WorldWideScience

Sample records for ultrafast plasmon dynamics

  1. Photovoltaic Properties and Ultrafast Plasmon Relaxation Dynamics of Diamond-Like Carbon Nanocomposite Films with Embedded Ag Nanoparticles.

    Science.gov (United States)

    Meškinis, Šarūnas; Peckus, Domantas; Vasiliauskas, Andrius; Čiegis, Arvydas; Gudaitis, Rimantas; Tamulevičius, Tomas; Yaremchuk, Iryna; Tamulevičius, Sigitas

    2017-12-01

    Ultrafast relaxation dynamics of diamond-like carbon (DLC) films with embedded Ag nanoparticles (DLC:Ag) and photovoltaic properties of heterojunctions consisting of DLC:Ag and crystalline silicon (DLC:Ag/Si) were investigated by means of transient absorption (TAS) spectroscopy and photovoltaic measurements. The heterojunctions using both p type and n type silicon were studied. It was found that TAS spectra of DLC:Ag films were dependent on the used excitation wavelength. At wavelengths where Ag nanoparticles absorbed light most intensively, only DLC signal was registered. This result is in good accordance with an increase of the DLC:Ag/Si heterojunction short circuit current and open circuit voltage with the excitation wavelength in the photovoltaic measurements. The dependence of the TAS spectra of DLC:Ag films and photovoltaic properties of DLC:Ag/Si heterostructures on the excitation wavelength was explained as a result of trapping of the photoexcited hot charge carriers in DLC matrix. The negative photovoltaic effect was observed for DLC:Ag/p-Si heterostructures and positive ("conventional") for DLC:Ag/n-Si ones. It was explained by the excitation of hot plasmonic holes in the Ag nanoparticles embedded into DLC matrix. Some decrease of DLC:Ag/Si heterostructures photovoltage as well as photocurrent with DLC:Ag film thickness was observed, indicating role of the interface in the charge transfer process of photocarriers excited in Ag nanoparticles.

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

    Science.gov (United States)

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

    2017-03-01

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

  3. Ultrafast magnetization dynamics

    OpenAIRE

    Woodford, Simon

    2008-01-01

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

  4. Ultra-fast transient plasmonics using transparent conductive oxides

    Science.gov (United States)

    Ferrera, Marcello; Carnemolla, Enrico G.

    2018-02-01

    During the last decade, plasmonic- and metamaterial-based applications have revolutionized the field of integrated photonics by allowing for deep subwavelength confinement and full control over the effective permittivity and permeability of the optical environment. However, despite the numerous remarkable proofs of principle that have been experimentally demonstrated, few key issues remain preventing a widespread of nanophotonic technologies. Among these fundamental limitations, we remind the large ohmic losses, incompatibility with semiconductor industry standards, and largely reduced dynamic tunability of the optical properties. In this article, in the larger context of the new emerging field of all-dielectric nanophotonics, we present our recent progresses towards the study of large optical nonlinearities in transparent conducting oxides (TCOs) also giving a general overview of the most relevant and recent experimental attainments using TCO-based technology. However, it is important to underline that the present article does not represent a review paper but rather an original work with a broad introduction. Our work lays in a sort of ‘hybrid’ zone in the middle between high index contrast systems, whose behaviour is well described by applying Mie scattering theory, and standard plasmonic elements where optical modes originate from the electromagnetic coupling with the electronic plasma at the metal-to-dielectric interface. Beside remaining in the context of plasmonic technologies and retaining all the fundamental peculiarities that promoted the success of plasmonics in the first place, our strategy has the additional advantage to allow for large and ultra-fast tunability of the effective complex refractive index by accessing the index-near-zero regime in bulk materials at telecom wavelength.

  5. Ultrafast optical control of terahertz surface plasmons in subwavelength hole-arrays at room temperature

    Energy Technology Data Exchange (ETDEWEB)

    Azad, Abul Kalam [Los Alamos National Laboratory; Chen, Hou - Tong [Los Alamos National Laboratory; Taylor, Antoinette [Los Alamos National Laboratory; O' Hara, John [Los Alamos National Laboratory

    2010-12-10

    Extraordinary optical transmission through subwavelength metallic hole-arrays has been an active research area since its first demonstration. The frequency selective resonance properties of subwavelength metallic hole arrays, generally known as surface plasmon polaritons, have potential use in functional plasmonic devices such as filters, modulators, switches, etc. Such plasmonic devices are also very promising for future terahertz applications. Ultrafast switching or modulation of the resonant behavior of the 2-D metallic arrays in terahertz frequencies is of particular interest for high speed communication and sensing applications. In this paper, we demonstrate optical control of surface plasmon enhanced resonant terahertz transmission in two-dimensional subwavelength metallic hole arrays fabricated on gallium arsenide based substrates. Optically pumping the arrays creates a conductive layer in the substrate reducing the terahertz transmission amplitude of both the resonant mode and the direct transmission. Under low optical fluence, the terahertz transmission is more greatly affected by resonance damping than by propagation loss in the substrate. An ErAs:GaAs nanoisland superlattice substrate is shown to allow ultrafast control with a switching recovery time of {approx}10 ps. We also present resonant terahertz transmission in a hybrid plasmonic film comprised of an integrated array of subwavelength metallic islands and semiconductor holes. A large dynamic transition between a dipolar localized surface plasmon mode and a surface plasmon resonance near 0.8 THz is observed under near infrared optical excitation. The reversal in transmission amplitude from a stopband to a passband and up to {pi}/2 phase shift achieved in the hybrid plasmonic film make it promising in large dynamic phase modulation, optical changeover switching, and active terahertz plasmonics.

  6. Silicon as a virtual plasmonic material: Acquisition of its transient optical constants and the ultrafast surface plasmon-polariton excitation

    Energy Technology Data Exchange (ETDEWEB)

    Danilov, P. A.; Ionin, A. A.; Kudryashov, S. I., E-mail: sikudr@sci.lebedev.ru; Makarov, S. V.; Rudenko, A. A. [Lebedev Physical Institute (Russian Federation); Saltuganov, P. N. [Moscow Institute of Physics and Technology (State University) (Russian Federation); Seleznev, L. V.; Yurovskikh, V. I.; Zayarny, D. A. [Lebedev Physical Institute (Russian Federation); Apostolova, T. [Bulgarian Academy of Sciences, Institute for Nuclear Research and Nuclear Energetics (Bulgaria)

    2015-06-15

    Ultrafast intense photoexcitation of a silicon surface is complementarily studied experimentally and theoretically, with its prompt optical dielectric function obtained by means of time-resolved optical reflection microscopy and the underlying electron-hole plasma dynamics modeled numerically, using a quantum kinetic approach. The corresponding transient surface plasmon-polariton (SPP) dispersion curves of the photo-excited material were simulated as a function of the electron-hole plasma density, using the derived optical dielectric function model, and directly mapped at several laser photon energies, measuring spatial periods of the corresponding SPP-mediated surface relief nanogratings. The unusual spectral dynamics of the surface plasmon resonance, initially increasing with the increase in the electron-hole plasma density but damped at high interband absorption losses induced by the high-density electron-hole plasma through instantaneous bandgap renormalization, was envisioned through the multi-color mapping.

  7. Hotspot-mediated non-dissipative and ultrafast plasmon passage

    Science.gov (United States)

    Roller, Eva-Maria; Besteiro, Lucas V.; Pupp, Claudia; Khorashad, Larousse Khosravi; Govorov, Alexander O.; Liedl, Tim

    2017-08-01

    Plasmonic nanoparticles hold great promise as photon handling elements and as channels for coherent transfer of energy and information in future all-optical computing devices. Coherent energy oscillations between two spatially separated plasmonic entities via a virtual middle state exemplify electron-based population transfer, but their realization requires precise nanoscale positioning of heterogeneous particles. Here, we show the assembly and optical analysis of a triple-particle system consisting of two gold nanoparticles with an inter-spaced silver island. We observe strong plasmonic coupling between the spatially separated gold particles, mediated by the connecting silver particle, with almost no dissipation of energy. As the excitation energy of the silver island exceeds that of the gold particles, only quasi-occupation of the silver transfer channel is possible. We describe this effect both with exact classical electrodynamic modelling and qualitative quantum-mechanical calculations. We identify the formation of strong hotspots between all particles as the main mechanism for the lossless coupling and thus coherent ultrafast energy transfer between the remote partners. Our findings could prove useful for quantum gate operations, as well as for classical charge and information transfer processes.

  8. Ultrafast Non-thermal Response of Plasmonic Resonance in Gold Nanoantennas

    Science.gov (United States)

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

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

  9. Ultrafast dynamics of correlated electrons

    International Nuclear Information System (INIS)

    Rettig, Laurenz

    2012-01-01

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

  10. 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

  11. Ultrafast molecular dynamics illuminated with synchrotron radiation

    International Nuclear Information System (INIS)

    Bozek, John D.; Miron, Catalin

    2015-01-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-12-07

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

  13. Ultrafast Plasmonic Electron Emission from Ag Nanolayers with Different Roughness

    Czech Academy of Sciences Publication Activity Database

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

    2016-01-01

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

  14. Advanced Plasmonic Materials for Dynamic Color Display.

    Science.gov (United States)

    Shao, Lei; Zhuo, Xiaolu; Wang, Jianfang

    2018-04-01

    Plasmonic structures exhibit promising applications in high-resolution and durable color generation. Research on advanced hybrid plasmonic materials that allow dynamically reconfigurable color control has developed rapidly in recent years. Some of these results may give rise to practically applicable reflective displays in living colors with high performance and low power consumption. They will attract broad interest from display markets, compared with static plasmonic color printing, for example, in applications such as digital signage, full-color electronic paper, and electronic device screens. In this progress report, the most promising recent examples of utilizing advanced plasmonic materials for the realization of dynamic color display are highlighted and put into perspective. The performances, advantages, and disadvantages of different technologies are discussed, with emphasis placed on both the potential and possible limitations of various hybrid materials for dynamic plasmonic color display. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. Dynamics of plasmonic field polarization induced by quantum coherence in quantum dot-metallic nanoshell structures.

    Science.gov (United States)

    Sadeghi, S M

    2014-09-01

    When a hybrid system consisting of a semiconductor quantum dot and a metallic nanoparticle interacts with a laser field, the plasmonic field of the metallic nanoparticle can be normalized by the quantum coherence generated in the quantum dot. In this Letter, we study the states of polarization of such a coherent-plasmonic field and demonstrate how these states can reveal unique aspects of the collective molecular properties of the hybrid system formed via coherent exciton-plasmon coupling. We show that transition between the molecular states of this system can lead to ultrafast polarization dynamics, including sudden reversal of the sense of variations of the plasmonic field and formation of circular and elliptical polarization.

  16. 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.

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

    Science.gov (United States)

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

    2018-03-15

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

  18. 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.

  19. Charge carrier dynamics and surface plasmon interaction in gold nanorod-blended organic solar cell

    International Nuclear Information System (INIS)

    Rana, Aniket; Lochan, Abhiram; Chand, Suresh; Kumar, Mahesh; Singh, Rajiv K.; Gupta, Neeraj; Sharma, G. D.

    2016-01-01

    The inclusion of plasmonic nanoparticles into organic solar cell enhances the light harvesting properties that lead to higher power conversion efficiency without altering the device configuration. This work defines the consequences of the nanoparticle overloading amount and energy transfer process between gold nanorod and polymer (active matrix) in organic solar cells. We have studied the hole population decay dynamics coupled with gold nanorods loading amount which provides better understanding about device performance limiting factors. The exciton and plasmon together act as an interacting dipole; however, the energy exchange between these two has been elucidated via plasmon resonance energy transfer (PRET) mechanism. Further, the charge species have been identified specifically with respect to their energy levels appearing in ultrafast time domain. The specific interaction of these charge species with respective surface plasmon resonance mode, i.e., exciton to transverse mode of oscillation and polaron pair to longitudinal mode of oscillations, has been explained. Thus, our analysis reveals that PRET enhances the carrier population density in polymer via non-radiative process beyond the concurrence of a particular plasmon resonance oscillation mode and polymer absorption range. These findings give new insight and reveal specifically the factors that enhance and control the performance of gold nanorods blended organic solar cells. This work would lead in the emergence of future plasmon based efficient organic electronic devices.

  20. Charge carrier dynamics and surface plasmon interaction in gold nanorod-blended organic solar cell

    Science.gov (United States)

    Rana, Aniket; Gupta, Neeraj; Lochan, Abhiram; Sharma, G. D.; Chand, Suresh; Kumar, Mahesh; Singh, Rajiv K.

    2016-08-01

    The inclusion of plasmonic nanoparticles into organic solar cell enhances the light harvesting properties that lead to higher power conversion efficiency without altering the device configuration. This work defines the consequences of the nanoparticle overloading amount and energy transfer process between gold nanorod and polymer (active matrix) in organic solar cells. We have studied the hole population decay dynamics coupled with gold nanorods loading amount which provides better understanding about device performance limiting factors. The exciton and plasmon together act as an interacting dipole; however, the energy exchange between these two has been elucidated via plasmon resonance energy transfer (PRET) mechanism. Further, the charge species have been identified specifically with respect to their energy levels appearing in ultrafast time domain. The specific interaction of these charge species with respective surface plasmon resonance mode, i.e., exciton to transverse mode of oscillation and polaron pair to longitudinal mode of oscillations, has been explained. Thus, our analysis reveals that PRET enhances the carrier population density in polymer via non-radiative process beyond the concurrence of a particular plasmon resonance oscillation mode and polymer absorption range. These findings give new insight and reveal specifically the factors that enhance and control the performance of gold nanorods blended organic solar cells. This work would lead in the emergence of future plasmon based efficient organic electronic devices.

  1. 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

  2. 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...

  3. 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.

  4. Carrier dynamics in graphene. Ultrafast many-particle phenomena

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-11-15

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

  5. Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

    International Nuclear Information System (INIS)

    Liu, Yuzhu; Knopp, Gregor; Qin, Chaochao; Gerber, Thomas

    2015-01-01

    Graphical abstract: - Highlights: • Relaxation dynamics of furan are tracked by femtosecond photoelectron imaging. • The mechanism for ultrafast formation of α-carbene and β-carbene is proposed. • Ultrafast internal conversion from S 2 to S 1 is observed. • The transient characteristics of the fragment ions are obtained. • Single-color multi-photon ionization dynamics at 800 nm are also studied. - Abstract: Ultrafast internal conversion dynamics of furan has been studied by femtosecond photoelectron imaging (PEI) coupled with photofragmentation (PF) spectroscopy. Photoelectron imaging of single-color multi-photon ionization and two-color pump–probe ionization are obtained and analyzed. Photoelectron bands are assigned to the related states. The time evolution of the photoelectron signal by pump–probe ionization can be well described by a biexponential decay: two rapid relaxation pathways with time constants of ∼15 fs and 85 (±11) fs. The rapid relaxation is ascribed to the ultrafast internal conversion (IC) from the S 2 state to the vibrationally hot S 1 state. The second relaxation process is attributed to the redistributions and depopulation of secondarily populated high vibronic S 1 state and the formation of α-carbene and β-carbene by H immigration. Additionally, the transient characteristics of the fragment ions are also measured and discussed as a complementary understanding

  6. 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.

  7. Plasmonics theory and applications

    CERN Document Server

    Shahbazyan, Tigran V

    2014-01-01

    This contributed volume summarizes recent theoretical developments in plasmonics and its applications in physics, chemistry, materials science, engineering, and medicine. It focuses on recent advances in several major areas of plasmonics including plasmon-enhanced spectroscopies, light scattering, many-body effects, nonlinear optics, and ultrafast dynamics. The theoretical and computational methods used in these investigations include electromagnetic calculations, density functional theory calculations, and nonequilibrium electron dynamics calculations. The book presents a comprehensive overview of these methods as well as their applications to various current problems of interest.

  8. Dynamically tunable slow light based on plasmon induced transparency in disk resonators coupled MDM waveguide system

    International Nuclear Information System (INIS)

    Han, Xu; Wang, Tao; Liu, Bo; He, Yu; Tang, Jian; Li, Xiaoming

    2015-01-01

    Ultrafast and low-power dynamically tunable single channel and multichannel slow light based on plasmon induced transparencies (PITs) in disk resonators coupled to a metal-dielectric-metal (MDM) waveguide system with a nonlinear optical Kerr medium is investigated both numerically and analytically. A coupled-mode theory (CMT) is introduced to analyze this dynamically tunable single channel slow light structure. Multichannel slow light is realized in this plasmonic waveguide structure based on a bright–dark mode coupling mechanism. In order to reduce the pump intensity and obtain ultrafast response time, the traditional nonlinear Kerr material is replaced by monolayer graphene. It is found that the magnitude of the single PIT window can be controlled between 0.08 and 0.48, while the corresponding group index is controlled between 14.5 and 2.0 by dynamically decreasing pump intensity from 11.7 to 4.4 MW cm −2 . Moreover, the phase shift multiplication effect is found in this structure. This work paves a new way towards the realization of highly integrated optical circuits and networks, especially for wavelength-selective, all-optical storage and nonlinear devices. (paper)

  9. Dynamical class of a two-dimensional plasmonic Dirac system.

    Science.gov (United States)

    Silva, Érica de Mello

    2015-10-01

    A current goal in plasmonic science and technology is to figure out how to manage the relaxational dynamics of surface plasmons in graphene since its damping constitutes a hinder for the realization of graphene-based plasmonic devices. In this sense we believe it might be of interest to enlarge the knowledge on the dynamical class of two-dimensional plasmonic Dirac systems. According to the recurrence relations method, different systems are said to be dynamically equivalent if they have identical relaxation functions at all times, and such commonality may lead to deep connections between seemingly unrelated physical systems. We employ the recurrence relations approach to obtain relaxation and memory functions of density fluctuations and show that a two-dimensional plasmonic Dirac system at long wavelength and zero temperature belongs to the same dynamical class of standard two-dimensional electron gas and classical harmonic oscillator chain with an impurity mass.

  10. Ultrafast quantum control of ionization dynamics in krypton.

    Science.gov (United States)

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

    2018-02-19

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

  11. 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.

  12. 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...

  13. Ultrafast dissociation: An unexpected tool for probing molecular dynamics

    International Nuclear Information System (INIS)

    Morin, Paul; Miron, Catalin

    2012-01-01

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

  14. Ultrafast surface-enhanced Raman spectroscopy.

    Science.gov (United States)

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

    2015-08-07

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

  15. Ultra-fast all-optical plasmonic switching in near infra-red spectrum using a Kerr nonlinear ring resonator

    Science.gov (United States)

    Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

    2018-03-01

    In this paper, an all-optical plasmonic switch based on metal-insulator-metal (MIM) nanoplasmonic waveguide with a Kerr nonlinear ring resonator is introduced and studied. Two-dimensional simulations utilizing the finite-difference time-domain algorithm are used to demonstrate an apparent optical bistability and significant switching mechanisms (in enabled-low condition: T(ON/OFF) =21.9 and in enabled-high condition: T(ON/OFF) =24.9) of the signal light arisen by altering the pump-light intensity. The proposed all-optical switching demonstrates femtosecond-scale feedback time (90 fs) and then ultra-fast switching can be achieved. The offered all-optical switch may recognize potential significant applications in integrated optical circuits.

  16. Pump–probe microscopy: Visualization and spectroscopy of ultrafast dynamics at the nanoscale

    Energy Technology Data Exchange (ETDEWEB)

    Grumstrup, Erik M., E-mail: erik.grumstrup@montana.edu [Department of Chemistry and Biochemistry, Montana State University, Bozeman, MT 59718 (United States); Gabriel, Michelle M.; Cating, Emma E.M.; Van Goethem, Erika M. [Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 (United States); Papanikolas, John M., E-mail: john_papanikolas@unc.edu [Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599 (United States)

    2015-09-08

    Highlights: • Diffraction limited pump–probe microscopy methods are described. • Spatial variation in dynamical phenomena across single structures. • Direct observation of carrier motion in individual nanostructures. - Abstract: Excited state dynamics at the nanoscale provide important insight into the influence of structural features such as interfaces, defects, and surfaces on material properties. Pump–probe microscopy combines the spatial resolution of far-field optical microscopy with the temporal resolution of ultrafast spectroscopy, and has emerged as a powerful technique for characterizing spatial variation in dynamical phenomena across nanometer length scales. It has helped correlate dynamical phenomena with specific structural features in a variety of materials, shedding light on how excited state behaviors can dramatically differ from one member of the ensemble to the next, and even at different points within a single structure. It has also enabled direct imaging of transport phenomena such as free carrier diffusion, exciton migration and plasmon propagation in nanostructures. This ability to observe individual objects provides unique insight into complex materials where heterogeneous behavior makes it difficult, if not impossible, to reach clear and quantitative conclusions.

  17. Probing ultrafast carrier dynamics, nonlinear absorption

    Indian Academy of Sciences (India)

    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 ...

  18. 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.

  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. DNA-Nanotechnology-Enabled Chiral Plasmonics: From Static to Dynamic.

    Science.gov (United States)

    Zhou, Chao; Duan, Xiaoyang; Liu, Na

    2017-12-19

    The development of DNA nanotechnology, especially the advent of DNA origami, has made DNA ideally suited to construct nanostructures with unprecedented complexity and arbitrariness. As a fully addressable platform, DNA origami can be used to organize discrete entities in space through DNA hybridization with nanometer accuracy. Among a variety of functionalized particles, metal nanoparticles such as gold nanoparticles (AuNPs) feature an important pathway to endow DNA-origami-assembled nanostructures with tailored optical functionalities. When metal particles are placed in close proximity, their particle plasmons, i.e., collective oscillations of conduction electrons, can be coupled together, giving rise to a wealth of interesting optical phenomena. Nevertheless, characterization methods that can read out the optical responses from plasmonic nanostructures composed of small metal particles, and especially can optically distinguish in situ their minute conformation changes, are very few. Circular dichroism (CD) spectroscopy has proven to be a successful means to overcome these challenges because of its high sensitivity in discrimination of three-dimensional conformation changes. In this Account, we discuss a variety of static and dynamic chiral plasmonic nanostructures enabled by DNA nanotechnology. In the category of static plasmonic systems, we first show chiral plasmonic nanostructures based on spherical AuNPs, including plasmonic helices, toroids, and tetramers. To enhance the CD responses, anisotropic gold nanorods with larger extinction coefficients are utilized to create chiral plasmonic crosses and helical superstructures. Next, we highlight the inevitable evolution from static to dynamic plasmonic systems along with the fast development of this interdisciplinary field. Several dynamic plasmonic systems are reviewed according to their working mechanisms. We first elucidate a reconfigurable plasmonic cross structure that can execute DNA-regulated conformational

  1. Dynamics of Tidally Locked, Ultrafast Rotating Atmospheres

    Science.gov (United States)

    Tan, Xianyu; Showman, Adam P.

    2017-10-01

    Tidally locked gas giants, which exhibit a novel regime of day-night thermal forcing and extreme stellar irradiation, are typically in several-day orbits, implying slow rotation and a modest role for rotation in the atmospheric circulation. Nevertheless, there exist a class of gas-giant, highly irradiated objects - brown dwarfs orbiting white dwarfs in extremely tight orbits - whose orbital and hence rotation periods are as short as 1-2 hours. Spitzer phase curves and other observations have already been obtained for this fascinating class of objects, which raise fundamental questions about the role of rotation in controlling the circulation. So far, most modeling studies have investigated rotation periods exceeding a day, as appropriate for typical hot Jupiters. In this work we investigate the dynamics of tidally locked atmospheres in shorter rotation periods down to about two hours. With increasing rotation rate (decreasing rotation period), we show that the width of the equatorial eastward jet decreases, consistent with the narrowing of wave-mean-flow interacting region due to decrease of the equatorial deformation radius. The eastward-shifted equatorial hot spot offset decreases accordingly, and the westward-shifted hot regions poleward of the equatorial jet associated with Rossby gyres become increasingly distinctive. At high latitudes, winds becomes weaker and more geostrophic. The day-night temperature contrast becomes larger due to the stronger influence of rotation. Our simulated atmospheres exhibit small-scale variability, presumably caused by shear instability. Unlike typical hot Jupiters, phase curves of fast-rotating models show an alignment of peak flux to secondary eclipse. Our results have important implications for phase curve observations of brown dwarfs orbiting white dwarfs in ultra tight orbits.

  2. Ultrafast Dynamic Pressure Sensors Based on Graphene Hybrid Structure.

    Science.gov (United States)

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

    2017-07-19

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

  3. Measuring protein dynamics with ultrafast two-dimensional infrared spectroscopy

    International Nuclear Information System (INIS)

    Adamczyk, Katrin; Candelaresi, Marco; Hunt, Neil T; Robb, Kirsty; Hoskisson, Paul A; Tucker, Nicholas P; Gumiero, Andrea; Walsh, Martin A; Parker, Anthony W

    2012-01-01

    Recent advances in the methodology and application of ultrafast two-dimensional infrared (2D-IR) spectroscopy to biomolecular systems are reviewed. A description of the 2D-IR technique and the molecular contributions to the observed spectra are presented followed by a discussion of recent literature relating to the use of 2D-IR and associated approaches for measuring protein dynamics. In particular, these include the use of diatomic ligand groups for measuring haem protein dynamics, isotopic labelling strategies and the use of vibrational probe groups. The final section reports on the current state of the art regarding the use of 2D-IR methods to provide insights into biological reaction mechanisms. (topical review)

  4. Ultrafast dynamic ellipsometry and spectroscopy of laser shocked materials

    Energy Technology Data Exchange (ETDEWEB)

    Mcgrane, Shawn David [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Bolme, Cindy B [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Whitley, Von H [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Moore, David S [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2010-01-01

    Shock waves create extreme states of matter with very high pressures, temperatures, and volumetric compressions, at an exceedingly rapid rate of change. We review how to use a beamsplitter and a note card to turn a typical chirp pulse amplified femtosecond laser system into an ultrafast shock dynamics machine. Open scientific questions that can be addressed with such an apparatus are described. We report on the development of several single shot time resolved diagnostics needed to answer these questions. These single shot diagnostics are expected to be broadly applicable to other types of laser ablation experiments. Experimental results measured from shocked material dynamics of several systems are detailed. Finally, we report on progress towards using transient absorption as a measure of electronic excitation and coherent Raman as a picosecond probe of temperature in shock compressed condensed matter.

  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. Ultrafast excited-state dynamics in shape- and composition-controlled gold–silver bimetallic nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Zarick, Holly F. [Vanderbilt Univ., Nashville, TN (United States); Boulesbaa, Abdelaziz [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Talbert, Eric M. [Vanderbilt Univ., Nashville, TN (United States); Puretzky, Alexander A. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Geohegan, David B. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Bardhan, Rizia [Vanderbilt Univ., Nashville, TN (United States)

    2017-02-01

    In this paper, we have examined the ultrafast dynamics of shape- and composition-controlled bimetallic Au/Ag core/shell nanostructures with transient absorption spectroscopy (TAS) as a function of Ag layer thickness (0–15 nm) and pump excitation fluence (50–500 nJ/pulse). Our synthesis approach generated both bimetallic nanocubes and nanopyramids with distinct dipolar plasmon resonances and plasmon dephasing behavior at the resonance. Lifetimes obtained from TAS at low powers (50 nJ/pulse) demonstrated minimal dependence on the Ag layer thickness, whereas at high power (500 nJ/pulse) a rise in electron–phonon coupling lifetime (τ1) was observed with increasing Ag shell thickness for both nanocubes and nanopyramids. This is attributable to the stronger absorption of the 400 nm pump pulse with higher Ag content, which induced higher electron temperatures. The phonon–phonon scattering lifetime (τ2) also rises with increasing Ag layer, contributed both by the increasing size of the Au/Ag nanostructures as well as by surface chemistry effects. Further, we observed that even the thinnest, 2 nm, Ag shell strongly impacts both τ1 and τ2 at high power despite minimal change in overall size, indicating that the nanostructure composition also strongly impacts the thermalization temperature following absorption of 400 nm light. We also observed a shape-dependent trend at high power, where τ2 increased for the nanopyramids with increasing Ag shell thickness and nanostructure size, but bimetallic nanocubes demonstrated an unexpected decrease in τ2 for the thickest, 15 nm, Ag shell. This was attributed to the larger number of corners and edges in the nanocubes relative to the nanopyramids.

  7. Graphene: A Dynamic Platform for Electrical Control of Plasmonic Resonance

    DEFF Research Database (Denmark)

    Emani, Naresh Kumar; Kildishev, Alexander V.; Shalaev, Vladimir M.

    2015-01-01

    Graphene has recently emerged as a viable platform for integrated optoelectronic and hybrid photonic devices because of its unique properties. The optical properties of graphene can be dynamically controlled by electrical voltage and have been used to modulate the plasmons in noble metal nanostru...

  8. THz dynamics of nanoconfined water by ultrafast optical spectroscopy

    International Nuclear Information System (INIS)

    Taschin, A; Bartolini, P; Torre, R

    2017-01-01

    We investigated the vibrational dynamics and structural relaxation of water nanoconfined in porous silica samples with a pore size of 4 nm at different levels of hydration and temperature. We used the time-resolved optical Kerr effect (OKE), a spectroscopic technique that enables investigation of ultrafast water dynamics in a wide time (0.1–10 ps) or frequency (10 – 0.1 THz) window. At low hydration levels corresponding to two complete superficial water layers, no freezing occurs and the water remains mobile at all investigated temperatures. Meanwhile, at full hydration we witness a partial ice formation at about 248 K that coexists with the surface water remaining in the supercooled state. At low hydration, both structural and vibrational dynamics show significant modifications compared to bulk liquid water. This is due to the strong interaction of the water molecules with silica surfaces. Inner water, however, reveals relaxation dynamics very similar to bulk water. (paper)

  9. Magneto-Plasmonics and Resonant Interaction of Light with Dynamic Magnetisation in Metallic and All-Magneto-Dielectric Nanostructures.

    Science.gov (United States)

    Maksymov, Ivan S

    2015-04-09

    A significant interest in combining plasmonics and magnetism at the nanoscale gains momentum in both photonics and magnetism sectors that are concerned with the resonant enhancement of light-magnetic-matter interaction in nanostructures. These efforts result in a considerable amount of literature, which is difficult to collect and digest in limited time. Furthermore, there is insufficient exchange of results between the two research sectors. Consequently, the goal of this review paper is to bridge this gap by presenting an overview of recent progress in the field of magneto-plasmonics from two different points of view: magneto-plasmonics, and magnonics and magnetisation dynamics. It is expected that this presentation style will make this review paper of particular interest to both general physical audience and specialists conducting research on photonics, plasmonics, Brillouin light scattering spectroscopy of magnetic nanostructures and magneto-optical Kerr effect magnetometry, as well as ultrafast all-optical and THz-wave excitation of spin waves. Moreover, readers interested in a new, rapidly emerging field of all-dielectric nanophotonics will find a section about all-magneto-dielectric nanostructures.

  10. Magneto-Plasmonics and Resonant Interaction of Light with Dynamic Magnetisation in Metallic and All-Magneto-Dielectric Nanostructures

    Directory of Open Access Journals (Sweden)

    Ivan S. Maksymov

    2015-04-01

    Full Text Available A significant interest in combining plasmonics and magnetism at the nanoscale gains momentum in both photonics and magnetism sectors that are concerned with the resonant enhancement of light-magnetic-matter interaction in nanostructures. These efforts result in a considerable amount of literature, which is difficult to collect and digest in limited time. Furthermore, there is insufficient exchange of results between the two research sectors. Consequently, the goal of this review paper is to bridge this gap by presenting an overview of recent progress in the field of magneto-plasmonics from two different points of view: magneto-plasmonics, and magnonics and magnetisation dynamics. It is expected that this presentation style will make this review paper of particular interest to both general physical audience and specialists conducting research on photonics, plasmonics, Brillouin light scattering spectroscopy of magnetic nanostructures and magneto-optical Kerr effect magnetometry, as well as ultrafast all-optical and THz-wave excitation of spin waves. Moreover, readers interested in a new, rapidly emerging field of all-dielectric nanophotonics will find a section about all-magneto-dielectric nanostructures.

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

    Science.gov (United States)

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

    2018-05-08

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

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

    Directory of Open Access Journals (Sweden)

    Luuk J G W van Wilderen

    2011-03-01

    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

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

    Science.gov (United States)

    van Wilderen, Luuk J G W; Lincoln, Craig N; van Thor, Jasper J

    2011-03-21

    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 modelling is

  14. Topological mass of magnetic Skyrmions probed by ultrafast dynamic imaging

    International Nuclear Information System (INIS)

    Buettner, Felix

    2013-01-01

    In this thesis, we investigate the GHz dynamics of skyrmionic spin structures by means of pump-probe dynamic imaging to determine the equation of motion that governs the behavior of these technologically relevant spin structures. To achieve this goal, we first designed and optimized a perpendicular magnetic anisotropy CoB/Pt multilayer material for low magnetic pinning, as required for ultrafast pump-probe imaging experiments. Second, we developed an integrated sample design for X-ray holography capable of tracking relative magnetic positional changes down to 3 nm spatial resolution. These advances enabled us to image the trajectory of a single magnetic Skyrmion. We find that the motion is comprised of two gyrotropic modes, one clockwise and one counterclockwise. The existence of two modes shows that Skyrmions are massive quasiparticles. From their derived frequencies we find an inertial mass for the Skyrmion which is a factor of five larger than expected based on existing models for inertia in magnetism. Our results demonstrate that the mass of Skyrmions is based on a novel mechanism emerging from their confined nature, which is a direct consequence of their topology.

  15. Ultrafast excited-state dynamics of 2,5-dimethylpyrrole.

    Science.gov (United States)

    Yang, Dongyuan; Min, Yanjun; Chen, Zhichao; He, Zhigang; Yuan, Kaijun; Dai, Dongxu; Yang, Xueming; Wu, Guorong

    2018-04-17

    The ultrafast excited-state dynamics of 2,5-dimethylpyrrole following excitation at wavelengths in the range of 265.7-216.7 nm is studied using the time-resolved photoelectron imaging method. It is found that excitation at longer wavelengths (265.7-250.2 nm) results in the population of the S1(1πσ*) state, which decays out of the photoionization window in about 90 fs. At shorter pump wavelengths (242.1-216.7 nm), the assignments are less clear-cut. We tentatively assign the initially photoexcited state(s) to the 1π3p Rydberg state(s) which has lifetimes of 159 ± 20, 125 ± 15, 102 ± 10 and 88 ± 10 fs for the pump wavelengths of 242.1, 238.1, 232.6 and 216.7 nm, respectively. Internal conversion to the S1(1πσ*) state represents at most a minor decay channel. The methyl substitution effects on the decay dynamics of the excited states of pyrrole are also discussed. Methyl substitution on the pyrrole ring seems to enhance the direct internal conversion from the 1π3p Rydberg state to the ground state, while methyl substitution on the N atom has less influence and the internal conversion to the S1(πσ*) state represents a main channel.

  16. Plasmonics

    DEFF Research Database (Denmark)

    Berini, P.; Bozhevolnyi, Sergey I.; Kim, D. S.

    2016-01-01

    referred to as “extraordinary optical transmission.” Surface plasmons are intimately involved in the response of “metamaterials” and “metasurfaces” constructed from deep subwavelength metallic features, producing esoteric macroscopic properties such as a negative refractive index, or a permittivity...... or localized at metal nanostructures. Light suitable for exciting surface plasmons is typically within or near the visible but may extend into the infrared and ultraviolet regions. Metallic structures that support surface plasmons are highly varied, including planar arrangements of metal films, stripes...

  17. Ultrafast Structural Dynamics in InSb Probed by Time-Resolved X-Ray Diffraction

    International Nuclear Information System (INIS)

    Chin, A.H.; Shank, C.V.; Chin, A.H.; Schoenlein, R.W.; Shank, C.V.; Glover, T.E.; Leemans, W.P.; Balling, P.

    1999-01-01

    Ultrafast structural dynamics in laser-perturbed InSb are studied using time-resolved x-ray diffraction with a novel femtosecond x-ray source. We report the first observation of a delay in the onset of lattice expansion, which we attribute to energy relaxation processes and lattice strain propagation. In addition, we observe direct indications of ultrafast disordering on a subpicosecond time scale. copyright 1999 The American Physical Society

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

    Science.gov (United States)

    Suri, Pranav Kumar

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

  19. Ultrafast Hydrogen-Bonding Dynamics in Amyloid Fibrils.

    Science.gov (United States)

    Pazos, Ileana M; Ma, Jianqiang; Mukherjee, Debopreeti; Gai, Feng

    2018-06-08

    While there are many studies on the subject of hydrogen bonding dynamics in biological systems, few, if any, have investigated this fundamental process in amyloid fibrils. Herein, we seek to add insight into this topic by assessing the dynamics of a hydrogen bond buried in the dry interface of amyloid fibrils. To prepare a suitable model peptide system for this purpose, we introduce two mutations into the amyloid-forming Aβ(16-22) peptide. The first one is a lysine analog at position 19, which is used to help form structurally homogeneous fibrils, and the second one is an aspartic acid derivative (DM) at position 17, which is intended (1) to be used as a site-specific infrared probe and (2) to serve as a hydrogen-bond acceptor to lysine so that an inter-β-sheet hydrogen bond can be formed in the fibrils. Using both infrared spectroscopy and atomic force microscopy, we show that (1) this mutant peptide indeed forms well defined fibrils, (2) when bulk solvent is removed, there is no detectable water present in the fibrils, (3) infrared results obtained with the DM probe are consistent with a protofibril structure that is composed of two antiparallel β-sheets stacked in a parallel fashion, leading to formation of the expected hydrogen bond. Using two-dimensional infrared spectroscopy, we further show that the dynamics of this hydrogen bond occur on a timescale of ~2.3 ps, which is attributed to the rapid rotation of the -NH3+ group of lysine around its Cε-Nζ bond. Taken together, these results suggest that (1) DM is a useful infrared marker in facilitating structure determination of amyloid fibrils and (2) even in the tightly packed core of amyloid fibrils certain amino acid sidechains can undergo ultrafast motions, hence contributing to the thermodynamic stability of the system.

  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. Imagerie de plasmons de surface et d’électrons chauds par thermoréflectance pompe-sonde femtoseconde

    OpenAIRE

    Lozan , Olga

    2015-01-01

    In this work we explored the ultrafast dynamics of photo-excited hot electrons in plasmonic structures. The particular interest of this field resides on the fact surface plasmons (SP), because of their unrivaled temporal and spatial characteristics, provide a technological route for ultrafast information processes at the nanoscale. In this context, this manuscript provides a comprehension and the harnessing of one of the major limitation of the SP-based technologies : absorption losses by Jou...

  2. Ultrafast phosphate hydration dynamics in bulk H2O

    International Nuclear Information System (INIS)

    Costard, Rene; Tyborski, Tobias; Fingerhut, Benjamin P.; Elsaesser, Thomas

    2015-01-01

    Phosphate vibrations serve as local probes of hydrogen bonding and structural fluctuations of hydration shells around ions. Interactions of H 2 PO 4 − 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 S (PO 2 − )) and asymmetric (ν AS (PO 2 − )) PO 2 − stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the δ(P-(OH) 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 S (PO 2 − ) and ν AS (PO 2 − ) transition frequencies with larger frequency excursions for ν AS (PO 2 − ). The calculated frequency-time correlation function is in good agreement with the experiment. The ν(PO 2 − ) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H 2 PO 4 − /H 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

  3. Ultrafast phosphate hydration dynamics in bulk H2O

    Science.gov (United States)

    Costard, Rene; Tyborski, Tobias; Fingerhut, Benjamin P.; Elsaesser, Thomas

    2015-06-01

    Phosphate vibrations serve as local probes of hydrogen bonding and structural fluctuations of hydration shells around ions. Interactions of H2PO4- 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 S ( PO2 - ) ) and asymmetric ( ν A S ( PO2 - ) ) PO 2- stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the δ(P-(OH)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 S ( PO2 - ) and ν A S ( PO2 - ) transition frequencies with larger frequency excursions for ν A S ( PO2 - ) . The calculated frequency-time correlation function is in good agreement with the experiment. The ν ( PO2 - ) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H2PO4-/H2O 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.

  4. Ultrafast dynamics of hydrogen bond exchange in aqueous ionic solutions.

    Science.gov (United States)

    Park, Sungnam; Odelius, Michael; Gaffney, Kelly J

    2009-06-04

    The structural and dynamical properties of aqueous ionic solutions influence a wide range of natural and biological processes. In these solutions, water has the opportunity to form hydrogen bonds with other water molecules and anions. Knowing the time scale with which these configurations interconvert represents a key factor to understanding the influence of molecular scale heterogeneity on chemical events in aqueous ionic solutions. We have used ultrafast IR spectroscopy and Car-Parrinello molecular dynamics (CPMD) simulations to investigate the hydrogen bond (H-bond) structural dynamics in aqueous 6 M sodium perchlorate (NaClO4) solution. We have measured the H-bond exchange dynamics between spectrally distinct water-water and water-anion H-bond configurations with 2DIR spectroscopy and the orientational relaxation dynamics of water molecules in different H-bond configurations with polarization-selective IR pump-probe experiments. The experimental H-bond exchange time correlates strongly with the experimental orientational relaxation time of water molecules. This agrees with prior observations in water and aqueous halide solutions, and has been interpreted within the context of an orientational jump model for the H-bond exchange. The CPMD simulations performed on aqueous 6 M NaClO4 solution clearly demonstrate that water molecules organize into two radially and angularly distinct structural subshells within the first solvation shell of the perchlorate anion, with one subshell possessing the majority of the water molecules that donate H-bonds to perchlorate anions and the other subshell possessing predominantly water molecules that donate two H-bonds to other water molecules. Due to the high ionic concentration used in the simulations, essentially all water molecules reside in the first ionic solvation shells. The CPMD simulations also demonstrate that the molecular exchange between these two structurally distinct subshells proceeds more slowly than the H

  5. Ultrafast dynamics of electronically excited molecules and clusters

    International Nuclear Information System (INIS)

    Lietard, Aude

    2014-01-01

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

  6. Dynamic Control of Plasmon-Exciton Coupling in Au Nanodisk–J-Aggregate Hybrid Nanostructure Arrays

    KAUST Repository

    Zheng, Yue Bing; Juluri, Bala Krishna; Jensen, Linlin; Jensen, Lasse; Huang, Tony Jun

    2009-01-01

    We report the dynamic control of plasmon-exciton coupling in Au nanodisk arrays adsorbed with J-aggregate molecules by incident angle of light. The angle-resolved spectra of an array of bare Au nanodisks exhibit continuous shifting of localized surface plasmon resonances. This characteristic enables the production of real-time, controllable spectral overlaps between molecular and plasmonic resonances, and the efficient measurement of plasmon-exciton coupling as a function of wavelength with one or fewer nanodisk arrays. Experimental observations of varying plasmon-exciton coupling match with coupled dipole approximation calculations.

  7. Exploring Ultrafast Structural Dynamics for Energetic Enhancement or Disruption

    Science.gov (United States)

    2016-03-01

    it. In a pump -push/ dump probe experiment, a secondary laser pulse (push/ dump ) is used after the initial perturbation due to the pump pulse. The...increased. The pump -push/ dump probe technique is a difficult experiment that requires a highly stable laser source. Ultrafast pump -probe experiments...decomposition of solids. Journal of Applied Physics. 2001;89:4156–4166. 17. Kee TW. Femtosecond pump -push-probe and pump - dump -probe spectroscopy of

  8. Spectroscopic Investigation of the Ultrafast Photoinduced Dynamics in pi-Conjugated Terpyridines

    NARCIS (Netherlands)

    Siebert, R.; Akimov, D.; Schmitt, M.; Winter, A.; Schubert, U.S.; Dietzek, B.; Popp, J.

    2009-01-01

    Time-resolved spectroscopy is applied to investigate the ultrafast relaxation dynamics of several pi-conjugated mono-, bis-, tris- and tetrakis(terpyridine) derivs. This particular series of structurally closely related systems was prepd. applying efficient synthetic strategies and resembles key

  9. Ultrafast Dynamics in Light-Driven Molecular Rotary Motors Probed by Femtosecond Stimulated Raman Spectroscopy

    NARCIS (Netherlands)

    Hall, Christopher R.; Conyard, Jamie; Heisler, Ismael A.; Jones, Garth; Frost, James; Browne, Wesley R.; Feringa, Ben L.; Meech, Stephen R.

    2017-01-01

    Photochemical isomerization in sterically crowded chiral alkenes is the driving force for molecular rotary motors in nanoscale machines. Here the excited-state dynamics and structural evolution of the prototypical light-driven rotary motor are followed on the ultrafast time scale by femtosecond

  10. 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...

  11. Spatiotemporal Ultrafast-Plasmon Control Based on Response Functions of Nanostructures Measured by Interferometric Cross-Correlation Microscopy

    Directory of Open Access Journals (Sweden)

    Kusaba Miyuki

    2013-03-01

    Full Text Available We demonstrate an electrical-field cross-correlation imaging technique to obtain a response function of localized plasmon generated by femtosecond laser pulses on gold nanostructures. Based on the measured response functions, we spatiotemporally control the plasmon by shaping the femtosecond excitation laser pulses.

  12. 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.

  13. Surface Plasmon-Mediated Nanoscale Localization of Laser-Driven sub-Terahertz Spin Dynamics in Magnetic Dielectrics

    Science.gov (United States)

    Chekhov, Alexander L.; Stognij, Alexander I.; Satoh, Takuya; Murzina, Tatiana V.; Razdolski, Ilya; Stupakiewicz, Andrzej

    2018-05-01

    Ultrafast all-optical control of spins with femtosecond laser pulses is one of the hot topics at the crossroads of photonics and magnetism with a direct impact on future magnetic recording. Unveiling light-assisted recording mechanisms for an increase of the bit density beyond the diffraction limit without excessive heating of the recording medium is an open challenge. Here we show that surface plasmon-polaritons in hybrid metal-dielectric structures can provide spatial confinement of the inverse Faraday effect, mediating the excitation of localized coherent spin precession with 0.41 THz frequency. We demonstrate a two orders of magnitude enhancement of the excitation efficiency at the surface plasmon resonance within the 100 nm layer in dielectric garnet. Our findings broaden the horizons of ultrafast spin-plasmonics and open pathways towards non-thermal opto-magnetic recording at the nano-scale.

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

    International Nuclear Information System (INIS)

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

    2015-01-01

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

  15. Roadmap on plasmonics

    Science.gov (United States)

    Stockman, Mark I.; Kneipp, Katrin; Bozhevolnyi, Sergey I.; Saha, Soham; Dutta, Aveek; Ndukaife, Justus; Kinsey, Nathaniel; Reddy, Harsha; Guler, Urcan; Shalaev, Vladimir M.; Boltasseva, Alexandra; Gholipour, Behrad; Krishnamoorthy, Harish N. S.; MacDonald, Kevin F.; Soci, Cesare; Zheludev, Nikolay I.; Savinov, Vassili; Singh, Ranjan; Groß, Petra; Lienau, Christoph; Vadai, Michal; Solomon, Michelle L.; Barton, David R., III; Lawrence, Mark; Dionne, Jennifer A.; Boriskina, Svetlana V.; Esteban, Ruben; Aizpurua, Javier; Zhang, Xiang; Yang, Sui; Wang, Danqing; Wang, Weijia; Odom, Teri W.; Accanto, Nicolò; de Roque, Pablo M.; Hancu, Ion M.; Piatkowski, Lukasz; van Hulst, Niek F.; Kling, Matthias F.

    2018-04-01

    Plasmonics is a rapidly developing field at the boundary of physical optics and condensed matter physics. It studies phenomena induced by and associated with surface plasmons—elementary polar excitations bound to surfaces and interfaces of good nanostructured metals. This Roadmap is written collectively by prominent researchers in the field of plasmonics. It encompasses selected aspects of nanoplasmonics. Among them are fundamental aspects, such as quantum plasmonics based on the quantum-mechanical properties of both the underlying materials and the plasmons themselves (such as their quantum generator, spaser), plasmonics in novel materials, ultrafast (attosecond) nanoplasmonics, etc. Selected applications of nanoplasmonics are also reflected in this Roadmap, in particular, plasmonic waveguiding, practical applications of plasmonics enabled by novel materials, thermo-plasmonics, plasmonic-induced photochemistry and photo-catalysis. This Roadmap is a concise but authoritative overview of modern plasmonics. It will be of interest to a wide audience of both fundamental physicists and chemists, as well as applied scientists and engineers.

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

    Science.gov (United States)

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

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

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

    International Nuclear Information System (INIS)

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

    2013-01-01

    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

  18. 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.

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

    International Nuclear Information System (INIS)

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

    2007-01-01

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

  20. Ultrafast Ge-Te bond dynamics in a phase-change superlattice

    Science.gov (United States)

    Malvestuto, Marco; Caretta, Antonio; Casarin, Barbara; Cilento, Federico; Dell'Angela, Martina; Fausti, Daniele; Calarco, Raffaella; Kooi, Bart J.; Varesi, Enrico; Robertson, John; Parmigiani, Fulvio

    2016-09-01

    A long-standing question for avant-garde data storage technology concerns the nature of the ultrafast photoinduced phase transformations in the wide class of chalcogenide phase-change materials (PCMs). Overall, a comprehensive understanding of the microstructural evolution and the relevant kinetics mechanisms accompanying the out-of-equilibrium phases is still missing. Here, after overheating a phase-change chalcogenide superlattice by an ultrafast laser pulse, we indirectly track the lattice relaxation by time resolved x-ray absorption spectroscopy (tr-XAS) with a sub-ns time resolution. The approach to the tr-XAS experimental results reported in this work provides an atomistic insight of the mechanism that takes place during the cooling process; meanwhile a first-principles model mimicking the microscopic distortions accounts for a straightforward representation of the observed dynamics. Finally, we envisage that our approach can be applied in future studies addressing the role of dynamical structural strain in PCMs.

  1. Synthesis, Characterization, and Ultrafast Dynamics of Metal, Metal Oxide, and Semiconductor Nanomaterials

    OpenAIRE

    Wheeler, Damon Andreas

    2013-01-01

    SYNTHESIS, CHARACTERIZATION, AND ULTRAFAST DYNAMICS OF METAL, METAL OXIDE, AND SEMICONDUCTOR NANOMATERIALSABSTRACTThe optical properties of each of the three main classes of inorganic nanomaterials, metals, metal oxides, and semiconductors differ greatly due to the intrinsically different nature of the materials. These optical properties are among the most fascinating and useful aspects of nanomaterials with applications spanning cancer treatment, sensors, lasers, and solar cells. One techn...

  2. 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......$factor) is theoretically predicted and demonstrated in the experiments. The fundamental analysis reveals the underlying physical processes and indicates limitations to QD-based devices....

  3. 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.

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

    KAUST Repository

    Sun, Jingya

    2016-02-25

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

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

    KAUST Repository

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

    2016-01-01

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

  6. Protonation-induced ultrafast torsional dynamics in 9-anthrylbenzimidazole: a pH activated molecular rotor.

    Science.gov (United States)

    Nandi, Amitabha; Kushwaha, Archana; Das, Dipanwita; Ghosh, Rajib

    2018-03-07

    We report the photophysical properties and excited state dynamics of 9-anthrylbenzimidazole (ANBI) which exhibits protonation-induced molecular rotor properties. In contrast to the highly emissive behavior of neutral ANBI, protonation of the benzimidazole group of ANBI induces efficient nonradiative deactivation by ultrafast torsional motion around the bond connecting the anthracene and benzimidazole units, as revealed by ultrafast transient absorption and fluorescence spectroscopy. Contrary to viscosity-independent fluorescence of neutral dyes, protonated ANBI is shown to display linear variation of emission yield and lifetime with solvent viscosity. The protonation-induced molecular rotor properties in the studied system are shown to be driven by enhanced charge transfer and are corroborated by quantum chemical calculations. Potential application as a microviscosity sensor of acidic regions in a heterogeneous environment by these proton-activated molecular rotor properties of ANBI is discussed.

  7. Ultrafast dynamics of Coulomb correlated excitons in GaAs quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Mycek, M.A. [Univ. of California, Berkeley, CA (United States). Dept. of Physics]|[Lawrence Berkeley National Lab., CA (United States). Materials Sciences Div.

    1995-12-01

    The author measures the transient nonlinear optical response of room temperature excitons in gallium arsenide quantum wells via multi-wave mixing experiments. The dynamics of the resonantly excited excitons is directly reflected by the ultrafast decay of the induced nonlinear polarization, which radiates the detected multi-wave mixing signal. She characterizes this ultrafast coherent emission in both amplitude and phase, using time- and frequency-domain measurement techniques, to better understand the role of Coulomb correlation in these systems. To interpret the experimental results, the nonlinear optical response of a dense medium is calculated using a model including Coulomb interaction. She contributes three new elements to previous theoretical and experimental studies of these systems. First, surpassing traditional time-integrated measurements, she temporally resolves the amplitude of the ultrafast coherent emission. Second, in addition to measuring the third-order four-wave mixing signal, she also investigates the fifth-order six-wave mixing response. Third, she characterizes the ultrafast phase dynamics of the nonlinear emission using interferometric techniques with an unprecedented resolution of approximately 140 attoseconds. The author finds that effects arising from Coulomb correlation dominate the nonlinear optical response when the density of excitons falls below 3 {times} 10{sup 11} cm{sup {minus}2}, the saturation density. These signatures of Coulomb correlation are investigated for increasing excitation density to gradually screen the interactions and test the validity of the model for dense media. The results are found to be qualitatively consistent with both the predictions of the model and with numerical solutions to the semiconductor Bloch equations. Importantly, the results also indicate current experimental and theoretical limitations, which should be addressed in future research.

  8. Ultrafast single-molecule photonics: Excited state dynamics in coherently coupled complexes

    International Nuclear Information System (INIS)

    Hernando, Jordi; Hoogenboom, Jacob; Dijk, Erik van; Garcia-Parajo, Maria; Hulst, Niek F. van

    2008-01-01

    We present a single-molecule study on femtosecond dynamics in multichromophoric systems, combining fs pump-probe, emission-spectra and fluorescence-lifetime analysis. The ultrafast fs approach gives direct information on the initial exciton dynamics after excitation. The lifetime data show superradiance, a direct measure for the extent of the coherent coupling and static disorder. The spectra finally reveal the role of exciton-phonon coupling. At the single-molecule level a wide range of exciton delocalization lengths and energy redistribution times is revealed

  9. Ultrafast single-molecule photonics: Excited state dynamics in coherently coupled complexes

    Energy Technology Data Exchange (ETDEWEB)

    Hernando, Jordi [Dept. de Quimica, Universitat Autonoma Barcelona, 08193 Cerdanyola del Valles (Spain); Hoogenboom, Jacob [ICFO-Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels, Barcelona (Spain); Dijk, Erik van [Applied Optics Group, MESA Institute for Nanotechnology, University of Twente, 7500AE Enschede (Netherlands); Garcia-Parajo, Maria [IBEC-Institute of BioEngineering of Catalunya, 08028 Barcelona (Spain); ICREA-Institucio Catalana de Recerca i Estudis Avancats, 08015 Barcelona (Spain); Hulst, Niek F. van [ICFO-Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels, Barcelona (Spain) and ICREA-Institucio Catalana de Recerca i Estudis Avancats, 08015 Barcelona (Spain)], E-mail: Niek.vanHulst@ICFO.es

    2008-05-15

    We present a single-molecule study on femtosecond dynamics in multichromophoric systems, combining fs pump-probe, emission-spectra and fluorescence-lifetime analysis. The ultrafast fs approach gives direct information on the initial exciton dynamics after excitation. The lifetime data show superradiance, a direct measure for the extent of the coherent coupling and static disorder. The spectra finally reveal the role of exciton-phonon coupling. At the single-molecule level a wide range of exciton delocalization lengths and energy redistribution times is revealed.

  10. 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. Copyright © 2016 Elsevier B.V. All rights reserved.

  11. 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.

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

    Science.gov (United States)

    Fushitani, Mizuho; Hishikawa, Akiyoshi

    2016-11-01

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

  13. A plasmonic fluid with dynamically tunable optical properties

    KAUST Repository

    Bhattacharjee, Rama Ranjan; Li, Ruipeng; Esté vez, Luis Antonio; Smilgies, Detlef Matthias; Amassian, Aram; Giannelis, Emmanuel P.

    2009-01-01

    We report the first synthesis of a gold nanorod (GNR)-based nanocomposite that exhibits solid-like plasmonic properties while behaving in a liquid-like manner. Tuning the degree of GNR clustering controls the material's responsiveness to external stimuli, such as mechanical shearing, due to the sensitivity of the localized surface plasmon resonance to interparticle interactions. © 2009 The Royal Society of Chemistry.

  14. Hot carrier dynamics in plasmonic transition metal nitrides

    Science.gov (United States)

    Habib, Adela; Florio, Fred; Sundararaman, Ravishankar

    2018-06-01

    Extraction of non-equilibrium hot carriers generated by plasmon decay in metallic nano-structures is an increasingly exciting prospect for utilizing plasmonic losses, but the search for optimum plasmonic materials with long-lived carriers is ongoing. Transition metal nitrides are an exciting class of new plasmonic materials with superior thermal and mechanical properties compared to conventional noble metals, but their suitability for plasmonic hot carrier applications remains unknown. Here, we present fully first principles calculations of the plasmonic response, hot carrier generation and subsequent thermalization of all group IV, V and VI transition metal nitrides, fully accounting for direct and phonon-assisted transitions as well as electron–electron and electron–phonon scattering. We find the largest frequency ranges for plasmonic response in ZrN, HfN and WN, between those of gold and silver, while we predict strongest absorption in the visible spectrum for the VN, NbN and TaN. Hot carrier generation is dominated by direct transitions for most of the relevant energy range in all these nitrides, while phonon-assisted processes dominate only below 1 eV plasmon energies primarily for the group IV nitrides. Finally, we predict the maximum hot carrier lifetimes to be around 10 fs for group IV and VI nitrides, a factor of 3–4 smaller than noble metals, due to strong electron–phonon scattering. However, we find longer carrier lifetimes for group V nitrides, comparable to silver for NbN and TaN, while exceeding 100 fs (twice that of silver) for VN, making them promising candidates for efficient hot carrier extraction.

  15. A plasmonic fluid with dynamically tunable optical properties

    KAUST Repository

    Bhattacharjee, Rama Ranjan

    2009-01-01

    We report the first synthesis of a gold nanorod (GNR)-based nanocomposite that exhibits solid-like plasmonic properties while behaving in a liquid-like manner. Tuning the degree of GNR clustering controls the material\\'s responsiveness to external stimuli, such as mechanical shearing, due to the sensitivity of the localized surface plasmon resonance to interparticle interactions. © 2009 The Royal Society of Chemistry.

  16. 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

  17. Ultrafast Dynamics in Vanadium Dioxide: Separating Spatially Segregated Mixed Phase Dynamics in the Time-domain

    Science.gov (United States)

    Hilton, David

    2011-10-01

    In correlated electronic systems, observed electronic and structural behavior results from the complex interplay between multiple, sometimes competing degrees-of- freedom. One such material used to study insulator-to-metal transitions is vanadium dioxide, which undergoes a phase transition from a monoclinic-insulating phase to a rutile-metallic phase when the sample is heated to 340 K. The major open question with this material is the relative influence of this structural phase transition (Peirels transition) and the effects of electronic correlations (Mott transition) on the observed insulator-to-metal transition. Answers to these major questions are complicated by vanadium dioxide's sensitivity to perturbations in the chemical structure in VO2. For example, related VxOy oxides with nearly a 2:1 ratio do not demonstrate the insulator-to- metal transition, while recent work has demonstrated that W:VO2 has demonstrated a tunable transition temperature controllable with tungsten doping. All of these preexisting results suggest that the observed electronic properties are exquisitely sensitive to the sample disorder. Using ultrafast spectroscopic techniques, it is now possible to impulsively excite this transition and investigate the photoinduced counterpart to this thermal phase transition in a strongly nonequilibrium regime. I will discuss our recent results studying the terahertz-frequency conductivity dynamics of this photoinduced phase transition in the poorly understood near threshold temperature range. We find a dramatic softening of the transition near the critical temperature, which results primarily from the mixed phase coexistence near the transition temperature. To directly study this mixed phase behavior, we directly study the nucleation and growth rates of the metallic phase in the parent insulator using non-degenerate optical pump-probe spectroscopy. These experiments measure, in the time- domain, the coexistent phase separation in VO2 (spatially

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

    Science.gov (United States)

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

    2018-05-10

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

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

    Science.gov (United States)

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

    2011-12-07

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

  20. Plasmon Geometric Phase and Plasmon Hall Shift

    Science.gov (United States)

    Shi, Li-kun; Song, Justin C. W.

    2018-04-01

    The collective plasmonic modes of a metal comprise a simple pattern of oscillating charge density that yields enhanced light-matter interaction. Here we unveil that beneath this familiar facade plasmons possess a hidden internal structure that fundamentally alters its dynamics. In particular, we find that metals with nonzero Hall conductivity host plasmons with an intricate current density configuration that sharply departs from that of ordinary zero Hall conductivity metals. This nontrivial internal structure dramatically enriches the dynamics of plasmon propagation, enabling plasmon wave packets to acquire geometric phases as they scatter. At boundaries, these phases accumulate allowing plasmon waves that reflect off to experience a nonreciprocal parallel shift. This plasmon Hall shift, tunable by Hall conductivity as well as plasmon wavelength, displaces the incident and reflected plasmon trajectories and can be readily probed by near-field photonics techniques. Anomalous plasmon geometric phases dramatically enrich the nanophotonics toolbox, and yield radical new means for directing plasmonic beams.

  1. 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

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

    Science.gov (United States)

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

    2018-05-03

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

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

    International Nuclear Information System (INIS)

    Schick, Daniel

    2013-01-01

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

  4. 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...... 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...

  5. 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.

  6. Ultrafast x-ray scattering on nanoparticle dynamics

    International Nuclear Information System (INIS)

    Plech, A; Ibrahimkutty, S; Issenmann, D; Kotaidis, V; Siems, A

    2013-01-01

    Pulsed X-ray scattering is used for the determination of structural dynamics of laser-irradiated gold particles. By combining several scattering methods such as powder scattering, small angle scattering and diffuse wide angle scattering it is possible to reconstruct the kinetics of structure evolution on several lengths scales and derive complementary information on the particles and their local environment. A generic structural phase diagram for the reaction as function of delay time after laser excitation and laser fluence can be constructed.

  7. Cavitation in confined water: ultra-fast bubble dynamics

    Science.gov (United States)

    Vincent, Olivier; Marmottant, Philippe

    2012-02-01

    In the hydraulic vessels of trees, water can be found at negative pressure. This metastable state, corresponding to mechanical tension, is achieved by evaporation through a porous medium. It can be relaxed by cavitation, i.e. the sudden nucleation of vapor bubbles. Harmful for the tree due to the subsequent emboli of sap vessels, cavitation is on the contrary used by ferns to eject spores very swiftly. We will focus here on the dynamics of the cavitation bubble, which is of primary importance to explain the previously cited natural phenomena. We use the recently developed method of artificial tress, using transparent hydrogels as the porous medium. Our experiments, on water confined in micrometric hydrogel cavities, show an extremely fast dynamics: bubbles are nucleated at the microsecond timescale. For cavities larger than 100 microns, the bubble ``rings'' with damped oscillations at MHz frequencies, whereas for smaller cavities the oscillations become overdamped. This rich dynamics can be accounted for by a model we developed, leading to a modified Rayleigh-Plesset equation. Interestingly, this model predicts the impossibility to nucleate bubbles above a critical confinement that depends on liquid negative pressure and corresponds to approximately 100 nm for 20 MPa tensions.

  8. Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode.

    Science.gov (United States)

    Bücker, K; Picher, M; Crégut, O; LaGrange, T; Reed, B W; Park, S T; Masiel, D J; Banhart, F

    2016-12-01

    High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. Copyright © 2016 Elsevier B.V. All rights reserved.

  9. Radio galaxies radiation transfer, dynamics, stability and evolution of a synchrotron plasmon

    CERN Document Server

    Pacholczyk, A G

    1977-01-01

    Radio Galaxies: Radiation Transfer, Dynamics, Stability and Evolution of a Synchrotron Plasmon deals with the physics of a region in space containing magnetic field and thermal and relativistic particles (a plasmon). The synchrotron emission and absorption of this region are discussed, along with the properties of its spectrum; its linear and circular polarization; transfer of radiation through such a region; its dynamics and expansion; and interaction with external medium.Comprised of eight chapters, this volume explores the stability, turbulence, and acceleration of particles in a synchrotro

  10. 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.

  11. Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode

    Energy Technology Data Exchange (ETDEWEB)

    Bücker, K.; Picher, M.; Crégut, O. [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France); LaGrange, T. [Interdisciplinary Centre for Electron Microscopy, École Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland); Reed, B.W.; Park, S.T.; Masiel, D.J. [Integrated Dynamic Electron Solutions, Inc., 5653 Stoneridge Drive 117, Pleasanton, CA 94588 (United States); Banhart, F., E-mail: florian.banhart@ipcms.unistra.fr [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France)

    2016-12-15

    High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. - Highlights: • A detailed characterization of electron

  12. Ultrafast studies of dynamic & complex systems: Understanding molecular and ionization dynamics

    OpenAIRE

    Hockett, Paul

    2016-01-01

    Presentation given at the ITAMP workshop "Ultrafast atomic and molecular physics with cutting-edge light sources: New opportunities and challenges", held at Kansas State University, Nov. 2013.  A video of the presentation can be found on the ITAMP Youtube channel, https://www.youtube.com/watch?v=x8RWWDWZJpk

  13. 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 (MAPbBr 3 ) 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 MAPbBr 3 perovskites. TAS also showed a decrease in carrier decay lifetimes, indicating that nanostructures enhance photoinduced carrier generation and promote efficient electron injection into TiO 2 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.

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

    International Nuclear Information System (INIS)

    Komolibus, K.; Piwonski, T.; Gradkowski, K.; Reyner, C. J.; Liang, B.; Huffaker, D. L.; Huyet, G.; Houlihan, J.

    2015-01-01

    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

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

    Energy Technology Data Exchange (ETDEWEB)

    Lad, Amit D; Mondal, S; Narayanan, V; Ahmed, Saima; Kumar, G Ravindra; Rajeev, P P; Robinson, A P L [Central Laser Facility, Rutherford-Appleton Laboratory, Chilton, Oxfordshire (United Kingdom); Pasley, J, E-mail: amitlad@tifr.res.i [Department of Physics, University of York, Heslington, York (United Kingdom)

    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 (10{sup 18} W/cm{sup 2}, 30 fs, 800 nm) on an aluminium target. We observe the Doppler shift of a time delayed probe laser beam (10{sup 12} W/cm{sup 2}, 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).

  16. 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...

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

    Science.gov (United States)

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

    2017-09-01

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

  18. Ultrafast surface carrier dynamics in the topological insulator Bi₂Te₃.

    Science.gov (United States)

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

    2012-07-11

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

  19. Ultrafast carrier dynamics in bilayer graphene studied by broadband infrared pump-probe spectroscopy

    Science.gov (United States)

    Limmer, Thomas; da Como, Enrico; Niggebaum, Alexander; Feldmann, Jochen

    2010-03-01

    Recently, bilayer graphene gained a large interest because of its electrically tunable gap appearing in the middle infrared part of the electromagnetic spectrum. This feature is expected to open a number of applications of bilayer graphene in optoelectronics. In this communication we report on the first pump-probe experiment on a single bilayer flake with an unprecedented probe photon energy interval (0.25 -- 1.3 eV). Single flakes were prepared by mechanical exfoliation of graphite and transferred to calcium fluoride substrates. When illuminated with 800 nm (1.5 eV) pump pulses the induced change in transmission shows an ultrafast saturation of the interband transitions from 1.3 to 0.5 eV. In this energy range the saturation recovery occurs within 3 ps and is consistent with an ultrafast relaxation of hot carriers. Interestingly, we report on the observation of a resonance at 0.4 eV characterized by a longer dynamics. The results are discussed considering many-body interactions.

  20. Dynamic Tuning of Plasmon-Exciton Coupling in Arrays of Nanodisk-J-aggregate Complexes

    KAUST Repository

    Zheng, Yue Bing

    2010-07-21

    Figure Presented Dynamic tuning of plasmon-exclton resonant coupling in arrays of nanodisk-J-aggregate complexes is demonstrated. The angle-resolved spectra of an array of bare gold nanodisks exhibit continuous shifting of localized surface plasmon resonance. This characteristic enables the production of real-time, controllable spectral overlap between molecular resonance and plasmóme resonance. The resonant interaction strength as a function of spectral overlap is explored and the coupling strength changes with the incident angle of a probe light, in accord with simulations based on coupled dipóle approximation method. © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  1. 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

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

    Science.gov (United States)

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

    2018-04-01

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

  3. Ultrafast fragmentation dynamics of triply charged carbon dioxide: Vibrational-mode-dependent molecular bond breakage

    Science.gov (United States)

    Yang, HongJiang; Wang, Enliang; Dong, WenXiu; Gong, Maomao; Shen, Zhenjie; Tang, Yaguo; Shan, Xu; Chen, Xiangjun

    2018-05-01

    The a b i n i t i o molecular dynamics (MD) simulations using an atom-centered density matrix propagation method have been carried out to investigate the fragmentation of the ground-state triply charged carbon dioxide, CO23 +→C+ + Oa+ + Ob+ . Ten thousands of trajectories have been simulated. By analyzing the momentum correlation of the final fragments, it is demonstrated that the sequential fragmentation dominates in the three-body dissociation, consistent with our experimental observations which were performed by electron collision at impact energy of 1500 eV. Furthermore, the MD simulations allow us to have detailed insight into the ultrafast evolution of the molecular bond breakage at a very early stage, within several tens of femtoseconds, and the result shows that the initial nuclear vibrational mode plays a decisive role in switching the dissociation pathways.

  4. Ultrafast method of calculating the dynamic spectral line shapes for integrated modelling of plasmas

    International Nuclear Information System (INIS)

    Lisitsa, V.S.

    2009-01-01

    An ultrafast code for spectral line shape calculations is presented to be used in the integrated modelling of plasmas. The code is based on the close analogy between two mechanisms: (i) Dicke narrowing of the Doppler-broadened spectral lines and (ii) transition from static to impact regime in the Stark broadening. The analogy makes it possible to describe the dynamic Stark broadening in terms of an analytical functional of the static line shape. A comparison of new method with the widely used Frequency Fluctuating Method (FFM) developed by the Marseille University group (B. Talin, R. Stamm, et al.) shows good agreement, with the new method being faster than the standard FFM by nearly two orders of magnitude. The method proposed may significantly simplify the radiation transport modeling and opens new possibilities for integrated modeling of the edge and divertor plasma in tokamaks. (author)

  5. A microfluidic flow-cell for the study of the ultrafast dynamics of biological systems

    Energy Technology Data Exchange (ETDEWEB)

    Chauvet, Adrien, E-mail: adrien.chauvet@epfl.ch; Chergui, Majed [Ecole Polytechnique Fédérale de Lausanne (EPFL), Laboratoire de Spectroscopie Ultrarapide, ISIC, Faculté des Sciences de Base, Station 6, 1015 Lausanne (Switzerland); Tibiletti, Tania; Caffarri, Stefano [Aix Marseille Université, CNRS, CEA, UMR 7265 Biologie Végétale et Microbiologie Environnementales, 13009 Marseille (France)

    2014-10-01

    The study of biochemical dynamics by ultrafast spectroscopic methods is often restricted by the limited amount of liquid sample available, while the high repetition rate of light sources can induce photodamage. In order to overcome these limitations, we designed a high flux, sub-ml, capillary flow-cell. While the 0.1 mm thin window of the 0.5 mm cross-section capillary ensures an optimal temporal resolution and a steady beam deviation, the cell-pump generates flows up to ~0.35 ml/s that are suitable to pump laser repetition rates up to ~14 kHz, assuming a focal spot-diameter of 100 μm. In addition, a decantation chamber efficiently removes bubbles and allows, via septum, for the addition of chemicals while preserving the closed atmosphere. The minimal useable amount of sample is ~250 μl.

  6. Ultrafast non-adiabatic dynamics of methyl substituted ethylenes: The π3s Rydberg state

    Science.gov (United States)

    Wu, Guorong; Boguslavskiy, Andrey E.; Schalk, Oliver; Schuurman, Michael S.; Stolow, Albert

    2011-10-01

    Excited state unimolecular reactions of some polyenes exhibit localization of their dynamics at a single ethylenic double bond. Here we present studies of the fundamental photophysical processes in the ethylene unit itself. Combined femtosecond time-resolved photoelectron spectroscopy (TRPES) and ab initio quantum chemical calculations was applied to the study of excited state dynamics in cis-butene, trans-butene, trimethylethylene, and tetramethylethylene, following initial excitation to their respective π3s Rydberg states. The wavelength dependence of the π3s Rydberg state dynamics of tetramethylethylene was investigated in more detail. The π3s Rydberg to ππ* valence state decay rate varies greatly with substituent: the 1,2-di- and tri-methyl substituted ethylenes (cis-butene, trans-butene, and trimethylethylene) show an ultrafast decay (˜20 fs), whereas the fully methylated tetramethylethylene shows a decay rate of 2 to 4 orders of magnitude slower. These observations are rationalized in terms of topographical trends in the relevant potential energy surfaces, as found from ab initio calculations: (1) the barrier between the π3s state and the ππ* state increases with increasing methylation, and (2) the π3s/ππ* minimum energy conical intersection displaces monotonically away from the π3s Franck-Condon region with increasing methylation. The use of systematic methylation in combination with TRPES and ab initio computation is emerging as an important tool in discerning the excited state dynamics of unsaturated hydrocarbons.

  7. A dynamic plasmonic manipulation technique assisted by phase modulation of an incident optical vortex beam

    International Nuclear Information System (INIS)

    Yuan, G H; Wang, Q; Tan, P S; Lin, J; Yuan, X-C

    2012-01-01

    A novel phase modulation method for dynamic manipulation of surface plasmon polaritons (SPPs) with a phase engineered optical vortex (OV) beam illuminating on nanoslits is experimentally demonstrated. Because of the unique helical phase carried by an OV beam, dynamic control of SPP multiple focusing and standing wave generation is realized by changing the OV beam’s topological charge constituent with the help of a liquid-crystal spatial light modulator. Measurement of SPP distributions with near-field scanning optical microscopy showed an excellent agreement with numerical predictions. The proposed phase modulation technique for manipulating SPPs features has seemingly dynamic and reconfigurable advantages, with profound potential for development of SPP coupling, routing, multiplexing and high-resolution imaging devices on plasmonic chips. (paper)

  8. Ultrafast dynamic computed tomography myelography for the precise identification of high-flow cerebrospinal fluid leaks caused by spiculated spinal osteophytes.

    Science.gov (United States)

    Thielen, Kent R; Sillery, John C; Morris, Jonathan M; Hoxworth, Joseph M; Diehn, Felix E; Wald, John T; Rosebrock, Richard E; Yu, Lifeng; Luetmer, Patrick H

    2015-03-01

    Precise localization and understanding of the origin of spontaneous high-flow spinal CSF leaks is required prior to targeted treatment. This study demonstrates the utility of ultrafast dynamic CT myelography for the precise localization of high-flow CSF leaks caused by spiculated spinal osteophytes. This study reports a series of 14 patients with high-flow CSF leaks caused by spiculated spinal osteophytes who underwent ultrafast dynamic CT myelography between March 2009 and December 2010. There were 10 male and 4 female patients, with an average age of 49 years (range 37-74 years). The value of ultrafast dynamic CT myelography in depicting the CSF leak site was qualitatively assessed. In all 14 patients, ultrafast dynamic CT myelography was technically successful at precisely demonstrating the site of the CSF leak, the causative spiculated osteophyte piercing the dura, and the relationship of the implicated osteophyte to adjacent structures. Leak sites included 3 cervical, 11 thoracic, and 0 lumbar levels, with 86% of the leaks occurring from C-5 to T-7. Information obtained from the ultrafast dynamic CT myelogram was considered useful in all treated CSF leaks. Spinal osteophytes piercing the dura are a more frequent cause of high-flow CSF leaks than previously recognized. Ultrafast dynamic CT myelography adds value beyond standard dynamic myelography or digital subtraction myelography in the diagnosis and anatomical characterization of high-flow spinal CSF leaks caused by these osteophytes. This information allows for appropriate planning for percutaneous or surgical treatment.

  9. Ultrafast carrier thermalization and cooling dynamics in few-layer MoS2.

    Science.gov (United States)

    Nie, Zhaogang; Long, Run; Sun, Linfeng; Huang, Chung-Che; Zhang, Jun; Xiong, Qihua; Hewak, Daniel W; Shen, Zexiang; Prezhdo, Oleg V; Loh, Zhi-Heng

    2014-10-28

    Femtosecond optical pump-probe spectroscopy with 10 fs visible pulses is employed to elucidate the ultrafast carrier dynamics of few-layer MoS2. A nonthermal carrier distribution is observed immediately following the photoexcitation of the A and B excitonic transitions by the ultrashort, broadband laser pulse. Carrier thermalization occurs within 20 fs and proceeds via both carrier-carrier and carrier-phonon scattering, as evidenced by the observed dependence of the thermalization time on the carrier density and the sample temperature. The n(-0.37 ± 0.03) scaling of the thermalization time with carrier density suggests that equilibration of the nonthermal carrier distribution occurs via non-Markovian quantum kinetics. Subsequent cooling of the hot Fermi-Dirac carrier distribution occurs on the ∼ 0.6 ps time scale via carrier-phonon scattering. Temperature- and fluence-dependence studies reveal the involvement of hot phonons in the carrier cooling process. Nonadiabatic ab initio molecular dynamics simulations, which predict carrier-carrier and carrier-phonon scattering time scales of 40 fs and 0.5 ps, respectively, lend support to the assignment of the observed carrier dynamics.

  10. Multiscale Modeling of Plasmon-Exciton Dynamics of Malachite Green Monolayers on Gold Nanoparticles

    Science.gov (United States)

    Smith, Holden; Karam, Tony; Haber, Louis; Lopata, Kenneth

    A multi-scale hybrid quantum/classical approach using classical electrodynamics and a collection of discrete two-level quantum system is used to investigate the coupling dynamics of malachite green monolayers adsorbed to the surface of a spherical gold nanoparticle (NP). This method utilizes finite difference time domain (FDTD) to describe the plasmonic response of the NP and a two-level quantum description for the molecule via the Maxwell/Liouville equation. The molecular parameters are parameterized using CASPT2 for the energies and transition dipole moments, with the dephasing lifetime fit to experiment. This approach is suited to simulating thousands of molecules on the surface of a plasmonic NP. There is good agreement with experimental extinction measurements, predicting the plasmon and molecule depletions. Additionally, this model captures the polariton peaks overlapped with a Fano-type resonance profile observed in the experimental extinction measurements. This technique shows promise for modeling plasmon/molecule interactions in chemical sensing and light harvesting in multi-chromophore systems. This material is based upon work supported by the National Science Foundation under the NSF EPSCoR Cooperative Agreement No. EPS-1003897 and by the Louisiana Board of Regents Research Competitiveness Subprogram under Contract Number LEQSF(2014-17)-RD-A-0.

  11. Dynamical coupling of plasmons and molecular excitations by hybrid quantum/classical calculations: time-domain approach

    International Nuclear Information System (INIS)

    Sakko, Arto; Rossi, Tuomas P; Nieminen, Risto M

    2014-01-01

    The presence of plasmonic material influences the optical properties of nearby molecules in untrivial ways due to the dynamical plasmon-molecule coupling. We combine quantum and classical calculation schemes to study this phenomenon in a hybrid system that consists of a Na 2 molecule located in the gap between two Au/Ag nanoparticles. The molecule is treated quantum-mechanically with time-dependent density-functional theory, and the nanoparticles with quasistatic classical electrodynamics. The nanoparticle dimer has a plasmon resonance in the visible part of the electromagnetic spectrum, and the Na 2 molecule has an electron-hole excitation in the same energy range. Due to the dynamical interaction of the two subsystems the plasmon and the molecular excitations couple, creating a hybridized molecular-plasmon excited state. This state has unique properties that yield e.g. enhanced photoabsorption compared to the freestanding Na 2 molecule. The computational approach used enables decoupling of the mutual plasmon-molecule interaction, and our analysis verifies that it is not legitimate to neglect the backcoupling effect when describing the dynamical interaction between plasmonic material and nearby molecules. Time-resolved analysis shows nearly instantaneous formation of the coupled state, and provides an intuitive picture of the underlying physics. (paper)

  12. 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...... 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. 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.

  14. A dynamically tunable plasmonic multi-functional device based on graphene nano-sheet pair arrays

    Science.gov (United States)

    Wang, Wei; Meng, Zhao; Liang, Ruisheng; Chen, Shijie; Ding, Li; Wang, Faqiang; Liu, Hongzhan; Meng, Hongyun; Wei, Zhongchao

    2018-05-01

    Dynamically tunable plasmonic multi-functional is particularly desirable for various nanotechnological applications. In this paper, graphene nano-sheet pair arrays separated by a substrate, which can act as a dynamically tunable plasmonic band stop filter with transmission at resonance wavelength lower than 1%, a high sensitivity refractive index sensor with sensitivity up to 4879 nm/RIU, figure of merit of 40.66 and a two circuit optical switch with the modulation depth up to 0.998, are proposed and numerically investigated. These excellent optical performances are calculated by using FDTD numerical modeling and theoretical deduction. Simulation results show that a slight variation of chemical potential of the graphene nano-sheet can achieve significant resonance wavelength shifts. In additional, the resonance wavelength and transmission of this plasmonic device can be tuned easily by two voltages owing to the simple patterned graphene. These studies may have great potential in fabrication of multi-functional and dynamically tunable optoelectronic integrated devices.

  15. Generation of nanoclusters by ultrafast laser ablation of Al: Molecular dynamics study

    Energy Technology Data Exchange (ETDEWEB)

    Miloshevsky, Alexander; Phillips, Mark C.; Harilal, Sivanandan S.; Dressman, Phillip; Miloshevsky, Gennady

    2017-11-01

    The laser ablation of materials induced by an ultrashort femtosecond pulse is a complex phenomenon, which depends on both the material properties and the properties of the laser pulse. The unique capability of a combination of molecular dynamics (MD) and Momentum Scaling Model (MSM) methods is developed and applied to a large atomic system for studying the process of ultrafast laser-material interactions, behavior of matter in a highly non-equilibrium state, material disintegration, and formation of nanoparticles (NPs). Laser pulses with several fluences in the range from 500 J/m2 to 5000 J/m2 interacting with a large system of aluminum atoms are simulated. The response of Al material to the laser energy deposition is investigated within the finite-size laser spot. It is found that the shape of the plasma plume is dynamically changing during an expansion process. At several tens of picoseconds it can be characterized as a long hollow ellipsoid surrounded by atomized and nano-clustered particles. The time evolution of NP clusters in the plume is investigated. The collisions between the single Al atoms and generated NPs and fragmentation of large NPs determine the fractions of different-size NP clusters in the plume. The MD-MSM simulations show that laser fluence greatly affects the size distribution of NPs, their polar angles, magnitude and direction vectors of NP velocities. These results and predictions are supported by the experimental data and previous MD simulations.

  16. Radiomics for ultrafast dynamic contrast-enhanced breast MRI in the diagnosis of breast cancer: a pilot study

    Science.gov (United States)

    Drukker, Karen; Anderson, Rachel; Edwards, Alexandra; Papaioannou, John; Pineda, Fred; Abe, Hiroyuke; Karzcmar, Gregory; Giger, Maryellen L.

    2018-02-01

    Radiomics for dynamic contrast-enhanced (DCE) breast MRI have shown promise in the diagnosis of breast cancer as applied to conventional DCE-MRI protocols. Here, we investigate the potential of using such radiomic features in the diagnosis of breast cancer applied on ultrafast breast MRI in which images are acquired every few seconds. The dataset consisted of 64 lesions (33 malignant and 31 benign) imaged with both `conventional' and ultrafast DCE-MRI. After automated lesion segmentation in each image sequence, we calculated 38 radiomic features categorized as describing size, shape, margin, enhancement-texture, kinetics, and enhancement variance kinetics. For each feature, we calculated the 95% confidence interval of the area under the ROC curve (AUC) to determine whether the performance of each feature in the task of distinguishing between malignant and benign lesions was better than random guessing. Subsequently, we assessed performance of radiomic signatures in 10-fold cross-validation repeated 10 times using a support vector machine with as input all the features as well as features by category. We found that many of the features remained useful (AUC>0.5) for the ultrafast protocol, with the exception of some features, e.g., those designed for latephase kinetics such as the washout rate. For ultrafast MRI, the radiomics enhancement-texture signature achieved the best performance, which was comparable to that of the kinetics signature for `conventional' DCE-MRI, both achieving AUC values of 0.71. Radiomic developed for `conventional' DCE-MRI shows promise for translation to the ultrafast protocol, where enhancement texture appears to play a dominant role.

  17. Ultrafast collinear scattering and carrier multiplication in graphene.

    Science.gov (United States)

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

    2013-01-01

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

  18. A novel optical tool for controlling and probing ultrafast surface dynamics

    International Nuclear Information System (INIS)

    Yang, Yudong

    2017-12-01

    Ultrashort pulse laser sources have been greatly developed over the past few decades. The available pulse duration has been reduced to the single-cycle pulse regime. The discovery of high harmonic generation has freed us from the limitation of the laser wavelength. Moreover, the demonstration of isolated attosecond pulse generation has indicated the advent of the attosecond science era. Attosecond pulses undoubtedly allow one to study ultrafast dynamics with unprecedented time resolution. However, physical systems with genuine attosecond time scale dynamics are rather challenging to find. Ultrafast surface charge transfer, which is an important process in photochemistry and electrochemistry, is a good candidate experimental system exhibiting attosecond electronic dynamics. Specifically, the ultrafast surface charge transfer on the c(4 x 2)S/Ru(0001) surface was previously studied and the charge transfer time inferred to be 320 as using core-hole clock spectroscopy at a synchrotron facility. In order to measure this benchmark attosecond electronic dynamics with real time-resolving methods, pump pulses centered at 160 eV and probe pulses centered at 40 eV are required. To this end, a dedicated attosecond experimental beamline including an ultrashort laser pulse source and an attosecond pulse generation and characterization setup has been designed and is being developed. The author of this thesis was responsible for the construction of the attosecond experimental beamline which will be used ultrafast surface charge transfer studies. In this thesis, a completely functional attosecond extreme ultraviolet (XUV) beamline, which includes a few-cycle laser pulse source, an attosecond pulse generation and characterization setup, is described. A commercial Ti:sapphire-based chirped-pulse amplification (CPA) laser system is the overall source of the beamline. The laser system is actively carrier-envelope phase (CEP) stabilized and the output pulse duration is ∝35 fs. The

  19. A novel optical tool for controlling and probing ultrafast surface dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Yudong

    2017-12-15

    Ultrashort pulse laser sources have been greatly developed over the past few decades. The available pulse duration has been reduced to the single-cycle pulse regime. The discovery of high harmonic generation has freed us from the limitation of the laser wavelength. Moreover, the demonstration of isolated attosecond pulse generation has indicated the advent of the attosecond science era. Attosecond pulses undoubtedly allow one to study ultrafast dynamics with unprecedented time resolution. However, physical systems with genuine attosecond time scale dynamics are rather challenging to find. Ultrafast surface charge transfer, which is an important process in photochemistry and electrochemistry, is a good candidate experimental system exhibiting attosecond electronic dynamics. Specifically, the ultrafast surface charge transfer on the c(4 x 2)S/Ru(0001) surface was previously studied and the charge transfer time inferred to be 320 as using core-hole clock spectroscopy at a synchrotron facility. In order to measure this benchmark attosecond electronic dynamics with real time-resolving methods, pump pulses centered at 160 eV and probe pulses centered at 40 eV are required. To this end, a dedicated attosecond experimental beamline including an ultrashort laser pulse source and an attosecond pulse generation and characterization setup has been designed and is being developed. The author of this thesis was responsible for the construction of the attosecond experimental beamline which will be used ultrafast surface charge transfer studies. In this thesis, a completely functional attosecond extreme ultraviolet (XUV) beamline, which includes a few-cycle laser pulse source, an attosecond pulse generation and characterization setup, is described. A commercial Ti:sapphire-based chirped-pulse amplification (CPA) laser system is the overall source of the beamline. The laser system is actively carrier-envelope phase (CEP) stabilized and the output pulse duration is ∝35 fs. The

  20. Dynamic placement of plasmonic hotspots for super-resolution surface-enhanced Raman scattering.

    Science.gov (United States)

    Ertsgaard, Christopher T; McKoskey, Rachel M; Rich, Isabel S; Lindquist, Nathan C

    2014-10-28

    In this paper, we demonstrate dynamic placement of locally enhanced plasmonic fields using holographic laser illumination of a silver nanohole array. To visualize these focused "hotspots", the silver surface was coated with various biological samples for surface-enhanced Raman spectroscopy (SERS) imaging. Due to the large field enhancements, blinking behavior of the SERS hotspots was observed and processed using a stochastic optical reconstruction microscopy algorithm enabling super-resolution localization of the hotspots to within 10 nm. These hotspots were then shifted across the surface in subwavelength (hotspots. Using this technique, we also show that such subwavelength shifting and localization of plasmonic hotspots has potential for imaging applications. Interestingly, illuminating the surface with randomly shifting SERS hotspots was sufficient to completely fill in a wide field of view for super-resolution chemical imaging.

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

    International Nuclear Information System (INIS)

    Stingl, Johannes

    2013-01-01

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

  2. 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)

  3. Structure and Ultrafast Dynamics of White-Light-Emitting CdSe Nanocrystals

    International Nuclear Information System (INIS)

    Bowers, Michael J.; McBride, James; Garrett, Maria Danielle; Sammons, Jessica A.; Dukes, Albert; Schreuder, Michael A.; Watt, Tony L.; Lupini, Andrew R.; Pennycook, Stephen J.; Rosenthal, Sandra

    2009-01-01

    White-light emission from ultrasmall CdSe nanocrystals offers an alternative approach to the realization of solid-state lighting as an appealing technology for consumers. Unfortunately, their extremely small size limits the feasibility of traditional methods for nanocrystal characterization. This paper reports the first images of their structure, which were obtained using aberration-corrected atomic number contrast scanning transmission electron microscopy (Z-STEM). With subangstrom resolution, Z-STEM is one of the few available methods that can be used to directly image the nanocrystal's structure. The initial images suggest that they are crystalline and approximately four lattice planes in diameter. In addition to the structure, for the first time, the exciton dynamics were measured at different wavelengths of the white-light spectrum using ultrafast fluorescence upconversion spectroscopy. The data suggest that a myriad of trap states are responsible for the broad-spectrum emission. It is hoped that the information presented here will provide a foundation for the future development and improvement of white-light-emitting nanocrystals.

  4. Probing ultrafast dynamics of solid-density plasma generated by high-contrast intense laser pulses

    Science.gov (United States)

    Jana, Kamalesh; Blackman, David R.; Shaikh, Moniruzzaman; Lad, Amit D.; Sarkar, Deep; Dey, Indranuj; Robinson, Alex P. L.; Pasley, John; Ravindra Kumar, G.

    2018-01-01

    We present ultrafast dynamics of solid-density plasma created by high-contrast (picosecond contrast ˜10-9), high-intensity (˜4 × 1018 W/cm2) laser pulses using time-resolved pump-probe Doppler spectrometry. Experiments show a rapid rise in blue-shift at early time delay (2-4.3 ps) followed by a rapid fall (4.3-8.3 ps) and then a slow rise in blue-shift at later time delays (>8.3 ps). Simulations show that the early-time observations, specifically the absence of any red-shifting of the reflected probe, can only be reproduced if the front surface is unperturbed by the laser pre-pulse at the moment that the high intensity pulse arrives. A flexible diagnostic which is capable of diagnosing the presence of low-levels of pre-plasma formation would be useful for potential applications in laser-produced proton and ion production, such as cancer therapy and security imaging.

  5. Exciton versus Free Carrier Photogeneration in Organometal Trihalide Perovskites Probed by Broadband Ultrafast Polarization Memory Dynamics

    Science.gov (United States)

    Sheng, ChuanXiang; Zhang, Chuang; Zhai, Yaxin; Mielczarek, Kamil; Wang, Weiwei; Ma, Wanli; Zakhidov, Anvar; Vardeny, Z. Valy

    2015-03-01

    We studied the ultrafast transient response of photoexcitations in two hybrid organic-inorganic perovskite films used for high efficiency photovoltaic cells, namely, CH3NH3PbI3 and CH3NH3PbI1.1Br1.9 using polarized broadband pump-probe spectroscopy in the spectral range of 0.3-2.7 eV with 300 fs time resolution. For CH3NH3PbI3 with above-gap excitation we found both photogenerated carriers and excitons, but only carriers are photogenerated with below-gap excitation. In contrast, mainly excitons are photogenerated in CH3NH3PbI1.1Br1.9 . Surprisingly, we also discovered in CH3NH3PbI3 , but not in CH3NH3PbI1.1Br1.9 , transient photoinduced polarization memory for both excitons and photocarriers, which is also reflected in the steady state photoluminescence. From the polarization memory dynamics we obtained the excitons diffusion constant in CH3NH3PbI3 , D ≈0.01 cm2 s-1 .

  6. Development of an Ultrafast Scanning Tunneling Microscope for Dynamic Surface Studies

    National Research Council Canada - National Science Library

    Nunes

    1999-01-01

    .... The microscope has demonstrated atomic resolution. We have a femtosecond laser system, optics for delivering ultrafast laser pulses to the STM, and a computer controlled delay line for time-resolved measurements...

  7. Ultrafast relaxation dynamics of electrons in Au clusters capped with dodecanethiol molecules

    International Nuclear Information System (INIS)

    Hamanaka, Y.; Fukagawa, K.; Tai, Y.; Murakami, J.; Nakamura, A.

    2006-01-01

    We have investigated electron relaxation dynamics of size-selected Au clusters capped by dodecanethiol molecules in the cluster sizes of 28-142 atoms using femtosecond pump-probe spectroscopy. Absorption spectra of 28-71-atom clusters show discrete peaks due to the optical transitions between quantized states, while an absorption band due to the surface plasmon is observed in 142-atom clusters. In the differential absorption spectra measured by the pump-probe experiments, a large redshift of 140 meV lasting over 10 ps and absorption bleaching decaying within 2 ps are observed at the absorption peaks of 28-atom clusters. The redshift is ascribed to a charge transfer between Au clusters and dodecanethiol molecules adsorbed on the cluster surface, and the bleaching is due to blocking of the optical transitions between the ground state and the occupied electronic states due to the Pauli's-exclusion principle. Such behavior is in contrast to the 142-atom clusters, where the cooling of hot electrons generated by photo-excitation determines the relaxation dynamics. These results indicate molecular properties of the 28-atom Au cluster-dodecanethiol system

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

    DEFF Research Database (Denmark)

    Bache, Morten; Lavrinenko, Andrei

    2017-01-01

    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...

  9. Plasmon dispersion and dynamic exchange-correlation potential from two-pair excitations in degenerate plasmas

    International Nuclear Information System (INIS)

    Boehm, H.M.; Conti, S.; Tosi, M.P.

    1995-11-01

    Electron energy loss experiments have shown a rapid softening of the bulk plasmon dispersion across the series of the alkali metals. Motivated by these observations, we reconsider the evaluation of the dynamic, long-wavelength exchange-correlation potential f xc (ω) in the electron fluid, which is of interest for applications in time-dependent density functional theory. The value of Re[f xc (ω pl )] at the plasma frequency ω pl determines the exchange-correlation contribution to the leading plasmon dispersion coefficient in the homogeneous electron fluid. Whereas an interpolation scheme originally proposed by Gross and Kohn assumes a monotonic increase of Re[f xc (ω) - f xc (0)] across the plasma frequency, we examine the possibility of strongly non-monotonic behaviour arising from a resonance process between plasmons and two-pair excitations. This process is evaluated with the help of sum rules and selfconsistency requirements with a single-pole approximation of the dielectric function. The cases of a fermion plasma and of a boson plasma are treated in parallel and the reliability of the results for the fermion plasma at low coupling is tested by calculations within a random phase approximation for the dielectric function. In all cases it is found that the resonance process accumulates oscillator strength in the neighbourhood of 2ω pl , thus decreasing the value of Re[f xc (ω pl )] below the static value f xc (0) fixed by the compressibility sum rule. Although this lowering does not suffice to account by itself for the measured plasmon dispersion coefficient in the low-density alkali metals, our results provide useful input for combined band-structure and exchange-correlation calculations. (author). 40 refs, 9 figs, 2 tabs

  10. 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

  11. 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

  12. 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.

  13. Sixteenth International Conference on Ultrafast Phenomena

    CERN Document Server

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

    2009-01-01

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

  14. Ultrafast carrier dynamics in a GaN/Al 0.18Ga0.82N superlattice

    Science.gov (United States)

    Mahler, Felix; Tomm, Jens W.; Reimann, Klaus; Woerner, Michael; Elsaesser, Thomas; Flytzanis, Christos; Hoffmann, Veit; Weyers, Markus

    2018-04-01

    Relaxation processes of photoexcited carriers in a GaN /Al0.18Ga0.82N superlattice are studied in femtosecond spectrally resolved reflectivity measurements at ambient temperature. The transient reflectivity reveals electron trapping into defect states close to the conduction-band minimum with a 150-200 fs time constant, followed by few-picosecond carrier cooling. A second slower trapping process into a different manifold of defect states is observed on a time scale of approximately 10 ps. Our results establish the prominent role of structural defects and disorder for ultrafast carrier dynamics in nitride semiconductor structures.

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

    DEFF Research Database (Denmark)

    Lorenz, Ulf

    Over the next few years, a new generation of x-ray sources is going online. These freeelectron lasers will provide extremely bright subpicosecond x-ray pulses. Traditionally, x-ray diraction has the advantage of directly determining the atomic positions within a sample. With these new machines......, 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...

  16. 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...

  17. Ultrafast Ge-Te bond dynamics in a phase-change superlattice

    NARCIS (Netherlands)

    Malvestuto, Marco; Caretta, Antonio; Casarin, Barbara; Cilento, Federico; Dell'Angela, Martina; Fausti, Daniele; Calarco, Raffaella; Kooi, Bart J.; Varesi, Enrico; Robertson, John; Parmigiani, Fulvio

    2016-01-01

    A long-standing question for avant-garde data storage technology concerns the nature of the ultrafast photoinduced phase transformations in the wide class of chalcogenide phase-change materials (PCMs). Overall, a comprehensive understanding of the microstructural evolution and the relevant kinetics

  18. Ultrafast excited and ground-state dynamics of the green fluorescent protein chromophore in solution

    NARCIS (Netherlands)

    Vengris, M.; van Stokkum, I.H.M.; He, X.; Bell, A.F.; Tonge, P.J.; van Grondelle, R.; Larsen, D.S.

    2004-01-01

    Ultrafast dispersed pump-dump-probe spectroscopy was applied to HBDI (4′-hydroxybenzylidene-2,3-dimethylimidazolinone), a model green fluorescent protein (GFP) chromophore in solution with different protonation states. The measured three-dimensional data was analyzed using a global analysis method

  19. 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.

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

    KAUST Repository

    Springer, D.; Nair, Saritha K.; He, Mi; Lu, C. L.; Cheong, S. A.; Wu, Tao; Panagopoulos, C.; Chia, Elbert E. M.; Zhu, Jian-Xin

    2016-01-01

    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.

  1. 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.

  2. 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.

  3. 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.

  4. Ultrafast dynamics in CeTe{sub 3} near the pressure-induced charge-density-wave transition

    Energy Technology Data Exchange (ETDEWEB)

    Tauch, Jonas; Obergfell, Manuel [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Schaefer, Hanjo [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Institute of Physics, Ilmenau University of Technology (Germany); Demsar, Jure [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Institute of Physics, Ilmenau University of Technology (Germany); Institute of Physics, Johannes Gutenberg-University Mainz (Germany); Giraldo, Paula; Fisher, Ian R. [Geballe Laboratory for Advanced Materials and Department of Applied Physics, Stanford University (United States); Pashkin, Alexej [Department of Physics and Center for Applied Photonics, University of Konstanz (Germany); Helmholtz-Zentrum Dresden-Rossendorf (Germany)

    2015-07-01

    Femtosecond pump-probe spectroscopy is an efficient tool for studying ultrafast dynamics in strongly correlated electronic systems, in particular, compounds with a charge-density-wave (CDW) order. Application of external pressure often leads to a suppression of a CDW state due to an impairment of the Fermi surface nesting. We combine time-resolved optical spectroscopy and diamond anvil cell technology to study electron and lattice dynamics in tri-telluride compound CeTe{sub 3}. Around pressures of 4 GPa we observe a gradual vanishing of the relaxation process related to the recombination of the photoexcited quasiparticles. The coherent oscillations of the phonon modes coupled to the CDW order parameter demonstrate even more dramatic suppression with increasing pressure. These observations clearly indicate a transition into the metallic state of CeTe{sub 3} induced by the external pressure.

  5. 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., Jr.; Sundström, V.

    2016-03-01

    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.

  6. Ultrafast carrier dynamics in microcrystalline silicon probed by time-resolved terahertz spectroscopy

    Czech Academy of Sciences Publication Activity Database

    Fekete, Ladislav; Kužel, Petr; Němec, Hynek; Kadlec, Filip; Deyneka, Alexander; Stuchlík, Jiří; Fejfar, Antonín

    2009-01-01

    Roč. 79, č. 11 (2009), 115306/1-115306/13 ISSN 1098-0121 R&D Projects: GA MŠk(CZ) LC06040; GA AV ČR(CZ) IAA100100902 Institutional research plan: CEZ:AV0Z10100520; CEZ:AV0Z10100521 Keywords : microcrystalline silicon * amorphous silicon * terahertz * ultrafast * photoconductivity Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.475, year: 2009

  7. Ultrafast internal rotational dynamics of the azido group in (4S)-azidoproline: Chemical exchange 2DIR spectroscopic investigations

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Kyung-Koo; Park, Kwang-Hee; Joo, Cheonik; Kwon, Hyeok-Jun; Han, Hogyu [Department of Chemistry, Korea University, Seoul 136-701 (Korea, Republic of); Ha, Jeong-Hyon [Multidimensional Spectroscopy Laboratory, Korea Basic Science Institute, Seoul 136-713 (Korea, Republic of); Park, Sungnam, E-mail: spark8@korea.ac.kr [Department of Chemistry, Korea University, Seoul 136-701 (Korea, Republic of); Multidimensional Spectroscopy Laboratory, Korea Basic Science Institute, Seoul 136-713 (Korea, Republic of); Cho, Minhaeng, E-mail: mcho@korea.ac.kr [Department of Chemistry, Korea University, Seoul 136-701 (Korea, Republic of); Multidimensional Spectroscopy Laboratory, Korea Basic Science Institute, Seoul 136-713 (Korea, Republic of); Research Institute for Natural Sciences, Korea University, Seoul 136-713 (Korea, Republic of)

    2012-03-02

    Graphical abstract: Internal rotational dynamics of the azido group in SA (Ac-(4S)-Azp-NHMe) was studied in real time by using ultrafast 2DIR spectroscopic method. The time constant of the internal rotation around the C{sup {gamma}}-N{sup {delta}} bond in SA was determined to be {tau}{sub ir} = 5.1 ps, which is found to be much faster than that around the C-C bond in ethane. Highlights: Black-Right-Pointing-Pointer Femtosecond two-dimensional IR spectroscopy of internal rotational dynamics. Black-Right-Pointing-Pointer Stereo-electronic effects of azido group in azido-derivatized proline peptide. Black-Right-Pointing-Pointer The timescale of the azido group internal rotation is about 5.1 ps. - Abstract: The azido group in 4-azidoproline (Azp) derivative, SA (Ac-(4S)-Azp-NHMe), can form an intramolecular electrostatic interaction with the backbone peptide in the s-trans and C{sup {gamma}}-endo conformations of SA. As a result, the azido group exists as two forms, bound and free, which are defined by the presence and absence of such interaction, respectively. The bound and free azido forms are spectrally resolved in the azido IR spectrum of SA in CHCl{sub 3}. Using the two-dimensional infrared (2DIR) and polarization-controlled IR pump-probe methods, we investigated the internal rotational and orientational relaxation dynamics of the azido group and determined the internal rotational time constant of the azido group to be 5.1 ps. The internal rotational motion is found to be responsible for the early part of the orientational relaxation of the azido group in SA. Thus, the femtosecond 2DIR spectroscopy is shown to be an ideal tool for studying ultrafast conformational dynamics of SA.

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

    Science.gov (United States)

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

    2018-04-01

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

  9. 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.

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

    KAUST Repository

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

    2015-01-01

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

  11. Non-equilibrium lattice dynamics of one-dimensional In chains on Si(111 upon ultrafast optical excitation

    Directory of Open Access Journals (Sweden)

    T. Frigge

    2018-03-01

    Full Text Available The photoinduced structural dynamics of the atomic wire system on the Si(111-In surface has been studied by ultrafast electron diffraction in reflection geometry. Upon intense fs-laser excitation, this system can be driven in around 1 ps from the insulating (8×2 reconstructed low temperature phase to a metastable metallic (4×1 reconstructed high temperature phase. Subsequent to the structural transition, the surface heats up on a 6 times slower timescale as determined from a transient Debye-Waller analysis of the diffraction spots. From a comparison with the structural response of the high temperature (4×1 phase, we conclude that electron-phonon coupling is responsible for the slow energy transfer from the excited electron system to the lattice. The significant difference in timescales is evidence that the photoinduced structural transition is non-thermally driven.

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

    Science.gov (United States)

    Tang, Jau

    2008-04-28

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

  13. Dynamics of liquids, molecules, and proteins measured with ultrafast 2D IR vibrational echo chemical exchange spectroscopy.

    Science.gov (United States)

    Fayer, M D

    2009-01-01

    A wide variety of molecular systems undergo fast structural changes under thermal equilibrium conditions. Such transformations are involved in a vast array of chemical problems. Experimentally measuring equilibrium dynamics is a challenging problem that is at the forefront of chemical research. This review describes ultrafast 2D IR vibrational echo chemical exchange experiments and applies them to several types of molecular systems. The formation and dissociation of organic solute-solvent complexes are directly observed. The dissociation times of 13 complexes, ranging from 4 ps to 140 ps, are shown to obey a relationship that depends on the complex's formation enthalpy. The rate of rotational gauche-trans isomerization around a carbon-carbon single bond is determined for a substituted ethane at room temperature in a low viscosity solvent. The results are used to obtain an approximate isomerization rate for ethane. Finally, the time dependence of a well-defined single structural transformation of a protein is measured.

  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 transient absorption revisited: Phase-flips, spectral fingers, and other dynamical features

    Energy Technology Data Exchange (ETDEWEB)

    Cina, Jeffrey A., E-mail: cina@uoregon.edu; Kovac, Philip A. [Department of Chemistry and Biochemistry, and Oregon Center for Optical, Molecular, and Quantum Science, University of Oregon, Eugene, Oregon 97403 (United States); Jumper, Chanelle C. [Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6 (Canada); Dean, Jacob C.; Scholes, Gregory D., E-mail: gscholes@princeton.edu [Department of Chemistry, Princeton University, Princeton, New Jersey 08544 (United States)

    2016-05-07

    We rebuild the theory of ultrafast transient-absorption/transmission spectroscopy starting from the optical response of an individual molecule to incident femtosecond pump and probe pulses. The resulting description makes use of pulse propagators and free molecular evolution operators to arrive at compact expressions for the several contributions to a transient-absorption signal. In this alternative description, which is physically equivalent to the conventional response-function formalism, these signal contributions are conveniently expressed as quantum mechanical overlaps between nuclear wave packets that have undergone different sequences of pulse-driven optical transitions and time-evolution on different electronic potential-energy surfaces. Using this setup in application to a simple, multimode model of the light-harvesting chromophores of PC577, we develop wave-packet pictures of certain generic features of ultrafast transient-absorption signals related to the probed-frequency dependence of vibrational quantum beats. These include a Stokes-shifting node at the time-evolving peak emission frequency, antiphasing between vibrational oscillations on opposite sides (i.e., to the red or blue) of this node, and spectral fingering due to vibrational overtones and combinations. Our calculations make a vibrationally abrupt approximation for the incident pump and probe pulses, but properly account for temporal pulse overlap and signal turn-on, rather than neglecting pulse overlap or assuming delta-function excitations, as are sometimes done.

  16. 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

  17. Photoinduced Ultrafast Intramolecular Excited-State Energy Transfer in the Silylene-Bridged Biphenyl and Stilbene (SBS) System: A Nonadiabatic Dynamics Point of View.

    Science.gov (United States)

    Wang, Jun; Huang, Jing; Du, Likai; Lan, Zhenggang

    2015-07-09

    The photoinduced intramolecular excited-state energy-transfer (EET) process in conjugated polymers has received a great deal of research interest because of its important role in the light harvesting and energy transport of organic photovoltaic materials in photoelectric devices. In this work, the silylene-bridged biphenyl and stilbene (SBS) system was chosen as a simplified model system to obtain physical insight into the photoinduced intramolecular energy transfer between the different building units of the SBS copolymer. In the SBS system, the vinylbiphenyl and vinylstilbene moieties serve as the donor (D) unit and the acceptor (A) unit, respectively. The ultrafast excited-state dynamics of the SBS system was investigated from the point of view of nonadiabatic dynamics with the surface-hopping method at the TDDFT level. The first two excited states (S1 and S2) are characterized by local excitations at the acceptor (vinylstilbene) and donor (vinylbiphenyl) units, respectively. Ultrafast S2-S1 decay is responsible for the intramolecular D-A excitonic energy transfer. The geometric distortion of the D moiety play an essential role in this EET process, whereas the A moiety remains unchanged during the nonadiabatic dynamics simulation. The present work provides a direct dynamical approach to understand the ultrafast intramolecular energy-transfer dynamics in SBS copolymers and other similar organic photovoltaic copolymers.

  18. Emission dynamics of hybrid plasmonic gold/organic GaN nanorods

    Science.gov (United States)

    Mohammadi, F.; Schmitzer, H.; Kunert, G.; Hommel, D.; Ge, J.; Duscher, G.; Langbein, W.; Wagner, H. P.

    2017-12-01

    We studied the emission of bare and aluminum quinoline (Alq3)/gold coated wurtzite GaN nanorods by temperature- and intensity-dependent time-integrated and time-resolved photoluminescence (PL). The GaN nanorods of ˜1.5 μm length and ˜250 nm diameter were grown by plasma-assisted molecular beam epitaxy. Gold/Alq3 coated GaN nanorods were synthesized by organic molecular beam deposition. The near band-edge and donor-acceptor pair luminescence was investigated in bare GaN nanorods and compared with multilevel model calculations providing the dynamical parameters for electron-hole pairs, excitons, impurity bound excitons, donors and acceptors. Subsequently, the influence of a 10 nm gold coating without and with an Alq3 spacer layer was studied and the experimental results were analyzed with the multilevel model. Without a spacer layer, a significant PL quenching and lifetime reduction of the near band-edge emission is found. The behavior is attributed to surface band-bending and Förster energy transfer from excitons to surface plasmons in the gold layer. Inserting a 5 nm Alq3 spacer layer reduces the PL quenching and lifetime reduction which is consistent with a reduced band-bending and Förster energy transfer. Increasing the spacer layer to 30 nm results in lifetimes which are similar to uncoated structures, showing a significantly decreased influence of the gold coating on the excitonic dynamics.

  19. 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.

  20. Ultrafast Relaxation Dynamics of the Optical Nonlinearity in Nanometric Gold Particles

    International Nuclear Information System (INIS)

    Puech, K.; Blau, W.J.

    2001-01-01

    Measurements of the resonantly enhanced, third-order nonlinear optical properties of gold nanostructures exhibiting reduced charge-carrier mobility in three dimensions were performed with a number of ultrafast nonlinear optical techniques. The size of the particles investigated was varied between 5 and 40 nm. The magnitude of the nonlinear susceptibility is of the order of 5.10 -16 m 2 V -2 at resonance and an order of magnitude lower off-resonance. The response time of the nonlinearity is found to be extremely fast and could not be resolved in the experiments undertaken here. The only statement that can be made in this regard is that the phase relaxation time is of the order of or less than 20 fs while the energy relaxation time is of the order of or less than 75 fs

  1. Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)

    Energy Technology Data Exchange (ETDEWEB)

    Hong, Sung-Young; Camillone, Nina R.; Camillone, Nicholas, E-mail: nicholas@bnl.gov [Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973 (United States); Xu, Pan [Department of Chemistry, Stony Brook University, Stony Brook, New York 11794 (United States); White, Michael G. [Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973 (United States); Department of Chemistry, Stony Brook University, Stony Brook, New York 11794 (United States)

    2016-07-07

    We report our ultrafast photoinduced desorption investigation of the coverage dependence of substrate–adsorbate energy transfer in carbon monoxide adlayers on the (111) surface of palladium. As the CO coverage is increased, the adsorption site population shifts from all threefold hollows (up to 0.33 ML), to bridge and near bridge (>0.5 to 0.6 ML) and finally to mixed threefold hollow plus top site (at saturation at 0.75 ML). We show that between 0.24 and 0.75 ML this progression of binding site motifs is accompanied by two remarkable features in the ultrafast photoinduced desorption of the adsorbates: (i) the desorption probability increases roughly two orders magnitude, and (ii) the adsorbate–substrate energy transfer rate observed in two-pulse correlation experiments varies nonmonotonically, having a minimum at intermediate coverages. Simulations using a phenomenological model to describe the adsorbate–substrate energy transfer in terms of frictional coupling indicate that these features are consistent with an adsorption-site dependent electron-mediated energy coupling strength, η{sub el}, that decreases with binding site in the order: three-fold hollow > bridge and near bridge > top site. This weakening of η{sub el} largely counterbalances the decrease in the desorption activation energy that accompanies this progression of adsorption site motifs, moderating what would otherwise be a rise of several orders of magnitude in the desorption probability. Within this framework, the observed energy transfer rate enhancement at saturation coverage is due to interadsorbate energy transfer from the copopulation of molecules bound in three-fold hollows to their top-site neighbors.

  2. Ultrafast Gap Dynamics and Electronic Interactions in a Photoexcited Cuprate Superconductor

    Directory of Open Access Journals (Sweden)

    S. Parham

    2017-10-01

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

  3. Nonponderomotive electron acceleration in ultrashort surface-plasmon fields

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-12-15

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

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

    Science.gov (United States)

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

    2018-02-01

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

  5. 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.

  6. Characterisation and setup of a noncollinear optical parametric amplifier and investigation of ultrafast dynamics of Na/Cu(111)

    Energy Technology Data Exchange (ETDEWEB)

    Wegkamp, Daniel; Krenz, Marcel; Wolf, Martin [Fritz Haber Institute of the MPG, Dept. of Physical Chemistry, Berlin (Germany); Freie Universitaet Berlin, Dept. of Physics, Berlin (Germany); Bovensiepen, Uwe [Universitaet Duisburg-Essen, Dept. of Physics, Duisburg (Germany); Freie Universitaet Berlin, Dept. of Physics, Berlin (Germany)

    2010-07-01

    To study ultrafast dynamics on a femtosecond timescale, laser pulses of comparable and shorter scale are used in this work in combination with 2-photon photoemission. Here, we report the principle, setup, and characterisation of a femtosecond light-source based on a noncollinear optical parametric amplifier (NOPA) and its application in studying the dynamics of Na/Cu(111) following. Laser pulses with duration <20 fs have been generated in the visible spectral range using a 300 kHz regenerative amplifier. In a single color scheme (h{nu}=2.3 eV) the NOPA pulses are used to excite and photoemit hot electrons, which are detected with a time of flight (TOF) spectrometer. With time independent measurements the binding energy of the adsorbate-induced resonance at 2 eV is observed in agreement with. As a function of pump-probe delay a time-dependent binding energy shift of the Na resonance with -2 meV/fs is observed. This shift is explained as a pump-induced movement of the sodium adsorbate away from the surface.

  7. Tailored Surfaces/Assemblies for Molecular Plasmonics and Plasmonic Molecular Electronics.

    Science.gov (United States)

    Lacroix, Jean-Christophe; Martin, Pascal; Lacaze, Pierre-Camille

    2017-06-12

    Molecular plasmonics uses and explores molecule-plasmon interactions on metal nanostructures for spectroscopic, nanophotonic, and nanoelectronic devices. This review focuses on tailored surfaces/assemblies for molecular plasmonics and describes active molecular plasmonic devices in which functional molecules and polymers change their structural, electrical, and/or optical properties in response to external stimuli and that can dynamically tune the plasmonic properties. We also explore an emerging research field combining molecular plasmonics and molecular electronics.

  8. 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....

  9. Femtosecond terahertz studies of many-body correlations. From ultrafast phonon-plasmon dynamics to an insulator-metal transition

    International Nuclear Information System (INIS)

    Kuebler, C.

    2007-01-01

    Phase-matched optical rectification together with standard EOS methods gives direct access to the real-time evolution of the electric field of ultrashort THz pulses. This opens up a new field of experiments, in which the complex dielectric function or equivalently the frequency-dependent conductivity of solid state systems is monitored resonantly throughout the MIR and FIR with a femtosecond temporal resolution. Optical rectification of amplified laser pulses allows for the generation of electric fields of several 10 kV cm-1 up to 1 MV cm-1, depending on the laser pulse energy. Such highly energetic field transients may be employed to coherently drive low-energy transitions into the nonlinear regime. The problems which are inherent to standard EOS, i.e. a fixed detector response and a limited bandwidth, are absent in phase-matched EOS. If this novel detection technique is combined with phase-matched optical rectification, an extremely versatile multi-THz spectrometer is obtained. The accessible frequency range is extended toward the near infrared. In addition, both the emission spectrum and the detector response may be custom tailored to fit specific spectroscopic requirements. Proper choice of the phasematching geometry eliminates multiple time delayed reflections of the main THz pulse, resulting in an essentially unlimited frequency resolution. In the context of optical pump - multi-THz probe experiments the implementation of a photoelastic modulator results in significant improvement of the signal-to-noise ratio: Balancing of the differential detector is rendered less critical and the measurement time in a 2D time-resolved experiment is reduced by up to two orders of magnitude. Finally, the combination of phase-matched optical rectification and phasematched electro-optic sampling shows great scaling potential with respect to both achieving higher field energies and shorter wavelengths. (orig.)

  10. Femtosecond terahertz studies of many-body correlations. From ultrafast phonon-plasmon dynamics to an insulator-metal transition

    Energy Technology Data Exchange (ETDEWEB)

    Kuebler, C.

    2007-07-30

    Phase-matched optical rectification together with standard EOS methods gives direct access to the real-time evolution of the electric field of ultrashort THz pulses. This opens up a new field of experiments, in which the complex dielectric function or equivalently the frequency-dependent conductivity of solid state systems is monitored resonantly throughout the MIR and FIR with a femtosecond temporal resolution. Optical rectification of amplified laser pulses allows for the generation of electric fields of several 10 kV cm-1 up to 1 MV cm-1, depending on the laser pulse energy. Such highly energetic field transients may be employed to coherently drive low-energy transitions into the nonlinear regime. The problems which are inherent to standard EOS, i.e. a fixed detector response and a limited bandwidth, are absent in phase-matched EOS. If this novel detection technique is combined with phase-matched optical rectification, an extremely versatile multi-THz spectrometer is obtained. The accessible frequency range is extended toward the near infrared. In addition, both the emission spectrum and the detector response may be custom tailored to fit specific spectroscopic requirements. Proper choice of the phasematching geometry eliminates multiple time delayed reflections of the main THz pulse, resulting in an essentially unlimited frequency resolution. In the context of optical pump - multi-THz probe experiments the implementation of a photoelastic modulator results in significant improvement of the signal-to-noise ratio: Balancing of the differential detector is rendered less critical and the measurement time in a 2D time-resolved experiment is reduced by up to two orders of magnitude. Finally, the combination of phase-matched optical rectification and phasematched electro-optic sampling shows great scaling potential with respect to both achieving higher field energies and shorter wavelengths. (orig.)

  11. Dynamic thermal effects of epidermal melanin and plasmonic nanoparticles during photoacoustic breast imaging

    Science.gov (United States)

    Ghassemi, Pejhman; Wang, Quanzeng; Pfefer, T. Joshua

    2016-03-01

    Photoacoustic Tomography (PAT) employs high-power near-infrared (near-IR) laser pulses to generate structural and functional information on tissue chromophores up to several centimeters below the surface. Such insights may facilitate detection of breast cancer - the most common cancer in women. PAT mammography has been the subject of extensive research, including techniques based on exogenous agents for PAT contrast enhancement and molecular specificity. However, photothermal safety risks of PAT due to strong chromophores such as epidermal melanin and plasmonic nanoparticles have not been rigorously studied. We have used computational and experimental approaches to elucidate highly dynamic optical-thermal processes during PAT. A Monte Carlo model was used to simulate light propagation at 800 and 1064 nm in a multi-layer breast tissue geometry with different epidermal pigmentation levels and a tumorsimulating inclusion incorporating nanoparticles. Energy deposition results were then used in a bioheat transfer model to simulate temperature transients. Experimental measurements involved multi-layer hydrogel phantoms with inclusions incorporating gold nanoparticles. Phantom optical properties were measured using the inverse adding-doubling technique. Thermal imaging was performed as phantoms were irradiated with 5 ns near-IR pulses. Scenarios using 10 Hz laser irradiation of breast tissue containing various nanoparticle concentrations were implemented experimentally and computationally. Laser exposure levels were based on ANSI/IEC limits. Surface temperature measurements were compared to corresponding simulation data. In general, the effect of highly pigmented skin on temperature rise was significant, whereas unexpectedly small levels of temperature rise during nanoparticle irradiation were attributed to rapid photodegradation. Results provide key initial insights into light-tissue interactions impacting the safety and effectiveness of PAT.

  12. 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.

  13. 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.

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

    Directory of Open Access Journals (Sweden)

    Shaozheng Ji

    2017-09-01

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

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

    Science.gov (United States)

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

    2017-09-01

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

  16. Dynamics-based selective 2D 1H/1H chemical shift correlation spectroscopy under ultrafast MAS conditions

    Science.gov (United States)

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-05-01

    Dynamics plays important roles in determining the physical, chemical, and functional properties of a variety of chemical and biological materials. However, a material (such as a polymer) generally has mobile and rigid regions in order to have high strength and toughness at the same time. Therefore, it is difficult to measure the role of mobile phase without being affected by the rigid components. Herein, we propose a highly sensitive solid-state NMR approach that utilizes a dipolar-coupling based filter (composed of 12 equally spaced 90° RF pulses) to selectively measure the correlation of 1H chemical shifts from the mobile regions of a material. It is interesting to find that the rotor-synchronized dipolar filter strength decreases with increasing inter-pulse delay between the 90° pulses, whereas the dipolar filter strength increases with increasing inter-pulse delay under static conditions. In this study, we also demonstrate the unique advantages of proton-detection under ultrafast magic-angle-spinning conditions to enhance the spectral resolution and sensitivity for studies on small molecules as well as multi-phase polymers. Our results further demonstrate the use of finite-pulse radio-frequency driven recoupling pulse sequence to efficiently recouple weak proton-proton dipolar couplings in the dynamic regions of a molecule and to facilitate the fast acquisition of 1H/1H correlation spectrum compared to the traditional 2D NOESY (Nuclear Overhauser effect spectroscopy) experiment. We believe that the proposed approach is beneficial to study mobile components in multi-phase systems, such as block copolymers, polymer blends, nanocomposites, heterogeneous amyloid mixture of oligomers and fibers, and other materials.

  17. Dynamics-based selective 2D 1H/1H chemical shift correlation spectroscopy under ultrafast MAS conditions

    International Nuclear Information System (INIS)

    Zhang, Rongchun; Ramamoorthy, Ayyalusamy

    2015-01-01

    Dynamics plays important roles in determining the physical, chemical, and functional properties of a variety of chemical and biological materials. However, a material (such as a polymer) generally has mobile and rigid regions in order to have high strength and toughness at the same time. Therefore, it is difficult to measure the role of mobile phase without being affected by the rigid components. Herein, we propose a highly sensitive solid-state NMR approach that utilizes a dipolar-coupling based filter (composed of 12 equally spaced 90° RF pulses) to selectively measure the correlation of 1 H chemical shifts from the mobile regions of a material. It is interesting to find that the rotor-synchronized dipolar filter strength decreases with increasing inter-pulse delay between the 90° pulses, whereas the dipolar filter strength increases with increasing inter-pulse delay under static conditions. In this study, we also demonstrate the unique advantages of proton-detection under ultrafast magic-angle-spinning conditions to enhance the spectral resolution and sensitivity for studies on small molecules as well as multi-phase polymers. Our results further demonstrate the use of finite-pulse radio-frequency driven recoupling pulse sequence to efficiently recouple weak proton-proton dipolar couplings in the dynamic regions of a molecule and to facilitate the fast acquisition of 1 H/ 1 H correlation spectrum compared to the traditional 2D NOESY (Nuclear Overhauser effect spectroscopy) experiment. We believe that the proposed approach is beneficial to study mobile components in multi-phase systems, such as block copolymers, polymer blends, nanocomposites, heterogeneous amyloid mixture of oligomers and fibers, and other materials

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

  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...

  20. 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

  1. Ultrafast Spectroscopy of Semiconductor Devices

    DEFF Research Database (Denmark)

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

    1999-01-01

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

  2. Development of Novel High Temperature Superconducting Detectors Based on Flux Activation and Ultrafast Dynamics

    National Research Council Canada - National Science Library

    Frankel, Anatoly

    1998-01-01

    It is proposed to study quasiparticle (QP) relaxation dynamics and flux mechanism of HTS using pump/probe femtosecond spectroscopy and nonequilibrium photoresponse in the presence of a magnetic field (and/or bias current...

  3. Ultrafast Dynamics of Dansylated POPAM Dendrimers and Energy Transfer in their Dye Complexes

    Science.gov (United States)

    Aumanen, J.; Kesti, T.; Sundström, V.; Vögtle, F.; Korppi-Tommola, J.

    We have studied internal dynamics of dansylated poly(propyleneamine) dendrimers of different generations in solution and excitation energy transfer from dansyl chromophores to xanthene dyes that form van der Waals complexes with the dendrimers

  4. Photo-conductive detection of continuous THz waves via manipulated ultrafast process in nanostructures

    Science.gov (United States)

    Moon, Kiwon; Lee, Eui Su; Lee, Il-Min; Park, Dong Woo; Park, Kyung Hyun

    2018-01-01

    Time-domain and frequency-domain terahertz (THz) spectroscopy systems often use materials fabricated with exotic and expensive methods that intentionally introduce defects to meet short carrier lifetime requirements. In this study, we demonstrate the development of a nano-photomixer that meets response speed requirements without using defect-incorporated, low-temperature-grown (LTG) semiconductors. Instead, we utilized a thin InGaAs layer grown on a semi-insulating InP substrate by metal-organic chemical vapor deposition (MOCVD) combined with nano-electrodes to manipulate local ultrafast photo-carrier dynamics via a carefully designed field-enhancement and plasmon effect. The developed nano-structured photomixer can detect continuous-wave THz radiation up to a frequency of 2 THz with a peak carrier collection efficiency of 5%, which is approximately 10 times better than the reference efficiency of 0.4%. The better efficiency results from the high carrier mobility of the MOCVD-grown InGaAs thin layer with the coincidence of near-field and plasmon-field distributions in the nano-structure. Our result not only provides a generally applicable methodology for manipulating ultrafast carrier dynamics by means of nano-photonic techniques to break the trade-off relation between the carrier lifetime and mobility in typical LTG semiconductors but also contributes to mass-producible photo-conductive THz detectors to facilitate the widespread application of THz technology.

  5. 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.

  6. Spectrally- and Time-Resolved Sum Frequency Generation (STiR-SFG): a new tool for ultrafast hydrogen bond dynamics at interfaces.

    Science.gov (United States)

    Benderskii, Alexander; Bordenyuk, Andrey; Weeraman, Champika

    2006-03-01

    The recently developed spectrally- and time-resolved Sum Frequency Generation (STiR-SFG) is a surface-selective 3-wave mixing (IR+visible) spectroscopic technique capable of measuring ultrafast spectral evolution of vibrational coherences. A detailed description of this measurement will be presented, and a noniterative method or deconvolving the laser pulses will be introduced to obtain the molecular response function. STiR-SFG, combined with the frequency-domain SFG spectroscopy, was applied to study hydrogen bonding dynamics at aqueous interfaces (D2O/CaF2). Spectral dynamics of the OD-stretch on the 50-150 fs time scale provides real-time observation of ultrafast H-bond rearrangement. Tuning the IR wavelength to the blue or red side of the OD-stretch transition, we selectively monitor the dynamics of different sub-ensembles in the distribution of the H-bond structures. The blue-side excitation (weaker H-bonding) shows monotonic red-shift of the OD-frequency. In contrast, the red-side excitation (stronger H-bonding structures) produces a blue-shift and a recursion, which may indicate the presence of an underdamped intermolecular mode of interfacial water. Effect of electrolyte concentration on the H-bond dynamics will be discussed.

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

    Directory of Open Access Journals (Sweden)

    Yulu Huang

    2016-08-01

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

  8. Ultrafast carrier dynamics of titanic acid nanotubes investigated by transient absorption spectroscopy.

    Science.gov (United States)

    Wang, Li; Zhao, Hui; Pan, Lin Yun; Weng, Yu Xiang; Nakato, Yoshihiro; Tamai, Naoto

    2010-12-01

    Carrier dynamics of titanic acid nanotubes (phase of H2Ti2O5.H2O) deposited on a quartz plate was examined by visible/near-IR transient absorption spectroscopy with an ultraviolet excitation. The carrier dynamics of titanic acid nanotubes follows the fast trapping process which attributed to the intrinsic tubular structure, the relaxation of shallow trapped carriers and the recombination as a second-order kinetic process. Transient absorption of titanic acid nanotubes was dominated by the absorption of surface-trapped holes in visible region around 500 nm, which was proved by the faster decay dynamics in the presence of polyvinyl alcohol as a hole-scavenger. However, the slow relaxation of free carriers was much more pronounced in the TiO2 single crystals, as compared with the transient absorption spectra of titanic acid nanotubes under the similar excitation.

  9. 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...

  10. 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...

  11. Photoelectron photoion coincidence imaging of ultrafast control in multichannel molecular dynamics.

    Science.gov (United States)

    Lehmann, C Stefan; Ram, N Bhargava; Irimia, Daniel; Janssen, Maurice H M

    2011-01-01

    The control of multichannel ionic fragmentation dynamics in CF3I is studied by femtosecond pulse shaping and velocity map photoelectron photoion coincidence imaging. When CF3I is photoexcited with femtosecond laser pulses around 540 nm there are two major ions observed in the time-of-flight mass spectrum, the parent CF3I+ ion and the CF3+ fragment ion. In this first study we focussed on the influence of LCD-shaped laser pulses on the molecular dynamics. The three-dimensional recoil distribution of electrons and ions were imaged in coincidence using a single time-of-flight delay line detector. By fast switching of the voltages on the various velocity map ion lenses after detection of the electron, both the electron and the coincident ion are measured with the same imaging detector. These results demonstrate that a significant simplification of a photoelectron-photoion coincidence imaging apparatus is in principle possible using switched lens voltages. It is observed that shaped laser fields like chirped pulses, double pulses, and multiple pulses can enhance the CF3+CF3I+ ratio by up to 100%. The total energetics of the dynamics is revealed by analysis of the coincident photoelectron spectra and the kinetic energy of the CF3+ and I fragments. Both the parent CF3I+ and the CF3+ fragment result from a five-photon excitation process. The fragments are formed with very low kinetic energy. The photoelectron spectra and CF3+/CF3I+ ratio vary with the center wavelength of the shaped laser pulses. An optimal enhancement of the CF3+/CF3I+ ratio by about 60% is observed for the double pulse excitation when the pulses are spaced 60 fs apart. We propose that the control mechanism is determined by dynamics on neutral excited states and we discuss the results in relation to the location of electronically excited (Rydberg) states of CF3I.

  12. Ultrafast photoionization dynamics at high laser intensities in the xuv regime

    Energy Technology Data Exchange (ETDEWEB)

    Kaiser, B.; Vagov, A.; Axt, V. M.; Pietsch, U. [Institut fuer Theoretische Physik III, Universitaet Bayreuth, D-95440 Bayreuth (Germany); Institut fuer Festkoerperphysik, Universitaet Siegen, D-57068 Siegen (Germany)

    2011-10-15

    We study the ionization dynamics in the soft-x-ray regime for high intensities and short pulses for excitations near the ionization threshold. Using a one-dimensional helium atom model, we compare exact numerical solutions with time-dependent Hartree-Fock results in order to identify the role of electron-electron correlations. At moderate intensities but still in the x-ray and short-pulse regime, we find that the Hartree-Fock theory reproduces well the dynamics of the ground-state occupation, while at high intensities strong correlation effects occur for excitations close to the threshold. From their characteristic momentum distributions, we can identify contributions to the double ionization from sequential three-photon and nonsequential or sequential two-photon processes. At elevated intensities these contributions deviate from their usual intensity scaling due to saturation effects, even though the total double-ionization probability stays below 10%. Furthermore, analysis of the time evolution of the momentum distribution reveals signatures of the energy-time uncertainty which indicate a coherent regime of the dynamics.

  13. Plasmonic biosensors.

    Science.gov (United States)

    Hill, Ryan T

    2015-01-01

    The unique optical properties of plasmon resonant nanostructures enable exploration of nanoscale environments using relatively simple optical characterization techniques. For this reason, the field of plasmonics continues to garner the attention of the biosensing community. Biosensors based on propagating surface plasmon resonances (SPRs) in films are the most well-recognized plasmonic biosensors, but there is great potential for the new, developing technologies to surpass the robustness and popularity of film-based SPR sensing. This review surveys the current plasmonic biosensor landscape with emphasis on the basic operating principles of each plasmonic sensing technique and the practical considerations when developing a sensing platform with the various techniques. The 'gold standard' film SPR technique is reviewed briefly, but special emphasis is devoted to the up-and-coming localized surface plasmon resonance and plasmonically coupled sensor technology. © 2014 Wiley Periodicals, Inc.

  14. Ultrafast relaxation dynamics of a biologically relevant probe dansyl at the micellar surface.

    Science.gov (United States)

    Sarkar, Rupa; Ghosh, Manoranjan; Pal, Samir Kumar

    2005-02-01

    We report picosecond-resolved measurement of the fluorescence of a well-known biologically relevant probe, dansyl chromophore at the surface of a cationic micelle (cetyltrimethylammonium bromide, CTAB). The dansyl chromophore has environmentally sensitive fluorescence quantum yields and emission maxima, along with large Stokes shift. In order to study the solvation dynamics of the micellar environment, we measured the fluorescence of dansyl chromophore attached to the micellar surface. The fluorescence transients were observed to decay (with time constant approximately 350 ps) in the blue end and rise with similar timescale in the red end, indicative of solvation dynamics of the environment. The solvation correlation function is measured to decay with time constant 338 ps, which is much slower than that of ordinary bulk water. Time-resolved anisotropy of the dansyl chromophore shows a bi-exponential decay with time constants 413 ps (23%) and 1.3 ns (77%), which is considerably slower than that in free solvents revealing the rigidity of the dansyl-micelle complex. Time-resolved area-normalized emission spectroscopic (TRANES) analysis of the time dependent emission spectra of the dansyl chromophore in the micellar environment shows an isoemissive point at 21066 cm-1. This indicates the fluorescence of the chromophore contains emission from two kinds of excited states namely locally excited state (prior to charge transfer) and charge transfer state. The nature of the solvation dynamics in the micellar environments is therefore explored from the time-resolved anisotropy measurement coupled with the TRANES analysis of the fluorescence transients. The time scale of the solvation is important for the mechanism of molecular recognition.

  15. Ultrafast dynamics in ZnO/ZnMgO multiple quantum wells

    International Nuclear Information System (INIS)

    Wen, X M; Davis, J A; McDonald, D; Dao, L V; Hannaford, P; Coleman, V A; Tan, H H; Jagadish, C; Koike, K; Sasa, S; Inoue, M; Yano, M

    2007-01-01

    We have investigated carrier relaxation and exciton recombination dynamics in ZnO/ZnMgO multiple quantum wells using femtosecond pump-probe techniques at room temperature. For a probe energy above the band gap, the hot carriers exhibit an effective relaxation by longitudinal optical phonon scattering with a cooling time of 700-850 fs. By detecting the emission near the band-gap, a longer decay time of a few picoseconds was observed which is attributed to acoustic phonon scattering. As the probe energy is decreased further, the decay time continues to increase due to the transitions of exciton recombination or localized carrier recombination

  16. Ultrafast table-top dynamic radiography of spontaneous or stimulated events

    Science.gov (United States)

    Smilowitz, Laura; Henson, Bryan

    2018-01-16

    Disclosed herein are representative embodiments of methods, apparatus, and systems for performing radiography. For example, certain embodiments concern X-ray radiography of spontaneous events. Particular embodiments of the disclosed technology provide continuous high-speed x-ray imaging of spontaneous dynamic events, such as explosions, reaction-front propagation, and even material failure. Further, in certain embodiments, x-ray activation and data collection activation are triggered by the object itself that is under observation (e.g., triggered by a change of state detected by one or more sensors monitoring the object itself).

  17. Nonequilibrium Dynamics in a Quasi-Two-Dimensional Electron Plasma after Ultrafast Intersubband Excitation

    International Nuclear Information System (INIS)

    Lutgen, S.; Kaindl, R.A.; Woerner, M.; Elsaesser, T.; Hase, A.; Kuenzel, H.; Gulia, M.; Meglio, D.; Lugli, P.

    1996-01-01

    The dynamics of electrons in GaInAs/AlInAs quantum wells is studied after excitation from the n=1 to the n=2 conduction subband. Femtosecond pump-probe experiments demonstrate for the first time athermal distributions of n=1 electrons on a surprisingly long time scale of 2ps. Thermalization involves intersubband scattering of excited electrons via optical phonon emission with a time constant of 1ps and intrasubband Coulomb and phonon scattering. Ensemble Monte Carlo simulations show that the slow electron equilibration results from Pauli blocking and screening of carrier-carrier scattering. copyright 1996 The American Physical Society

  18. Ultrafast carrier dynamics in Br.sup.+./sup.-bombarded InP studied by time-resolved terahertz spectroscopy

    Czech Academy of Sciences Publication Activity Database

    Němec, Hynek; Fekete, Ladislav; Kadlec, Filip; Kužel, Petr

    2008-01-01

    Roč. 78, č. 23 (2008), 235206/1-235206/7 ISSN 1098-0121 R&D Projects: GA MŠk LC512 Institutional research plan: CEZ:AV0Z10100520 Keywords : InP * carrier lifetime * carrier mobility * ultrafast * ion-bombardment * terahertz Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.322, year: 2008

  19. 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.

  20. Ultrafast carrier dynamics in a p-type GaN wafer under different carrier distributions

    Science.gov (United States)

    Fang, Yu; Yang, Junyi; Yang, Yong; Wu, Xingzhi; Xiao, Zhengguo; Zhou, Feng; Song, Yinglin

    2016-02-01

    The dependence of the carrier distribution on photoexcited carrier dynamics in a p-type Mg-doped GaN (GaN:Mg) wafer were systematically measured by femtosecond transient absorption (TA) spectroscopy. The homogeneity of the carrier distribution was modified by tuning the wavelength of the UV pulse excitation around the band gap of GaN:Mg. The TA kinetics appeared to be biexponential for all carrier distributions, and only the slower component decayed faster as the inhomogeneity of the carrier distribution increased. It was concluded that the faster component (50-70 ps) corresponded to the trap process of holes by the Mg acceptors, and the slower component (150-600 ps) corresponded to the combination of non-radiative surface recombination and intrinsic carrier recombination via dislocations. Moreover, the slower component increased gradually with the incident fluence due to the saturation of surface states.

  1. Ultrafast Doublon Dynamics in Photoexcited 1 T -TaS2

    Science.gov (United States)

    Ligges, M.; Avigo, I.; Golež, D.; Strand, H. U. R.; Beyazit, Y.; Hanff, K.; Diekmann, F.; Stojchevska, L.; Kalläne, M.; Zhou, P.; Rossnagel, K.; Eckstein, M.; Werner, P.; Bovensiepen, U.

    2018-04-01

    Strongly correlated materials exhibit intriguing properties caused by intertwined microscopic interactions that are hard to disentangle in equilibrium. Employing nonequilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1 T -Ta S2 , we identify a spectroscopic signature of doubly occupied sites (doublons) that reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on timescales of electronic hopping ℏ/J ≈14 fs . Despite strong electron-phonon coupling, the dynamics can be explained by purely electronic effects captured by the single-band Hubbard model under the assumption of weak hole doping, in agreement with our static sample characterization. This sensitive interplay of static doping and vicinity to the metal-insulator transition suggests a way to modify doublon relaxation on the few-femtosecond timescale.

  2. Computational Benchmarking for Ultrafast Electron Dynamics: Wave Function Methods vs Density Functional Theory.

    Science.gov (United States)

    Oliveira, Micael J T; Mignolet, Benoit; Kus, Tomasz; Papadopoulos, Theodoros A; Remacle, F; Verstraete, Matthieu J

    2015-05-12

    Attosecond electron dynamics in small- and medium-sized molecules, induced by an ultrashort strong optical pulse, is studied computationally for a frozen nuclear geometry. The importance of exchange and correlation effects on the nonequilibrium electron dynamics induced by the interaction of the molecule with the strong optical pulse is analyzed by comparing the solution of the time-dependent Schrödinger equation based on the correlated field-free stationary electronic states computed with the equationof-motion coupled cluster singles and doubles and the complete active space multi-configurational self-consistent field methodologies on one hand, and various functionals in real-time time-dependent density functional theory (TDDFT) on the other. We aim to evaluate the performance of the latter approach, which is very widely used for nonlinear absorption processes and whose computational cost has a more favorable scaling with the system size. We focus on LiH as a toy model for a nontrivial molecule and show that our conclusions carry over to larger molecules, exemplified by ABCU (C10H19N). The molecules are probed with IR and UV pulses whose intensities are not strong enough to significantly ionize the system. By comparing the evolution of the time-dependent field-free electronic dipole moment, as well as its Fourier power spectrum, we show that TD-DFT performs qualitatively well in most cases. Contrary to previous studies, we find almost no changes in the TD-DFT excitation energies when excited states are populated. Transitions between states of different symmetries are induced using pulses polarized in different directions. We observe that the performance of TD-DFT does not depend on the symmetry of the states involved in the transition.

  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. An ultrafast programmable electrical tester for enabling time-resolved, sub-nanosecond switching dynamics and programming of nanoscale memory devices

    Science.gov (United States)

    Shukla, Krishna Dayal; Saxena, Nishant; Manivannan, Anbarasu

    2017-12-01

    Recent advancements in commercialization of high-speed non-volatile electronic memories including phase change memory (PCM) have shown potential not only for advanced data storage but also for novel computing concepts. However, an in-depth understanding on ultrafast electrical switching dynamics is a key challenge for defining the ultimate speed of nanoscale memory devices that demands for an unconventional electrical setup, specifically capable of handling extremely fast electrical pulses. In the present work, an ultrafast programmable electrical tester (PET) setup has been developed exceptionally for unravelling time-resolved electrical switching dynamics and programming characteristics of nanoscale memory devices at the picosecond (ps) time scale. This setup consists of novel high-frequency contact-boards carefully designed to capture extremely fast switching transient characteristics within 200 ± 25 ps using time-resolved current-voltage measurements. All the instruments in the system are synchronized using LabVIEW, which helps to achieve various programming characteristics such as voltage-dependent transient parameters, read/write operations, and endurance test of memory devices systematically using short voltage pulses having pulse parameters varied from 1 ns rise/fall time and 1.5 ns pulse width (full width half maximum). Furthermore, the setup has successfully demonstrated strikingly one order faster switching characteristics of Ag5In5Sb60Te30 (AIST) PCM devices within 250 ps. Hence, this novel electrical setup would be immensely helpful for realizing the ultimate speed limits of various high-speed memory technologies for future computing.

  5. Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics

    Science.gov (United States)

    Wang, Huihui; Bokarev, Sergey I.; Aziz, Saadullah G.; Kühn, Oliver

    2017-08-01

    Recent developments in attosecond spectroscopy yield access to the correlated motion of electrons on their intrinsic timescales. 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 timescale. 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→3d) excited states of a prototypical Fe(II) complex. This process occurs on a timescale, which is faster than that of Auger decay (∼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 control by soft X-ray light.

  6. Ultra-fast bright field and fluorescence imaging of the dynamics of micrometer-sized objects

    Science.gov (United States)

    Chen, Xucai; Wang, Jianjun; Versluis, Michel; de Jong, Nico; Villanueva, Flordeliza S.

    2013-06-01

    High speed imaging has application in a wide area of industry and scientific research. In medical research, high speed imaging has the potential to reveal insight into mechanisms of action of various therapeutic interventions. Examples include ultrasound assisted thrombolysis, drug delivery, and gene therapy. Visual observation of the ultrasound, microbubble, and biological cell interaction may help the understanding of the dynamic behavior of microbubbles and may eventually lead to better design of such delivery systems. We present the development of a high speed bright field and fluorescence imaging system that incorporates external mechanical waves such as ultrasound. Through collaborative design and contract manufacturing, a high speed imaging system has been successfully developed at the University of Pittsburgh Medical Center. We named the system "UPMC Cam," to refer to the integrated imaging system that includes the multi-frame camera and its unique software control, the customized modular microscope, the customized laser delivery system, its auxiliary ultrasound generator, and the combined ultrasound and optical imaging chamber for in vitro and in vivo observations. This system is capable of imaging microscopic bright field and fluorescence movies at 25 × 106 frames per second for 128 frames, with a frame size of 920 × 616 pixels. Example images of microbubble under ultrasound are shown to demonstrate the potential application of the system.

  7. Ultrafast dynamics of photoexcited charge and spin currents in semiconductor nanostructures

    Science.gov (United States)

    Meier, Torsten; Pasenow, Bernhard; Duc, Huynh Thanh; Vu, Quang Tuyen; Haug, Hartmut; Koch, Stephan W.

    2007-02-01

    Employing the quantum interference among one- and two-photon excitations induced by ultrashort two-color laser pulses it is possible to generate charge and spin currents in semiconductors and semiconductor nanostructures on femtosecond time scales. Here, it is reviewed how the excitation process and the dynamics of such photocurrents can be described on the basis of a microscopic many-body theory. Numerical solutions of the semiconductor Bloch equations (SBE) provide a detailed description of the time-dependent material excitations. Applied to the case of photocurrents, numerical solutions of the SBE for a two-band model including many-body correlations on the second-Born Markov level predict an enhanced damping of the spin current relative to that of the charge current. Interesting effects are obtained when the scattering processes are computed beyond the Markovian limit. Whereas the overall decay of the currents is basically correctly described already within the Markov approximation, quantum-kinetic calculations show that memory effects may lead to additional oscillatory signatures in the current transients. When transitions to coupled heavy- and light-hole valence bands are incorporated into the SBE, additional charge and spin currents, which are not described by the two-band model, appear.

  8. Ultrafast vibronic dynamics of dye molecules studied by the induced grating method

    International Nuclear Information System (INIS)

    Liu, C.H.; Troeger, P.; Laubereau, A.

    1985-08-01

    Previous work on transient polarization spectroscopy applying the induced grating technique concentrated on the time scale > 10 -11 s. Only one earlier study on a shorter time scale showed the occurrence of the so-called coherence peak without a detailed explanation for this phenomena. We report new theoretical and experimental data on a polarization effect that occurs in the nonlinear Rayleigh scattering of delayed probing pulses from induced population gratings. The periodic population changes are generated by two synchronized pumping pulses of the same frequency. Model calculations are presented, which carefully evaluate the orientational distribution and give quantitative information on the scattering signal for various polarization conditions. The scattering mechanism for the coherence peak is explained as a two step process with one photon absorption and emission process; it depends on the vibronic relaxation of the terminating level in the excited electronic state. Experimental results are reported for the vibrational and orientational relaxation times. For example values of tausub(v)=0.2+-0.2 ps and tausub(v)=0.8+-0.3 ps are measured respectively for Rhodamine 6G in ethanol and phenoxazone 9 in dioxane. Our three-beam transient grating technique under general polarization conditions can be used for the study of a variety of dynamic processes of molecules in the excited electronic or ground state. An important advantage compared to nonlinear absorption or induced dichroism techniques is that the scattering method avoids undesirable background signals. (author)

  9. Ultrafast spectroscopy of biological photoreceptors

    NARCIS (Netherlands)

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

    2007-01-01

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

  10. Ultrafast electron dynamics at alkali/ice structures adsorbed on a metal surface

    International Nuclear Information System (INIS)

    Meyer, Michael

    2011-01-01

    The goal of this work is to study the interaction between excess electrons in water ice structures adsorbed on metal surfaces and other charged or neutral species, like alkali ions, or chemically reactive molecules, like chlorofluorocarbons (CFC), respectively. The excess electrons in the ice can interact with the ions directly or indirectly via the hydrogen bonded water molecules. In both cases the presence of the alkali influences the population, localization, and lifetime of electronic states of excess electrons in the ice adlayer. These properties are of great relevance when considering the highly reactive character of the excess electrons, which can mediate chemical reactions by dissociative electron attachment (DEA). The influence of alkali adsorption on electron solvation and transfer dynamics in ice structures is investigated for two types of adsorption configurations using femtosecond time-resolved two-photon photoelectron spectroscopy. In the first system alkali atoms are coadsorbed on top of a wetting amorphous ice film adsorbed on Cu(111). At temperatures between 60 and 100 K alkali adsorption leads to the formation of positively charged alkali ions at the ice/vacuum interface. The interaction between the alkali ions at the surface and the dipole moments of the surrounding water molecules results in a reorientation of the water molecules. As a consequence new electron trapping sites, i.e. at local potential minima, are formed. Photoinjection of excess electrons into these alkali-ion covered amorphous ice layers, results in the trapping of a solvated electron at an alkali-ion/water complex. In contrast to solvation in pure amorphous ice films, where the electrons are located in the bulk of the ice layer, solvated electrons at alkali-ion/water complexes are located at the ice/vacuum interface. They exhibit lifetimes of several picoseconds and show a fast energetic stabilization. With ongoing solvation, i.e. pump-probe time delay, the electron transfer is

  11. 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.

  12. 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

  13. PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

    Science.gov (United States)

    Kono, Junichiro

    2013-02-01

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

  14. Self-organized plasmonic metasurfaces for all-optical modulation

    Science.gov (United States)

    Della Valle, G.; Polli, D.; Biagioni, P.; Martella, C.; Giordano, M. C.; Finazzi, M.; Longhi, S.; Duò, L.; Cerullo, G.; Buatier de Mongeot, F.

    2015-06-01

    We experimentally demonstrate a self-organized metasurface with a polarization dependent transmittance that can be dynamically controlled by optical means. The configuration consists of tightly packed plasmonic nanowires with a large dispersion of width and height produced by the defocused ion-beam sputtering of a thin gold film supported on a silica glass. Our results are quantitatively interpreted according to a theoretical model based on the thermomodulational nonlinearity of gold and a finite-element numerical analysis of the absorption and scattering cross-sections of the nanowires. We found that the polarization sensitivity of the metasurface can be strongly enhanced by pumping with ultrashort laser pulses, leading to potential applications in ultrafast all-optical modulation and switching of light.

  15. Modern plasmonics

    CERN Document Server

    Maradudin, Alexei A; Barnes, William L

    2014-01-01

    Plasmonics is entering the curriculum of many universities, either as a stand alone subject, or as part of some course or courses. Nanotechnology institutes have been, and are being, established in universities, in which plasmonics is a significant topic of research. Modern Plasmonics book offers a comprehensive presentation of the properties of surface plasmon polaritons, in systems of different structures and various natures, e.g. active, nonlinear, graded, theoretical/computational and experimental techniques for studying them, and their use in a variety of applications. Contains materia

  16. 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.

  17. 2D heterodyne-detected sum frequency generation study on the ultrafast vibrational dynamics of H{sub 2}O and HOD water at charged interfaces

    Energy Technology Data Exchange (ETDEWEB)

    Inoue, Ken-ichi; Singh, Prashant C. [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Nihonyanagi, Satoshi; Tahara, Tahei, E-mail: tahei@riken.jp [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Ultrafast Spectroscopy Research Team, RIKEN Center for Advanced Photonics, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Yamaguchi, Shoichi [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 (Japan); Department of Applied Chemistry, Saitama University, 255 Shimo-Okubo, Saitama 338-8570 (Japan)

    2015-06-07

    Two-dimensional heterodyne-detected vibrational sum-frequency generation (2D HD-VSFG) spectroscopy is applied to study the ultrafast vibrational dynamics of water at positively charged aqueous interfaces, and 2D HD-VSFG spectra of cetyltrimethylammonium bromide (CTAB)/water interfaces in the whole hydrogen-bonded OH stretch region (3000 cm{sup −1} ≤ ω{sub pump} ≤ 3600 cm{sup −1}) are measured. 2D HD-VSFG spectrum of the CTAB/isotopically diluted water (HOD-D{sub 2}O) interface exhibits a diagonally elongated bleaching lobe immediately after excitation, which becomes round with a time constant of ∼0.3 ps due to spectral diffusion. In contrast, 2D HD-VSFG spectrum of the CTAB/H{sub 2}O interface at 0.0 ps clearly shows two diagonal peaks and their cross peaks in the bleaching region, corresponding to the double peaks observed at 3230 cm{sup −1} and 3420 cm{sup −1} in the steady-state HD-VSFG spectrum. Horizontal slices of the 2D spectrum show that the relative intensity of the two peaks of the bleaching at the CTAB/H{sub 2}O interface gradually change with the change of the pump frequency. We simulate the pump-frequency dependence of the bleaching feature using a model that takes account of the Fermi resonance and inhomogeneity of the OH stretch vibration, and the simulated spectra reproduce the essential features of the 2D HD-VSFG spectra of the CTAB/H{sub 2}O interface. The present study demonstrates that heterodyne detection of the time-resolved VSFG is critically important for studying the ultrafast dynamics of water interfaces and for unveiling the underlying mechanism.

  18. Hybrid plasmonic systems: from optical transparencies to strong coupling and entanglement

    Science.gov (United States)

    Gray, Stephen K.

    2018-02-01

    Classical electrodynamics and quantum mechanical models of quantum dots and molecules interacting with plasmonic systems are discussed. Calculations show that just one quantum dot interacting with a plasmonic system can lead to interesting optical effects, including optical transparencies and more general Fano resonance features that can be tailored with ultrafast laser pulses. Such effects can occur in the limit of moderate coupling between quantum dot and plasmonic system. The approach to the strong coupling regime is also discussed. In cases with two or more quantum dots within a plasmonic system, the possibility of quantum entanglement mediated through the dissipative plasmonic structure arises.

  19. Dynamics of coupled plasmon polariton wave packets excited at a subwavelength slit in optically thin metal films

    Science.gov (United States)

    Wang, Lei-Ming; Zhang, Lingxiao; Seideman, Tamar; Petek, Hrvoje

    2012-10-01

    We study by numerical simulations the excitation and propagation dynamics of coupled surface plasmon polariton (SPP) wave packets (WPs) in optically thin Ag films and a bulk Ag/vacuum interface under the illumination of a subwavelength slit by 400 nm continuous wave (cw) and femtosecond pulsed light. The generated surface fields include contributions from both SPPs and quasicylindrical waves, which dominate in different regimes. We explore aspects of the coupled SPP modes in Ag thin films, including symmetry, propagation, attenuation, and the variation of coupling with incident angle and film thickness. Simulations of the electromagnetic transients initiated with femtosecond pulses reveal new features of coupled SPP WP generation and propagation in thin Ag films. Our results show that, under pulsed excitation, the SPP modes in an Ag thin film break up into two distinct bound surface wave packets characterized by marked differences in symmetries, group velocities, attenuation lengths, and dispersion properties. The nanometer spatial and femtosecond temporal scale excitation and propagation dynamics of the coupled SPP WPs are revealed in detail by movies recording the evolution of their transient field distributions.

  20. Few-cycle surface plasmon enhanced electron acceleration

    International Nuclear Information System (INIS)

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

    2010-01-01

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

  1. Time-resolved detection of surface plasmon polaritons with a scanning tunneling microscope

    DEFF Research Database (Denmark)

    Keil, Ulrich Dieter Felix; Ha, T.; Jensen, Jacob Riis

    1998-01-01

    We present the time-resolved detection of surface plasmon polaritons with an STM. The results indicate that the time resolved signal is due to rectification of coherently superimposed plasmon voltages. The comparison with differential reflectivity measurements shows that the tip itself influences...... the decay of the plasmon-field coherence. Generation of the measured signal at the tunneling junction offers the possibility to observe ultrafast effects with a spatial resolution determined by the tunneling junction...

  2. 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.

  3. 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.

  4. Dye gain gold NW array of surface plasmon polariton waveguide

    Directory of Open Access Journals (Sweden)

    Jun Zhu

    Full Text Available Plasmon lasers can support ultrasmall mode confinement and ultrafast dynamics with device feature sizes below the diffraction limit. At present in the single visible light frequency, the optical gain method of constraint SPP on metal nanowires structure reported less. We design the gold nanowire array structure, consisting of PMMA and R6G dye molecules as gain, by 488 nm pump in the middle of the nanowires position for wide range of light, use symmetry broken overcome that momentum does not match the photonic and SPP energy conversion. Theoretical analysis shows that dyes provide coherent optical feedback, resulting in nanowires face will observe laser properties of surface plasmons. Feature analysis: the incident light and pump joint strength is greater than the sum of strength which is the incident light, pump respectively. Under the effect of dye molecules gain effective, length of SPP transmission can increase 1 µm. The results achieved in a single optical frequency of stimulated radiation, application of dye optical gain can achieve continuous gain effect. This is for the future development of plasma amplifier and the wavelength laser. Keywords: SPP, Stimulated radiation, Gold nanowires array, Dye molecules

  5. Ultrafast photoinduced structure phase transition in antimony single crystals

    NARCIS (Netherlands)

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

    2009-01-01

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

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

    International Nuclear Information System (INIS)

    Rajkovic, Ivan

    2008-01-01

    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.)

  7. 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.)

  8. Hydrodynamic theory for quantum plasmonics: Linear-response dynamics of the inhomogeneous electron gas

    DEFF Research Database (Denmark)

    Yan, Wei

    2015-01-01

    We investigate the hydrodynamic theory of metals, offering systematic studies of the linear-response dynamics for an inhomogeneous electron gas. We include the quantum functional terms of the Thomas-Fermi kinetic energy, the von Weizsa¨cker kinetic energy, and the exchange-correlation Coulomb...... energies under the local density approximation. The advantages, limitations, and possible improvements of the hydrodynamic theory are transparently demonstrated. The roles of various parameters in the theory are identified. We anticipate that the hydrodynamic theory can be applied to investigate the linear...... response of complex metallic nanostructures, including quantum effects, by adjusting theory parameters appropriately....

  9. Plasmonic sensing

    DEFF Research Database (Denmark)

    Mogensen, Klaus Bo

    2015-01-01

    Plasmonic sensors typically rely on detection of changes in the refractive index of the surrounding medium. Here, an alternative approach is reported based on electrical surface screening and controlled dissolution of ultrasmall silver nanoparticles (NPs; R ... in the plasmon band. This is demonstrated by using the strong nucleophiles, cyanide and cysteamine, as ligands. The “dissolution paths” in terms of peak wavelength and amplitude shifts differ significantly between different types of analytes, which are suggested as a means to obtain selectivity of the detection...... that cannot be obtained by traditional refractive index sensing, without the use of bioprobes. A simple modified Drude model is used to account for shifts in the plasmon band position due to electrical charging. Here, a screening parameter is introduced in the expression for the free electron density...

  10. Light-matter Interactions in Semiconductors and Metals: From Nitride Optoelectronics to Quantum Plasmonics

    Science.gov (United States)

    Narang, Prineha

    This thesis puts forth a theory-directed approach coupled with spectroscopy aimed at the discovery and understanding of light-matter interactions in semiconductors and metals. The first part of the thesis presents the discovery and development of Zn-IV nitride materials. The commercial prominence in the optoelectronics industry of tunable semiconductor alloy materials based on nitride semiconductor devices, specifically InGaN, motivates the search for earth-abundant alternatives for use in efficient, high-quality optoelectronic devices. II-IV-N2 compounds, which are closely related to the wurtzite-structured III-N semiconductors, have similar electronic and optical properties to InGaN namely direct band gaps, high quantum efficiencies and large optical absorption coefficients. The choice of different group II and group IV elements provides chemical diversity that can be exploited to tune the structural and electronic properties through the series of alloys. The first theoretical and experimental investigation of the ZnSnxGe1--xN2 series as a replacement for III-nitrides is discussed here. The second half of the thesis shows ab-initio calculations for surface plasmons and plasmonic hot carrier dynamics. Surface plasmons, electromagnetic modes confined to the surface of a conductor-dielectric interface, have sparked renewed interest because of their quantum nature and their broad range of applications. The decay of surface plasmons is usually a detriment in the field of plasmonics, but the possibility to capture the energy normally lost to heat would open new opportunities in photon sensors, energy conversion devices and switching. A theoretical understanding of plasmon-driven hot carrier generation and relaxation dynamics in the ultrafast regime is presented here. Additionally calculations for plasmon-mediated upconversion as well as an energy-dependent transport model for these non-equilibrium carriers are shown. Finally, this thesis gives an outlook on the

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

    Science.gov (United States)

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

    2015-03-01

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

  12. Ultrafast photo-initiated molecular quantum dynamics in the DNA dinucleotide d(ApG) revealed by broadband transient absorption spectroscopy.

    Science.gov (United States)

    Stuhldreier, Mayra C; Temps, Friedrich

    2013-01-01

    The ultrafast photo-initiated quantum dynamics of the adenine-guanine dinucleotide d(ApG) in aqueous solution (pH 7) has been studied by femtosecond time-resolved spectroscopy after excitation at lambda = 260 nm. The results reveal a hierarchy of processes on time scales from tau 100 ps. Characteristic spectro-temporal signatures are observed indicating the transformation of the molecules in the electronic relaxation from the photo-excited state to a long-lived exciplex. In particular, broadband UV/VIS excited-state absorption (ESA) measurements detected a distinctive absorption by the excited dinucleotide around lambda = 335 nm, approximately 0.5 eV to the blue compared to the maximum of the broad and unstructured ESA spectrum after excitation of an equimolar mixture of the mononucleotides dAMP and dGMP. A similar feature has been identified as signature of the excimer in the dynamics of the adenine dinucleotide d(ApA). The lifetime of the d(ApG) exciplex was found to be tau = 124 +/- 4 ps both from the ESA decay time and from the ground-state recovery time, far longer than the sub-picosecond lifetimes of excited dAMP or dGMP. Fluorescence-time profiles measured by the up-conversion technique indicate that the exciplex state is reached around approximately 6 ps after excitation. Very weak residual fluorescence at longer times red-shifted to the emission from the photo-excited state shows that the exciplex is almost optically dark, but still has enough oscillator strength to give rise to the dual fluorescence of the dinucleotide in the static fluorescence spectrum.

  13. Ultrafast spectral dynamics of dual-color-soliton intracavity collision in a mode-locked fiber laser

    Science.gov (United States)

    Wei, Yuan; Li, Bowen; Wei, Xiaoming; Yu, Ying; Wong, Kenneth K. Y.

    2018-02-01

    The single-shot spectral dynamics of dual-color-soliton collisions inside a mode-locked laser is experimentally and numerically investigated. By using the all-optically dispersive Fourier transform, we spectrally unveil the collision-induced soliton self-reshaping process, which features dynamic spectral fringes over the soliton main lobe, and the rebuilding of Kelly sidebands with wavelength drifting. Meanwhile, the numerical simulations validate the experimental observation and provide additional insights into the physical mechanism of the collision-induced spectral dynamics from the temporal domain perspective. It is verified that the dynamic interference between the soliton and the dispersive waves is responsible for the observed collision-induced spectral evolution. These dynamic phenomena not only demonstrate the role of dispersive waves in the sophisticated soliton interaction inside the laser cavity, but also facilitate a deeper understanding of the soliton's inherent stability.

  14. 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

  15. Progress in Ultrafast Intense Laser Science II

    CERN Document Server

    Yamanouchi, Kaoru; Agostini, Pierre; Ferrante, Gaetano

    2007-01-01

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

  16. Generation of attosecond electron packets via conical surface plasmon electron acceleration

    Science.gov (United States)

    Greig, S. R.; Elezzabi, A. Y.

    2016-01-01

    We present a method for the generation of high kinetic energy attosecond electron packets via magnetostatic and aperture filtering of conical surface plasmon (SP) accelerated electrons. The conical SP waves are excited by coupling an ultrafast radially polarized laser beam to a conical silica lens coated with an Ag film. Electromagnetic and particle tracking models are employed to characterize the ultrafast electron packets. PMID:26764129

  17. On-chip plasmon-induced transparency based on plasmonic coupled nanocavities.

    Science.gov (United States)

    Zhu, Yu; Hu, Xiaoyong; Yang, Hong; Gong, Qihuang

    2014-01-17

    On-chip plasmon-induced transparency offers the possibility of realization of ultrahigh-speed information processing chips. Unfortunately, little experimental progress has been made to date because it is difficult to obtain on-chip plasmon-induced transparency using only a single meta-molecule in plasmonic circuits. Here, we report a simple and efficient strategy to realize on-chip plasmon-induced transparency in a nanoscale U-shaped plasmonic waveguide side-coupled nanocavity pair. High tunability in the transparency window is achieved by covering the pair with different organic polymer layers. It is possible to realize ultrafast all-optical tunability based on pump light-induced refractive index change of a graphene cover layer. Compared with previous reports, the overall feature size of the plasmonic nanostructure is reduced by more than three orders of magnitude, while ultrahigh tunability of the transparency window is maintained. This work also provides a superior platform for the study of the various physical effects and phenomena of nonlinear optics and quantum optics.

  18. Numerical study of propagation properties of surface plasmon polaritons in nonlinear media

    KAUST Repository

    Sagor, Rakibul Hasan

    2016-03-29

    We present a time-domain algorithm for simulating nonlinear propagation of surface plasmon polaritons (SPPs) in chalcogenide glass. Due to the high non-linearity property and strong dispersion and confinement chalcogenide glasses are widely known as ultrafast nonlinear materials. We have used the finite difference time domain (FDTD) method to develop the simulation algorithm for the current analysis. We have modeled the frequency dependent dispersion properties and third order nonlinearity property of chalcogenide glass utilizing the general polarization algorithm merged in the auxiliary differential equation (ADE) method. The propagation dynamics of the whole structure with and without third order nonlinearity property of chalcogenide glass have been simulated and the effect of nonlinearity on the propagation properties of SPP has been investigated. © 2016 EDP Sciences, SIF, Springer-Verlag Berlin Heidelberg.

  19. Nanoscale and femtosecond optical autocorrelator based on a single plasmonic nanostructure

    International Nuclear Information System (INIS)

    Melentiev, P N; Afanasiev, A E; Balykin, V I; Tausenev, A V; Konyaschenko, A V; Klimov, V V

    2014-01-01

    We demonstrated a nanoscale size, ultrafast and multiorder optical autocorrelator with a single plasmonic nanostructure for measuring the spatio-temporal dynamics of femtosecond laser light. As a nanostructure, we use a split hole resonator (SHR), which was made in an aluminium nanofilm. The Al material yields the fastest response time (100 as). The SHR nanostructure ensures a high nonlinear optical efficiency of the interaction with laser radiation, which leads to (1) the second, (2) the third harmonics generation and (3) the multiphoton luminescence, which, in turn, are used to perform multi-order autocorrelation measurements. The nano-sized SHR makes it possible to conduct autocorrelation measurements (i) with a subwavelength spatial resolution and (ii) with no significant influence on the duration of the laser pulse. The time response realized by the SHR nanostructure is about 10 fs. (letter)

  20. Mechanisms of ultrafast fluorescence depletion spectroscopy and applications to measure slovation dynamics of coummarin 153 in methanol

    International Nuclear Information System (INIS)

    Yang Songqiu; Liu Jianyong; Zhou Panwang; Chen Junsheng; Han Keli; He Guozhong

    2012-01-01

    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: ► Mechanisms of subpicosecond fluorescence depletion spectroscopy. ► Quasi-continuous model was used to describe the solvational relaxation. ► The solvation dynamics of coumarin 153 in methanol has been measured.

  1. Multi-mode-multi-state quantum dynamics of key five-membered heterocycles: spectroscopy and ultrafast internal conversion

    International Nuclear Information System (INIS)

    Koeppel, H.; Gromov, E.V.; Trofimov, A.B.

    2004-01-01

    The multi-mode and multi-state vibronic interactions in the heterocyclic molecules furan, pyrrole, thiophene and their radical cations are investigated theoretically, employing a linear vibronic coupling scheme. The underlying system parameters are determined from large-scale ab initio computations. Previous time-independent dynamical calculations on the radical cations are extended by wave-packet propagations (using the MCTDH method) confirming the strong nonadiabatic coupling effects. For the singlet excited states of furan and thiophene quantum dynamical calculations are presented which go beyond the two-state approximation frequently applied in the literature. The characteristic spectral structures are well reproduced, especially in the case of furan. The implications of these results on the photochemical reaction dynamics of these species are discussed

  2. 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.

  3. Ultrafast dynamics of hydrophilic carbonyl carotenoids - Relation between structure and excited-state properties in polar solvents

    Czech Academy of Sciences Publication Activity Database

    Chábera, P.; Fuciman, M.; Naqvi, K.R.; Polívka, Tomáš

    2010-01-01

    Roč. 373, 1-2 (2010), s. 56-64 ISSN 0301-0104 Institutional research plan: CEZ:AV0Z50510513 Keywords : hydrophilic carotenoids * excited-state dynamics * charge-transfer state Subject RIV: BO - Biophysics Impact factor: 2.017, year: 2010

  4. 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.

  5. 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

    The anionic wild-type Green Fluorescent Protein (GFP) chromophore defines the 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 cha...

  6. Resolving electrical conductivities from collisionally damped plasmons in isochorically heated warm dense aluminum

    Energy Technology Data Exchange (ETDEWEB)

    Sperling, P. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Fletcher, L. B. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Chung, H. -K. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Gamboa, E. J. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Lee, H. J. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Omarbakiyeva, Y. [International IT Univ., Almaty (Kazakhstan); Univ. Rostock (Germany); Reinholz, H. [Univ. Rostock (Germany); ; Univ. of Western Australia, Crawley, WA (Australia); Ropke, G. [Univ. Rostock (Germany); Rosmej, S. [Univ. Rostock (Germany); Zastrau, U. [European XFEL, Hamburg (Germany); Glenzer, S. H. [SLAC National Accelerator Lab., Menlo Park, CA (United States)

    2016-03-29

    We measure the highly-resolved inelastic x-ray scattering spectrum of isochorically ultrafast heated aluminum. In the x-ray forward scattering spectra the electron temperature could be measured from the down- and upshifted plasmon, where the electron density of ne = 1:8 1023 cm3 is known a priori. We have studied the plasmon damping by applying electron-particle collision models beyond the Born approximation determining the electrical conductivity of warm dense aluminum.

  7. Measurements of ultrafast dynamics in a superconductor, YBa{sub 2}Cu{sub 3}O{sub 7-{delta}}, and a semiconductor, GaSb

    Energy Technology Data Exchange (ETDEWEB)

    Smith, D.C

    1998-07-01

    Measurements of ultrafast dynamics in GaSb and YBa{sub 2}Cu{sub 3}O{sub 7-}{delta} (YBCO) have been made with 1 ps or better resolution using time-resolved optical spectroscopy; pump-probe transmission and reflection, and time-resolved Raman spectroscopy. The study of carrier dynamics in GaSb focuses on the scattering of electrons between the F and L conduction band valleys by zone-boundary phonons {gamma}-L scattering in bulk GaSb and a GaSb/AlSb multiple quantum well sample has been investigated in a series of room temperature degenerate pump-probe transmission experiments with near bandgap excitation. There is a clear difference in the dynamics between experiments where electrons excited in {gamma} can/cannot directly scatter to the L valleys. Ensemble Monte Carlo simulations are presented which are in good agreement with the experiments. The strength of {gamma}-L scattering is quantified using an intervalley deformation potential for a single 'effective' zone-boundary phonon (25meV). A deformation potential of 3.6{+-}0.4 eVA{sup -1} is consistent with both the bulk and quantum well results. The temperature dependence of the dynamics in bulk GaSb is also explored. Time-resolved Raman spectroscopy (E{sub laser}{approx}E{sub 0}+{delta}{sub 0}) has been used to study {gamma}-F scattering by measuring the dynamics of phonons emitted during intravalley scattering. All the measured non-equilibrium phonon populations have a component whose lifetime is greater the phonons anharmonic lifetime. This component is interpreted as following the return of electrons from L to {gamma}. Comparison of the results with the pump-probe experiments indicates that this return is slowed by blocking of {gamma} states. The study of YBCO consists of pump-probe transmission and reflection measurements of thin films and single crystals in both the normal and superconducting states. Measurements of dynamics have been made with a wide range of probe energies lower than in any

  8. Ultrafast Multi-Dimensional Infrared Vibrational Echo Spectroscopy of Molecular Dynamics on Surfaces and in Bulk Systems

    Science.gov (United States)

    2012-02-28

    dimethylsulfoxide ( DMSO ). When chloroform is dissolved in a mixed solvent consisting of acetone and DMSO , both types of hydrogen bonded complexes exist. The...transition (negative) in the 2D IR spectrum. Also, line shape distortions caused by solvent background absorption and finite pulse durations do not affect...conditions as  = 7  1 ps. This is the first direct measurement of hydrogen bond exchange. b. Solute- Solvent Complex Switching Dynamics3 Hydrogen

  9. Ultrafast Multi-Dimentional Infrared Vibrational Echo Spectroscopy of Molecular Dynamics on Surfaces and in Bulk Systems

    Science.gov (United States)

    2012-02-28

    dimethylsulfoxide ( DMSO ). When chloroform is dissolved in a mixed solvent consisting of acetone and DMSO , both types of hydrogen bonded complexes exist. The...transition (negative) in the 2D IR spectrum. Also, line shape distortions caused by solvent background absorption and finite pulse durations do not affect...conditions as  = 7  1 ps. This is the first direct measurement of hydrogen bond exchange. b. Solute- Solvent Complex Switching Dynamics3 Hydrogen

  10. Ultrafast carrier dynamics and third-order nonlinear optical properties of AgInS2/ZnS nanocrystals

    Science.gov (United States)

    Yu, Kuai; Yang, Yang; Wang, Junzhong; Tang, Xiaosheng; Xu, Qing-Hua; Wang, Guo Ping

    2018-06-01

    Broad photoluminescence (PL) emission, a large Stokes shift and extremely long-lived radiative lifetimes are the characteristics of ternary I–III–VI semiconductor nanocrystals (NCs), such as CuInS2 and AgInS2. However, the lack of understanding regarding the intriguing PL mechanisms and photo-carrier dynamics limits their further applications. Here, AgInS2 and AgInS2/ZnS NCs were chemically synthesized and their carrier dynamics were studied by time-resolved PL spectroscopy. The results demonstrated that the surface defect state, which contributed dominantly to the non-radiative decay processes, was effectively passivated through ZnS alloying. Femtosecond transient absorption spectroscopy was also used to investigate the carrier dynamics, revealing the electron storage at the surface state and donor state. Furthermore, the two photon absorption properties of AgInS2 and AgInS2/ZnS NCs were measured using an open-aperture Z-scan technique. The improved third-order nonlinear susceptibility {χ }(3) of AgInS2 through ZnS alloying demonstrates potential application in two photon PL biological imaging.

  11. Optical Detection in Ultrafast Short Wavelength Science

    International Nuclear Information System (INIS)

    Fullagar, Wilfred K.; Hall, Chris J.

    2010-01-01

    A new approach to coherent detection of ionising radiation is briefly motivated and recounted. The approach involves optical scattering of coherent light fields by colour centres in transparent solids. It has significant potential for diffractive imaging applications that require high detection dynamic range from pulsed high brilliance short wavelength sources. It also motivates new incarnations of Bragg's X-ray microscope for pump-probe studies of ultrafast molecular structure-dynamics.

  12. 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.

  13. The significant role of plasmonic effects in femtosecond laser-induced grating fabrication on the nanoscale

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Min; Zhao, Fuli [State Key Laboratory of Optoelectronic Materials and Technologies, Sun Yat-sen University, Guangzhou, 510275 (China); Cheng, Ya; Xu, Zhizhan [State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, P.O. Box 800-211, Shanghai, 201800 (China)

    2013-02-15

    Nowadays, plasmonics aiming at manipulating light beyond the diffraction limit has aroused great interest on account of the promise of nanoscale optical devices. Generally, the ability to break diffraction barrier is achieved via controlling surface plasmons (SPs) on artificial structures as products of human ingenuity. Here, nevertheless, it is demonstrated that in short-pulse laser ablation ultrafast active plasmonic structures spontaneously generate by virtue of plasmonic effects rather than human will. First, with the experimental results on ZnO, Si, and GaAs, explicit evidence is provided for the grating-splitting phenomenon that acts as a direct route for the formation of laser-induced deep-subwavelength gratings. The splitting mechanism can break through the diffraction limit and push laser-induced structures towards the nanoscale. Then, through comprehensive numerical studies based on the viewpoint of plasmonics, it can be confirmed that the grating-splitting phenomenon originates in the conversion of SP modes from the resonant to the nonresonant mode and further to the inphase or antiphase asymmetric mode. In short, plasmonic effects play an important role in ultrafast laser-induced grating splitting towards the nanoscale, which will provide new insights into the mechanisms of ultrafast laser-induced nanostructures. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  14. The significant role of plasmonic effects in femtosecond laser-induced grating fabrication on the nanoscale

    International Nuclear Information System (INIS)

    Huang, Min; Zhao, Fuli; Cheng, Ya; Xu, Zhizhan

    2013-01-01

    Nowadays, plasmonics aiming at manipulating light beyond the diffraction limit has aroused great interest on account of the promise of nanoscale optical devices. Generally, the ability to break diffraction barrier is achieved via controlling surface plasmons (SPs) on artificial structures as products of human ingenuity. Here, nevertheless, it is demonstrated that in short-pulse laser ablation ultrafast active plasmonic structures spontaneously generate by virtue of plasmonic effects rather than human will. First, with the experimental results on ZnO, Si, and GaAs, explicit evidence is provided for the grating-splitting phenomenon that acts as a direct route for the formation of laser-induced deep-subwavelength gratings. The splitting mechanism can break through the diffraction limit and push laser-induced structures towards the nanoscale. Then, through comprehensive numerical studies based on the viewpoint of plasmonics, it can be confirmed that the grating-splitting phenomenon originates in the conversion of SP modes from the resonant to the nonresonant mode and further to the inphase or antiphase asymmetric mode. In short, plasmonic effects play an important role in ultrafast laser-induced grating splitting towards the nanoscale, which will provide new insights into the mechanisms of ultrafast laser-induced nanostructures. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  15. Ultrafast Photodissociation Dynamics of the F State of Sulfur Dioxide by Femtosecond Time-Resolved Pump-Probe Method

    International Nuclear Information System (INIS)

    Zhang Dong-Dong; Ni Qiang; Luo Si-Zuo; Zhang Jing; Liu Hang; Xu Hai-Feng; Jin Ming-Xing; Ding Da-Jun

    2011-01-01

    A femtosecond pump-probe method is employed to study the dissociation dynamics of sulfur dioxide. SO 2 molecules are excited to the F state by absorbing two photons of 267 nm femtosecond laser pulses, and ionized by 400 nm laser pulses at different delay times between the two lasers. Transients of both parent ions (SO + 2 ) and the fragment ions (SO + , S + and O + ) are observed. The SO + 2 transient can be well fitted to a biexponential decay comprising a fast and a slow component of 280 fs and 2.97 ps lifetimes, respectively. The SO + transient consists of two growth components of 270 fs and 2.50 ps. The results clearly show that the F state of SO 2 dissociates along an S-O bond. The transients of S + and O + , however, have different behavior, which consist of a fast growth and a long decay component. A possible mechanism of the fragment formation is discussed to understand the dissociation dynamics of the F state of SO 2 . (atomic and molecular physics)

  16. 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.

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

    KAUST Repository

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

    2015-01-01

    , we establish a second generation of four-dimensional scanning ultrafast electron microscopy (4D S-UEM) and demonstrate the ability to record time-resolved images (snapshots) of material surfaces with 650 fs and ∼5 nm temporal and spatial resolutions

  18. Ab initio multiple spawning dynamics study of dimethylnitramine and dimethylnitramine-Fe complex to model their ultrafast nonadiabatic chemistry.

    Science.gov (United States)

    Bera, Anupam; Ghosh, Jayanta; Bhattacharya, Atanu

    2017-07-28

    Conical intersections are now firmly established to be the key features in the excited electronic state processes of polyatomic energetic molecules. In the present work, we have explored conical intersection-mediated nonadiabatic chemical dynamics of a simple analogue nitramine molecule, dimethylnitramine (DMNA, containing one N-NO 2 energetic group), and its complex with an iron atom (DMNA-Fe). For this task, we have used the ab initio multiple spawning (AIMS) dynamics simulation at the state averaged-complete active space self-consistent field(8,5)/6-31G(d) level of theory. We have found that DMNA relaxes back to the ground (S 0 ) state following electronic excitation to the S 1 excited state [which is an (n,π*) excited state] with a time constant of approximately 40 fs. This AIMS result is in very good agreement with the previous surface hopping-result and femtosecond laser spectroscopy result. DMNA does not dissociate during this fast internal conversion from the S 1 to the S 0 state. DMNA-Fe also undergoes extremely fast relaxation from the upper S 1 state to the S 0 state; however, this relaxation pathway is dissociative in nature. DMNA-Fe undergoes initial Fe-O, N-O, and N-N bond dissociations during relaxation from the upper S 1 state to the ground S 0 state through the respective conical intersection. The AIMS simulation reveals the branching ratio of these three channels as N-N:Fe-O:N-O = 6:3:1 (based on 100 independent simulations). Furthermore, the AIMS simulation reveals that the Fe-O bond dissociation channel exhibits the fastest (time constant 24 fs) relaxation, while the N-N bond dissociation pathway features the slowest (time constant 128 fs) relaxation. An intermediate time constant (30 fs) is found for the N-O bond dissociation channel. This is the first nonadiabatic chemical dynamics study of metal-contained energetic molecules through conical intersections.

  19. Ab initio multiple spawning dynamics study of dimethylnitramine and dimethylnitramine-Fe complex to model their ultrafast nonadiabatic chemistry

    Science.gov (United States)

    Bera, Anupam; Ghosh, Jayanta; Bhattacharya, Atanu

    2017-07-01

    Conical intersections are now firmly established to be the key features in the excited electronic state processes of polyatomic energetic molecules. In the present work, we have explored conical intersection-mediated nonadiabatic chemical dynamics of a simple analogue nitramine molecule, dimethylnitramine (DMNA, containing one N-NO2 energetic group), and its complex with an iron atom (DMNA-Fe). For this task, we have used the ab initio multiple spawning (AIMS) dynamics simulation at the state averaged-complete active space self-consistent field(8,5)/6-31G(d) level of theory. We have found that DMNA relaxes back to the ground (S0) state following electronic excitation to the S1 excited state [which is an (n,π*) excited state] with a time constant of approximately 40 fs. This AIMS result is in very good agreement with the previous surface hopping-result and femtosecond laser spectroscopy result. DMNA does not dissociate during this fast internal conversion from the S1 to the S0 state. DMNA-Fe also undergoes extremely fast relaxation from the upper S1 state to the S0 state; however, this relaxation pathway is dissociative in nature. DMNA-Fe undergoes initial Fe-O, N-O, and N-N bond dissociations during relaxation from the upper S1 state to the ground S0 state through the respective conical intersection. The AIMS simulation reveals the branching ratio of these three channels as N-N:Fe-O:N-O = 6:3:1 (based on 100 independent simulations). Furthermore, the AIMS simulation reveals that the Fe-O bond dissociation channel exhibits the fastest (time constant 24 fs) relaxation, while the N-N bond dissociation pathway features the slowest (time constant 128 fs) relaxation. An intermediate time constant (30 fs) is found for the N-O bond dissociation channel. This is the first nonadiabatic chemical dynamics study of metal-contained energetic molecules through conical intersections.

  20. Molecular plasmonics

    CERN Document Server

    Fritzsche, Wolfgang

    2014-01-01

    Adopting a novel approach, this book provides a unique ""molecular perspective"" on plasmonics, concisely presenting the fundamentals and applications in a way suitable for beginners entering this hot field as well as for experienced researchers and practitioners. It begins by introducing readers to the optical effects that occur at the nanoscale and particularly their modification in the presence of biomolecules, followed by a concise yet thorough overview of the different methods for the actual fabrication of nanooptical materials. Further chapters address the relevant nanooptics, as well as

  1. Plasmonic Encoding

    Science.gov (United States)

    2014-10-06

    Mangelson, B. F.; Schatz, G. C.; and Mirkin, C. A. “ Silver -based Nanodisk Codes,” ACS Nano, 2010, 9, 5446-5452. 6. Zhang, J.; Langille, M. R...Wei, W. D.; Zhang, H.; Schatz, G.; Boey, F.; Mirkin, C. A. “Free Standing Bimetallic Nanorings and Nanoring Arrays Made by On-Wire Lithography (OWL...Mirkin, C. A.; Marks, L. D.; Van Duyne, R. P. “Correlating the Structure and Localized Surface Plasmon Resonance of Single Silver Right Bipyramids

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

    International Nuclear Information System (INIS)

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

    2003-01-01

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

  3. 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.

  4. Imaging the ultrafast Kerr effect, free carrier generation, relaxation and ablation dynamics of Lithium Niobate irradiated with femtosecond laser pulses

    International Nuclear Information System (INIS)

    Garcia-Lechuga, Mario; Siegel, Jan; Hernandez-Rueda, Javier; Solis, Javier

    2014-01-01

    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.

  5. Ultrafast photoinduced carrier dynamics in GaNAs probed using femtosecond time-resolved scanning tunnelling microscopy

    International Nuclear Information System (INIS)

    Terada, Yasuhiko; Aoyama, Masahiro; Kondo, Hiroyuki; Taninaka, Atsushi; Takeuchi, Osamu; Shigekawa, Hidemi

    2007-01-01

    The combination of scanning tunnelling microscopy (STM) with optical excitation using ultrashort laser pulses enables us, in principle, to simultaneously obtain ultimate spatial and temporal resolutions. We have developed the shaken-pulse-pair-excited STM (SPPX-STM) and succeeded in detecting a weak time-resolved tunnelling current signal from a low-temperature-grown GaNAs sample. To clarify the underlying physics in SPPX-STM measurements, we performed optical pump-probe reflectivity measurements with a wavelength-changeable ultrashort-pulse laser. By comparing the results obtained from the two methods with an analysis based on the nonlinear relationship between the photocarrier density and tunnelling current, we obtained a comprehensive explanation that the photocarrier dynamics is reflected in the SPPX-STM signal through the surface photovoltage effect

  6. Optimal laser control of ultrafast photodissociation of I2- in water: Mixed quantum/classical molecular dynamics simulation

    International Nuclear Information System (INIS)

    Nishiyama, Yoshikazu; Kato, Tsuyoshi; Ohtsuki, Yukiyoshi; Fujimura, Yuichi

    2004-01-01

    A linearized optimal control method in combination with mixed quantum/classical molecular dynamics simulation is used for numerically investigating the possibility of controlling photodissociation wave packets of I 2 - in water. Optimal pulses are designed using an ensemble of photodissociation samples, aiming at the creation of localized dissociation wave packets. Numerical results clearly show the effectiveness of the control although the control achievement is reduced with an increase in the internuclear distance associated with a target region. We introduce effective optimal pulses that are designed using a statistically averaged effective dissociation potential, and show that they semiquantitatively reproduce the control achievements calculated by using optimal pulses. The control mechanisms are interpreted from the time- and frequency-resolved spectra of the effective optimal pulses

  7. Surface plasmon coupling dynamics in InGaN/GaN quantum-well structures and radiative efficiency improvement

    DEFF Research Database (Denmark)

    Fadil, Ahmed; Iida, Daisuke; Chen, Yuntian

    2014-01-01

    for InGaN/GaN quantum-well structures. By using a thin SiN dielectric layer between Ag and GaN we manage to modify and improve surface plasmon coupling effects, and we attribute this to the improved scattering of the nanoparticles at the quantum-well emission wavelength. The results are interpreted using...... numerical simulations, where absorption and scattering cross-sections are studied for different sized particles on GaN and GaN/SiN substrates....

  8. Effects of ambient pressure on dynamics of near-nozzle diesel sprays studied by ultrafast x-radiography

    International Nuclear Information System (INIS)

    Cheong, S. K.; Liu, J.; Shu, D.; Wang, J.; Powell, C. F.; Experimental Facilities Division

    2004-01-01

    A time-resolved x-radiographic technique has been employed for measuring the fuel distribution close to a single-hole nozzle fitted in a high-pressure diesel injector. Using a monochromatic synchrotron x-ray beam, it is possible to perform quantitative x-ray absorption measurements and obtain two-dimensional projections of the mass of the fuel spray. We have completed a series of spray measurements in the optically dense, near-nozzle region (ml 15 mm from the nozzle orifice) under ambient pressures of 1, 2, and 5.2 bar Nd2 and 1 bar SFd6 at room temperature with injection pressures of 500 and 1000 bar. The focus of the measurements is on the dynamical behaviors of the fuel jets with an emphasis on their penetration in the near-nozzle region. Careful analysis of the time-resolved, x-radiographic data revealed that the spray penetration in this near-nozzle region was not significantly affected by the limited change of the ambient pressure. In addition, well-defined features of the spray, such as the leading and trailing edges, and fluctuations of fuel mass density in the spray body, allowed us to calculate the leading, trailing, and internal speeds of the sprays

  9. 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...

  10. 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.

  11. Experimental Study of Electron and Phonon Dynamics in Nanoscale Materials by Ultrafast Laser Time-Domain Spectroscopy

    Science.gov (United States)

    Shen, Xiaohan

    With the rapid advances in the development of nanotechnology, nowadays, the sizes of elementary unit, i.e. transistor, of micro- and nanoelectronic devices are well deep into nanoscale. For the pursuit of cheaper and faster nanoscale electronic devices, the size of transistors keeps scaling down. As the miniaturization of the nanoelectronic devices, the electrical resistivity increases dramatically, resulting rapid growth in the heat generation. The heat generation and limited thermal dissipation in nanoscale materials have become a critical problem in the development of the next generation nanoelectronic devices. Copper (Cu) is widely used conducting material in nanoelectronic devices, and the electron-phonon scattering is the dominant contributor to the resistivity in Cu nanowires at room temperature. Meanwhile, phonons are the main carriers of heat in insulators, intrinsic and lightly doped semiconductors. The thermal transport is an ensemble of phonon transport, which strongly depends on the phonon frequency. In addition, the phonon transport in nanoscale materials can behave fundamentally different than in bulk materials, because of the spatial confinement. However, the size effect on electron-phonon scattering and frequency dependent phonon transport in nanoscale materials remain largely unexplored, due to the lack of suitable experimental techniques. This thesis is mainly focusing on the study of carrier dynamics and acoustic phonon transport in nanoscale materials. The weak photothermal interaction in Cu makes thermoreflectance measurement difficult, we rather measured the reflectivity change of Cu induced by absorption variation. We have developed a method to separately measure the processes of electron-electron scattering and electron-phonon scattering in epitaxial Cu films by monitoring the transient reflectivity signal using the resonant probe with particular wavelengths. The enhancement on electron-phonon scattering in epitaxial Cu films with thickness

  12. Terahertz plasmon and surface-plasmon modes in cylindrical metallic nanowires

    International Nuclear Information System (INIS)

    Wu Ping; Xu Wen; Li Long-Long; Lu Tie-Cheng; Wu Wei-Dong

    2014-01-01

    We present a theoretical study on collective excitation modes associated with plasmon and surface-plasmon oscillations in cylindrical metallic nanowires. Based on a two-subband model, the dynamical dielectric function matrix is derived under the random-phase approximation. An optic-like branch and an acoustic-like branch, which are free of Landau damping, are observed for both plasmon and surface-plasmon modes. Interestingly, for surface-plasmon modes, we find that two branches of the dispersion relation curves converge at a wavevector q z = q max beyond which no surface-plasmon mode exists. Moreover, we examine the dependence of these excitation modes on sample parameters such as the radius of the nanowires. It is found that in metallic nanowires realized by state-of-the-art nanotechnology the intra- and inter-subband plasmon and surface-plasmon frequencies are in the terahertz bandwidth. The frequency of the optic-like modes decreases with increasing radius of the nanowires, whereas that of the acoustic-like modes is not sensitive to the variation of the radius. This study is pertinent to the application of metallic nanowires as frequency-tunable terahertz plasmonic devices. (condensed matter: electronic structure, electrical, magnetic, and optical properties)

  13. Ultrafast spontaneous emission modulation of graphene quantum dots interacting with Ag nanoparticles in solution

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, Jianwei [Department of Physics, Shanghai University, Shanghai 200444 (China); Research Center of Quantum Macro-Phenomenon and Application, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210 (China); Lu, Jian, E-mail: luj@sari.ac.cn; Wang, Zhongyang, E-mail: wangzy@sari.ac.cn [Research Center of Quantum Macro-Phenomenon and Application, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210 (China); Wang, Liang [School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444 (China); Institute of Nanochemistry and Nanobiology, Shanghai University, Shanghai 200444 (China); Tian, Linfan [Research Center of Quantum Macro-Phenomenon and Application, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210 (China); School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210 (China); Deng, Xingxia [Research Center of Quantum Macro-Phenomenon and Application, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210 (China); School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Tian, Lijun [Department of Physics, Shanghai University, Shanghai 200444 (China); Pan, Dengyu [School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444 (China)

    2016-07-11

    We investigated the strong interaction between graphene quantum dots and silver nanoparticles in solution using time-resolved photoluminescence techniques. In solution, the silver nanoparticles are surrounded by graphene quantum dots and interacted with graphene quantum dots through exciton-plasmon coupling. An ultrafast spontaneous emission process (lifetime 27 ps) was observed in such a mixed solution. This ultrafast lifetime corresponds to the emission rate exceeding 35 GHz, with the purcell enhancement by a factor of ∼12. These experiment results pave the way for the realization of future high speed light sources applications.

  14. Reviews in plasmonics 2010

    CERN Document Server

    Geddes, Chris D

    2011-01-01

    Reviews in Plasmonics 2010, the first volume of the new book serial from Springer, serves as a comprehensive collection of current trends and emerging hot topics in the field of Plasmonics and closely related disciplines. It summarizes the year's progress in surface plasmon phenomena and its applications, with authoritative analytical reviews specialized enough to be attractive to professional researchers, yet also appealing to the wider audience of scientists in related disciplines of Plasmonics. Reviews in Plasmonics offers an essential reference material for any lab working in the Plasmonic

  15. Bismuth ferrite as low-loss switchable material for plasmonic waveguide modulator

    DEFF Research Database (Denmark)

    Babicheva, Viktoriia; Zhukovsky, Sergei; Lavrinenko, Andrei

    2014-01-01

    We propose new designs of plasmonic modulators, which can beused for dynamic signal switching in photonic integrated circuits. We studyperformance of a plasmonic waveguide modulator with bismuth ferrite as atunable material. The bismuth ferrite core is sandwiched between metalplates (metal...

  16. Ultrafast gas switching experiments

    International Nuclear Information System (INIS)

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

    1993-01-01

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

  17. 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.

  18. Perspective: Ultrafast magnetism and THz spintronics

    International Nuclear Information System (INIS)

    Walowski, Jakob; Münzenberg, Markus

    2016-01-01

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

  19. Ultrafast Holographic Image Recording by Single Shot Femtosecond Spectral Hole Burning

    National Research Council Canada - National Science Library

    Rebane, Aleksander

    2001-01-01

    .... This allowed us to record image holograms with 150-fs duration pulses without need to accumulate the SHB effect from many exposures. Results of this research show that it is possible to perform optical recording of data in frequency-domain on ultrafast time scale. These results can be used also as a new diagnostic tool for femtosecond dynamics in various ultrafast optical interactions.

  20. Visualizing hybridized quantum plasmons in coupled nanowires

    DEFF Research Database (Denmark)

    Andersen, Kirsten; Jensen, Kristian Lund; Mortensen, N. Asger

    2013-01-01

    of the dynamical dielectric function, which is computed using time-dependent density functional theory (TDDFT). For freestanding wires, the energy of both surface and bulk plasmon modes deviate from the classical result for low wire radii and high momentum transfer due to effects of electron spill-out, nonlocal......˚ separation, this mode is replaced by a charge-transfer plasmon, which blue shifts with decreasing separation in agreement with experiment and marks the onset of the strong tunneling regime....

  1. Ultrafast Silicon Photonics with Visible to Mid-Infrared Pumping of Silicon Nanocrystals.

    Science.gov (United States)

    Diroll, Benjamin T; Schramke, Katelyn S; Guo, Peijun; Kortshagen, Uwe R; Schaller, Richard D

    2017-10-11

    Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows for selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective mass at high effective hole temperatures lead to a subpicosecond change of the dielectric function, resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27%, and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates subpicosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting the modulation of transmittance at telecommunications wavelengths. The results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics.

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

    Science.gov (United States)

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

    2013-12-01

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

  3. Ultrafast S1 and ICT state dynamics of a marine carotenoid probed by femtosecond one- and two-photon pump-probe spectroscopy

    International Nuclear Information System (INIS)

    Kosumi, Daisuke; Kusumoto, Toshiyuki; Fujii, Ritsuko; Sugisaki, Mitsuru; Iinuma, Yoshiro; Oka, Naohiro; Takaesu, Yuki; Taira, Tomonori; Iha, Masahiko; Frank, Harry A.; Hashimoto, Hideki

    2011-01-01

    Ultrafast relaxation kinetics of fucoxanthin in polar and non-polar solvents have been studied by femtosecond pump-probe spectroscopy. Transient absorption associated with S 1 or intramolecular charge transfer (ICT) excited state has been observed following either one-photon excitation to the optically allowed S 2 state or two-photon excitation to the symmetry-forbidden S 1 state. The results suggest that the ICT state formed after excitation of fucoxanthin in a polar solvent is a distinct excited state from S 1 .

  4. Ultrafast S{sub 1} and ICT state dynamics of a marine carotenoid probed by femtosecond one- and two-photon pump-probe spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Kosumi, Daisuke, E-mail: kosumi@sci.osaka-cu.ac.j [CREST/JST and Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); Kusumoto, Toshiyuki [CREST/JST and Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); Fujii, Ritsuko; Sugisaki, Mitsuru [CREST/JST and Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); Osaka City University Advanced Research Institute for Natural Science and Technology (OCARINA), Osaka (Japan); Iinuma, Yoshiro; Oka, Naohiro; Takaesu, Yuki; Taira, Tomonori; Iha, Masahiko [South Product Co. Ltd., 12-75 Suzaki, Uruma-shi, Okinawa 904-2234 (Japan); Frank, Harry A. [Department of Chemistry, University of Connecticut, Storrs, CT 06269-3060 (United States); Hashimoto, Hideki, E-mail: hassy@sci.osaka-cu.ac.j [CREST/JST and Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); Osaka City University Advanced Research Institute for Natural Science and Technology (OCARINA), Osaka (Japan)

    2011-03-15

    Ultrafast relaxation kinetics of fucoxanthin in polar and non-polar solvents have been studied by femtosecond pump-probe spectroscopy. Transient absorption associated with S{sub 1} or intramolecular charge transfer (ICT) excited state has been observed following either one-photon excitation to the optically allowed S{sub 2} state or two-photon excitation to the symmetry-forbidden S{sub 1} state. The results suggest that the ICT state formed after excitation of fucoxanthin in a polar solvent is a distinct excited state from S{sub 1}.

  5. Ultrafast magnetodynamics with free-electron lasers

    Science.gov (United States)

    Malvestuto, Marco; Ciprian, Roberta; Caretta, Antonio; Casarin, Barbara; Parmigiani, Fulvio

    2018-02-01

    The study of ultrafast magnetodynamics has entered a new era thanks to the groundbreaking technological advances in free-electron laser (FEL) light sources. The advent of these light sources has made possible unprecedented experimental schemes for time-resolved x-ray magneto-optic spectroscopies, which are now paving the road for exploring the ultimate limits of out-of-equilibrium magnetic phenomena. In particular, these studies will provide insights into elementary mechanisms governing spin and orbital dynamics, therefore contributing to the development of ultrafast devices for relevant magnetic technologies. This topical review focuses on recent advancement in the study of non-equilibrium magnetic phenomena from the perspective of time-resolved extreme ultra violet (EUV) and soft x-ray spectroscopies at FELs with highlights of some important experimental results.

  6. The Physics and Applications of a 3D Plasmonic Nanostructure

    Science.gov (United States)

    Terranova, Brandon B.

    In this work, the dynamics of electromagnetic field interactions with free electrons in a 3D metallic nanostructure is evaluated theoretically. This dissertation starts by reviewing the relevant fundamentals of plasmonics and modern applications of plasmonic systems. Then, motivated by the need to have a simpler way of understanding the surface charge dynamics on complex plasmonic nanostructures, a new plasmon hybridization tree method is introduced. This method provides the plasmonicist with an intuitive way to determine the response of free electrons to incident light in complex nanostructures within the electrostatic regime. Next, a novel 3D plasmonic nanostructure utilizing reflective plasmonic coupling is designed to perform biosensing and plasmonic tweezing applications. By applying analytical and numerical methods, the effectiveness of this nanostructure at performing these applications is determined from the plasmonic response of the nanostructure to an excitation beam of coherent light. During this analysis, it was discovered that under certain conditions, this 3D nanostructure exhibits a plasmonic Fano resonance resulting from the interference of an in-plane dark mode and an out-of-plane bright mode. In evaluating this nanostructure for sensing changes in the local dielectric environment, a figure of merit of 68 is calculated, which is competitive with current localized surface plasmon resonance refractometric sensors. By evaluating the Maxwell stress tensor on a test particle in the vicinity of the nanostructure, it was found that under the right conditions, this plasmonic nanostructure design is capable of imparting forces greater than 10.5 nN on dielectric objects of nanoscale dimensions. The results obtained in these studies provides new routes to the design and engineering of 3D plasmonic nanostructures and Fano resonances in these systems. In addition, the nanostructure presented in this work and the design principles it utilizes have shown

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

    Science.gov (United States)

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

    2004-05-15

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

  8. Dynamic Dispersal of Surface Layer Biofilm Induced by Nanosized TiO2 Based on Surface Plasmon Resonance and Waveguide.

    Science.gov (United States)

    Zhang, Peng; Guo, Jin-Song; Yan, Peng; Chen, You-Peng; Wang, Wei; Dai, You-Zhi; Fang, Fang; Wang, Gui-Xue; Shen, Yu

    2018-05-01

    Pollutant degradation is present mainly in the surface layer of biofilms, and the surface layer is the most vulnerable to impairment by toxic pollutants. In this work, the effects of nanosized TiO 2 (n-TiO 2 ) on the average thicknesses of Bacillus subtilis biofilm and on bacterial attachment on different surfaces were investigated. The binding mechanism of n-TiO 2 to the cell surface was also probed. The results revealed that n-TiO 2 caused biofilm dispersal and the thicknesses decreased by 2.0 to 2.6 μm after several hours of exposure. The attachment abilities of bacteria with extracellular polymeric substances (EPS) on hydrophilic surfaces were significantly reduced by 31% and 81% under 10 and 100 mg/liter of n-TiO 2 , respectively, whereas those of bacteria without EPS were significantly reduced by 43% and 87%, respectively. The attachment abilities of bacteria with and without EPS on hydrophobic surfaces were significantly reduced by 50% and 56%, respectively, under 100 mg/liter of n-TiO 2 The results demonstrated that biofilm dispersal can be attributed to the changes in the cell surface structure and the reduction of microbial attachment ability. IMPORTANCE Nanoparticles can penetrate into the outer layer of biofilm in a relatively short period and can bind onto EPS and bacterial surfaces. The current work probed the effects of nanosized TiO 2 (n-TiO 2 ) on biofilm thickness, bacterial migration, and surface properties of the cell in the early stage using the surface plasmon resonance waveguide mode. The results demonstrated that n-TiO 2 decreased the adhesive ability of both cell and EPS and induced bacterial migration and biofilm detachment in several hours. The decreased adhesive ability of microbes and EPS worked against microbial aggregation, reducing the effluent quality in the biological wastewater treatment process. Copyright © 2018 American Society for Microbiology.

  9. Reviews in plasmonics 2016

    CERN Document Server

    2017-01-01

    Reviews in Plasmonics 2016, the third volume of the new book series from Springer, serves as a comprehensive collection of current trends and emerging hot topics in the field of Plasmonics and closely related disciplines. It summarizes the year’s progress in surface plasmon phenomena and its applications, with authoritative analytical reviews in sufficient detail to be attractive to professional researchers, yet also appealing to the wider audience of scientists in related disciplines of Plasmonics. Reviews in Plasmonics offers an essential source of reference material for any lab working in the Plasmonics field and related areas. All academics, bench scientists, and industry professionals wishing to take advantage of the latest and greatest in the continuously emerging field of Plasmonics will find it an invaluable resource.

  10. Reviews in plasmonics 2015

    CERN Document Server

    2016-01-01

    Reviews in Plasmonics 2015, the second volume of the new book series from Springer, serves as a comprehensive collection of current trends and emerging hot topics in the field of Plasmonics and closely related disciplines. It summarizes the year’s progress in surface plasmon phenomena and its applications, with authoritative analytical reviews in sufficient detail to be attractive to professional researchers, yet also appealing to the wider audience of scientists in related disciplines of Plasmonics. Reviews in Plasmonics offers an essential source of reference material for any lab working in the Plasmonics field and related areas. All academics, bench scientists, and industry professionals wishing to take advantage of the latest and greatest in the continuously emerging field of Plasmonics will find it an invaluable resource.

  11. Plasmonic colour generation

    DEFF Research Database (Denmark)

    Kristensen, Anders; Yang, Joel K. W.; Bozhevolnyi, Sergey I.

    2016-01-01

    Plasmonic colours are structural colours that emerge from resonant interactions between light and metallic nanostructures. The engineering of plasmonic colours is a promising, rapidly emerging research field that could have a large technological impact. We highlight basic properties of plasmonic...... colours and recent nanofabrication developments, comparing technology-performance indicators for traditional and nanophotonic colour technologies. The structures of interest include diffraction gratings, nanoaperture arrays, thin films, and multilayers and structures that support Mie resonances...... and whispering-gallery modes. We discuss plasmonic colour nanotechnology based on localized surface plasmon resonances, such as gap plasmons and hybridized disk–hole plasmons, which allow for colour printing with sub-diffraction resolution. We also address a range of fabrication approaches that enable large...

  12. Ultra-compact plasmonic waveguide modulators

    DEFF Research Database (Denmark)

    Babicheva, Viktoriia

    of developing new material platforms for integrated plasmonic devices. Furthermore, novel plasmonic materials such as transparent conductive oxides and transition metal nitrides can offer a variety of new opportunities. In particular, they offer adjustable/tailorable and nonlinear optical properties, dynamic...... modulators based on ultra-compact waveguides with different active cores. Plasmonic modulators with the active core such as indium phosphides or ferroelectrics sandwiched between metal plates have promising characteristics. Apart from the speed and dimensions advantages, the metal plates can serve...... as electrodes for electrical pumping of the active material making it easier to integrate. Including an additional layer in the plasmonic waveguide, in particular an ultrathin transparent conductive oxide film, allows the control of the dispersive properties of the waveguide and thus the higher efficiency...

  13. SPASER as a complex system: femtosecond dynamics traced by ab-initio simulations

    KAUST Repository

    Gongora, J. S. Totero; Miroshnichenko, Andrey E.; Kivshar, Yuri S.; Fratalocchi, Andrea

    2016-01-01

    Integrating coherent light sources at the nanoscale with spasers is one of the most promising applications of plasmonics. A spaser is a nano-plasmonic counterpart of a laser, with photons replaced by surface plasmon polaritons and the resonant cavity replaced by a nanoparticle supporting localized plasmonic modes. Despite the large body of experimental and theoretical studies, the understanding of the fundamental properties of the spaser emission is still challenging. In this work, we investigated the ultrafast dynamics of the emission from a core-shell spaser by developing a rigorous first-principle numerical model. Our results show that the spaser is a highly nonlinear system with many interacting degrees of freedom, whose emission sustain a rich manifold of different spatial phases. In the regime of strong interaction we observed that the spaser emission manifests an irreversible ergodic evolution, where energy is equally shared among all the available degrees of freedom. Under this condition, the spaser generates ultrafast vortex lasing modes that are spinning on the femtosecond scale, acquiring the character of a nanoparticle with an effective spin. Interestingly, the spin orientation is defined by spontaneous symmetry breaking induced by quantum noise, which is a fundamental component of our ab-initio model. This opens up interesting possibilities of achieving unidirectional emission from a perfectly spherical nanoparticle, stimulating a broad range of applications for nano-plasmonic lasers as unidirectional couplers, random information sources and novel form of photonics neural-networks. © (2016) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.

  14. SPASER as a complex system: femtosecond dynamics traced by ab-initio simulations

    KAUST Repository

    Gongora, J. S. Totero

    2016-03-14

    Integrating coherent light sources at the nanoscale with spasers is one of the most promising applications of plasmonics. A spaser is a nano-plasmonic counterpart of a laser, with photons replaced by surface plasmon polaritons and the resonant cavity replaced by a nanoparticle supporting localized plasmonic modes. Despite the large body of experimental and theoretical studies, the understanding of the fundamental properties of the spaser emission is still challenging. In this work, we investigated the ultrafast dynamics of the emission from a core-shell spaser by developing a rigorous first-principle numerical model. Our results show that the spaser is a highly nonlinear system with many interacting degrees of freedom, whose emission sustain a rich manifold of different spatial phases. In the regime of strong interaction we observed that the spaser emission manifests an irreversible ergodic evolution, where energy is equally shared among all the available degrees of freedom. Under this condition, the spaser generates ultrafast vortex lasing modes that are spinning on the femtosecond scale, acquiring the character of a nanoparticle with an effective spin. Interestingly, the spin orientation is defined by spontaneous symmetry breaking induced by quantum noise, which is a fundamental component of our ab-initio model. This opens up interesting possibilities of achieving unidirectional emission from a perfectly spherical nanoparticle, stimulating a broad range of applications for nano-plasmonic lasers as unidirectional couplers, random information sources and novel form of photonics neural-networks. © (2016) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.

  15. Comparison of arterial input functions measured from ultra-fast dynamic contrast enhanced MRI and dynamic contrast enhanced computed tomography in prostate cancer patients

    Science.gov (United States)

    Wang, Shiyang; Lu, Zhengfeng; Fan, Xiaobing; Medved, Milica; Jiang, Xia; Sammet, Steffen; Yousuf, Ambereen; Pineda, Federico; Oto, Aytekin; Karczmar, Gregory S.

    2018-02-01

    The purpose of this study was to evaluate the accuracy of arterial input functions (AIFs) measured from dynamic contrast enhanced (DCE) MRI following a low dose of contrast media injection. The AIFs measured from DCE computed tomography (CT) were used as ‘gold standard’. A total of twenty patients received CT and MRI scans on the same day. Patients received 120 ml Iohexol in DCE-CT and a low dose of (0.015 mM kg-1) of gadobenate dimeglumine in DCE-MRI. The AIFs were measured in the iliac artery and normalized to the CT and MRI contrast agent doses. To correct for different temporal resolution and sampling periods of CT and MRI, an empirical mathematical model (EMM) was used to fit the AIFs first. Then numerical AIFs (AIFCT and AIFMRI) were calculated based on fitting parameters. The AIFMRI was convolved with a ‘contrast agent injection’ function (AIFMRICON ) to correct for the difference between MRI and CT contrast agent injection times (~1.5 s versus 30 s). The results show that the EMMs accurately fitted AIFs measured from CT and MRI. There was no significant difference (p  >  0.05) between the maximum peak amplitude of AIFs from CT (22.1  ±  4.1 mM/dose) and MRI after convolution (22.3  ±  5.2 mM/dose). The shapes of the AIFCT and AIFMRICON were very similar. Our results demonstrated that AIFs can be accurately measured by MRI following low dose contrast agent injection.

  16. Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

    Science.gov (United States)

    Mongin, Denis; Shaviv, Ehud; Maioli, Paolo; Crut, Aurélien; Banin, Uri; Del Fatti, Natalia; Vallée, Fabrice

    2012-08-28

    Hybrid nano-objects formed by two or more disparate materials are among the most promising and versatile nanosystems. A key parameter in their properties is interaction between their components. In this context we have investigated ultrafast charge separation in semiconductor-metal nanohybrids using a model system of gold-tipped CdS nanorods in a matchstick architecture. Experiments are performed using an optical time-resolved pump-probe technique, exciting either the semiconductor or the metal component of the particles, and probing the light-induced change of their optical response. Electron-hole pairs photoexcited in the semiconductor part of the nanohybrids are shown to undergo rapid charge separation with the electron transferred to the metal part on a sub-20 fs time scale. This ultrafast gold charging leads to a transient red-shift and broadening of the metal surface plasmon resonance, in agreement with results for free clusters but in contrast to observation for static charging of gold nanoparticles in liquid environments. Quantitative comparison with a theoretical model is in excellent agreement with the experimental results, confirming photoexcitation of one electron-hole pair per nanohybrid followed by ultrafast charge separation. The results also point to the utilization of such metal-semiconductor nanohybrids in light-harvesting applications and in photocatalysis.

  17. Quantum modeling of ultrafast photoinduced charge separation

    Science.gov (United States)

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

    2018-01-01

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

  18. High efficiency all-optical plasmonic diode based on a nonlinear side-coupled waveguide-cavity structure with broken symmetry

    Science.gov (United States)

    Liang, Hong-Qin; Liu, Bin; Hu, Jin-Feng; He, Xing-Dao

    2018-05-01

    An all-optical plasmonic diode, comprising a metal-insulator-metal waveguide coupled with a stub cavity, is proposed based on a nonlinear Fano structure. The key technique used is to break structural spatial symmetry by a simple reflector layer in the waveguide. The spatial asymmetry of the structure gives rise to the nonreciprocity of coupling efficiencies between the Fano cavity and waveguides on both sides of the reflector layer, leading to a nonreciprocal nonlinear response. Transmission properties and dynamic responses are numerically simulated and investigated by the nonlinear finite-difference time-domain method. In the proposed structure, high-efficiency nonreciprocal transmission can be achieved with a low power threshold and an ultrafast response time (subpicosecond level). A high maximum transmittance of 89.3% and an ultra-high transmission contrast ratio of 99.6% can also be obtained. The device can be flexibly adjusted for working wavebands by altering the stub cavity length.

  19. Novel plasmon nano-lasers

    NARCIS (Netherlands)

    Hill, M.T.; Marell, M.J.H.

    2010-01-01

    We will discuss some of the latest developments in metallic and plasmonic nano-lasers. Furthermore we will present our latest results on further miniaturization of electrically pumped plasmonic nano-lasers and also DFB Plasmon mode devices.

  20. Real-time visualization of soliton molecules with evolving behavior in an ultrafast fiber laser

    Science.gov (United States)

    Liu, Meng; Li, Heng; Luo, Ai-Ping; Cui, Hu; Xu, Wen-Cheng; Luo, Zhi-Chao

    2018-03-01

    Ultrafast fiber lasers have been demonstrated to be great platforms for the investigation of soliton dynamics. The soliton molecules, as one of the most fascinating nonlinear phenomena, have been a hot topic in the field of nonlinear optics in recent years. Herein, we experimentally observed the real-time evolving behavior of soliton molecule in an ultrafast fiber laser by using the dispersive Fourier transformation technology. Several types of evolving soliton molecules were obtained in our experiments, such as soliton molecules with monotonically or chaotically evolving phase, flipping and hopping phase. These results would be helpful to the communities interested in soliton nonlinear dynamics as well as ultrafast laser technologies.

  1. 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.

  2. 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...

  3. Patellofemoral joint motion: Evaluation by ultrafast computed tomography

    International Nuclear Information System (INIS)

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

    1988-01-01

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

  4. Patellofemoral joint motion: Evaluation by ultrafast computed tomography

    Energy Technology Data Exchange (ETDEWEB)

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

    1988-10-01

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

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

    DEFF Research Database (Denmark)

    Turchinovich, Dmitry; Hoffmann, M. V.

    2011-01-01

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

  6. Ultrafast Graphene Photonics and Optoelectronics

    Science.gov (United States)

    2017-04-14

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

  7. 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.

  8. Ultrafast carrier dynamics unravel role of surface ligands and metal domain size on the photocatalytic hydrogen evolution efficiency of Au-tipped CdS nanorods: an ultrafast transient absorption spectroscopy study

    Science.gov (United States)

    Ben-Shahar, Yuval; Kriegel, Ilka; Scotognella, Francesco; Waiskopf, Nir; Dal Conte, Stefano; Moretti, Luca; Cerullo, Giulio; Rabani, Eran; Banin, Uri

    2017-02-01

    Semiconductor-metal hybrid nanostructures are interesting materials for photocatalysis. Their tunable properties offer a highly controllable platform to design light-induced charge separation, a key to their function in photocatalytic water splitting. Hydrogen evolution quantum yields are influenced by factors as size, shape, material and morphology of the system, additionally the surface coating or the metal domain size play a dominant role. In this paper we present a study on a well-defined model system of Au-tipped CdS nanorods. We use transient absorption spectroscopy to get insights into the charge carrier dynamics after photoexcitation of the bandgap of CdS nanorods. The study of charge transfer processes combined with the hydrogen evolution efficiency unravels the effects of surface coating and the gold tip size on the photocatalytic efficiency. Differences in efficiency with various surface ligands are primarily ascribed to the effects of surface passivation. Surface trapping of charge carriers is competing with effective charge separation, a prerequisite for photocatalysis, leading to the observed lower hydrogen production quantum yields. Interestingly, non-monotonic hydrogen evolution efficiency with size of the gold tip is observed, resulting in an optimal metal domain size for the most efficient photocatalysis. These results are explained by the sizedependent interplay of the metal domain charging and the relative band-alignments. Taken together our findings are of major importance for the potential application of hybrid nanoparticles as photocatalysts.

  9. 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.

  10. Tunable plasmonic toroidal terahertz metamodulator

    Science.gov (United States)

    Gerislioglu, Burak; Ahmadivand, Arash; Pala, Nezih

    2018-04-01

    Optical modulators are essential and strategic parts of micro- and nanophotonic circuits to encode electro-optical signals in the optical domain. Here, by using arrays of multipixel toroidal plasmonic terahertz (THz) metamolecules, we developed a functional plasmonic metamodulator with high efficiency and tunability. Technically, the dynamic toroidal dipole induces nonradiating charge-current arrangements leading to have an exquisite role in defining the inherent spectral features of various materials. By categorizing in a different family of multipoles far from the traditional electromagnetic multipoles, the toroidal dipole corresponds to poloidal currents flowing on the surface of a closed-loop torus. Utilizing the sensitivity of the optically driven toroidal momentum to the incident THz beam power and by employing both numerical tools and experimental analysis, we systematically studied the spectral response of the proposed THz plasmonic metadevice. In this Rapid Communication, we uncover a correlation between the existence and the excitation of the toroidal response and the incident beam power. This mechanism is employed to develop THz toroidal metamodulators with a strong potential to be employed for practical advanced and next-generation communication, filtering, and routing applications.

  11. Fourteenth International Conference on Ultrafast Phenomena

    CERN Document Server

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

    2005-01-01

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

  12. Femtosecond Snapshots of quantum mechanics at work in plasmonic nano-structures

    Science.gov (United States)

    Carbone, Fabrizio

    Ultrafast Transmission Electron Microscopy enabled a new technique (Photon-Induced Near Field Electron Microscopy, PINEM), capable of controlling electromagnetic fields confined on the surface of nanostructures and image their properties with nm-resolution in direct space and fs resolution in time. In this presentation, we will show some recent results where the standing wave formed by the plasmonic field confined on the surface of one silver nano-wire was imaged together with its energy exchange with the imaging electrons. In these results, both the interference and the quantization of the plasmonic near field could be imaged simultaneously, revealing both a quantum and a classical aspect of the electromagnetic field in one snapshot. The implications of these results will be discussed, and we will also present new ideas and methodologies to go beyond such an experiment and image the interaction between single electrons and single plasmons. We will also show that shaping the electron density in a thin film via light pulses is possible by taking advantage of the plasmon-plasmon interference and the ability of light polarization to control the excitation of different plasmonic field geometries in ad hoc designed nanostructures. Movies of the propagation of plasmons will also be presented, providing insights into their speed, propagation losses and the effect of confinment. This work was supported by an ERC Grant USED.

  13. Qualitative assessment of ultra-fast non-Grotthuss proton dynamics in S1 excited state of liquid H2O from ab initio time-dependent density functional theory★

    Science.gov (United States)

    Ziaei, Vafa; Bredow, Thomas

    2017-11-01

    We study qualitatively ultra-fast proton transfer (PT) in the first singlet (S1) state of liquid water (absorption onset) through excited-state dynamics by means of time-dependent density functional theory and ab initio Born-Oppenheimer molecular dynamics. We find that after the initial excitation, a PT occurs in S1 in form of a rapid jump to a neighboring water molecule, on which the proton either may rest for a relatively long period of time (as a consequence of possible defect in the hydrogen bond network) followed by back and forth hops to its neighboring water molecule or from which it further moves to the next water molecule accompanied by back and forth movements. In this way, the proton may become delocalized over a long water wire branch, followed again by back and forth jumps or short localization on a water molecule for some femtoseconds. As a result, the mechanism of PT in S1 is in most cases highly non-Grotthuss-like, delayed and discrete. Furthermore, upon PT an excess charge is ejected to the solvent trap, the so-called solvated electron. The spatial extent of the ejected solvated electron is mainly localized within one solvent shell with overlappings on the nearest neighbor water molecules and delocalizing (diffuse) tails extending beyond the first solvent sphere. During the entire ultra-short excited-state dynamics the remaining OH radical from the initially excited water molecule exhibits an extremely low mobility and is non-reactive. Supplementary material in the form of one pdf file available from the Journal web page at http://https://doi.org/10.1140/epjb/e2017-80329-7.

  14. Ultrafast transient-absorption of the solvated electron in water

    International Nuclear Information System (INIS)

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

    1994-01-01

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

  15. Ultrafast laser-semiconductor interactions

    International Nuclear Information System (INIS)

    Schile, L.A.

    1996-01-01

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

  16. Electronically controllable spoof localized surface plasmons

    Science.gov (United States)

    Zhou, Yong Jin; Zhang, Chao; Yang, Liu; Xun Xiao, Qian

    2017-10-01

    Electronically controllable multipolar spoof localized surface plasmons (LSPs) are experimentally demonstrated in the microwave frequencies. It has been shown that half integer order LSPs modes exist on the corrugated ring loaded with a slit, which actually arise from the Fabry-Perot-like resonances. By mounting active components across the slit in the corrugated rings, electronic switchability and tunability of spoof LSPs modes have been accomplished. Both simulated and measured results demonstrate efficient dynamic control of the spoof LSPs. These elements may form the basis of highly integrated programmable plasmonic circuits in microwave and terahertz regimes.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-07-15

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

  18. Smart textile plasmonic fiber dew sensors.

    Science.gov (United States)

    Esmaeilzadeh, Hamid; Rivard, Maxime; Arzi, Ezatollah; Légaré, François; Hassani, Alireza

    2015-06-01

    We propose a novel Surface Plasmon Resonance (SPR)-based sensor that detects dew formation in optical fiber-based smart textiles. The proposed SPR sensor facilitates the observation of two phenomena: condensation of moisture and evaporation of water molecules in air. This sensor detects dew formation in less than 0.25 s, and determines dew point temperature with an accuracy of 4%. It can be used to monitor water layer depth changes during dew formation and evaporation in the range of a plasmon depth probe, i.e., 250 nm, with a resolution of 7 nm. Further, it facilitates estimation of the relative humidity of a medium over a dynamic range of 30% to 70% by measuring the evaporation time via the plasmon depth probe.

  19. Hot Charge Carrier Transmission from Plasmonic Nanostructures

    Science.gov (United States)

    Christopher, Phillip; Moskovits, Martin

    2017-05-01

    Surface plasmons have recently been harnessed to carry out processes such as photovoltaic current generation, redox photochemistry, photocatalysis, and photodetection, all of which are enabled by separating energetic (hot) electrons and holes—processes that, previously, were the domain of semiconductor junctions. Currently, the power conversion efficiencies of systems using plasmon excitation are low. However, the very large electron/hole per photon quantum efficiencies observed for plasmonic devices fan the hope of future improvements through a deeper understanding of the processes involved and through better device engineering, especially of critical interfaces such as those between metallic and semiconducting nanophases (or adsorbed molecules). In this review, we focus on the physics and dynamics governing plasmon-derived hot charge carrier transfer across, and the electronic structure at, metal-semiconductor (molecule) interfaces, where we feel the barriers contributing to low efficiencies reside. We suggest some areas of opportunity that deserve early attention in the still-evolving field of hot carrier transmission from plasmonic nanostructures to neighboring phases.

  20. Robust plasmonic substrates

    DEFF Research Database (Denmark)

    Kostiučenko, Oksana; Fiutowski, Jacek; Tamulevicius, Tomas

    2014-01-01

    Robustness is a key issue for the applications of plasmonic substrates such as tip-enhanced Raman spectroscopy, surface-enhanced spectroscopies, enhanced optical biosensing, optical and optoelectronic plasmonic nanosensors and others. A novel approach for the fabrication of robust plasmonic...... substrates is presented, which relies on the coverage of gold nanostructures with diamond-like carbon (DLC) thin films of thicknesses 25, 55 and 105 nm. DLC thin films were grown by direct hydrocarbon ion beam deposition. In order to find the optimum balance between optical and mechanical properties...

  1. Propagation of complex shaped ultrafast pulses in highly optically dense samples

    International Nuclear Information System (INIS)

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

    2008-01-01

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

  2. Ultrafast strain engineering in complex oxide heterostructures

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-07-01

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

  3. Topographical coloured plasmonic coins

    OpenAIRE

    Guay, Jean-Michel; Lesina, Antonino Calà; Côté, Guillaume; Charron, Martin; Ramunno, Lora; Berini, Pierre; Weck, Arnaud

    2016-01-01

    Plasmonic resonances in metallic nanoparticles have been used since antiquity to colour glasses. The use of metal nanostructures for surface colourization has attracted considerable interest following recent developments in plasmonics. However, current top-down colourization methods are not ideally suited to large-scale industrial applications. Here we use a bottom-up approach where picosecond laser pulses can produce a full palette of non-iridescent colours on silver, gold, copper and alumin...

  4. Nonsymmorphic symmetry-protected topological modes in plasmonic nanoribbon lattices

    Science.gov (United States)

    Zhang, Yong-Liang; Wu, Raymond P. H.; Kumar, Anshuman; Si, Tieyan; Fung, Kin Hung

    2018-04-01

    Using a dynamic eigenresponse theory, we study the topological edge plasmon modes in dispersive plasmonic lattices constructed by unit cells of multiple nanoribbons. In dipole approximation, the bulk-edge correspondence in the lattices made of dimerized unit cell and one of its square-root daughter with nonsymmorphic symmetry are demonstrated. Calculations with consideration of dynamic long-range effects and retardation are compared to those given by nearest-neighbor approximations. It is shown that nonsymmorphic symmetry opens up two symmetric gaps where versatile topological edge plasmon modes are found. Unprecedented spectral shifts of the edge states with respect to the zero modes due to long-range coupling are found. The proposed ribbon structure is favorable to electrical gating and thus could serve as an on-chip platform for electrically controllable subwavelength edge states at optical wavelengths. Our eigenresponse approach provides a powerful tool for the radiative topological mode analysis in strongly coupled plasmonic lattices.

  5. Plasmon resonance in single- and double-layer CVD graphene nanoribbons

    DEFF Research Database (Denmark)

    Wang, Di; Emani, Naresh K.; Chung, Ting Fung

    2015-01-01

    Dynamic tunability of the plasmonic resonance in graphene nanoribbons is desirable in the near-infrared. We demonstrated a constant blue shift of plasmonic resonances in double-layer graphene nanoribbons with respect to single-layer graphene nanoribbons. © OSA 2015.......Dynamic tunability of the plasmonic resonance in graphene nanoribbons is desirable in the near-infrared. We demonstrated a constant blue shift of plasmonic resonances in double-layer graphene nanoribbons with respect to single-layer graphene nanoribbons. © OSA 2015....

  6. Ultrafast photocurrents in monolayer MoS2

    Science.gov (United States)

    Parzinger, Eric; Wurstbauer, Ursula; Holleitner, Alexander W.

    Two-dimensional transition metal dichalcogenides such as MoS2 have emerged as interesting materials for optoelectronic devices. In particular, the ultrafast dynamics and lifetimes of photoexcited charge carriers have attracted great interest during the last years. We investigate the photocurrent response of monolayer MoS2 on a picosecond time scale utilizing a recently developed pump-probe spectroscopy technique based on coplanar striplines. We discuss the ultrafast dynamics within MoS2 including photo-thermoelectric currents and the impact of built-in fields due to Schottky barriers as well as the Fermi level pinning at the contact region. We acknowledge support by the ERC via Project 'NanoREAL', the DFG via excellence cluster 'Nanosystems Initiative Munich' (NIM), and through the TUM International Graduate School of Science and Engineering (IGSSE) and BaCaTeC.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-08-15

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

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

    International Nuclear Information System (INIS)

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

    2015-01-01

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

  9. Photothermal modification of plasmonic structures

    DEFF Research Database (Denmark)

    2016-01-01

    There is presented a method for geometrically modifying plasmonic structures on a support structure, such as for printing or recording, said method comprising changing a geometry specifically of plasmonic structures, wherein said changing the geometry is carried out by photothermally melting...... at least a portion of each of the plasmonic structures within the second plurality of plasmonic structures by irradiating, the plasmonic structures with incident electromagnetic radiation having an incident intensity in a plane of the second plurality of plasmonic structures, wherein said incident...... intensity is less than an incident intensity required to melt a film of a corresponding material and a corresponding thickness as the plasmonic structures within the second plurality of plasmonic structures....

  10. 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...

  11. Fabricating plasmonic components for nanophotonics

    DEFF Research Database (Denmark)

    Boltasseva, Alexandra; Nielsen, Rasmus Bundgaard; Jeppesen, Claus

    2009-01-01

    We report on experimental realization of different metal-dielectric structures that are used as surface plasmon polariton waveguides and as plasmonic metamaterials. Fabrication approaches based on different lithographic and deposition techniques are discussed....

  12. Searching for better plasmonic materials

    DEFF Research Database (Denmark)

    West, P.; Ishii, S.; Naik, G.

    2010-01-01

    Plasmonics is a research area merging the fields of optics and nanoelectronics by confining light with relatively large free-space wavelength to the nanometer scale - thereby enabling a family of novel devices. Current plasmonic devices at telecommunication and optical frequencies face significan...... for realizing optimal plasmonic material properties for specific frequencies and applications, thereby providing a reference for those searching for better plasmonic materials....

  13. Metal Nitrides for Plasmonic Applications

    DEFF Research Database (Denmark)

    Naik, Gururaj V.; Schroeder, Jeremy; Guler, Urcan

    2012-01-01

    Metal nitrides as alternatives to metals such as gold could offer many advantages when used as plasmonic material. We show that transition metal nitrides can replace metals providing equally good optical performance for many plasmonic applications.......Metal nitrides as alternatives to metals such as gold could offer many advantages when used as plasmonic material. We show that transition metal nitrides can replace metals providing equally good optical performance for many plasmonic applications....

  14. Probing in space and time the nuclear motion driven by nonequilibrium electronic dynamics in ultrafast pumped N.sub.2./sub.

    Czech Academy of Sciences Publication Activity Database

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

    2016-01-01

    Roč. 120, č. 19 (2016), s. 3335-3342 ISSN 1089-5639 Institutional support: RVO:68378271 Keywords : molecular dynamics * dissociation * excitation * ions Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 2.847, year: 2016

  15. Use of ultrafast dispersed pump-dump-probe and pump-repump-probe spectroscopies to explore the light-induced dynamics of peridinin in solution

    NARCIS (Netherlands)

    Papagiannakis, E.; Vengris, M.; Larsen, D.S.; van Stokkum, I.H.M.; Hiller, R.G.; van Grondelle, R.

    2006-01-01

    Optical pump-induced dynamics of the highly asymmetric carotenoid peridinin in methanol was studied by dispersed pump-probe, pump-dump-probe, and pump-repump-probe transient absorption spectroscopy in the visible region. Dispersed pump-probe measurements show that the decay of the initially excited

  16. Towards transparent all-optical label-swapped networks: 40 Gbit/s ultra-fast dynamic wavelength routing using integrated devices

    DEFF Research Database (Denmark)

    Seoane, Jorge; Holm-Nielsen, Pablo Villanueva; Jeppesen, Palle

    2006-01-01

    All-optical routing of 40 Gbit/s 1.6 ns packets is demonstrated employing integrated devices based on SOA-MZIs. The scheme allows wavelength transparent operation and sub-nanosecond dynamic wavelength selection for future packet/label switched networks....

  17. Ultrafast vibrations of gold nanorings

    DEFF Research Database (Denmark)

    Kelf, T; Tanaka, Y; Matsuda, O

    2011-01-01

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

  18. Ultrafast vibrations of gold nanorings

    DEFF Research Database (Denmark)

    Kelf, T; Tanaka, Y; Matsuda, O

    2011-01-01

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

  19. Measurements of ionic structure in shock compressed lithium hydride from ultrafast x-ray Thomson scattering.

    Science.gov (United States)

    Kritcher, A L; Neumayer, P; Brown, C R D; Davis, P; Döppner, T; Falcone, R W; Gericke, D O; Gregori, G; Holst, B; Landen, O L; Lee, H J; Morse, E C; Pelka, A; Redmer, R; Roth, M; Vorberger, J; Wünsch, K; Glenzer, S H

    2009-12-11

    We present the first ultrafast temporally, spectrally, and angularly resolved x-ray scattering measurements from shock-compressed matter. The experimental spectra yield the absolute elastic and inelastic scattering intensities from the measured density of free electrons. Laser-compressed lithium-hydride samples are well characterized by inelastic Compton and plasmon scattering of a K-alpha x-ray probe providing independent measurements of temperature and density. The data show excellent agreement with the total intensity and structure when using the two-species form factor and accounting for the screening of ion-ion interactions.

  20. Plasmon-exciton-polariton lasing

    NARCIS (Netherlands)

    Ramezani, M.; Halpin, A.; Fernández-Dominguez, A.I.; Feist, J.; Rodriguez, S.R.K.; Gómez-Rivas, J.; Garcia-Vidal, F.J.

    2016-01-01

    Strong coupling of Frenkel excitons with surface plasmons leads to the formation of bosonic quasi-particles known as plasmon-exciton-polaritons (PEPs).Localized surface plasmons in nanoparticles are lossy due to radiative and nonradiative decays, which has hampered the realization of polariton

  1. Plasmon-induced carrier polarization in semiconductor nanocrystals

    Science.gov (United States)

    Yin, Penghui; Tan, Yi; Fang, Hanbing; Hegde, Manu; Radovanovic, Pavle V.

    2018-06-01

    Spintronics1 and valleytronics2 are emerging quantum electronic technologies that rely on using electron spin and multiple extrema of the band structure (valleys), respectively, as additional degrees of freedom. There are also collective properties of electrons in semiconductor nanostructures that potentially could be exploited in multifunctional quantum devices. Specifically, plasmonic semiconductor nanocrystals3-10 offer an opportunity for interface-free coupling between a plasmon and an exciton. However, plasmon-exciton coupling in single-phase semiconductor nanocrystals remains challenging because confined plasmon oscillations are generally not resonant with excitonic transitions. Here, we demonstrate a robust electron polarization in degenerately doped In2O3 nanocrystals, enabled by non-resonant coupling of cyclotron magnetoplasmonic modes11 with the exciton at the Fermi level. Using magnetic circular dichroism spectroscopy, we show that intrinsic plasmon-exciton coupling allows for the indirect excitation of the magnetoplasmonic modes, and subsequent Zeeman splitting of the excitonic states. Splitting of the band states and selective carrier polarization can be manipulated further by spin-orbit coupling. Our results effectively open up the field of plasmontronics, which involves the phenomena that arise from intrinsic plasmon-exciton and plasmon-spin interactions. Furthermore, the dynamic control of carrier polarization is readily achieved at room temperature, which allows us to harness the magnetoplasmonic mode as a new degree of freedom in practical photonic, optoelectronic and quantum-information processing devices.

  2. Active molecular plasmonics: tuning surface plasmon resonances by exploiting molecular dimensions

    Science.gov (United States)

    Chen, Kai; Leong, Eunice Sok Ping; Rukavina, Michael; Nagao, Tadaaki; Liu, Yan Jun; Zheng, Yuebing

    2015-06-01

    Molecular plasmonics explores and exploits the molecule-plasmon interactions on metal nanostructures to harness light at the nanoscale for nanophotonic spectroscopy and devices. With the functional molecules and polymers that change their structural, electrical, and/or optical properties in response to external stimuli such as electric fields and light, one can dynamically tune the plasmonic properties for enhanced or new applications, leading to a new research area known as active molecular plasmonics (AMP). Recent progress in molecular design, tailored synthesis, and self-assembly has enabled a variety of scenarios of plasmonic tuning for a broad range of AMP applications. Dimension (i.e., zero-, two-, and threedimensional) of the molecules on metal nanostructures has proved to be an effective indicator for defining the specific scenarios. In this review article, we focus on structuring the field of AMP based on the dimension of molecules and discussing the state of the art of AMP. Our perspective on the upcoming challenges and opportunities in the emerging field of AMP is also included.

  3. Active molecular plasmonics: tuning surface plasmon resonances by exploiting molecular dimensions

    Directory of Open Access Journals (Sweden)

    Chen Kai

    2015-06-01

    Full Text Available Molecular plasmonics explores and exploits the molecule–plasmon interactions on metal nanostructures to harness light at the nanoscale for nanophotonic spectroscopy and devices. With the functional molecules and polymers that change their structural, electrical, and/or optical properties in response to external stimuli such as electric fields and light, one can dynamically tune the plasmonic properties for enhanced or new applications, leading to a new research area known as active molecular plasmonics (AMP. Recent progress in molecular design, tailored synthesis, and self-assembly has enabled a variety of scenarios of plasmonic tuning for a broad range of AMP applications. Dimension (i.e., zero-, two-, and threedimensional of the molecules on metal nanostructures has proved to be an effective indicator for defining the specific scenarios. In this review article, we focus on structuring the field of AMP based on the dimension of molecules and discussing the state of the art of AMP. Our perspective on the upcoming challenges and opportunities in the emerging field of AMP is also included.

  4. Carbon Incorporation and Anion Dynamics as Synergistic Drivers for Ultrafast Diffusion in Superionic LiCB11H12 and NaCB11H12

    Energy Technology Data Exchange (ETDEWEB)

    Dimitrievska, Mirjana [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Shea, Patrick [Lawrence Livermore National Laboratory; Kweon, Kyoung E. [Lawrence Livermore National Laboratory; Bercx, Marnik [University of Antwerp; Varley, Joel B. [Lawrence Livermore National Laboratory; Tang, Wan Si [National Institute of Standards and Technology; University of Maryland; Skripov, Alexander V. [Ural Division of the Russian Academy of Sciences; Stavila, Vitalie [Sandia National Laboratories; Udovic, Terrence J. [National Institute of Standards and Technology; Wood, Brandon C. [Lawrence Livermore National Laboratory

    2018-02-02

    The disordered phases of LiCB11H12 and NaCB11H12 possess superb superionic conductivities that make them suitable as solid electrolytes. In these materials, cation diffusion correlates with high orientational mobilities of the CB11H12- anions; however, the precise relationship has yet to be demonstrated. In this work, ab initio molecular dynamics and quasielastic neutron scattering are combined to probe anion reorientations and their mechanistic connection to cation mobility over a range of timescales and temperatures. It is found that anions do not rotate freely, but rather transition rapidly between orientations defined by the cation sublattice symmetry. The symmetry-breaking carbon atom in CB11H12- also plays a critical role by perturbing the energy landscape along the instantaneous orientation of the anion dipole, which couples fluctuations in the cation probability density directly to the anion motion. Anion reorientation rates exceed 3 x 1010 s-1, suggesting the underlying energy landscape fluctuates dynamically on diffusion-relevant timescales. Furthermore, carbon is found to modify the orientational preferences of the anions and aid rotational mobility, creating additional symmetry incompatibilities that inhibit ordering. The results suggest that synergy between the anion reorientational dynamics and the carbon-modified cation-anion interaction accounts for the higher ionic conductivity in CB11H12- salts compared with B12H122-.

  5. Single Nanoparticle Plasmonic Sensors

    Directory of Open Access Journals (Sweden)

    Manish Sriram

    2015-10-01

    Full Text Available The adoption of plasmonic nanomaterials in optical sensors, coupled with the advances in detection techniques, has opened the way for biosensing with single plasmonic particles. Single nanoparticle sensors offer the potential to analyse biochemical interactions at a single-molecule level, thereby allowing us to capture even more information than ensemble measurements. We introduce the concepts behind single nanoparticle sensing and how the localised surface plasmon resonances of these nanoparticles are dependent upon their materials, shape and size. Then we outline the different synthetic approaches, like citrate reduction, seed-mediated and seedless growth, that enable the synthesis of gold and silver nanospheres, nanorods, nanostars, nanoprisms and other nanostructures with tunable sizes. Further, we go into the aspects related to purification and functionalisation of nanoparticles, prior to the fabrication of sensing surfaces. Finally, the recent developments in single nanoparticle detection, spectroscopy and sensing applications are discussed.

  6. Nonlinear graphene plasmonics

    Science.gov (United States)

    Ooi, Kelvin J. A.; Tan, Dawn T. H.

    2017-10-01

    The rapid development of graphene has opened up exciting new fields in graphene plasmonics and nonlinear optics. Graphene's unique two-dimensional band structure provides extraordinary linear and nonlinear optical properties, which have led to extreme optical confinement in graphene plasmonics and ultrahigh nonlinear optical coefficients, respectively. The synergy between graphene's linear and nonlinear optical properties gave rise to nonlinear graphene plasmonics, which greatly augments graphene-based nonlinear device performance beyond a billion-fold. This nascent field of research will eventually find far-reaching revolutionary technological applications that require device miniaturization, low power consumption and a broad range of operating wavelengths approaching the far-infrared, such as optical computing, medical instrumentation and security applications.

  7. Quantum theory of plasmon

    International Nuclear Information System (INIS)

    Nguyen, Van Hieu; Nguyen, Bich Ha

    2014-01-01

    Since very early works on plasma oscillations in solids, it was known that in collective excitations (fluctuations of the charge density) of the electron gas there exists the resonance appearing as a quasiparticle of a special type called the plasmon. The elaboration of the quantum theory of plasmon in the framework of the canonical formalism is the purpose of the present work. We start from the establishment of the Lagrangian of the system of itinerant electrons in metal and the definition of the generalized coordinates and velocities of this system. Then we determine the expression of the Hamiltonian and perform the quantization procedure in the canonical formalism. By means of this rigorous method we can derive the expressions of the Hamiltonians of the interactions of plasmon with photon and all quasiparticles in solid from the first principles. (papers)

  8. Surface Plasmon Nanophotonics

    CERN Document Server

    Brongersma, Mark L

    2007-01-01

    The development of advanced dielectric photonic structures has enabled tremendous control over the propagation and manipulation of light. Structures such as waveguides, splitters, mixers, and resonators now play a central role in the telecommunications industry. This book will discuss an exciting new class of photonic devices, known as surface plasmon nanophotonic structures. Surface plasmons are easily accessible excitations in metals and semiconductors and involve a collective motion of the conduction electrons. These excitations can be exploited to manipulate electromagnetic waves at optical frequencies ("light") in new ways that are unthinkable in conventional dielectric structures. The field of plasmon nanophotonics is rapidly developing and impacting a wide range of areas including: electronics, photonics, chemistry, biology, and medicine. The book will highlight several exciting new discoveries that have been made, while providing a clear discussion of the underlying physics, the nanofabrication issues...

  9. Ultrafast X-Ray Spectroscopy of Conical Intersections

    Science.gov (United States)

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

    2018-06-01

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

  10. Terahertz plasmonic Bessel beamformer

    International Nuclear Information System (INIS)

    Monnai, Yasuaki; Shinoda, Hiroyuki; Jahn, David; Koch, Martin; Withayachumnankul, Withawat

    2015-01-01

    We experimentally demonstrate terahertz Bessel beamforming based on the concept of plasmonics. The proposed planar structure is made of concentric metallic grooves with a subwavelength spacing that couple to a point source to create tightly confined surface waves or spoof surface plasmon polaritons. Concentric scatterers periodically incorporated at a wavelength scale allow for launching the surface waves into free space to define a Bessel beam. The Bessel beam defined at 0.29 THz has been characterized through terahertz time-domain spectroscopy. This approach is capable of generating Bessel beams with planar structures as opposed to bulky axicon lenses and can be readily integrated with solid-state terahertz sources

  11. Plasmonic colour laser printing

    DEFF Research Database (Denmark)

    Zhu, Xiaolong; Vannahme, Christoph; Højlund-Nielsen, Emil

    2016-01-01

    -beam lithography (EBL) or focused ion beam (FIB), both expensive and not scalable processes that are not suitable for post-processing customization. Here we show a method of colour printing on nanoimprinted plasmonic metasurfaces using laser post-writing. Laser pulses induce transient local heat generation...... that leads to melting and reshaping of the imprinted nanostructures. Depending on the laser pulse energy density, different surface morphologies that support different plasmonic resonances leading to different colour appearances can be created. Using this technique we can print all primary colours...

  12. Plasmonic transparent conductors

    Science.gov (United States)

    Liapis, Andreas C.; Sfeir, Matthew Y.; Black, Charles T.

    2016-09-01

    Many of today's technological applications, such as solar cells, light-emitting diodes, displays, and touch screens, require materials that are simultaneously optically transparent and electrically conducting. Here we explore transparent conductors based on the excitation of surface plasmons in nanostructured metal films. We measure both the optical and electrical properties of films perforated with nanometer-scale features and optimize the design parameters in order to maximize optical transmission without sacrificing electrical conductivity. We demonstrate that plasmonic transparent conductors can out-perform indium tin oxide in terms of both their transparency and their conductivity.

  13. Origin of optical non-linear response in TiN owing to excitation dynamics of surface plasmon resonance electronic oscillations

    Science.gov (United States)

    Divya, S.; Nampoori, V. P. N.; Radhakrishnan, P.; Mujeeb, A.

    2014-08-01

    TiN nanoparticles of average size 55 nm were investigated for their optical non-linear properties. During the experiment the irradiated laser wavelength coincided with the surface plasmon resonance (SPR) peak of the nanoparticle. The large non-linearity of the nanoparticle was attributed to the plasmon resonance, which largely enhanced the local field within the nanoparticle. Both open and closed aperture Z-scan experiments were performed and the corresponding optical constants were explored. The post-excitation absorption spectra revealed the interesting phenomenon of photo fragmentation leading to the blue shift in band gap and red shift in the SPR. The results are discussed in terms of enhanced interparticle interaction simultaneous with size reduction. Here, the optical constants being intrinsic constants for a particular sample change unusually with laser power intensity. The dependence of χ(3) is discussed in terms of the size variation caused by photo fragmentation. The studies proved that the TiN nanoparticles are potential candidates in photonics technology offering huge scope to study unexplored research for various expedient applications.

  14. Magnetic field effects on ultrafast lattice compression dynamics of Si(111) crystal when excited by linearly-polarized femtosecond laser pulses

    Science.gov (United States)

    Hatanaka, Koji; Odaka, Hideho; Ono, Kimitoshi; Fukumura, Hiroshi

    2007-03-01

    Time-resolved X-ray diffraction measurements of Si (111) single crystal are performed when excited by linearly-polarized femtosecond laser pulses (780 nm, 260 fs, negatively-chirped, 1 kHz) under a magnetic field (0.47 T). Laser fluence on the sample surface is 40 mJ/cm^2, which is enough lower than the ablation threshold at 200 mJ/cm^2. Probing X-ray pulses of iron characteristic X-ray lines at 0.193604 and 0.193998 nm are generated by focusing femtosecond laser pulses onto audio-cassette tapes in air. Linearly-polarized femtosecond laser pulse irradiation onto Si(111) crystal surface induces transient lattice compression in the picosecond time range, which is confirmed by transient angle shift of X-ray diffraction to higher angles. Little difference of compression dynamics is observed when the laser polarization is changed from p to s-pol. without a magnetic field. On the other hand, under a magnetic field, the lattice compression dynamics changes when the laser is p-polarized which is vertical to the magnetic field vector. These results may be assigned to photo-carrier formation and energy-band distortion.

  15. Ultrafast MR Imaging in Pediatric Neuroradiology

    International Nuclear Information System (INIS)

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

    2003-01-01

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

  16. Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-01-01

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

  17. Array of nanoparticles coupling with quantum-dot: Lattice plasmon quantum features

    Science.gov (United States)

    Salmanogli, Ahmad; Gecim, H. Selcuk

    2018-06-01

    In this study, we analyze the interaction of lattice plasmon with quantum-dot in order to mainly examine the quantum features of the lattice plasmon containing the photonic/plasmonic properties. Despite optical properties of the localized plasmon, the lattice plasmon severely depends on the array geometry, which may influence its quantum features such as uncertainty and the second-order correlation function. To investigate this interaction, we consider a closed system containing an array of the plasmonic nanoparticles and quantum-dot. We analyze this system with full quantum theory by which the array electric far field is quantized and the strength coupling of the quantum-dot array is analytically calculated. Moreover, the system's dynamics are evaluated and studied via the Heisenberg-Langevin equations to attain the system optical modes. We also analytically examine the Purcell factor, which shows the effect of the lattice plasmon on the quantum-dot spontaneous emission. Finally, the lattice plasmon uncertainty and its time evolution of the second-order correlation function at different spatial points are examined. These parameters are dramatically affected by the retarded field effect of the array nanoparticles. We found a severe quantum fluctuation at points where the lattice plasmon occurs, suggesting that the lattice plasmon photons are correlated.

  18. Plasmonics light modulators

    DEFF Research Database (Denmark)

    Babicheva, Viktoriia; Malureanu, Radu; Lavrinenko, Andrei

    Surface plasmon polaritons (SPPs) are waves propagating at the interface between a metal and a dielectric and, due to their tight confinement, may be used for nanoscale control of the light propagation. Thus, photonic integrated circuits can benefit from devices using SPPs because of their highly...

  19. Ultrafast Thermal Transport at Interfaces

    Energy Technology Data Exchange (ETDEWEB)

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

    2014-10-21

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

  20. Use of ultrafast dispersed pump-dump-probe and pump-repump-probe spectroscopies to explore the light-induced dynamics of peridinin in solution.

    Science.gov (United States)

    Papagiannakis, Emmanouil; Vengris, Mikas; Larsen, Delmar S; van Stokkum, Ivo H M; Hiller, Roger G; van Grondelle, Rienk

    2006-01-12

    Optical pump-induced dynamics of the highly asymmetric carotenoid peridinin in methanol was studied by dispersed pump-probe, pump-dump-probe, and pump-repump-probe transient absorption spectroscopy in the visible region. Dispersed pump-probe measurements show that the decay of the initially excited S2 state populates two excited states, the S1 and the intramolecular charge-transfer (ICT) state, at a ratio determined by the excitation wavelength. The ensuing spectral evolution occurs on the time scale of a few picoseconds and suggests the equilibration of these states. Dumping the stimulated emission of the ICT state with an additional 800-nm pulse after 400- and 530-nm excitation preferentially removes the ICT state contribution from the broad excited-state absorption, allowing for its spectral characterization. At the same time, an unrelaxed ground-state species, which has a subpicosecond lifetime, is populated. The application of the 800-nm pulse at early times, when the S2 state is still populated, led to direct generation of the peridinin cation, observed for the first time in a transient absorption experiment. The excited and ground electronic states manifold of peridinin has been reconstructed using target analysis; this approach combined with the measured multipulse spectroscopic data allows us to estimate the spectra and time scales of the corresponding transient states.

  1. Ultrafast, laser-based, x-ray science: the dawn of atomic-scale cinematography

    International Nuclear Information System (INIS)

    Barty, C.P.J.

    2000-01-01

    The characteristics of ultrafast chirped pulse amplification systems are reviewed. Application of ultrafast chirped pulse amplification to the generation of femtosecond, incoherent, 8-keV line radiation is outlined and the use of femtosecond laser-based, x-rays for novel time-resolved diffraction studies of crystalline dynamics with sub-picosecond temporal resolution and sub-picometer spatial resolution is reviewed in detail. Possible extensions of laser-based, x-ray technology and evaluation of alternative x-ray approaches for time-resolved studies of the atomic scale dynamics are given. (author)

  2. Ultrafast, laser-based, x-ray science: the dawn of atomic-scale cinematography

    Energy Technology Data Exchange (ETDEWEB)

    Barty, C.P.J. [University of California, Department of Applied Mechanics and Engineering Science, Urey Hall, Mali Code 0339, San Diego, La Jolla, CA (United States)

    2000-03-01

    The characteristics of ultrafast chirped pulse amplification systems are reviewed. Application of ultrafast chirped pulse amplification to the generation of femtosecond, incoherent, 8-keV line radiation is outlined and the use of femtosecond laser-based, x-rays for novel time-resolved diffraction studies of crystalline dynamics with sub-picosecond temporal resolution and sub-picometer spatial resolution is reviewed in detail. Possible extensions of laser-based, x-ray technology and evaluation of alternative x-ray approaches for time-resolved studies of the atomic scale dynamics are given. (author)

  3. Ultrafast comparison of personal genomes

    OpenAIRE

    Mauldin, Denise; Hood, Leroy; Robinson, Max; Glusman, Gustavo

    2017-01-01

    We present an ultra-fast method for comparing personal genomes. We transform the standard genome representation (lists of variants relative to a reference) into 'genome fingerprints' that can be readily compared across sequencing technologies and reference versions. Because of their reduced size, computation on the genome fingerprints is fast and requires little memory. This enables scaling up a variety of important genome analyses, including quantifying relatedness, recognizing duplicative s...

  4. Entangled plasmon generation in nonlinear spaser system under the action of external magnetic field

    Science.gov (United States)

    Gubin, M. Yu.; Shesterikov, A. V.; Karpov, S. N.; Prokhorov, A. V.

    2018-02-01

    The present paper theoretically investigates features of quantum dynamics for localized plasmons in three-particle or four-particle spaser systems consisting of metal nanoparticles and semiconductor quantum dots. In the framework of the mean field approximation, the conditions for the observation of stable stationary regimes for single-particle plasmons in spaser systems are revealed, and realization of these regimes is discussed. The strong dipole-dipole interaction between adjacent nanoparticles for the four-particle spaser system is investigated. We show that this interaction can lead to the decreasing of the autocorrelation function values for plasmons. The generation of entangled plasmons in a three-particle spaser system with nonlinear plasmon-exciton interaction is predicted. The use of an external magnetic field is proposed for control of the cross correlations between plasmons in the three-particle spaser system.

  5. Modeling of ultrafast THz interactions in molecular crystals

    DEFF Research Database (Denmark)

    Pedersen, Pernille Klarskov; Clark, Stewart J.; Jepsen, Peter Uhd

    2014-01-01

    In this paper we present a numerical study of terahertz pulses interacting with crystals of cesium iodide. We model the molecular dynamics of the cesium iodide crystals with the Density Functional Theory software CASTEP, where ultrafast terahertz pulses are implemented to the CASTEP software...... to interact with molecular crystals. We investigate the molecular dynamics of cesium iodide crystals when interacting with realistic terahertz pulses of field strengths from 0 to 50 MV/cm. We find nonlinearities in the response of the CsI crystals at field strengths higher than 10 MV/cm....

  6. Desolvation of polymers by ultrafast heating: Influence of hydrophilicity

    Science.gov (United States)

    Sun, Si Neng; Urbassek, Herbert M.

    2010-10-01

    Using molecular-dynamics simulation, we investigate the consequences of ultrafast laser-induced heating of a small water droplet containing a solvated polymer. Two polymers are studied: polyethylene as an example of a hydrophobic, and polyketone as an example of a hydrophilic polymer. In both cases, when the droplet is heated below the critical temperature of water, strong water evaporation is started, but the polymer remains in contact with a central water cluster. However, upon heating beyond the critical temperature, the hydrophilic polyethylene becomes completely desolvated, while polyketone still remains solvated. We analyze this behavior in terms of the intermolecular interactions and of the expansion dynamics of the heated droplet.

  7. Fano coil-type resonances: a plasmonic tool for the magnetic field manipulation (Conference Presentation)

    Science.gov (United States)

    Panaro, Simone; Proietti Zaccaria, Remo; Toma, Andrea

    2017-02-01

    Spintronics and spin-based technology rely on the ultra-fast unbalance of the electronic spin population in quite localized spatial regions. However, as a matter of fact, the low susceptibility of conventional materials at high frequencies strongly limits these phenomena, rendering the efficiency of magnetically active devices insufficient for application purposes. Among the possible strategies which can be envisaged, plasmonics offers a direct approach to increase the effect of local electronic unbalancing processes. By confining and enhancing free radiation in nm-size spatial regions, plasmonic nano-assemblies have demonstrated to support very intense electric and magnetic hot-spots. In particular, very recent studies have proven the fine control of magnetic fields in Fano resonance condition. The near-field-induced out-of-phase oscillation of localized surface plasmons has manifested itself with the arising of magnetic sub-diffractive hot-spots. Here, we show how this effect can be further boosted in the mid-infrared regime via the introduction of higher order plasmonic modes. The investigated system, namely Moon Trimer Resonator (MTR), combines the high efficiency of a strongly coupled nano-assembly in Fano interferential condition with the elevated tunability of the quadrupolar resonance supported by a moon-like geometry. The fine control of the apical gap in this unique nanostructure, characterizes a plasmonic device able to tune its resonance without any consequence on the magnetic hot-spot size, thus enabling an efficient squeezing in the infrared.

  8. Plasmonic Organic Photovoltaics: Unraveling Plasmonic Enhancement for Realistic Cell Geometries

    DEFF Research Database (Denmark)

    Beliatis, Michail

    2018-01-01

    Incorporating plasmonic nanoparticles in organic photovoltaic (OPV) devices can increase the optical thickness of the organic absorber layer while keeping its physical thickness small. However, trade-offs between various structure parameters have caused contradictions regarding the effectiveness...... of plasmonics in the literature, that have somewhat stunted the progressing of a unified theoretical understanding for practical applications. We examine the optical enhancement mechanisms of practical PCDTBT:PC70BM OPV cells incorporating metal nanoparticles. The plasmonic near- and far-field contributions...... show that an already optimized PCDTBT:PC70BM cell can be further optically enhanced by plasmonic effects by at least 20% with the incorporation of Ag nanoparticles....

  9. Photoinduced Electron Transfer in the Strong Coupling Regime: Waveguide-Plasmon Polaritons.

    Science.gov (United States)

    Zeng, Peng; Cadusch, Jasper; Chakraborty, Debadi; Smith, Trevor A; Roberts, Ann; Sader, John E; Davis, Timothy J; Gómez, Daniel E

    2016-04-13

    Reversible exchange of photons between a material and an optical cavity can lead to the formation of hybrid light-matter states where material properties such as the work function [ Hutchison et al. Adv. Mater. 2013 , 25 , 2481 - 2485 ], chemical reactivity [ Hutchison et al. Angew. Chem., Int. Ed. 2012 , 51 , 1592 - 1596 ], ultrafast energy relaxation [ Salomon et al. Angew. Chem., Int. Ed. 2009 , 48 , 8748 - 8751 ; Gomez et al. J. Phys. Chem. B 2013 , 117 , 4340 - 4346 ], and electrical conductivity [ Orgiu et al. Nat. Mater. 2015 , 14 , 1123 - 1129 ] of matter differ significantly to those of the same material in the absence of strong interactions with the electromagnetic fields. Here we show that strong light-matter coupling between confined photons on a semiconductor waveguide and localized plasmon resonances on metal nanowires modifies the efficiency of the photoinduced charge-transfer rate of plasmonic derived (hot) electrons into accepting states in the semiconductor material. Ultrafast spectroscopy measurements reveal a strong correlation between the amplitude of the transient signals, attributed to electrons residing in the semiconductor and the hybridization of waveguide and plasmon excitations.

  10. Tunneling Plasmonics in Bilayer Graphene.

    Science.gov (United States)

    Fei, Z; Iwinski, E G; Ni, G X; Zhang, L M; Bao, W; Rodin, A S; Lee, Y; Wagner, M; Liu, M K; Dai, S; Goldflam, M D; Thiemens, M; Keilmann, F; Lau, C N; Castro-Neto, A H; Fogler, M M; Basov, D N

    2015-08-12

    We report experimental signatures of plasmonic effects due to electron tunneling between adjacent graphene layers. At subnanometer separation, such layers can form either a strongly coupled bilayer graphene with a Bernal stacking or a weakly coupled double-layer graphene with a random stacking order. Effects due to interlayer tunneling dominate in the former case but are negligible in the latter. We found through infrared nanoimaging that bilayer graphene supports plasmons with a higher degree of confinement compared to single- and double-layer graphene, a direct consequence of interlayer tunneling. Moreover, we were able to shut off plasmons in bilayer graphene through gating within a wide voltage range. Theoretical modeling indicates that such a plasmon-off region is directly linked to a gapped insulating state of bilayer graphene, yet another implication of interlayer tunneling. Our work uncovers essential plasmonic properties in bilayer graphene and suggests a possibility to achieve novel plasmonic functionalities in graphene few-layers.

  11. Ultrafast Hierarchical OTDM/WDM Network

    Directory of Open Access Journals (Sweden)

    Hideyuki Sotobayashi

    2003-12-01

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

  12. Avant-Garde Ultrafast Laser Writing

    Directory of Open Access Journals (Sweden)

    Kazansky P. G.

    2013-11-01

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

  13. Ultrafast Science Opportunities with Electron Microscopy

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-04-28

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

  14. Energy transfer in plasmonic systems

    International Nuclear Information System (INIS)

    Pustovit, Vitaliy N; Urbas, Augustine M; Shahbazyan, Tigran V

    2014-01-01

    We present our results on energy transfer between donor and acceptor molecules or quantum dots near a plasmonic nanoparticle. In such systems, the Förster resonance energy transfer is strongly modified due to plasmon-mediated coupling between donors and acceptors. The transfer efficiency is determined by a competition between transfer, radiation and dissipation that depends sensitively on system parameters. When donor and accepror spectral bands overlap with dipole surface plasmon resonance, the dominant transfer mechanism is through plasmon-enhanced radiative coupling. When transfer takes place from an ensemble of donors to an acceptor, a cooperative amplification of energy transfer takes place in a wide range of system parameters. (paper)

  15. An Introduction to Graphene Plasmonics

    DEFF Research Database (Denmark)

    Gonçalves, P.A.D.; Peres, N. M. R.

    This book is meant as an introduction to graphene plasmonics and aims at the advanced undergraduate and graduate students entering the field of plasmonics in graphene. In it different theoretical methods are introduced, starting with an elementary description of graphene plasmonics and evolving...... the chapters to get acquainted with the field of plasmonics in graphene or reading the chapters and studying the appendices to get a working knowledge of the topic. The study of the material in this book will bring the students to the forefront of the research in this field....

  16. Coulomb Blockade Plasmonic Switch.

    Science.gov (United States)

    Xiang, Dao; Wu, Jian; Gordon, Reuven

    2017-04-12

    Tunnel resistance can be modulated with bias via the Coulomb blockade effect, which gives a highly nonlinear response current. Here we investigate the optical response of a metal-insulator-nanoparticle-insulator-metal structure and show switching of a plasmonic gap from insulator to conductor via Coulomb blockade. By introducing a sufficiently large charging energy in the tunnelling gap, the Coulomb blockade allows for a conductor (tunneling) to insulator (capacitor) transition. The tunnelling electrons can be delocalized over the nanocapacitor again when a high energy penalty is added with bias. We demonstrate that this has a huge impact on the plasmonic resonance of a 0.51 nm tunneling gap with ∼70% change in normalized optical loss. Because this structure has a tiny capacitance, there is potential to harness the effect for high-speed switching.

  17. Surface Plasmon Singularities

    Directory of Open Access Journals (Sweden)

    Gabriel Martínez-Niconoff

    2012-01-01

    Full Text Available With the purpose to compare the physical features of the electromagnetic field, we describe the synthesis of optical singularities propagating in the free space and on a metal surface. In both cases the electromagnetic field has a slit-shaped curve as a boundary condition, and the singularities correspond to a shock wave that is a consequence of the curvature of the slit curve. As prototypes, we generate singularities that correspond to fold and cusped regions. We show that singularities in free space may generate bifurcation effects while plasmon fields do not generate these kinds of effects. Experimental results for free-space propagation are presented and for surface plasmon fields, computer simulations are shown.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-06-23

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

  19. Plasmons in strong superconductors

    International Nuclear Information System (INIS)

    Baldo, M.; Ducoin, C.

    2011-01-01

    We present a study of the possible plasmon excitations that can occur in systems where strong superconductivity is present. In these systems the plasmon energy is comparable to or smaller than the pairing gap. As a prototype of these systems we consider the proton component of Neutron Star matter just below the crust when electron screening is not taken into account. For the realistic case we consider in detail the different aspects of the elementary excitations when the proton, electron components are considered within the Random-Phase Approximation generalized to the superfluid case, while the influence of the neutron component is considered only at qualitative level. Electron screening plays a major role in modifying the proton spectrum and spectral function. At the same time the electron plasmon is strongly modified and damped by the indirect coupling with the superfluid proton component, even at moderately low values of the gap. The excitation spectrum shows the interplay of the different components and their relevance for each excitation modes. The results are relevant for neutrino physics and thermodynamical processes in neutron stars. If electron screening is neglected, the spectral properties of the proton component show some resemblance with the physical situation in high-T c superconductors, and we briefly discuss similarities and differences in this connection. In a general prospect, the results of the study emphasize the role of Coulomb interaction in strong superconductors.

  20. A nonlinear plasmonic waveguide based all-optical bidirectional switching

    Science.gov (United States)

    Bana, Xiaoqiang; Pang, Xingxing; Li, Xiaohui; Hu, Bin; Guo, Yixuan; Zheng, Hairong

    2018-01-01

    In this paper, an all-optical switching with a nanometer coupled ring resonator is demonstrated based on the nonlinear material. By adjusting the light intensity, we implement the resonance wavelength from 880 nm to 940 nm in the nonlinear material structure monocyclic. In the bidirectional switch structure, the center wavelength (i.e. 880 nm) is fixed. By changing the light intensity from I = 0 to I = 53 . 1 MW /cm2, the function of optical switching can be obtained. The results demonstrate that both the single-ring cavity and the T-shaped double-ring structure can realize the optical switching effect. This work takes advantage of the simple structure. The single-ring cavity plasmonic switches have many advantages, such as nanoscale size, low pumping light intensity, ultrafast response time (femtosecond level), etc. It is expected that the proposed all-optical integrated devices can be potentially applied in optical communication, signal processing, and signal sensing, etc.

  1. Plasmon-plasmon coupling in nested fullerenes: photoexcitation of interlayer plasmonic cross modes

    International Nuclear Information System (INIS)

    McCune, Mathew A; De, Ruma; Chakraborty, Himadri S; Madjet, Mohamed E; Manson, Steven T

    2011-01-01

    Considering the photoionization of a two-layer fullerene-onion system, C 60 -C 240 , strong plasmonic couplings between the nested fullerenes are demonstrated. The resulting hybridization produces four cross-over plasmons generated from the bonding and antibonding mixing of excited charge clouds of individual fullerenes. This suggests the possibility of designing buckyonions exhibiting plasmon resonances with specified properties and may motivate future research to modify the resonances with encaged atoms, molecules or clusters. (fast track communication)

  2. Impact system for ultrafast synchrotron experiments

    International Nuclear Information System (INIS)

    Jensen, B. J.; Owens, C. T.; Ramos, K. J.; Yeager, J. D.; Saavedra, R. A.; Luo, S. N.; Hooks, D. E.; Iverson, A. J.; Fezzaa, K.

    2013-01-01

    The impact system for ultrafast synchrotron experiments, or IMPULSE, is a 12.6-mm bore light-gas gun (<1 km/s projectile velocity) designed specifically for performing dynamic compression experiments using the advanced imaging and X-ray diffraction methods available at synchrotron sources. The gun system, capable of reaching projectile velocities up to 1 km/s, was designed to be portable for quick insertion/removal in the experimental hutch at Sector 32 ID-B of the Advanced Photon Source (Argonne, IL) while allowing the target chamber to rotate for sample alignment with the beam. A key challenge in using the gun system to acquire dynamic data on the nanosecond time scale was synchronization (or bracketing) of the impact event with the incident X-ray pulses (80 ps width). A description of the basic gun system used in previous work is provided along with details of an improved launch initiation system designed to significantly reduce the total system time from launch initiation to impact. Experiments were performed to directly measure the gun system time and to determine the gun performance curve for projectile velocities ranging from 0.3 to 0.9 km/s. All results show an average system time of 21.6 ± 4.5 ms, making it possible to better synchronize the gun system and detectors to the X-ray beam.

  3. Surface plasmon polariton propagation in organic nanofiber based plasmonic waveguides

    DEFF Research Database (Denmark)

    Leißner, Till; Lemke, Christoph; Jauernik, Stephan

    2013-01-01

    Plasmonic wave packet propagation is monitored in dielectric-loaded surface plasmon polariton waveguides realized from para-hexaphenylene nanofibers deposited onto a 60 nm thick gold film. Using interferometric time resolved two-photon photoemission electron microscopy we are able to determine...

  4. Graphene plasmonics: physics and potential applications

    Directory of Open Access Journals (Sweden)

    Huang Shenyang

    2016-10-01

    Full Text Available Plasmon in graphene possesses many unique properties. It originates from the collective motion of massless Dirac fermions, and the carrier density dependence is distinctively different from conventional plasmons. In addition, graphene plasmon is highly tunable and shows strong energy confinement capability. Most intriguingly, as an atom-thin layer, graphene and its plasmon are very sensitive to the immediate environment. Graphene plasmons strongly couple to polar phonons of the substrate, molecular vibrations of the adsorbates, and lattice vibrations of other atomically thin layers. In this review, we present the most important advances in graphene plasmonics field. The topics include terahertz plasmons, mid-infrared plasmons, plasmon-phonon interactions, and potential applications. Graphene plasmonics opens an avenue for reconfigurable metamaterials and metasurfaces; it is an exciting and promising new subject in the nanophotonics and plasmonics research field.

  5. Chapter IV: ultrafast biochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Chergui, M. [Swiss Federal Institute of Technology (EPFL), Lausanne (Switzerland); Kjelstrup, S. [Norwegian University of Science and Technology (NTNU), Trondheim (Norway); Meuwly, M. [Universitaet Basel, Basel (Switzerland); Schuler, B. [University of Zuerich (ETH), Zurich (Switzerland); Thor, J. van [Imperial College London (IC), London (United Kingdom)

    2009-09-15

    The whole report issued by the Paul Scherrer Institute (PSI) in Switzerland takes a look at the scientific opportunities offered by the institute's SwissFEL X-ray Laser facility. In this sixth part, initial events and fluctuations in biochemical processes at the atomic scale are discussed. Sub-nanosecond processes are fundamental to biochemistry and will be accessible to the ultra-short pulses of the SwissFEL. Time and length scales of biochemical reactions are discussed, as is the photo-initiation of biochemical processes. Time-resolved measurement techniques are looked at. Fluorescence resonant energy transfer is discussed. As an example, the photo cycle of bacteriorhodopsin is examined. The dynamics of protein folding and catalytic action are also looked at. Mesoscopic non-equilibrium thermodynamics is discussed

  6. Ultrafast excited-state dynamics of isocytosine

    Czech Academy of Sciences Publication Activity Database

    Szabla, Rafal; Gora, R.W.; Šponer, Jiří

    2016-01-01

    Roč. 18, č. 30 (2016), s. 20208-20218 ISSN 1463-9076 R&D Projects: GA ČR(CZ) GA14-12010S Institutional support: RVO:68081707 Keywords : perturbation-theory * relaxation mechanisms Subject RIV: BO - Biophysics Impact factor: 4.123, year: 2016

  7. Ultrafast dynamics of electrons at interfaces

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-05-03

    Electronic states of a thin layer of material on a surface possess unique physical and chemical properties. Some of these properties arise from the reduced dimensionality of the thin layer with respect to the bulk or the properties of the electric field where two materials of differing dielectric constants meet at an interface. Other properties are related to the nature of the surface chemical bond. Here, the properties of excess electrons in thin layers of Xenon, Krypton, and alkali metals are investigated, and the bound state energies and effective masses of the excess electrons are determined using two-photon photoemission. For Xenon, the dependence of bound state energy, effective mass, and lifetime on layer thickness from one to nine layers is examined. Not all quantities were measured at each coverage. The two photon photoemission spectra of thin layers of Xenon on a Ag(111) substrate exhibit a number of sharp, well-defined peaks. The binding energy of the excess electronic states of Xenon layers exhibited a pronounced dependence on coverage. A discrete energy shift was observed for each additional atomic layer. At low coverage, a series of states resembling a Rydberg series is observed. This series is similar to the image state series observed on clean metal surfaces. Deviations from image state energies can be described in terms of the dielectric constant of the overlayer material and its effect on the image potential. For thicker layers of Xe (beyond the first few atomic layers), the coverage dependence of the features begins to resemble that of quantum well states. Quantum well states are related to bulk band states. However, the finite thickness of the layer restricts the perpendicular wavevector to a discrete set of values. Therefore, the spectrum of quantum well states contains a series of peaks which correspond to the various allowed values of the perpendicular wavevector. Analysis of the quantum well spectrum yields electronic band structure information. In this case, the quantum well states examined are derived from the Xenon conduction band. Measurements of the energies as a function of coverage yield the dispersion along the axis perpendicular to the surface while angle-resolved two-photon photoemission measurements yield information about dispersion along the surface parallel. The relative importance of the image potential and the overlayer band structure also depends on the quantum number and energy of the state. Some members of the image series may have an energy which is in an energy gap of the layer material, therefore such states may tend to remain physically outside the layer and retain much of their image character even at higher coverages. This is the case for the n = 1 image state of the Xe/Ag(111) system. The energies of image states which are excluded from the layer have a complex dependence on the thickness of the layer and its dielectric constant. The population decay kinetics of excited electronic states of the layer were also determined. Lifetimes are reported for the first three excited states for 1-6 atomic layers of Xe on Ag(111). As the image states evolve into quantum well states with increasing coverage, the lifetimes undergo an oscillation which marks a change in the spatial extent of the state. For example, the n = 2 quantum well state decreases substantially at 3-5 layers as the electron probability density in the layer increases. The lifetime data are modeled by extending the two-band nearly-free-electron approximation to account for the insulating Xe layer.

  8. Intensified CCD for ultrafast diagnostics

    International Nuclear Information System (INIS)

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

    1978-01-01

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

  9. Compression of Ultrafast Laser Beams

    Science.gov (United States)

    2016-03-01

    Copyright 2003, AIP Publishing LLC. DOI: http://dx.doi.org/10.1063/1.1611998.) When designing the pulse shaper, the laser beam must completely fill the...for the design of future versions of this device. The easiest way to align the pulse shaper is to use the laser beam that will be shaped, without...Afterward, an ultrafast thin beam splitter is placed into the system after the diameter of the laser beam is reduced; this is done to monitor the beam

  10. Ultrafast Charge Photogeneration in MEH-PPV Charge-Transfer Complexes

    NARCIS (Netherlands)

    Bakulin, Artem A.; Paraschuk, Dmitry Yu; Pshenichnikov, Maxim S.; van Loosdrecht, Paul H. M.; Corkum, P; DeSilvestri, S; Nelson, KA; Riedle, E; Schoenlein, RW

    2009-01-01

    Visible-pump - IR-probe spectroscopy is used to study the ultrafast charge dynamics in MEH-PPV based charge-transfer complexes and donor-acceptor blends. Transient anisotropy of the polymer polaron band provides invaluable insights into excitation localisation and charge-transfer pathways.

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

    NARCIS (Netherlands)

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

    2016-01-01

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

  12. Plasmon-exciton-polariton lasing

    NARCIS (Netherlands)

    Ramezani, M.; Halpin, A.; Fernandez, A. I.; Feist, J.; Rodriguez, S. R. K.; Garcia-Vidal, F. J.; J. Gomez Rivas,

    2017-01-01

    Metallic nanostructures provide a toolkit for the generation of coherent light below the diffraction limit. Plasmonic-based lasing relies on the population inversion of emitters (such as organic fluorophores) along with feedback provided by plasmonic resonances. In this regime, known as weak

  13. Interference effects with surface plasmons

    NARCIS (Netherlands)

    Kuzmin, Nikolay Victorovich

    2008-01-01

    A surface plasmon is a purely two-dimensional electromagnetic excitation bound to the interface between metal and dielectric and quickly decaying away from it. A surface plasmon is able to concentrate light on sub-wavelength scales – a feature that is attractive for nano-photonics and integrated

  14. Quantum interference in plasmonic circuits.

    Science.gov (United States)

    Heeres, Reinier W; Kouwenhoven, Leo P; Zwiller, Valery

    2013-10-01

    Surface plasmon polaritons (plasmons) are a combination of light and a collective oscillation of the free electron plasma at metal/dielectric interfaces. This interaction allows subwavelength confinement of light beyond the diffraction limit inherent to dielectric structures. As a result, the intensity of the electromagnetic field is enhanced, with the possibility to increase the strength of the optical interactions between waveguides, light sources and detectors. Plasmons maintain non-classical photon statistics and preserve entanglement upon transmission through thin, patterned metallic films or weakly confining waveguides. For quantum applications, it is essential that plasmons behave as indistinguishable quantum particles. Here we report on a quantum interference experiment in a nanoscale plasmonic circuit consisting of an on-chip plasmon beamsplitter with integrated superconducting single-photon detectors to allow efficient single plasmon detection. We demonstrate a quantum-mechanical interaction between pairs of indistinguishable surface plasmons by observing Hong-Ou-Mandel (HOM) interference, a hallmark non-classical interference effect that is the basis of linear optics-based quantum computation. Our work shows that it is feasible to shrink quantum optical experiments to the nanoscale and offers a promising route towards subwavelength quantum optical networks.

  15. Ultrafast gain recovery and modulation limitations in self-assembled quantum-dot devices

    DEFF Research Database (Denmark)

    Berg, Tommy Winther; Bischoff, Svend; Magnúsdóttir, Ingibjörg

    2001-01-01

    Measurements of ultrafast gain recovery in self-assembled InAs quantum-dot (QD) amplifiers are explained by a comprehensive numerical model. The on excited state carriers are found to act as a reservoir for the optically active ground state carriers resulting in an ultrafast gain recovery as long...... as the excited state is well populated. However, when pulses are injected into the device at high-repetition frequencies, the response of a on amplifier is found to be limited by the wetting-layer dynamics....

  16. Multilayer-WS2:ferroelectric composite for ultrafast tunable metamaterial-induced transparency applications

    Science.gov (United States)

    Yang, Xiaoyu; Yang, Jinghuan; Hu, Xiaoyong; Zhu, Yu; Yang, Hong; Gong, Qihuang

    2015-08-01

    An ultrafast and low-power all-optical tunable metamaterial-induced transparency is realized, using polycrystalline barium titanate doped gold nanoparticles and multilayer tungsten disulfide microsheets as nonlinear optical materials. Large nonlinearity enhancement is obtained associated with quantum confinement effect, local-field effect, and reinforced interaction between light and multilayer tungsten disulfide. Low threshold pump intensity of 20 MW/cm2 is achieved. An ultrafast response time of 85 ps is maintained because of fast carrier relaxation dynamics in nanoscale crystal grains of polycrystalline barium titanate. This may be useful for the study of integrated photonic devices based on two-dimensional materials.

  17. Multilayer-WS2:ferroelectric composite for ultrafast tunable metamaterial-induced transparency applications

    International Nuclear Information System (INIS)

    Yang, Xiaoyu; Yang, Jinghuan; Zhu, Yu; Yang, Hong; Hu, Xiaoyong; Gong, Qihuang

    2015-01-01

    An ultrafast and low-power all-optical tunable metamaterial-induced transparency is realized, using polycrystalline barium titanate doped gold nanoparticles and multilayer tungsten disulfide microsheets as nonlinear optical materials. Large nonlinearity enhancement is obtained associated with quantum confinement effect, local-field effect, and reinforced interaction between light and multilayer tungsten disulfide. Low threshold pump intensity of 20 MW/cm 2 is achieved. An ultrafast response time of 85 ps is maintained because of fast carrier relaxation dynamics in nanoscale crystal grains of polycrystalline barium titanate. This may be useful for the study of integrated photonic devices based on two-dimensional materials

  18. A cross-stacked plasmonic nanowire network for high-contrast femtosecond optical switching.

    Science.gov (United States)

    Lin, Yuanhai; Zhang, Xinping; Fang, Xiaohui; Liang, Shuyan

    2016-01-21

    We report an ultrafast optical switching device constructed by stacking two layers of gold nanowires into a perpendicularly crossed network, which works at a speed faster than 280 fs with an on/off modulation depth of about 22.4%. The two stacks play different roles in enhancing consistently the optical switching performance due to their different dependence on the polarization of optical electric fields. The cross-plasmon resonance based on the interaction between the perpendicularly stacked gold nanowires and its Fano-coupling with Rayleigh anomaly is the dominant mechanism for such a high-contrast optical switching device.

  19. Enhanced absorption of graphene in the visible region by use of plasmonic nanostructures

    DEFF Research Database (Denmark)

    Hashemi, Mahdieh; Farzad, Mahmood Hosseini; Mortensen, N. Asger

    2013-01-01

    Low absorption of graphene in the visible range of the spectrum makes it difficult to uniquely benefit from this material in ultra-fast optoelectronic applications. We numerically propose to utilize patterned metallic nanostructures to increase light absorption in single-layer graphene. Simulation...... results show that excitation of surface plasmon resonances in the metallic nanostructures significantly enhances the local electromagnetic field near the graphene layer, therefore leading to a dramatic enhancement of the absorption in the graphene layer itself. Broadband high optical absorption can...

  20. Plasmon holographic experiments: theoretical framework

    International Nuclear Information System (INIS)

    Verbeeck, J.; Dyck, D. van; Lichte, H.; Potapov, P.; Schattschneider, P.

    2005-01-01

    A theoretical framework is described to understand the results of plasmon holography experiments leading to insight in the meaning of the experimental results and pointing out directions for future experiments. The framework is based on the formalism of mutual intensity to describe how coherence is transferred through an optical system. For the inelastic interaction with the object, an expression for the volume plasmon excitations in a free electron gas is used as a model for the behaviour of aluminium. The formalism leads to a clear graphical intuitive tool for understanding the experiments. It becomes evident that the measured coherence is solely related to the angular distribution of the plasmon scattering in the case of bulk plasmons. After describing the framework, the special case of coherence outside a spherical particle is treated and the seemingly controversial idea of a plasmon with a limited coherence length obtained from experiments is clarified

  1. Active components for integrated plasmonic circuits

    DEFF Research Database (Denmark)

    Krasavin, A.V.; Bolger, P.M.; Zayats, A.V.

    2009-01-01

    We present a comprehensive study of highly efficient and compact passive and active components for integrated plasmonic circuit based on dielectric-loaded surface plasmon polariton waveguides.......We present a comprehensive study of highly efficient and compact passive and active components for integrated plasmonic circuit based on dielectric-loaded surface plasmon polariton waveguides....

  2. Partial Polarization in Interfered Plasmon Fields

    Directory of Open Access Journals (Sweden)

    P. Martínez Vara

    2014-01-01

    Full Text Available We describe the polarization features for plasmon fields generated by the interference between two elemental surface plasmon modes, obtaining a set of Stokes parameters which allows establishing a parallelism with the traditional polarization model. With the analysis presented, we find the corresponding coherence matrix for plasmon fields incorporating to the plasmon optics the study of partial polarization effects.

  3. Analogy of electromagnetically induced transparency in plasmonic nanodisk with a square ring resonator

    International Nuclear Information System (INIS)

    Li, Xianping; Wei, Zhongchao; Liu, Yuebo; Zhong, Nianfa; Tan, Xiaopei; Shi, Songsong; Liu, Hongzhan; Liang, Ruisheng

    2016-01-01

    We have demonstrated the analogy of electromagnetically induced transparency in plasmonic nanodisk with a square ring resonator. A reasonable analysis of the transmission feature based on the temporal coupled-mode theory is given and shows good agreement with the Finit-Difference Time-Domain simulation. The transparency window can be easily tuned by changing the geometrical parameters and the insulator filled in the resonator. The transmission of the resonator system is close to 80% and the full width at half maximum is less than 46 nm. The sensitivity of the structure is about 812 nm/RIU. These characteristics make the new system with potential to apply for optical storage, ultrafast plasmonic switch and slow-light devices.

  4. Analogy of electromagnetically induced transparency in plasmonic nanodisk with a square ring resonator

    Energy Technology Data Exchange (ETDEWEB)

    Li, Xianping; Wei, Zhongchao, E-mail: wzc@scnu.edu.cn; Liu, Yuebo; Zhong, Nianfa; Tan, Xiaopei; Shi, Songsong; Liu, Hongzhan; Liang, Ruisheng

    2016-01-08

    We have demonstrated the analogy of electromagnetically induced transparency in plasmonic nanodisk with a square ring resonator. A reasonable analysis of the transmission feature based on the temporal coupled-mode theory is given and shows good agreement with the Finit-Difference Time-Domain simulation. The transparency window can be easily tuned by changing the geometrical parameters and the insulator filled in the resonator. The transmission of the resonator system is close to 80% and the full width at half maximum is less than 46 nm. The sensitivity of the structure is about 812 nm/RIU. These characteristics make the new system with potential to apply for optical storage, ultrafast plasmonic switch and slow-light devices.

  5. Ultrafast Librational Relaxation of H2O in Liquid Water

    DEFF Research Database (Denmark)

    Petersen, Jakob; Møller, Klaus Braagaard; Rey, Rossend

    2013-01-01

    The ultrafast librational (hindered rotational) relaxation of a rotationally excited H2O molecule in pure liquid water is investigated by means of classical nonequilibrium molecular dynamics simulations and a power and work analysis. This analysis allows the mechanism of the energy transfer from...... the excited H2O to its water neighbors, which occurs on a sub-100 fs time scale, to be followed in molecular detail, i.e., to determine which water molecules receive the energy and in which degrees of freedom. It is found that the dominant energy flow is to the four hydrogen-bonded water partners in the first...

  6. Ultrafast coherence transfer in DNA-templated silver nanoclusters

    DEFF Research Database (Denmark)

    Thyrhaug, Erling; Bogh, Sidsel Ammitzbøll; Carro, Miguel

    2017-01-01

    DNA-templated silver nanoclusters of a few tens of atoms or less have come into prominence over the last several years due to very strong absorption and efficient emission. Applications in microscopy and sensing have already been realized, however little is known about the excited-state structure...... and dynamics in these clusters. Here we report on a multidimensional spectroscopy investigation of the energy-level structure and the early-time relaxation cascade, which eventually results in the population of an emitting state. We find that the ultrafast intramolecular relaxation is strongly coupled...

  7. Nonlocal response in plasmonic waveguiding with extreme light confinement

    DEFF Research Database (Denmark)

    Toscano, Giuseppe; Raza, Søren; Yan, Wei

    2013-01-01

    We present a novel wave equation for linearized plasmonic response, obtained by combining the coupled real-space differential equations for the electric field and current density. Nonlocal dynamics are fully accounted for, and the formulation is very well suited for numerical implementation, allo...

  8. Plasmonic percolation: Plasmon-manifested dielectric-to-metal transition

    KAUST Repository

    Chen, Huanjun

    2012-08-28

    Percolation generally refers to the phenomenon of abrupt variations in electrical, magnetic, or optical properties caused by gradual volume fraction changes of one component across a threshold in bicomponent systems. Percolation behaviors have usually been observed in macroscopic systems, with most studies devoted to electrical percolation. We report on our observation of plasmonic percolation in Au nanorod core-Pd shell nanostructures. When the Pd volume fraction in the shell consisting of palladium and water approaches the plasmonic percolation threshold, ∼70%, the plasmon of the nanostructure transits from red to blue shifts with respect to that of the unshelled Au nanorod. This plasmonic percolation behavior is also confirmed by the scattering measurements on the individual core-shell nanostructures. Quasistatic theory and numerical simulations show that the plasmonic percolation originates from a positive-to-negative transition in the real part of the dielectric function of the shell as the Pd volume fraction is increased. The observed plasmonic percolation is found to be independent of the metal type in the shell. Moreover, compared to the unshelled Au nanorods with similar plasmon wavelengths, the Au nanorod core-Pd shell nanostructures exhibit larger refractive index sensitivities, which is ascribed to the expulsion of the electric field intensity from the Au nanorod core by the adsorbed Pd nanoparticles. © 2012 American Chemical Society.

  9. Plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites

    Science.gov (United States)

    Bityurin, N.; Ermolaev, N.; Smirnov, A. A.; Afanasiev, A.; Agareva, N.; Koryukina, T.; Bredikhin, V.; Kamensky, V.; Pikulin, A.; Sapogova, N.

    2016-03-01

    UV irradiation of materials consisting of a polymer matrix that possesses precursors of different kinds can result in creation of nanoparticles within the irradiated domains. Such photoinduced nanocomposites are promising for photonic applications due to the strong alteration of their optical properties compared to initial non-irradiated materials. We report our results on the synthesis and investigation of plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites. Plasmonic nanocomposites contain metal nanoparticles of noble metals with a pronounced plasmon resonance. Excitonic nanocomposites possess semiconductor nanoclusters (quantum dots). We consider the CdS-Au pair because the luminescent band of CdS nanoparticles enters the plasmon resonance band of gold nanoparticles. The obtaining of such particles within the same composite materials is promising for the creation of media with exciton-plasmon resonance. We demonstrate that it is possible to choose appropriate precursor species to obtain the initially transparent poly(methyl methacrylate) (PMMA) films containing both types of these molecules either separately or together. Proper irradiation of these materials by a light-emitting diode operating at the wavelength of 365 nm provides material alteration demonstrating light-induced optical absorption and photoluminescent properties typical for the corresponding nanoparticles. Thus, an exciton-plasmonic photoinduced nanocomposite is obtained. It is important that here we use the precursors that are different from those usually employed.

  10. Plasmonic percolation: Plasmon-manifested dielectric-to-metal transition

    KAUST Repository

    Chen, Huanjun; Wang, Feng; Li, Kun; Woo, Katchoi; Wang, Jianfang; Li, Quan; Sun, Ling Dong; Zhang, Xixiang; Lin, Haiqing; YAN, Chunhua

    2012-01-01

    Percolation generally refers to the phenomenon of abrupt variations in electrical, magnetic, or optical properties caused by gradual volume fraction changes of one component across a threshold in bicomponent systems. Percolation behaviors have usually been observed in macroscopic systems, with most studies devoted to electrical percolation. We report on our observation of plasmonic percolation in Au nanorod core-Pd shell nanostructures. When the Pd volume fraction in the shell consisting of palladium and water approaches the plasmonic percolation threshold, ∼70%, the plasmon of the nanostructure transits from red to blue shifts with respect to that of the unshelled Au nanorod. This plasmonic percolation behavior is also confirmed by the scattering measurements on the individual core-shell nanostructures. Quasistatic theory and numerical simulations show that the plasmonic percolation originates from a positive-to-negative transition in the real part of the dielectric function of the shell as the Pd volume fraction is increased. The observed plasmonic percolation is found to be independent of the metal type in the shell. Moreover, compared to the unshelled Au nanorods with similar plasmon wavelengths, the Au nanorod core-Pd shell nanostructures exhibit larger refractive index sensitivities, which is ascribed to the expulsion of the electric field intensity from the Au nanorod core by the adsorbed Pd nanoparticles. © 2012 American Chemical Society.

  11. Ultrafast photoelectron spectroscopy of small molecule organic films

    Science.gov (United States)

    Read, Kendall Laine

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

  12. Active Molecular Plasmonics: Controlling Plasmon Resonances with Molecular Switches

    KAUST Repository

    Zheng, Yue Bing

    2009-02-11

    A gold nanodisk array, coated with bistable, redox-controllable [2]rotaxane molecules, when exposed to chemical oxidants and reductants, undergoes switching of its plasmonic properties reversibly. By contrast, (i) bare gold nanodisks and (ii) disks coated with a redox-active, but mechanically inert, control compound do not display surface-plasmon-based switching. Along with calculations based on time-dependent density functional theory, these experimental observations suggest that the nanoscale movements within surface-bound “molecular machines” can be used as the active components in plasmonic devices.

  13. Active Molecular Plasmonics: Controlling Plasmon Resonances with Molecular Switches

    KAUST Repository

    Zheng, Yue Bing; Yang, Ying-Wei; Jensen, Lasse; Fang, Lei; Juluri, Bala Krishna; Flood, Amar H.; Weiss, Paul S.; Stoddart, J. Fraser; Huang, Tony Jun

    2009-01-01

    A gold nanodisk array, coated with bistable, redox-controllable [2]rotaxane molecules, when exposed to chemical oxidants and reductants, undergoes switching of its plasmonic properties reversibly. By contrast, (i) bare gold nanodisks and (ii) disks coated with a redox-active, but mechanically inert, control compound do not display surface-plasmon-based switching. Along with calculations based on time-dependent density functional theory, these experimental observations suggest that the nanoscale movements within surface-bound “molecular machines” can be used as the active components in plasmonic devices.

  14. Nonlocal plasmonic response of doped and optically pumped graphene, MoS2, and black phosphorus

    Science.gov (United States)

    Petersen, René; Pedersen, Thomas Garm; Javier García de Abajo, F.

    2017-11-01

    Plasmons in two-dimensional (2D) materials have emerged as a new source of physical phenomena and optoelectronic applications due in part to the relatively small number of charge carriers on which they are supported. Unlike conventional plasmonic materials, they possess a large Fermi wavelength, which can be comparable with the plasmon wavelength, thus leading to unusually strong nonlocal effects. Here, we study the optical response of a selection of 2D crystal layers (graphene, MoS2, and black phosphorus) with inclusion of nonlocal and thermal effects. We extensively analyze their plasmon dispersion relations and focus on the Purcell factor for the decay of an optical emitter in close proximity to the material as a way to probe nonlocal and thermal effects, with emphasis placed on the interplay between temperature and doping. The results are based on tight-binding modeling of the electronic structure combined with the random-phase approximation response function in which the temperature enters through the Fermi-Dirac electronic occupation distribution. Our study provides a route map for the exploration and exploitation of the ultrafast optical response of 2D materials.

  15. Plasmonic enhancement of electroluminescence

    Science.gov (United States)

    Guzatov, D. V.; Gaponenko, S. V.; Demir, H. V.

    2018-01-01

    Here plasmonic effect specifically on electroluminescence (EL) is studied in terms of radiative and nonradiative decay rates for a dipole near a metal spherical nanoparticle (NP). Contribution from scattering is taken into account and is shown to play a decisive role in EL enhancement owing to pronounced size-dependent radiative decay enhancement and weak size effect on non-radiative counterpart. Unlike photoluminescence where local incident field factor mainly determines the enhancement possibility and level, EL enhancement is only possible by means of quantum yield rise, EL enhancement being feasible only for an intrinsic quantum yield Q0 red-orange range only. Independently of positive effect on quantum yield, metal nanoparticles embedded in an electroluminescent device will improve its efficiency at high currents owing to enhanced overall recombination rate which will diminish manifestation of Auger processes. The latter are believed to be responsible for the known undesirable efficiency droop in semiconductor commercial quantum well based LEDs at higher current. For the same reason plasmonics can diminish quantum dot photodegradation from Auger process induced non-radiative recombination and photoionization thus opening a way to avoid negative Auger effects in emerging colloidal semiconductor LEDs.

  16. Active Plasmonics: Principles, Structures, and Applications.

    Science.gov (United States)

    Jiang, Nina; Zhuo, Xiaolu; Wang, Jianfang

    2018-03-28

    Active plasmonics is a burgeoning and challenging subfield of plasmonics. It exploits the active control of surface plasmon resonance. In this review, a first-ever in-depth description of the theoretical relationship between surface plasmon resonance and its affecting factors, which forms the basis for active plasmon control, will be presented. Three categories of active plasmonic structures, consisting of plasmonic structures in tunable dielectric surroundings, plasmonic structures with tunable gap distances, and self-tunable plasmonic structures, will be proposed in terms of the modulation mechanism. The recent advances and current challenges for these three categories of active plasmonic structures will be discussed in detail. The flourishing development of active plasmonic structures opens access to new application fields. A significant part of this review will be devoted to the applications of active plasmonic structures in plasmonic sensing, tunable surface-enhanced Raman scattering, active plasmonic components, and electrochromic smart windows. This review will be concluded with a section on the future challenges and prospects for active plasmonics.

  17. Molecular cavity optomechanics as a theory of plasmon-enhanced Raman scattering.

    Science.gov (United States)

    Roelli, Philippe; Galland, Christophe; Piro, Nicolas; Kippenberg, Tobias J

    2016-02-01

    The exceptional enhancement of Raman scattering by localized plasmonic resonances in the near field of metallic nanoparticles, surfaces or tips (SERS, TERS) has enabled spectroscopic fingerprinting down to the single molecule level. The conventional explanation attributes the enhancement to the subwavelength confinement of the electromagnetic field near nanoantennas. Here, we introduce a new model that also accounts for the dynamical nature of the plasmon-molecule interaction. We thereby reveal an enhancement mechanism not considered before: dynamical backaction amplification of molecular vibrations. We first map the system onto the canonical Hamiltonian of cavity optomechanics, in which the molecular vibration and the plasmon are parametrically coupled. We express the vacuum optomechanical coupling rate for individual molecules in plasmonic 'hot-spots' in terms of the vibrational mode's Raman activity and find it to be orders of magnitude larger than for microfabricated optomechanical systems. Remarkably, the frequency of commonly studied molecular vibrations can be comparable to or larger than the plasmon's decay rate. Together, these considerations predict that an excitation laser blue-detuned from the plasmon resonance can parametrically amplify the molecular vibration, leading to a nonlinear enhancement of Raman emission that is not predicted by the conventional theory. Our optomechanical approach recovers known results, provides a quantitative framework for the calculation of cross-sections, and enables the design of novel systems that leverage dynamical backaction to achieve additional, mode-selective enhancements. It also provides a quantum mechanical framework to analyse plasmon-vibrational interactions in terms of molecular quantum optomechanics.

  18. Ultrafast THz Saturable Absorption in Doped Semiconductors

    DEFF Research Database (Denmark)

    Turchinovich, Dmitry; Hoffmann, Matthias C.

    2011-01-01

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

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

    International Nuclear Information System (INIS)

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

    2005-01-01

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

  20. Plasmonic Horizon in Gold Nanosponges.

    Science.gov (United States)

    Vidal, Cynthia; Sivun, Dmitry; Ziegler, Johannes; Wang, Dong; Schaaf, Peter; Hrelescu, Calin; Klar, Thomas A

    2018-02-14

    An electromagnetic wave impinging on a gold nanosponge coherently excites many electromagnetic hot-spots inside the nanosponge, yielding a polarization-dependent scattering spectrum. In contrast, a hole, recombining with an electron, can locally excite plasmonic hot-spots only within a horizon given by the lifetime of localized plasmons and the speed carrying the information that a plasmon has been created. This horizon is about 57 nm, decreasing with increasing size of the nanosponge. Consequently, photoluminescence from large gold nanosponges appears unpolarized.

  1. Coupled plasmon modes and their localization in graded plasmonic chains

    International Nuclear Information System (INIS)

    Xiao, J.J.; Yakubo, K.; Yu, K.W.

    2007-01-01

    Plasmonic waves occur in the subwavelength scale with transverse confinement below the diffraction limit. In this work, we report results of longitudinal localization-delocalization transitions of coupled plasmon modes in graded chains of metallic nanodots. Two graded models are studied: graded index of refraction in the host medium and incremental spacing between the nanoparticles. The coupled plasmon modes in these graded systems exhibit strong localization, showing a tunable passband in finite size systems. These localized modes survive in presence of weak loss in the nanodots. To understand the localization mechanism, we construct equivalent systems of one-dimensional coupled harmonic oscillators, whose coupling strength or masses are gradually varied from one end to the other, with additional on-site potentials. Confining and transmitting electromagnetic energy in these structures may pave new way for many fruitful applications in plasmonics

  2. Reconfigurable Three-Dimensional Gold Nanorod Plasmonic Nanostructures Organized on DNA Origami Tripod.

    Science.gov (United States)

    Zhan, Pengfei; Dutta, Palash K; Wang, Pengfei; Song, Gang; Dai, Mingjie; Zhao, Shu-Xia; Wang, Zhen-Gang; Yin, Peng; Zhang, Wei; Ding, Baoquan; Ke, Yonggang

    2017-02-28

    Distinct electromagnetic properties can emerge from the three-dimensional (3D) configuration of a plasmonic nanostructure. Furthermore, the reconfiguration of a dynamic plasmonic nanostructure, driven by physical or chemical stimuli, may generate a tailored plasmonic response. In this work, we constructed a 3D reconfigurable plasmonic nanostructure with controllable, reversible conformational transformation using bottom-up DNA self-assembly. Three gold nanorods (AuNRs) were positioned onto a reconfigurable DNA origami tripod. The internanorod angle and distance were precisely tuned through operating the origami tripod by toehold-mediated strand displacement. The transduction of conformational change manifested into a controlled shift of the plasmonic resonance peak, which was studied by dark-field microscopy, and agrees well with electrodynamic calculations. This new 3D plasmonic nanostructure not only provides a method to study the plasmonic resonance of AuNRs at prescribed 3D conformations but also demonstrates that DNA origami can serve as a general self-assembly platform for constructing various 3D reconfigurable plasmonic nanostructures with customized optical properties.

  3. An introduction to graphene plasmonics

    CERN Document Server

    Goncalves, P A D

    2016-01-01

    This book is meant as an introduction to graphene plasmonics and aims at the advanced undergraduate and graduate students entering the field of plasmonics in graphene. In it different theoretical methods are introduced, starting with an elementary description of graphene plasmonics and evolving towards more advanced topics. This book is essentially self-contained and brings together a number of different topics about the field that are scattered in the vast literature. The text is composed of eleven chapters and of a set of detailed appendices. It can be read in two different ways: Reading only the chapters to get acquainted with the field of plasmonics in graphene or reading the chapters and studying the appendices to get a working knowledge of the topic. The study of the material in this book will bring the students to the forefront of the research in this field.

  4. Group-IV midinfrared plasmonics

    Science.gov (United States)

    Biagioni, Paolo; Frigerio, Jacopo; Samarelli, Antonio; Gallacher, Kevin; Baldassarre, Leonetta; Sakat, Emilie; Calandrini, Eugenio; Millar, Ross W.; Giliberti, Valeria; Isella, Giovanni; Paul, Douglas J.; Ortolani, Michele

    2015-01-01

    The use of heavily doped semiconductors to achieve plasma frequencies in the mid-IR has been recently proposed as a promising way to obtain high-quality and tunable plasmonic materials. We introduce a plasmonic platform based on epitaxial n-type Ge grown on standard Si wafers by means of low-energy plasma-enhanced chemical vapor deposition. Due to the large carrier concentration achieved with P dopants and to the compatibility with the existing CMOS technology, SiGe plasmonics hold promises for mid-IR applications in optoelectronics, IR detection, sensing, and light harvesting. As a representative example, we show simulations of mid-IR plasmonic waveguides based on the experimentally retrieved dielectric constants of the grown materials.

  5. Controlling light with plasmonic multilayers

    DEFF Research Database (Denmark)

    Orlov, Alexey A.; Zhukovsky, Sergei; Iorsh, Ivan V.

    2014-01-01

    metamaterials and describe their use for light manipulation at the nanoscale. While demonstrating the recently emphasized hallmark effect of hyperbolic dispersion, we put special emphasis to the comparison between multilayered hyperbolic metamaterials and more broadly defined plasmonic-multilayer metamaterials...

  6. Plasmonic Nanostructures for Biosensor Applications

    Science.gov (United States)

    Gadde, Akshitha

    Improving the sensitivity of existing biosensors is an active research topic that cuts across several disciplines, including engineering and biology. Optical biosensors are the one of the most diverse class of biosensors which can be broadly categorized into two types based on the detection scheme: label-based and label-free detection. In label-based detection, the target bio-molecules are labeled with dyes or tags that fluoresce upon excitation, indicating the presence of target molecules. Label-based detection is highly-sensitive, capable of single molecule detection depending on the detector type used. One method of improving the sensitivity of label-based fluorescence detection is by enhancement of the emission of the labels by coupling them with metal nanostructures. This approach is referred as plasmon-enhanced fluorescence (PEF). PEF is achieved by increasing the electric field around the nano metal structures through plasmonics. This increased electric field improves the enhancement from the fluorophores which in turn improves the photon emission from the fluorophores which, in turn, improves the limit of detection. Biosensors taking advantage of the plasmonic properties of metal films and nanostructures have emerged an alternative, low-cost, high sensitivity method for detecting labeled DNA. Localized surface plasmon resonance (LSPR) sensors employing noble metal nanostructures have recently attracted considerable attention as a new class of plasmonic nanosensors. In this work, the design, fabrication and characterization of plasmonic nanostructures is carried out. Finite difference time domain (FDTD) simulations were performed using software from Lumerical Inc. to design a novel LSPR structure that exhibit resonance overlapping with the absorption and emission wavelengths of quantum dots (QD). Simulations of a composite Au/SiO2 nanopillars on silicon substrate were performed using FDTD software to show peak plasmonic enhancement at QD emission wavelength

  7. Semiconductors for plasmonics and metamaterials

    DEFF Research Database (Denmark)

    Naik, G.V.; Boltasseva, Alexandra

    2010-01-01

    Plasmonics has conventionally been in the realm of metal-optics. However, conventional metals as plasmonic elements in the near-infrared (NIR) and visible spectral ranges suffer from problems such as large losses and incompatibility with semiconductor technology. Replacing metals with semiconduct......Plasmonics has conventionally been in the realm of metal-optics. However, conventional metals as plasmonic elements in the near-infrared (NIR) and visible spectral ranges suffer from problems such as large losses and incompatibility with semiconductor technology. Replacing metals...... with semiconductors can alleviate these problems if only semiconductors could exhibit negative real permittivity. Aluminum doped zinc oxide (AZO) is a low loss semiconductor that can show negative real permittivity in the NIR. A comparative assessment of AZO-based plasmonic devices such as superlens and hyperlens...... with their metal-based counterparts shows that AZO-based devices significantly outperform at a wavelength of 1.55 µm. This provides a strong stimulus in turning to semiconductor plasmonics at the telecommunication wavelengths. (© 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)....

  8. Ultrafast excited state relaxation in long-chain polyenes

    International Nuclear Information System (INIS)

    Antognazza, Maria Rosa; Lueer, Larry; Polli, Dario; Christensen, Ronald L.; Schrock, Richard R.; Lanzani, Guglielmo; Cerullo, Giulio

    2010-01-01

    Graphical abstract: Excited state dynamics of a long-chain polyene studied by femtosecond pump-probe spectroscopy. - Abstract: We present a comprehensive study, by femtosecond pump-probe spectroscopy, of excited state dynamics in a polyene that approaches the infinite chain limit. By excitation with sub-10-fs pulses resonant with the 0-0 S 0 → S 2 transition, we observe rapid loss of stimulated emission from the bright excited state S 2 , followed by population of the hot S 1 state within 150 fs. Vibrational cooling of S 1 takes place within 500 fs and is followed by decay back to S 0 with 1 ps time constant. By excitation with excess vibrational energy we also observe the ultrafast formation of a long-living absorption, that is assigned to the triplet state generated by singlet fission.

  9. Theory of dispersions and dampin.o of plasmons in electron liquid

    International Nuclear Information System (INIS)

    Monga, M.R.; Pathak, K.N.

    1980-01-01

    A general expression for the dynamical response function has been obtained using equation of motion method. The expression is exact upto second order in Coulomb potential as well as in wave vector q. The results correspond to taking into account the mechanism of damping of plasmons by excitation of two particles-two holes from the Fermi sea. The closed form expressions for the plasmon dispersion and damping have been obtained for the electron density parameter rsub(s) → 0. (author)

  10. Modeling, Simulation and Design of Plasmonic Interconnects for On-Chip Signal Processing

    Science.gov (United States)

    2011-02-14

    Transactions on Nanotechnology. (already available in IEEE Xplore , though the paper version has not been scheduled yet). 7. K. Song, and P. Mazumder, “One...in Nanoelectronics and Plasmonics,” Proceedings on IEEE Conference on Nanotechnology, Cincinnati, July 2006. 2. K. Song and P. Mazumder, “Surface...Plasmon Dynamics of a Metallic Nanoparticle,” Proceedings on IEEE Conference on Nanotechnology, Hong Kong, Aug. 2007. 3. K. Song and P. Mazumder

  11. Ultrafast disk lasers and amplifiers

    Science.gov (United States)

    Sutter, Dirk H.; Kleinbauer, Jochen; Bauer, Dominik; Wolf, Martin; Tan, Chuong; Gebs, Raphael; Budnicki, Aleksander; Wagenblast, Philipp; Weiler, Sascha

    2012-03-01

    Disk lasers with multi-kW continuous wave (CW) output power are widely used in manufacturing, primarily for cutting and welding applications, notably in the automotive industry. The ytterbium disk technology combines high power (average and/or peak power), excellent beam quality, high efficiency, and high reliability with low investment and operating costs. Fundamental mode picosecond disk lasers are well established in micro machining at high throughput and perfect precision. Following the world's first market introduction of industrial grade 50 W picosecond lasers (TruMicro 5050) at the Photonics West 2008, the second generation of the TruMicro series 5000 now provides twice the average power (100 W at 1030 nm, or 60 W frequency doubled, green output) at a significantly reduced footprint. Mode-locked disk oscillators achieve by far the highest average power of any unamplified lasers, significantly exceeding the 100 W level in laboratory set-ups. With robust long resonators their multi-microjoule pulse energies begin to compete with typical ultrafast amplifiers. In addition, significant interest in disk technology has recently come from the extreme light laser community, aiming for ultra-high peak powers of petawatts and beyond.

  12. Ultra-Fast Hadronic Calorimetry

    Energy Technology Data Exchange (ETDEWEB)

    Denisov, Dmitri [Fermilab; Lukić, Strahinja [VINCA Inst. Nucl. Sci., Belgrade; Mokhov, Nikolai [Fermilab; Striganov, Sergei [Fermilab; Ujić, Predrag [VINCA Inst. Nucl. Sci., Belgrade

    2017-12-18

    Calorimeters for particle physics experiments with integration time of a few ns will substantially improve the capability of the experiment to resolve event pileup and to reject backgrounds. In this paper time development of hadronic showers induced by 30 and 60 GeV positive pions and 120 GeV protons is studied using Monte Carlo simulation and beam tests with a prototype of a sampling steel-scintillator hadronic calorimeter. In the beam tests, scintillator signals induced by hadronic showers in steel are sampled with a period of 0.2 ns and precisely time-aligned in order to study the average signal waveform at various locations w.r.t. the beam particle impact. Simulations of the same setup are performed using the MARS15 code. Both simulation and test beam results suggest that energy deposition in steel calorimeters develop over a time shorter than 3 ns providing opportunity for ultra-fast calorimetry. Simulation results for an "ideal" calorimeter consisting exclusively of bulk tungsten or copper are presented to establish the lower limit of the signal integration window.

  13. Ultrafast palladium diffusion in germanium

    KAUST Repository

    Tahini, Hassan Ali

    2015-01-01

    The slow transport of dopants through crystal lattices has hindered the development of novel devices. Typically atoms are contained within deep potential energy wells which necessitates multiple attempts to hop between minimum energy positions. This is because the bonds that constrain atoms are strongest at the minimum positions. As they hop between sites the bonds must be broken, only to re-form as the atoms slide into adjacent minima. Here we demonstrate that the Pd atoms introduced into the Ge lattice behave differently. They retain bonds as the atoms shift across so that at the energy maximum between sites Pd still exhibits strong bonding characteristics. This reduces the energy maximum to almost nothing (a migration energy of only 0.03 eV) and means that the transport of Pd through the Ge lattice is ultrafast. We scrutinize the bonding characteristics at the atomic level using quantum mechanical simulation tools and demonstrate why Pd behaves so differently to other metals we investigated (i.e. Li, Cu, Ag, Pt and Au). Consequently, this fundamental understanding can be extended to systems where extremely rapid diffusion is desired, such as radiation sensors, batteries and solid oxide fuel cells.

  14. Ultralow-loss CMOS copper plasmonic waveguides

    DEFF Research Database (Denmark)

    Fedyanin, Dmitry Yu.; Yakubovsky, Dmitry I.; Kirtaev, Roman V.

    2016-01-01

    with microelectronics manufacturing technologies. This prevents plasmonic components from integration with both silicon photonics and silicon microelectronics. Here, we demonstrate ultralow-loss copper plasmonic waveguides fabricated in a simple complementary metal-oxide semiconductor (CMOS) compatible process, which...

  15. Surface Plasmon-Assisted Solar Energy Conversion.

    Science.gov (United States)

    Dodekatos, Georgios; Schünemann, Stefan; Tüysüz, Harun

    2016-01-01

    The utilization of localized surface plasmon resonance (LSPR) from plasmonic noble metals in combination with semiconductors promises great improvements for visible light-driven photocatalysis, in particular for energy conversion. This review summarizes the basic principles of plasmonic photocatalysis, giving a comprehensive overview about the proposed mechanisms for enhancing the performance of photocatalytically active semiconductors with plasmonic devices and their applications for surface plasmon-assisted solar energy conversion. The main focus is on gold and, to a lesser extent, silver nanoparticles in combination with titania as semiconductor and their usage as active plasmonic photocatalysts. Recent advances in water splitting, hydrogen generation with sacrificial organic compounds, and CO2 reduction to hydrocarbons for solar fuel production are highlighted. Finally, further improvements for plasmonic photocatalysts, regarding performance, stability, and economic feasibility, are discussed for surface plasmon-assisted solar energy conversion.

  16. Probing plasmonic nanostructures by photons and electrons

    DEFF Research Database (Denmark)

    Kneipp, Katrin; Kneipp, Harald; Kneipp, Janina

    2015-01-01

    We discuss recent developments for studying plasmonic metal nanostructures. Exploiting photons and electrons opens up new capabilities to probe the complete plasmon spectrum including bright and dark modes and related local optical fields at subnanometer spatial resolution. This comprehensive cha...

  17. A review on plasmonic metal–TiO{sub 2} composite for generation, trapping, storing and dynamic vectorial transfer of photogenerated electrons across the Schottky junction in a photocatalytic system

    Energy Technology Data Exchange (ETDEWEB)

    Gomathi Devi, L., E-mail: gomatidevi_naik@yahoo.co.in; Kavitha, R.

    2016-01-01

    loadings on the interfacial charge carrier dynamics. The metal deposition onto the varied hierarchical morphology, crystal structure, defective surface of titania along with extended modification like simultaneous doping and heterostructure coupling with other semiconductors is also highlighted. It was revealed that deposited metal is involved in multiple crucial roles like; (i) it serves as passive electron sink with high capacity to store electrons to suppress photogenerated charge carrier recombination; (ii) it facilitates rapid dioxygen reduction to generate reactive free radicals; (iii) visible light response for titania can be achieved through surface plasmon resonance effect; (iv) direct excitation of metal nanoparticles especially under visible light and vectorial electron transfer to the TiO{sub 2} CB. This review attempts to provide a comprehensive update of design and fabrication of metallization on the surface of TiO{sub 2} semiconductor particles highlighting some of the advancements made in the energy and environment applications.

  18. Electrically Tunable Plasmonic Resonances with Graphene

    DEFF Research Database (Denmark)

    Emani, Naresh K.; Chung, Ting-Fung; Ni, Xingjie

    2012-01-01

    Real time switching of a plasmonic resonance may find numerous applications in subwavelength optoelectronics, spectroscopy and sensing. We take advantage of electrically tunable interband transitions in graphene to control the strength of the plasmonic resonance.......Real time switching of a plasmonic resonance may find numerous applications in subwavelength optoelectronics, spectroscopy and sensing. We take advantage of electrically tunable interband transitions in graphene to control the strength of the plasmonic resonance....

  19. Ultrafast photon counting applied to resonant scanning STED microscopy.

    Science.gov (United States)

    Wu, Xundong; Toro, Ligia; Stefani, Enrico; Wu, Yong

    2015-01-01

    To take full advantage of fast resonant scanning in super-resolution stimulated emission depletion (STED) microscopy, we have developed an ultrafast photon counting system based on a multigiga sample per second analogue-to-digital conversion chip that delivers an unprecedented 450 MHz pixel clock (2.2 ns pixel dwell time in each scan). The system achieves a large field of view (∼50 × 50 μm) with fast scanning that reduces photobleaching, and advances the time-gated continuous wave STED technology to the usage of resonant scanning with hardware-based time-gating. The assembled system provides superb signal-to-noise ratio and highly linear quantification of light that result in superior image quality. Also, the system design allows great flexibility in processing photon signals to further improve the dynamic range. In conclusion, we have constructed a frontier photon counting image acquisition system with ultrafast readout rate, excellent counting linearity, and with the capacity of realizing resonant-scanning continuous wave STED microscopy with online time-gated detection. © 2014 The Authors Journal of Microscopy © 2014 Royal Microscopical Society.

  20. Near field plasmon and force microscopy

    NARCIS (Netherlands)

    de Hollander, R.B.G.; van Hulst, N.F.; Kooyman, R.P.H.

    1995-01-01

    A scanning plasmon near field optical microscope (SPNM) is presented which combines a conventional far field surface plasmon microscope with a stand-alone atomic force microscope (AFM). Near field plasmon and force images are recorded simultaneously both with a lateral resolution limited by the

  1. Time-resolved single-shot terahertz time-domain spectroscopy for ultrafast irreversible processes

    Science.gov (United States)

    Zhai, Zhao-Hui; Zhong, Sen-Cheng; Li, Jun; Zhu, Li-Guo; Meng, Kun; Li, Jiang; Liu, Qiao; Peng, Qi-Xian; Li, Ze-Ren; Zhao, Jian-Heng

    2016-09-01

    Pulsed terahertz spectroscopy is suitable for spectroscopic diagnostics of ultrafast events. However, the study of irreversible or single shot ultrafast events requires ability to record transient properties at multiple time delays, i.e., time resolved at single shot level, which is not available currently. Here by angular multiplexing use of femtosecond laser pulses, we developed and demonstrated a time resolved, transient terahertz time domain spectroscopy technique, where burst mode THz pulses were generated and then detected in a single shot measurement manner. The burst mode THz pulses contain 2 sub-THz pulses, and the time gap between them is adjustable up to 1 ns with picosecond accuracy, thus it can be used to probe the single shot event at two different time delays. The system can detect the sub-THz pulses at 0.1 THz-2.5 THz range with signal to noise ratio (SNR) of ˜400 and spectrum resolution of 0.05 THz. System design was described here, and optimizations of single shot measurement of THz pulses were discussed in detail. Methods to improve SNR were also discussed in detail. A system application was demonstrated where pulsed THz signals at different time delays of the ultrafast process were successfully acquired within single shot measurement. This time resolved transient terahertz time domain spectroscopy technique provides a new diagnostic tool for irreversible or single shot ultrafast events where dynamic information can be extracted at terahertz range within one-shot experiment.

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

    Science.gov (United States)

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

    2017-12-26

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

  3. Fusion of Ultraviolet-Visible and Infrared Transient Absorption Spectroscopy Data to Model Ultrafast Photoisomerization.

    Science.gov (United States)

    Debus, Bruno; Orio, Maylis; Rehault, Julien; Burdzinski, Gotard; Ruckebusch, Cyril; Sliwa, Michel

    2017-08-03

    Ultrafast photoisomerization reactions generally start at a higher excited state with excess of internal vibrational energy and occur via conical intersections. This leads to ultrafast dynamics which are difficult to investigate with a single transient absorption spectroscopy technique, be it in the ultraviolet-visible (UV-vis) or infrared (IR) domain. On one hand, the information available in the UV-vis domain is limited as only slight spectral changes are observed for different isomers. On the other hand, the interpretation of vibrational spectra is strongly hindered by intramolecular relaxation and vibrational cooling. These limitations can be circumvented by fusing UV-vis and IR transient absorption spectroscopy data in a multiset multivariate curve resolution analysis. We apply this approach to describe the spectrodynamics of the ultrafast cis-trans photoisomerization around the C-N double bond observed for aromatic Schiff bases. Twisted intermediate states could be elucidated, and isomerization was shown to occur through a continuous complete rotation. More broadly, data fusion can be used to rationalize a vast range of ultrafast photoisomerization processes of interest in photochemistry.

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

    Science.gov (United States)

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

    2015-10-01

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

  5. Microgrooved plasmonic bottle microresonator

    Science.gov (United States)

    Mohd Nasir, M. N.; Ding, M.; Murugan, G. S.; Zervas, M. N.

    2015-06-01

    In this paper, we demonstrate an enhancement to SPW cavity through the incorporation of high-Q WGM bottle microresonator (BMR) with surface microgrooves. A standard BMR fabricated through the “soften-and-compress” technique with initial length of 280 μm, bottle diameter of 187 μm and stem diameter of 125 μm was utilized in the experiment for supporting WGMs. Thin gold film was deposited on top of the BMR for generating SPWs. 21 microgrooves was then inscribed on the metal surface of the BMR along the azimuthal direction with 10 μm length, 485 nm width, 6 μm depth and pitch of 1.5 μm. Due to surface curvature, the gold film only covered half of the BMR with a characteristic meniscus shape and maximum thickness of 30 nm. The meniscus provides appropriately tapered metal edges that facilitate the adiabatic transformation of BMR WGMs to SPWs and vice-versa. Lorentzian shape-line fit performed on the TM excited resonances show that plasmonic Q values in excess of 4000 could be achieved from such structure with ∼ 25% coupling efficiency.

  6. Progress in ultrafast intense laser science XI

    CERN Document Server

    Yamanouchi, Kaoru; Martin, Philippe

    2014-01-01

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

  7. Progress in ultrafast intense laser science

    CERN Document Server

    Yamanouchi, Kaoru; Mathur, Deepak

    2014-01-01

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

  8. 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....

  9. Spatially Probed Plasmonic Photothermic Nanoheater Enhanced Hybrid Polymeric-Metallic PVDF-Ag Nanogenerator.

    Science.gov (United States)

    Liow, Chi Hao; Lu, Xin; Tan, Chuan Fu; Chan, Kwok Hoe; Zeng, Kaiyang; Li, Shuzhou; Ho, Ghim Wei

    2018-02-01

    Surface plasmon-based photonics offers exciting opportunities to enable fine control of the site, span, and extent of mechanical harvesting. However, the interaction between plasmonic photothermic and piezoresponse still remains underexplored. Here, spatially localized and controllable piezoresponse of a hybrid self-polarized polymeric-metallic system that correlates to plasmonic light-to-heat modulation of the local strain is demonstrated. The piezoresponse is associated to the localized plasmons that serve as efficient nanoheaters leading to self-regulated strain via thermal expansion of the electroactive polymer. Moreover, the finite-difference time-domain simulation and linear thermal model also deduce the local strain to the surface plasmon heat absorption. The distinct plasmonic photothermic-piezoelectric phenomenon mediates not only localized external stimulus light response but also enhances dynamic piezoelectric energy harvesting. The present work highlights a promising surface plasmon coordinated piezoelectric response which underpins energy localization and transfer for diversified design of unique photothermic-piezotronic technology. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. Characterization of Nanostructured Semiconductors by Ultrafast Luminescence Imaging

    Science.gov (United States)

    Blake, Jolie

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

  11. Plasmon polaritons in nanostructured graphene

    DEFF Research Database (Denmark)

    Xiao, Sanshui

    2013-01-01

    Graphene has attracted considerable attention due to its unique electronic and optical properties. When graphene is electrically/chemically doped, it can support surface plasmon where the light propagates along the surface with a very short wavelength and an extremely small mode volume. The optical...... properties of graphene can be tuned by electrical gating, thus proving a promising way to realize a tunable plasmonic material. We firstly investigate the performance of bends and splitters in graphene nanoribbon waveguides, and show that bends and splitters do not induce any additional loss provided...... that the nanoribbon width is sub-wavelength. Then we experimentally demonstrate the excitation of graphene plasmon polaritons in a continuous graphene monolayer resting on a two-dimensional subwavelength silicon grating. The silicon grating is realized by a nanosphere lithography technique with a self...

  12. Influence of thickness-dependent structural evolution on ultrafast magnetization dynamics in C o2F e0.4M n0.6Si Heusler alloy thin films

    Science.gov (United States)

    Pan, Santanu; Mondal, Sucheta; Seki, Takeshi; Takanashi, Koki; Barman, Anjan

    2016-11-01

    We experimentally investigate thickness (t )-dependent evolution of structural and magnetic properties in C o2F e0.4M n0.6Si (CFMS) thin films and correlate them with ultrafast demagnetization time (τd) and relaxation time (τ1) as well as the Gilbert damping coefficient (α ). Structural ordering and magnetic parameters, including α , exhibit a nonmonotonic variation with increasing t . A remarkably low value of α of 0.009 is obtained for the CFMS film with t =20 nm without any buffer layers, which helps to avoid possible diffusion of the buffer layer into CFMS. Highest saturation magnetization, lowest coercivity, and the α value imply CFMS film with t =20 nm is most suitable for integrated spintronics devices, viz. low-current switched spin transfer torque, and magnetic tunnel junction with a high tunnel magnetoresistance ratio at room temperature. Despite the presence of strain, a lower degree of chemical ordering in the low-t regime, and increased defect density in the high-t regime, we obtained a reasonably low value of damping. In addition to the intrinsic fourfold magnetocrystalline anisotropy, an induced uniaxial anisotropy is found, which also varies nonmonotonically with t . Finally, unique band structure controlled demagnetization and fast relaxation in half-metallic CFMS is correlated to α .

  13. Broad electrical tuning of plasmonic nanoantennas at visible frequencies

    Energy Technology Data Exchange (ETDEWEB)

    Hoang, Thang B. [Department of Physics, Duke University, Durham, North Carolina 27708 (United States); Center for Metamaterials and Integrated Plasmonics, Duke University, Durham, North Carolina 27708 (United States); Mikkelsen, Maiken H., E-mail: m.mikkelsen@duke.edu [Department of Physics, Duke University, Durham, North Carolina 27708 (United States); Center for Metamaterials and Integrated Plasmonics, Duke University, Durham, North Carolina 27708 (United States); Department of Electrical and Computer Engineering, Duke University, Durham, North Carolina 27708 (United States)

    2016-05-02

    We report an experimental demonstration of electrical tuning of plasmon resonances of optical nanopatch antennas over a wide wavelength range. The antennas consist of silver nanocubes separated from a gold film by a thin 8 nm polyelectrolyte spacer layer. By using ionic liquid and indium tin oxide coated glass as a top electrode, we demonstrate dynamic and reversible tuning of the plasmon resonance over 100 nm in the visible wavelength range using low applied voltages between −3.0 V and 2.8 V. The electrical potential is applied across the nanoscale gap causing changes in the gap thickness and dielectric environment which, in turn, modifies the plasmon resonance. The observed tuning range is greater than the full-width-at-half-maximum of the plasmon resonance, resulting in a tuning figure of merit of 1.05 and a tuning contrast greater than 50%. Our results provide an avenue to create active and reconfigurable integrated nanophotonic components for applications in optoelectronics and sensing.

  14. Ultrafast measurements of chlorine dioxide photochemistry

    Energy Technology Data Exchange (ETDEWEB)

    Ludowise, P.D.

    1997-08-01

    Time-resolved mass spectrometry and time-resolved photoelectron spectroscopy are used to study the ultrafast photodissociation dynamics of chlorine dioxide, an important constituent in stratospheric ozone depletion. Chapter 1 introduces these pump/probe techniques, in which a femtosecond pump pulse excites a molecule to a dissociative state. At a later time, a second femtosecond probe pulse ionizes the molecule. The resulting mass and photoelectron spectra are acquired as a function of the delay between the pump and probe pulses, which follows the evolution of the molecule on the excited state. A comparison to other techniques used to study reaction dynamics is discussed. Chapter 2 includes a detailed description of the design and construction of the experimental apparatus, which consists of a femtosecond laser system, a molecular beam time-of-flight spectrometer, and a data acquisition system. The time-of-flight spectrometer is specifically designed to have a short flight distance to maximize the photoelectron collection efficiency without degrading the resolution, which is limited by the bandwidth of the femtosecond laser system. Typical performance of the apparatus is demonstrated in a study of the time-resolved photoelectron spectroscopy of nitric oxide. The results of the time-resolved mass spectrometry experiments of chlorine dioxide are presented in Chapter 3. Upon excitation to the A {sup 2}A{sub 2} state near 3.2 eV, the molecule dissociates through an indirect two-step mechanism. The direct dissociation channel has been predicted to be open, but is not observed. A quantum beat is observed in the OClO{sup +} species, which is described as a vibrational coherence of the optically prepared A {sup 2}A{sub 2} state. Chapter 4 presents the results of the time-resolved photoelectron experiments of chlorine dioxide. At short delay time, the quantum beat of the OClO{sup +} species is observed in the X {sup 1}A{sub 1} state of the ion. At infinite delay, the signal

  15. Graphene-protected copper and silver plasmonics

    DEFF Research Database (Denmark)

    Kravets, V. G.; Jalil, R.; Kim, Y. J.

    2014-01-01

    suitable for plasmonic applications. To this end, there has been a continuous search for alternative plasmonic materials that are also compatible with complementary metal oxide semiconductor technology. Here we show that copper and silver protected by graphene are viable candidates. Copper films covered...... with one to a few graphene layers show excellent plasmonic characteristics. They can be used to fabricate plasmonic devices and survive for at least a year, even in wet and corroding conditions. As a proof of concept, we use the graphene-protected copper to demonstrate dielectric loaded plasmonic...

  16. Active resonance tuning of stretchable plasmonic structures

    DEFF Research Database (Denmark)

    Zhu, Xiaolong; Xiao, Sanshui; Mortensen, N. Asger

    2012-01-01

    Active resonance tuning is highly desired for the applications of plasmonic structures, such as optical switches and surface enhanced Raman substrates. In this paper, we demonstrate the active tunable plasmonic structures, which composed of monolayer arrays of metallic semishells with dielectric...... cores on stretchable elastic substrates. These composite structures support Bragg-type surface plasmon resonances whose frequencies are sensitive to the arrangement of the metallic semishells. Under uniaxial stretching, the lattice symmetry of these plasmonic structures can be reconfigured from...... applications of the stretch-tunable plasmonic structures in sensing, switching, and filtering....

  17. Nanofocusing in a tapered graphene plasmonic waveguide

    DEFF Research Database (Denmark)

    Dai, Yunyun; Zhu, Xiaolong; Mortensen, N. Asger

    2015-01-01

    Gated or doped graphene can support plasmons making it a promising plasmonic material in the terahertz regime. Here, we show numerically that in a tapered graphene plasmonic waveguide mid- and far-infrared light can be focused in nanometer scales, far beyond the diffraction limit. The underlying...... physics lies in that when propagating along the direction towards the tip both the group and phase velocities of the plasmons supported by the tapered graphene waveguide are reduced accordingly, eventually leading to nanofocusing at the tip with a huge enhancement of optical fields. The nanofocusing...... of optical fields in tapered graphene plasmonic waveguides could be potentially exploited in the enhancement of light–matter interactions....

  18. Sub-wavelength plasmon laser

    Science.gov (United States)

    Bora, Mihail; Bond, Tiziana C.

    2016-04-19

    A plasmonic laser device has resonant nanocavities filled with a gain medium containing an organic dye. The resonant plasmon frequencies of the nanocavities are tuned to align with both the absorption and emission spectra of the dye. Variables in the system include the nature of the dye and the wavelength of its absorption and emission, the wavelength of the pumping radiation, and the resonance frequencies of the nanocavities. In addition the pumping frequency of the dye is selected to be close to the absorption maximum.

  19. Plasmon assisted control of photo-induced excitation energy transfer in a molecular chain

    Science.gov (United States)

    Wang, Luxia; May, Volkhard

    2017-08-01

    The strong and ultrafast laser pulse excitation of a molecular chain in close vicinity to a spherical metal nano-particle (MNP) is studied theoretically. Due to local-field enhancement around the MNP, pronounced excited-state formation has to be expected for the part of the chain which is in proximity to the MNP. Here, the description of this phenomenon will be based on a uniform quantum theory of the MNP-molecule system. It accounts for local-field effects due to direct consideration of the strong excitation energy transfer coupling between the MNP and the various molecules. The molecule-MNP distances are chosen in such a way as to achieve a correct description of the MNP via dipole-plasmon excitations. Short plasmon life-times are incorporated in the framework of a density matrix approach. By extending earlier work the present description allows for multi-exciton formation and multiple dipole-plasmon excitation. The region of less intense and not-too-short optical excitation is identified as being best suited for excitation energy localization in the chain.

  20. Surface Plasmon Resonance Biosensor

    Directory of Open Access Journals (Sweden)

    Nina GRIDINA

    2013-02-01

    Full Text Available Performed in this paper is numerical modeling of the angular dependence for light reflectivity R(F in surface plasmon-polariton resonance (SPR realized in Kretschmann geometry when studying the interface gold/suspension of spherical particles (cells in the assumption that the dielectric permittivity of particles suspension is described by the theory of effective medium. It has been shown that availability of suspended particles in solution inevitably results in appearance of an intermediate layer with the ε gradient between gold surface and suspension bulk, as a result of which the SPR angle shifts to lower values. Near the critical angle, the first derivative dR/dF demonstrates a clearly pronounced peak, which allows determining the value for suspension bulk and the gradient in the intermediate layer. Obtained in our experiments were SPR curves for two suspensions of erythrocytes – the dense one (erythrocyte mass after centrifuging and loose solution (whole blood. In the case of erythrocyte mass, fitting the experimental and calculated curves enabled us to quantitatively determine the bulk value for this erythrocyte mass (εb =1.96, thickness of the intermediate layer dm (300…400 nm and gradient in the intermediate layer. On the contrary, the SPR curve for whole blood appeared to be close to that of pure plasma. This fact allows only estimation of the thickness dm~2000...3000 nm as well as minimum ε value in the intermediate layer, which is close to that of plasma (ε = 1.79. Also, discussed is the mechanism of influence of the cell shape near the gold surface on the SPR effect.

  1. Versatile ultrafast pump-probe imaging with high sensitivity CCD camera

    OpenAIRE

    Pezeril , Thomas; Klieber , Christoph; Temnov , Vasily; Huntzinger , Jean-Roch; Anane , Abdelmadjid

    2012-01-01

    International audience; A powerful imaging technique based on femtosecond time-resolved measurements with a high dynamic range, commercial CCD camera is presented. Ultrafast phenomena induced by a femtosecond laser pump are visualized through the lock-in type acquisition of images recorded by a femtosecond laser probe. This technique allows time-resolved measurements of laser excited phenomena at multiple probe wavelengths (spectrometer mode) or conventional imaging of the sample surface (ima...

  2. Plasmon Enhanced Photoemission

    Energy Technology Data Exchange (ETDEWEB)

    Polyakov, Aleksandr [Univ. of California, Berkeley, CA (United States)

    2012-05-08

    Next generation ultrabright light sources will operate at megahertz repetition rates with temporal resolution in the attosecond regime. For an X-Ray Free Electron Laser (FEL) to operate at such repetition rate requires a high quantum efficiency (QE) cathode to produce electron bunches of 300 pC per 1.5 μJ incident laser pulse. Semiconductor photocathodes have sufficient QE in the ultraviolet (UV) and the visible spectrum, however, they produce picosecond electron pulses due to the electron-phonon scattering. On the other hand, metals have two orders of magnitude less QE, but can produce femtosecond pulses, that are required to form the optimum electron distribution for high efficiency FEL operation. In this work, a novel metallic photocathode design is presented, where a set of nano-cavities is introduced on the metal surface to increase its QE to meet the FEL requirements, while maintaining the fast time response. Photoemission can be broken up into three steps: (1) photon absorption, (2) electron transport to the surface, and (3) crossing the metal-vacuum barrier. The first two steps can be improved by making the metal completely absorbing and by localizing the fields closer to the metal surface, thereby reducing the electron travel distance. Both of these effects can be achieved by coupling the incident light to an electron density wave on the metal surface, represented by a quasi-particle, the Surface Plasmon Polariton (SPP). The photoemission then becomes a process where the photon energy is transferred to an SPP and then to an electron. The dispersion relation for the SPP defines the region of energies where such process can occur. For example, for gold, the maximum SPP energy is 2.4 eV, however, the work function is 5.6 eV, therefore, only a fourth order photoemission process is possible. In such process, four photons excite four plasmons that together excite only one electron. The yield of such non-linear process depends strongly on the light intensity. In

  3. Functional MRI of the patellofemoral joint: comparison of ultrafast MRI, motion-triggered cine MRI and static MRI

    Energy Technology Data Exchange (ETDEWEB)

    Muhle, C. [Klinik fuer Radiologische Diagnostik, Univ. Kiel (Germany); Brossmann, J. [Klinik fuer Radiologische Diagnostik, Univ. Kiel (Germany); Melchert, U.H. [Klinik fuer Radiologische Diagnostik, Univ. Kiel (Germany); Schroeder, C. [Radiologische Abt., Universitaets-Kinderklinik, Christian-Albrechts-Universitaet, Kiel (Germany); Boer, R. de [Philips Medical Systems, Best (Netherlands); Spielmann, R.P. [Klinik fuer Radiologische Diagnostik, Univ. Kiel (Germany); Heller, M. [Klinik fuer Radiologische Diagnostik, Univ. Kiel (Germany)

    1995-12-31

    To evaluate the feasibility and usefulness of ultrafast MRI (u), patellar tracking from 30 of flexion to knee extension (0 ) was analysed and compared with motion-triggered cine MRI (m) and a static MRI technique (s). The different imaging methods were compared in respect of the patellofemoral relationship, the examination time and image quality. Eight healthy subjects and four patients (in total 18 joints) with patellar subluxation or luxation were examined. Significant differences between the static MRI series without quadriceps contraction and the functional MRI studies (motion-triggered cine MRI and ultrafast MRI) were found for the patellar tilt angle. In the dynamic joint studies there was no statistical difference of the regression coefficients between the motion-triggered cine MRI studies and the ultrafast MRI studies. The findings of the functional MRI studies compared with the static MRI images were significantly different for the lateralisation of the patella, expressed by the lateral patellar displacement and bisect offset. No significant differences in patellar lateralisation were found between motion-triggered cine MRI and ultrafast MRI. Ultrafast MRI was superior to motion-triggered cine MRI in terms of the reduction in imaging time and improvement of the image quality. (orig.)

  4. Functional MRI of the patellofemoral joint: comparison of ultrafast MRI, motion-triggered cine MRI and static MRI

    International Nuclear Information System (INIS)

    Muhle, C.; Brossmann, J.; Melchert, U.H.; Schroeder, C.; Boer, R. de; Spielmann, R.P.; Heller, M.

    1995-01-01

    To evaluate the feasibility and usefulness of ultrafast MRI (u), patellar tracking from 30 of flexion to knee extension (0 ) was analysed and compared with motion-triggered cine MRI (m) and a static MRI technique (s). The different imaging methods were compared in respect of the patellofemoral relationship, the examination time and image quality. Eight healthy subjects and four patients (in total 18 joints) with patellar subluxation or luxation were examined. Significant differences between the static MRI series without quadriceps contraction and the functional MRI studies (motion-triggered cine MRI and ultrafast MRI) were found for the patellar tilt angle. In the dynamic joint studies there was no statistical difference of the regression coefficients between the motion-triggered cine MRI studies and the ultrafast MRI studies. The findings of the functional MRI studies compared with the static MRI images were significantly different for the lateralisation of the patella, expressed by the lateral patellar displacement and bisect offset. No significant differences in patellar lateralisation were found between motion-triggered cine MRI and ultrafast MRI. Ultrafast MRI was superior to motion-triggered cine MRI in terms of the reduction in imaging time and improvement of the image quality. (orig.)

  5. Quantum Computation with Ultrafast Laser Pulse Shaping

    Indian Academy of Sciences (India)

    Home; Journals; Resonance – Journal of Science Education; Volume 10; Issue 6. Quantum Computation with Ultrafast Laser Pulse Shaping. Debabrata Goswami. General Article Volume 10 Issue 6 June 2005 pp 8-14. Fulltext. Click here to view fulltext PDF. Permanent link:

  6. Photonic-assisted ultrafast THz wireless access

    DEFF Research Database (Denmark)

    Yu, Xianbin; Chen, Ying; Galili, Michael

    THz technology has been considered feasible for ultrafast wireless data communi- cation, to meet the increasing demand on next-generation fast wireless access, e.g., huge data file transferring and fast mobile data stream access. This talk reviews recent progress in high-speed THz wireless...

  7. Ultraconfined Plasmonic Hotspots Inside Graphene Nanobubbles.

    Science.gov (United States)

    Fei, Z; Foley, J J; Gannett, W; Liu, M K; Dai, S; Ni, G X; Zettl, A; Fogler, M M; Wiederrecht, G P; Gray, S K; Basov, D N

    2016-12-14

    We report on a nanoinfrared (IR) imaging study of ultraconfined plasmonic hotspots inside graphene nanobubbles formed in graphene/hexagonal boron nitride (hBN) heterostructures. The volume of these plasmonic hotspots is more than one-million-times smaller than what could be achieved by free-space IR photons, and their real-space distributions are controlled by the sizes and shapes of the nanobubbles. Theoretical analysis indicates that the observed plasmonic hotspots are formed due to a significant increase of the local plasmon wavelength in the nanobubble regions. Such an increase is attributed to the high sensitivity of graphene plasmons to its dielectric environment. Our work presents a novel scheme for plasmonic hotspot formation and sheds light on future applications of graphene nanobubbles for plasmon-enhanced IR spectroscopy.

  8. Plasmonic superfocusing on metallic tips for near-field optical imaging and spectroscopy

    Science.gov (United States)

    Neacsu, Catalin C.; Olmon, Rob; Berweger, Samuel; Kappus, Alexandria; Kirchner, Friedrich; Ropers, Claus; Saraf, Lax; Raschke, Markus B.

    2008-03-01

    Realization of localized light sources through nonlocal excitation is important in the context of plasmon photonics, molecular sensing, and in particular near-field optical techniques. Here, the efficient conversion of propagating surface plasmons, launched on the shaft of a scanning probe tip, into localized plasmon at the apex provides a true nanoconfined light source. Focused ion beam milling is used to generate periodic surface nanostructures on the tip shaft that allow for tailoring the plasmon excitation. Using ultrashort visible and mid-IR transients the dynamics of the propagation and subsequent scattered emission is characterized. The strong field enhancement and spatial field confinement at the apex is demonstrated studying the coupling of the tip in near-field interaction with a flat sample surface. It is used in scattering near-field spectroscopic imaging (s-SNOM) to probe surface nanostructures with spatial resolution down to 10 nm.

  9. Strong Coupling and Entanglement of Quantum Emitters Embedded in a Nanoantenna-Enhanced Plasmonic Cavity

    Energy Technology Data Exchange (ETDEWEB)

    Hensen, Matthias [Institut; Heilpern, Tal [Center; Gray, Stephen K. [Center; Pfeiffer, Walter [Fakultät

    2017-10-12

    Establishing strong coupling between spatially separated and thus selectively addressable quantum emitters is a key ingredient to complex quantum optical schemes in future technologies. Insofar as many plasmonic nanostructures are concerned, however, the energy transfer and mutual interaction strength between distant quantum emitters can fail to provide strong coupling. Here, based on mode hybridization, the longevity and waveguide character of an elliptical plasmon cavity are combined with intense and highly localized field modes of suitably designed nanoantennas. Based on FDTD simulations a quantum emitter-plasmon coupling strength hg = 16.7 meV is reached while simultaneously keeping a small plasmon resonance line width h gamma(s) = 33 meV. This facilitates strong coupling, and quantum dynamical simulations reveal an oscillatory exchange of excited state population arid a notable degree of entanglement between the quantum emitters spatially separated by 1.8 mu m, i.e., about twice the operating wavelength.

  10. Roadmap of ultrafast x-ray atomic and molecular physics

    Science.gov (United States)

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

    2018-02-01

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

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

    Science.gov (United States)

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

    2010-11-05

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

  12. Ultrafast stimulated Raman spectroscopy in the near-infrared region

    International Nuclear Information System (INIS)

    Takaya, Tomohisa

    2016-01-01

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

  13. Real-Time Observation of Internal Motion within Ultrafast Dissipative Optical Soliton Molecules

    Science.gov (United States)

    Krupa, Katarzyna; Nithyanandan, K.; Andral, Ugo; Tchofo-Dinda, Patrice; Grelu, Philippe

    2017-06-01

    Real-time access to the internal ultrafast dynamics of complex dissipative optical systems opens new explorations of pulse-pulse interactions and dynamic patterns. We present the first direct experimental evidence of the internal motion of a dissipative optical soliton molecule generated in a passively mode-locked erbium-doped fiber laser. We map the internal motion of a soliton pair molecule by using a dispersive Fourier-transform imaging technique, revealing different categories of internal pulsations, including vibrationlike and phase drifting dynamics. Our experiments agree well with numerical predictions and bring insights to the analogy between self-organized states of lights and states of the matter.

  14. Compact plasmonic variable optical attenuator

    DEFF Research Database (Denmark)

    Leosson, Kristjan; Rosenzveig, Tiberiu; Hermannsson, Pétur Gordon

    2008-01-01

    We demonstrate plasmonic nanowire-based thermo-optic variable optical attenuators operating in the 1525-1625 nm wavelength range. The devices have a footprint as low as 1 mm, extinction ratio exceeding 40 dB, driving voltage below 3 V, and full modulation bandwidth of 1 kHz. The polarization...

  15. Capturing inhomogeneous broadening of the -CN stretch vibration in a Langmuir monolayer with high-resolution spectra and ultrafast vibrational dynamics in sum-frequency generation vibrational spectroscopy (SFG-VS)

    Science.gov (United States)

    Velarde, Luis; Wang, Hong-fei

    2013-08-01

    While in principle the frequency-domain and time-domain spectroscopic measurements should generate identical information for a given molecular system, the inhomogeneous character of surface vibrations in sum-frequency generation vibrational spectroscopy (SFG-VS) studies has only been studied with time-domain SFG-VS by mapping the decay of the vibrational polarization using ultrafast lasers, this due to the lack of SFG vibrational spectra with high enough spectral resolution and accurate enough lineshape. Here, with the recently developed high-resolution broadband SFG-VS (HR-BB-SFG-VS) technique, we show that the inhomogeneous lineshape can be obtained in the frequency-domain for the anchoring CN stretch of the 4-n-octyl-4'-cyanobiphenyl (8CB) Langmuir monolayer at the air-water interface, and that an excellent agreement with the time-domain SFG free-induction-decay can be established. We found that the 8CB CN stretch spectrum consists of a single peak centered at 2234.00 ± 0.01 cm-1 with a total linewidth of 10.9 ± 0.3 cm-1 at half maximum. The Lorentzian contribution accounts only for 4.7 ± 0.4 cm-1 to this width and the Gaussian (inhomogeneous) broadening for as much as 8.1 ± 0.2 cm-1. Polarization analysis of the -CN spectra showed that the -CN group is tilted 57° ± 2° from the surface normal. The large heterogeneity in the -CN spectrum is tentatively attributed to the -CN group interactions with the interfacial water molecules penetrated/accommodated into the 8CB monolayer, a unique phenomenon for the nCB Langmuir monolayers reported previously.

  16. Parametric spectro-temporal analyzer (PASTA) for ultrafast optical performance monitoring

    Science.gov (United States)

    Zhang, Chi; Wong, Kenneth K. Y.

    2013-12-01

    Ultrafast optical spectrum monitoring is one of the most challenging tasks in observing ultrafast phenomena, such as the spectroscopy, dynamic observation of the laser cavity, and spectral encoded imaging systems. However, conventional method such as optical spectrum analyzer (OSA) spatially disperses the spectrum, but the space-to-time mapping is realized by mechanical rotation of a grating, so are incapable of operating at high speed. Besides the spatial dispersion, temporal dispersion provided by dispersive fiber can also stretches the spectrum in time domain in an ultrafast manner, but is primarily confined in measuring short pulses. In view of these constraints, here we present a real-time spectrum analyzer called parametric spectro-temporal analyzer (PASTA), which is based on the time-lens focusing mechanism. It achieves a 100-MHz frame rate and can measure arbitrary waveforms. For the first time, we observe the dynamic spectrum of an ultrafast swept-source: Fourier domain mode-locked (FDML) laser, and the spectrum evolution of a laser cavity during its stabilizing process. In addition to the basic single-lens structure, the multi-lens configurations (e.g. telescope or wide-angle scope) will provide a versatile operating condition, which can zoom in to achieve 0.05-nm resolution and zoom out to achieve 10-nm observation range, namely 17 times zoom in/out ratio. In view of the goal of achieving spectrum analysis with fine accuracy, PASTA provides a promising path to study the real-time spectrum of some dynamic phenomena and non-repetitive events, with orders of magnitude enhancement in the frame rate over conventional OSAs.

  17. Spin-controlled ultrafast vertical-cavity surface-emitting lasers

    Science.gov (United States)

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

    2014-05-01

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

  18. Parameter estimation in plasmonic QED

    Science.gov (United States)

    Jahromi, H. Rangani

    2018-03-01

    We address the problem of parameter estimation in the presence of plasmonic modes manipulating emitted light via the localized surface plasmons in a plasmonic waveguide at the nanoscale. The emitter that we discuss is the nitrogen vacancy centre (NVC) in diamond modelled as a qubit. Our goal is to estimate the β factor measuring the fraction of emitted energy captured by waveguide surface plasmons. The best strategy to obtain the most accurate estimation of the parameter, in terms of the initial state of the probes and different control parameters, is investigated. In particular, for two-qubit estimation, it is found although we may achieve the best estimation at initial instants by using the maximally entangled initial states, at long times, the optimal estimation occurs when the initial state of the probes is a product one. We also find that decreasing the interqubit distance or increasing the propagation length of the plasmons improve the precision of the estimation. Moreover, decrease of spontaneous emission rate of the NVCs retards the quantum Fisher information (QFI) reduction and therefore the vanishing of the QFI, measuring the precision of the estimation, is delayed. In addition, if the phase parameter of the initial state of the two NVCs is equal to πrad, the best estimation with the two-qubit system is achieved when initially the NVCs are maximally entangled. Besides, the one-qubit estimation has been also analysed in detail. Especially, we show that, using a two-qubit probe, at any arbitrary time, enhances considerably the precision of estimation in comparison with one-qubit estimation.

  19. A high figure of merit localized surface plasmon sensor based on a gold nanograting on the top of a gold planar film

    International Nuclear Information System (INIS)

    Zhang Zu-Yin; Wang Li-Na; Hu Hai-Feng; Li Kang-Wen; Ma Xun-Peng; Song Guo-Feng

    2013-01-01

    We investigate the sensitivity and figure of merit (FOM) of a localized surface plasmon (LSP) sensor with gold nanograting on the top of planar metallic film. The sensitivity of the localized surface plasmon sensor is 317 nm/RIU, and the FOM is predicted to be above 8, which is very high for a localized surface plasmon sensor. By employing the rigorous coupled-wave analysis (RCWA) method, we analyze the distribution of the magnetic field and find that the sensing property of our proposed system is attributed to the interactions between the localized surface plasmon around the gold nanostrips and the surface plasmon polarition on the surface of the gold planar metallic film. These findings are important for developing high FOM localized surface plasmon sensors. (electromagnetism, optics, acoustics, heat transfer, classical mechanics, and fluid dynamics)

  20. Ultracompact Pseudowedge Plasmonic Lasers and Laser Arrays.

    Science.gov (United States)

    Chou, Yu-Hsun; Hong, Kuo-Bin; Chang, Chun-Tse; Chang, Tsu-Chi; Huang, Zhen-Ting; Cheng, Pi-Ju; Yang, Jhen-Hong; Lin, Meng-Hsien; Lin, Tzy-Rong; Chen, Kuo-Ping; Gwo, Shangjr; Lu, Tien-Chang

    2018-02-14

    Concentrating light at the deep subwavelength scale by utilizing plasmonic effects has been reported in various optoelectronic devices with intriguing phenomena and functionality. Plasmonic waveguides with a planar structure exhibit a two-dimensional degree of freedom for the surface plasmon; the degree of freedom can be further reduced by utilizing metallic nanostructures or nanoparticles for surface plasmon resonance. Reduction leads to different lightwave confinement capabilities, which can be utilized to construct plasmonic nanolaser cavities. However, most theoretical and experimental research efforts have focused on planar surface plasmon polariton (SPP) nanolasers. In this study, we combined nanometallic structures intersecting with ZnO nanowires and realized the first laser emission based on pseudowedge SPP waveguides. Relative to current plasmonic nanolasers, the pseudowedge plasmonic lasers reported in our study exhibit extremely small mode volumes, high group indices, high spontaneous emission factors, and high Purell factors beneficial for the strong interaction between light and matter. Furthermore, we demonstrated that compact plasmonic laser arrays can be constructed, which could benefit integrated plasmonic circuits.