electronic excitation to singlet states above the fluorescent state vary significantly as a function of cyanine structure and conjugation length. In particular, for the 4-quinolyl series the cyanine with an intermediate conjugation length (three methinic carbons) has the slowest S2 decays with lifetimes of 5.4 ps in ethanol and 6.6 ps in ethylene glycol. On the other hand, we observed that the 2-quinolyl family has S2 decay times in the subpicosecond range independent of the conjugation length between the end groups. The slowest internal conversion was observed for the benzothiazolyl type cyanine with five methinic carbons, with an S2 lifetime of 17.3 ps in ethanol. For the planar cyanines of this study we observed for the first time a clear systematic trend in the S2 decay times which closely follow the energy gap law. It was also demonstrated that a slow S2 decay is as well observed upon excitation through degenerate two-photon absorption with near-IR pulses. The present study isolates the most important variables for the design of cyanines with long S2 lifetimes.

  3. 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.

  4. Ultrafast carrier dynamics in bimetallic nanostructure-enhanced methylammonium lead bromide perovskites.

    Science.gov (United States)

    Zarick, Holly F; Boulesbaa, Abdelaziz; Puretzky, Alexander A; Talbert, Eric M; DeBra, Zachary R; Soetan, Naiya; Geohegan, David B; Bardhan, Rizia

    2017-01-26

    In this work, we examine the impact of hybrid bimetallic Au/Ag core/shell nanostructures on the carrier dynamics of methylammonium lead tribromide (MAPbBr3) mesoporous perovskite solar cells (PSCs). Plasmon-enhanced PSCs incorporated with Au/Ag nanostructures demonstrated improved light harvesting and increased power conversion efficiency by 26% relative to reference devices. Two complementary spectral techniques, transient absorption spectroscopy (TAS) and time-resolved photoluminescence (trPL), were employed to gain a mechanistic understanding of plasmonic enhancement processes. TAS revealed a decrease in the photobleach formation time, which suggests that the nanostructures improve hot carrier thermalization to an equilibrium distribution, relieving hot phonon bottleneck in MAPbBr3 perovskites. TAS also showed a decrease in carrier decay lifetimes, indicating that nanostructures enhance photoinduced carrier generation and promote efficient electron injection into TiO2 prior to bulk recombination. Furthermore, nanostructure-incorporated perovskite films demonstrated quenching in steady-state PL and decreases in trPL carrier lifetimes, providing further evidence of improved carrier injection in plasmon-enhanced mesoporous PSCs.

  5. Ultrafast photoinduced dynamics in quantum dot-based systems for light harvesting

    Institute of Scientific and Technical Information of China (English)

    Kaibo Zheng; Khadga Karki; Karel Zidek; Tonu Pullerits

    2015-01-01

    Colloidal semiconductor nanocrystals, referred to as quantum dots, offer simple low-temperature solution-based methods for constructing optoelectronic devices such as light emitting diodes and solar cells. We review recent progress in the understanding of photoinduced processes in key components of a certain type of quantum dot solar cells where the dots sensitize a suitable metal oxide, such as ZnO or TiO2, for electron injection, and NiO for hole injection. The electron and hole injection dynamics are discussed in detail as a function of the quantum dot size and core-shell structure, the linker molecule type, and the morphology of the accepting metal oxide. Hole trapping is identified as a major factor limiting the performance of quantum dot-based devices. We review possible strategies for improvement that use core-shell structures and directed excitation energy transfer between quantum dots. Finally, the generation and injection of multiple excitons are revisited. We show that the assumption of a linear relationship between the intensity of transient absorption signal and the number of excitons does not generally hold, and this observation can partially explain highly disparate results for the effidency of generating multiple exdtons. A consistent calculation procedure for studies of multiple exciton generation is provided. Finally we offer a brief personal outlook on the topic.

  6. Smart macrocyclic molecules: induced fit and ultrafast self-sorting inclusion behavior through dynamic covalent chemistry.

    Science.gov (United States)

    Han, Ji-Min; Pan, Jin-Long; Lei, Ting; Liu, Chenjiang; Pei, Jian

    2010-12-10

    A family of macrocycles with oligo(ethylene glycol) chains, 4O, 5O, and 6O, was developed to construct a series of new incorporated macrocycles through dynamic covalent chemistry. These flexible macrocycles exhibited excellent "self-sorting" abilities with diamine compounds, which depended on the "induced-fit" rule. For instance, the host macrocycles underwent conformational modulation to accommodate the diamine guests, affording [1+1] intramolecular addition compounds regardless of the flexibility of the diamine. These macrocycles folded themselves to fit various diamines with different chain length through modulation of the flexible polyether chain, and afforded intramolecular condensation products. However, if the chain of the diamine was too long and rigid, oligomers or polymers were obtained from the mixture of the macromolecule and the diamine. All results demonstrated that inclusion compounds involving conformationally suitable aromatic diamines were thermodynamically favorable candidates in the mixture due to the restriction of the macrocycle size. Furthermore, kinetic and thermodynamic studies of self-sorting behaviors of both mixed 4O-5O and 4O-6O systems were investigated in detail. Finally, theoretical calculations were also employed to further understand such self-sorting behavior, and indicated that the large enthalpy change of H(2)NArArNH(2)@4O is the driving force for the sorting behavior. Our system may provide a model to further understand the principle of biomolecules with high specificity due only to their conformational self-adjusting ability.

  7. Density matrix based time-dependent configuration interaction approach to ultrafast spin-flip dynamics

    CERN Document Server

    Wang, H; Kühn, O

    2016-01-01

    Recent developments in attosecond spectroscopy yield access to the correlated motion of electrons on their intrinsic time scales. Spin-flip dynamics is usually considered in the context of valence electronic states, where spin-orbit coupling is weak and processes related to the electron spin are usually driven by nuclear motion. However, for core-excited states, where the core hole has a nonzero angular momentum, spin-orbit coupling is strong enough to drive spin-flips on a much shorter time scale. Using density matrix based time-dependent restricted active space configuration interaction including spin-orbit coupling, we address an unprecedentedly short spin-crossover for the example of L-edge (2p$\\rightarrow$3d) excited states of a prototypical Fe(II) complex. This process occurs on a time scale, which is faster than that of Auger decay ($\\sim$4\\,fs) treated here explicitly. Modest variations of carrier frequency and pulse duration can lead to substantial changes in the spin-state yield, suggesting its cont...

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

    Science.gov (United States)

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

    2012-12-07

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

  9. Ultrafast exciton relaxation dynamics of PbS and core/shell PbS/CdS quantum dots

    Institute of Scientific and Technical Information of China (English)

    WHEELER Damon A.; FITZMORRIS Bob C.; ZHAO HaiGuang; MA DongLing; ZHANG JinZhong

    2012-01-01

    Optical properties and ultrafast exciton relaxation dynamics in PbS and core/shell PbS/CdS quantum dots (QDs) have been studied using UV-vis absorption and fluorescence spectroscopy as well as femtosecond (fs) transient absorption spectroscopy.The electronic absorption spectrum of the PbS QDs features broad absorption in the entire near IR-vis-UV region with a monotonic increase in intensity towards shorter wavelength.Relative to PbS,the absorption of the core/shell PbS/CdS QDs shows a slight blue shift in the 600-800 nm region,due to the decrease of the PbS crystal size caused by the synthetic process of the core/shell structure,and increased absorption near 400 nm due to the CdS shell.The PL of the PbS/CdS QDs was ~2.6 times more intense than that of the PbS QDs,due to surface passivation of PbS by CdS,and blue-shifted,attributable to smaller PbS size and thereby stronger quantum confinement in the core/shell QDs.Fs transient absorption measurements of both systems showed a strong transient absorption feature from 600 to 750 nm following excitation at 750 nm.The transient absorption decays can be fit to a biexponential with time constants of 8 and 100 ps for PbS and 6 and 80 ps for PbS/CdS.The amplitude and lifetime of the fast component were excitation intensity dependent,with the amplitude increasing more than linearly with increasing excitation intensity and the lifetime decreasing with increasing intensity.The fast decay is attributed to exciton-exciton annihilation and it occurs more readily for the PbS/CdS than the PbS QDs,which is attributed to a lower density of trap states in the core/shell ODs,as supported by their stronger PL.

  10. Exploring ultrafast dynamics of excitons and multiexcitons in "giant" nanocrystal quantum dots

    Science.gov (United States)

    Sampat, Siddharth

    In this work, we have performed extensive time resolved photoluminescence (PL) studies to further the understanding of charge dynamics in semiconductor nanocrystal quantum dots (QDs). Recent developments in QD synthesis have introduced a new set of QD known as "giant" quantum dots (gQDs) that consist of a CdSe core coated with up to 19 monolayers of a CdS shell. The thick shell layer is grown using a SILAR method resulting in a defect free, alloyed CdSe/CdS interface. This has been attributed to gQDs exhibiting excellent optical properties such as high excitonic quantum yield (QY), prolonged photostability and inhibition of flourescence intermittency ("blinking"), which is regularly observed in conventional QDs. In gQDs, however, owing to unique fabrication methods and material selection, the Auger process is strongly suppressed resulting in efficient radiative recombination of photogenerated excitons as well as high PL QY of charged excitonic and multiexcitonic species. We perform extensive single gQDs studies that establish the role played by gQD shell thickness and core size in governing their optical properties. It is found that both the core and shell dimensions can be tuned in order to achieve the smallest gQDs with the highest vii Auger suppression resulting in photostable dots with high QYs. Next, we perform a study of multiexcitonic species in gQDs that are encapsulated in an insulating SiO2shell. These silica-coated gQDs exhibit strong PL from charged excitons, biexcitons as well as triexcitons. This observation has led to an accurate description of excitonic and multiexcitonic behavior which is modeled using a statistical scaling approach. As a demonstration of the practical applicability of gQDs, energy transfer of excitons as well as multiexcitons to different substrates is studied. Finally, a back gated silicon nanomembrane FET device is discussed that exhibits a large photocurrent increase when sensitized with QDs.

  11. The effect of higher-order dispersion on slow light propagation in photonic crystal waveguides

    NARCIS (Netherlands)

    Engelen, R.J.P.; Engelen, R.J.P.; Sugimoto, Y.; Watanabe, Y.; Korterik, Jeroen P.; Ikeda, N.; van Hulst, N.F.; Asakawa, K.; Kuipers, L.

    2006-01-01

    We have studied the dispersion of ultrafast pulses in a photonic crystal waveguide as a function of optical frequency, in both experiment and theory. With phase-sensitive and time-resolved near-field microscopy, the light was probed inside the waveguide in a non-invasive manner. The effect of

  12. Mask-less lithography for fabrication of optical waveguides

    Science.gov (United States)

    Dubov, M.; Natarajan, S. R.; Williams, J. A. R.; Bennion, I.

    2008-02-01

    A flexible method for fabricating shallow optical waveguides by using femtosecond laser writing of patterns on a metal coated glass substrate followed by ion-exchange is described. This overcomes the drawbacks of low index contrast and high induced stress in waveguides directly written using low-repetition rate ultrafast laser systems. When compared to conventional lithography, the technique is simpler and has advantages in terms of flexibility in the types of structures which can be fabricated.

  13. Ultrafast infrared studies of chemical reaction dynamics in room-temperature liquids

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Haw [Univ. of California, Berkeley, CA (United States)

    1999-11-01

    Femtosecond infrared spectroscopy provides sufficient spectral and temporal resolution to support a detailed investigation of the early events of a photochemical reaction. Previously unreported transient species that arise as intermediates during the course of a reaction may have lifetimes that are too short for conventional characterization. For these species, quantum-mechanical (density functional theoretical and ab initio) electronic structure calculations provide invaluable insight into chemical properties including molecular structure and energetic. With the combination of experimental and theoretical results, it is possible to assemble a comprehensive picture of the reaction dynamics of a system that is intricately influenced by the surrounding solvent molecules. The mechanisms of several important organometallic reactions, such as alkane C– H bond activation by η3-Tp*Rh(CO), silane Si–H bond activation by η5-CpMn(CO)2 and η5-CpRe(CO)2, as well as chlorinated methane C–Cl bond cleavage by the Re(CO)5 radical are elucidated. The results demonstrate the importance of molecular morphology change (C–H and Si–H act ivat ion), solvent rearrangement (Si–H activation), intersystem crossing (Si–H activation), and solvent caging (C–Cl cleavage) in understanding the reactivity of the organometallic species, The nature of the apparent free-energy barrier for C–H, Si–H, and C–Cl bond activation reaction is found to be- cleavage of an alkane C–H bond, rearrangement of a silane molecule HSiR3 (R = alkyl group) from a nonreactive alkyl site to the reactive Si–H bond, and Cl atom transfer from a chlorinated methane molecule to Re(CO)5, respectively. These results support previous d initio calculations for C–H and Si–H bond activation reaction profiles which suggest that cleavage of an alkane C–H bond by a transition metal center, unlike that of a silane

  14. Ultrafast dual photoresponse of isolated biological chromophores: link to the photoinduced mode-specific non-adiabatic dynamics in proteins

    DEFF Research Database (Denmark)

    Bochenkova, Anastasia; Andersen, Lars Henrik

    2013-01-01

    channels. Deactivation includes vibrational resonant photodetachment and internal conversion. Here, we provide a detailed insight in the efficiency of different vibrational modes in promoting a selective photoresponse in the bare GFP chromophore anion. We introduce a general theoretical model...... that is capable to account for the alternative non-equivalent pathways in internal conversion, and we outline the factors, by which the photo-initiated response may be altered in this channel. The topography around the planar minimum in S1 and the two distinct types of the S1/S0 conical intersections obtained...... the ultrafast non-statistical electron emission coupled with vibrational (de)coherence, whereas a vibrational pre-excitation in the ground state may lead to the ultrafast non-statistical internal conversion through a conical intersection. We also discuss the implication of our results to the photo-initiated non...

  15. EDITORIAL: Ultrafast magnetization processes

    Science.gov (United States)

    Hillebrands, Burkard

    2008-09-01

    injected spin-polarized electron pulses on short time scales, ranging from a small disturbance of the system up to the reversal of the magnetization direction.' Now, seven years later, the subject of ultrafast magnetization processes has grown into a mainstream research direction in modern magnetism. The major international conferences on magnetism, such as the Annual Conference on Magnetism and Magnetic Materials (MMM), the INTERMAG, the International Conference of Magnetism, as well as many regional conferences, schedule dedicated sessions to ultrafast magnetization processes, very often several of them. The large share in research in this field from German scientists has been made possible by this Priority Programme. Since its beginning, new developments have been picked up by the Priority Programme 1133 and addressed by projects. Spin torque phenomena in spin dynamics, although foreseen at the time of establishing the Priority Programme, have been taken up. The field of dissipation has been addressed and extended by several groups, with contributions both from theoretical and experimental groups. A first set of contributions addresses ultrafast dynamics and materials. T Roth et al [article 164001] in this issue] study the dynamics of coercivity in ultrafast pump-probe experiments on the femtosecond time scale. They show that an all optical pump-probe technique is, in general, not suitable for gaining access to the time-dependent behaviour of the coercivity, since the switching in a fixed external field is an irreversible process. They comment on the possible mechanisms leading to the observed reduction of the coercivity with increasing pump power and propose a potential solution to clarify the origin of such a behaviour. B Heitkamp et al [164002] discuss the femtosecond spin dynamics of ferromagnetic CoPt thin films and nanodots, which they probe using spin-polarized photoemission electron microscopy. They show by photoelectron spin analysis, that enhanced optical near

  16. Wave-guided optical waveguides

    DEFF Research Database (Denmark)

    Palima, Darwin; Bañas, Andrew Rafael; Vizsnyiczai, George

    2012-01-01

    This work primarily aims to fabricate and use two photon polymerization (2PP) microstructures capable of being optically manipulated into any arbitrary orientation. We have integrated optical waveguides into the structures and therefore have freestanding waveguides, which can be positioned anywhe...... bridge the diffraction barrier. This structure-mediated paradigm may be carried forward to open new possibilities for exploiting beams from far-field optics down to the subwavelength domain....

  17. Quantum and semiclassical physics behind ultrafast optical nonlinearity in the midinfrared: the role of ionization dynamics within the field half cycle.

    Science.gov (United States)

    Serebryannikov, E E; Zheltikov, A M

    2014-07-25

    Ultrafast ionization dynamics within the field half cycle is shown to be the key physical factor that controls the properties of optical nonlinearity as a function of the carrier wavelength and intensity of a driving laser field. The Schrödinger-equation analysis of a generic hydrogen quantum system reveals universal tendencies in the wavelength dependence of optical nonlinearity, shedding light on unusual properties of optical nonlinearities in the midinfrared. For high-intensity low-frequency fields, free-state electrons are shown to dominate over bound electrons in the overall nonlinear response of a quantum system. In this regime, semiclassical models are shown to offer useful insights into the physics behind optical nonlinearity.

  18. Ultrafast carrier dynamics and third order nonlinear optical properties of aluminum doped zinc oxide (AZO) thin films

    Science.gov (United States)

    Htwe, Zin Maung; Zhang, Yun-Dong; Yao, Cheng-Bao; Li, Hui; Yuan, Ping

    2017-04-01

    Aluminum doped zinc oxide (AZO) thin films were fabricated by simultaneous RF/DC magnetron sputtering technique on sapphire (Al2O3) substrate with different DC sputtering power 2, 6, 8 and 10 W respectively. The sputtered thin films were annealed at 350 °C in order to improve the crystal quality. AZO thin films are systematically analyzed using X-ray diffraction (XRD), scanning electron microscopy (SEM) and UV-VIS spectrometer for structural and optical properties. XRD patterns show that all sputtered thin films are well crystallized with hexagonal wurtzite structure. SEM images reveal the average crystallite sizes are increased after doping Al in ZnO which agreed with the calculated values from XRD. All thin films possess high optical transmittance in visible region and optical band gap values are relatively increased with Al concentration. The ultrafast transient absorption (TA) of AZO was analyzed by femtosecond pump-probe spectroscopy. The kinetic TA curves were fitted by tri-exponential decay function and obtained decay time constants are found to be in few picosecond and nanosecond range for ultrafast and slow processes respectively. Third order nonlinear optical absorption and refraction coefficients were investigated by using Z-scan technique. The observed nonlinear coefficients are enhanced with Al concentration in ZnO.

  19. Ultrafast charge separation dynamics in opaque, operational dye-sensitized solar cells revealed by femtosecond diffuse reflectance spectroscopy

    Science.gov (United States)

    Ghadiri, Elham; Zakeeruddin, Shaik M.; Hagfeldt, Anders; Grätzel, Michael; Moser, Jacques-E.

    2016-04-01

    Efficient dye-sensitized solar cells are based on highly diffusive mesoscopic layers that render these devices opaque and unsuitable for ultrafast transient absorption spectroscopy measurements in transmission mode. We developed a novel sub-200 femtosecond time-resolved diffuse reflectance spectroscopy scheme combined with potentiostatic control to study various solar cells in fully operational condition. We studied performance optimized devices based on liquid redox electrolytes and opaque TiO2 films, as well as other morphologies, such as TiO2 fibers and nanotubes. Charge injection from the Z907 dye in all TiO2 morphologies was observed to take place in the sub-200 fs time scale. The kinetics of electron-hole back recombination has features in the picosecond to nanosecond time scale. This observation is significantly different from what was reported in the literature where the electron-hole back recombination for transparent films of small particles is generally accepted to occur on a longer time scale of microseconds. The kinetics of the ultrafast electron injection remained unchanged for voltages between +500 mV and -690 mV, where the injection yield eventually drops steeply. The primary charge separation in Y123 organic dye based devices was clearly slower occurring in two picoseconds and no kinetic component on the shorter femtosecond time scale was recorded.

  20. Ultrafast scanning tunneling microscopy

    Energy Technology Data Exchange (ETDEWEB)

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

    1995-09-01

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

  1. Strong influence of coadsorbate interaction on CO desorption dynamics on Ru(0001) probed by ultrafast x-ray spectroscopy and ab initio simulations

    Energy Technology Data Exchange (ETDEWEB)

    Xin, H. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); LaRue, J. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Oberg, H. [Stockholm Univ., Stockholm (Sweden); Beye, M. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Helmholtz Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Dell' Angela, M. [Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany); Turner, J. J. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Gladh, J. [Stockholm Univ., Stockholm (Sweden); Ng, M. L. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Sellberg, J. A. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Helmholtz Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Kaya, S. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Mercurio, G. [Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany); Hieke, F. [Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany); Nordlund, D. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Schlotter, W. F. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Dakovski, G. L. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Minitti, M. P. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Fohlisch, A. [Helmholtz Zentrum Berlin fur Materialien und Energie GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany); Wolf, M. [Fritz-Haber Institute of the Max-Planck-Society, Berlin (Germany); Wurth, W. [Univ. of Hamburg and Center for Free Electron Laser Science, Hamburg (Germany); DESY Photon Science, Hamburg (Germany); Ogasawara, H. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Norskov, J. K. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Ostrom, H. [Stockholm Univ., Stockholm (Sweden); Pettersson, L. G. M. [Stockholm Univ., Stockholm (Sweden); Nilsson, A. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stockholm Univ., Stockholm (Sweden); Ablid-Pedersen, F. [SLAC National Accelerator Lab., Menlo Park, CA (United States)

    2015-04-16

    We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5σ and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process.

  2. Dual-tip-enhanced ultrafast CARS nanoscopy

    CERN Document Server

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

    2013-01-01

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

  3. Four-dimensional ultrafast electron microscopy.

    Science.gov (United States)

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

    2005-05-17

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

  4. Analysis of piezoelectric ultrasonic transducers attached to waveguides using waveguide finite elements.

    Science.gov (United States)

    Loveday, Philip W

    2007-10-01

    A finite-element modeling procedure for computing the frequency response of piezoelectric transducers attached to infinite constant cross-section waveguides, as encountered in guided wave ultrasonic inspection, is presented. Two-dimensional waveguide finite elements are used to model the waveguide. Conventional three-dimensional finite elements are used to model the piezoelectric transducer. The harmonic forced response of the waveguide is used to obtain a dynamic stiffness matrix (complex and frequency dependent), which represents the waveguide in the transducer model. The electrical and mechanical frequency response of the transducer, attached to the waveguide, can then be computed. The forces applied to the waveguide are calculated and are used to determine the amplitude of each mode excited in the waveguide. The method is highly efficient compared to time integration of a conventional finite-element model of a length of waveguide. In addition, the method provides information about each mode that is excited in the waveguide. The method is demonstrated by modeling a sandwich piezoelectric transducer exciting a waveguide of rectangular cross section, although it could be applied to more complex situations. It is expected that the modeling method will be useful during the optimization of piezoelectric transducers for exciting specific wave propagation modes in waveguides.

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

    Energy Technology Data Exchange (ETDEWEB)

    Rajkovic, Ivan

    2008-10-21

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

  6. Spectrally narrowed leaky waveguide edge emission and transient electrluminescent dynamics of OLEDs

    Energy Technology Data Exchange (ETDEWEB)

    Zhengqing, Gan [Iowa State Univ., Ames, IA (United States)

    2010-01-01

    In summary, there are two major research works presented in this dissertation. The first research project (Chapter 4) is spectrally narrowed edge emission from Organic Light Emitting Diodes. The second project (Chapter 5) is about transient electroluminescent dynamics in OLEDs. Chapter 1 is a general introduction of OLEDs. Chapter 2 is a general introduction of organic semiconductor lasers. Chapter 3 is a description of the thermal evaporation method for OLED fabrication. The detail of the first project was presented in Chapter 4. Extremely narrowed spectrum was observed from the edge of OLED devices. A threshold thickness exists, above which the spectrum is narrow, and below which the spectrum is broad. The FWHM of spectrum depends on the material of the organic thin films, the thickness of the organic layers, and length of the OLED device. A superlinear relationship between the output intensity of the edge emission and the length of the device was observed, which is probably due to the misalignment of the device edge and the optical fiber detector. The original motivation of this research is for organic semiconductor laser that hasn't been realized due to the extremely high photon absorption in OLED devices. Although we didn't succeed in fabricating an electrically pumped organic laser diode, we made a comprehensive research in edge emission of OLEDs which provides valuable results in understanding light distribution and propagation in OLED devices. Chapter 5 focuses on the second project. A strong spike was observed at the falling edge of a pulse, and a long tail followed. The spike was due to the recombination of correlated charge pair (CCP) created by trapped carriers in guest molecules of the recombination zone. When the bias was turned off, along with the decreasing of electric field in the device, the electric field induced quenching decreases and the recombination rate of the CCP increases which result in the spike. This research project provides

  7. Ultrafast energy and momentum resolved dynamics of magnetic correlations in photo-doped Mott insulator Sr2IrO4

    Energy Technology Data Exchange (ETDEWEB)

    Dean, M. P. M.; Cao, Yue; Liu, X.; Wall, S.; Zhu, D.; Mankowsky, R.; Thampy, V.; Chen, X. M.; Vale, J. G.; Casa, D.; Kim, Jungho; Said, A. H.; Juhas, P.; Alonso-Mori, R.; Glownia, J. M.; Robert, A.; Robinson, J.; Sikorski, M.; Song, S.; Kozina, M.; Lemke, H.; Patthey, L; Owada, S.; Katayama, T.; Yabashi, M.; Tanaka, Yoshikazu; Togashi, T.; Liu, Jian; Rayan-Serrao, C.; Kim, B. J.; Huber, L.; Chang, C. -L; McMorrow, D. F.; Forst, M.; Hill, J. P.

    2016-06-01

    Measuring how the magnetic correlations throughout the Brillouin zone evolve in a Mott insulator as charges are introduced dramatically improved our understanding of the pseudogap, non-Fermi liquids and high TC superconductivity. Recently, photoexcitation has been used to induce similarly exotic states transiently. However, understanding how these states emerge has been limited because of a lack of available probes of magnetic correlations in the time domain, which hinders further investigation of how light can be used to control the properties of solids. Here we implement magnetic resonant inelastic X-ray scattering at a free electron laser, and directly determine the magnetization dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state 2~ps after the excitation has strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. The magnetism recovers its two-dimensional (2D) in-plane N\\'eel correlations on a timescale of a few ps, while the three-dimensional (3D) long-range magnetic order restores over a far longer, fluence-dependent timescale of a few hundred ps. The dramatic difference in these two timescales, implies that characterizing the dimensionality of magnetic correlations will be vital in our efforts to understand ultrafast magnetic dynamics.

  8. Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4.

    Science.gov (United States)

    Dean, M P M; Cao, Y; Liu, X; Wall, S; Zhu, D; Mankowsky, R; Thampy, V; Chen, X M; Vale, J G; Casa, D; Kim, Jungho; Said, A H; Juhas, P; Alonso-Mori, R; Glownia, J M; Robert, A; Robinson, J; Sikorski, M; Song, S; Kozina, M; Lemke, H; Patthey, L; Owada, S; Katayama, T; Yabashi, M; Tanaka, Yoshikazu; Togashi, T; Liu, J; Rayan Serrao, C; Kim, B J; Huber, L; Chang, C-L; McMorrow, D F; Först, M; Hill, J P

    2016-06-01

    Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity. Recently, photo-excitation has been used to induce similarly exotic states transiently. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. The marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.

  9. Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr2IrO4

    Science.gov (United States)

    Dean, M. P. M.; Cao, Y.; Liu, X.; Wall, S.; Zhu, D.; Mankowsky, R.; Thampy, V.; Chen, X. M.; Vale, J. G.; Casa, D.; Kim, Jungho; Said, A. H.; Juhas, P.; Alonso-Mori, R.; Glownia, J. M.; Robert, A.; Robinson, J.; Sikorski, M.; Song, S.; Kozina, M.; Lemke, H.; Patthey, L.; Owada, S.; Katayama, T.; Yabashi, M.; Tanaka, Yoshikazu; Togashi, T.; Liu, J.; Rayan Serrao, C.; Kim, B. J.; Huber, L.; Chang, C.-L.; McMorrow, D. F.; Först, M.; Hill, J. P.

    2016-06-01

    Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity. Recently, photo-excitation has been used to induce similarly exotic states transiently. However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr2IrO4. We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. The marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.

  10. Ultrafast Dynamics of Localized and Delocalized Polaron Transitions in P3HT/PCBM Blend Materials: The Effects of PCBM Concentration

    Directory of Open Access Journals (Sweden)

    Alexandrou Ioannis

    2009-01-01

    Full Text Available Abstract Nowadays, organic solar cells have the interest of engineers for manufacturing flexible and low cost devices. The considerable progress of this nanotechnology area presents the possibility of investigating new effects from a fundamental science point of view. In this letter we highlight the influence of the concentration of fullerene molecules on the ultrafast transport properties of charged electrons and polarons in P3HT/PCBM blended materials which are crucial for the development of organic solar cells. Especially, we report on the femtosecond dynamics of localized (P2at 1.45 eV and delocalized (DP2at 1.76 eV polaron states of P3HT matrix with the addition of fullerene molecules as well as the free-electron relaxation dynamics of PCBM-related states. Our study shows that as PCBM concentration increases, the amplified exciton dissociation at bulk heterojunctions leads to increased polaron lifetimes. However, the increase in PCBM concentration can be directly related to the localization of polarons, creating thus two competing trends within the material. Our methodology shows that the effect of changes in structure and/or composition can be monitored at the fundamental level toward optimization of device efficiency.

  11. Ultrafast Dynamics of Localized and Delocalized Polaron Transitions in P3HT/PCBM Blend Materials: The Effects of PCBM Concentration

    Science.gov (United States)

    Lioudakis, Emmanouil; Alexandrou, Ioannis; Othonos, Andreas

    2009-12-01

    Nowadays, organic solar cells have the interest of engineers for manufacturing flexible and low cost devices. The considerable progress of this nanotechnology area presents the possibility of investigating new effects from a fundamental science point of view. In this letter we highlight the influence of the concentration of fullerene molecules on the ultrafast transport properties of charged electrons and polarons in P3HT/PCBM blended materials which are crucial for the development of organic solar cells. Especially, we report on the femtosecond dynamics of localized (P2 at 1.45 eV) and delocalized (DP2 at 1.76 eV) polaron states of P3HT matrix with the addition of fullerene molecules as well as the free-electron relaxation dynamics of PCBM-related states. Our study shows that as PCBM concentration increases, the amplified exciton dissociation at bulk heterojunctions leads to increased polaron lifetimes. However, the increase in PCBM concentration can be directly related to the localization of polarons, creating thus two competing trends within the material. Our methodology shows that the effect of changes in structure and/or composition can be monitored at the fundamental level toward optimization of device efficiency.

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

    Science.gov (United States)

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

    2011-02-10

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

  13. Ultrafast optical beam deflection in a pump probe configuration

    Science.gov (United States)

    Liang, Lingliang; Tian, Jinshou; Wang, Tao; Wu, Shengli; Li, Fuli; Wang, Junfeng; Gao, Guilong

    2016-09-01

    Propagation of a signal beam in an AlGaAs/GaAs waveguide multiple-prism light deflector is theoretically investigated by solving the scalar Helmholtz equation to obtain the dependences of the temporal and spatial resolvable characteristics of the ultrafast deflector on the material dispersion of GaAs including group velocity dispersion and angular dispersion, interface reflection, and interface scattering of multiple-prism deflector. Furthermore, we experimentally confirm that, in this ultrafast beam deflection device, the deflecting angle of the signal light beam is linear with the pump fluence and the temporal resolution of the ultrafast deflection is 10 ps. Our results show that the improvement of the temporal and spatial resolvable performances is possible by properly choosing the structural parameters and enhancing the quality of the device. Project supported by the National Natural Science Foundation of China (Grant Nos. 11274377 and 61176006) and the State Major Research Equipment Project, China (Grant No. ZDY2011-2).

  14. Analysis of the dynamic changes in the soft palate and uvula in obstructive sleep apnea-hypopnea using ultrafast magnetic resonance imaging.

    Science.gov (United States)

    Wang, Y L; Mcdonald, J P; Liu, Y H; Pan, K F; Zhang, X H; Hu, R D

    2014-01-24

    Apnea and the respiratory cycle are dynamic processes in obstructive sleep apnea-hypopnea (OSAH), which occur only during sleep. Our study aimed to observe the dynamic changes in the soft palate and the uvula during wakefulness and sleep using ultrafast magnetic resonance imaging (UMRI) to provide reference data for the pathogenesis and treatment of OSAH. The dynamic changes in the soft palate and uvular tip of 15 male patients (average age: 50.43 ± 9.82 years) with OSAH were evaluated using UMRI of the upper airway while asleep and awake after 1 night of sleep deprivation. A series of midline sagittal images of the upper airway were obtained. The distance from the center of the soft palate to the x-axis (an extended line from the anterior nasal spine to the posterior nasal spine), from the uvular tip to the x-axis, from the center of the soft palate to the y-axis (a perpendicular line from the center of the pituitary to the x-axis), and from the uvular tip to the y-axis (designated as PX, UX, PY, and UY, respectively) were measured during sleep and wakefulness. The minimum PX, PY, UX, and UY were shorter during sleep than during wakefulness, whereas the maxima were longer during sleep (P UX, and UY were larger during sleep (P < 0.01). The upward, downward, forward, and backward ranges of movement of the soft palate and the uvular tip were larger during sleep in OSAH patients. This increased compliance may trigger each airway obstructive event.

  15. Excited state carrier dynamics in CdS{sub x}Se{sub 1-x} semisconductor alloys as studied by ultrafast fluorescence spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Gadd, S.E.

    1995-08-01

    This dissertation discusses studies of the electron-hole pair dynamics of CdS{sub x}Se{sub 1-x} semiconductor alloys for the entire compositional range from x = 1 to x = 0 as examined by the ultrafast fluorescence techniques of time correlated single photon counting and fluorescence upconversion. Specifically, samples with x = 1, .75, .5, .25, and 0 were studied each at a spread of wavelengths about its respective emission maximum which varies according to {lambda} = 718nm - 210x nm. The decays of these samples were found to obey a Kohlrausch distribution, exp [(t/{tau}){sup {beta}}], with the exponent 3 in the range .5-.7 for the alloys. These results are in agreement with those expected for localization due to local potential variations resulting from the random distribution of sulfur and selenium atoms on the element VI A sub-lattice. This localization can be understood in terms of Anderson localization of the holes in states whose energy distribution tails into the forbidden energy band-gap. Because these states have energy dependent lifetimes, the carriers can decay via many parallel channels. This distribution of channels is the ultimate source of the Kohlrausch form of the fluorescence decays.

  16. Excited state carrier dynamics in CdSxSe1-x semisconductor alloys as studied by ultrafast fluorescence spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Gadd, Steven Edward [Univ. of California, Berkeley, CA (United States)

    1995-08-01

    This dissertation discusses studies of the electron-hole pair dynamics of CdSxSe1-x semiconductor alloys for the entire compositional range from x = 1 to x = 0 as examined by the ultrafast fluorescence techniques of time correlated single photon counting and fluorescence upconversion. Specifically, samples with x = 1, .75, .5, .25, and 0 were studied each at a spread of wavelengths about its respective emission maximum which varies according to λ = 718nm - 210x nm. The decays of these samples were found to obey a Kohlrausch distribution, exp [(t/τ)β], with the exponent 3 in the range .5-.7 for the alloys. These results are in agreement with those expected for localization due to local potential variations resulting from the random distribution of sulfur and selenium atoms on the element VI A sub-lattice. This localization can be understood in terms of Anderson localization of the holes in states whose energy distribution tails into the forbidden energy band-gap. Because these states have energy dependent lifetimes, the carriers can decay via many parallel channels. This distribution of channels is the ultimate source of the Kohlrausch form of the fluorescence decays.

  17. Ultrafast dynamics of strong-field dissociative ionization ofCH2Br2 probed by femtosecond soft x-ray transient absorptionspectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Loh, Zhi-Heng; Leone, Stephen R.

    2008-01-15

    Femtosecond time-resolved soft x-ray transient absorption spectroscopy based on a high-order harmonic generation source is used to investigate the dissociative ionization of CH{sub 2}Br{sub 2} induced by 800 nm strong-field irradiation. At moderate peak intensities (2.0 x 10{sup 14} W/cm{sup 2}), strong-field ionization is accompanied by ultrafast C-Br bond dissociation, producing both neutral Br ({sup 2}P{sub 3/2}) and Br* ({sup 2}P{sub 1/2}) atoms together with the CH{sub 2}Br{sup +} fragment ion. The measured rise times for Br and Br* are 130 {+-} 22 fs and 74 {+-} 10 fs, respectively. The atomic bromine quantum state distribution shows that the Br/Br* population ratio is 8.1 {+-} 3.8 and that the Br {sup 2}P{sub 3/2} state is not aligned. The observed product distribution and the timescales of the photofragment appearances suggest that multiple field-dressed potential energy surfaces are involved in the dissociative ionization process. In addition, the transient absorption spectrum of CH{sub 2}Br{sub 2}{sup +} suggests that the alignment of the molecule relative to the polarization axis of the strong-field ionizing pulse determines the electronic symmetry of the resulting ion; alignment of the Br-Br, H-H, and C{sub 2} axis of the molecule along the polarization axis results in the production of the ion {tilde X}({sup 2}B{sub 2}), {tilde B}({sup 2}B{sub 1}) and {tilde C}({sup 2}A{sub 1}) states, respectively. At higher peak intensities (6.2 x 10{sup 14} W/cm{sup 2}), CH{sub 2}Br{sub 2}{sup +} undergoes sequential ionization to form the metastable CH{sub 2}Br{sub 2}{sup 2+} dication. These results demonstrate the potential of core-level probing with high-order harmonic transient absorption spectroscopy for studying ultrafast molecular dynamics.

  18. Polymers in Waveguide Packaging

    Institute of Scientific and Technical Information of China (English)

    Zhiyi Zhang; G. Z.Xiao; Jiaren Liu; C. P. Grover

    2003-01-01

    Polymers were successfully used in the packaging of waveguide-based photonic components in the area of fiber-to-waveguide coupling, waveguide die attachment, strain relief, and waveguide encapsulation. The application results of these polymers were described in this paper.

  19. Q-switched waveguide laser based on two-dimensional semiconducting materials: tungsten disulfide and black phosphorous.

    Science.gov (United States)

    Tan, Yang; Guo, Zhinan; Ma, Linan; Zhang, Han; Akhmadaliev, Shavkat; Zhou, Shengqiang; Chen, Feng

    2016-02-01

    Owing to their unique properties, graphene-like two dimensional semiconducting materials, including Tungsten Disulfide (WS2) and Black Phosphorous (BP), have attracted increasing interest from basic research to practical applications. Herein, we demonstrated the ultrafast nonlinear saturable absorption response of WS2 and BP films in the waveguide structure. Through fabricating WS2 and BP films by evaporating the solutions on glass wafers. Saturable absorber films were attached onto the end-facet of the waveguide, which therefore constitutes a resonant cavity for the waveguide laser. Under a pump laser at 810 nm, we could obtain a stable Q-switched operation in the waveguide structure. This work indicated the significant potential of WS2 and BP for the ultrafast waveguide laser.

  20. Integrated photonic building blocks for next-generation astronomical instrumentation I: the multimode waveguide

    CERN Document Server

    Jovanovic, Nemanja; Gross, Simon; Ireland, Michael; Lawrence, Jon S; Miese, Christopher; Fuerbach, Alexander; Withford, Michael J

    2012-01-01

    We report on the fabrication and characterization of composite multimode waveguide structures that consist of a stack of single-mode waveguides fabricated by ultrafast laser inscription. We explore 2 types of composite structures; those that consist of overlapping single-mode waveguides which offer the maximum effective index contrast and non overlapped structures which support multiple modes via strong evanescent coupling. We demonstrate that both types of waveguides have negligible propagation losses (to within experimental uncertainty) for light injected with focal ratios >8, which corresponds to the cutoff of the waveguides. We also show that right below cutoff, there is a narrow region where the injected focal ratio is preserved (to within experimental uncertainty) at the output. Finally, we outline the major application of these highly efficient waveguides; in a device that is used to reformat the light in the focal plane of a telescope to a slit, in order to feed a diffraction-limited spectrograph.

  1. Efficient supercontinuum generation in quadratic nonlinear waveguides without quasi-phase matching

    CERN Document Server

    Guo, Hairun; Steinert, Michael; Setzpfandt, Frank; Pertsch, Thomas; Chung, Hung-ping; Chen, Yen-Hung; Bache, Morten

    2014-01-01

    Efficient supercontinuum generation (SCG) requires excitation of solitons at the pump laser wavelength. Quadratic nonlinear waveguides may support an effective self-defocusing nonlinearity so solitons can directly be generated at common ultrafast laser wavelengths without any waveguide dispersion engineering. We here experimentally demonstrate efficient SCG in a standard lithium niobate (LN) waveguide without using quasi-phase matching (QPM). By using femtosecond pumps with wavelengths in the $1.25-1.5 \\mu\\rm m$ range, where LN has normal dispersion and thus supports self-defocusing solitons, octave-spanning SCG is observed. An optimized mid-IR waveguide design is expected to support even broader spectra. The QPM-free design reduces production complexity, allows longer waveguides, limits undesired spectral resonances and effectively allows using nonlinear crystals where QPM is inefficient or impossible. This result is important for mid-IR SCG, where QPM-free self-defocusing waveguides in common mid-IR nonline...

  2. Photonic-crystal waveguide biosensor

    DEFF Research Database (Denmark)

    Skivesen, Nina; Têtu, Amélie; Kristensen, Martin

    2007-01-01

    A photonic-crystal waveguide sensor is presented for biosensing. The sensor is applied for refractive index measurements and detection of protein-concentrations. Concentrations around 10 μg/ml (0.15μMolar) are measured with excellent signal to noise ratio, and a broad, dynamic refractive index se...

  3. Efficient 2.9 μm fluorozirconate glass waveguide chip laser.

    Science.gov (United States)

    Lancaster, David G; Gross, Simon; Ebendorff-Heidepriem, Heike; Withford, Michael J; Monro, Tanya M; Jackson, Stuart D

    2013-07-15

    We report a large mode-area holmium-doped ZBLAN waveguide laser operating at 2.9 μm, which was pumped by a 1150 nm diode laser. The laser is based on ultrafast laser inscribed depressed cladding waveguides fabricated in uniformly rare-earth-doped bulk glass. It has a threshold of 28 mW and produced up to 27 mW of output power at an internal slope efficiency of approximately 20%.

  4. Ultrafast chemistry in complex and confined systems

    Indian Academy of Sciences (India)

    Partha Dutta; Kankan Bhattacharyya

    2004-01-01

    Self-organized molecular assemblies play a crucial role in many natural and biological processes. Recent applications of ultrafast laser spectroscopy and computer simulations revealed that chemistry in a confined environment is fundamentally different from that in ordinary solutions. Many recent examples of slow dynamics in constrained environments and their biological implications are discussed.

  5. 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 membr

  6. Ultrafast cyclic voltammetry with asymmetrical potential scan

    Institute of Scientific and Technical Information of China (English)

    Zhi Yong Guo; Xiang Qin Lin

    2008-01-01

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

  7. Ultrafast, correlated multidimensional shell dynamics of neon matrices after photoexcitation of an NO impurity: An MCTDH approach

    Science.gov (United States)

    Uranga-Piña, L.; Meier, C.; Rubayo-Soneira, J.

    2012-08-01

    Photoexcitation of NO embedded in rare gas matrices triggers a shock-wave like radial perturbation of the surrounding rare gas atoms. In this Letter, we present quantum dynamical studies of this process, based on a radial shell model. The high-dimensional quantum dynamics is preformed with the multi-configuration time dependent Hartree (MCTDH) method. By comparison with time-dependent Hartree (TDH) results, we study the effects of dynamical correlations. Their inclusion modifies the high-dimensional wavefunction, however, mean values are well described within the TDH ansatz. Finally, pump-probe signals are simulated and shown to lead to small but measurable effects when including the correlations.

  8. Ultrafast spectroscopic imaging of exfoliated graphene

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-12-15

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

  9. Ultrafast, In Situ Probing of Shocked Solids at the Mesoscale and Beyond: A New Paradigm for Materials Dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Lorenzana, H; Belak, J; Campbell, G; King, W; Nikkel, D; Bradley, K; McNaney, J; Kinney, J; Becker, R; Kalantar, D; Yaakobi, B

    2007-02-15

    Understanding material response under dynamic conditions and extreme pressures at the lattice level is important for being able to generate predictive models of material response. Despite many decades of study, material behavior is primarily inferred from bulk measurements on dynamically loaded samples or the microstructure from recovery experiments and not determined from lattice level measurements made in-situ at the relevant length scale of the governing physics. In the work described here, we report on progress made in advancing this frontier with research conducted under LDRD 04-ERD-071. Specifically, we present advances in, and applications of, dynamic x-ray diffraction, Extended X-ray Absorption Fine Structure and dynamic transmission electron microscopy.

  10. Compact waveguide circular polarizer

    Science.gov (United States)

    Tantawi, Sami G.

    2016-08-16

    A multi-port waveguide is provided having a rectangular waveguide that includes a Y-shape structure with first top arm having a first rectangular waveguide port, a second top arm with second rectangular waveguide port, and a base arm with a third rectangular waveguide port for supporting a TE.sub.10 mode and a TE.sub.20 mode, where the end of the third rectangular waveguide port includes rounded edges that are parallel to a z-axis of the waveguide, a circular waveguide having a circular waveguide port for supporting a left hand and a right hand circular polarization TE.sub.11 mode and is coupled to a base arm broad wall, and a matching feature disposed on the base arm broad wall opposite of the circular waveguide for terminating the third rectangular waveguide port, where the first rectangular waveguide port, the second rectangular waveguide port and the circular waveguide port are capable of supporting 4-modes of operation.

  11. Mechanisms of ultrafast fluorescence depletion spectroscopy and applications to measure slovation dynamics of coummarin 153 in methanol

    Energy Technology Data Exchange (ETDEWEB)

    Yang Songqiu, E-mail: sqyang@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Graduate School of the Chinese Academy of Sciences, Beijing 100039 (China); Liu Jianyong, E-mail: beam@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Zhou Panwang, E-mail: pwzhou@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Chen Junsheng, E-mail: junshengchen@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); Graduate School of the Chinese Academy of Sciences, Beijing 100039 (China); Han Keli, E-mail: klhan@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China); He Guozhong, E-mail: gzhe@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 (China)

    2012-09-15

    Subpicosecond fluorescence depletion spectroscopy (FDS) was used to measure the solvation dynamics of coumarin 153 (C153) in methanol. The FDS mechanisms were discussed. A quasi-continuous model was used to describe the solvational relaxation of excited states. The perturbations of the probe pulse on the excited sample system, including up-conversion and stimulated emission, were sufficiently discussed. For a probe molecule used in the FDS experiment, ensuring that the up-conversion perturbation can be negligible is important. FDS was found to be a good technique for measuring the solvation dynamics of C153 in methanol. - Highlights: Black-Right-Pointing-Pointer Mechanisms of subpicosecond fluorescence depletion spectroscopy. Black-Right-Pointing-Pointer Quasi-continuous model was used to describe the solvational relaxation. Black-Right-Pointing-Pointer The solvation dynamics of coumarin 153 in methanol has been measured.

  12. Spin dynamics induced by ultrafast heating with ferromagnetic/antiferromagnetic interfacial exchange in perpendicularly magnetized hard/soft bilayers

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Q. L., E-mail: maqinli@gmail.com, E-mail: mizukami@wpi-aimr.tohoku.ac.jp; Miyazaki, T.; Mizukami, S., E-mail: maqinli@gmail.com, E-mail: mizukami@wpi-aimr.tohoku.ac.jp [WPI Advanced Institute for Materials Research, Tohoku University, 2-1-1, Katahira, 980-8577 Sendai (Japan); Iihama, S. [Department of Applied Physics, Tohoku University, 6-6-05 Aza-Aoba, Aramaki, Aoba-ku, Sendai 980-8579 (Japan); Zhang, X. M. [Key Laboratory for Anisotropy and Texture of Materials, Ministry of Education, Northeastern University, Shenyang 110819 (China)

    2015-11-30

    The laser-induced spin dynamics of FeCo in perpendicularly magnetized L1{sub 0}-MnGa/FeCo bilayers with ferromagnetic and antiferromagnetic interfacial exchange coupling (IEC) are examined using the time-resolved magneto-optical Kerr effect. We found a precessional phase reversal of the FeCo layer as the IEC changes from ferromagnetic to antiferromagnetic. Moreover, a precession-suspension window was observed when the magnetic field was applied in a certain direction for the bilayer with ferromagnetic IEC. Our observations reveal that the spin dynamics modulation is strongly dependent on the IEC type within the Landau-Lifshitz-Gilbert depiction. The IEC dependence of the precessional phase and amplitude suggests the interesting method for magnetization dynamics modulation.

  13. Complete ultrafast charge carrier dynamics in photo-excited all-inorganic perovskite nanocrystals (CsPbX3).

    Science.gov (United States)

    Mondal, Navendu; Samanta, Anunay

    2017-02-02

    Understanding the nature and dynamics of the photo-induced transients of all-inorganic perovskite nanocrystals (NCs) is key to their exploitation in potential applications. In order to determine the nature of charge carriers, their deactivation pathways and dynamics, the photo-induced transients of CsPbBr3, CsPbBr2I, CsPbBr1.5I1.5 and CsPbI3 NCs are spectrally and temporally characterized employing a combination of femtosecond transient absorption (TA) and photoluminescence (PL) up-conversion techniques and global analysis of the data. The results provide distinct identities of the excitons and free charge carriers and distinguish the hot charge carriers from the cold ones. The carrier trapping is attributed to the electrons and their dynamics is unaffected in mixed halide perovskites. The excitation energy dependence of the TA dynamics suggests that the trap states are shallow in nature and mainly limited near the band-edge level. In mixed halide perovskites, an increase in the iodine content leads to hole trapping in a short time scale (photo-response of these substances and their better utilization in light-based applications.

  14. Ultrafast dynamics of laser-pulse excited semiconductors: non-Markovian quantum kinetic equations with nonequilibrium correlations

    Directory of Open Access Journals (Sweden)

    V.V.Ignatyuk

    2004-01-01

    Full Text Available Non-Markovian kinetic equations in the second Born approximation are derived for a two-zone semiconductor excited by a short laser pulse. Both collision dynamics and running nonequilibrium correlations are taken into consideration. The energy balance and relaxation of the system to equilibrium are discussed. Results of numerical solution of the kinetic equations for carriers and phonons are presented.

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

    Science.gov (United States)

    Lee, Cheng-Wei; Schleife, André

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

  16. Ultrafast science using Laser Wakefield Accelerators

    Science.gov (United States)

    Thomas, Alec G. R.

    2016-10-01

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

  17. Ultrafast infrared spectroscopy in photosynthesis.

    Science.gov (United States)

    Di Donato, Mariangela; Groot, Marie Louise

    2015-01-01

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

  18. Ultrafast structural dynamics of the orthorhombic distortion in the Fe-pnictide parent compound BaFe2As2.

    Science.gov (United States)

    Rettig, L; Mariager, S O; Ferrer, A; Grübel, S; Johnson, J A; Rittmann, J; Wolf, T; Johnson, S L; Ingold, G; Beaud, P; Staub, U

    2016-03-01

    Using femtosecond time-resolved hard x-ray diffraction, we investigate the structural dynamics of the orthorhombic distortion in the Fe-pnictide parent compound BaFe2As2. The orthorhombic distortion analyzed by the transient splitting of the (1 0 3) Bragg reflection is suppressed on an initial timescale of 35 ps, which is much slower than the suppression of magnetic and nematic order. This observation demonstrates a transient state with persistent structural distortion and suppressed magnetic/nematic order which are strongly linked in thermal equilibrium. We suggest a way of quantifying the coupling between structural and nematic degrees of freedom based on the dynamics of the respective order parameters.

  19. Ultrafast structural dynamics of the orthorhombic distortion in the Fe-pnictide parent compound BaFe2As2

    Directory of Open Access Journals (Sweden)

    L. Rettig

    2016-03-01

    Full Text Available Using femtosecond time-resolved hard x-ray diffraction, we investigate the structural dynamics of the orthorhombic distortion in the Fe-pnictide parent compound BaFe2As2. The orthorhombic distortion analyzed by the transient splitting of the (1 0 3 Bragg reflection is suppressed on an initial timescale of 35 ps, which is much slower than the suppression of magnetic and nematic order. This observation demonstrates a transient state with persistent structural distortion and suppressed magnetic/nematic order which are strongly linked in thermal equilibrium. We suggest a way of quantifying the coupling between structural and nematic degrees of freedom based on the dynamics of the respective order parameters.

  20. Multipactor radiation analysis within a waveguide region based on a frequency-domain representation of the dynamics of charged particles.

    Science.gov (United States)

    Gimeno, B; Sorolla, E; Anza, S; Vicente, C; Gil, J; Pérez, A M; Boria, V E; Pérez-Soler, F J; Quesada, F; Alvarez, A; Raboso, D

    2009-04-01

    A technique for the accurate computation of the electromagnetic fields radiated by a charged particle moving within a parallel-plate waveguide is presented. Based on a transformation of the time-varying current density of the particle into a time-harmonic current density, this technique allows the evaluation of the radiated electromagnetic fields both in the frequency and time domains, as well as in the near- and far-field regions. For this purpose, several accelerated versions of the parallel-plate Green's function in the frequency domain have been considered. The theory has been successfully applied to the multipactor discharge occurring within a two metal-plates region. The proposed formulation has been tested with a particle-in-cell code based on the finite-difference time-domain method, obtaining good agreement.

  1. Multi-phonon dynamics of the ultra-fast photoinduced transition of (EDO-TTF)2SbF6

    Science.gov (United States)

    Lorenc, Maciej; Moisan, Nicolas; Servol, Marina; Cailleau, Hervé; Koshihara, Shin-ya; Maesato, Mitsuhiko; Shao, Xiangfeng; Nakano, Yoshiaki; Yamochi, Hideki; Saito, Gunzi; Collet, Eric

    2009-02-01

    We report here the first observation of the photoinduced insulating-to-metal phase transition in the (EDO-TTF)2SbF6 salt, which occurs on the picosecond time-scale. The time-resolved optical experiments performed with 80 fs time-resolution demonstrate that the dynamical process involves several low-frequency phonons, as the crystalline structure is destabilized upon laser excitation.

  2. Plasmonic modulator based on gain-assisted metal-semiconductor-metal waveguide

    DEFF Research Database (Denmark)

    Babicheva, Viktoriia E.; Kulkova, Irina V.; Malureanu, Radu;

    2012-01-01

    We investigate plasmonic modulators with a gain material to be implemented as ultra-compact and ultra-fast active nanodevices in photonic integrated circuits. We analyze metal-semiconductor-metal (MSM) waveguides with InGaAsP-based active material layers as ultra-compact plasmonic modulators. The...

  3. Waveguide cooling system

    Science.gov (United States)

    Chen, B. C. J.; Hartop, R. W.

    1981-04-01

    An improved system is described for cooling high power waveguides by the use of cooling ducts extending along the waveguide, which minimizes hot spots at the flanges where waveguide sections are connected together. The cooling duct extends along substantially the full length of the waveguide section, and each flange at the end of the section has a through hole with an inner end connected to the duct and an opposite end that can be aligned with a flange hole in another waveguide section. Earth flange is formed with a drainage groove in its face, between the through hole and the waveguide conduit to prevent leakage of cooling fluid into the waveguide. The ducts have narrowed sections immediately adjacent to the flanges to provide room for the installation of fasteners closely around the waveguide channel.

  4. Microfabricated Waveguide Atom Traps.

    Energy Technology Data Exchange (ETDEWEB)

    Jau, Yuan-Yu

    2017-09-01

    A nano - scale , microfabricated waveguide structure can in - principle be used to trap atoms in well - defined locations and enable strong photon - atom interactions . A neutral - atom platf orm based on this microfabrication technology will be pre - aligned , which is especially important for quantum - control applications. At present, there is still no reported demonstration of evanescent - field atom trapping using a microfabricated waveguide structure. We described the capabilities established by our team for future development of the waveguide atom - trapping technology at SNL and report our studies to overcome the technical challenges of loading cold atoms into the waveguide atom traps, efficient and broadband optical coupling to a waveguide, and the waveguide material for high - power optical transmission. From the atomic - physics and the waveguide modeling, w e have shown that a square nano - waveguide can be utilized t o achieve better atomic spin squeezing than using a nanofiber for first time.

  5. Ultrafast Transient Absorption Spectroscopy Investigation of Photoinduced Dynamics in POLY(3-HEXYLTHIOPHENE)-BLOCK-OLIGO(ANTHRACENE-9,10-DIYL)

    Science.gov (United States)

    Strain, Jacob; Rathnayake, Hemali; Liu, Jinjun

    2017-06-01

    Semiconducting polymer nanostructures featuring bulk heterojunction (BHJ) architecture are promising light harvesters in photovoltaic (PV) devices because they allow control of individual domain sizes, internal structure and ordering, as well as well-defined contact between the electron donor and acceptor. Power conversion efficiency (PCE) of PV devices strongly depends on photoinduced dynamics. Understanding and optimizing photoinduced charge transfer processes in BHJ's hence help improve the performance of PV devices and increase their PCE in particular. We have investigated the photoinduced dynamics of a block polymer containing moieties of poly-3-hexylthiophene (P3HT) and polyanthracene (PANT) in solution and in solid state with femtosecond transient absorption (TA) spectroscopy. The dynamics of the polymer PANT alone are also studied as a control. The TA spectra of PANT includes a strong excited state absorption centered at 610 (nm) along with a stimulated emission signal stretching past the detection limit into the UV region which is absent in the monomer's spectra in the detection window. The block polymer's TA spectra strongly resembles that of P3HT but a noticeable positive pull on P3HT's stimulated emission signal residing at 575-620 (nm) is indicative of the excited state absorption of PANT in the adjacent spectral region. The doubling of the lifetime exciton delocalization on the block polymer versus P3HT alone have alluded that the lifetime of P3HT is extended by the covalent addition of PANT. The current spectroscopic investigation represents an interesting example of photoinduced processes in systems with complex energy level structure. Studies of dependence of change generation and separation on composition, dimension, and morphology of the heterojunctions are in process.

  6. Ultrafast pump-probe study of the excited-state charge-transfer dynamics in blue copper rusticyanin.

    Science.gov (United States)

    Bizzarri, Anna Rita; Brida, Daniele; Santini, Simona; Cerullo, Giulio; Cannistraro, Salvatore

    2012-04-12

    We have used femtosecond pump-probe spectroscopy to investigate the excited-state dynamics of the anticancer blue copper protein rusticyanin, by exciting its ligand to metal charge-transfer band with 25 fs pump pulses centered at 585 nm. The charge-transfer excited state decays exponentially to the ground state with a time constant of about 230 fs, and its recovery is modulated by coherent oscillations. The Fourier transform of the oscillatory component of the signal provides most of the vibrational modes obtained by means of conventional resonance Raman studies, in addition to the low frequency modes below 80 cm(-1) believed to reflect collective motions of biological relevance.

  7. Phase- and intensity-dependence of ultrafast dynamics in hydrocarbon molecules in few-cycle laser fields

    CERN Document Server

    Kübel, Matthias; Siemering, Robert; Kling, Nora G; Bergues, Boris; Alnaser, Ali S; Ben-Itzhak, Itzik; Moshammer, Robert; de Vivie-Riedle, Regina; Kling, Matthias F

    2016-01-01

    In strong laser fields, sub-femtosecond control of chemical reactions with the carrier-envelope phase (CEP) becomes feasible. We have studied the control of reaction dynamics of acetylene and allene in intense few-cycle laser pulses at 750 nm, where ionic fragments are recorded with a reaction microscope. We find that by varying the CEP and intensity of the laser pulses it is possible to steer the motion of protons in the molecular dications, enabling control over deprotonation and isomerization reactions. The experimental results are compared to predictions from a quantum dynamical model, where the control is based on the manipulation of the phases of a vibrational wave packet by the laser waveform. The measured intensity dependence in the CEP-controlled deprotonation of acetylene is well captured by the model. In the case of the isomerization of acetylene, however, we find differences in the intensity dependence between experiment and theory. For the isomerization of allene, an inversion of the CEP-dependen...

  8. Ultrafast Transient Absorption Spectroscopy Investigation of Excited-State Dynamics of Methyl Ammonium Lead Bromide Perovskite Nanostructures

    Science.gov (United States)

    Jamhawi, Abdelqader; Telfah, Hamzeh; Teunis, Meghan B.; Sardar, Rajesh; Liu, Jinjun

    2017-06-01

    Metal halide perovskites are promising materials for light harvesting. Power conversion efficiency (PCE) of such materials can be improved by tuning the band gap energy and suppressing the trap states. In particular, quantum confinement and shape control of nanostructures are two effective approaches to enhance the photovoltaic properties. Here we report femtosecond transient absorption (TA) spectroscopy studies on the photo-induced dynamics of a series of different nanostructures of methyl ammonium lead bromide (MALB) CH_3NH_3PbBr_3: nanoplatelets (2D), nanowires (1D), nonoparticles (0D), and nanocubes (0D). Experimentally obtained TA spectra are simulated using a global model in both the time and wavelength domains. The fit values of center wavelengths and time constants for various processes demonstrate that dimensional and structural confinement affects not only band structure but also exciton dynamics: Sub-picosecond electron and hole relaxation (in the conduction and valence band, respectively) have been observed, while the exciton recombination process is on the timescale of hundreds of picoseconds. Comparison between TA spectra of different nanostructures suggest that the confinement effect plays a significant role in tuning band gaps and minimizing trap states, which can be utilized to improve the PCE of photovoltaic devices.

  9. Ultrafast IR spectroscopic study of coherent phonons and dynamic spin-lattice coupling in multiferroic LuMnO3

    Science.gov (United States)

    Jang, Kyeong-Jin; Lim, Jongseok; Ahn, Jaewook; Kim, Ji-Hee; Yee, Ki-Ju; Ahn, Jai Seok; Cheong, Sang-Wook

    2010-02-01

    The concurrent existence of ferroelectricity and magnetism within a single crystalline system characterizes the multiferroic materials discovered in recent years. To understand and develop the multiferroic phenomenon, we need to investigate the unusual coupling between spin and lattice degrees of freedom. Spins in multiferroics are expected to be elastically coupled to phonons. Therefore, the time-dependent study can be a crucial factor in understanding the coupled dynamics. Here, we report the observations of strong dynamic spin-lattice coupling in multiferroic LuMnO3. A coherent optical phonon of 3.6 THz and its temperature dependence is measured for the first time from our femtosecond IR pump and probe spectroscopy. Also, we observed a coherent acoustic phonon of 47 GHz similar to a previous report (Lim et al 2003 Appl. Phys. Lett. 83 4800). Temperature-dependent measurements show that both optical and acoustic phonons become significantly underdamped as temperature decreases to TN, and they disappear below TN. These observations reveal that phonons are coupled to spins by magneto-elastic coupling, and the disappearance of phonon modes at TN is consistent with the isostructural coupling scheme suggested by Lee et al (2008 Nature 451 805).

  10. Control of dynamical self-assembly of strongly Brownian nanoparticles through convective forces induced by ultrafast laser

    Science.gov (United States)

    Ilday, Serim; Akguc, Gursoy B.; Tokel, Onur; Makey, Ghaith; Yavuz, Ozgun; Yavuz, Koray; Pavlov, Ihor; Ilday, F. Omer; Gulseren, Oguz

    We report a new dynamical self-assembly mechanism, where judicious use of convective and strong Brownian forces enables effective patterning of colloidal nanoparticles that are almost two orders of magnitude smaller than the laser beam. Optical trapping or tweezing effects are not involved, but the laser is used to create steep thermal gradients through multi-photon absorption, and thereby guide the colloids through convective forces. Convective forces can be thought as a positive feedback mechanism that helps to form and reinforce pattern, while Brownian motion act as a competing negative feedback mechanism to limit the growth of the pattern, as well as to increase the possibilities of bifurcation into different patterns, analogous to the competition observed in reaction-diffusion systems. By steering stochastic processes through these forces, we are able to gain control over the emergent pattern such as to form-deform-reform of a pattern, to change its shape and transport it spatially within seconds. This enables us to dynamically initiate and control large patterns comprised of hundreds of colloids. Further, by not relying on any specific chemical, optical or magnetic interaction, this new method is, in principle, completely independent of the material type being assembled.

  11. Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes

    Science.gov (United States)

    Sturm, F. P.; Tong, X. M.; Palacios, A.; Wright, T. W.; Zalyubovskaya, I.; Ray, D.; Shivaram, N.; Martín, F.; Belkacem, A.; Ranitovic, P.; Weber, Th.

    2017-01-01

    We used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H2 molecules. A nuclear wave packet is created in the B Σ+1u state of the neutral H2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the B Σ+1u electronic state, the effective H2+ ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H2*, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis.

  12. Ultrafast spectroscopy of linear carbon chains: the case of dinaphthylpolyynes

    Directory of Open Access Journals (Sweden)

    Negro M.

    2013-03-01

    Full Text Available The dynamics of excited streets in a special class of linear carbon chains, e.g. dinaphthyl polyynes, has been investigated by ultrafast transient absorption spectroscopy and DFT//TDDFT calculations. The ultrafast formation of a narrow photo-induced absorption band has been observed and assigned to an inter-system crossing event bringing to the formation of triplet excited streets.

  13. Dynamic stiffness of chemically and physically ageing rubber vibration isolators in the audible frequency range: Part 2—waveguide solution

    Science.gov (United States)

    Kari, Leif

    2017-09-01

    The dynamic stiffness of a chemically and physically ageing rubber vibration isolator in the audible frequency range is modelled as a function of ageing temperature, ageing time, actual temperature, time, frequency and isolator dimension. In particular, the dynamic stiffness for an axially symmetric, homogeneously aged rubber vibration isolator is derived by waveguides where the eigenmodes given by the dispersion relation for an infinite cylinder satisfying traction free radial surface boundary condition are matched to satisfy the displacement boundary conditions at the lateral surface ends of the finite rubber cylinder. The constitutive equations are derived in a companion paper (Part 1). The dynamic stiffness is calculated over the whole audible frequency range 20-20,000 Hz at several physical ageing times for a temperature history starting at thermodynamic equilibrium at +25°C and exposed by a sudden temperature step down to -60°C and at several chemical ageing times at temperature +25°C with simultaneous molecular network scission and reformation. The dynamic stiffness results are displaying a strong frequency dependence at a short physical ageing time, showing stiffness magnitude peaks and troughs, and a strong physical ageing time dependence, showing a large stiffness magnitude increase with the increased physical ageing time, while the peaks and troughs are smoothed out. Likewise, stiffness magnitude peaks and troughs are frequency-shifted with increased chemical ageing time. The developed model is possible to apply for dynamic stiffness prediction of rubber vibration isolator over a broad audible frequency range under realistic environmental condition of chemical ageing, mainly attributed to oxygen exposure from outside and of physical ageing, primarily perceived at low-temperature steps.

  14. Direct observation of charge-transfer-to-solvent (CTTS) reactions: Ultrafast dynamics of the photoexcited alkali metal anion sodide (Na-)

    Science.gov (United States)

    Barthel, Erik R.; Martini, Ignacio B.; Schwartz, Benjamin J.

    2000-06-01

    Charge-transfer-to-solvent (CTTS) transitions have been the subject of a great deal of interest recently because they represent the simplest possible charge transfer reaction: The CTTS electron transfer from an atomic ion to a cavity in the surrounding solvent involves only electronic degrees of freedom. Most of the work in this area, both experimental and theoretical, has focused on aqueous halides. Experimentally, however, halides make a challenging choice for studying the CTTS phenomenon because the relevant spectroscopic transitions are deep in the UV and because the charge-transfer dynamics can be monitored only indirectly through the appearance of the solvated electron. In this paper, we show that these difficulties can be overcome by taking advantage of the CTTS transitions in solutions of alkali metal anions, in particular, the near-IR CTTS band of sodide (Na-) in tetrahydrofuran (THF). Using femtosecond pump-probe techniques, we have been able to spectroscopically separate and identify transient absorption contributions not only from the solvated electron, but also from the bleaching dynamics of the Na- ground state and from the absorption of the neutral sodium atom. Perhaps most importantly, we also have been able to directly observe the decay of the Na-* excited CTTS state, providing the first direct measure of the electron transfer rate for any CTTS system. Taken together, the data at a variety of pump and probe wavelengths provide a direct test for several kinetic models of the CTTS process. The model which best fits the data assumes a delayed ejection of the electron from the CTTS excited state in ˜700 fs. Once ejected, a fraction of the electrons, which remain localized in the vicinity of the neutral sodium parent atom, recombine on a ˜1.5-ps time scale. The fraction of electrons that recombine depends sensitively on the choice of excitation wavelength, suggesting multiple pathways for charge transfer. The spectrum of the neutral sodium atom, which

  15. Imaging the ultrafast Kerr effect, free carrier generation, relaxation and ablation dynamics of Lithium Niobate irradiated with femtosecond laser pulses

    Energy Technology Data Exchange (ETDEWEB)

    Garcia-Lechuga, Mario, E-mail: mario@io.cfmac.csic.es; Siegel, Jan, E-mail: j.siegel@io.cfmac.csic.es; Hernandez-Rueda, Javier; Solis, Javier [Laser Processing Group, Instituto de Optica, CSIC, Serrano 121, 28006 Madrid (Spain)

    2014-09-21

    The interaction of high-power single 130 femtosecond (fs) laser pulses with the surface of Lithium Niobate is experimentally investigated in this work. The use of fs-resolution time-resolved microscopy allows us to separately observe the instantaneous optical Kerr effect induced by the pulse and the generation of a free electron plasma. The maximum electron density is reached 550 fs after the peak of the Kerr effect, confirming the presence of a delayed carrier generation mechanism. We have also observed the appearance of transient Newton rings during the ablation process, related to optical interference of the probe beam reflected at the front and back surface of the ablating layer. Finally, we have analyzed the dynamics of the photorefractive effect on a much longer time scale by measuring the evolution of the transmittance of the irradiated area for different fluences below the ablation threshold.

  16. Elucidating the Ultrafast Dynamics of Photoinduced Charge Separation in Metalloporphyrin-Fullerene Dyads Across the Electromagnetic Spectrum

    DEFF Research Database (Denmark)

    Zhang, J.; Pápai, Mátyás Imre; Hirsch, A.

    2016-01-01

    Metalloporphyrins are prominent building blocks in the synthetic toolbox of advanced photodriven molecular devices. When the central ion is paramagnetic, the relaxation pathways within the manifold of excited states are highly intricate so that unravelling the intramolecular energy and electron...... transfer processes is usually a very complex task. This fact is critically hampering the development of applications based on the enhanced coupling offered by the electronic exchange interaction. In this work, the dynamics of charge separation in a copper porphyrin-fullerene are studied with several...... complementary spectroscopic tools across the electromagnetic spectrum (from near-infrared to X-ray wavelengths), each of them providing specific diagnostics. Correlating the various rates clearly demonstrates that the lifetime of the photoinduced charge-separated state exceeds by about 10-fold...

  17. Vibronic Dynamics of the Ultrafast all-trans to 13-cis Photoisomerization of Retinal in Channelrhodopsin-1.

    Science.gov (United States)

    Schnedermann, Christoph; Muders, Vera; Ehrenberg, David; Schlesinger, Ramona; Kukura, Philipp; Heberle, Joachim

    2016-04-13

    Channelrhodopsins are light-gated ion channels with extensive applications in optogenetics. Channelrhodopsin-1 from Chlamydomonas augustae (CaChR1) exhibits a red-shifted absorption spectrum as compared to Channelrhodopsin-2, which is highly beneficial for optogenetic application. The primary event in the photocycle of CaChR1 involves an isomerization of the protein-bound retinal chromophore. Here, we apply highly time-resolved vibronic spectroscopy to reveal the electronic and structural dynamics associated with the first step of the photocycle of CaChR1. We observe vibrationally coherent formation of the P1 intermediate exhibiting a twisted 13-cis retinal with a 110 ± 7 fs time constant. Comparison with low-temperature resonance Raman spectroscopy of the corresponding trapped photoproduct demonstrates that this rapidly formed P1 intermediate is stable for several hundreds of nanoseconds.

  18. Collective excitations in liquid DMSO : FIR spectrum, Low frequency vibrational density of states and ultrafast dipolar solvation dynamics

    CERN Document Server

    Hazra, Milan

    2016-01-01

    Valuable dynamical and structural information about neat liquid DMSO at ambient conditions can be obtained through study of low frequency vibrations in the far infrared (FIR), that is, terahertz regime. For DMSO, collective excitations as well as single molecule stretches and bends have been measured by different kinds of experiments such as OHD-RIKES and terahertz spectroscopy. In the present work we investigate the intermolecular vibrational spectrum of DMSO through three different computational techniques namely (i) the far-infra red spectrum obtained through Fourier transform of total dipole moment auto time correlation function, (ii) from Fourier transform of the translational and angular velocity time autocorrelation functions and a (iii) quenched normal mode analysis of the parent liquid at 300K. The three spectrum, although exhibit differences among each other, reveal similar features which are in good, semi-quantitative, agreement with experimental results. Study of participation ratio of the density...

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

    Science.gov (United States)

    Govind, Chinju; Karunakaran, Venugopal

    2017-04-13

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

  20. Plasmonic antennas as design elements for coherent ultrafast nanophotonics.

    Science.gov (United States)

    Brinks, Daan; Castro-Lopez, Marta; Hildner, Richard; van Hulst, Niek F

    2013-11-12

    Broadband excitation of plasmons allows control of light-matter interaction with nanometric precision at femtosecond timescales. Research in the field has spiked in the past decade in an effort to turn ultrafast plasmonics into a diagnostic, microscopy, computational, and engineering tool for this novel nanometric-femtosecond regime. Despite great developments, this goal has yet to materialize. Previous work failed to provide the ability to engineer and control the ultrafast response of a plasmonic system at will, needed to fully realize the potential of ultrafast nanophotonics in physical, biological, and chemical applications. Here, we perform systematic measurements of the coherent response of plasmonic nanoantennas at femtosecond timescales and use them as building blocks in ultrafast plasmonic structures. We determine the coherent response of individual nanoantennas to femtosecond excitation. By mixing localized resonances of characterized antennas, we design coupled plasmonic structures to achieve well-defined ultrafast and phase-stable field dynamics in a predetermined nanoscale hotspot. We present two examples of the application of such structures: control of the spectral amplitude and phase of a pulse in the near field, and ultrafast switching of mutually coherent hotspots. This simple, reproducible and scalable approach transforms ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid-state physics, and quantum biology.

  1. In Situ Laser Crystallization of Amorphous Silicon for TFT Applications: Controlled Ultrafast Studies in the Dynamic TEM

    Energy Technology Data Exchange (ETDEWEB)

    Taheri, M; Teslich, N; Lu, J P; Morgan, D; Browning, N

    2008-02-08

    An in situ method for studying the role of laser energy on the microstructural evolution of polycrystalline Si is presented. By monitoring both laser energy and microstructural evolution simultaneously in the dynamic transmission electron microscope, information on grain size and defect concentration can be correlated directly with processing conditions. This proof of principle study provides fundamental scientific information on the crystallization process that has technological importance for the development of thin film transistors. In conclusion, we successfully developed a method for studying UV laser processing of Si films in situ on nanosecond time scales, with ultimate implications for TFT application improvements. In addition to grain size distribution as a function of laser energy density, we found that grain size scaled with laser energy in general. We showed that nanosecond time resolution allowed us to see the nucleation and growth front during processing, which will help further the understanding of microstructural evolution of poly-Si films for electronic applications. Future studies, coupled with high resolution TEM, will be performed to study grain boundary migration, intergranular defects, and grain size distribution with respect to laser energy and adsorption depth.

  2. Ultrafast dynamics of a near-solid-density layer in an intense femtosecond laser-excited plasma

    Energy Technology Data Exchange (ETDEWEB)

    Adak, Amitava; Chatterjee, Gourab; Kumar Singh, Prashant; Lad, Amit D.; Brijesh, P.; Kumar, G. Ravindra, E-mail: grk@tifr.res.in [Tata Institute of Fundamental Research, Dr. Homi Bhabha Road, Colaba, Mumbai 400005 (India); Blackman, David R. [York Plasma Institute, University of York, Heslington, York YO10 5DQ (United Kingdom); Robinson, A. P. L. [Central Laser Facility, Rutherford-Appleton Laboratory, Chilton, Didcot OX10 0QX (United Kingdom); Pasley, John [York Plasma Institute, University of York, Heslington, York YO10 5DQ (United Kingdom); Central Laser Facility, Rutherford-Appleton Laboratory, Chilton, Didcot OX10 0QX (United Kingdom)

    2014-06-15

    We report on the picosecond dynamics of a near-solid-density plasma generated by an intense, infrared (λ = 800 nm) femtosecond laser using time-resolved pump-probe Doppler spectrometry. An initial red-shift is observed in the reflected third harmonic (λ = 266 nm) probe pulse, which gets blue-shifted at longer probe-delays. A combination of particle-in-cell and radiation-hydrodynamics modelling is performed to model the pump laser interaction with the solid target. The results are post-processed to predict the Doppler shift. An excellent agreement is found between the results of such modelling and the experiment. The modelling suggests that the initial inward motion of the critical surface observed in the experiment is due to the passage of a shock-wave-like disturbance, launched by the pump interaction, propagating into the target. Furthermore, in order to achieve the best possible fit to the experimental data, it was necessary to incorporate the effects of bulk ion-acceleration resulting from the electrostatic field set up by the expulsion of electrons from the laser envelope. We also present results of time-resolved pump-probe reflectometry, which are corroborated with the spectrometry results using a 1-D reflectivity model.

  3. Carrier envelope phase effects in ultrafast, strong-field ionization dynamics of multielectron systems: Xe and CS$_2$

    CERN Document Server

    Mathur, D; Dharmadhikari, A K; Dharmadhikari, J A

    2013-01-01

    Carrier envelope phase (CEP) stabilized 5 fs and 22 fs pulses of intense 800 nm light are used to probe the strong-field ionization dynamics of multielectron entities, xenon and carbon disulfide. We compare ion yields obtained with and without CEP-stabilization: with 8-cycle (22 fs) pulses, Xe$^{6+}$ yields are suppressed (relative to Xe$^+$ yields) by between 30% and 50%, depending on phase, reflecting the phase dependence of non-sequential ionization and its contribution to the formation of higher charge states. On the other hand, ion yields for Xe$^{q+}$ ($q$=2-4) with CEP-stablized pulses are enhanced (by up to 50%) compared to those with CEP-unstabilized pulses. Such enhancment is particulary pronounced with 2-cycle (5 fs) pulses and is distinctly phase-dependent. Orbital shape and symmetry are found to have a bearing on the response of CS$_2$ to variations in optical field that are effected as CE phase is controllably altered, keeping the overall intensity constant. Molecular fragmentation is found to d...

  4. Ultrafast nuclear dynamics in halomethanes studied with time-resolved Coulomb explosion imaging and channel-selective Fourier spectroscopy

    Science.gov (United States)

    Malakar, Y.; Kaderiya, B.; Pearson, W. L.; Ziaee, F.; Kanaka Raju, P.; Zohrabi, M.; Jensen, K.; Rajput, J.; Ben-Itzhak, I.; Rolles, D.; Rudenko, A.

    2016-05-01

    Halomethanes have recently attracted considerable attention since they often serve as prototype systems for laser-controlled chemistry (e.g., selective bond breaking or concerted elimination reactions), and are important molecules in atmospheric chemistry. Here we combine a femtosecond laser pump-probe setup with coincident 3D ion momentum imaging apparatus to study strong-field induced nuclear dynamics in methane and several of its halogenated derivatives (CH3 I, CH2 I2, CH2 ICl). We apply a time-resolved Coulomb explosion imaging technique to map the nuclear motion on both, bound and continuum potential surfaces, disentangle different fragmentation pathways and, for halogenated molecules, observe clear signatures of vibrational wave packets in neutral or ionized states. Channel-selective and kinetic-energy resolved Fourier analysis of these data allows for unique identification of different electronic states and vibrational modes responsible for a particular structure. Supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. DOE. K. R. P. and W. L. P. supported by NSF Award No. IIA-143049. K.J. supported by the NSF-REU Grant No. PHYS-1461251.

  5. 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...

  6. Roadmap on ultrafast optics

    Science.gov (United States)

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

    2016-09-01

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

  7. All-optical switching in optically induced nonlinear waveguide couplers

    Energy Technology Data Exchange (ETDEWEB)

    Diebel, Falko, E-mail: falko.diebel@uni-muenster.de; Boguslawski, Martin; Rose, Patrick; Denz, Cornelia [Institut für Angewandte Physik and Center for Nonlinear Science (CeNoS), Westfälische Wilhelms-Universität Münster, 48149 Münster (Germany); Leykam, Daniel; Desyatnikov, Anton S. [Nonlinear Physics Centre, Research School of Physics and Engineering, The Australian National University, Canberra ACT 0200 (Australia)

    2014-06-30

    We experimentally demonstrate all-optical vortex switching in nonlinear coupled waveguide arrays optically induced in photorefractive media. Our technique is based on multiplexing of nondiffracting Bessel beams to induce various types of waveguide configurations. Using double- and quadruple-well potentials, we demonstrate precise control over the coupling strength between waveguides, the linear and nonlinear dynamics and symmetry-breaking bifurcations of guided light, and a power-controlled optical vortex switch.

  8. Ultrafast Carrier Dynamics Measured by the Transient Change in the Reflectance of InP and GaAs Film

    Energy Technology Data Exchange (ETDEWEB)

    Klopf, John [Helmholtz Association of German Research Centers, Dresden (Germany)

    2005-10-31

    the dynamics of the hot carrier distributions in these materials, but also provide the basis for future development of better diagnostic instruments for the non-destructive evaluation of these important materials. A theoretical model describing the change in reflectance due to the photoexcited hot carrier distribution has also been developed. By applying this model to the experimental results, several important material parameters such as the electron-phonon scattering time and the rates for diffusion and several recombination processes are determined. These values are compared with those reported for similar materials, and the validity of the results is discussed. A complete description of the experimental technique as well as the theoretical reflectance model is presented.

  9. Ultrafast and nanoscale diodes

    Science.gov (United States)

    Zhang, Peng; Lau, Y. Y.

    2016-10-01

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

  10. Quantum dynamics on a three-sheeted six-dimensional ab initio potential-energy surface of the phosphine cation: Simulation of the photoelectron spectrum and the ultrafast radiationless decay dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Bhattacharyya, Swarnendu, E-mail: swarnendu.bhattacharyya@ch.tum.de; Domcke, Wolfgang, E-mail: wolfgang.domcke@ch.tum.de [Department of Chemistry, Technische Universität München, D-85748, Garching (Germany); Dai, Zuyang [Department of Physics and State Key Laboratory of Low-Dimensional Quantum Physics, Tsinghua University, Beijing 100084 (China)

    2015-11-21

    A diabatic three-sheeted six-dimensional potential-energy surface has been constructed for the ground state and the lowest excited state of the PH{sub 3}{sup +} cation. Coupling terms of Jahn-Teller and pseudo-Jahn-Teller origin up to eighth order had to be included to describe the pronounced anharmonicity of the surface due to multiple conical intersections. The parameters of the diabatic Hamiltonian have been optimized by fitting the eigenvalues of the potential-energy matrix to ab initio data calculated at the CASSCF/MRCI level employing the correlation-consistent triple-ζ basis. The theoretical photoelectron spectrum of phosphine and the non-adiabatic nuclear dynamics of the phosphine cation have been computed by propagating nuclear wave packets with the multiconfiguration time-dependent Hartree method. The theoretical photoelectron bands obtained by Fourier transformation of the autocorrelation function agree well with the experimental results. It is shown that the ultrafast non-radiative decay dynamics of the first excited state of PH{sub 3}{sup +} is dominated by the exceptionally strong Jahn-Teller coupling of the asymmetric bending vibrational mode together with a hyperline of conical intersections with the electronic ground state induced by the umbrella mode. Time-dependent population probabilities have been computed for the three adiabatic electronic states. The non-adiabatic Jahn-Teller dynamics within the excited state takes place within ≈5 fs. Almost 80% of the excited-state population decay to the ground state within about 10 fs. The wave packets become highly complex and delocalized after 20 fs and no further significant transfer of electronic population seems to occur up to 100 fs propagation time.

  11. Ultrafast laser inscription of an integrated photonic lantern

    Science.gov (United States)

    Thomson, R.; Birks, T.; Leon-Saval, S.; Kar, A.; Bland-Hawthorn, J.

    2011-03-01

    We used ultrafast laser inscription to fabricate three-dimensional integrated optical transitions that efficiently couple light from a multimode waveguide to a two-dimensional array of single mode waveguides and back. Although the entire device has an average insertion loss of 5.7 dB at 1539 nm, only ≈0.7 dB is due to mode coupling losses. Based on an analysis which is presented in the paper, we expect that our device should convert a multimode input into an array of single modes with a loss of ≈2.0 dB, assuming the input coupling losses are zero. Such devices have applications in astrophotonics and remote sensing.

  12. 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.

  13. Perspective: Ultrafast magnetism and THz spintronics

    Science.gov (United States)

    Walowski, Jakob; Münzenberg, Markus

    2016-10-01

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

  14. Ultrafast spectroscopy of quantum dots

    CERN Document Server

    Foo, E

    2001-01-01

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

  15. Graphene antidot lattice waveguides

    DEFF Research Database (Denmark)

    Pedersen, Jesper Goor; Gunst, Tue; Markussen, Troels

    2012-01-01

    We introduce graphene antidot lattice waveguides: nanostructured graphene where a region of pristine graphene is sandwiched between regions of graphene antidot lattices. The band gaps in the surrounding antidot lattices enable localized states to emerge in the central waveguide region. We model...... the waveguides via a position-dependent mass term in the Dirac approximation of graphene and arrive at analytical results for the dispersion relation and spinor eigenstates of the localized waveguide modes. To include atomistic details we also use a tight-binding model, which is in excellent agreement...... with the analytical results. The waveguides resemble graphene nanoribbons, but without the particular properties of ribbons that emerge due to the details of the edge. We show that electrons can be guided through kinks without additional resistance and that transport through the waveguides is robust against...

  16. Ultra-fast cell counters based on microtubular waveguides

    Science.gov (United States)

    Bausch, Cornelius S.; Heyn, Christian; Hansen, Wolfgang; Wolf, Insa M. A.; Diercks, Björn-Philipp; Guse, Andreas H.; Blick, Robert H.

    2017-01-01

    We present a radio-frequency impedance-based biosensor embedded inside a semiconductor microtube for the in-flow detection of single cells. An impedance-matched tank circuit and a tight wrapping of the electrodes around the sensing region, which creates a close, leakage current-free contact between cells and electrodes, yields a high signal-to-noise ratio. We experimentally show a twofold improved sensitivity of our three-dimensional electrode structure to conventional planar electrodes and support these findings by finite element simulations. Finally, we report on the differentiation of polystyrene beads, primary mouse T lymphocytes and Jurkat T lymphocytes using our device. PMID:28134293

  17. Ultra-Fast Optical Signal Processing in Nonlinear Silicon Waveguides

    DEFF Research Database (Denmark)

    Oxenløwe, Leif Katsuo; Galili, Michael; Pu, Minhao;

    2011-01-01

    We describe recent demonstrations of exploiting highly nonlinear silicon nanowires for processing Tbit/s optical data signals. We perform demultiplexing and optical waveform sampling of 1.28 Tbit/s and wavelength conversion of 640 Gbit/s data signals....

  18. Characterization of UV written waveguides with luminescence microscopy

    DEFF Research Database (Denmark)

    Svalgaard, Mikael; Harpøth, Anders; Rosbirk, Tue

    2005-01-01

    Luminescence microscopy is used to measure the refractive index profile and molecular defect distribution of UV written waveguides with a spatial resolution of ~0.4 mm and high signal-to-noise ratio. The measurements reveal comlex waveguide formation dynamics with significant topological changes...

  19. Optical amplitude and phase modulation dynamics at the single-photon level in a quantum dot ridge waveguide

    CERN Document Server

    Moody, Galan; Feldman, Ari; Harvey, Todd; Mirin, Richard P; Silverman, Kevin L

    2016-01-01

    The amplitude and phase of a material's nonlinear optical response provide insight into the underlying electronic dynamics that determine its optical properties. Phase-sensitive nonlinear spectroscopy techniques are widely implemented to explore these dynamics through demodulation of the complex optical signal field into its quadrature components; however, complete reconstruction of the optical response requires measuring both the amplitude and phase of each quadrature, which is often lost in standard detection methods. Here, we implement a heterodyne-detection scheme to fully reconstruct the amplitude and phase response of spectral hole-burning from InAs/GaAs charged quantum dots. We observe an ultra-narrow absorption profile and a corresponding dispersive lineshape of the phase, which reflect the nanosecond optical coherence time of the charged exciton transition. Simultaneously, the measurements are sensitive to electron spin relaxation dynamics on a millisecond timescale, as this manifests as a magnetic-f...

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

    CERN Document Server

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

    2013-01-01

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

  1. Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO 3

    Energy Technology Data Exchange (ETDEWEB)

    Kozina, M.; Driel, T.van; Chollet, M.; Sato, T.; Glownia, J.M.; Wandel, S.; /SLAC; Radovic, M.; /PSI, SLS /PSI, Villigen; Staub, U.; /PSI, Villigen; Hoffmann, M.C.; /SLAC

    2017-09-01

    We use ultrafast X-ray pulses to characterize the lattice response of SrTiO3 when driven by strong terahertz fields. We observe transient changes in the diffraction intensity with a delayed onset with respect to the driving field. Fourier analysis reveals two frequency components corresponding to the two lowest energy zone-center optical modes in SrTiO3. The lower frequency mode exhibits clear softening as the temperature is decreased while the higher frequency mode shows slight temperature dependence.

  2. Waveguide arrangements based on adiabatic elimination

    Energy Technology Data Exchange (ETDEWEB)

    Suchowski, Haim; Mrejen, Michael; Wu, Chihhui; Zhang, Xiang

    2016-09-13

    This disclosure provides systems, methods, and apparatus related to nanophotonics. In one aspect, an arrangement of waveguides includes a substrate and three waveguides. Each of the three waveguides may be a linear waveguide. A second waveguide is positioned between a first waveguide and a third waveguide. The dimensions and positions of the first, the second, and the third waveguides are specified to substantially eliminate coupling between the first waveguide and the third waveguide over a distance of about 1 millimeter to 2 millimeters along lengths of the first waveguide, the second waveguide, and the third waveguide.

  3. Ptychographic ultrafast pulse reconstruction

    CERN Document Server

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

    2014-01-01

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

  4. Dielectric Waveguide lasers

    NARCIS (Netherlands)

    Pollnau, Markus; Orlovic, V.A.; Pachenko, V.; Scherbakov, I.A.

    2007-01-01

    Our recent results on planar and channel waveguide fabrication and lasers in the dielectric oxide materials Ti:sapphire and rare-earth-ion-doped potassium yttrium double tungstate (KYW) are reviewed. We have employed waveguide fabrication methods such as liquid phase epitaxy and reactive ion etching

  5. Exact equivalent straight waveguide model for bent and twisted waveguides

    DEFF Research Database (Denmark)

    Shyroki, Dzmitry

    2008-01-01

    Exact equivalent straight waveguide representation is given for a waveguide of arbitrary curvature and torsion. No assumptions regarding refractive index contrast, isotropy of materials, or particular morphology in the waveguide cross section are made. This enables rigorous full-vector modeling o...... of in-plane curved or helically wound waveguides with use of available simulators for straight waveguides without the restrictions of the known approximate equivalent-index formulas....

  6. Comprehensive Studies of Ultrafast Laser Excited Warm Dense Gold

    Science.gov (United States)

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

    2016-10-01

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

  7. Ultrafast electron transport in graphene and magnetic nanostructures

    Science.gov (United States)

    Turchinovich, Dmitry

    2016-03-01

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

  8. Ultrafast dynamics of free carriers induced by two-photon excitation in bulk ZnSe crystal%双光子激发ZnSe自由载流子超快动力学研究∗

    Institute of Scientific and Technical Information of China (English)

    2015-01-01

    Semiconductor materials exhibiting large optical nonlinearities and ultrafast nonlinear response have received ex-tensive attention because of their potential applications in optical limiting, all-optical devices, optical telecommunication, and so on. As a direct-gap II-VI bulk semiconductor, ZnSe crystal has been exploited as the nonlinear optical devices in the regimes of nanoseconds and picoseconds during the past years. Owing to today’s fast advance of laser sources with ultrashort femtosecond pulse duration, it is possible to investigate the ultrafast optical nonlinearities in the bulk ZnSe crystal. In this paper, we experimentally investigate the ultrafast dynamics of free-carriers induced by two-photon excitation in the bulk ZnSe crystal. By performing open-aperture Z-scan experiments with 41 fs laser pulses at the wavelength of 532 nm under the condition of low excitation intensity, the two-photon absorption coefficient is measured. As the excitation intensity exceeds a critical value, the interplay between third- and fifth-order nonlinear absorption processes is observed. To evaluate the ultrafast dynamics of free carriers, we have carried out femtosecond time-resolved degen-erate pump-probe measurements with the same laser system used for Z-scan experiments in different levels of pump intensities. It is shown that the transient absorption signals peaked at the zero delay is a linearly increasing function of pump intensity, indicating that the observed instantaneous nonlinear absorption is dominated by the interband two-photon absorption process. At moderate irradiance, the transient absorption signals obviously indicate two components, arising from the two-photon absorption-induced free-carrier absorption, which is equivalent to the fifth-order nonlinear absorption process. Under the excitation of relatively high pump intensity, the magnitude of the reduction of free-carrier absorption signal becomes faster, suggesting that the ZnSe crystal exhibits a

  9. Tunable Broadband Radiation Generated Via Ultrafast Laser Illumination of an Inductively Charged Superconducting Ring.

    Science.gov (United States)

    Bulmer, John; Bullard, Thomas; Dolasinski, Brian; Murphy, John; Sparkes, Martin; Pangovski, Krste; O'Neill, William; Powers, Peter; Haugan, Timothy

    2015-12-11

    An electromagnetic transmitter typically consists of individual components such as a waveguide, antenna, power supply, and an oscillator. In this communication we circumvent complications associated with connecting these individual components and instead combine them into a non-traditional, photonic enabled, compact transmitter device for tunable, ultrawide band (UWB) radiation. This device is a centimeter scale, continuous, thin film superconducting ring supporting a persistent super-current. An ultrafast laser pulse (required) illuminates the ring (either at a point or uniformly around the ring) and perturbs the super-current by the de-pairing and recombination of Cooper pairs. This generates a microwave pulse where both ring and laser pulse geometry dictates the radiated spectrum's shape. The transmitting device is self contained and completely isolated from conductive components that are observed to interfere with the generated signal. A rich spectrum is observed that extends beyond 30 GHz (equipment limited) and illustrates the complex super-current dynamics bridging optical, THz, and microwave wavelengths.

  10. Optical waveguide enhanced photovoltaics.

    Science.gov (United States)

    Rühle, Sven; Greenwald, Shlomit; Koren, Elad; Zaban, Arie

    2008-12-22

    Enhanced light to electric power conversion efficiency of photovoltaic cells with a low absorbance was achieved using waveguide integration. We present a proof of concept using a very thin dye-sensitized solar cell which absorbed only a small fraction of the light at normal incidence. The glass substrate in conjunction with the solar cells reflecting back contact formed a planar waveguide, which lead to more than four times higher conversion efficiency compared to conventional illumination at normal incidence. This illumination concept leads to a new type of multi-junction PV systems based on enforced spectral splitting along the waveguide.

  11. Photonic integration using asymmetric twin-waveguides

    Science.gov (United States)

    Studenkov, Pavel V.

    A novel approach to fabrication of monolithic photonic integrated circuits based on the asymmetric twin- waveguide (ATG) structure is proposed and demonstrated. In contrast to the conventional integration methods relying on semiconductor regrowth, the ATG approach requires only one epitaxy step, while the integrated devices are defined by post-growth patterning. The ATG structure contains two evanescently coupled waveguide layers separated by a cladding layer. The upper layer provides optical gain for the active devices such as lasers and semiconductor optical amplifiers. The transparent lower layer is used to make waveguides and optical interconnects on the chip. Thus the ATG represents a versatile integration platform for cost- effective fabrication of photonic integrated circuits, similar in some respects to the electronic CMOS platform. Light propagation and coupling in the ATG structure are analyzed using the beam propagation method to optimize the layer design. It is shown that the asymmetric refractive index profile eliminates undesirable optical coupling between the waveguide layers. At the interfaces between the active and passive devices, lateral tapers are used to induce vertical coupling of light with a coupling loss of typically integrated devices can be separately optimized to achieve performance close to that of the conventional discrete components. The design of taper couplers is described in detail, and their performance is experimentally verified. Using the ATG approach, several integrated devices were fabricated in the InGaAsP/InP material system for λ = 1.55 μm wavelength operation. Lasers and semiconductor optical amplifiers with integrated waveguides were characterized to test the integration approach. Single-frequency, distributed Bragg reflector (DBR) lasers achieved output power of 11 mW with a 40 dB side-mode suppression ratio. A DBR laser with integrated electroabsorption modulator had a 24 dB extinction ratio between 0V and -2V bias

  12. An ultrafast study of Zinc Phthalocyanine in DMSO

    CSIR Research Space (South Africa)

    Ombinda-Lemboumba, Saturnin

    2010-10-01

    Full Text Available The ultrafast dynamics of Zinc Phthalocyanine was studied using trasient absorption pump probe spectroscopy. Zinc Phthalocyanine was excited (pumped) at 672nm and probed by a white light continuum. The pump-probe technique used in this study...

  13. 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.

  14. Light-Sound Interaction in Nanoscale Silicon Waveguides

    CERN Document Server

    Van Laer, Raphaël

    2016-01-01

    This thesis studies the interaction between near-infrared light and gigahertz sound in nanoscale silicon waveguides. Chapter 2 introduces photon-phonon coupling and its theoretical description, describing basic mechanisms and developing a quantum field theory of the process. Chapter 3 explores the dynamical effects in both waveguides and cavities. It also proves a connection between the Brillouin gain coefficient and the vacuum coupling rate. Chapter 4 deals with the observation of Brillouin scattering in nanoscale silicon waveguides. The waveguides tightly confine $193 \\, \\text{THz}$ light and $10 \\, \\text{GHz}$ acoustic vibrations. The acoustic quality factor remains limited to about $300$ because of leakage into silica substrate. These waveguides are optically transparent in a narrow band of frequencies at a pump power of $25 \\, \\text{mW}$. Besides this amplification, we translate a $10 \\, \\text{GHz}$ microwave signal across $1 \\, \\text{THz}$. Chapter 5 extends the experimental work of chapter 4 by fabrica...

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

    Science.gov (United States)

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

    2014-08-01

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

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

    Science.gov (United States)

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

    2016-05-01

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

  17. Omnidirectional optical waveguide

    Science.gov (United States)

    Bora, Mihail; Bond, Tiziana C.

    2016-08-02

    In one embodiment, a system includes a scintillator material; a detector coupled to the scintillator material; and an omnidirectional waveguide coupled to the scintillator material, the omnidirectional waveguide comprising: a plurality of first layers comprising one or more materials having a refractive index in a first range; and a plurality of second layers comprising one or more materials having a refractive index in a second range, the second range being lower than the first range, a plurality of interfaces being defined between alternating ones of the first and second layers. In another embodiment, a method includes depositing alternating layers of a material having a relatively high refractive index and a material having a relatively low refractive index on a substrate to form an omnidirectional waveguide; and coupling the omnidirectional waveguide to at least one surface of a scintillator material.

  18. Extreme skin depth waveguides

    CERN Document Server

    Jahani, Saman

    2014-01-01

    Recently, we introduced a paradigm shift in light confinement strategy and introduced a class of extreme skin depth (e-skid) photonic structures (S. Jahani and Z. Jacob, "Transparent sub-diffraction optics: nanoscale light confinement without metal," Optica 1, 96-100 (2014)). Here, we analytically establish that figures of merit related to light confinement in dielectric waveguides are fundamentally tied to the skin depth of waves in the cladding. We contrast the propagation characteristics of the fundamental mode of e-skid waveguides and conventional waveguides to show that the decay constant in the cladding is dramatically larger in e-skid waveguides, which is the origin of sub-diffraction confinement. Finally, we propose an approach to verify the reduced skin depth in experiment using the decrease in the Goos-H\\"anchen phase shift.

  19. Nanoscale waveguiding methods.

    Science.gov (United States)

    Wang, Chia-Jean; Lin, Lih Y

    2007-05-01

    While 32 nm lithography technology is on the horizon for integrated circuit (IC) fabrication, matching the pace for miniaturization with optics has been hampered by the diffraction limit. However, development of nanoscale components and guiding methods is burgeoning through advances in fabrication techniques and materials processing. As waveguiding presents the fundamental issue and cornerstone for ultra-high density photonic ICs, we examine the current state of methods in the field. Namely, plasmonic, metal slot and negative dielectric based waveguides as well as a few sub-micrometer techniques such as nanoribbons, high-index contrast and photonic crystals waveguides are investigated in terms of construction, transmission, and limitations. Furthermore, we discuss in detail quantum dot (QD) arrays as a gain-enabled and flexible means to transmit energy through straight paths and sharp bends. Modeling, fabrication and test results are provided and show that the QD waveguide may be effective as an alternate means to transfer light on sub-diffraction dimensions.

  20. Ultrafast spectroscopy of linear carbon chains: the case of dinaphthylpolyynes.

    Science.gov (United States)

    Fazzi, D; Scotognella, F; Milani, A; Brida, D; Manzoni, C; Cinquanta, E; Devetta, M; Ravagnan, L; Milani, P; Cataldo, F; Lüer, L; Wannemacher, R; Cabanillas-Gonzalez, J; Negro, M; Stagira, S; Vozzi, C

    2013-06-21

    The dynamics of excited states in α,ω-dinaphthylpolyyne, a class of linear sp-carbon chains, has been investigated by ultrafast transient absorption spectroscopy and DFT//TDDFT calculations. We show that the role of molecular conformers, in which end-capped naphthalene rings are planar or perpendicular to the polyyne plane, is fundamental for understanding both the steady state properties, such as UV-Vis absorption spectra and vibronic transitions, and the ultrafast transient absorption features. In particular, we observed in one of the conformers the ultrafast formation of a narrow photo-induced absorption band rising within 30 ps. This band can be assigned to an inter-system crossing event leading to the formation of triplet excited states.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-03-15

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

  2. 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.

  3. Resolving Ultrafast Heating of Dense Cryogenic Hydrogen

    Science.gov (United States)

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

    2014-03-01

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

  4. Development and Implementation of an Ultrafast Vacuum-UV (8eV) Light Source for use in UV-VUV Pump Probe Experiments of Neutral Excited State Dynamics

    Science.gov (United States)

    Liu, Yusong; Horton, Spencer; Matsika, Spiridoula; Weinacht, Thomas

    2016-05-01

    Probing neutral excited state dynamics in polyatomic molecules with ultrafast laser systems enables us to study phenomena such as internal conversion, isomerization, intersystem crossing, and dissociation. Using the third harmonic (260 nm) and the fifth harmonic (156 nm) of our laser system we have developed an apparatus to perform pump-probe experiments for the study neutral excited state dynamics in various polyatomic molecules. The fifth harmonic of our laser system is generated through the four-wave-mixing process of k5 ω = 2k3 ω -kω performed with a non-collinear geometry in an argon gas cell. In several polyatomic molecular systems of interest a photon with 8 eV of energy gives us the unique ability to ionize from essentially anywhere along the excited state potential, but does not produce any ionization yield from the ground state. This enables us to measure excited state lifetimes without the photon energy becoming too low to ionize while the nuclear wave-packet is traveling on the excited state potential. We also have the advantage of working in the perturbative weak-field ionization regime. These experiments can also be directly compare to strong-field ionization experiments conducted with a UV-pump and an IR-probe conducted on the same molecules.

  5. Quasiparticle dynamics across the full Brillouin zone of Bi2Sr2CaCu2O8+δ traced with ultrafast time and angle-resolved photoemission spectroscopy

    Directory of Open Access Journals (Sweden)

    Georgi L. Dakovski

    2015-09-01

    Full Text Available A hallmark in the cuprate family of high-temperature superconductors is the nodal-antinodal dichotomy. In this regard, angle-resolved photoemission spectroscopy (ARPES has proven especially powerful, providing band structure information directly in energy-momentum space. Time-resolved ARPES (trARPES holds great promise of adding ultrafast temporal information, in an attempt to identify different interaction channels in the time domain. Previous studies of the cuprates using trARPES were handicapped by the low probing energy, which significantly limits the accessible momentum space. Using 20.15 eV, 12 fs pulses, we show for the first time the evolution of quasiparticles in the antinodal region of Bi2Sr2CaCu2O8+δ and demonstrate that non-monotonic relaxation dynamics dominates above a certain fluence threshold. The dynamics is heavily influenced by transient modification of the electron-phonon interaction and phase space restrictions, in stark contrast to the monotonic relaxation in the nodal and off-nodal regions.

  6. Ultrafast photophysics of transition metal complexes.

    Science.gov (United States)

    Chergui, Majed

    2015-03-17

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-08-15

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

  8. Ultrafast Graphene Photonics and Optoelectronics

    Science.gov (United States)

    2017-04-14

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

  9. Investigation of Confinement Induced Resonance in Atomic Waveguides with Different Geometries by Quantum Monte Carlo Methods

    CERN Document Server

    Azizi, Sajad

    2016-01-01

    We have investigated the quantum dynamics of two ultracold bosons inside an atomic waveguide for two different confinement geometries (cigar-shaped and toroidal waveguides) by quantum Monte Carlo methods. For quasi-1D gases, the confining potential of the waveguide leads to the so-called confinement induced resonance (CIR), results in the phase transition of the gas to the impenetrable bosonic regime (known as TG gas). In this regime the bosons repel each other strongly and behave like fermions. We reproduce CIR for a cigar-shaped waveguide and analyze the behavior of the system for different conditions. Moreover, our analysis demonstrates appearance of CIR for a toroidal waveguide. Particularly, we show that the resonance position is dependent on the size of the waveguide, which is in contrast to the cigar shaped waveguides for which it is universal.

  10. Partially coherent ultrafast spectrography.

    Science.gov (United States)

    Bourassin-Bouchet, C; Couprie, M-E

    2015-03-06

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

  11. Gap Surface Plasmon Waveguide Analysis

    DEFF Research Database (Denmark)

    Nielsen, Michael Grøndahl; Bozhevolnyi, Sergey I.

    2014-01-01

    Plasmonic waveguides supporting gap surface plasmons (GSPs) localized in a dielectric spacer between metal films are investigated numerically and the waveguiding properties at telecommunication wavelengths are presented. Especially, we emphasize that the mode confinement can advantageously...

  12. Effects of electronic coherence in ultrafast spectroscopy

    Science.gov (United States)

    Bennett, Kochise

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

  13. Experimental Demonstration of Luneburg Waveguides

    Directory of Open Access Journals (Sweden)

    Vera N. Smolyaninova

    2015-04-01

    Full Text Available Transformation optics gives rise to numerous unusual optical devices, such as novel metamaterial lenses and invisibility cloaks. Very recently, Mattheakis et al. (Luneburg lens waveguide networks. J. Opt. 2012, 14, 114006 have suggested theoretical design of an optical waveguide, based on a network of Luneburg lenses, which may be useful in sensing and nonlinear optics applications. Here, we report the first experimental realization of such Luneburg waveguides. We have studied wavelength and polarization dependent performance of the waveguides.

  14. Nanoporous polymer liquid core waveguides

    DEFF Research Database (Denmark)

    Gopalakrishnan, Nimi; Christiansen, Mads Brøkner; Ndoni, Sokol

    2010-01-01

    We demonstrate liquid core waveguides defined by UV to enable selective water infiltration in nanoporous polymers, creating an effective refractive index shift Δn=0.13. The mode confinement and propagation loss in these waveguides are presented.......We demonstrate liquid core waveguides defined by UV to enable selective water infiltration in nanoporous polymers, creating an effective refractive index shift Δn=0.13. The mode confinement and propagation loss in these waveguides are presented....

  15. Ultrafast photoinduced dynamics of the organolead trihalide perovskite CH3NH3PbI3 on mesoporous TiO2 scaffolds in the 320-920 nm range.

    Science.gov (United States)

    Flender, Oliver; Klein, Johannes R; Lenzer, Thomas; Oum, Kawon

    2015-07-15

    We present femtosecond broadband transient absorption experiments for the investigation of the carrier dynamics in the organolead trihalide perovskite CH3NH3PbI3. The perovskite was prepared on a mesoporous TiO2 scaffold either by 1-step deposition from solution or by 2-step methods employing deposition of lead iodide followed by an on-surface reaction with methylammonium iodide. The thin films were characterized by XRD and FTIR chemical mapping. After pumping with an ultrashort laser pulse at 400 or 500 nm, the dynamics were monitored by a broadband supercontinuum reaching from the near IR (920 nm) into the UV. Specifically, the usage of quartz substrates and thin perovskite/TiO2 films enabled us to cover the spectral development down to 320 nm. The charge carrier dynamics were largely independent from the specific route of perovskite preparation: initial ultrafast carrier relaxation steps with time constants τCC and τCOP of 1000 ps) and Auger recombination (τAR = 9, 75 and 450 ps). Carrier relaxation was accompanied by formation of an absorption band around 550 nm, with a characteristic structure assignable to a transient Stark effect, i.e. a red-shift of the perovskite spectrum due to the appearance of a directed electric field in the material and possibly additional influence of lattice heating. We observed a substantial Stokes shift between the relaxed photobleach and photoluminescence bands. Contributions of unreacted PbI2 to the transient absorption features appear to be negligible.

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

    Science.gov (United States)

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

    2013-06-20

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

  17. DESIGN OF INTEGRATING WAVEGUIDE BIOSENSOR

    Science.gov (United States)

    The Integrating Waveguide Biosensor allows for rapid and sensitive detection of pathogenic agents, cells and proteins via immunoassay or PCR products. The analytes are captured on the surface of the waveguide and then tagged with fluorescent labels. The waveguides are illuminated by excitation light...

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

    Science.gov (United States)

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

    2015-07-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-07-01

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

  20. Active Photonic Crystal Waveguides

    DEFF Research Database (Denmark)

    Ek, Sara

    This thesis deals with the fabrication and characterization of active photonic crystal waveguides, realized in III-V semiconductor material with embedded active layers. The platform offering active photonic crystal waveguides has many potential applications. One of these is a compact photonic...... crystal semiconductor optical amplier. As a step towards such a component, photonic crystal waveguides with a single quantum well, 10 quantum wells and three layers of quantum dots are fabricated and characterized. An experimental study of the amplied spontaneous emission and a implied transmission...... are presented in this thesis. A variation of photonic crystal design parameters are used leading to a spectral shift of the dispersion, it is veried that the observed effects shift accordingly. An enhancement of the amplified spontaneous emission was observed close to the band edge, where light is slowed down...