WorldWideScience

Sample records for femtosecond coherent spectroscopy

  1. Coherent Femtosecond Spectroscopy and Nonlinear Optical Imaging on the Nanoscale

    Science.gov (United States)

    Kravtsov, Vasily

    Optical properties of many materials and macroscopic systems are defined by ultrafast dynamics of electronic, vibrational, and spin excitations localized on the nanoscale. Harnessing these excitations for material engineering, optical computing, and control of chemical reactions has been a long-standing goal in science and technology. However, it is challenging due to the lack of spectroscopic techniques that can resolve processes simultaneously on the nanometer spatial and femtosecond temporal scales. This thesis describes the fundamental principles, implementation, and experimental demonstration of a novel type of ultrafast microscopy based on the concept of adiabatic plasmonic nanofocusing. Simultaneous spatio-temporal resolution on a nanometer-femtosecond scale is achieved by using a near-field nonlinear optical response induced by ultrafast surface plasmon polaritons nanofocused on a metal tip. First, we study the surface plasmon response in metallic structures and evaluate its prospects and limitations for ultrafast near-field microscopy. Through plasmon emission-based spectroscopy, we investigate dephasing times and interplay between radiative and non-radiative decay rates of localized plasmons and their modification due to coupling. We identify a new regime of quantum plasmonic coupling, which limits the achievable spatial resolution to several angstroms but at the same time provides a potential channel for generating ultrafast electron currents at optical frequencies. Next, we study propagation of femtosecond wavepackets of surface plasmon polaritons on a metal tip. In time-domain interferometric measurements we detect group delays that correspond to slowing of the plasmon polaritons down to 20% of the speed of light at the tip apex. This provides direct experimental verification of the plasmonic nanofocusing mechanism and suggests enhanced nonlinear optical interactions at the tip apex. We then measure a plasmon-generated third-order nonlinear optical

  2. Femtosecond Coherent Anti-Stokes Raman Spectroscopy (CARS) As Next Generation Nonlinear LIDAR Spectroscopy and Microscopy

    International Nuclear Information System (INIS)

    Ooi, C. H. Raymond

    2009-01-01

    Nonlinear spectroscopy using coherent anti-Stokes Raman scattering and femtosecond laser pulses has been successfully developed as powerful tools for chemical analysis and biological imaging. Recent developments show promising possibilities of incorporating CARS into LIDAR system for remote detection of molecular species in airborne particles. The corresponding theory is being developed to describe nonlinear scattering of a mesoscopic particle composed of complex molecules by laser pulses with arbitrary shape and spectral content. Microscopic many-body transform theory is used to compute the third order susceptibility for CARS in molecules with known absorption spectrum and vibrational modes. The theory is combined with an integral scattering formula and Mie-Lorentz formulae, giving a rigorous formalism which provides powerful numerical experimentation of CARS spectra, particularly on the variations with the laser parameters and the direction of detection.

  3. Femtosecond spectroscopy in semiconductors: a key to coherences, correlations and quantum kinetics

    International Nuclear Information System (INIS)

    Axt, V M; Kuhn, T

    2004-01-01

    The application of femtosecond spectroscopy to the study of ultrafast dynamics in semiconductor materials and nanostructures is reviewed with particular emphasis on the physics that can be learned from it. Excitation with ultrashort optical pulses in general results in the creation of coherent superpositions and correlated many-particle states. The review comprises a discussion of the dynamics of this correlated many-body system during and after pulsed excitation as well as its analysis by means of refined measurements and advanced theories. After an introduction of basic concepts-such as coherence, correlation and quantum kinetics-a brief overview of the most important experimental techniques and theoretical approaches is given. The remainder of this paper is devoted to specific results selected in order to highlight how femtosecond spectroscopy gives access to the physics of coherences, correlations and quantum kinetics involving charge, spin and lattice degrees of freedom. First examples deal with the dynamics of basic laser-induced coherences that can be observed, e.g. in quantum beat spectroscopy, in coherent control measurements or in experiments using few-cycle pulses. The phenomena discussed here are basic in the sense that they can be understood to a large extent on the mean-field level of the theory. Nevertheless, already on this level it is found that semiconductors behave substantially differently from atomic systems. Subsequent sections report on the occurrence of coherences and correlations beyond the mean-field level that are mediated either by carrier-phonon or carrier-carrier interactions. The corresponding analysis gives deep insight into fundamental issues such as the energy-time uncertainty, pure dephasing in quantum dot structures, the role of two-pair or even higher correlations and the build-up of screening. Finally results are presented concerning the ultrafast dynamics of resonantly coupled excitations, where a combination of different

  4. Femtosecond laser spectroscopy

    CERN Document Server

    Hannaford, Peter

    2005-01-01

    As concepts and methodologies have evolved over the past two decades, the realm of ultrafast science has become vast and exciting and has impacted many areas of chemistry, biology and physics, and other fields such as materials science, electrical engineering, and optical communication. The field has recently exploded with the announcement of a series of remarkable new developments and advances. This volume surveys this recent growth in eleven chapters written by leading international researchers in the field. It includes sections on femtosecond optical frequency combs, soft x-ray femtosecond laser sources, and attosecond laser sources. In addition, the contributors address real-time spectroscopy of molecular vibrations with sub-5-fs pulses and multidimensional femtosecond coherent spectroscopies for studying molecular and electron dynamics. Novel methods for measuring and characterizing ultrashort laser pulses and ultrashort pulses of light are also described. The topics covered are revolutionizing the field...

  5. Resolving fine spectral features in lattice vibrational modes using femtosecond coherent spectroscopy

    Directory of Open Access Journals (Sweden)

    A. Card

    2016-02-01

    Full Text Available We show resolution of fine spectral features within several Raman active vibrational modes in potassium titanyl phosphate (KTP crystal. Measurements are performed using a femtosecond time-domain coherent anti-Stokes Raman scattering spectroscopy technique that is capable of delivering equivalent spectral resolution of 0.1 cm−1. The Raman spectra retrieved from our measurements show several spectral components corresponding to vibrations of different symmetry with distinctly different damping rates. In particular, linewidths for unassigned optical phonon mode triplet centered at around 820 cm−1 are found to be 7.5 ± 0.2 cm−1, 9.1 ± 0.3 cm−1, and 11.2 ± 0.3 cm−1. Results of our experiments will ultimately help to design an all-solid-state source for sub-optical-wavelength waveform generation that is based on stimulated Raman scattering.

  6. Temperature Measurements in Reacting Flows Using Time-Resolved Femtosecond Coherent Anti-Stokes Raman Scattering (fs-CARS) Spectroscopy (Postprint)

    National Research Council Canada - National Science Library

    Roy, Sukesh; Kinnius, Paul J; Lucht, Robert P; Gord, James R

    2007-01-01

    Time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of the nitrogen molecule is used for the measurement of temperature in atmospheric-pressure, near-adiabatic, hydrogen-air diffusion flames...

  7. Femtosecond pulse laser notch shaping via fiber Bragg grating for the excitation source on the coherent anti-Stokes Raman spectroscopy

    Science.gov (United States)

    Oh, Seung Ryeol; Kwon, Won Sik; Kim, Jin Hwan; Kim, Kyung-Soo; Kim, Soohyun

    2015-03-01

    Single-pulse coherently controlled nonlinear Raman spectroscopy is the simplest method among the coherent anti-Stokes Raman spectroscopy systems. In recent research, it has been proven that notch-shaped femtosecond pulse laser can be used to collect the coherent anti-Stokes Raman signals. In this study, we applied a fiber Bragg grating to the notch filtering component on the femtosecond pulse lasers. The experiment was performed incorporating a titanium sapphire femtosecond pulse laser source with a 100 mm length of 780-HP fiber which is inscribed 30 mm of Bragg grating. The fiber Bragg grating has 785 nm Bragg wavelength with 0.9 nm bandwidth. We proved that if the pulse lasers have above a certain level of positive group delay dispersion, it is sufficient to propagate in the fiber Bragg grating without any spectral distortion. After passing through the fiber Bragg grating, the pulse laser is reflected on the chirped mirror for 40 times to make the transform-limited pulse. Finally, the pulse time duration was 37 fs, average power was 50mW, and showed an adequate notch shape. Furthermore, the simulation of third order polarization signal is performed using MATLAB tools and the simulation result shows that spectral characteristic and time duration of the pulse is sufficient to use as an excitation source for single-pulse coherent anti-Stokes Raman spectroscopy. In conclusion, the proposed method is more simple and cost-effective than the methods of previous research which use grating pairs and resonant photonic crystal slab.

  8. A multi-channel THz and infrared spectrometer for femtosecond electron bunch diagnostics by single-shot spectroscopy of coherent radiation

    Energy Technology Data Exchange (ETDEWEB)

    Wesch, Stephan; Schmidt, Bernhard; Behrens, Christopher; Delsim-Hashemi, Hossein; Schmueser, Peter

    2011-08-15

    The high peak current required in free-electron lasers (FELs) is realized by longitudinal compression of the electron bunches to sub-picosecond length. In this paper, a frequency-domain diagnostic method is described that is capable of resolving structures in the femtosecond regime. A novel in-vacuum spectrometer has been developed for spectroscopy of coherent radiation in the THz and infrared range. The spectrometer is equipped with five consecutive dispersion gratings and 120 parallel readout channels; it can be operated either in short wavelength mode (5-44 {mu}m) or in long wavelength mode (45-430 {mu}m). Fast parallel readout permits the spectroscopy of coherent radiation from single electron bunches. Test measurements at the soft X-ray free-electron laser FLASH, using coherent transition radiation, demonstrate excellent performance of the spectrometer. The high sensitivity down to a few micrometers allows study of short bunch features caused for example by microbunching e ects in magnetic chicanes. The device is planned for use as an online bunch profile monitor during regular FEL operation. (orig.)

  9. A multi-channel THz and infrared spectrometer for femtosecond electron bunch diagnostics by single-shot spectroscopy of coherent radiation

    International Nuclear Information System (INIS)

    Wesch, Stephan; Schmidt, Bernhard; Behrens, Christopher; Delsim-Hashemi, Hossein; Schmueser, Peter

    2011-08-01

    The high peak current required in free-electron lasers (FELs) is realized by longitudinal compression of the electron bunches to sub-picosecond length. In this paper, a frequency-domain diagnostic method is described that is capable of resolving structures in the femtosecond regime. A novel in-vacuum spectrometer has been developed for spectroscopy of coherent radiation in the THz and infrared range. The spectrometer is equipped with five consecutive dispersion gratings and 120 parallel readout channels; it can be operated either in short wavelength mode (5-44 μm) or in long wavelength mode (45-430 μm). Fast parallel readout permits the spectroscopy of coherent radiation from single electron bunches. Test measurements at the soft X-ray free-electron laser FLASH, using coherent transition radiation, demonstrate excellent performance of the spectrometer. The high sensitivity down to a few micrometers allows study of short bunch features caused for example by microbunching e ects in magnetic chicanes. The device is planned for use as an online bunch profile monitor during regular FEL operation. (orig.)

  10. Femtosecond Broadband Stimulated Raman Spectroscopy

    International Nuclear Information System (INIS)

    Lee, Soo-Y; Yoon, Sagwoon; Mathies, Richard A

    2006-01-01

    Femtosecond broadband stimulated Raman spectroscopy (FSRS) is a new technique where a narrow bandwidth picosecond Raman pump pulse and a red-shifted broadband femtosecond Stokes probe pulse (with or without time delay between the pulses) act on a sample to produce a high resolution Raman gain spectrum with high efficiency and speed, free from fluorescence background interference. It can reveal vibrational structural information and dynamics of stationary or transient states. Here, the quantum picture for femtosecond broadband stimulated Raman spectroscopy (FSRS) is used to develop the semiclassical coupled wave theory of the phenomenon and to derive an expression for the measurable Raman gain in FSRS. The semiclassical theory is applied to study the dependence of lineshapes in FSRS on the pump-probe time delay and to deduce vibrational dephasing times in cyclohexane in the ground state

  11. Femtosecond coherent emission from GaAs bulk microcavities

    Science.gov (United States)

    Gurioli, Massimo; Bogani, Franco; Ceccherini, Simone; Colocci, Marcello; Beltram, Fabio; Sorba, Lucia

    1999-02-01

    The emission from a λ/2 GaAs bulk microcavity resonantly excited by femtosecond pulses has been characterized by using an interferometric correlation technique. It is found that the emission is dominated by the coherent signal due to light elastically scattered by disorder, and that scattering is predominantly originated from the lower polariton branch.

  12. Multichannel Selective Femtosecond Coherent Control Based on Symmetry Properties

    International Nuclear Information System (INIS)

    Amitay, Zohar; Gandman, Andrey; Chuntonov, Lev; Rybak, Leonid

    2008-01-01

    We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of ''two-photon dark pulses'' inducing widely tunable three-photon absorption

  13. Two-dimensional electronic femtosecond stimulated Raman spectroscopy

    Directory of Open Access Journals (Sweden)

    Ogilvie J.P.

    2013-03-01

    Full Text Available We report two-dimensional electronic spectroscopy with a femtosecond stimulated Raman scattering probe. The method reveals correlations between excitation energy and excited state vibrational structure following photoexcitation. We demonstrate the method in rhodamine 6G.

  14. Coherent atomic spectroscopy

    International Nuclear Information System (INIS)

    Garton, W.R.S.

    1988-01-01

    The Argonne Spectroscopy Laboratory, initiated and advanced over several decades by F.S. Tomkins and M. Fred, has been a major international facility. A range of collaborative work in atomic spectroscopy is selected to illustrate advances in experimental physics which have been made possible by combination of the talents of Tomkins and Fred with the unique facilities of the Argonne Laboratory. (orig.)

  15. Femtosecond infrared spectroscopy: study, development and applications

    International Nuclear Information System (INIS)

    Bonvalet, Adeline

    1997-01-01

    This work has been devoted to the development and the applications of a new technique of infrared (5-20 μm) spectroscopy allowing a temporal resolution of 100 fs. This technique relies on a source of ultrashort infrared pulses obtained by frequency mixing in a nonlinear material. In particular, the optical rectification of 12-fs visible pulses in gallium arsenide has allowed us to obtain 40-fs infrared pulses with a spectrum extending from 5 pm up to 15 μm. Spectral resolution has been achieved by Fourier transform spectroscopy, using a novel device we have called Diffracting FTIR. These developments allow to study inter-subband transitions in quantum-well structures. The inter-subband relaxation time has been measured by a pump-probe experiment, in which the sample was excited with a visible pulse, and the variations of inter-subband absorption probed with an infrared pulse. Besides, we have developed a method of coherent emission spectroscopy allowing to monitor the electric field emitted by coherent charge oscillations in quantum wells. The decay of the oscillations due to the loss of coherence between excited levels yields a direct measurement of the dephasing time between these levels. Other applications include biological macromolecules like reaction centers of photosynthetic bacteria. We have shown that we were able to monitor variations of infrared absorption of about 10 -4 optical densities with a temporal resolution of 100 fs. This would constitute a relevant tool to study the role of molecular vibrations during the primary steps of biological processes. (author) [fr

  16. Undulators to FELs: Nanometers, Femtoseconds, Coherence and Applications

    Energy Technology Data Exchange (ETDEWEB)

    Attwood, David [University of California Berkeley

    2011-11-30

    For scientists in many fields, from material science to the life sciences and archeology, synchrotron radiation, and in particular undulator radiation, has provide an intense source of x-rays which are tunable to the absorption edges of particular elements of interest, often permitting studies at high spatial and spectral resolution. Now a close cousin to the undulator, the x-ray free electron laser (XFEL) has emerged with improved spatial coherence and, perhaps more importantly, femtosecond pulse durations which permit dynamical studies. In the future attosecond x-ray capabilities are anticipated. In this colloqium we will describe some state of the art undulator studies, how undulators work, the evolution to FELs, their pulse and coherence properties, and the types of experiments envisioned.

  17. Xanthines Studied via Femtosecond Fluorescence Spectroscopy

    Directory of Open Access Journals (Sweden)

    Pascale Changenet-Barret

    2016-12-01

    Full Text Available Xanthines represent a wide class of compounds closely related to the DNA bases adenine and guanine. Ubiquitous in the human body, they are capable of replacing natural bases in double helices and give rise to four-stranded structures. Although the use of their fluorescence for analytical purposes was proposed, their fluorescence properties have not been properly characterized so far. The present paper reports the first fluorescence study of xanthine solutions relying on femtosecond spectroscopy. Initially, we focus on 3-methylxanthine, showing that this compound exhibits non-exponential fluorescence decays with no significant dependence on the emission wavelength. The fluorescence quantum yield (3 × 10−4 and average decay time (0.9 ps are slightly larger than those found for the DNA bases. Subsequently, we compare the dynamical fluorescence properties of seven mono-, di- and tri-methylated derivatives. Both the fluorescence decays and fluorescence anisotropies vary only weakly with the site and the degree of methylation. These findings are in line with theoretical predictions suggesting the involvement of several conical intersections in the relaxation of the lowest singlet excited state.

  18. Femtosecond two-dimensional spectroscopy of molecular motion in liquids

    NARCIS (Netherlands)

    Steffen, T; Duppen, K.

    1996-01-01

    Intermolecular motion in CS2 and benzene is investigated by femtosecond nonresonant four- and six-wave mixing. Impulsive stimulated six-wave mixing yields new information on dephasing of coherent nuclear motion, not accessible from four-wave mixing experiments. The results cannot be modeled by two

  19. Clocking Femtosecond Collisional Dynamics via Resonant X-Ray Spectroscopy

    Science.gov (United States)

    van den Berg, Q. Y.; Fernandez-Tello, E. V.; Burian, T.; Chalupský, J.; Chung, H.-K.; Ciricosta, O.; Dakovski, G. L.; Hájková, V.; Hollebon, P.; Juha, L.; Krzywinski, J.; Lee, R. W.; Minitti, M. P.; Preston, T. R.; de la Varga, A. G.; Vozda, V.; Zastrau, U.; Wark, J. S.; Velarde, P.; Vinko, S. M.

    2018-02-01

    Electron-ion collisional dynamics is of fundamental importance in determining plasma transport properties, nonequilibrium plasma evolution, and electron damage in diffraction imaging applications using bright x-ray free-electron lasers (FELs). Here we describe the first experimental measurements of ultrafast electron impact collisional ionization dynamics using resonant core-hole spectroscopy in a solid-density magnesium plasma, created and diagnosed with the Linac Coherent Light Source x-ray FEL. By resonantly pumping the 1 s →2 p transition in highly charged ions within an optically thin plasma, we have measured how off-resonance charge states are populated via collisional processes on femtosecond time scales. We present a collisional cross section model that matches our results and demonstrates how the cross sections are enhanced by dense-plasma effects including continuum lowering. Nonlocal thermodynamic equilibrium collisional radiative simulations show excellent agreement with the experimental results and provide new insight on collisional ionization and three-body-recombination processes in the dense-plasma regime.

  20. Coherent vs Incoherent Emission from Semiconductor Structures after Resonant Femtosecond Excitation

    Science.gov (United States)

    Gurioli, Massimo; Bogani, Franco; Ceccherini, Simone; Colocci, Marcello

    1997-04-01

    We show that an interferometric correlation measurement with fs time resolution provides an unambiguous discrimination between coherent and incoherent emission after resonant femtosecond excitation. The experiment directly probes the most important difference between the two emissions, that is, the phase correlation with the excitation pulse. The comparison with cw frequency resolved measurements demonstrates that the relationship between coherent and incoherent emission is similar under femtosecond and steady-state excitation.

  1. Femtosecond pump–probe spectroscopy of graphene oxide in water

    International Nuclear Information System (INIS)

    Shang, Jingzhi; Ma, Lin; Li, Jiewei; Ai, Wei; Yu, Ting; Gurzadyan, Gagik G

    2014-01-01

    Transient absorption properties of aqueous graphene oxide (GO) have been studied by use of femtosecond pump–probe spectroscopy. Excited state absorption and photobleaching are observed in the wide spectral range. The observed fast three lifetime components are attributed to the absorption of upper excited states and localized states, which is confirmed by both laser induced absorption and transmission kinetics. The longest time component is assigned to the lowest excited state of GO, which mainly originates from the sp2 domains. With the increase of the excitation power, two-quantum absorption occurs, which results in an additional rise-time component of the observed transients. (paper)

  2. Rotational coherence spectroscopy at FLASH. Toward dynamic studies in nanosuperfluids

    Energy Technology Data Exchange (ETDEWEB)

    Kickermann, Andreas

    2013-07-15

    The field of molecular physics, which is focusing on molecular motion in the transition states of physical, chemical, and biological changes, is a wide-spread research area. It strives to reveal the structural and functional properties of molecules, the chemical bonds between atoms and the time evolution. Many processes occurring in nature upon electronic excitation proceed on the ultrafast femtosecond timescale and can be triggered by modern ultrashort femtosecond-laser sources under laboratory conditions. In the present thesis pump-probe studies were performed to follow molecular motion using ultrashort light pulses in the nanometer wavelength range provided by an XUV freeelectron laser (FEL). In detail, alignment of molecular species in space under field-free conditions was investigated. In the specific case of rotational wave packets in molecules the rotational dynamics shows characteristic temporal features, which contain a wealth of information on molecular structure and give insight into molecular coupling mechanisms, i.e. rotational constants and transition frequencies. Within this thesis, Rotational Coherence Spectroscopy (RCS) reveals wave-packet motion observed by subsequent Coulomb explosion of Raman excited carbon monoxide, which results in a time-dependent asymmetry of spatial fragmentation patterns. With the method presented here, the time resolution to elucidate the fast dynamics of strong couplings can be pushed toward a single rotational period even for the fastest rotors. This is due to large pump-probe delays with small subpicosecond step size. This kind of spectroscopy can also be expanded to molecular species, which are not accessible by other powerful spectroscopic methods, such as Fourier-transform microwave spectroscopy (FTMW). Furthermore, it allows to measure weak molecular couplings on a long timescale (large pump-probe delays), e.g. couplings of molecules in a solution or molecules dissolved in quantum fluids. This is valuable to

  3. Rotational coherence spectroscopy at FLASH. Toward dynamic studies in nanosuperfluids

    International Nuclear Information System (INIS)

    Kickermann, Andreas

    2013-07-01

    The field of molecular physics, which is focusing on molecular motion in the transition states of physical, chemical, and biological changes, is a wide-spread research area. It strives to reveal the structural and functional properties of molecules, the chemical bonds between atoms and the time evolution. Many processes occurring in nature upon electronic excitation proceed on the ultrafast femtosecond timescale and can be triggered by modern ultrashort femtosecond-laser sources under laboratory conditions. In the present thesis pump-probe studies were performed to follow molecular motion using ultrashort light pulses in the nanometer wavelength range provided by an XUV freeelectron laser (FEL). In detail, alignment of molecular species in space under field-free conditions was investigated. In the specific case of rotational wave packets in molecules the rotational dynamics shows characteristic temporal features, which contain a wealth of information on molecular structure and give insight into molecular coupling mechanisms, i.e. rotational constants and transition frequencies. Within this thesis, Rotational Coherence Spectroscopy (RCS) reveals wave-packet motion observed by subsequent Coulomb explosion of Raman excited carbon monoxide, which results in a time-dependent asymmetry of spatial fragmentation patterns. With the method presented here, the time resolution to elucidate the fast dynamics of strong couplings can be pushed toward a single rotational period even for the fastest rotors. This is due to large pump-probe delays with small subpicosecond step size. This kind of spectroscopy can also be expanded to molecular species, which are not accessible by other powerful spectroscopic methods, such as Fourier-transform microwave spectroscopy (FTMW). Furthermore, it allows to measure weak molecular couplings on a long timescale (large pump-probe delays), e.g. couplings of molecules in a solution or molecules dissolved in quantum fluids. This is valuable to

  4. Multidimensional coherent spectroscopy made easy

    Energy Technology Data Exchange (ETDEWEB)

    Gundogdu, Kenan; Stone, Katherine W.; Turner, Daniel B. [Department of Chemistry, Massachusetts Institute of Technology, 77 Mass Ave. 6-026 Cambridge, MA 02139 (United States); Nelson, Keith A. [Department of Chemistry, Massachusetts Institute of Technology, 77 Mass Ave. 6-026 Cambridge, MA 02139 (United States)], E-mail: kanelson@mit.edu

    2007-11-15

    We have demonstrated a highly efficient fully coherent 2D spectrometer based on 2D pulse shaping and Fourier beam shaping. The versatility of the design allows one to measure different 2D spectral surfaces consecutively. Easy alignment, inherent phase stability, rotating wave frame detection, and arbitrary waveform generation in all of the beams are important features of this design. We have demonstrated the functionality of the 2D spectrometer by measuring a 2D spectral surface of a GaAs quantum well.

  5. Multidimensional coherent spectroscopy made easy

    International Nuclear Information System (INIS)

    Gundogdu, Kenan; Stone, Katherine W.; Turner, Daniel B.; Nelson, Keith A.

    2007-01-01

    We have demonstrated a highly efficient fully coherent 2D spectrometer based on 2D pulse shaping and Fourier beam shaping. The versatility of the design allows one to measure different 2D spectral surfaces consecutively. Easy alignment, inherent phase stability, rotating wave frame detection, and arbitrary waveform generation in all of the beams are important features of this design. We have demonstrated the functionality of the 2D spectrometer by measuring a 2D spectral surface of a GaAs quantum well

  6. Simultaneous Femtosecond X-ray Spectroscopy and Diffraction of Photosystem II at Room Temperature

    Science.gov (United States)

    Kern, Jan; Alonso-Mori, Roberto; Tran, Rosalie; Hattne, Johan; Gildea, Richard J.; Echols, Nathaniel; Glöckner, Carina; Hellmich, Julia; Laksmono, Hartawan; Sierra, Raymond G.; Lassalle-Kaiser, Benedikt; Koroidov, Sergey; Lampe, Alyssa; Han, Guangye; Gul, Sheraz; DiFiore, Dörte; Milathianaki, Despina; Fry, Alan R.; Miahnahri, Alan; Schafer, Donald W.; Messerschmidt, Marc; Seibert, M. Marvin; Koglin, Jason E.; Sokaras, Dimosthenis; Weng, Tsu-Chien; Sellberg, Jonas; Latimer, Matthew J.; Grosse-Kunstleve, Ralf W.; Zwart, Petrus H.; White, William E.; Glatzel, Pieter; Adams, Paul D.; Bogan, Michael J.; Williams, Garth J.; Boutet, Sébastien; Messinger, Johannes; Zouni, Athina; Sauter, Nicholas K.; Yachandra, Vittal K.; Bergmann, Uwe; Yano, Junko

    2013-01-01

    Intense femtosecond X-ray pulses produced at the Linac Coherent Light Source (LCLS) were used for simultaneous X-ray diffraction (XRD) and X-ray emission spectroscopy (XES) of microcrystals of Photosystem II (PS II) at room temperature. This method probes the overall protein structure and the electronic structure of the Mn4CaO5 cluster in the oxygen-evolving complex of PS II. XRD data are presented from both the dark state (S1) and the first illuminated state (S2) of PS II. Our simultaneous XRD/XES study shows that the PS II crystals are intact during our measurements at the LCLS, not only with respect to the structure of PS II, but also with regard to the electronic structure of the highly radiation sensitive Mn4CaO5 cluster, opening new directions for future dynamics studies. PMID:23413188

  7. Femtosecond time-resolved impulsive stimulated Raman spectroscopy using sub-7-fs pulses: Apparatus and applications

    Energy Technology Data Exchange (ETDEWEB)

    Kuramochi, Hikaru [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako 351-0198 (Japan); Takeuchi, Satoshi; Tahara, Tahei, E-mail: tahei@riken.jp [Molecular Spectroscopy Laboratory, RIKEN, 2-1 Hirosawa, Wako 351-0198 (Japan); Ultrafast Spectroscopy Research Team, RIKEN Center for Advanced Photonics (RAP), 2-1 Hirosawa, Wako 351-0198 (Japan)

    2016-04-15

    We describe details of the setup for time-resolved impulsive stimulated Raman spectroscopy (TR-ISRS). In this method, snapshot molecular vibrational spectra of the photoreaction transients are captured via time-domain Raman probing using ultrashort pulses. Our instrument features transform-limited sub-7-fs pulses to impulsively excite and probe coherent nuclear wavepacket motions, allowing us to observe vibrational fingerprints of transient species from the terahertz to 3000-cm{sup −1} region with high sensitivity. Key optical components for the best spectroscopic performance are discussed. The TR-ISRS measurements for the excited states of diphenylacetylene in cyclohexane are demonstrated, highlighting the capability of our setup to track femtosecond dynamics of all the Raman-active fundamental molecular vibrations.

  8. Development of Femtosecond Stimulated Raman Spectroscopy: Stimulated Raman Gain via Elimination of Cross Phase Modulation

    International Nuclear Information System (INIS)

    Jin, Seung Min; Lee, Young Jong; Yu, Jong Wan; Kim, Seong Keun

    2004-01-01

    We have developed a new femtosecond probe technique by using stimulated Raman spectroscopy. The cross phase modulation in femtosecond time scale associated with off-resonant interaction was shown to be eliminated by integrating the transient gain/loss signal over the time delay between the Raman pump pulse and the continuum pulse. The stimulated Raman gain of neat cyclohexane was obtained to demonstrate the feasibility of the technique. Spectral and temporal widths of stimulated Raman spectra were controlled by using a narrow band pass filter. Femtosecond stimulated Raman spectroscopy was proposed as a highly useful probe in time-resolved vibrational spectroscopy

  9. Optimally shaped narrowband picosecond pulses for femtosecond stimulated Raman spectroscopy.

    Science.gov (United States)

    Hoffman, David P; Valley, David; Ellis, Scott R; Creelman, Mark; Mathies, Richard A

    2013-09-09

    A comparison between a Fabry-Pérot etalon filter and a conventional grating filter for producing the picosecond (ps) Raman pump pulses for femtosecond stimulated Raman spectroscopy (FSRS) is presented. It is shown that for pulses of equal energy the etalon filter produces Raman signals twice as large as that of the grating filter while suppressing the electronically resonant background signal. The time asymmetric profile of the etalon-generated pulse is shown to be responsible for both of these observations. A theoretical discussion is presented which quantitatively supports this hypothesis. It is concluded that etalons are the ideal method for the generation of narrowband ps pulses for FSRS because of the optical simplicity, efficiency, improved FSRS intensity and reduced backgrounds.

  10. Femtosecond upconverted photocurrent spectroscopy of InAs quantum nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Yamada, Yasuhiro [Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011 (Japan); Tex, David M.; Kanemitsu, Yoshihiko, E-mail: kanemitu@scl.kyoto-u.ac.jp [Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011 (Japan); Japan Science and Technology Agency, CREST, Kyoto University, Uji, Kyoto 611-0011 (Japan); Kamiya, Itaru [Toyota Technological Institute, Nagoya, Aichi 468-8511 (Japan)

    2015-07-06

    The carrier upconversion dynamics in InAs quantum nanostructures are studied for intermediate-band solar-cell applications via ultrafast photoluminescence and photocurrent (PC) spectroscopy based on femtosecond excitation correlation (FEC) techniques. Strong upconverted PC-FEC signals are observed under resonant excitation of quantum well islands (QWIs), which are a few monolayer-thick InAs quantum nanostructures. The PC-FEC signal typically decays within a few hundred picoseconds at room temperature, which corresponds to the carrier lifetime in QWIs. The photoexcited electron and hole lifetimes in InAs QWIs are evaluated as functions of temperature and laser fluence. Our results provide solid evidence for electron–hole–hole Auger process, dominating the carrier upconversion in InAs QWIs at room temperature.

  11. Optical spectroscopy using gas-phase femtosecond laser filamentation.

    Science.gov (United States)

    Odhner, Johanan; Levis, Robert

    2014-01-01

    Femtosecond laser filamentation occurs as a dynamic balance between the self-focusing and plasma defocusing of a laser pulse to produce ultrashort radiation as brief as a few optical cycles. This unique source has many properties that make it attractive as a nonlinear optical tool for spectroscopy, such as propagation at high intensities over extended distances, self-shortening, white-light generation, and the formation of an underdense plasma. The plasma channel that constitutes a single filament and whose position in space can be controlled by its input parameters can span meters-long distances, whereas multifilamentation of a laser beam can be sustained up to hundreds of meters in the atmosphere. In this review, we briefly summarize the current understanding and use of laser filaments for spectroscopic investigations of molecules. A theoretical framework of filamentation is presented, along with recent experimental evidence supporting the established understanding of filamentation. Investigations carried out on vibrational and rotational spectroscopy, filament-induced breakdown, fluorescence spectroscopy, and backward lasing are discussed.

  12. Coherence Properties of Individual Femtosecond Pulses of an X-ray Free-Electron Laser

    Energy Technology Data Exchange (ETDEWEB)

    Vartanyants, I.A.; /DESY /Moscow Phys. Eng. Inst.; Singer, A.; Mancuso, A.P.; Yefanov, O.M.; /DESY; Sakdinawat, A.; Liu, Y.; Bang, E.; /UC, Berkeley; Williams, G.J.; /SLAC; Cadenazzi, G.; Abbey, B.; /Melbourne U.; Sinn, H.; /European XFEL, Hamburg; Attwood, D.; /UC, Berkeley; Nugent, K.A.; /Melbourne U.; Weckert, E.; /DESY; Wang, T.; Zhu, D.; Wu, B.; Graves, C.; Scherz, A.; Turner, J.J.; Schlotter, W.F.; /SLAC /LERMA, Ivry /Zurich, ETH /LBL, Berkeley /ANL, APS /Argonne /SLAC /LLNL, Livermore /Latrobe U. /SLAC /SLAC /European XFEL, Hamburg /SLAC /Hamburg U.

    2012-06-06

    Measurements of the spatial and temporal coherence of single, femtosecond x-ray pulses generated by the first hard x-ray free-electron laser, the Linac Coherent Light Source, are presented. Single-shot measurements were performed at 780 eV x-ray photon energy using apertures containing double pinholes in 'diffract-and-destroy' mode. We determined a coherence length of 17 {micro}m in the vertical direction, which is approximately the size of the focused Linac Coherent Light Source beam in the same direction. The analysis of the diffraction patterns produced by the pinholes with the largest separation yields an estimate of the temporal coherence time of 0.55 fs. We find that the total degree of transverse coherence is 56% and that the x-ray pulses are adequately described by two transverse coherent modes in each direction. This leads us to the conclusion that 78% of the total power is contained in the dominant mode.

  13. Coherence and population dynamics of chlorophyll excitations in FCP complex: Two-dimensional spectroscopy study

    Energy Technology Data Exchange (ETDEWEB)

    Butkus, Vytautas; Gelzinis, Andrius; Valkunas, Leonas [Department of Theoretical Physics, Faculty of Physics, Vilnius University, Sauletekio Ave. 9-III, 10222 Vilnius (Lithuania); Center for Physical Sciences and Technology, Savanoriu Ave. 231, 02300 Vilnius (Lithuania); Augulis, Ramūnas [Center for Physical Sciences and Technology, Savanoriu Ave. 231, 02300 Vilnius (Lithuania); Gall, Andrew; Robert, Bruno [Institut de Biologie et Technologies de Saclay, Bât 532, Commissariat à l’Energie Atomique Saclay, 91191 Gif sur Yvette (France); Büchel, Claudia [Institut für Molekulare Biowissenschaften, Universität Frankfurt, Max-von-Laue-Straße 9, Frankfurt (Germany); Zigmantas, Donatas [Department of Chemical Physics, Lund University, P.O. Box 124, 22100 Lund (Sweden); Abramavicius, Darius, E-mail: darius.abramavicius@ff.vu.lt [Department of Theoretical Physics, Faculty of Physics, Vilnius University, Sauletekio Ave. 9-III, 10222 Vilnius (Lithuania)

    2015-06-07

    Energy transfer processes and coherent phenomena in the fucoxanthin–chlorophyll protein complex, which is responsible for the light harvesting function in marine algae diatoms, were investigated at 77 K by using two-dimensional electronic spectroscopy. Experiments performed on femtosecond and picosecond timescales led to separation of spectral dynamics, witnessing evolutions of coherence and population states of the system in the spectral region of Q{sub y} transitions of chlorophylls a and c. Analysis of the coherence dynamics allowed us to identify chlorophyll (Chl) a and fucoxanthin intramolecular vibrations dominating over the first few picoseconds. Closer inspection of the spectral region of the Q{sub y} transition of Chl c revealed previously not identified, mutually non-interacting chlorophyll c states participating in femtosecond or picosecond energy transfer to the Chl a molecules. Consideration of separated coherent and incoherent dynamics allowed us to hypothesize the vibrations-assisted coherent energy transfer between Chl c and Chl a and the overall spatial arrangement of chlorophyll molecules.

  14. Femtosecond transient absorption spectroscopy of silanized silicon quantum dots

    Science.gov (United States)

    Kuntermann, Volker; Cimpean, Carla; Brehm, Georg; Sauer, Guido; Kryschi, Carola; Wiggers, Hartmut

    2008-03-01

    Excitonic properties of colloidal silicon quantum dots (Si qdots) with mean sizes of 4nm were examined using stationary and time-resolved optical spectroscopy. Chemically stable silicon oxide shells were prepared by controlled surface oxidation and silanization of HF-etched Si qdots. The ultrafast relaxation dynamics of photogenerated excitons in Si qdot colloids were studied on the picosecond time scale from 0.3psto2.3ns using femtosecond-resolved transient absorption spectroscopy. The time evolution of the transient absorption spectra of the Si qdots excited with a 150fs pump pulse at 390nm was observed to consist of decays of various absorption transitions of photoexcited electrons in the conduction band which overlap with both the photoluminescence and the photobleaching of the valence band population density. Gaussian deconvolution of the spectroscopic data allowed for disentangling various carrier relaxation processes involving electron-phonon and phonon-phonon scatterings or arising from surface-state trapping. The initial energy and momentum relaxation of hot carriers was observed to take place via scattering by optical phonons within 0.6ps . Exciton capturing by surface states forming shallow traps in the amorphous SiOx shell was found to occur with a time constant of 4ps , whereas deeper traps presumably localized in the Si-SiOx interface gave rise to exciton trapping processes with time constants of 110 and 180ps . Electron transfer from initially populated, higher-lying surface states to the conduction band of Si qdots (>2nm) was observed to take place within 400 or 700fs .

  15. Femtosecond time-resolved studies of coherent vibrational Raman scattering in large gas-phase molecules

    International Nuclear Information System (INIS)

    Hayden, C.C.; Chandler, D.W.

    1995-01-01

    Results are presented from femtosecond time-resolved coherent Raman experiments in which we excite and monitor vibrational coherence in gas-phase samples of benzene and 1,3,5-hexatriene. Different physical mechanisms for coherence decay are seen in these two molecules. In benzene, where the Raman polarizability is largely isotropic, the Q branch of the vibrational Raman spectrum is the primary feature excited. Molecules in different rotational states have different Q-branch transition frequencies due to vibration--rotation interaction. Thus, the macroscopic polarization that is observed in these experiments decays because it has many frequency components from molecules in different rotational states, and these frequency components go out of phase with each other. In 1,3,5-hexatriene, the Raman excitation produces molecules in a coherent superposition of rotational states, through (O, P, R, and S branch) transitions that are strong due to the large anisotropy of the Raman polarizability. The coherent superposition of rotational states corresponds to initially spatially oriented, vibrationally excited, molecules that are freely rotating. The rotation of molecules away from the initial orientation is primarily responsible for the coherence decay in this case. These experiments produce large (∼10% efficiency) Raman shifted signals with modest excitation pulse energies (10 μJ) demonstrating the feasibility of this approach for a variety of gas phase studies. copyright 1995 American Institute of Physics

  16. Clinical coherent anti-Stokes Raman scattering and multiphoton tomography of human skin with a femtosecond laser and photonic crystal fiber

    International Nuclear Information System (INIS)

    Breunig, Hans Georg; Weinigel, Martin; Bückle, Rainer; Kellner-Höfer, Marcel; König, Karsten; Lademann, Jürgen; Darvin, Maxim E; Sterry, Wolfram

    2013-01-01

    We report on in vivo coherent anti-Stokes Raman scattering spectroscopy (CARS), two-photon fluorescence and second-harmonic-generation imaging on human skin with a novel multimodal clinical CARS/multiphoton tomograph. CARS imaging is realized by a combination of femtosecond pulses with broadband continuum pulses generated by a photonic crystal fiber. The images reveal the microscopic distribution of (i) non-fluorescent lipids, (ii) endogenous fluorophores and (iii) the collagen network inside the human skin in vivo with subcellular resolution. Examples of healthy as well as cancer-affected skin are presented. (letter)

  17. Clinical coherent anti-Stokes Raman scattering and multiphoton tomography of human skin with a femtosecond laser and photonic crystal fiber

    Science.gov (United States)

    Breunig, Hans Georg; Weinigel, Martin; Bückle, Rainer; Kellner-Höfer, Marcel; Lademann, Jürgen; Darvin, Maxim E.; Sterry, Wolfram; König, Karsten

    2013-02-01

    We report on in vivo coherent anti-Stokes Raman scattering spectroscopy (CARS), two-photon fluorescence and second-harmonic-generation imaging on human skin with a novel multimodal clinical CARS/multiphoton tomograph. CARS imaging is realized by a combination of femtosecond pulses with broadband continuum pulses generated by a photonic crystal fiber. The images reveal the microscopic distribution of (i) non-fluorescent lipids, (ii) endogenous fluorophores and (iii) the collagen network inside the human skin in vivo with subcellular resolution. Examples of healthy as well as cancer-affected skin are presented.

  18. Femtosecond stimulated Raman spectroscopy by six-wave mixing

    Energy Technology Data Exchange (ETDEWEB)

    Molesky, Brian P.; Guo, Zhenkun; Moran, Andrew M., E-mail: ammoran@email.unc.edu [Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 (United States)

    2015-06-07

    Femtosecond Stimulated Raman Spectroscopy (FSRS) is motivated by the knowledge of the molecular geometry changes that accompany sub-picosecond chemical reactions. The detection of vibrational resonances throughout the entire fingerprint region of the spectrum with sub-100-fs delay precision is fairly straightforward to accomplish with the FSRS technique. Despite its utility, FSRS must contend with substantial technical challenges that stem from a large background of residual laser light and lower-order nonlinearities when all laser pulses are electronically resonant with the equilibrium system. In this work, a geometry based on five incident laser beams is used to eliminate much of this undesired background in experiments conducted on metmyoglobin. Compared to a three-beam FSRS geometry with all electronically resonant laser pulses, the five-beam approach described here offers major improvements in the data acquisition rate, sensitivity, and background suppression. The susceptibility of the five-beam geometry to experimental artifacts is investigated using control experiments and model calculations. Of particular concern are undesired cascades of third-order nonlinearities, which are known to challenge FSRS measurements carried out on electronically off-resonant systems. It is generally understood that “forbidden” steps in the desired nonlinear optical processes are the origin of the problems encountered under off-resonant conditions. In contrast, the present experiments are carried out under electronically resonant conditions, where such unfortunate selection rules do not apply. Nonetheless, control experiments based on spectroscopic line shapes, signal phases, and sample concentrations are conducted to rule out significant contributions from cascades of third-order processes. Theoretical calculations are further used to estimate the relative intensities of the direct and cascaded responses. Overall, the control experiments and model calculations presented in

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

    Energy Technology Data Exchange (ETDEWEB)

    Feist, Armin; Bach, Nora; Rubiano da Silva, Nara; Danz, Thomas; Möller, Marcel; Priebe, Katharina E.; Domröse, Till; Gatzmann, J. Gregor; Rost, Stefan; Schauss, Jakob; Strauch, Stefanie; Bormann, Reiner; Sivis, Murat; Schäfer, Sascha, E-mail: sascha.schaefer@phys.uni-goettingen.de; Ropers, Claus, E-mail: claus.ropers@uni-goettingen.de

    2017-05-15

    We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9 Å focused beam diameter, 200 fs pulse duration and 0.6 eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free-electron beams. - Highlights: • First implementation of an ultrafast TEM employing a nanoscale photocathode. • Localized single photon-photoemission from nanoscopic field emitter yields low emittance ultrashort electron pulses. • Electron pulses focused down to ~9 Å, with a duration of 200 fs and an energy width of 0.6 eV are demonstrated. • Quantitative characterization of ultrafast electron gun emittance and brightness. • A range of applications of high coherence ultrashort electron pulses is shown.

  20. Dual-Comb Coherent Raman Spectroscopy with Lasers of 1-GHz Pulse Repetition Frequency

    OpenAIRE

    Mohler, Kathrin J.; Bohn, Bernhard J.; Yan, Ming; Hänsch, Theodor W.; Picqué, Nathalie

    2016-01-01

    We extend the technique of multiplex coherent Raman spectroscopy with two femtosecond mode-locked lasers to oscillators of a pulse repetition frequency of 1 GHz. We demonstrate spectra of liquids, which span 1100 cm$^{-1}$ of Raman shifts. At a resolution of 6 cm$^{-1}$, their measurement time may be as short as 5 microseconds for a refresh rate of 2 kHz. The waiting period between acquisitions is improved ten-fold compared to previous experiments with two lasers of 100-MHz repetition frequen...

  1. Dual-comb coherent Raman spectroscopy with lasers of 1-GHz pulse repetition frequency.

    Science.gov (United States)

    Mohler, Kathrin J; Bohn, Bernhard J; Yan, Ming; Mélen, Gwénaëlle; Hänsch, Theodor W; Picqué, Nathalie

    2017-01-15

    We extend the technique of multiplex coherent Raman spectroscopy with two femtosecond mode-locked lasers to oscillators of a pulse repetition frequency of 1 GHz. We demonstrate a spectra of liquids, which span 1100  cm-1 of Raman shifts. At a resolution of 6  cm-1, their measurement time may be as short as 5 μs for a refresh rate of 2 kHz. The waiting period between acquisitions is improved 10-fold compared to previous experiments with two lasers of 100-MHz repetition frequencies.

  2. Coherent control of bond making: the performance of rationally phase-shaped femtosecond laser pulses

    International Nuclear Information System (INIS)

    Levin, Liat; Amitay, Zohar; Skomorowski, Wojciech; Koch, Christiane P; Kosloff, Ronnie

    2015-01-01

    The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses (Levin et al 2015 Phys. Rev. Lett. 114 233003). The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses fits very well the vibrational frequency of the generated intermediate wavepacket. These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms. (paper)

  3. Effects of moderate pump and Stokes chirp on chirped-probe pulse femtosecond coherent anti-Stokes Raman scattering thermometry

    KAUST Repository

    Gu, Mingming; Satija, Aman; Lucht, Robert P.

    2018-01-01

    The effects of moderate levels of chirp in the pump and Stokes pulses on chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CPP fs CARS) were investigated. The frequency chirp in the pump and Stokes pulses was introduced

  4. Coherent spectroscopies on ultrashort time and length scales

    Directory of Open Access Journals (Sweden)

    Schneider C.

    2013-03-01

    Full Text Available Three spectroscopic techniques are presented that provide simultaneous spatial and temporal resolution: modified confocal microscopy with heterodyne detection, space-time-resolved spectroscopy using coherent control concepts, and coherent two-dimensional nano-spectroscopy. Latest experimental results are discussed.

  5. Coherent infrared radiation from the ALS generated via femtosecond laser modulation of the electron beam

    International Nuclear Information System (INIS)

    Byrd, J.M.; Hao, Z.; Martin, M.C.; Robin, D.S.; Sannibale, F.; Schoenlein, R.W.; Venturini, M.; Zholents, A.A.; Zolotorev, M.S.

    2004-01-01

    Interaction of an electron beam with a femtosecond laser pulse co-propagating through a wiggler at the ALS produces large modulation of the electron energies within a short ∼100 fs slice of the electron bunch. Propagating around the storage ring, this bunch develops a longitudinal density perturbation due to the dispersion of electron trajectories. The length of the perturbation evolves with a distance from the wiggler but is much shorter than the electron bunch length. This perturbation causes the electron bunch to emit short pulses of temporally and spatially coherent infrared light which are automatically synchronized to the modulating laser. The intensity and spectra of the infrared light were measured in two storage ring locations for a nominal ALS lattice and for an experimental lattice with the higher momentum compaction factor. The onset of instability stimulated by laser e-beam interaction had been discovered. The infrared signal is now routinely used as a sensitive monitor for a fine tuning of the laser beam alignment during data accumulation in the experiments with femtosecond x-ray pulses

  6. Coherent electron - hole state and femtosecond cooperative emission in bulk GaAs

    International Nuclear Information System (INIS)

    Vasil'ev, Petr P; Kan, H; Ohta, H; Hiruma, T

    2002-01-01

    The conditions for obtaining a collective coherent electron - hole state in semiconductors are discussed. The results of the experimental study of the regime of cooperative recombination of high-density electrons and holes (more than 3 x 10 18 cm -3 ) in bulk GaAs at room temperature are presented. It is shown that the collective pairing of electrons and holes and their condensation cause the formation of a short-living coherent electron - hole BCS-like state, which exhibits radiative recombination in the form of high-power femtosecond optical pulses. It is experimentally demonstrated that almost all of the electrons and holes available are condensed at the very bottoms of the bands and are at the cooperative state. The average lifetime of this state is measured to be of about 300 fs. The dependences of the order parameter (the energy gap of the spectrum of electrons and holes) and the Fermi energy of the coherent BCS state on the electron - hole concentration are obtained. (special issue devoted to the 80th anniversary of academician n g basov's birth)

  7. Wave-length-modulated femtosecond stimulated raman spectroscopy-approach towards automatic data processing

    NARCIS (Netherlands)

    Kloz, M.; van Grondelle, R.; Kennis, J.T.M.

    2011-01-01

    A new wavelength modulator based on a custom-made chopper blade and a slit placed in the Fourier plane of a pulse shaper was used to detect explicitly the first derivative of the time-resolved femtosecond stimulated Raman spectroscopy (FSRS) signals. This approach resulted in an unprecedented

  8. Structural Evolution in Photoactive Yellow Protein Studied by Femtosecond Stimulated Raman Spectroscopy

    Directory of Open Access Journals (Sweden)

    Yoshizawa M.

    2013-03-01

    Full Text Available Ultrafast structural evolution in photoactive yellow protein (PYP is studied by femtosecond stimulated Raman spectroscopy. A comparison between wild-type PYP and E46Q mutant reveals that the hydrogen-bonding network surrounding the chromophore of PYP is immediately rearranged in the electronic excited state.

  9. Probing spin-vibronic dynamics using femtosecond X-ray spectroscopy

    DEFF Research Database (Denmark)

    Penfold, T. J.; Pápai, Mátyás Imre; Rozgonyi, T.

    2016-01-01

    Ultrafast pump-probe spectroscopy within the X-ray regime is now possible owing to the development of X-ray Free Electrons Lasers (X-FELs) and is opening new opportunities for the direct probing of femtosecond evolution of the nuclei, the electronic and spin degrees of freedom. In this contributi...

  10. Nonlinear optics in germanium mid-infrared fiber material: Detuning oscillations in femtosecond mid-infrared spectroscopy

    Directory of Open Access Journals (Sweden)

    M. Ordu

    2017-09-01

    Full Text Available Germanium optical fibers hold great promise in extending semiconductor photonics into the fundamentally important mid-infrared region of the electromagnetic spectrum. The demonstration of nonlinear response in fabricated Ge fiber samples is a key step in the development of mid-infrared fiber materials. Here we report the observation of detuning oscillations in a germanium fiber in the mid-infrared region using femtosecond dispersed pump-probe spectroscopy. Detuning oscillations are observed in the frequency-resolved response when mid-infrared pump and probe pulses are overlapped in a fiber segment. The oscillations arise from the nonlinear frequency resolved nonlinear (χ(3 response in the germanium semiconductor. Our work represents the first observation of coherent oscillations in the emerging field of germanium mid-infrared fiber optics.

  11. Construction of coherent antistokes Raman spectroscopy (CARS)

    International Nuclear Information System (INIS)

    Zidan, M. D.; Jazmati, A.

    2007-01-01

    Coherent Antistokes Raman Spectroscopy (CARS) has been built. It consists of a Raman cell, which is filled with CO 2 gas at 5 atm pressure and a frequency doubled Nd-YAG laser pumped dye laser. The two beams are focused by means of a bi-convex lens into Raman cell. The Antistokes signals (CARS signals) are generated due to Four-wave mixing process. The antistokes signals were directed to monochrometer entrance slit by prism . The signals are detected by photomultiplier detector which is fixed on the exit slit and connected to data acquisition card located inside the computed case. The dye laser frequency has to be tuned to satisfy the energy difference between the ν 1 beam (Nd- YAG laser beam) and the ν 2 beam (the stokes beam or the dye laser beam) exactly corresponds to a vibrational - rotational Raman resonance (ν 2 - ν 1 = ν M ) in the 12 CO 2 or 13 CO 2 molecule, then the antistokes signals (ν 3 ) will be generated. The spectra of the CARS signals have been recorded to determine the isotope shift of 12 CO 2 , 13 CO 2 , which is 18.3 cm -1 . (author)

  12. Coherent scatter-controlled phase-change grating structures in silicon using femtosecond laser pulses.

    Science.gov (United States)

    Fuentes-Edfuf, Yasser; Garcia-Lechuga, Mario; Puerto, Daniel; Florian, Camilo; Garcia-Leis, Adianez; Sanchez-Cortes, Santiago; Solis, Javier; Siegel, Jan

    2017-07-04

    Periodic structures of alternating amorphous-crystalline fringes have been fabricated in silicon using repetitive femtosecond laser exposure (800 nm wavelength and 120 fs duration). The method is based on the interference of the incident laser light with far- and near-field scattered light, leading to local melting at the interference maxima, as demonstrated by femtosecond microscopy. Exploiting this strategy, lines of highly regular amorphous fringes can be written. The fringes have been characterized in detail using optical microscopy combined modelling, which enables a determination of the three-dimensional shape of individual fringes. 2D micro-Raman spectroscopy reveals that the space between amorphous fringes remains crystalline. We demonstrate that the fringe period can be tuned over a range of 410 nm - 13 µm by changing the angle of incidence and inverting the beam scan direction. Fine control over the lateral dimensions, thickness, surface depression and optical contrast of the fringes is obtained via adjustment of pulse number, fluence and spot size. Large-area, highly homogeneous gratings composed of amorphous fringes with micrometer width and millimeter length can readily be fabricated. The here presented fabrication technique is expected to have applications in the fields of optics, nanoelectronics, and mechatronics and should be applicable to other materials.

  13. Electron transfer dynamics of triphenylamine dyes bound to TiO2 nanoparticles from femtosecond stimulated Raman spectroscopy

    KAUST Repository

    Hoffman, David P.; Lee, Olivia P.; Millstone, Jill E.; Chen, Mark S.; Su, Timothy A.; Creelman, Mark; Frechet, Jean; Mathies, Richard A.

    2013-01-01

    Interfacial electron transfer between sensitizers and semiconducting nanoparticles is a crucial yet poorly understood process. To address this problem, we have used transient absorption (TA) and femtosecond stimulated Raman spectroscopy (FSRS

  14. Femtosecond spectroscopy on alkali-doped helium nanodroplets; Femtosekundenspektroskopie an alkalidotierten Helium-Nanotroepfchen

    Energy Technology Data Exchange (ETDEWEB)

    Claas, P.

    2006-01-15

    In the present thesis first studies on the short-time dynamics in alkali dimers and microclusters, which were bound on the surface of superfluid helium droplets, were presented. The experiments comprehended pump-probe measurements on the fs scale on the vibration dynamics on the dimers and on the fragmentation dynamics on the clusters. Generally by the studies it was shown that such extremely short slopes can also be observed on helium droplets by means of the femtosecond spectroscopy.

  15. Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser

    DEFF Research Database (Denmark)

    Lemke, Henrik T.; Bressler, Christian; Chen, Lin X.

    2013-01-01

    X-ray free electron lasers (XFELs) deliver short (current (SASE based) XFELs, they can be used for measuring high......-quality X-ray absorption data and we report femtosecond time-resolved X-ray absorption near-edge spectroscopy (XANES) measurements of a spin-crossover system, iron(II) tris(2,2'-bipyridine) in water. The data indicate that the low-spin to high-spin transition can be modeled by single-exponential kinetics...

  16. Femtosecond spectral phase shaping for CARS spectroscopy and imaging

    NARCIS (Netherlands)

    Postma, S.; van Rhijn, A.C.W.; Korterik, Jeroen P.; Herek, Jennifer Lynn; Offerhaus, Herman L.; Corkum, P.; de Silvestri, S.; Nelson, K.A.; Riedle, E.; Schoenlein, R.W.

    2009-01-01

    Coherent Anti-Stokes Raman Scattering (CARS) is a third-order non-linear optical process that provides label-free, chemically selective microscopy by probing the internal vibrational structure of molecules. Due to the resonant enhancement of the CARS process, faster imaging is possible compared to

  17. Femtosecond pulse shaping using the geometric phase.

    Science.gov (United States)

    Gökce, Bilal; Li, Yanming; Escuti, Michael J; Gundogdu, Kenan

    2014-03-15

    We demonstrate a femtosecond pulse shaper that utilizes polarization gratings to manipulate the geometric phase of an optical pulse. This unique approach enables circular polarization-dependent shaping of femtosecond pulses. As a result, it is possible to create coherent pulse pairs with orthogonal polarizations in a 4f pulse shaper setup, something until now that, to our knowledge, was only achieved via much more complex configurations. This approach could be used to greatly simplify and enhance the functionality of multidimensional spectroscopy and coherent control experiments, in which multiple coherent pulses are used to manipulate quantum states in materials of interest.

  18. From Femtosecond Dynamics to Breast Cancer Diagnosis by Raman Spectroscopy

    International Nuclear Information System (INIS)

    Abramczyk, H.; Placek, I.; Brozek-Pluska, B.; Kurczewski, K.; Morawiec, Z.; Tazbir, M.

    2007-01-01

    This paper presents new results based on Raman spectroscopy and demonstrates its utilisation as a diagnostic and development tool with the key advantage in breast cancer research. Applications of Raman spectroscopy in cancer research are in the early stages of development. However, research presented here as well as performed in a few other laboratories demonstrate the ability of Raman spectroscopy to accurately characterize cancer tissue and distinguish between normal, malignant and benign types. The main goals of bio-Raman spectroscopy at this stage are threefold. Firstly, the aim is to develop the diagnostic ability of Raman spectroscopy so it can be implemented in a clinical environment, producing accurate and rapid diagnoses. Secondly, the aim is to optimize the technique as a diagnostic tool for the non-invasive real time medical applications. Thirdly, the aim is to formulate some hypothesis based on Raman spectroscopy on the molecular mechanism which drives the transformation of normal human cells into highly malignant derivatives. To the best of our knowledge, this is the most statistically reliable report on Raman spectroscopy-based diagnosis of breast cancers among the world women population

  19. Femtosecond laser-induced breakdown spectroscopy of sea water

    International Nuclear Information System (INIS)

    Ilyin, Alexey A.; Golik, Sergey S.

    2013-01-01

    The composition of the line and band spectra of the plasma induced by a femtosecond laser pulse on the surface of sea water is determined. The temporal behaviors of the intensity of the continuum and the Ca II, Mg II and Na I lines are investigated. It is shown that the time dependence of the intensity of the Na I line is described by a monoexponential function. The characteristic decay times of the line intensities of Mg II and Na I were used to estimate the three-body recombination times. Using these values, we estimate the electron number density and the feasibility of Local Thermodynamic Equilibrium (LTE) criterion. A method involving excitation rate constants is proposed for the comparison of detection limits. For a plasma generated on a liquid surface, the following relation among detection limits will be obtained: LOD(Na) 2 were recorded. • Recombination determines characteristic decay time of line intensity. • Three-body recombination time was used to estimate electron density. • Excitation rate constants allow to determine relation of detection limits

  20. Femtosecond time-resolved transient absorption spectroscopy of xanthophylls

    Czech Academy of Sciences Publication Activity Database

    Niedzwiedzki, D.; Sullivan, J.O.; Polívka, Tomáš; Birge, R.R.; Frank, H.A.

    2006-01-01

    Roč. 110, č. 45 (2006), s. 22872-22885 ISSN 1520-6106 Institutional research plan: CEZ:AV0Z50510513 Keywords : xanthophyll * spectroscopy study Subject RIV: BO - Biophysics Impact factor: 4.115, year: 2006

  1. Coherent cavity-enhanced dual-comb spectroscopy

    OpenAIRE

    Fleisher, Adam J.; Long, David A.; Reed, Zachary D.; Hodges, Joseph T.; Plusquellic, David F.

    2016-01-01

    Dual-comb spectroscopy allows for the rapid, multiplexed acquisition of high-resolution spectra without the need for moving parts or low-resolution dispersive optics. This method of broadband spectroscopy is most often accomplished via tight phase locking of two mode-locked lasers or via sophisticated signal processing algorithms, and therefore, long integration times of phase coherent signals are difficult to achieve. Here we demonstrate an alternative approach to dual-comb spectroscopy usin...

  2. Femtosecond luminescence spectroscopy of core states in silicon nanocrystals

    Czech Academy of Sciences Publication Activity Database

    Žídek, K.; Trojánek, F.; Malý, P.; Ondič, Lukáš; Pelant, Ivan; Dohnalová, Kateřina; Šiller, L.; Little, R.; Horrocks, B.R.

    2010-01-01

    Roč. 18, č. 24 (2010), s. 25241-25249 ISSN 1094-4087 R&D Projects: GA AV ČR KAN400100701; GA AV ČR(CZ) IAA101120804; GA MŠk LC510 Institutional research plan: CEZ:AV0Z10100521 Keywords : silicon nanocrystals * ultrafast spectroscopy * photoluminescence spectroscopy Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.749, year: 2010 http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-18-24-25241

  3. Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion

    International Nuclear Information System (INIS)

    Glownia, J. M.; Natan, A.; Cryan, J. P.; Hartsock, R.; Kozina, M.

    2016-01-01

    Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with a temporal and spatial resolution of 30 fs and 0.3 Å. This high fidelity is due to interference between the nonstationary excitation and the stationary initial charge distribution. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on ångstrom and femtosecond scales. This x-ray interference has not been employed to image internal motion in molecules before. In conclusion, coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.

  4. Observation of coherent optical phonons excited by femtosecond laser radiation in Sb films by ultrafast electron diffraction method

    Energy Technology Data Exchange (ETDEWEB)

    Mironov, B. N.; Kompanets, V. O.; Aseev, S. A., E-mail: isanfemto@yandex.ru [Russian Academy of Sciences, Institute of Spectroscopy (Russian Federation); Ischenko, A. A. [Moscow Technological University, Institute of High Chemical Technologies (Russian Federation); Kochikov, I. V. [Moscow State University (Russian Federation); Misochko, O. V. [Russian Academy of Sciences, Institute of Solid State Physics (Russian Federation); Chekalin, S. V.; Ryabov, E. A. [Russian Academy of Sciences, Institute of Spectroscopy (Russian Federation)

    2017-03-15

    The generation of coherent optical phonons in a polycrystalline antimony film sample has been investigated using femtosecond electron diffraction method. Phonon vibrations have been induced in the Sb sample by the main harmonic of a femtosecond Ti:Sa laser (λ = 800 nm) and probed by a pulsed ultrashort photoelectron beam synchronized with the pump laser. The diffraction patterns recorded at different times relative to the pump laser pulse display oscillations of electron diffraction intensity corresponding to the frequencies of vibrations of optical phonons: totally symmetric (A{sub 1g}) and twofold degenerate (E{sub g}) phonon modes. The frequencies that correspond to combinations of these phonon modes in the Sb sample have also been experimentally observed.

  5. Spectroscopie résolue en temps par continuum femtoseconde Applications en neurobiologie

    Science.gov (United States)

    Ramstein, S.; Mottin, S.

    2003-06-01

    La spectroscopie résolue en temps utilisant un laser blanc femtoseconde est appliquée à la mesure in vivo des principaux absorbeurs du cerveau. Après génération adéquate du continuum de lumière blanche femtoseconde (50mW/[580-756nm] à 1Hz), cette source se propage dans la calvaria, les méninges et le cortex chez le rat anesthésié. La transmission est étudiée sur 7mm de distance entre l'impact laser et la fibre optique de collection. Le signal transmis est analysé dans la fenêtre 580-760nm, par un spectromètre couplé à une caméra à balayage de fente permettant la décorrélation de l'absorption et de la diffusion.

  6. Black Hole Spectroscopy with Coherent Mode Stacking.

    Science.gov (United States)

    Yang, Huan; Yagi, Kent; Blackman, Jonathan; Lehner, Luis; Paschalidis, Vasileios; Pretorius, Frans; Yunes, Nicolás

    2017-04-21

    The measurement of multiple ringdown modes in gravitational waves from binary black hole mergers will allow for testing the fundamental properties of black holes in general relativity and to constrain modified theories of gravity. To enhance the ability of Advanced LIGO/Virgo to perform such tasks, we propose a coherent mode stacking method to search for a chosen target mode within a collection of multiple merger events. We first rescale each signal so that the target mode in each of them has the same frequency and then sum the waveforms constructively. A crucial element to realize this coherent superposition is to make use of a priori information extracted from the inspiral-merger phase of each event. To illustrate the method, we perform a study with simulated events targeting the ℓ=m=3 ringdown mode of the remnant black holes. We show that this method can significantly boost the signal-to-noise ratio of the collective target mode compared to that of the single loudest event. Using current estimates of merger rates, we show that it is likely that advanced-era detectors can measure this collective ringdown mode with one year of coincident data gathered at design sensitivity.

  7. Ionization and dissociation dynamics of vinyl bromide probed by femtosecond extreme ultraviolet transient absorption spectroscopy

    International Nuclear Information System (INIS)

    Lin, Ming-Fu; Neumark, Daniel M.; Gessner, Oliver; Leone, Stephen R.

    2014-01-01

    Strong-field induced ionization and dissociation dynamics of vinyl bromide, CH 2 =CHBr, are probed using femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy. Strong-field ionization is initiated with an intense femtosecond, near infrared (NIR, 775 nm) laser field. Femtosecond XUV pulses covering the photon energy range of 50-72 eV probe the subsequent dynamics by measuring the time-dependent spectroscopic features associated with transitions of the Br (3d) inner-shell electrons to vacancies in molecular and atomic valence orbitals. Spectral signatures are observed for the depletion of neutral C 2 H 3 Br, the formation of C 2 H 3 Br + ions in their ground (X ~ ) and first excited (A ~ ) states, the production of C 2 H 3 Br ++ ions, and the appearance of neutral Br ( 2 P 3/2 ) atoms by dissociative ionization. The formation of free Br ( 2 P 3/2 ) atoms occurs on a timescale of 330 ± 150 fs. The ionic A ~ state exhibits a time-dependent XUV absorption energy shift of ∼0.4 eV within the time window of the atomic Br formation. The yield of Br atoms correlates with the yield of parent ions in the A ~ state as a function of NIR peak intensity. The observations suggest that a fraction of vibrationally excited C 2 H 3 Br + (A ~ ) ions undergoes intramolecular vibrational energy redistribution followed by the C–Br bond dissociation. The C 2 H 3 Br + (X ~ ) products and the majority of the C 2 H 3 Br ++ ions are relatively stable due to a deeper potential well and a high dissociation barrier, respectively. The results offer powerful new insights about orbital-specific electronic processes in high field ionization, coupled vibrational relaxation and dissociation dynamics, and the correlation of valence hole-state location and dissociation in polyatomic molecules, all probed simultaneously by ultrafast table-top XUV spectroscopy

  8. Adaptive sampling dual terahertz comb spectroscopy using dual free-running femtosecond lasers.

    Science.gov (United States)

    Yasui, Takeshi; Ichikawa, Ryuji; Hsieh, Yi-Da; Hayashi, Kenta; Cahyadi, Harsono; Hindle, Francis; Sakaguchi, Yoshiyuki; Iwata, Tetsuo; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Minoshima, Kaoru; Inaba, Hajime

    2015-06-02

    Terahertz (THz) dual comb spectroscopy (DCS) is a promising method for high-accuracy, high-resolution, broadband THz spectroscopy because the mode-resolved THz comb spectrum includes both broadband THz radiation and narrow-line CW-THz radiation characteristics. In addition, all frequency modes of a THz comb can be phase-locked to a microwave frequency standard, providing excellent traceability. However, the need for stabilization of dual femtosecond lasers has often hindered its wide use. To overcome this limitation, here we have demonstrated adaptive-sampling THz-DCS, allowing the use of free-running femtosecond lasers. To correct the fluctuation of the time and frequency scales caused by the laser timing jitter, an adaptive sampling clock is generated by dual THz-comb-referenced spectrum analysers and is used for a timing clock signal in a data acquisition board. The results not only indicated the successful implementation of THz-DCS with free-running lasers but also showed that this configuration outperforms standard THz-DCS with stabilized lasers due to the slight jitter remained in the stabilized lasers.

  9. Spectroscopy and coherent manipulation of single and coupled flux qubits

    International Nuclear Information System (INIS)

    Wu Yu-Lin; Deng Hui; Huang Ke-Qiang; Tian Ye; Yu Hai-Feng; Xue Guang-Ming; Jin Yi-Rong; Li Jie; Zhao Shi-Ping; Zheng Dong-Ning

    2013-01-01

    Measurements of three-junction flux qubits, both single flux qubits and coupled flux qubits, using a coupled direct current superconducting quantum interference device (dc-SQUID) for readout are reported. The measurement procedure is described in detail. We performed spectroscopy measurements and coherent manipulations of the qubit states on a single flux qubit, demonstrating quantum energy levels and Rabi oscillations, with Rabi oscillation decay time T Rabi = 78 ns and energy relaxation time T 1 = 315 ns. We found that the value of T Rabi depends strongly on the mutual inductance between the qubit and the magnetic coil. We also performed spectroscopy measurements on inductively coupled flux qubits. (general)

  10. Laser spectroscopy

    CERN Document Server

    Demtröder, Wolfgang

    2008-01-01

    Keeping abreast of the latest techniques and applications, this new edition of the standard reference and graduate text on laser spectroscopy has been completely revised and expanded. While the general concept is unchanged, the new edition features a broad array of new material, e.g., frequency doubling in external cavities, reliable cw-parametric oscillators, tunable narrow-band UV sources, more sensitive detection techniques, tunable femtosecond and sub-femtosecond lasers (X-ray region and the attosecond range), control of atomic and molecular excitations, frequency combs able to synchronize independent femtosecond lasers, coherent matter waves, and still more applications in chemical analysis, medical diagnostics, and engineering.

  11. Time resolved infrared spectroscopy of femtosecond proton dynamics in the liquid phase

    International Nuclear Information System (INIS)

    Amir, W.

    2003-12-01

    This work of thesis aims to understand the strong mobility of protons in water. Water is fundamental to life and mediates many chemical and biological processes. However this liquid is poorly understood at the molecular level. The richness of interdisciplinary sciences allows us to study the properties which make it so unique. The technique used for this study was the femtosecond time resolved vibrational spectroscopy. Several experiments were carried out to characterize the femtosecond proton dynamics in water. The visualization of the rotation of water molecules obtained by anisotropy measurements will be presented. This experiment is carried out in isotopic water HDO/D 2 O for reasons of experimental and theoretical suitability. However this is not water. Pure water H 2 O was also studied without thermal effects across vibrations modes. An intermolecular energy resonant transfer was observed. Finally the localized structure of the proton in water (called Eigen form) was clearly experimentally observed. This molecule is implicated in the abnormal mobility of the proton in water (Grotthuss mechanism). (author)

  12. Femtosecond stimulated Raman spectroscopy as a tool to detect molecular vibrations in ground and excited electronic states

    Energy Technology Data Exchange (ETDEWEB)

    Gelin, Maxim F.; Domcke, Wolfgang [Department of Chemistry, Technische Universität München, D-85747 Garching (Germany); Rao, B. Jayachander [Departamento de Química and Centro de Química, Universidade de Coimbra, 3004-535 Coimbra (Portugal)

    2016-05-14

    We give a detailed theoretical analysis of the simplest variant of femtosecond stimulated Raman spectroscopy, where a picosecond Raman pump pulse and a femtosecond Raman probe pulse are applied resonantly to a chromophore in thermal equilibrium in the ground electronic state. We demonstrate that this technique is capable of the detection of dephasing-free Raman-like lines revealing vibrational modes not only in the electronic ground state but also in the excited electronic state of the chromophore. The analytical results obtained with simplifying assumptions for the shape of the laser pulses are substantiated by numerical simulations with realistic laser pulses, employing the equation-of-motion phase-matching approach.

  13. Terahertz Coherent Synchrotron Radiation from Femtosecond Laser Modulation of the Electron Beam at the Advanced Light Source

    CERN Document Server

    Byrd, John; Martin, Michael C; Robin, David; Sannibale, Fernando; Schönlein, Robert W; Zholents, Alexander; Zolotorev, Max S

    2005-01-01

    At the Advanced Light Source (ALS), the "femtoslicing" beamline is in operation since 1999 for the production of x-ray synchrotron radiation pulses with femtosecond duration. The mechanism used for generating the short x-ray pulses induces at the same time temporary structures in the electron bunch longitudinal distribution with very short characteristic length. Such structures emit intense coherent synchrotron radiation (CSR) in the terahertz frequency range. This CSR, whose measured intensity is routinely used as a diagnostics for the tune-up of the femtoslicing experiments, represents a potential source of terahertz radiation with very interesting features. Several measurements have been performed for its characterization and in this paper an updated description of the experimental results and of their interpretation is presented.

  14. Optimization methods of pulse-to-pulse alignment using femtosecond pulse laser based on temporal coherence function for practical distance measurement

    Science.gov (United States)

    Liu, Yang; Yang, Linghui; Guo, Yin; Lin, Jiarui; Cui, Pengfei; Zhu, Jigui

    2018-02-01

    An interferometer technique based on temporal coherence function of femtosecond pulses is demonstrated for practical distance measurement. Here, the pulse-to-pulse alignment is analyzed for large delay distance measurement. Firstly, a temporal coherence function model between two femtosecond pulses is developed in the time domain for the dispersive unbalanced Michelson interferometer. Then, according to this model, the fringes analysis and the envelope extraction process are discussed. Meanwhile, optimization methods of pulse-to-pulse alignment for practical long distance measurement are presented. The order of the curve fitting and the selection of points for envelope extraction are analyzed. Furthermore, an averaging method based on the symmetry of the coherence function is demonstrated. Finally, the performance of the proposed methods is evaluated in the absolute distance measurement of 20 μ m with path length difference of 9 m. The improvement of standard deviation in experimental results shows that these approaches have the potential for practical distance measurement.

  15. Photodissociation and charge transfer dynamics of negative ions studied with femtosecond photoelectron spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Zanni, Martin Thomas [Univ. of California, Berkeley, CA (United States)

    1999-12-01

    This dissertation presents studies aimed at understanding the potential energy surfaces and dynamics of isolated negative ions, and the effects of solvent on each. Although negative ions play important roles in atmospheric and solution phase chemistry, to a large extent the ground and excited state potential energy surfaces of gas phase negative ions are poorly characterized, and solvent effects even less well understood. In an effort to fill this gap, the author's coworkers and the author have developed a new technique, anion femtosecond photoelectron spectroscopy, and applied it to gas phase photodissociation and charge transfer processes. Studies are presented that (1) characterize the ground and excited states of isolated and clustered anions, (2) monitor the photodissociation dynamics of isolated and clustered anions, and (3) explore the charge-transfer-to-solvent states of atomic iodide clustered with polar and non-polar solvents.

  16. Characterization of organic photovoltaic devices using femtosecond laser induced breakdown spectroscopy

    Science.gov (United States)

    Banerjee, S. P.; Sarnet, Thierry; Siozos, Panayiotis; Loulakis, Michalis; Anglos, Demetrios; Sentis, Marc

    2017-10-01

    The potential of laser induced breakdown spectroscopy (LIBS) as a non-contact probe, for characterizing organic photovoltaic devices during selective laser scribing, was investigated. Samples from organic solar cells were studied, which consisted of several layers of materials including a top electrode (Al, Mg or Mo), organic layer, bottom electrode (indium tin oxide), silicon nitride barrier layer and substrate layer situated from the top consecutively. The thickness of individual layers varies from 115 to 250 nm. LIBS measurements were performed by use of a 40 femtosecond Ti:Sapphire laser operated at very low pulse energy (solar cell structure, demonstrating the potential of LIBS for fast, non-contact characterization of organic photovoltaic coatings.

  17. Photodissociation and charge transfer dynamics of negative ions studied with femtosecond photoelectron spectroscopy

    International Nuclear Information System (INIS)

    Zanni, Martin T.

    1999-01-01

    This dissertation presents studies aimed at understanding the potential energy surfaces and dynamics of isolated negative ions, and the effects of solvent on each. Although negative ions play important roles in atmospheric and solution phase chemistry, to a large extent the ground and excited state potential energy surfaces of gas phase negative ions are poorly characterized, and solvent effects even less well understood. In an effort to fill this gap, the author's coworkers and the author have developed a new technique, anion femtosecond photoelectron spectroscopy, and applied it to gas phase photodissociation and charge transfer processes. Studies are presented that (1) characterize the ground and excited states of isolated and clustered anions, (2) monitor the photodissociation dynamics of isolated and clustered anions, and (3) explore the charge-transfer-to-solvent states of atomic iodide clustered with polar and non-polar solvents

  18. Surface-enhanced Raman spectroscopy with Au-nanoparticle substrate fabricated by using femtosecond pulse

    Science.gov (United States)

    Zhang, Wending; Li, Cheng; Gao, Kun; Lu, Fanfan; Liu, Min; Li, Xin; Zhang, Lu; Mao, Dong; Gao, Feng; Huang, Ligang; Mei, Ting; Zhao, Jianlin

    2018-05-01

    Au-nanoparticle (Au-NP) substrates for surface-enhanced Raman spectroscopy (SERS) were fabricated by grid-like scanning a Au-film using a femtosecond pulse. The Au-NPs were directly deposited on the Au-film surface due to the scanning process. The experimentally obtained Au-NPs presented local surface plasmon resonance effect in the visible spectral range, as verified by finite difference time domain simulations and measured reflection spectrum. The SERS experiment using the Au-NP substrates exhibited high activity and excellent substrate reproducibility and stability, and a clearly present Raman spectra of target analytes, e.g. Rhodamine-6G, Rhodamine-B and Malachite green, with concentrations down to 10‑9 M. This work presents an effective approach to producing Au-NP SERS substrates with advantages in activity, reproducibility and stability, which could be used in a wide variety of practical applications for trace amount detection.

  19. Coherent radio-frequency detection for narrowband direct comb spectroscopy.

    Science.gov (United States)

    Anstie, James D; Perrella, Christopher; Light, Philip S; Luiten, Andre N

    2016-02-22

    We demonstrate a scheme for coherent narrowband direct optical frequency comb spectroscopy. An extended cavity diode laser is injection locked to a single mode of an optical frequency comb, frequency shifted, and used as a local oscillator to optically down-mix the interrogating comb on a fast photodetector. The high spectral coherence of the injection lock generates a microwave frequency comb at the output of the photodiode with very narrow features, enabling spectral information to be further down-mixed to RF frequencies, allowing optical transmittance and phase to be obtained using electronics commonly found in the lab. We demonstrate two methods for achieving this step: a serial mode-by-mode approach and a parallel dual-comb approach, with the Cs D1 transition at 894 nm as a test case.

  20. Coherent cavity-enhanced dual-comb spectroscopy.

    Science.gov (United States)

    Fleisher, Adam J; Long, David A; Reed, Zachary D; Hodges, Joseph T; Plusquellic, David F

    2016-05-16

    Dual-comb spectroscopy allows for the rapid, multiplexed acquisition of high-resolution spectra without the need for moving parts or low-resolution dispersive optics. This method of broadband spectroscopy is most often accomplished via tight phase locking of two mode-locked lasers or via sophisticated signal processing algorithms, and therefore, long integration times of phase coherent signals are difficult to achieve. Here we demonstrate an alternative approach to dual-comb spectroscopy using two phase modulator combs originating from a single continuous-wave laser capable of > 2 hours of coherent real-time averaging. The dual combs were generated by driving the phase modulators with step-recovery diodes where each comb consisted of > 250 teeth with 203 MHz spacing and spanned > 50 GHz region in the near-infrared. The step-recovery diodes are passive devices that provide low-phase-noise harmonics for efficient coupling into an enhancement cavity at picowatt optical powers. With this approach, we demonstrate the sensitivity to simultaneously monitor ambient levels of CO2, CO, HDO, and H2O in a single spectral region at a maximum acquisition rate of 150 kHz. Robust, compact, low-cost and widely tunable dual-comb systems could enable a network of distributed multiplexed optical sensors.

  1. Study of the Bulk Charge Carrier Dynamics in Anatase and Rutile TiO2 Single Crystals by Femtosecond Time Resolved Spectroscopy

    KAUST Repository

    Maity, Partha; Mohammed, Omar F.; Katsiev, Khabiboulakh; Idriss, Hicham

    2018-01-01

    as the best model for fundamental studies. Their ultrafast charge carrier dynamics especially on TiO2 anatase single crystal (the most active phase) are unresolved. Here femtosecond time resolved spectroscopy (TRS) was carried out to explore the dynamics

  2. Doping-controlled Coherent Electron-Phonon Coupling in Vanadium Dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Appavoo, Kannatassen [Vanderbilt Univ., Nashville, TN (United States) Interdisciplinary Materials Science; Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Wang, Bin [Vanderbilt Univ., Nashville, TN (United States) Dept. of Physics and Astronomy; Nag, Joyeeta [Vanderbilt Univ., Nashville, TN (United States) Dept. of Physics and Astronomy; Sfeir, Matthew Y. [Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials; Pantelides, Sokrates T. [Vanderbilt Univ., Nashville, TN (United States) Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Vanderbilt Univ., Nashville, TN (United States). Dept. of Electrical Engineering and Computer Science; Haglund, Richard F. [Vanderbilt Univ., Nashville, TN (United States) Interdisciplinary Materials Science and Dept. of Physics and Astronomy

    2015-05-10

    Broadband femtosecond transient spectroscopy and density functional calculations reveal that substitutional tungsten doping of a VO2 film changes the coherent phonon response compared to the undoped film due to altered electronic and structural dynamics.

  3. XIX International Youth School on Coherent Optics and Optical Spectroscopy

    International Nuclear Information System (INIS)

    2016-01-01

    The XIX International Youth School on Coherent Optics and Optical Spectroscopy (COOS2015) was held in Kazan, Russia, from October 5 to October 7 at the Nikolai Lobachevsky Scientific Library of Kazan Federal University. The School follows the global tendency toward comprehensive studies of matter properties and its interaction with electromagnetic fields. Since 1997 more than 100 famous scientists from USA, Germany, Ukraine, Belarussia and Russia had plenary lecture presentations. This is the right place, where over 1000 young scientists had an opportunity to participate in hot discussions regarding the latest scientific news. Many young people have submitted interesting reports on photonics, quantum electronics, laser physics, quantum optics, traditional optical and laser spectroscopy, non-linear optics, material science and nanotechnology. Here we are publishing the full-size papers prepared from the most interesting lectures and reports selected by the Program Committee of the School. (paper)

  4. Femtosecond time-resolved vibrational SFG spectroscopy of CO/Ru( 0 0 1 )

    Science.gov (United States)

    Hess, Ch.; Wolf, M.; Roke, S.; Bonn, M.

    2002-04-01

    Vibrational sum-frequency generation (SFG) employing femtosecond infrared (IR) laser pulses is used to study the dynamics of the C-O stretch vibration on Ru(0 0 1). Time-resolved measurements of the free induction decay (FID) of the IR-polarization for 0.33 ML CO/Ru(0 0 1) exhibit single exponential decays over three decades corresponding to dephasing times of T2=1.94 ps at 95 K and T2=1.16 ps at 340 K. This is consistent with pure homogeneous broadening due to anharmonic coupling with the thermally activated low-frequency dephasing mode together with a contribution from saturation of the IR transition. In pump-probe SFG experiments using a strong visible (VIS) pump pulse the perturbation of the FID leads to transient line shifts even at negative delay times, i.e. when the IR-VIS SFG probe pair precedes the pump pulse. Based on an analysis of the time-dependent polarization we discuss the influence of the perturbed FID on time-resolved SFG spectra. We investigate how coherent effects affect the SFG spectra and we examine the time resolution in these experiments, in particular in dependence of the dephasing time.

  5. Coherent photoluminescence excitation spectroscopy of semicrystalline polymeric semiconductors

    Science.gov (United States)

    Silva, Carlos; Grégoire, Pascal; Thouin, Félix

    In polymeric semiconductors, the competition between through-bond (intrachain) and through-space (interchain) electronic coupling determines two-dimensional spatial coherence of excitons. The balance of intra- and interchain excitonic coupling depends very sensitively on solid-state microstructure of the polymer film (polycrystalline, semicrystalline with amorphous domains, etc.). Regioregular poly(3-hexylthiophene) has emerged as a model material because its photoluminescence (PL) spectral lineshape reveals intricate information on the magnitude of excitonic coupling, the extent of energetic disorder, and on the extent to which the disordered energy landscape is correlated. I discuss implementation of coherent two-dimensional electronic spectroscopy. We identify cross peaks between 0-0 and 0-1 excitation peaks, and we measure their time evolution, which we interpret within the context of a hybrid HJ aggregate model. By measurement of the homogeneous linewidth in diverse polymer microstructures, we address the nature of optical transitions within such hynbrid aggregate model. These depend strongly on sample processing, and I discuss the relationship between microstructure, steady-state absorption and PL spectral lineshape, and 2D coherent PL excitation spectral lineshapes.

  6. Dynamic cerebral autoregulation measured with coherent hemodynamics spectroscopy (CHS)

    Science.gov (United States)

    Kainerstorfer, Jana M.; Sassaroli, Angelo; Tgavalekos, Kristen T.; Fantini, Sergio

    2015-03-01

    Coherent Hemodynamics Spectroscopy (CHS) is a novel technique for non-invasive measurements of local microcirculation quantities such as the capillary blood transit times and dynamic autoregulation. The basis of CHS is to measure, for instance with near-infrared spectroscopy (NIRS), peripheral coherent hemodynamic changes that are induced by controlled perturbations in the systemic mean arterial pressure (MAP). In this study, the MAP perturbation was induced by the fast release of two pneumatic cuffs placed around the subject's thighs after they were kept inflated (at 200 mmHg) for two minutes. The resulting transient changes in cerebral oxy- (O) and deoxy- (D) hemoglobin concentrations measured with NIRS on the prefrontal cortex are then described by a novel hemodynamic model, from which quantifiable parameters such as the capillary blood transit time and a cutoff frequency for cerebral autoregulation are obtained. We present results on eleven healthy volunteers in a protocol involving measurements during normal breathing and during hyperventilation, which is known to cause a hypocapnia-induced increase in cerebral autoregulation. The measured capillary transit time was unaffected by hyperventilation (normal breathing: 1.1±0.1 s; hyperventilation: 1.1±0.1 s), whereas the cutoff frequency of autoregulation, which increases for higher autoregulation efficiency, was indeed found to be significantly greater during hyperventilation (normal breathing: 0.017±0.002 Hz; hyperventilation: 0.034±0.005 Hz). These results provide a validation of local cerebral autoregulation measurements with the new technique of CHS.

  7. Femtosecond Pump-Push-Probe and Pump-Dump-Probe Spectroscopy of Conjugated Polymers: New Insight and Opportunities.

    Science.gov (United States)

    Kee, Tak W

    2014-09-18

    Conjugated polymers are an important class of soft materials that exhibit a wide range of applications. The excited states of conjugated polymers, often referred to as excitons, can either deactivate to yield the ground state or dissociate in the presence of an electron acceptor to form charge carriers. These interesting properties give rise to their luminescence and the photovoltaic effect. Femtosecond spectroscopy is a crucial tool for studying conjugated polymers. Recently, more elaborate experimental configurations utilizing three optical pulses, namely, pump-push-probe and pump-dump-probe, have been employed to investigate the properties of excitons and charge-transfer states of conjugated polymers. These studies have revealed new insight into femtosecond torsional relaxation and detrapping of bound charge pairs of conjugated polymers. This Perspective highlights (1) the recent achievements by several research groups in using pump-push-probe and pump-dump-probe spectroscopy to study conjugated polymers and (2) future opportunities and potential challenges of these techniques.

  8. Analysis of copper contamination in transformer insulating material with nanosecond- and femtosecond-laser-induced breakdown spectroscopy

    Science.gov (United States)

    Aparna, N.; Vasa, N. J.; Sarathi, R.

    2018-06-01

    This work examines the oil-impregnated pressboard insulation of high-voltage power transformers, for the determination of copper contamination. Nanosecond- and femtosecond-laser-induced breakdown spectroscopy revealed atomic copper lines and molecular copper monoxide bands due to copper sulphide diffusion. X-ray diffraction studies also indicated the presence of CuO emission. Elemental and molecular mapping compared transformer insulating material ageing in different media—air, N2, He and vacuum.

  9. Ultra-short laser pulse ablation using shear-force feedback: Femtosecond laser induced breakdown spectroscopy feasibility study

    International Nuclear Information System (INIS)

    Samek, Ota; Kurowski, Andre; Kittel, Silke; Kukhlevsky, Sergei; Hergenroeder, Roland

    2005-01-01

    This work reports on a feasibility study of proximity ablation using femtosecond pulses. Ultra-short pulses were launched to a bare tapered optical fiber and delivered to the sample. The tip-sample distance was controlled by means of shear-force feedback. Consequently, ablation craters with submicrometer dimensions were obtained. Potential analytical applications for Laser Induced Breakdown Spectroscopy (LIBS) technique, such as e.g. inclusions in steel or bio cells, are suggested

  10. Structural dynamics of a noncovalent charge transfer complex from femtosecond stimulated Raman spectroscopy.

    Science.gov (United States)

    Fujisawa, Tomotsumi; Creelman, Mark; Mathies, Richard A

    2012-09-06

    Femtosecond stimulated Raman spectroscopy is used to examine the structural dynamics of photoinduced charge transfer within a noncovalent electron acceptor/donor complex of pyromellitic dianhydride (PMDA, electron acceptor) and hexamethylbenzene (HMB, electron donor) in ethylacetate and acetonitrile. The evolution of the vibrational spectrum reveals the ultrafast structural changes that occur during the charge separation (Franck-Condon excited state complex → contact ion pair) and the subsequent charge recombination (contact ion pair → ground state complex). The Franck-Condon excited state is shown to have significant charge-separated character because its vibrational spectrum is similar to that of the ion pair. The charge separation rate (2.5 ps in ethylacetate and ∼0.5 ps in acetonitrile) is comparable to solvation dynamics and is unaffected by the perdeuteration of HMB, supporting the dominant role of solvent rearrangement in charge separation. On the other hand, the charge recombination slows by a factor of ∼1.4 when using perdeuterated HMB, indicating that methyl hydrogen motions of HMB mediate the charge recombination process. Resonance Raman enhancement of the HMB vibrations in the complex reveals that the ring stretches of HMB, and especially the C-CH(3) deformations are the primary acceptor modes promoting charge recombination.

  11. Surface State Dynamics of Topological Insulators Investigated by Femtosecond Time- and Angle-Resolved Photoemission Spectroscopy

    Directory of Open Access Journals (Sweden)

    Hamoon Hedayat

    2018-04-01

    Full Text Available Topological insulators (TI are known for striking quantum phenomena associated with their spin-polarized topological surface state (TSS. The latter in particular forms a Dirac cone that bridges the energy gap between valence and conduction bands, providing a unique opportunity for prospective device applications. In TI of the BixSb2−xTeySe3−y (BSTS family, stoichiometry determines the morphology and position of the Dirac cone with respect to the Fermi level. In order to engineer specific transport properties, a careful tuning of the TSS is highly desired. Therefore, we have systematically explored BSTS samples with different stoichiometries by time- and angle-resolved photoemission spectroscopy (TARPES. This technique provides snapshots of the electronic structure and discloses the carrier dynamics in surface and bulk states, providing crucial information for the design of electro-spin current devices. Our results reveal the central role of doping level on the Dirac cone structure and its femtosecond dynamics. In particular, an extraordinarily long TSS lifetime is observed when the the vertex of the Dirac cone lies at the Fermi level.

  12. Sum-Frequency-Generation-Based Laser Sidebands for Tunable Femtosecond Raman Spectroscopy in the Ultraviolet

    Directory of Open Access Journals (Sweden)

    Liangdong Zhu

    2015-04-01

    Full Text Available Femtosecond stimulated Raman spectroscopy (FSRS is an emerging molecular structural dynamics technique for functional materials characterization typically in the visible to near-IR range. To expand its applications we have developed a versatile FSRS setup in the ultraviolet region. We use the combination of a narrowband, ~400 nm Raman pump from a home-built second harmonic bandwidth compressor and a tunable broadband probe pulse from sum-frequency-generation-based cascaded four-wave mixing (SFG-CFWM laser sidebands in a thin BBO crystal. The ground state Raman spectrum of a laser dye Quinolon 390 in methanol that strongly absorbs at ~355 nm is systematically studied as a standard sample to provide previously unavailable spectroscopic characterization in the vibrational domain. Both the Stokes and anti-Stokes Raman spectra can be collected by selecting different orders of SFG-CFWM sidebands as the probe pulse. The stimulated Raman gain with the 402 nm Raman pump is >21 times larger than that with the 550 nm Raman pump when measured at the 1317 cm−1 peak for the aromatic ring deformation and ring-H rocking mode of the dye molecule, demonstrating that pre-resonance enhancement is effectively achieved in the unique UV-FSRS setup. This added tunability in the versatile and compact optical setup enables FSRS to better capture transient conformational snapshots of photosensitive molecules that absorb in the UV range.

  13. Femtosecond induced transparency and absorption in the extreme ultraviolet by coherent coupling of the He 2s2p (1Po) and 2p2 (1Se) double excitation states with 800 nm light

    International Nuclear Information System (INIS)

    Loh, Z.-H.; Greene, C.H.; Leone, S.R.

    2007-01-01

    Femtosecond high-order harmonic transient absorption spectroscopy is used to observe electromagnetically induced transparency-like behavior as well as induced absorption in the extreme ultraviolet by laser dressing of the He 2s2p ( 1 P 0 ) and 2p 2 ( 1 S e ) double excitation states with an intense 800 nm field. Probing in the vicinity of the 1s 2 → 2s2p transition at 60.15 eV reveals the formation of an Autler-Townes doublet due to coherent coupling of the double excitation states. Qualitative agreement with the experimental spectra is obtained only when optical field ionization of both double excitation states into the N = 2 continuum is included in the theoretical model. Because the Fano q-parameter of the unperturbed probe transition is finite, the laser-dressed He atom exhibits both enhanced transparency and absorption at negative and positive probe energy detunings, respectively

  14. Effects of moderate pump and Stokes chirp on chirped-probe pulse femtosecond coherent anti-Stokes Raman scattering thermometry

    KAUST Repository

    Gu, Mingming

    2018-01-08

    The effects of moderate levels of chirp in the pump and Stokes pulses on chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CPP fs CARS) were investigated. The frequency chirp in the pump and Stokes pulses was introduced by placing SF11 glass disks with thicknesses of 10 mm or 20 mm in the optical path for these beams. The magnitude of the chirp in the probe beam was much greater and was induced by placing a 30-cm rod of SF10 glass in the beam path. The temperature measurements were performed in hydrogen/air non-premixed flames stabilized on a Hencken burner at equivalence ratios of 0.3, 0.5, 0.7, and 1.0. We performed measurements with no disks in pump and Stokes beam paths, and then with disks of 10 mm and 20 mm placed in both beam paths. The spectrum of the nonresonant background four-wave mixing signal narrowed considerably with increasing pump and Stokes chirp, while the resonant CARS signal was relatively unaffected. Consequently, the interference of the nonresonant background with the resonant CARS signal in the frequency-spread dephasing region of the spectrum was minimized. The increased rate of decay of the resonant CARS signal with increasing temperature was thus readily apparent. We have started to analyze the CPP fs CARS thermometry data and initial results indicate improved accuracy and precision are obtained due to moderate chirp in the pump and Stokes laser pulses.

  15. Terahertz Coherent Synchrotron Radiation from Femtosecond Laser Modulation of the Electron Beam at the Advanced Light Source

    International Nuclear Information System (INIS)

    Byrd, John M.; Hao, Zhao; Martin, Michael C.; Robin, David S.; Sannibale, Fernando; Schoenlein, Robert W.; Zholents, Alexander A.; Zolotorev, Max S.

    2005-01-01

    At the Advanced Light Source (ALS), the ''femtoslicing'' beamline is in operation since 1999 for the production of x-ray synchrotron radiation pulses with femtosecond duration. The mechanism used for generating the short x-ray pulses induces at the same time temporary structures in the electron bunch longitudinal distribution with very short characteristic length. Such structures emit intense coherent synchrotron radiation (CSR) in the terahertz frequency range. These CSR pulses were first observed at the ALS, and the measurement of their intensity is now routinely used as a diagnostics for the tune-up of the femtoslicing x-ray experiments. At the same time, these CSR pulses synchronous with the modulating laser, represent a potential source of terahertz radiation with very interesting features. Several measurements have been performed for their characterization and in this paper we present an updated description of the experimental results and of their interpretation. In particular, we include more data on the interesting interaction, previously observed at the ALS, between the slicing and the microbunching instability (MBI), where under particular circumstances, the slicing seems to trigger the onset of the instability

  16. Toward Femtosecond X-ray Spectroscopy at the Advanced Light Source

    International Nuclear Information System (INIS)

    Chong, Henry Herng Wei

    2004-01-01

    The realization of tunable, ultrashort pulse x-ray sources promises to open new venues of science and to shed new light on long-standing problems in condensed matter physics and chemistry. Fundamentally new information can now be accessed. Used in a pump-probe spectroscopy, ultrashort x-ray pulses provide a means to monitor atomic rearrangement and changes in electronic structure in condensed-matter and chemical systems on the physically-limiting time-scales of atomic motion. This opens the way for the study of fast structural dynamics and the role they play in phase transitions, chemical reactions and the emergence of exotic properties in materials with strongly interacting degrees of freedom. The ultrashort pulse x-ray source developed at the Advanced Light Source at the Lawrence Berkeley Laboratory is based on electron slicing in storage rings, and generates ∼100 femtosecond pulses of synchrotron radiation spanning wavelengths from the far-infrared to the hard x-ray region of the electromagnetic spectrum. The tunability of the source allows for the adaptation of a broad range of static x-ray spectroscopies to useful pump-probe measurements. Initial experiments are attempted on transition metal complexes that exhibit relatively large structural changes upon photo-excitation and which have excited-state evolution determined by strongly interacting structural, electronic and magnetic degrees of freedom. Specifically, iron(II) complexes undergo a spin-crossover transition upon optical irradiation. The dynamics of the transition involve a metal-to-ligand charge transfer, a ΔS = 2 change in magnetic moment and 10% bond dilation in the first coordination shell of the iron. Studies of the electronic dynamics are studied with time-resolved optical absorption measurements. The current progress of time-resolved structural studies to complete the picture of the spin-crossover transition is presented

  17. Temporal dependence of the enhancement of material removal in femtosecond-nanosecond dual-pulse laser-induced breakdown spectroscopy

    International Nuclear Information System (INIS)

    Scaffidi, Jon; Pearman, William; Carter, J. Chance; Colston, Bill W. Jr.; Angel, S. Michael

    2004-01-01

    Despite the large neutral atomic and ionic emission enhancements that have been noted in collinear and orthogonal dual-pulse laser-induced breakdown spectroscopy, the source or sources of these significant signal and signal-to-noise ratio improvements have yet to be explained. In the research reported herein, the combination of a femtosecond preablative air spark and a nanosecond ablative pulse yields eightfold and tenfold material removal improvement for brass and aluminum, respectively, but neutral atomic emission is enhanced by only a factor of 3-4. Additionally, temporal correlation between enhancement of material removal and of atomic emission is quite poor, suggesting that the atomic-emission enhancements noted in the femtosecond-nanosecond pulse configuration result in large part from some source other than simple improvement in material removal

  18. Femtosecond pump probe spectroscopy for the study of energy transfer of light-harvesting complexes from extractions of spinach leaves

    Directory of Open Access Journals (Sweden)

    L. van Rensburg

    2010-01-01

    Full Text Available Measurements of ultrafast transient processes, of temporal durations in the picosecond and femtosecond regime, are made possible by femtosecond pump probe transient absorption spectroscopy. Such an ultrafast pump probe transient absorption setup has been implemented at the CSIR National Laser Centre and has been applied to investigate energy transfer processes in different parts of photosynthetic systems. In this paper we report on our first results obtained with Malachite green as a benchmark. Malachite green was chosen because the lifetime of its excited state is well known. We also present experimental results of the ultrafast energy transfer of light-harvesting complexes in samples prepared from spinach leaves. Various pump wavelengths in the range 600–680 nm were used; the probe was a white light continuum spanning 420–700 nm. The experimental setup is described in detail in this paper. Results obtained with these samples are consistent with those expected and achieved by other researchers in this field.

  19. Femtosecond spectroscopy of bacterial photosynthesis--towards an understanding of the most important energy conversion process on earth

    International Nuclear Information System (INIS)

    Zinth, W.; Hamm, P.; Arlt, T.; Wachtveitl, J.

    1996-01-01

    Reaction centers of bacterial photosynthesis are ideal systems to study photosynthetic energy conversion. Femtosecond spectroscopy has delivered extensive information on the molecular mechanisms of the primary electron transfer. The data show, that primary electron transfer is an ultrafast stepwise reaction, where the electron is transferred via closely spaced pigments with reaction times as fast as 0.9 ps and 3.5 ps. Experiments on mutated and modified reaction centers allow to determine the energetics of the various intermediates in the reaction center. Recently, femtosecond experiments with light pulses in the mid infrared have shown, that an additional fast process occurs on the 200 fs timescale in the initially excited special pair. Only afterwards the well established electron transfer reactions take place. This fast process may be of importance for the optimization of the primary reaction

  20. 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.

  1. Comparative study of femtosecond and nanosecond laser-induced breakdown spectroscopy of depleted uranium

    International Nuclear Information System (INIS)

    Emmert, Luke A.; Chinni, Rosemarie C.; Cremers, David A.; Jones, C. Randy; Rudolph, Wolfgang

    2011-01-01

    We present spectra of depleted uranium metal from laser plasmas generated by nanosecond Nd:YAG (1064 nm) and femtosecond Ti:sapphire (800 nm) laser pulses. The latter pulses produce short-lived and relatively cool plasmas in comparison to the longer pulses, and the spectra of neutral uranium atoms appear immediately after excitation. Evidence for nonequilibrium excitation with femtosecond pulses is found in the dependence of spectral line intensities on the pulse chirp.

  2. Chromophore dynamics in the PYP photocycle from femtosecond stimulated Raman spectroscopy.

    Science.gov (United States)

    Creelman, Mark; Kumauchi, Masato; Hoff, Wouter D; Mathies, Richard A

    2014-01-23

    Femtosecond stimulated Raman spectroscopy (FSRS) is used to examine the structural dynamics of the para-hydroxycinnamic acid (HCA) chromophore during the first 300 ps of the photoactive yellow protein (PYP) photocycle, as the system transitions from its vertically excited state to the early ground state cis intermediate, I0. A downshift in both the C7═C8 and C1═O stretches upon photoexcitation reveals that the chromophore has shifted to an increasingly quinonic form in the excited state, indicating a charge shift from the phenolate moiety toward the C9═O carbonyl, which continues to increase for 170 fs. In addition, there is a downshift in the C9═O carbonyl out-of-plane vibration on an 800 fs time scale as PYP transitions from its excited state to I0, indicating that weakening of the hydrogen bond with Cys69 and out-of-plane rotation of the C9═O carbonyl are key steps leading to photoproduct formation. HOOP intensity increases on a 3 ps time scale during the formation of I0, signifying distortion about the C7═C8 bond. Once on the I0 surface, the C7═C8 and C1═O stretches blue shift, indicating recovery of charge to the phenolate, while persistent intensity in the HOOP and carbonyl out-of-plane modes reveal HCA to be a cissoid structure with significant distortion about the C7═C8 bond and of C9═O out of the molecular plane.

  3. Optical Biopsy Using Tissue Spectroscopy and Optical Coherence Tomography

    Directory of Open Access Journals (Sweden)

    Norman S Nishioka

    2003-01-01

    Full Text Available ‘Optical biopsy’ or ‘optical diagnostics’ is a technique whereby light energy is used to obtain information about the structure and function of tissues without disrupting them. In fluorescence spectroscopy, light energy (usually provided by a laser is used to excite tissues and the resulting fluorescence provides information about the target tissue. Its major gastrointestinal application has been in the evaluation of colonic polyps, in which it can reliably distinguish malignant from benign lesions. Optical coherence tomography (OCT has been used in the investigation of Barrett’s epithelium (and dysplasia, although a variety of other applications are feasible. For example, OCT could assist in the identification and staging of mucosal and submucosal neoplasms, the grading of inflammation in the stomach and intestine, the diagnosis of biliary tumours and the assessment of villous architecture. OCT differs from endoscopic ultrasound, a complementary modality, in that it has a much higher resolution but lesser depth of penetration. The images correlate with the histopathological appearance of tissues, and the addition of Doppler methods may enable it to evaluate the vascularity of tumours and the amount of blood flow in varices. Refinements in these new optical techniques will likely make them valuable in clinical practice, although their specific roles have yet to be determined.

  4. Femtosecond photoelectron spectroscopy: a new tool for the study of anion dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Greenblatt, Benjamin J. [Univ. of California, Berkeley, CA (United States)

    1999-02-01

    A new experimental technique for the time-resolved study of anion reactions is presented. Using femtosecond laser pulses, which provide extremely fast (~100 fs) time resolution, in conjunction with photoelectron spectroscopy, which reveals differences between anion and neutral potential energy surfaces, a complex anion reaction can be followed from its inception through the formation of asymptotic products. Experimental data can be modeled quantitatively using established theoretical approaches, allowing for the refinement of potential energy surfaces as well as dynamical models. After a brief overview, a detailed account of the construction of the experimental apparatus is presented. Documentation of the data acquisition program is contained in the Appendix. The first experimental demonstration of the technique is then presented for I2- photodissociation, modeled using a simulation program which is also detailed in the Appendix. The investigation of I2- photodissociation in several size-selected I2-(Ar)n (n = 6-20) and I2-(CO2)n (n = 4-16) clusters forms the heart of the dissertation. In a series of chapters, the numerous effects of solvation on this fundamental bond-breaking reaction are explored, the most notable of which is the recombination of I2- on the ground $\\tilde{X}$(2Σu+) state in sufficiently large clusters. Recombination and trapping of I2- on the excited $\\tilde{A}$(2π3/2,g) state is also observed in both types of clusters. The studies have revealed electronic state transitions, the first step in recombination, on a ~500 fs to ~10 ps timescale. Accompanying the changes in electronic state is solvent reorganization, which occurs on a similar timescale. Over longer periods (~1 ps to >200 ps), energy is transferred from vibrationally

  5. 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

  6. Femtosecond fluorescence upconversion spectroscopy of vapor-deposited tris(8-hydroxyquinoline) aluminum films.

    NARCIS (Netherlands)

    Humbs, W.; Zhang, H.; Glasbeek, M.

    2000-01-01

    Abstract Vapor-deposited Alq3 is used as the green emitting layer in a class of organic light-emitting diodes. In this paper, the time dependence of the fluorescence from thin Alq3 films has been studied by means of the femtosecond fluorescence upconversion technique. From the temporally resolved

  7. Selective interaction between Xanthophylls and Chlorophylls in LHCII probed by femtosecond transient absoprtion spectroscopy

    NARCIS (Netherlands)

    Gradinaru, C.C.; Grondelle, van R.; Amerongen, van H.

    2003-01-01

    We have performed femtosecond transient absorption measurements on trimeric light-harvesting complex II from spinach. Either chlorophyll (Chl) a (675 nm) or Chl b (650 nm) was excited, and the spectral response was probed for wavelengths longer than 470 nm. Excitation of Chl b led to instantaneous

  8. Conductivity peak, relaxation dynamics, and superconducting gap of YBa2Cu3O7 studied by terahertz and femtosecond optical spectroscopies

    International Nuclear Information System (INIS)

    Frenkel, A.; Gao, F.; Liu, Y.; Whitaker, J.F.; Uher, C.; Hou, S.Y.; Phillips, J.M.

    1996-01-01

    Recent measurements at microwave, terahertz (THz), and infrared frequencies have revealed a peak in σ 1 below T c . Based on our THz measurements, which were performed on high quality, single crystal films of YBCO (900 and 500 A), we have found that σ 1 features a peak which increases in amplitude and shifts to lower temperatures as frequency changes from 1.2 to 0.4 THz. Although the quasiparticle relaxation time extracted from these results using the two-fluid Drude model exhibits an enhancement below T c , the analysis may not be adequate to account for the strong frequency dependence of the conductivity peak by the competition between the drop in scattering rate and the decreasing normal fluid density with temperature. On the contrary, we were able to account for the frequency dependent σ 1 by fitting with Mattis-Bardeen theory (modified to include scattering) using a slower average rate of increase of the anisotropic gap than for the BCS case as temperature decreases below T c . This is consistent with the higher normal fluid density (higher than Gorter-Casimir values) from the two-fluid model interpretation of our THz results. Thus, we have found evidence of BCS coherence factors in a high-T c superconductor with a slower than BCS gap increase below T c . We have discussed the role of coherence factors to account for the presence of the conductivity peak and the absence of the peak in NMR relaxation rate. Furthermore, we have presented a model for the quasiparticle relaxation time measured by the femtosecond pump-probe spectroscopy. This model allowed us to find a fit to the temperature-dependent energy gap function which is also consistent with the slower gap increase below T c

  9. Selective Coherent Excitation of Charged Density Waves

    NARCIS (Netherlands)

    Tsvetkov, A.A.; Sagar, D.M.; Loosdrecht, P.H.M. van; Marel, D. van der

    2003-01-01

    Real time femtosecond pump-probe spectroscopy is used to study collective and single particle excitations in the charge density wave state of the quasi-1D metal, blue bronze. Along with the previously observed collective amplitudon excitation, the spectra show several additional coherent features.

  10. Time resolved infrared spectroscopy of femtosecond proton dynamics in the liquid phase; Spectroscopie infrarouge resolue en temps pour l'etude de la dynamique femtoseconde du proton en phase liquide

    Energy Technology Data Exchange (ETDEWEB)

    Amir, W

    2003-12-15

    This work of thesis aims to understand the strong mobility of protons in water. Water is fundamental to life and mediates many chemical and biological processes. However this liquid is poorly understood at the molecular level. The richness of interdisciplinary sciences allows us to study the properties which make it so unique. The technique used for this study was the femtosecond time resolved vibrational spectroscopy. Several experiments were carried out to characterize the femtosecond proton dynamics in water. The visualization of the rotation of water molecules obtained by anisotropy measurements will be presented. This experiment is carried out in isotopic water HDO/D{sub 2}O for reasons of experimental and theoretical suitability. However this is not water. Pure water H{sub 2}O was also studied without thermal effects across vibrations modes. An intermolecular energy resonant transfer was observed. Finally the localized structure of the proton in water (called Eigen form) was clearly experimentally observed. This molecule is implicated in the abnormal mobility of the proton in water (Grotthuss mechanism). (author)

  11. Laser spectroscopy

    CERN Document Server

    Demtröder, Wolfgang

    Keeping abreast of the latest techniques and applications, this new edition of the standard reference and graduate text on laser spectroscopy has been completely revised and expanded. While the general concept is unchanged, the new edition features a broad array of new material, e.g., ultrafast lasers (atto- and femto-second lasers) and parametric oscillators, coherent matter waves, Doppler-free Fourier spectroscopy with optical frequency combs, interference spectroscopy, quantum optics, the interferometric detection of gravitational waves and still more applications in chemical analysis, medical diagnostics, and engineering.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-04-21

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

  13. Coherent atomic and molecular spectroscopy in the far infrared

    International Nuclear Information System (INIS)

    Inguscio, M.

    1988-01-01

    Recent advances in far infrared spectroscopy of atoms (fine structure transitions) and molecules (rotational transitions) are reviewed. Results obtained by means of Laser Magnetic Resonance, using fixed frequency lasers, and Tunable Far Infrared spectrometers are illustrated. The importance of far infrared spectroscopy for several fields, including astrophysics, atmospheric physics, atomic structure and metology, is discussed. (orig.)

  14. Communication: Coherences observed in vivo in photosynthetic bacteria using two-dimensional electronic spectroscopy

    International Nuclear Information System (INIS)

    Dahlberg, Peter D.; Norris, Graham J.; Wang, Cheng; Viswanathan, Subha; Singh, Ved P.; Engel, Gregory S.

    2015-01-01

    Energy transfer through large disordered antenna networks in photosynthetic organisms can occur with a quantum efficiency of nearly 100%. This energy transfer is facilitated by the electronic structure of the photosynthetic antennae as well as interactions between electronic states and the surrounding environment. Coherences in time-domain spectroscopy provide a fine probe of how a system interacts with its surroundings. In two-dimensional electronic spectroscopy, coherences can appear on both the ground and excited state surfaces revealing detailed information regarding electronic structure, system-bath coupling, energy transfer, and energetic coupling in complex chemical systems. Numerous studies have revealed coherences in isolated photosynthetic pigment-protein complexes, but these coherences have not been observed in vivo due to the small amplitude of these signals and the intense scatter from whole cells. Here, we present data acquired using ultrafast video-acquisition gradient-assisted photon echo spectroscopy to observe quantum beating signals from coherences in vivo. Experiments were conducted on isolated light harvesting complex II (LH2) from Rhodobacter sphaeroides, whole cells of R. sphaeroides, and whole cells of R. sphaeroides grown in 30% deuterated media. A vibronic coherence was observed following laser excitation at ambient temperature between the B850 and the B850 ∗ states of LH2 in each of the 3 samples with a lifetime of ∼40-60 fs

  15. Communication: Coherences observed in vivo in photosynthetic bacteria using two-dimensional electronic spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Dahlberg, Peter D. [Graduate Program in the Biophysical Sciences, Institute for Biophysical Dynamics, and The James Franck Institute, The University of Chicago, Chicago, Illinois 60637 (United States); Norris, Graham J.; Wang, Cheng; Viswanathan, Subha; Singh, Ved P.; Engel, Gregory S., E-mail: gsengel@uchicago.edu [Department of Chemistry, Institute for Biophysical Dynamics, and The James Franck Institute, The University of Chicago, Chicago, Illinois 60637 (United States)

    2015-09-14

    Energy transfer through large disordered antenna networks in photosynthetic organisms can occur with a quantum efficiency of nearly 100%. This energy transfer is facilitated by the electronic structure of the photosynthetic antennae as well as interactions between electronic states and the surrounding environment. Coherences in time-domain spectroscopy provide a fine probe of how a system interacts with its surroundings. In two-dimensional electronic spectroscopy, coherences can appear on both the ground and excited state surfaces revealing detailed information regarding electronic structure, system-bath coupling, energy transfer, and energetic coupling in complex chemical systems. Numerous studies have revealed coherences in isolated photosynthetic pigment-protein complexes, but these coherences have not been observed in vivo due to the small amplitude of these signals and the intense scatter from whole cells. Here, we present data acquired using ultrafast video-acquisition gradient-assisted photon echo spectroscopy to observe quantum beating signals from coherences in vivo. Experiments were conducted on isolated light harvesting complex II (LH2) from Rhodobacter sphaeroides, whole cells of R. sphaeroides, and whole cells of R. sphaeroides grown in 30% deuterated media. A vibronic coherence was observed following laser excitation at ambient temperature between the B850 and the B850{sup ∗} states of LH2 in each of the 3 samples with a lifetime of ∼40-60 fs.

  16. Laser excitation of SF6: spectroscopy and coherent pulse propagation effects

    International Nuclear Information System (INIS)

    Cantrell, C.D.; Makarov, A.A.; Louisell, W.H.

    1978-01-01

    Recent theoretical studies of coherent propagation effects in SF 6 and other polyatomic molecules are summarized beginning with an account of relevant aspects of the high-resolution spectroscopy of the ν 3 band of SF 6 . A laser pulse propagating in a molecular gas can acquire new frequencies which were not initially present in the pulse, and, in fact, a wave is coherently generated at the frequency of every molecular transition accessible from the initial molecular energy levels. The possible consequences of coherent generation of sidebands for the multiple-photon excitation of SF 6 and other polyatomic molecules are discussed

  17. Precise Control of Molecular Dynamics with a Femtosecond Frequency Comb - A Weak Field Route to Strong Field Coherent Control

    OpenAIRE

    Pe'er, Avi; Shapiro, Evgeny A.; Stowe, Matthew C.; Shapiro, Moshe; Ye, Jun

    2006-01-01

    We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful combination of pump-d...

  18. High-resolution coherent three-dimensional spectroscopy of Br2.

    Science.gov (United States)

    Chen, Peter C; Wells, Thresa A; Strangfeld, Benjamin R

    2013-07-25

    In the past, high-resolution spectroscopy has been limited to small, simple molecules that yield relatively uncongested spectra. Larger and more complex molecules have a higher density of peaks and are susceptible to complications (e.g., effects from conical intersections) that can obscure the patterns needed to resolve and assign peaks. Recently, high-resolution coherent two-dimensional (2D) spectroscopy has been used to resolve and sort peaks into easily identifiable patterns for molecules where pattern-recognition has been difficult. For very highly congested spectra, however, the ability to resolve peaks using coherent 2D spectroscopy is limited by the bandwidth of instrumentation. In this article, we introduce and investigate high-resolution coherent three-dimensional spectroscopy (HRC3D) as a method for dealing with heavily congested systems. The resulting patterns are unlike those in high-resolution coherent 2D spectra. Analysis of HRC3D spectra could provide a means for exploring the spectroscopy of large and complex molecules that have previously been considered too difficult to study.

  19. Linearity of Air-Biased Coherent Detection for Terahertz Time-Domain Spectroscopy

    DEFF Research Database (Denmark)

    Wang, Tianwu; Iwaszczuk, Krzysztof; Wrisberg, Emil Astrup

    2016-01-01

    The performance of air-biased coherent detection (ABCD) in a broadband two-color laser-induced air plasma system for terahertz time-domain spectroscopy (THz-TDS) has been investigated. Fundamental parameters of the ABCD detection, including signal-to-noise ratio (SNR), dynamic range (DR), and lin...

  20. 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.

  1. Optical spectroscopy in channel waveguides made in Nd:YAG crystals by femtosecond laser writing

    International Nuclear Information System (INIS)

    Torchia, G.A.; Mendez, C.; Roso, L.; Tocho, J.O.

    2008-01-01

    In this work, we present an optical characterization of channel waveguides fabricated by means of femtosecond laser writing on Nd:YAG substrates. These guiding structures show a refractive index increment of about 1x10 -3 which allows TE propagation. By pumping with a CW solid-state laser at 532 nm reaching the 2 G 9/2 and 4 G 7/2 manifolds of Nd 3+ ions, we have explored the emission band corresponding to 4 F 3/2 → 4 I 9/2 optical transitions (peaked at 890 nm). From data, we have found that emission showed similar characteristics for waveguide and bulk. On the other hand, the lifetime corresponding to the 4 F 3/2 metaestable level was determined to be 240 μs for bulk and waveguide. Summarizing, we have made suitable channel waveguides in Nd:YAG crystals, by fs interaction, with similar spectroscopic properties to those of the bulk, a fact that boosters the photonics application of these devices. For the first time to our knowledge, a direct index increment waveguide made by interaction with ultra-short intense pulses in YAG crystals has been performed. This fabrication procedure can be an efficient tool to make several optical circuits in active materials by means of the one-step, fast and low-cost processing

  2. Linear photophysics, two-photon absorption and femtosecond transient absorption spectroscopy of styryl dye bases

    Energy Technology Data Exchange (ETDEWEB)

    Shaydyuk, Ye.O. [Institute of Physics, Prospect Nauki, 46, Kyiv-28 03028 Ukraine (Ukraine); Levchenko, S.M. [Institute of Molecular Biology and Genetics, 150, Akademika Zabolotnoho Str., Kyiv 036803 (Ukraine); Kurhuzenkau, S.A. [Department of Chemistry, University of Parma, Parco Area delle Scienze 17/A, Parma 43124 (Italy); Anderson, D. [NanoScienece Technology Center, University of Central Florida, 12424 Research Parkway, PAV400, Orlando, FL 32826 (United States); Department of Chemistry, University of Central Florida, 4111 Libra Drive, PSB225, Orlando, FL 32816 (United States); Masunov, A.E. [NanoScienece Technology Center, University of Central Florida, 12424 Research Parkway, PAV400, Orlando, FL 32826 (United States); Department of Chemistry, University of Central Florida, 4111 Libra Drive, PSB225, Orlando, FL 32816 (United States); South Ural State University, Lenin pr. 76, Chelyabinsk 454080 (Russian Federation); Department of Condensed Matter Physics, National Research Nuclear University MEPhI, Kashirskoye shosse 31, Moscow 115409 (Russian Federation); Photochemistry Center RAS, ul. Novatorov 7a, Moscow 119421 (Russian Federation); Kachkovsky, O.D.; Slominsky, Yu.L.; Bricks, J.L. [Insitute of Organic Chemistry, Murmanskaya Street, 5, Kyiv 03094 (Ukraine); Belfield, K.D. [College of Science and Liberal Arts, New Jersey Institute of Technology, University Heights, Newark, NJ 07102 (United States); School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an, 710062 (China); Bondar, M.V., E-mail: mbondar@mail.ucf.edu [Institute of Physics, Prospect Nauki, 46, Kyiv-28 03028 Ukraine (Ukraine)

    2017-03-15

    The steady-state and time-resolved linear spectral properties, two-photon absorption spectra and fast relaxation processes in the excited states of styryl base-type derivatives were investigated. The nature of linear absorption, fluorescence and excitation anisotropy spectra were analyzed in solvents of different polarity at room temperature and specific dependence of the solvatochromic behavior on the donor-acceptor strength of the terminal substituents was shown. Two-photon absorption (2PA) efficiency of styryl dye bases was determined in a broad spectral range using two-photon induced fluorescence technique, and cross-sections maxima of ~ 100 GM were found. The excited state absorption (ESA) and fast relaxation processes in the molecular structures were investigated by transient absorption femtosecond pump-probe methodology. The role of twisted intramolecular charge transfer (TICT) effect in the excited state of styryl dye base with dimethylamino substituent was shown. The experimental spectroscopic data were also verified by quantum chemical calculations at the Time Dependent Density Functional Theory level, combined with a polarizable continuum model.

  3. Femtosecond Two-Photon Absorption Spectroscopy of Poly(fluorene Derivatives Containing Benzoselenadiazole and Benzothiadiazole

    Directory of Open Access Journals (Sweden)

    Marcelo Gonçalves Vivas

    2017-05-01

    Full Text Available We have investigated the molecular structure and two-photon absorption (2PA properties relationship of two push–pull poly(fluorene derivatives containing benzoselenadiazole and benzothiadiazole units. For that, we have used the femtosecond wavelength-tunable Z-scan technique with a low repetition rate (1 kHz and an energy per pulse on the order of nJ. Our results show that both 2PA spectra present a strong 2PA (around 600 GM (1 GM = 1 × 10−50 cm4·s·photon−1 band at around 720 nm (transition energy 3.45 eV ascribed to the strongly 2PA-allowed 1Ag-like → mAg-like transition, characteristic of poly(fluorene derivatives. Another 2PA band related to the intramolecular charge transfer was also observed at around 900 nm (transition energy 2.75 eV. In both 2PA bands, we found higher 2PA cross-section values for the poly(fluorene containing benzothiadiazole unit. This outcome was explained through the higher charge redistribution at the excited state caused by the benzothiadiazole group as compared to the benzoselenadiazole and confirmed by means of solvatochromic Stokes shift measurements. To shed more light on these results, we employed the sum-over-states approach within the two-energy level model to estimate the maximum permanent dipole moment change related to the intramolecular charge transfer transition.

  4. Electron transfer dynamics of triphenylamine dyes bound to TiO2 nanoparticles from femtosecond stimulated Raman spectroscopy

    KAUST Repository

    Hoffman, David P.

    2013-04-11

    Interfacial electron transfer between sensitizers and semiconducting nanoparticles is a crucial yet poorly understood process. To address this problem, we have used transient absorption (TA) and femtosecond stimulated Raman spectroscopy (FSRS) to investigate the photoexcited dynamics of a series of triphenylamine-coumarin dye/TiO2 conjugates. The TA decay is multiexponential, spanning time scales from 100 fs to 100 ps, while the characteristic transient Raman spectrum of the radical cation decays biexponentially with a dominant ∼3 ps component. To explain these observations, we propose a model in which the decay of the TA is due to hot electrons migrating from surface trap states to the conduction band of TiO 2 while the decay of the Raman signature is due to internal conversion of the dye molecule. Furthermore, the S1 Raman spectrum of TPAC3, a dye wherein a vinyl group separates the triphenylamine and coumarin moieties, is similar to the S1 Raman spectrum of trans-stilbene; we conclude that their S1 potential energy surfaces and reactivity are also similar. This correlation suggests that dyes containing vinyl linkers undergo photoisomerization that competes with electron injection. © 2013 American Chemical Society.

  5. Raman spectroscopy of femtosecond multipulse irradiation of vitreous silica: Experiment and simulation

    Science.gov (United States)

    Shcheblanov, N. S.; Povarnitsyn, M. E.; Mishchik, K. N.; Tanguy, A.

    2018-02-01

    We report an experimental and numerical study of femtosecond multipulse laser-induced densification in vitreous silica (v -SiO2 ) and its signature in Raman spectra. We compare the experimental findings to the recently developed molecular dynamics (MD) approach accounting for bond breaking due to laser irradiation, together with a dynamical matrix approach and bond polarizability model based on first-principles calculations for the estimation of Raman spectra. We observe two stages of the laser-induced densification and Raman spectrum evolution: growth during several hundreds of pulses followed by further saturation. At the medium range, the network connectivity change in v -SiO2 is expressed in reduction of the major ring fractions leading to more compacted structure. With the help of the Sen and Thorpe model, we also study the short-range order transformation and derive the interbonding Si-O-Si angle change from the Raman measurements. Experimental findings are in excellent agreement with our MD simulations and hence support a bond-breaking mechanism of laser-induced densification. Thus, our modeling explains well the laser-induced changes both in the short-range order caused by the appearance of Si coordination defects and medium-range order connected to evolution of the ring distribution. Finally, our findings disclose similarities between sheared, permanently densified, and laser-induced glass and suggest interesting future experiments in order to clarify the impact of the thermomechanical history on glasses under shear, cold and hot compression, and laser-induced densification.

  6. Femtosecond coherent control of absorption and free induction decay in a GaAs multiple quantum well

    CERN Document Server

    Yee, D S

    2000-01-01

    Excitonic polarizations are coherently excited using two phase-locked pulses. By probing the linear propagation of the pulses through a GaAs/AlGaAs multiple quantum well sample, we directly demonstrate the intriguing interaction between the coherent exciton polarizations and the controlling pulses. It is shown that the second pulse can be either strongly amplified by taking up energy gained from the destruction of the exciton polarization or drastically decreased by giving up all its energy to excitons. The temporal signatures of the transmitted pulse shapes agree well with model calculations.

  7. Investigation of the S1/ICT equilibrium in fucoxanthin by ultrafast pump-dump-probe and femtosecond stimulated Raman scattering spectroscopy.

    Science.gov (United States)

    Redeckas, Kipras; Voiciuk, Vladislava; Vengris, Mikas

    2016-05-01

    Time-resolved multi-pulse spectroscopic methods-pump-dump-probe (PDP) and femtosecond stimulated Raman spectroscopy-were used to investigate the excited state photodynamics of the carbonyl group containing carotenoid fucoxanthin (FX). PDP experiments show that S1 and ICT states in FX are strongly coupled and that the interstate equilibrium is rapidly (<5 ps) reestablished after one of the interacting states is deliberately depopulated. Femtosecond stimulated Raman scattering experiments indicate that S1 and ICT are vibrationally distinct species. Identification of the FSRS modes on the S1 and ICT potential energy surfaces allows us to predict a possible coupling channel for the state interaction.

  8. Spectroscopie de Fourier par peignes de fréquences femtosecondes

    OpenAIRE

    Mandon , Julien

    2009-01-01

    This work presents results towards the development of a novel frequency-comb based Fourier transform spectroscopy (FTS). Since 1970, due to its exceptional qualities, FTS has offered a simple way for spectral analysis and has assumed a position of dominance for the measurement of broadband well-resolved accurate spectra. However, FTS doesn't satisfy the new requirements in molecular physics. Acquisition time at the limit, extreme resolution, broad spectral extension, high sensitivity, and acc...

  9. A versatile setup for ultrafast broadband optical spectroscopy of coherent collective modes in strongly correlated quantum systems

    Directory of Open Access Journals (Sweden)

    Edoardo Baldini

    2016-11-01

    Full Text Available A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide temperature range. By combining high temporal resolution and a broad detection window, this apparatus can investigate the interplay between coherent collective modes and high-energy electronic excitations, which is a distinctive characteristic of correlated electron systems. Using a single-shot readout array detector at frame rates of 10 kHz allows resolving coherent oscillations with amplitudes <10−4. We demonstrate its operation on the charge-transfer insulator La2CuO4, revealing coherent phonons with frequencies up to 13 THz and providing access into their Raman matrix elements.

  10. Femtosecond nonlinear spectroscopy at surfaces: Second-harmonic probing of hole burning at the Si(111)7x7 surface and Fourier-transform sum-frequency vibrational spectroscopy

    International Nuclear Information System (INIS)

    McGuire, John Andrew

    2004-01-01

    The high temporal resolution and broad bandwidth of a femtosecond laser system are exploited in a pair of nonlinear optical studies of surfaces. The dephasing dynamics of resonances associated with the adatom dangling bonds of the Si(111)7 x 7 surface are explored by transient second-harmonic hole burning, a process that can be described as a fourth-order nonlinear optical process. Spectral holes produced by a 100 fs pump pulse at about 800 nm are probed by the second harmonic signal of a 100 fs pulse tunable around 800 nm. The measured spectral holes yield homogeneous dephasing times of a few tens of femtoseconds. Fits with a Lorentzian spectral hole centered at zero probe detuning show a linear dependence of the hole width on pump fluence, which suggests that charge carrier-carrier scattering dominates the dephasing dynamics at the measured excitation densities. Extrapolation of the deduced homogeneous dephasing times to zero excitation density yields an intrinsic dephasing time of ∼ 70 fs. The presence of a secondary spectral hole indicates that scattering of the surface electrons with surface optical phonons at 570 cm -1 occurs within the first 200 fs after excitation. The broad bandwidth of femtosecond IR pulses is used to perform IR-visible sum frequency vibrational spectroscopy. By implementing a Fourier-transform technique, we demonstrate the ability to obtain sub-laser-bandwidth spectral resolution. FT-SFG yields a greater signal when implemented with a stretched visible pulse than with a femtosecond visible pulse. However, when compared with multichannel spectroscopy using a femtosecond IR pulse but a narrowband visible pulse, Fourier-transform SFG is found to have an inferior signal-to-noise ratio. A mathematical analysis of the signal-to-noise ratio illustrates the constraints on the Fourier-transform approach

  11. Femtosecond nonlinear spectroscopy at surfaces: Second-harmonic probing of hole burning at the Si(111)7x7 surface and fourier-transform sum-frequency vibrational spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    McGuire, John Andrew [Univ. of California, Berkeley, CA (United States)

    2004-11-24

    The high temporal resolution and broad bandwidth of a femtosecond laser system are exploited in a pair of nonlinear optical studies of surfaces. The dephasing dynamics of resonances associated with the adatom dangling bonds of the Si(111)7 x 7 surface are explored by transient second-harmonic hole burning, a process that can be described as a fourth-order nonlinear optical process. Spectral holes produced by a 100 fs pump pulse at about 800 nm are probed by the second harmonic signal of a 100 fs pulse tunable around 800 nm. The measured spectral holes yield homogeneous dephasing times of a few tens of femtoseconds. Fits with a Lorentzian spectral hole centered at zero probe detuning show a linear dependence of the hole width on pump fluence, which suggests that charge carrier-carrier scattering dominates the dephasing dynamics at the measured excitation densities. Extrapolation of the deduced homogeneous dephasing times to zero excitation density yields an intrinsic dephasing time of {approx} 70 fs. The presence of a secondary spectral hole indicates that scattering of the surface electrons with surface optical phonons at 570 cm-1 occurs within the first 200 fs after excitation. The broad bandwidth of femtosecond IR pulses is used to perform IR-visible sum frequency vibrational spectroscopy. By implementing a Fourier-transform technique, we demonstrate the ability to obtain sub-laser-bandwidth spectral resolution. FT-SFG yields a greater signal when implemented with a stretched visible pulse than with a femtosecond visible pulse. However, when compared with multichannel spectroscopy using a femtosecond IR pulse but a narrowband visible pulse, Fourier-transform SFG is found to have an inferior signal-to-noise ratio. A mathematical analysis of the signal-to-noise ratio illustrates the constraints on the Fourier-transform approach.

  12. Observing Solvation Dynamics with Simultaneous Femtosecond X-ray Emission Spectroscopy and X-ray Scattering

    DEFF Research Database (Denmark)

    Haldrup, Kristoffer; Gawelda, Wojciech; Abela, Rafael

    2016-01-01

    and structural changes, and local solvent structural changes are desired. We have studied the intra- and intermolecular dynamics of a model chromophore, aqueous [Fe(bpy)3]2+, with complementary X-ray tools in a single experiment exploiting intense XFEL radiation as a probe. We monitored the ultrafast structural...... rearrangement of the solute with X-ray emission spectroscopy, thus establishing time zero for the ensuing X-ray diffuse scattering analysis. The simultaneously recorded X-ray diffuse scattering atterns reveal slower subpicosecond dynamics triggered by the intramolecular structural dynamics of the photoexcited...

  13. Nonadiabatic Dynamics May Be Probed through Electronic Coherence in Time-Resolved Photoelectron Spectroscopy.

    Science.gov (United States)

    Bennett, Kochise; Kowalewski, Markus; Mukamel, Shaul

    2016-02-09

    We present a hierarchy of Fermi golden rules (FGRs) that incorporate strongly coupled electronic/nuclear dynamics in time-resolved photoelectron spectroscopy (TRPES) signals at different levels of theory. Expansion in the joint electronic and nuclear eigenbasis yields the numerically most challenging exact FGR (eFGR). The quasistatic Fermi Golden Rule (qsFGR) neglects nuclear motion during the photoionization process but takes into account electronic coherences as well as populations initially present in the pumped matter as well as those generated internally by coupling between electronic surfaces. The standard semiclassical Fermi Golden Rule (scFGR) neglects the electronic coherences and the nuclear kinetic energy during the ionizing pulse altogether, yielding the classical Condon approximation. The coherence contributions depend on the phase-profile of the ionizing field, allowing coherent control of TRPES signals. The photoelectron spectrum from model systems is simulated using these three levels of theory. The eFGR and the qsFGR show temporal oscillations originating from the electronic or vibrational coherences generated as the nuclear wave packet traverses a conical intersection. These oscillations, which are missed by the scFGR, directly reveal the time-evolving splitting between electronic states of the neutral molecule in the curve-crossing regime.

  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. Dynamical behavior of the wave packets on adiabatic potential surfaces observed by femtosecond luminescence spectroscopy

    International Nuclear Information System (INIS)

    Suemoto, Tohru; Nakajima, Makoto; Matsuoka, Taira; Yasukawa, Keizo; Koyama, Takeshi

    2007-01-01

    The wave packet dynamics on adiabatic potential surfaces studied by means of time-resolved luminescence spectroscopy is reviewed and the advantages of this method are discussed. In quasi-one-dimensional bromine-bridged platinum complexes, a movie representing the time evolution of the wave packet motion and shape was constructed. A two-dimensional Lissajous-like motion of the wave packet was suggested in the same material at low temperature. In F-centers in KI, evidence for tunneling of the wave packet between the adjacent adiabatic potential surfaces was found. Selective observation of the wave packet motion on the excited state was demonstrated for F-centers in KBr and compared with the results from pump-and-probe experiments in literature

  16. Femtosecond optical parametric oscillators toward real-time dual-comb spectroscopy

    Science.gov (United States)

    Jin, Yuwei; Cristescu, Simona M.; Harren, Frans J. M.; Mandon, Julien

    2015-04-01

    We demonstrate mid-infrared dual-comb spectroscopy with an optical parametric oscillator (OPO) toward real-time field measurement. A singly resonant OPO based on a MgO-doped periodically poled lithium niobate (PPLN) crystal is demonstrated. Chirped mirrors are used to compensate the dispersion caused by the optical cavity and the crystal. A low threshold of 17 mW has been achieved. The OPO source generates a tunable idler frequency comb between 2.7 and 4.7 μm. Dual-comb spectroscopy is achieved by coupling two identical Yb-fiber mode-locked lasers to this OPO with slightly different repetition frequencies. A measured absorption spectrum of methane is presented with a spectral bandwidth of , giving an instrumental resolution of . In addition, a second OPO containing two MgO-doped PPLN crystals in a singly resonant ring cavity is demonstrated. As such, this OPO generates two idler combs (average power up to 220 mW), covering a wavelength range between 2.7 and 4.2 μm, from which a mid-infrared dual-comb Fourier transform spectrometer is constructed. By detecting the heterodyned signal between the two idler combs, broadband spectra of molecular gases can be observed over a spectral bandwidth of more than . This special cavity design allows the spectral resolution to be improved to without locking the OPO cavity, indicating that this OPO represents an ideal high-power broadband mid-infrared source for real-time gas sensing.

  17. Improved Carrier Transport in Perovskite Solar Cells Probed by Femtosecond Transient Absorption Spectroscopy.

    Science.gov (United States)

    Serpetzoglou, Efthymis; Konidakis, Ioannis; Kakavelakis, George; Maksudov, Temur; Kymakis, Emmanuel; Stratakis, Emmanuel

    2017-12-20

    CH 3 NH 3 PbI 3 perovskite thin films have been deposited on glass/indium tin oxide/hole transport layer (HTL) substrates, utilizing two different materials as the HTLs. In the first configuration, the super hydrophilic polymer poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate), known as PEDOT:PSS, was employed as the HTL material, whereas in the second case, the nonwetting poly(triarylamine) semiconductor polymer, known as PTAA, was used. It was found that when PTAA is used as the HTL material, the averaged power conversion efficiency (PCE) of the perovskite solar cells (PSCs) remarkably increases from 12.60 to 15.67%. To explore the mechanism behind this enhancement, the aforementioned perovskite/HTL arrangements were investigated by time-resolved transient absorption spectroscopy (TAS) performed under inert conditions. By means of TAS, the charge transfer, carrier trapping, and hole injection dynamics from the photoexcited perovskite layers to the HTL can be directly monitored via the characteristic bleaching profile of the perovskite at ∼750 nm. TAS studies revealed faster relaxation times and decay dynamics when the PTAA polymer is employed, which potentially account for the enhanced PCE observed. The TAS results are correlated with the structure and crystalline quality of the corresponding perovskite films, investigated by scanning electron microscopy, X-ray diffraction, atomic force microscopy, micro-photoluminescence, and transmittance spectroscopy. It is concluded that TAS is a benchmark technique for the understanding of the carrier transport mechanisms in PSCs and constitutes a figure-of-merit tool toward their efficiency improvement.

  18. 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 .

  19. 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}.

  20. Vibrational motions associated with primary processes in bacteriorhodopsin studied by coherent infrared emission spectroscopy.

    Science.gov (United States)

    Groma, Géza I; Colonna, Anne; Martin, Jean-Louis; Vos, Marten H

    2011-03-16

    The primary energetic processes driving the functional proton pump of bacteriorhodopsin take place in the form of complex molecular dynamic events after excitation of the retinal chromophore into the Franck-Condon state. These early events include a strong electronic polarization, skeletal stretching, and all-trans-to-13-cis isomerization upon formation of the J intermediate. The effectiveness of the photoreaction is ensured by a conical intersection between the electronic excited and ground states, providing highly nonadiabatic coupling to nuclear motions. Here, we study real-time vibrational coherences associated with these motions by analyzing light-induced infrared emission from oriented purple membranes in the 750-1400 cm(-)(1) region. The experimental technique applied is based on second-order femtosecond difference frequency generation on macroscopically ordered samples that also yield information on phase and direction of the underlying motions. Concerted use of several analysis methods resulted in the isolation and characterization of seven different vibrational modes, assigned as C-C stretches, out-of-plane methyl rocks, and hydrogen out-of-plane wags, whereas no in-plane H rock was found. Based on their lifetimes and several other criteria, we deduce that the majority of the observed modes take place on the potential energy surface of the excited electronic state. In particular, the direction sensitivity provides experimental evidence for large intermediate distortions of the retinal plane during the excited-state isomerization process. Copyright © 2011 Biophysical Society. Published by Elsevier Inc. All rights reserved.

  1. Rapid-scan Fourier-transform coherent anti-Stokes Raman scattering spectroscopy with heterodyne detection.

    Science.gov (United States)

    Hiramatsu, Kotaro; Luo, Yizhi; Ideguchi, Takuro; Goda, Keisuke

    2017-11-01

    High-speed Raman spectroscopy has become increasingly important for analyzing chemical dynamics in real time. To address the need, rapid-scan Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) spectroscopy has been developed to realize broadband CARS measurements at a scan rate of more than 20,000 scans/s. However, the detection sensitivity of FT-CARS spectroscopy is inherently low due to the limited number of photons detected during each scan. In this Letter, we show our experimental demonstration of enhanced sensitivity in rapid-scan FT-CARS spectroscopy by heterodyne detection. Specifically, we implemented heterodyne detection by superposing the CARS electric field with an external local oscillator (LO) for their interference. The CARS signal was amplified by simply increasing the power of the LO without the need for increasing the incident power onto the sample. Consequently, we achieved enhancement in signal intensity and the signal-to-noise ratio by factors of 39 and 5, respectively, compared to FT-CARS spectroscopy with homodyne detection. The sensitivity-improved rapid-scan FT-CARS spectroscopy is expected to enable the sensitive real-time observation of chemical dynamics in a broad range of settings, such as combustion engines and live biological cells.

  2. Precision of coherence analysis to detect cerebral autoregulation by near-infrared spectroscopy in preterm infants

    DEFF Research Database (Denmark)

    Hahn, GH; Christensen, KB; Leung, TS

    2010-01-01

    Coherence between spontaneous fluctuations in arterial blood pressure (ABP) and the cerebral near-infrared spectroscopy signal can detect cerebral autoregulation. Because reliable measurement depends on signals with high signal-to-noise ratio, we hypothesized that coherence is more precisely...... determined when fluctuations in ABP are large rather than small. Therefore, we investigated whether adjusting for variability in ABP (variabilityABP) improves precision. We examined the impact of variabilityABP within the power spectrum in each measurement and between repeated measurements in preterm infants....... We also examined total monitoring time required to discriminate among infants with a simulation study. We studied 22 preterm infants (GAABP within the power spectrum did not improve the precision. However, adjusting...

  3. Versatile silicon-waveguide supercontinuum for coherent mid-infrared spectroscopy

    Science.gov (United States)

    Nader, Nima; Maser, Daniel L.; Cruz, Flavio C.; Kowligy, Abijith; Timmers, Henry; Chiles, Jeff; Fredrick, Connor; Westly, Daron A.; Nam, Sae Woo; Mirin, Richard P.; Shainline, Jeffrey M.; Diddams, Scott

    2018-03-01

    Laser frequency combs, with their unique combination of precisely defined spectral lines and broad bandwidth, are a powerful tool for basic and applied spectroscopy. Here, we report offset-free, mid-infrared frequency combs and dual-comb spectroscopy through supercontinuum generation in silicon-on-sapphire waveguides. We leverage robust fabrication and geometrical dispersion engineering of nanophotonic waveguides for multi-band, coherent frequency combs spanning 70 THz in the mid-infrared (2.5 μm-6.2 μm). Precise waveguide fabrication provides significant spectral broadening with engineered spectra targeted at specific mid-infrared bands. We characterize the relative-intensity-noise of different bands and show that the measured levels do not pose any limitation for spectroscopy applications. Additionally, we use the fabricated photonic devices to demonstrate dual-comb spectroscopy of a carbonyl sulfide gas sample at 5 μm. This work forms the technological basis for applications such as point sensors for fundamental spectroscopy, atmospheric chemistry, trace and hazardous gas detection, and biological microscopy.

  4. Versatile silicon-waveguide supercontinuum for coherent mid-infrared spectroscopy

    Directory of Open Access Journals (Sweden)

    Nima Nader

    2018-03-01

    Full Text Available Laser frequency combs, with their unique combination of precisely defined spectral lines and broad bandwidth, are a powerful tool for basic and applied spectroscopy. Here, we report offset-free, mid-infrared frequency combs and dual-comb spectroscopy through supercontinuum generation in silicon-on-sapphire waveguides. We leverage robust fabrication and geometrical dispersion engineering of nanophotonic waveguides for multi-band, coherent frequency combs spanning 70 THz in the mid-infrared (2.5 μm–6.2 μm. Precise waveguide fabrication provides significant spectral broadening with engineered spectra targeted at specific mid-infrared bands. We characterize the relative-intensity-noise of different bands and show that the measured levels do not pose any limitation for spectroscopy applications. Additionally, we use the fabricated photonic devices to demonstrate dual-comb spectroscopy of a carbonyl sulfide gas sample at 5 μm. This work forms the technological basis for applications such as point sensors for fundamental spectroscopy, atmospheric chemistry, trace and hazardous gas detection, and biological microscopy.

  5. Optically controlled locking of the nuclear field via coherent dark-state spectroscopy.

    Science.gov (United States)

    Xu, Xiaodong; Yao, Wang; Sun, Bo; Steel, Duncan G; Bracker, Allan S; Gammon, Daniel; Sham, L J

    2009-06-25

    A single electron or hole spin trapped inside a semiconductor quantum dot forms the foundation for many proposed quantum logic devices. In group III-V materials, the resonance and coherence between two ground states of the single spin are inevitably affected by the lattice nuclear spins through the hyperfine interaction, while the dynamics of the single spin also influence the nuclear environment. Recent efforts have been made to protect the coherence of spins in quantum dots by suppressing the nuclear spin fluctuations. However, coherent control of a single spin in a single dot with simultaneous suppression of the nuclear fluctuations has yet to be achieved. Here we report the suppression of nuclear field fluctuations in a singly charged quantum dot to well below the thermal value, as shown by an enhancement of the single electron spin dephasing time T(2)*, which we measure using coherent dark-state spectroscopy. The suppression of nuclear fluctuations is found to result from a hole-spin assisted dynamic nuclear spin polarization feedback process, where the stable value of the nuclear field is determined only by the laser frequencies at fixed laser powers. This nuclear field locking is further demonstrated in a three-laser measurement, indicating a possible enhancement of the electron spin T(2)* by a factor of several hundred. This is a simple and powerful method of enhancing the electron spin coherence time without use of 'spin echo'-type techniques. We expect that our results will enable the reproducible preparation of the nuclear spin environment for repetitive control and measurement of a single spin with minimal statistical broadening.

  6. Study of high-temperature multiplex HCl coherent anti-Stokes Raman spectroscopy spectra.

    Science.gov (United States)

    Singh, J P; Yueh, F Y; Kao, W; Cook, R L

    1993-02-20

    A feasibility study of temperature measurement with multiplex HCl coherent anti-Stokes Raman spectroscopy (CARS) is investigated. The HCl CARS spectra of a 100% HCl gas sample are recorded in a quartz sample cell placed in a furnace at 1 atm pressure and at different temperatures. The nonlinear susceptibility of HCl (chi(nr)(HCl)), which is measured with the present CARS experimental setup, is reported. The experimental spectra are fit by using a library of simulated HCl CARS spectra with a least-squares-fitting program to infer the temperature. The inferred temperatures from HCl CARS spectra are in agreement with thermocouple temperatures.

  7. Metrological-grade tunable coherent source in the mid-infrared for molecular precision spectroscopy

    Science.gov (United States)

    Insero, G.; Clivati, C.; D'Ambrosio, D.; Cancio Pastor, P.; Verde, M.; Schunemann, P. G.; Zondy, J.-J.; Inguscio, M.; Calonico, D.; Levi, F.; De Natale, P.; Santambrogio, G.; Borri, S.

    2018-02-01

    We report on a metrological-grade mid-IR source with a 10-14 short-term instability for high-precision spectroscopy. Our source is based on the combination of a quantum cascade laser and a coherent radiation obtained by difference-frequency generation in an orientation-patterned gallium phosphide (OP-GaP) crystal. The pump and signal lasers are locked to an optical frequency comb referenced to the primary frequency standard via an optical fiber link. We demonstrate the robustness of the apparatus by measuring a vibrational transition around 6 μm on a metastable state of CO molecuels with 11 digits of precision.

  8. Control of phase transition dynamics in media with nanoscale nonuniformities by coherence loss spectroscopy

    International Nuclear Information System (INIS)

    Brodsky, Anatol M

    2010-01-01

    The optical nondestructive characterization of chemical transformation dynamics and diffusion kinetics, including phase transitions, in heterogeneous media with a random distribution of nanoparticles (nano-nonuniformities), is of great theoretical and practical importance. Such characterization, with the help of coherence loss spectroscopy, considered in this paper can be applied for the control of a number of industrial processes dynamics, environmental monitoring, and medical diagnostics and therapy. As a specific example, the growth of crystal nuclei (embrions) as a result of the diffusion to them of a substance from the surrounding supersaturated solution is considered

  9. Dicke coherent narrowing in two-photon and Raman spectroscopy of thin vapor cells

    International Nuclear Information System (INIS)

    Dutier, Gabriel; Todorov, Petko; Hamdi, Ismahene; Maurin, Isabelle; Saltiel, Solomon; Bloch, Daniel; Ducloy, Martial

    2005-01-01

    The principle of coherent Dicke narrowing in a thin vapor cell, in which sub-Doppler spectral line shapes are observed under a normal irradiation for a λ/2 thickness, is generalized to two-photon spectroscopy. Only the sum of the two wave vectors must be normal to the cell, making the two-photon scheme highly versatile. A comparison is provided between the Dicke narrowing with copropagating fields, and the residual Doppler broadening occurring with counterpropagating geometries. The experimental feasibility is discussed on the basis of a first observation of a two-photon resonance in a 300-nm-thick Cs cell. Extension to the Raman situation is finally considered

  10. Spectral watermarking in femtosecond stimulated Raman spectroscopy: resolving the nature of the carotenoid S-star state

    NARCIS (Netherlands)

    Kloz, Miroslav; Weissenborn, J.; Polivka, T.; Frank, H.A.; Kennis, J.T.M.

    2016-01-01

    A new method for recording femtosecond stimulated Raman spectra was developed that dramatically improves and automatizes baseline problems. Instead of using a narrowband Raman source, the experiment is performed using shaping of a broadband source. This allows locking the signal into carefully

  11. Photoinduced electron-transfer in perylenediimide triphenylamine-based dendrimers : single photon timing and femtosecond transient absorption spectroscopy

    NARCIS (Netherlands)

    Fron, Eduard; Pilot, Roberto; Schweitzer, Gerd; Qu, Jianqiang; Herrmann, Andreas; Müllen, Klaus; Hofkens, Johan; Auweraer, Mark Van der; Schryver, Frans C. De

    2008-01-01

    The excited state dynamics of two generations perylenediimide chromophores substituted in the bay area with dendritic branches bearing triphenylamine units as well as those of the respective reference compounds are investigated. Using single photon timing and multi-pulse femtosecond transient

  12. Analysis of organic pollutant degradation in pulsed plasma by coherent anti-Stokes Raman spectroscopy

    International Nuclear Information System (INIS)

    Bratescu, Maria Antoneta; Hieda, Junko; Umemura, Tomonari; Saito, Nagahiro; Takai, Osamu

    2011-01-01

    The degradation of p-benzoquinone (p-BQ) in water was investigated by the coherent anti-Stokes Raman spectroscopy (CARS) method, in which the change of the anti-Stokes signal intensity corresponding to the vibrational transitions of the molecule is monitored during and after solution plasma processing (SPP). In the beginning of SPP treatment, the CARS signal intensity of the ring vibrational molecular transitions at 1233 and 1660 cm -1 increases under the influence of the electric field of the plasma, depending on the delay time between the plasma pulse and the laser firing pulse. At the same time, the plasma contributes to the degradation of p-BQ molecules by generating hydrogen and hydroxyl radicals, which decompose p-BQ into different carboxylic acids. After SPP, the CARS signal intensity of the vibrational bands of p-BQ ceased and the degradation of p-BQ was confirmed by UV-visible absorption spectroscopy and liquid chromatography analysis.

  13. Coherent spectroscopy of a {Lambda} atomic system and its prospective application to tunable frequency offset locking

    Energy Technology Data Exchange (ETDEWEB)

    Kale, Y B [Laser and Plasma Technology Division, Bhabha Atomic Research Centre, Mumbai 400 085 (India); Ray, Ayan [Radioactive Ion Beam Group, Variable Energy Cyclotron Centre, Kolkata 700064 (India); Lawande, Q V [Theoretical Physics Division, Bhabha Atomic Research Centre, Mumbai 400 085 (India); Jagatap, B N, E-mail: yogeshwar84@rediffmail.com, E-mail: ayan_ray_in@rediffmail.com, E-mail: bnj@barc.gov.in [Atomic and Molecular Physics Division and Homi Bhabha National Institute, Bhabha Atomic Research Centre, Mumbai 400 085 (India)

    2011-09-15

    We investigate the coherent pump-probe spectroscopy of a three-level {Lambda} system, 6s{sub 1/2}F = 3,4{yields}6p{sub 3/2}F{sup '}= 4, in the hyperfine manifold of D{sub 2} transition (852 nm) of cesium with particular reference to the sub-Doppler linewidth resonance arising from Aulter-Townes (AT) splitting and the possibility of using it for realizing a scheme for tunable atomic frequency offset locking (AFOL). We discuss here the theoretical framework for a {Lambda} system interacting with a coherent pump and probe and use it to describe the process of modulation transfer in the AT and electromagnetically induced transparency regimes. We further employ an experimental scheme consisting of a strong pump and a pair of weak probes to resolve the sub-Doppler linewidth ({approx}8 MHz) AT resonance and study its dependence on pump intensity and detuning. In order to explore the possibility of using such a sub-Doppler linewidth resonance for AFOL, we use its first derivative signal as a frequency discriminator to stabilize the probe laser. The frequency stability of the probe is characterized by means of error signal analysis. This study reveals that while the frequency stability of the AT locked laser is limited by the pump laser, the tuning range of the offset frequency lock can cover the entire Doppler profile and its immediate neighbourhood, thereby providing a simple and cost effective alternative to the external modulator. The study described in this paper contributes to the discussion on the subtle link between dressed state spectroscopy and AFOL, which is relevant for developing a master-slave-type laser system in the domain of coherent photon-atom interaction.

  14. Characterizing interstate vibrational coherent dynamics of surface adsorbed catalysts by fourth-order 3D SFG spectroscopy

    Science.gov (United States)

    Li, Yingmin; Wang, Jiaxi; Clark, Melissa L.; Kubiak, Clifford P.; Xiong, Wei

    2016-04-01

    We report the first fourth-order 3D SFG spectroscopy of a monolayer of the catalyst Re(diCN-bpy)(CO)3Cl on a gold surface. Besides measuring the vibrational coherences of single vibrational modes, the fourth-order 3D SFG spectrum also measures the dynamics of interstate coherences and vibrational coherences states between two vibrational modes. By comparing the 3D SFG to the corresponding 2D and third-order 3D IR spectroscopy of the same molecules in solution, we found that the interstate coherences exist in both liquid and surface systems, suggesting that the interstate coherence is not disrupted by surface interactions. However, by analyzing the 3D spectral lineshape, we found that the interstate coherences also experience non-negligible homogenous dephasing dynamics that originate from surface interactions. This unique ability of determining interstate vibrational coherence dynamics of the molecular monolayer can help in understanding of how energy flows within surface catalysts and other molecular monolayers.

  15. Femtosecond time-resolved optical and Raman spectroscopy of photoinduced spin crossover: temporal resolution of low-to-high spin optical switching.

    Science.gov (United States)

    Smeigh, Amanda L; Creelman, Mark; Mathies, Richard A; McCusker, James K

    2008-10-29

    A combination of femtosecond electronic absorption and stimulated Raman spectroscopies has been employed to determine the kinetics associated with low-spin to high-spin conversion following charge-transfer excitation of a FeII spin-crossover system in solution. A time constant of tau = 190 +/- 50 fs for the formation of the 5T2 ligand-field state was assigned based on the establishment of two isosbestic points in the ultraviolet in conjunction with changes in ligand stretching frequencies and Raman scattering amplitudes; additional dynamics observed in both the electronic and vibrational spectra further indicate that vibrational relaxation in the high-spin state occurs with a time constant of ca. 10 ps. The results set an important precedent for extremely rapid, formally forbidden (DeltaS = 2) nonradiative relaxation as well as defining the time scale for intramolecular optical switching between two electronic states possessing vastly different spectroscopic, geometric, and magnetic properties.

  16. Characterization of Cs vapor cell coated with octadecyltrichlorosilane using coherent population trapping spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Hafiz, Moustafa Abdel; Maurice, Vincent; Chutani, Ravinder; Passilly, Nicolas; Gorecki, Christophe; Boudot, Rodolphe [FEMTO-ST, CNRS, UFC, 26 Chemin de l' Epitaphe, 25030 Besançon Cedex (France); Guérandel, Stéphane; Clercq, Emeric de [LNE-SYRTE, Observatoire de Paris, CNRS, UPMC, 61 avenue de l' Observatoire, 75014 Paris (France)

    2015-05-14

    We report the realization and characterization using coherent population trapping (CPT) spectroscopy of an octadecyltrichlorosilane (OTS)-coated centimeter-scale Cs vapor cell. The dual-structure of the resonance lineshape, with presence of a narrow structure line at the top of a Doppler-broadened structure, is clearly observed. The linewidth of the narrow resonance is compared to the linewidth of an evacuated Cs cell and of a buffer gas Cs cell of similar size. The Cs-OTS adsorption energy is measured to be (0.42 ± 0.03) eV, leading to a clock frequency shift rate of 2.7 × 10{sup −9}/K in fractional unit. A hyperfine population lifetime, T{sub 1}, and a microwave coherence lifetime, T{sub 2}, of 1.6 and 0.5 ms are reported, corresponding to about 37 and 12 useful bounces, respectively. Atomic-motion induced Ramsey narrowing of dark resonances is observed in Cs-OTS cells by reducing the optical beam diameter. Ramsey CPT fringes are detected using a pulsed CPT interrogation scheme. Potential applications of the Cs-OTS cell to the development of a vapor cell atomic clock are discussed.

  17. Characterization of Cs vapor cell coated with octadecyltrichlorosilane using coherent population trapping spectroscopy

    International Nuclear Information System (INIS)

    Hafiz, Moustafa Abdel; Maurice, Vincent; Chutani, Ravinder; Passilly, Nicolas; Gorecki, Christophe; Boudot, Rodolphe; Guérandel, Stéphane; Clercq, Emeric de

    2015-01-01

    We report the realization and characterization using coherent population trapping (CPT) spectroscopy of an octadecyltrichlorosilane (OTS)-coated centimeter-scale Cs vapor cell. The dual-structure of the resonance lineshape, with presence of a narrow structure line at the top of a Doppler-broadened structure, is clearly observed. The linewidth of the narrow resonance is compared to the linewidth of an evacuated Cs cell and of a buffer gas Cs cell of similar size. The Cs-OTS adsorption energy is measured to be (0.42 ± 0.03) eV, leading to a clock frequency shift rate of 2.7 × 10 −9 /K in fractional unit. A hyperfine population lifetime, T 1 , and a microwave coherence lifetime, T 2 , of 1.6 and 0.5 ms are reported, corresponding to about 37 and 12 useful bounces, respectively. Atomic-motion induced Ramsey narrowing of dark resonances is observed in Cs-OTS cells by reducing the optical beam diameter. Ramsey CPT fringes are detected using a pulsed CPT interrogation scheme. Potential applications of the Cs-OTS cell to the development of a vapor cell atomic clock are discussed

  18. Spin-resolved photoelectron spectroscopy using femtosecond extreme ultraviolet light pulses from high-order harmonic generation

    Energy Technology Data Exchange (ETDEWEB)

    Plötzing, M.; Adam, R., E-mail: r.adam@fz-juelich.de; Weier, C.; Plucinski, L.; Schneider, C. M. [Forschungszentrum Jülich GmbH, Peter Grünberg Institut (PGI-6), 52425 Jülich (Germany); Eich, S.; Emmerich, S.; Rollinger, M.; Aeschlimann, M. [University of Kaiserslautern and Research Center OPTIMAS, 67663 Kaiserslautern (Germany); Mathias, S. [Georg-August-Universität Göttingen, I. Physikalisches Institut, 37077 Göttingen (Germany)

    2016-04-15

    The fundamental mechanism responsible for optically induced magnetization dynamics in ferromagnetic thin films has been under intense debate since almost two decades. Currently, numerous competing theoretical models are in strong need for a decisive experimental confirmation such as monitoring the triggered changes in the spin-dependent band structure on ultrashort time scales. Our approach explores the possibility of observing femtosecond band structure dynamics by giving access to extended parts of the Brillouin zone in a simultaneously time-, energy- and spin-resolved photoemission experiment. For this purpose, our setup uses a state-of-the-art, highly efficient spin detector and ultrashort, extreme ultraviolet light pulses created by laser-based high-order harmonic generation. In this paper, we present the setup and first spin-resolved spectra obtained with our experiment within an acquisition time short enough to allow pump-probe studies. Further, we characterize the influence of the excitation with femtosecond extreme ultraviolet pulses by comparing the results with data acquired using a continuous wave light source with similar photon energy. In addition, changes in the spectra induced by vacuum space-charge effects due to both the extreme ultraviolet probe- and near-infrared pump-pulses are studied by analyzing the resulting spectral distortions. The combination of energy resolution and electron count rate achieved in our setup confirms its suitability for spin-resolved studies of the band structure on ultrashort time scales.

  19. Accelerating two-dimensional nuclear magnetic resonance correlation spectroscopy via selective coherence transfer

    Science.gov (United States)

    Ye, Qimiao; Chen, Lin; Qiu, Wenqi; Lin, Liangjie; Sun, Huijun; Cai, Shuhui; Wei, Zhiliang; Chen, Zhong

    2017-01-01

    Nuclear magnetic resonance (NMR) spectroscopy serves as an important tool for both qualitative and quantitative analyses of various systems in chemistry, biology, and medicine. However, applications of one-dimensional 1H NMR are often restrained by the presence of severe overlap among different resonances. The advent of two-dimensional (2D) 1H NMR constitutes a promising alternative by extending the crowded resonances into a plane and thereby alleviating the spectral congestions. However, the enhanced ability in discriminating resonances is achieved at the cost of extended experimental duration due to necessity of various scans with progressive delays to construct the indirect dimension. Therefore, in this study, we propose a selective coherence transfer (SECOT) method to accelerate acquisitions of 2D correlation spectroscopy by converting chemical shifts into spatial positions within the effective sample length and then performing an echo planar spectroscopic imaging module to record the spatial and spectral information, which generates 2D correlation spectrum after 2D Fourier transformation. The feasibility and effectiveness of SECOT have been verified by a set of experiments under both homogeneous and inhomogeneous magnetic fields. Moreover, evaluations of SECOT for quantitative analyses are carried out on samples with a series of different concentrations. Based on these experimental results, the SECOT may open important perspectives for fast, accurate, and stable investigations of various chemical systems both qualitatively and quantitatively.

  20. Resonant acoustic spectroscopy of soft tissues using embedded magnetomotive nanotransducers and optical coherence tomography

    International Nuclear Information System (INIS)

    Oldenburg, Amy L; Boppart, Stephen A

    2010-01-01

    We present a new method for performing dynamic elastography of soft tissue samples. By sensing nanoscale displacements with optical coherence tomography, a chirped, modulated force is applied to acquire the mechanical spectrum of a tissue sample within a few seconds. This modulated force is applied via magnetic nanoparticles, named 'nanotransducers', which are diffused into the tissue, and which contribute negligible inertia to the soft tissue mechanical system. Using this novel system, we observed that excised tissues exhibit mechanical resonance modes which are well described by a linear damped harmonic oscillator. Results are validated by using cylindrical tissue phantoms of agarose in which resonant frequencies (30-400 Hz) are consistent with longitudinal modes and the sample boundary conditions. We furthermore show that the Young's modulus can be computed from their measured resonance frequencies, analogous to resonant ultrasound spectroscopy for stiff material analysis. Using this new technique, named magnetomotive resonant acoustic spectroscopy (MRAS), we monitored the relative stiffening of an excised rat liver during a chemical fixation process.

  1. Femtosecond Coherent Spectroscopy at 800nm: MI-FROG Measures High-Field Ionization Rates in Gases

    International Nuclear Information System (INIS)

    Siders, C.W.; Siders, J.L.W.; Taylor, A.J.

    1999-01-01

    The authors report the first quantitative phase-sensitive measurement of ultrafast ionization rates in gases using Multi-phase Interferometric Frequency-Resolved Optical Gating. Ultrafast probe depletion via frequency mixing in the ionization front is observed

  2. Characterization and control of femtosecond electron and X-ray beams at free-electron lasers

    International Nuclear Information System (INIS)

    Behrens, Christopher

    2012-11-01

    X-ray free-electron lasers (FELs) open up new frontiers in photon science, and in order to take full advantage of these unique accelerator-based light sources, the characterization and control of the femtosecond electron and X-ray beams is essential. Within this cumulative thesis, recent results achieved within the active research field of femtosecond electron and X-ray beams at FELs are reported.The basic principles of X-ray FELs are described, and concepts of longitudinal electron beam diagnostics with femtosecond accuracy are covered. Experimental results obtained with a transverse deflecting structure (TDS) and spectroscopy of coherent terahertz radiation are presented, and the suppression of coherent optical radiation effects, required for diagnostics utilizing a TDS, is demonstrated. Control of the longitudinal phase space by using multiple radio frequencies for longitudinal electron beam tailoring is presented, and a new technique of reversible electron beam heating with two TDSs is described. For the characterization of femtosecond X-ray pulses, a novel method based on dedicated longitudinal phase space diagnostics for electron beams is introduced, and recent measurements with a streaking technique using external terahertz fields are presented.

  3. Characterization and control of femtosecond electron and X-ray beams at free-electron lasers

    Energy Technology Data Exchange (ETDEWEB)

    Behrens, Christopher

    2012-11-15

    X-ray free-electron lasers (FELs) open up new frontiers in photon science, and in order to take full advantage of these unique accelerator-based light sources, the characterization and control of the femtosecond electron and X-ray beams is essential. Within this cumulative thesis, recent results achieved within the active research field of femtosecond electron and X-ray beams at FELs are reported.The basic principles of X-ray FELs are described, and concepts of longitudinal electron beam diagnostics with femtosecond accuracy are covered. Experimental results obtained with a transverse deflecting structure (TDS) and spectroscopy of coherent terahertz radiation are presented, and the suppression of coherent optical radiation effects, required for diagnostics utilizing a TDS, is demonstrated. Control of the longitudinal phase space by using multiple radio frequencies for longitudinal electron beam tailoring is presented, and a new technique of reversible electron beam heating with two TDSs is described. For the characterization of femtosecond X-ray pulses, a novel method based on dedicated longitudinal phase space diagnostics for electron beams is introduced, and recent measurements with a streaking technique using external terahertz fields are presented.

  4. Femtosecond Nanofocusing with Full Optical Waveform Control

    International Nuclear Information System (INIS)

    Berweger, Samuel; Atkin, Joanna M.; Xu, Xiaoji G.; Olmon, Robert L.; Raschke, Markus Bernd

    2011-01-01

    The simultaneous nanometer spatial confinement and femtosecond temporal control of an optical excitation has been a long-standing challenge in optics. Previous approaches using surface plasmon polariton (SPP) resonant nanostructures or SPP waveguides have suffered from, for example, mode mismatch, or possible dependence on the phase of the driving laser field to achieve spatial localization. Here we take advantage of the intrinsic phase- and amplitude-independent nanofocusing ability of a conical noble metal tip with weak wavelength dependence over a broad bandwidth to achieve a 10 nm spatially and few-femtosecond temporally confined excitation. In combination with spectral pulse shaping and feedback on the second-harmonic response of the tip apex, we demonstrate deterministic arbitrary optical waveform control. In addition, the high efficiency of the nanofocusing tip provided by the continuous micro- to nanoscale mode transformation opens the door for spectroscopy of elementary optical excitations in matter on their natural length and time scales and enables applications from ultrafast nano-opto-electronics to single molecule quantum coherent control.

  5. Measurements of coherent hemodynamics to enrich the physiological information provided by near-infrared spectroscopy (NIRS) and functional MRI

    Science.gov (United States)

    Sassaroli, Angelo; Tgavalekos, Kristen; Pham, Thao; Krishnamurthy, Nishanth; Fantini, Sergio

    2018-02-01

    Hemodynamic-based neuroimaging techniques such as functional magnetic resonance imaging (fMRI) and near-infrared spectroscopy (NIRS) sense hemoglobin concentration in cerebral tissue. The local concentration of hemoglobin, which is differentiated into oxy- and deoxy-hemoglobin by NIRS, features spontaneous oscillations over time scales of 10-100 s in response to a number of local and systemic physiological processes. If one of such processes becomes the dominant source of cerebral hemodynamics, there is a high coherence between this process and the associated hemodynamics. In this work, we report a method to identify such conditions of coherent hemodynamics, which may be exploited to study and quantify microvasculature and microcirculation properties. We discuss how a critical value of significant coherence may depend on the specific data collection scheme (for example, the total acquisition time) and the nature of the hemodynamic data (in particular, oxy- and deoxy-hemoglobin concentrations measured with NIRS show an intrinsic level of correlation that must be taken into account). A frequency-resolved study of coherent hemodynamics is the basis for the new technique of coherent hemodynamics spectroscopy (CHS), which aims to provide measures of cerebral blood flow and cerebral autoregulation. While these concepts apply in principle to both fMRI and NIRS data, in this article we focus on NIRS data.

  6. Stationary and coherent spectroscopy of 167Er3+ in waveguides in 7LiYF4 crystal

    Directory of Open Access Journals (Sweden)

    Minnegaliev Mansur

    2017-01-01

    Full Text Available We have conducted a spectroscopic investigation of 167Er3+ ions in optical waveguides on an optical transition between the hyperfine sublevels of 4I15/2 and 4I9/2 multiplets. Waveguides with diameters ranging from 20 to 100 µm were produced in the crystal by a femtosecond laser using the depressed-cladding approach. The spectroscopy results of 167Er3+ ions inside the waveguides show additional broadening and an overall shifts of the spectra compared to the bulk spectrum of ions. The sign of the observed frequency shift depends on the diameter of the specific waveguide. We have also observed a two-pulse photon echo in several waveguides. The acquired results show the possibility for integrated quantum schemes in rare-earth ions doped crystals.

  7. Resolution enhancement in MR spectroscopy of red bone marrow fat via intermolecular double-quantum coherences

    Science.gov (United States)

    Bao, Jianfeng; Cui, Xiaohong; Huang, Yuqing; Zhong, Jianhui; Chen, Zhong

    2015-08-01

    High-resolution 1H magnetic resonance spectroscopy (MRS) is generally inaccessible in red bone marrow (RBM) tissues using conventional MRS techniques. This is because signal from these tissues suffers from severe inhomogeneity in the main static B0 field originated from the intrinsic honeycomb structures in trabecular bone. One way to reduce effects of B0 field inhomogeneity is by using the intermolecular double quantum coherence (iDQC) technique, which has been shown in other systems to obtain signals insensitive to B0 field inhomogeneity. In the present study, we employed an iDQC approach to enhance the spectral resolution of RBM. The feasibility and performance of this method for achieving high resolution MRS was verified by experiments on phantoms and pig vertebral bone samples. Unsaturated fatty acid peaks which overlap in the conventional MRS were well resolved and identified in the iDQC spectrum. Quantitative comparison of fractions of three types of fatty acids was performed between iDQC spectra on the in situ RMB and conventional MRS on the extracted fat from the same RBM. Observations of unsaturated fatty acids with iDQC MRS may provide valuable information and may hold potential in diagnosis of diseases such as obesity, diabetes, and leukemia.

  8. Coherent anti-Stokes Raman spectroscopy temperature measurements in an internal combustion engine

    Science.gov (United States)

    Ball, Don; Driver, H. Steve T.; Hutcheon, Richard J.; Lockett, Russel J.; Robertson, Gerald N.

    1994-09-01

    Part of a project to investigate the physics and chemistry of alternative fuels in internal combustion engines is reported. Coherent anti-Stokes Raman spectroscopy (CARS) is used to probe the fuel-air mixture in the cylinder of a Richardo E6 variable compression ratio research engine. The laser system comprises a passively Q- switched single-longitudinal-mode frequency-doubled Nd:YAG laser and a broadband dye laser, both with a pulse length of 15 ns. A crankshaft encoder and electronic delay are used to fire the lasers at specified times during the engine cycle, and CARS spectra are acquired using a 0.75 m spectrometer and a 1024 optical multichannel analyzer. Because of the uncertainties associated with collisional narrowing in the theoretical modeling of high-pressure CARS spectra, temperatures are determined by comparing the engine spectra with a library of experimental CARS spectra from a calibrated high-pressure, high- temperature cell. This purely experimental technique is shown to be superior to two theoretical models under the considered conditions, giving temperatures during the compression stroke of the engine with standard deviations of typically 10 K and a possible systematic error of 15 K. Together with pressure records, this information is used as input data for chemical kinetic modeling of the combustion process.

  9. Theory of coherent Stark nonlinear spectroscopy in a three-level system

    International Nuclear Information System (INIS)

    Loiko, Yurii; Serrat, Carles

    2007-01-01

    Coherent Stark nonlinear spectroscopy (CSNS) is a spectroscopic tool based on the cancellation of the phase sensitivity at frequency 5ω in the ultrafast four-wave mixing (FWM) of two-color pulses with frequencies ω and 3ω. We develop a theory for CSNS in three-level V-type systems, and reveal that the mechanism for the phase sensitivity at 5ω is the quantum interference between the two primary paths in the FWM of the ω and 3ω fields. We find that the cancellation phenomenon occurs when the probability amplitude of one of these two primary pathways becomes equal to zero due to the competition effect between the two allowed transitions in the V-type system. The analytical expressions that describe the phase-sensitivity phenomenon and the conditions for its cancellation have been derived on the basis of perturbation theory, and are confirmed by numerical integration of the density matrix and Maxwell equations. We argue that CSNS can be utilized, in particular, for the investigation of optically dense media

  10. Nonequilibrium Supersonic Freestream Studied Using Coherent Anti-Stokes Raman Spectroscopy

    Science.gov (United States)

    Cutler, Andrew D.; Cantu, Luca M.; Gallo, Emanuela C. A.; Baurle, Rob; Danehy, Paul M.; Rockwell, Robert; Goyne, Christopher; McDaniel, Jim

    2015-01-01

    Measurements were conducted at the University of Virginia Supersonic Combustion Facility of the flow in a constant-area duct downstream of a Mach 2 nozzle. The airflow was heated to approximately 1200 K in the facility heater upstream of the nozzle. Dual-pump coherent anti-Stokes Raman spectroscopy was used to measure the rotational and vibrational temperatures of N2 and O2 at two planes in the duct. The expectation was that the vibrational temperature would be in equilibrium, because most scramjet facilities are vitiated air facilities and are in vibrational equilibrium. However, with a flow of clean air, the vibrational temperature of N2 along a streamline remains approximately constant between the measurement plane and the facility heater, the vibrational temperature of O2 in the duct is about 1000 K, and the rotational temperature is consistent with the isentropic flow. The measurements of N2 vibrational temperature enabled cross-stream nonuniformities in the temperature exiting the facility heater to be documented. The measurements are in agreement with computational fluid dynamics models employing separate lumped vibrational and translational/rotational temperatures. Measurements and computations are also reported for a few percent steam addition to the air. The effect of the steam is to bring the flow to thermal equilibrium, also in agreement with the computational fluid dynamics.

  11. Molecular couplings and energy exchange between DNA and water mapped by femtosecond infrared spectroscopy of backbone vibrations

    Directory of Open Access Journals (Sweden)

    Yingliang Liu

    2017-07-01

    Full Text Available Molecular couplings between DNA and water together with the accompanying processes of energy exchange are mapped via the ultrafast response of DNA backbone vibrations after OH stretch excitation of the water shell. Native salmon testes DNA is studied in femtosecond pump-probe experiments under conditions of full hydration and at a reduced hydration level with two water layers around the double helix. Independent of their local hydration patterns, all backbone vibrations in the frequency range from 940 to 1120 cm–1 display a quasi-instantaneous reshaping of the spectral envelopes of their fundamental absorption bands upon excitation of the water shell. The subsequent reshaping kinetics encompass a one-picosecond component, reflecting the formation of a hot ground state of the water shell, and a slower contribution on a time scale of tens of picoseconds. Such results are benchmarked by measurements with resonant excitation of the backbone modes, resulting in distinctly different absorption changes. We assign the fast changes of DNA absorption after OH stretch excitation to structural changes in the water shell which couple to DNA through the local electric fields. The second slower process is attributed to a flow of excess energy from the water shell into DNA, establishing a common heated ground state in the molecular ensemble. This interpretation is supported by theoretical calculations of the electric fields exerted by the water shell at different temperatures.

  12. Debris of potassium–magnesium silicate glass generated by femtosecond laser-induced ablation in air: An analysis by near edge X-ray absorption spectroscopy, micro Raman and energy dispersive X-ray spectroscopy

    International Nuclear Information System (INIS)

    Grehn, M.; Seuthe, T.; Reinhardt, F.; Höfner, M.; Griga, N.; Eberstein, M.; Bonse, J.

    2014-01-01

    The redeposited material (debris) resulting from ablation of a potassium–magnesium silicate glass upon scanning femtosecond laser pulse irradiation (130 fs, 800 nm) in air environment is investigated by means of three complementary surface analytical methods. Changes in the electronic band structure of the glass constituent Magnesium (Mg) were identified by X-ray Absorption Near Edge Structure spectroscopy (XANES) using synchrotron radiation. An up-shift of ≈0.8 eV of a specific Magnesium K-edge absorption peak in the spectrum of the redeposited material along with a significant change in its leading edge position was detected. In contrast, the surface left after laser ablation exhibits a downshift of the peak position by ≈0.9 eV. Both observations may be related to a change of the Mg coordinative state of the laser modified/redeposited glass material. The presence of carbon in the debris is revealed by micro Raman spectroscopy (μ-RS) and was confirmed by energy dispersive X-ray spectroscopy (EDX). These observations are attributed to structural changes and chemical reactions taking place during the ablation process.

  13. Ultrafast optical responses of {beta}-carotene and lycopene probed by sub-20-fs time-resolved coherent spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Fujiwara, M.; Sugisaki, M. [CREST-JST and Department of Physics, Osaka City University, Osaka 558-8585 (Japan); Gall, A.; Robert, B. [CEA, Institut de Biologie et Technologies de Saclay, and CNRS, Gif-sur-Yvette F-91191 (France); Cogdell, R.J. [IBLS, Glasgow Biomedical Research Centre, University of Glasgow, Glasgow G12 8QQ, Scotland (United Kingdom); Hashimoto, H., E-mail: hassy@sci.osaka-cu.ac.j [CREST-JST and Department of Physics, Osaka City University, Osaka 558-8585 (Japan)

    2009-12-15

    We investigate how structural distortions in carotenoid cause decoherences of its high-frequency vibrational modes by applying the sub-20-fs time-resolved transient grating spectroscopy to {beta}-carotene and lycopene. The results indicate that the C=C central stretching mode shows significant loss of coherence under the effects of the steric hindrance between {beta}-ionone ring and polyene backbone, whereas the other high-frequency modes do not show such dependency on the structural distortions.

  14. Ultrafast optical responses of β-carotene and lycopene probed by sub-20-fs time-resolved coherent spectroscopy

    International Nuclear Information System (INIS)

    Fujiwara, M.; Sugisaki, M.; Gall, A.; Robert, B.; Cogdell, R.J.; Hashimoto, H.

    2009-01-01

    We investigate how structural distortions in carotenoid cause decoherences of its high-frequency vibrational modes by applying the sub-20-fs time-resolved transient grating spectroscopy to β-carotene and lycopene. The results indicate that the C=C central stretching mode shows significant loss of coherence under the effects of the steric hindrance between β-ionone ring and polyene backbone, whereas the other high-frequency modes do not show such dependency on the structural distortions.

  15. In-Situ Probing Plasmonic Energy Transfer in Cu(In, Ga)Se2 Solar Cells by Ultrabroadband Femtosecond Pump-Probe Spectroscopy.

    Science.gov (United States)

    Chen, Shih-Chen; Wu, Kaung-Hsiung; Li, Jia-Xing; Yabushita, Atsushi; Tang, Shih-Han; Luo, Chih Wei; Juang, Jenh-Yih; Kuo, Hao-Chung; Chueh, Yu-Lun

    2015-12-18

    In this work, we demonstrated a viable experimental scheme for in-situ probing the effects of Au nanoparticles (NPs) incorporation on plasmonic energy transfer in Cu(In, Ga)Se2 (CIGS) solar cells by elaborately analyzing the lifetimes and zero moment for hot carrier relaxation with ultrabroadband femtosecond pump-probe spectroscopy. The signals of enhanced photobleach (PB) and waned photoinduced absorption (PIA) attributable to surface plasmon resonance (SPR) of Au NPs were in-situ probed in transient differential absorption spectra. The results suggested that substantial carriers can be excited from ground state to lower excitation energy levels, which can reach thermalization much faster with the existence of SPR. Thus, direct electron transfer (DET) could be implemented to enhance the photocurrent of CIGS solar cells. Furthermore, based on the extracted hot carrier lifetimes, it was confirmed that the improved electrical transport might have been resulted primarily from the reduction in the surface recombination of photoinduced carriers through enhanced local electromagnetic field (LEMF). Finally, theoretical calculation for resonant energy transfer (RET)-induced enhancement in the probability of exciting electron-hole pairs was conducted and the results agreed well with the enhanced PB peak of transient differential absorption in plasmonic CIGS film. These results indicate that plasmonic energy transfer is a viable approach to boost high-efficiency CIGS solar cells.

  16. Femtosecond Laser Fabricated Ag@Au and Cu@Au Alloy Nanoparticles for Surface Enhanced Raman Spectroscopy Based Trace Explosives Detection

    Directory of Open Access Journals (Sweden)

    Moram Sree Satya Bharati

    2018-03-01

    Full Text Available Herein we present results from our detailed studies on the fabrication of Ag@Au and Cu@Au alloy nanoparticles (NPs using the femtosecond laser ablation in liquid technique. The NPs were obtained by ablating the pure Ag, Cu targets (bulk in HAuCl4 (5 mM solution. The absorption properties of the obtained NPs colloids were characterized using UV-Visible absorption spectrometer and their size, shape, and crystallinity were investigated using the XRD, FESEM and TEM techniques. The fabricated NPs were utilized for sensing of explosive molecules such as 2,4,6-trinitrophenol (PA, 2,4-dinitrotoluene (DNT and a common dye methylene blue (MB using the surface enhanced Raman spectroscopy (SERS technique. The detection limit in terms of weight was as low as few nano-grams in the case of nitroaromatic explosive compounds (PA, DNT and few picograms in the case of a common dye molecule (MB. Typical enhancement factors achieved were estimated to be ~104, ~105, and ~107, respectively, for PA, DNT, and MB. The significance of the present work lies in exploring the performance of the prepared NPs being used as SERS substrates for explosives detection using a portable Raman instrument. Such capability enables one to carry the spectrometer to the point of interest in the field and evaluate any hazardous samples within a short period of time.

  17. Primary processes of the electron-protic species coupling in pure aqueous phases: - femtosecond laser spectroscopy study; - quantum approach of the electron-water interaction

    International Nuclear Information System (INIS)

    Pommeret, Stanislas

    1991-01-01

    This thesis work deals with the coupling mechanisms between an electron, water molecules or protic species (hydronium ion, hydroxyl radical). Two complementary studies have been carry out in pure aqueous phases. The first one is concerned with the structural aspect of the hydrated electron which is studied via a semi-quantum approach Splitting Operator Method. The results indicates the importance of the second hydration shell in the localisation of an electron at 77 and 300 Kelvin. The second part of this work relates to the dynamic of the primary processes in light or heavy water at room temperature: the ion-molecule reaction, radical pair formation, geminate recombination of the hydrated electron with the hydronium ion and the hydroxyl radical. The dynamic of these reactions is studied by time resolved absorption spectroscopy from the near infrared to the near ultraviolet with a few tens femto-seconds temporal precision. The analysis of the primary processes takes into account the protic properties of water molecules. (author) [fr

  18. Dynamics of Charged Excitons and Biexcitons in CsPbBr3 Perovskite Nanocrystals Revealed by Femtosecond Transient-Absorption and Single-Dot Luminescence Spectroscopy.

    Science.gov (United States)

    Yarita, Naoki; Tahara, Hirokazu; Ihara, Toshiyuki; Kawawaki, Tokuhisa; Sato, Ryota; Saruyama, Masaki; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

    2017-04-06

    Metal-halide perovskite nanocrystals (NCs) are promising photonic materials for use in solar cells, light-emitting diodes, and lasers. The optoelectronic properties of these devices are determined by the excitons and exciton complexes confined in their NCs. In this study, we determined the relaxation dynamics of charged excitons and biexcitons in CsPbBr 3 NCs using femtosecond transient-absorption (TA), time-resolved photoluminescence (PL), and single-dot second-order photon correlation spectroscopy. Decay times of ∼40 and ∼200 ps were obtained from the TA and PL decay curves for biexcitons and charged excitons, respectively, in NCs with an average edge length of 7.7 nm. The existence of charged excitons even under weak photoexcitation was confirmed by the second-order photon correlation measurements. We found that charged excitons play a dominant role in luminescence processes of CsPbBr 3 NCs. Combining different spectroscopic techniques enabled us to clarify the dynamical behaviors of excitons, charged excitons, and biexcitons.

  19. One-, two- and three-photon spectroscopy of π-conjugated dendrimers: cooperative enhancement and coherent domains

    International Nuclear Information System (INIS)

    Drobizhev, M.; Rebane, A.; Suo, Z.; Spangler, C.W.

    2005-01-01

    We use wavelength tunable femtosecond pulses to measure intrinsic (simultaneous) two-photon absorption (2PA) and three-photon absorption (3PA) molecular cross section in two series of π-conjugated dendrimers built of identical 4,4'-bis(diphenylamino) stilbene (BDPAS) and 4,4'-bis(diphenylamino) distyrylbenzene (BDPADSB) repeat units. Record large 2PA cross sections, σ 2 =10 -46 cm 4 s are obtained for the largest second-generation BDPAS-based dendrimer, as well as zeroth-generation 4-arm BDPADSB-based dendrimer. In both series, maximum 2PA cross section increases nonlinearly with the number of π-electrons, whereas for higher generations this dependence turns to linear one. 3PA cross section also increases nonlinearly with the size of the system in the series of BDPAS-based molecules, amounting a record large value, σ 3 =10 -79 cm 6 s 2 , for the largest, second-generation dendrimer. We interpret these results in terms of direct inter-branch conjugation, which facilitates cooperative enhancement of the nonlinear-optical response. We propose a simple model which allows us to determine the effective size of coherent domains (extent of conjugation), which, in turn, determines the optimum dendrimer size for most efficient nonlinear response

  20. Multi-modal approach using Raman spectroscopy and optical coherence tomography for the discrimination of colonic adenocarcinoma from normal colon

    Science.gov (United States)

    Ashok, Praveen C.; Praveen, Bavishna B.; Bellini, Nicola; Riches, Andrew; Dholakia, Kishan; Herrington, C. Simon

    2013-01-01

    We report a multimodal optical approach using both Raman spectroscopy and optical coherence tomography (OCT) in tandem to discriminate between colonic adenocarcinoma and normal colon. Although both of these non-invasive techniques are capable of discriminating between normal and tumour tissues, they are unable individually to provide both the high specificity and high sensitivity required for disease diagnosis. We combine the chemical information derived from Raman spectroscopy with the texture parameters extracted from OCT images. The sensitivity obtained using Raman spectroscopy and OCT individually was 89% and 78% respectively and the specificity was 77% and 74% respectively. Combining the information derived using the two techniques increased both sensitivity and specificity to 94% demonstrating that combining complementary optical information enhances diagnostic accuracy. These data demonstrate that multimodal optical analysis has the potential to achieve accurate non-invasive cancer diagnosis. PMID:24156073

  1. Laser Spectroscopy and Frequency Combs

    International Nuclear Information System (INIS)

    Hänsch, Theodor W; Picqué, Nathalie

    2013-01-01

    The spectrum of a frequency comb, commonly generated by a mode-locked femtosecond laser consists of several hundred thousand precisely evenly spaced spectral lines. Such laser frequency combs have revolutionized the art measuring the frequency of light, and they provide the long-missing clockwork for optical atomic clocks. The invention of the frequency comb technique has been motivated by precision laser spectroscopy of the simple hydrogen atom. The availability of commercial instruments is facilitating the evolution of new applications far beyond the original purpose. Laser combs are becoming powerful instruments for broadband molecular spectroscopy by dramatically improving the resolution and recording speed of Fourier spectrometers and by creating new opportunities for highly multiplexed nonlinear spectroscopy, such as two-photon spectroscopy or coherent Raman spectroscopy. Other emerging applications of frequency combs range from fundamental research in astronomy, chemistry, or attosecond science to telecommunications and satellite navigation

  2. Two-pulse atomic coherent control spectroscopy of Eley-Rideal reactions: An application of an atom laser

    International Nuclear Information System (INIS)

    Joergensen, Solvejg; Kosloff, Ronnie

    2003-01-01

    A spectroscopic application of the atom laser is suggested. The spectroscopy termed 2PACC (two-pulse atomic coherent control) employs the coherent properties of matter waves from a two-pulse atom laser. These waves are employed to control a gas-surface chemical recombination reaction. The method is demonstrated for an Eley-Rideal reaction of a hydrogen or alkali atom-laser pulse where the surface target is an adsorbed hydrogen atom. The reaction yields either a hydrogen or alkali hydride molecule. The desorbed gas-phase molecular yield and its internal state is shown to be controlled by the time and phase delay between two atom-laser pulses. The calculation is based on solving the time-dependent Schroedinger equation in a diabatic framework. The probability of desorption which is the predicted 2PACC signal has been calculated as a function of the pulse parameters

  3. Broadband pump-probe spectroscopy with sub-10-fs resolution for probing ultrafast internal conversion and coherent phonons in carotenoids

    International Nuclear Information System (INIS)

    Polli, D.; Antognazza, M.R.; Brida, D.; Lanzani, G.; Cerullo, G.; De Silvestri, S.

    2008-01-01

    We use pump-probe spectroscopy with broadband detection to study electronic energy relaxation and coherent vibrational dynamics in carotenoids. A fast optical multichannel analyzer combined with a non-collinear optical parametric amplifier allows simultaneous acquisition of the differential transmission dynamics on the 500-700 nm wavelength range with sub-10-fs temporal resolution. The broad spectral coverage enables on the one hand a detailed study of the ultrafast bright-to-dark state internal conversion process; on the other hand, the tracking of the motion of the vibrational wavepacket launched on the ground state multidimensional potential energy surface. We present results on all-trans β-carotene and on a long-chain polyene in solution. The developed experimental setup enables the straightforward acquisition and analysis of coherent vibrational dynamics, highlighting time-frequency domain features with extreme resolution

  4. Resonance laser-plasma excitation of coherent terahertz phonons in the bulk of fluorine-bearing crystals under high-intensity femtosecond laser irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Potemkin, F V; Mareev, E I [International Laser Center, M. V. Lomonosov Moscow State University, Moscow (Russian Federation); Khodakovskii, N G [A M Prokhorov General Physics Institute, Russian Academy of Sciences, Moscow (Russian Federation); Mikheev, P M

    2013-08-31

    The dynamics of coherent phonons in fluorine-containing crystals was investigated by pump-probe technique in the plasma production regime. Several phonon modes, whose frequencies are overtones of the 0.38-THz fundamental frequency, were simultaneously observed in a lithium fluoride crystal. Phonons with frequencies of 1 and 0.1 THz were discovered in a calcium fluoride crystal and coherent phonons with frequencies of 1 THz and 67 GHz were observed in a barium fluoride crystal. Furthermore, in the latter case the amplitudes of phonon mode oscillations were found to significantly increase 15 ps after laser irradiation. (interaction of laser radiation with matter)

  5. Femtosecond X-ray magnetic circular dichroism absorption spectroscopy at an X-ray free electron laser

    Energy Technology Data Exchange (ETDEWEB)

    Higley, Daniel J., E-mail: dhigley@stanford.edu; Yuan, Edwin [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Department of Applied Physics, Stanford University, Stanford, California 94305 (United States); Hirsch, Konstantin; Dakovski, Georgi L.; Jal, Emmanuelle; Lutman, Alberto A.; Coslovich, Giacomo; Hart, Philip; Hoffmann, Matthias C.; Mitra, Ankush; Moeller, Stefan; Ohldag, Hendrik; Seaberg, Matthew; Stöhr, Joachim; Nuhn, Heinz-Dieter; Reid, Alex H.; Dürr, Hermann A.; Schlotter, William F. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Liu, Tianmin; MacArthur, James P. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Department of Physics, Stanford University, Stanford, California 94305 (United States); and others

    2016-03-15

    X-ray magnetic circular dichroism spectroscopy using an X-ray free electron laser is demonstrated with spectra over the Fe L{sub 3,2}-edges. The high brightness of the X-ray free electron laser combined with high accuracy detection of incident and transmitted X-rays enables ultrafast X-ray magnetic circular dichroism studies of unprecedented sensitivity. This new capability is applied to a study of all-optical magnetic switching dynamics of Fe and Gd magnetic sublattices in a GdFeCo thin film above its magnetization compensation temperature.

  6. Ultrafast photo-induced nuclear relaxation of a conformationally disordered conjugated polymer probed with transient absorption and femtosecond stimulated Raman spectroscopies

    Energy Technology Data Exchange (ETDEWEB)

    Yu, Wenjian; Donohoo-Vallett, Paul J.; Zhou, Jiawang; Bragg, Arthur E., E-mail: artbragg@jhu.edu [Department of Chemistry, Johns Hopkins University, 3400 N. Charles St., Baltimore, Maryland 21218 (United States)

    2014-07-28

    A combination of transient absorption (TAS) and femtosecond stimulated Raman (FSRS) spectroscopies were used to interrogate the photo-induced nuclear relaxation dynamics of poly(3-cyclohexyl,4-methylthiophene) (PCMT). The large difference in inter-ring dihedral angles of ground and excited-state PCMT make it an ideal candidate for studying large-amplitude vibrational relaxation associated with exciton trapping. Spectral shifting in the S{sub 1} TA spectra on sub-ps timescales (110 ± 20 and 800 ± 100 fs) is similar to spectroscopic signatures of excited-state relaxation observed with related photoexcited conjugated polymers and which have been attributed to exciton localization and a combination of resonant energy transfer and torsional relaxation, respectively. Measurements made with both techniques reveal fast PCMT S{sub 1} decay and triplet formation (τ{sub S1} = 25–32 ps), which is similar to the excited-state dynamics of short oligothiophenes and highly twisted polyconjugated molecules. On ultrafast timescales FSRS of S{sub 1} PCMT offers a new perspective on the nuclear dynamics that underlie localization of excitons in photoexcited conjugated polymers: Spectral dynamics in the C=C stretching region (1400–1600 cm{sup −1}) include a red-shift of the in-phase C=C stretching frequency, as well as a change in the relative intensity of in-phase and out-of-phase stretch intensities on a timescale of ∼100 fs. Both changes indicate an ultrafast vibrational distortion that increases the conjugation length in the region of the localized excitation and are consistent with exciton self-localization or trapping. Wavelength-dependent excited-state FSRS measurements further demonstrate that the C=C stretching frequency provides a useful spectroscopic handle for interrogating the degree of delocalization in excited conjugated polymers given the selectivity achieved via resonance enhancement.

  7. Study of the Bulk Charge Carrier Dynamics in Anatase and Rutile TiO2 Single Crystals by Femtosecond Time Resolved Spectroscopy

    KAUST Repository

    Maity, Partha

    2018-04-02

    Understanding of the fundamentals behind charge carriers of photo-catalytic materials are still illusive hindering progress in our quest for renewable energy. TiO2 anatase and rutile are the most understood phases in photo-catalysis and serve as the best model for fundamental studies. Their ultrafast charge carrier dynamics especially on TiO2 anatase single crystal (the most active phase) are unresolved. Here femtosecond time resolved spectroscopy (TRS) was carried out to explore the dynamics of photo-excited charge carriers’ recombination in anatase single crystal, for the first time using pump fluence effects, and compares it to that of the rutile single crystal. A significant difference in charge carrier recombination rates between both crystals is observed. We found that the time constants for carrier recombination are two orders of magnitude slower for anatase (101) when compared to those of rutile (110). Moreover, bulk defects introduced by reduction of the samples via annealing in ultra-high vacuum resulted in faster recombination rates for both polymorphs. Both states (fresh and reduced) probed by pump fluence dependence measurements revealed that the major recombination channel in fresh and reduced anatase and reduced rutile is the first-order Shockley–Reed mediated. However, for fresh rutile, third-body Auger recombination was observed, attributed to the presence of higher density of intrinsic charge carriers. At all excitation wavelengths and fluence investigated, anatase (101) single crystal show longer charge carrier lifetime when compared to rutile (110) single. This may explain the superiority of the anatase phase for the electron transfer H+ reduction to molecular hydrogen.

  8. Femtosecond and Subfemtosecond X-Ray Pulses from a SASE Based Free-Electron Laser

    Energy Technology Data Exchange (ETDEWEB)

    Emma, P

    2004-03-10

    We propose a novel method to generate femtosecond and sub-femtosecond photon pulses in a free electron laser by selectively spoiling the transverse emittance of the electron beam. Its merits are simplicity and ease of implementation. When the system is applied to the Linac Coherent Light Source, it can provide x-ray pulses the order of 1 femtosecond in duration containing about 1010 transversely coherent photons.

  9. Generation of Femtosecond Electron and Photon Pulses

    CERN Document Server

    Thongbai, Chitrlada; Kangrang, Nopadol; Kusoljariyakul, Keerati; Rhodes, Michael W; Rimjaem, Sakhorn; Saisut, Jatuporn; Vilaithong, Thiraphat; Wichaisirimongkol, Pathom; Wiedemann, Helmut

    2005-01-01

    Femtosecond electron and photon pulses become a tool of interesting important to study dynamics at molecular or atomic levels. Such short pulses can be generated from a system consisting of an RF-gun with a thermionic cathode, an alpha magnet as a magnetic bunch compressor, and a linear accelerator. The femtosecond electron pulses can be used directly or used as sources to produce electromagnetic radiation of equally short pulses by choosing certain kind of radiation pruduction processes. At the Fast Neutron Research Facility (Thailand), we are especially interested in production of radiation in Far-infrared and X-ray regime. In the far-infrared wavelengths which are longer than the femtosecond pulse length, the radiation is emitted coherently producing intense radiation. In the X-ray regime, development of femtosecond X-ray source is crucial for application in ultrafast science.

  10. Detection of Intramolecular Charge Transfer and Dynamic Solvation in Eosin B by Femtosecond Two-Dimensional Electronic Spectroscopy

    Science.gov (United States)

    Ghosh, Soumen; Roscioli, Jerome D.; Beck, Warren F.

    2014-06-01

    We have employed 2D electronic photon echo spectroscopy to study intramolecular charge-transfer dynamics in eosin B. After preparation of the first excited singlet state (S_1) with 40-fs excitation pulses at 520 nm, the nitro group (--NO_2) in eosin B undergoes excited state torsional motion towards a twisted intramolecular charge transfer (TICT) state. As the viscosity of the surrounding solvent increases, the charge-transfer rate decreases because the twisting of the --NO_2 group is hindered. These conclusions are supported by the time evolution of the 2D spectrum, which provides a direct measure of the the ground-to-excited-state energy gap time-correlation function, M(t). In comparison to the inertial and diffusive solvation time scales exhibited by eosin Y, which lacks the nitro group, the M(t) function for eosin B exhibits under the same conditions an additional component on the 150-fs timescale that arises from quenching of the S_1 state by crossing to the TICT state. These results indicate that 2D electronic spectroscopy can be used as a sensitive probe of the rate of charge transfer in a molecular system and of the coupling to the motions of the surrounding solvent. (Supported by grant DE-SC0010847 from the Department of Energy, Office of Basic Energy Sciences, Photosynthetic Systems program.)

  11. Distortion dependent intersystem crossing: A femtosecond time-resolved photoelectron spectroscopy study of benzene, toluene, and p-xylene

    Directory of Open Access Journals (Sweden)

    Anne B. Stephansen

    2017-07-01

    Full Text Available The competition between ultrafast intersystem crossing and internal conversion in benzene, toluene, and p-xylene is investigated with time-resolved photoelectron spectroscopy and quantum chemical calculations. By exciting to S2 out-of-plane symmetry breaking, distortions are activated at early times whereupon spin-forbidden intersystem crossing becomes (partly allowed. Natural bond orbital analysis suggests that the pinnacle carbon atoms distorting from the aromatic plane change hybridization between the planar Franck-Condon geometry and the deformed (boat-shaped S2 equilibrium geometry. The effect is observed to increase in the presence of methyl-groups on the pinnacle carbon-atoms, where largest extents of σ and π orbital-mixing are observed. This is fully consistent with the time-resolved spectroscopy data: Toluene and p-xylene show evidence for ultrafast triplet formation competing with internal conversion, while benzene appears to only decay via internal conversion within the singlet manifold. For toluene and p-xylene, internal conversion to S1 and intersystem crossing to T3 occur within the time-resolution of our instrument. The receiver triplet state (T3 is found to undergo internal conversion in the triplet manifold within ≈100–150 fs (toluene or ≈180–200 fs (p-xylene as demonstrated by matching rise and decay components of upper and lower triplet states. Overall, the effect of methylation is found to both increase the intersystem crossing probability and direct the molecular axis of the excited state dynamics.

  12. Ultrafast Carrier Trapping of a Metal-Doped Titanium Dioxide Semiconductor Revealed by Femtosecond Transient Absorption Spectroscopy

    KAUST Repository

    Sun, Jingya; Yang, Yang; Khan, Jafar I.; Alarousu, Erkki; Guo, Zaibing; Zhang, Xixiang; Zhang, Qiang; Mohammed, Omar F.

    2014-01-01

    We explored for the first time the ultrafast carrier trapping of a metal-doped titanium dioxide (TiO2) semiconductor using broad-band transient absorption (TA) spectroscopy with 120 fs temporal resolution. Titanium dioxide was successfully doped layer-by-layer with two metal ions, namely tungsten and cobalt. The time-resolved data demonstrate clearly that the carrier trapping time decreases progressively as the doping concentration increases. A global-fitting procedure for the carrier trapping suggests the appearance of two time components: a fast one that is directly associated with carrier trapping to the defect state in the vicinity of the conduction band and a slow one that is attributed to carrier trapping to the deep-level state from the conduction band. With a relatively long doping deposition time on the order of 30 s, a carrier lifetime of about 1 ps is obtained. To confirm that the measured ultrafast carrier dynamics are associated with electron trapping by metal doping, we explored the carrier dynamics of undoped TiO2. The findings reported here may be useful for the implementation of high-speed optoelectronic applications and fast switching devices.

  13. Ultrafast Carrier Trapping of a Metal-Doped Titanium Dioxide Semiconductor Revealed by Femtosecond Transient Absorption Spectroscopy

    KAUST Repository

    Sun, Jingya

    2014-06-11

    We explored for the first time the ultrafast carrier trapping of a metal-doped titanium dioxide (TiO2) semiconductor using broad-band transient absorption (TA) spectroscopy with 120 fs temporal resolution. Titanium dioxide was successfully doped layer-by-layer with two metal ions, namely tungsten and cobalt. The time-resolved data demonstrate clearly that the carrier trapping time decreases progressively as the doping concentration increases. A global-fitting procedure for the carrier trapping suggests the appearance of two time components: a fast one that is directly associated with carrier trapping to the defect state in the vicinity of the conduction band and a slow one that is attributed to carrier trapping to the deep-level state from the conduction band. With a relatively long doping deposition time on the order of 30 s, a carrier lifetime of about 1 ps is obtained. To confirm that the measured ultrafast carrier dynamics are associated with electron trapping by metal doping, we explored the carrier dynamics of undoped TiO2. The findings reported here may be useful for the implementation of high-speed optoelectronic applications and fast switching devices.

  14. Nanoflow electrospinning serial femtosecond crystallography

    Energy Technology Data Exchange (ETDEWEB)

    Sierra, Raymond G.; Laksmono, Hartawan [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Kern, Jan [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Tran, Rosalie; Hattne, Johan [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Alonso-Mori, Roberto [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Lassalle-Kaiser, Benedikt [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Glöckner, Carina; Hellmich, Julia [Technische Universität Berlin, Strasse des 17 Juni 135, 10623 Berlin (Germany); Schafer, Donald W. [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W. [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Sellberg, Jonas [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Stockholm University, S-106 91 Stockholm (Sweden); McQueen, Trevor A. [Stanford University, Stanford, CA 94025 (United States); Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Zwart, Petrus H. [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Glatzel, Pieter [European Synchrotron Radiation Facility, Grenoble (France); Milathianaki, Despina; White, William E. [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Adams, Paul D. [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Williams, Garth J.; Boutet, Sébastien [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Zouni, Athina [Technische Universität Berlin, Strasse des 17 Juni 135, 10623 Berlin (Germany); Messinger, Johannes [Umeå Universitet, Umeå (Sweden); Sauter, Nicholas K. [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Bergmann, Uwe [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); Yano, Junko; Yachandra, Vittal K. [Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States); Bogan, Michael J., E-mail: mbogan@slac.stanford.edu [SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States); SLAC National Accelerator Laboratory, Menlo Park, CA 94025 (United States)

    2012-11-01

    A low flow rate liquid microjet method for delivery of hydrated protein crystals to X-ray lasers is presented. Linac Coherent Light Source data demonstrates serial femtosecond protein crystallography with micrograms, a reduction of sample consumption by orders of magnitude. An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min{sup −1} to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min{sup −1} and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption.

  15. Nanoflow electrospinning serial femtosecond crystallography

    International Nuclear Information System (INIS)

    Sierra, Raymond G.; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W.; Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W.; Sellberg, Jonas; McQueen, Trevor A.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H.; Glatzel, Pieter; Milathianaki, Despina; White, William E.; Adams, Paul D.; Williams, Garth J.; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K.; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K.; Bogan, Michael J.

    2012-01-01

    A low flow rate liquid microjet method for delivery of hydrated protein crystals to X-ray lasers is presented. Linac Coherent Light Source data demonstrates serial femtosecond protein crystallography with micrograms, a reduction of sample consumption by orders of magnitude. An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min −1 to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min −1 and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption

  16. Atomic and molecular spectroscopy with optical-frequency-comb-referenced IR coherent sources

    International Nuclear Information System (INIS)

    Cancio, P.; Bartalini, S.; De Rosa, M.; Giusfredi, G.; Mazzotti, D.; Maddaloni, P.; Vitiello, M. S.; De Natale, P.

    2013-01-01

    We provide a review of progress in the development of metrological-grade measurements in atomic and molecular systems through the extension, in the mid-infrared and far-infrared range, of optical frequency combs (OFCs) and the introduction of new techniques and highly coherent sources. (authors)

  17. Observation and control of coherent torsional dynamics in a quinquethiophene molecule.

    Science.gov (United States)

    Cirmi, Giovanni; Brida, Daniele; Gambetta, Alessio; Piacenza, Manuel; Della Sala, Fabio; Favaretto, Laura; Cerullo, Giulio; Lanzani, Guglielmo

    2010-07-28

    By applying femtosecond pump-probe spectroscopy to a substituted quinquethiophene molecule in solution, we observe in the time domain the coherent torsional dynamics that drives planarization of the excited state. Our interpretation is based on numerical modeling of the ground and excited state potential energy surfaces and simulation of wavepacket dynamics, which reveals two symmetric excited state deactivation pathways per oscillation period. We use the acquired knowledge on torsional dynamics to coherently control the excited state population with a pump-dump scheme, exploiting the non-stationary Franck-Condon overlap between ground and excited states.

  18. Polarization Sensitive Coherent Anti-Stokes Raman Spectroscopy of DCVJ in Doped Polymer

    Science.gov (United States)

    Ujj, Laszlo

    2014-05-01

    Coherent Raman Microscopy is an emerging technic and method to image biological samples such as living cells by recording vibrational fingerprints of molecules with high spatial resolution. The race is on to record the entire image during the shortest time possible in order to increase the time resolution of the recorded cellular events. The electronically enhanced polarization sensitive version of Coherent anti-Stokes Raman scattering is one of the method which can shorten the recording time and increase the sharpness of an image by enhancing the signal level of special molecular vibrational modes. In order to show the effectiveness of the method a model system, a highly fluorescence sample, DCVJ in a polymer matrix is investigated. Polarization sensitive resonance CARS spectra are recorded and analyzed. Vibrational signatures are extracted with model independent methods. Details of the measurements and data analysis will be presented. The author gratefully acknowledge the UWF for financial support.

  19. Method and system to measure temperature of gases using coherent anti-stokes doppler spectroscopy

    Science.gov (United States)

    Rhodes, Mark

    2013-12-17

    A method of measuring a temperature of a noble gas in a chamber includes providing the noble gas in the chamber. The noble gas is characterized by a pressure and a temperature. The method also includes directing a first laser beam into the chamber and directing a second laser beam into the chamber. The first laser beam is characterized by a first frequency and the second laser beam is characterized by a second frequency. The method further includes converting at least a portion of the first laser beam and the second laser beam into a coherent anti-Stokes beam, measuring a Doppler broadening of the coherent anti-Stokes beam, and computing the temperature using the Doppler broadening.

  20. Quantum coherence spectroscopy reveals complex dynamics in bacterial light-harvesting complex 2 (LH2).

    Science.gov (United States)

    Harel, Elad; Engel, Gregory S

    2012-01-17

    Light-harvesting antenna complexes transfer energy from sunlight to photosynthetic reaction centers where charge separation drives cellular metabolism. The process through which pigments transfer excitation energy involves a complex choreography of coherent and incoherent processes mediated by the surrounding protein and solvent environment. The recent discovery of coherent dynamics in photosynthetic light-harvesting antennae has motivated many theoretical models exploring effects of interference in energy transfer phenomena. In this work, we provide experimental evidence of long-lived quantum coherence between the spectrally separated B800 and B850 rings of the light-harvesting complex 2 (LH2) of purple bacteria. Spectrally resolved maps of the detuning, dephasing, and the amplitude of electronic coupling between excitons reveal that different relaxation pathways act in concert for optimal transfer efficiency. Furthermore, maps of the phase of the signal suggest that quantum mechanical interference between different energy transfer pathways may be important even at ambient temperature. Such interference at a product state has already been shown to enhance the quantum efficiency of transfer in theoretical models of closed loop systems such as LH2.

  1. High-resolution x-ray spectroscopy of coherent bremsstrahlung fine structure

    International Nuclear Information System (INIS)

    Lund, M.W.

    1989-01-01

    The aim of this research was to provide experimental evidence for fine structure due to umklapp by distinct reciprocal lattice vectors in coherent bremsstrahlung spectra. The spontaneous emission of photons by relativistic electrons transversing thin crystals is made possible by recoil of the crystal, which absorbs momentum in multiples of ℎG where G is a reciprocal lattice vector. Previous work in the MeV-GeV beam energy range used detectors whose energy resolution was greater than 10%. By fitting a Johann wavelength dispersive spectrometer to a transmission electron microscope the author obtained coherent bremsstrahlung spectra of very high quality with energy resolution of 1%. Important to this result were also the fine angular collimation, small energy width of the electron beam in the microscope, and the accurate control of crystal orientation possible in a modern goniometer stage. The theory of the design of bent crystal x-ray spectrometers is extended to include effects of defocus and aberrations. The theory for diffraction from a stationary three dimensional grating due to a dipole radiator moving at relativistic speeds is derived as well as several other broadening mechanisms stemming from experimental variables. This dissertation provides the first experimental observations and corresponding theoretical background for the fine structure of coherent bremsstrahlung due to umklapp by different G-vectors in the same reciprocal lattice plane

  2. Recent results on solvation dynamics of electron and spur reactions of solvated electron in polar solvents studied by femtosecond laser spectroscopy and picosecond pulse radiolysis

    International Nuclear Information System (INIS)

    Mostafavi, M.

    2006-01-01

    Here, we report several studies done recently at ELYSE laboratory on the solvation dynamics of electron and on the kinetics of solvated electron in the spur reactions, performed by femtosecond laser spectroscopy and picosecond pulse radiolysis, respectively. Solvated electrons have been produced in polyol (1,2-Etanediol, 1,2-Propanediol and 1,3-Propanediol) by two-photon ionization of the solvent with 263 nm femtosecond laser pulses at room temperature. The two-photon absorption coefficient of these solvents at 263 nm has been determined. The dynamics of electron solvation in polyols has been studied by pump-probe transient absorption spectroscopy. So, time resolved absorption spectra ranging from 430 to 720 nm have been measured (Figure 1). A blue shift of the spectra is observed for the first tens of picoseconds. Using Bayesian data analysis method, the observed solvation dynamics are reconstructed with different models: stepwise mechanisms, continuous relaxation models or combinations of stepwise and continuous relaxation. That analysis clearly indicates that it is not obvious to select a unique model to describe the solvation dynamics of electron in diols. We showed that several models are able to reproduce correctly the data: a two-step model, a heterogeneous or bi-exponential continuous relaxation model and even a hybrid model with a stepwise transition and homogeneous continuous relaxation. Nevertheless, the best fits are given by the continuous spectral relaxation models. The fact that the time-evolution of the absorption spectrum of the solvated electron in diols can be accurately described by the temperature dependent absorption spectrum of the ground state solvated electron suggests that the spectral blue shift is mostly caused by the continuous relaxation of the electron trapped in a large distribution of solvent cages. Similar trends on electron solvation dynamics are observed in the cases of 1,2-ethanediol, 1,3-propanediol and 1,2 propanediol

  3. Femtosecond tunneling response of surface plasmon polaritons

    DEFF Research Database (Denmark)

    Keil, Ulrich Dieter Felix; Ha, Taekjip; Jensen, Jacob Riis

    1998-01-01

    We obtain femtosecond (200 fs) time resolution using a scanning tunneling microscope on surface plasmon polaritons (SPPs) generated by two 100 fs laser beams in total internal reflection geometry. The tunneling gap dependence of the signal clearly indicates the tunneling origin of the signal...... and suggests that nanometer spatial resolution can be obtained together with femtosecond temporal resolution. This fast response, in contrast to the picosecond decay time of SPPs revealed by differential reflectivity measurements, can be attributed to a coherent superposition of SPPs rectified at the tunneling...

  4. Femtosecond profiling of shaped x-ray pulses

    Science.gov (United States)

    Hoffmann, M. C.; Grguraš, I.; Behrens, C.; Bostedt, C.; Bozek, J.; Bromberger, H.; Coffee, R.; Costello, J. T.; DiMauro, L. F.; Ding, Y.; Doumy, G.; Helml, W.; Ilchen, M.; Kienberger, R.; Lee, S.; Maier, A. R.; Mazza, T.; Meyer, M.; Messerschmidt, M.; Schorb, S.; Schweinberger, W.; Zhang, K.; Cavalieri, A. L.

    2018-03-01

    Arbitrary manipulation of the temporal and spectral properties of x-ray pulses at free-electron lasers would revolutionize many experimental applications. At the Linac Coherent Light Source at Stanford National Accelerator Laboratory, the momentum phase-space of the free-electron laser driving electron bunch can be tuned to emit a pair of x-ray pulses with independently variable photon energy and femtosecond delay. However, while accelerator parameters can easily be adjusted to tune the electron bunch phase-space, the final impact of these actuators on the x-ray pulse cannot be predicted with sufficient precision. Furthermore, shot-to-shot instabilities that distort the pulse shape unpredictably cannot be fully suppressed. Therefore, the ability to directly characterize the x-rays is essential to ensure precise and consistent control. In this work, we have generated x-ray pulse pairs via electron bunch shaping and characterized them on a single-shot basis with femtosecond resolution through time-resolved photoelectron streaking spectroscopy. This achievement completes an important step toward future x-ray pulse shaping techniques.

  5. Two-beam ultrabroadband coherent anti-Stokes Raman spectroscopy for high resolution gas-phase multiplex imaging

    Energy Technology Data Exchange (ETDEWEB)

    Bohlin, Alexis; Kliewer, Christopher J., E-mail: cjkliew@sandia.gov [Combustion Research Facility, Sandia National Laboratories, Livermore, California 94550 (United States)

    2014-01-20

    We propose and develop a method for wideband coherent anti-Stokes Raman spectroscopy (CARS) in the gas phase and demonstrate the single-shot measurement of N{sub 2}, H{sub 2}, CO{sub 2}, O{sub 2}, and CH{sub 4}. Pure-rotational and vibrational O-, Q-, and S- branch spectra are collected simultaneously, with high spectral and spatial resolution, and within a single-laser-shot. The relative intensity of the rotational and vibrational signals can be tuned arbitrarily using polarization techniques. The ultrashort 7 fs pump and Stokes pulses are automatically overlapped temporally and spatially using a two-beam CARS technique, and the crossed probe beam allows for excellent spatial sectioning of the probed location.

  6. The Israeli EA-FEL Upgrade Towards Long Pulse Operation for Ultra-High Resolution Single Pulse Coherent Spectroscopy

    CERN Document Server

    Gover, A; Kanter, M; Kapilevich, B; Litvak, B; Peleg, S; Socol, Y; Volshonok, M

    2005-01-01

    The Israeli Electrostatic Accelerator FEL (EA-FEL) is now being upgraded towards long pulse (1005s) operation and ultra-high resolution (10(-6)) single pulse coherent spectroscopy. We present quantitative estimations regarding the applications of controlled radiation chirp for spectroscopic applications with pulse-time Fourier Transform limited spectral resolution. Additionally, we describe a novel extraction-efficiency-improving scheme based on increase of accelerating voltage (boosting) after saturation is achieved. The efficiency of the proposed scheme is confirmed by theoretical and numerical calculations. The latter are performed using software, based on 3D space-frequency domain model. The presentation provides an overview of the upgrade status: the high-voltage terminal is being reconfigured to accept the accelerating voltage boost system; a new broad band low-loss resonator is being manufactured; multi-stage depressed collector is assembled.

  7. Two-beam ultrabroadband coherent anti-Stokes Raman spectroscopy for high resolution gas-phase multiplex imaging

    International Nuclear Information System (INIS)

    Bohlin, Alexis; Kliewer, Christopher J.

    2014-01-01

    We propose and develop a method for wideband coherent anti-Stokes Raman spectroscopy (CARS) in the gas phase and demonstrate the single-shot measurement of N 2 , H 2 , CO 2 , O 2 , and CH 4 . Pure-rotational and vibrational O-, Q-, and S- branch spectra are collected simultaneously, with high spectral and spatial resolution, and within a single-laser-shot. The relative intensity of the rotational and vibrational signals can be tuned arbitrarily using polarization techniques. The ultrashort 7 fs pump and Stokes pulses are automatically overlapped temporally and spatially using a two-beam CARS technique, and the crossed probe beam allows for excellent spatial sectioning of the probed location

  8. Localized vibrations in superconducting YB a2C u3O7 revealed by ultrafast optical coherent spectroscopy

    Science.gov (United States)

    Novelli, Fabio; Giovannetti, Gianluca; Avella, Adolfo; Cilento, Federico; Patthey, Luc; Radovic, Milan; Capone, Massimo; Parmigiani, Fulvio; Fausti, Daniele

    2017-05-01

    The interaction between phonons and high-energy excitations of electronic origin in cuprates and their role in the superconducting mechanisms is still controversial. Here we use coherent vibrational time-domain spectroscopy together with density functional and dynamical mean-field theory calculations to establish a direct link between the c -axis phonon modes and the in-plane electronic charge excitations in optimally doped YB a2C u3O7 . The nonequilibrium Raman tensor is measured by means of the broadband "coherent-phonon" response in pump-probe experiments and is qualitatively described by our model using density functional theory in the frozen-phonon approximation plus single-band dynamical mean-field theory to account for the electronic correlations. The major outcome of our experimental and theoretical study is to establish the link between out-of-plane copper ion displacements and the in-plane electronic correlations, and to estimate at a few unit cells the correlation length of the associated phonon mode. The approach introduced here could help in revealing the complex interplay between fluctuations of different nature and spatial correlation in several strongly correlated materials.

  9. Dispersion-based stimulated Raman scattering spectroscopy, holography, and optical coherence tomography.

    Science.gov (United States)

    Robles, Francisco E; Fischer, Martin C; Warren, Warren S

    2016-01-11

    Stimulated Raman scattering (SRS) enables fast, high resolution imaging of chemical constituents important to biological structures and functional processes, both in a label-free manner and using exogenous biomarkers. While this technology has shown remarkable potential, it is currently limited to point scanning and can only probe a few Raman bands at a time (most often, only one). In this work we take a fundamentally different approach to detecting the small nonlinear signals based on dispersion effects that accompany the loss/gain processes in SRS. In this proof of concept, we demonstrate that the dispersive measurements are more robust to noise compared to amplitude-based measurements, which then permit spectral or spatial multiplexing (potentially both, simultaneously). Finally, we illustrate how this method may enable different strategies for biochemical imaging using phase microscopy and optical coherence tomography.

  10. Differentiation of bacterial versus viral otitis media using a combined Raman scattering spectroscopy and low coherence interferometry probe (Conference Presentation)

    Science.gov (United States)

    Zhao, Youbo; Shelton, Ryan L.; Tu, Haohua; Nolan, Ryan M.; Monroy, Guillermo L.; Chaney, Eric J.; Boppart, Stephen A.

    2016-02-01

    Otitis media (OM) is a highly prevalent disease that can be caused by either a bacterial or viral infection. Because antibiotics are only effective against bacterial infections, blind use of antibiotics without definitive knowledge of the infectious agent, though commonly practiced, can lead to the problems of potential harmful side effects, wasteful misuse of medical resources, and the development of antimicrobial resistance. In this work, we investigate the feasibility of using a combined Raman scattering spectroscopy and low coherence interferometry (LCI) device to differentiate OM infections caused by viruses and bacteria and improve our diagnostic ability of OM. Raman spectroscopy, an established tool for molecular analysis of biological tissue, has been shown capable of identifying different bacterial species, although mostly based on fixed or dried sample cultures. LCI has been demonstrated recently as a promising tool for determining tympanic membrane (TM) thickness and the presence and thickness of middle-ear biofilm located behind the TM. We have developed a fiber-based ear insert that incorporates spatially-aligned Raman and LCI probes for point-of-care diagnosis of OM. As shown in human studies, the Raman probe provides molecular signatures of bacterial- and viral-infected OM and normal middle-ear cavities, and LCI helps to identify depth-resolved structural information as well as guide and monitor positioning of the Raman spectroscopy beam for relatively longer signal acquisition time. Differentiation of OM infections is determined by correlating in vivo Raman data collected from human subjects with the Raman features of different bacterial and viral species obtained from cultured samples.

  11. Coherent Spectroscopy of Ultra-Cold Mercury for the UV to VUV

    Science.gov (United States)

    2015-11-20

    cw   laser   source.  The  spectroscopy   laser  system  utilizes  a   cw  fiber   laser  that  is  amplified  and...this,  we  first  lock  a   secondary  external  cavity  semiconductor   diode   laser  to  an  ultrastable  ULE  reference...system  to   the   diode   laser .  This

  12. Optical phase nanoscopy in red blood cells using low-coherence spectroscopy.

    Science.gov (United States)

    Shock, Itay; Barbul, Alexander; Girshovitz, Pinhas; Nevo, Uri; Korenstein, Rafi; Shaked, Natan T

    2012-10-01

    We propose a low-coherence spectral-domain phase microscopy (SDPM) system for accurate quantitative phase measurements in red blood cells (RBCs) for the prognosis and monitoring of disease conditions that affect the visco-elastic properties of RBCs. Using the system, we performed time-recordings of cell membrane fluctuations, and compared the nano-scale fluctuation dynamics of healthy and glutaraldehyde-treated RBCs. Glutaraldehyde-treated RBCs possess lower amplitudes of fluctuations, reflecting an increased membrane stiffness. To demonstrate the ability of our system to measure fluctuations of lower amplitudes than those measured by the commonly used holographic phase microscopy techniques, we also constructed wide-field digital interferometry (WFDI) system and compared the performances of both systems. Due to its common-path geometry, the optical-path-delay stability of SDPM was found to be less than 0.3 nm in liquid environment, at least three times better than WFDI under the same conditions. In addition, due to the compactness of SDPM and its inexpensive and robust design, the system possesses a high potential for clinical applications.

  13. Coherent Two-Dimensional Terahertz Magnetic Resonance Spectroscopy of Collective Spin Waves.

    Science.gov (United States)

    Lu, Jian; Li, Xian; Hwang, Harold Y; Ofori-Okai, Benjamin K; Kurihara, Takayuki; Suemoto, Tohru; Nelson, Keith A

    2017-05-19

    We report a demonstration of two-dimensional (2D) terahertz (THz) magnetic resonance spectroscopy using the magnetic fields of two time-delayed THz pulses. We apply the methodology to directly reveal the nonlinear responses of collective spin waves (magnons) in a canted antiferromagnetic crystal. The 2D THz spectra show all of the third-order nonlinear magnon signals including magnon spin echoes, and 2-quantum signals that reveal pairwise correlations between magnons at the Brillouin zone center. We also observe second-order nonlinear magnon signals showing resonance-enhanced second-harmonic and difference-frequency generation. Numerical simulations of the spin dynamics reproduce all of the spectral features in excellent agreement with the experimental 2D THz spectra.

  14. Longitudinal bunch diagnostics using coherent transition radiation spectroscopy. Physical principles, multichannel spectrometer, experimental results, mathematical methods

    International Nuclear Information System (INIS)

    Schmidt, Bernhard; Wesch, Stephan; Behrens, Christopher; Koevener, Toke; Hass, Eugen; Casalbuoni, Sara

    2018-03-01

    The generation and properties of transition radiation (TR) are thoroughly treated. The spectral energy density, as described by the Ginzburg-Frank formula, is computed analytically, and the modifications caused by the finite size of the TR screen and by near-field diffraction effects are carefully analyzed. The principles of electron bunch shape reconstruction using coherent transition radiation are outlined. Spectroscopic measurements yield only the magnitude of the longitudinal form factor but not its phase. Two phase retrieval methods are investigated and illustrated with model calculations: analytic phase computation by means of the Kramers-Kronig dispersion relation, and iterative phase retrieval. Particular attention is paid to the ambiguities which are unavoidable in the reconstruction of longitudinal charge density profiles from spectroscopic data. The origin of these ambiguities has been identified and a thorough mathematical analysis is presented. The experimental part of the paper comprises a description of our multichannel infrared and THz spectrometer and a selection of measurements at FLASH, comparing the bunch profiles derived from spectroscopic data with those determined with a transversely deflecting microwave structure. A rigorous derivation of the Kramers-Kronig phase formula is presented in Appendix A. Numerous analytic model calculations can be found in Appendix B. The differences between normal and truncated Gaussians are discussed in Appendix C. Finally, Appendix D contains a short description of the propagation of an electromagnetic wave front by two-dimensional fast Fourier transformation. This is the basis of a powerful numerical Mathematica trademark code THzTransport, which permits the propagation of electromagnetic wave fronts through a beam line consisting of drift spaces, lenses, mirrors and apertures.

  15. Longitudinal bunch diagnostics using coherent transition radiation spectroscopy. Physical principles, multichannel spectrometer, experimental results, mathematical methods

    Energy Technology Data Exchange (ETDEWEB)

    Schmidt, Bernhard; Wesch, Stephan; Behrens, Christopher [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Koevener, Toke [Hamburg Univ. (Germany); European Organization for Nuclear Research (CERN), Geneva (Switzerland); Hass, Eugen [Hamburg Univ. (Germany); Casalbuoni, Sara [Karlsruhe Institute of Technology (Germany). Inst. for Beam Physics and Technology; Schmueser, Peter [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Hamburg Univ. (Germany)

    2018-03-15

    The generation and properties of transition radiation (TR) are thoroughly treated. The spectral energy density, as described by the Ginzburg-Frank formula, is computed analytically, and the modifications caused by the finite size of the TR screen and by near-field diffraction effects are carefully analyzed. The principles of electron bunch shape reconstruction using coherent transition radiation are outlined. Spectroscopic measurements yield only the magnitude of the longitudinal form factor but not its phase. Two phase retrieval methods are investigated and illustrated with model calculations: analytic phase computation by means of the Kramers-Kronig dispersion relation, and iterative phase retrieval. Particular attention is paid to the ambiguities which are unavoidable in the reconstruction of longitudinal charge density profiles from spectroscopic data. The origin of these ambiguities has been identified and a thorough mathematical analysis is presented. The experimental part of the paper comprises a description of our multichannel infrared and THz spectrometer and a selection of measurements at FLASH, comparing the bunch profiles derived from spectroscopic data with those determined with a transversely deflecting microwave structure. A rigorous derivation of the Kramers-Kronig phase formula is presented in Appendix A. Numerous analytic model calculations can be found in Appendix B. The differences between normal and truncated Gaussians are discussed in Appendix C. Finally, Appendix D contains a short description of the propagation of an electromagnetic wave front by two-dimensional fast Fourier transformation. This is the basis of a powerful numerical Mathematica trademark code THzTransport, which permits the propagation of electromagnetic wave fronts through a beam line consisting of drift spaces, lenses, mirrors and apertures.

  16. Coherent Synchrotron Radiation for Rotational Spectroscopy: Application to the Rotational Spectrum of Propynal in the 200-750 GHz Range

    Science.gov (United States)

    Barros, J.; Roy, P.; Appadoo, D.; Naughton, D. Mc; Robertson, E.; Manceron, L.

    2013-06-01

    In storage rings, short electron bunches can produce an intense THz radiation called Coherent Synchrotron Radiation (CSR). The flux of this emission between 250 and 750 GHz (in the mW range, up the 10000 times the regular synchrotron emission) is very advantageous for broad band absorption spectroscopy, using interferometric techniques. This source is, however, inherently difficult to stabilize, and intensity fluctuations lead to artifacts on the FT-based measurements, which strongly limit the use of CSR in particular for high-resolution measurements. At SOLEIL however, by screening different currents and bunch lengths, we defined stable CSR conditions for which the signal-to-noise ratio (S/N) allows for measurements at high resolution. Moreover, we developed an artifact correction system, based on a simultaneous detection of the input and the output signals of the interferometer, which allows to further improve the S/N. For this purpose, the optics and electronics of two bolometers were matched. The stable CSR combined with this ingenious technique allowed us to record for the first time high-resolution FT spectra in the sub-THz range, with a S/N of 100 in a few hours. This enables many applications such as broadband rotational spectra in the THz range, studies of molecules with low frequency torsional modes, absolute intensities determinations, or studies of unstable species. Results obtained on Propynal illustrate these possibilities and enabled to improve significantly the ground state spectroscopic constants.

  17. Signatures of Förster and Dexter transfer processes in coupled nanostructures for linear and two-dimensional coherent optical spectroscopy

    Science.gov (United States)

    Specht, Judith F.; Richter, Marten

    2015-03-01

    In this manuscript, we study the impact of the two Coulomb induced resonance energy transfer processes, Förster and Dexter coupling, on the spectral signatures obtained by double quantum coherence spectroscopy. We show that the specific coupling characteristics allow us to identify the underlying excitation transfer mechanism by means of specific signatures in coherent spectroscopy. Therefore, we control the microscopic calculated coupling strength of spin preserving and spin flipping Förster transfer processes by varying the mutual orientation of the two quantum emitters. The calculated spectra reveal the optical selection rules altered by Förster and Dexter coupling between two semiconductor quantum dots. We show that Dexter coupling between bright and dark two-exciton states occurs.

  18. Compensation of spectral artifacts in dual-modality intravascular optical coherence tomography and near-infrared spectroscopy (Conference Presentation)

    Science.gov (United States)

    Fard, Ali M.; Gardecki, Joseph A.; Ughi, Giovanni J.; Hyun, Chulho; Tearney, Guillermo J.

    2016-02-01

    Intravascular optical coherence tomography (OCT) is a high-resolution catheter-based imaging method that provides three-dimensional microscopic images of coronary artery in vivo, facilitating coronary artery disease treatment decisions based on detailed morphology. Near-infrared spectroscopy (NIRS) has proven to be a powerful tool for identification of lipid-rich plaques inside the coronary walls. We have recently demonstrated a dual-modality intravascular imaging technology that integrates OCT and NIRS into one imaging catheter using a two-fiber arrangement and a custom-made dual-channel fiber rotary junction. It therefore enables simultaneous acquisition of microstructural and composition information at 100 frames/second for improved diagnosis of coronary lesions. The dual-modality OCT-NIRS system employs a single wavelength-swept light source for both OCT and NIRS modalities. It subsequently uses a high-speed photoreceiver to detect the NIRS spectrum in the time domain. Although use of one light source greatly simplifies the system configuration, such light source exhibits pulse-to-pulse wavelength and intensity variation due to mechanical scanning of the wavelength. This can be in particular problematic for NIRS modality and sacrifices the reliability of the acquired spectra. In order to address this challenge, here we developed a robust data acquisition and processing method that compensates for the spectral variations of the wavelength-swept light source. The proposed method extracts the properties of the light source, i.e., variation period and amplitude from a reference spectrum and subsequently calibrates the NIRS datasets. We have applied this method on datasets obtained from cadaver human coronary arteries using a polygon-scanning (1230-1350nm) OCT system, operating at 100,000 sweeps per second. The results suggest that our algorithm accurately and robustly compensates the spectral variations and visualizes the dual-modality OCT-NIRS images. These

  19. Laser pulses for coherent xuv Raman excitation

    Science.gov (United States)

    Greenman, Loren; Koch, Christiane P.; Whaley, K. Birgitta

    2015-07-01

    We combine multichannel electronic structure theory with quantum optimal control to derive femtosecond-time-scale Raman pulse sequences that coherently populate a valence excited state. For a neon atom, Raman target populations of up to 13% are obtained. Superpositions of the ground and valence Raman states with a controllable relative phase are found to be reachable with up to 4.5% population and arbitrary phase control facilitated by the pump pulse carrier-envelope phase. Analysis of the optimized pulse structure reveals a sequential mechanism in which the valence excitation is reached via a fast (femtosecond) population transfer through an intermediate resonance state in the continuum rather than avoiding intermediate-state population with simultaneous or counterintuitive (stimulated Raman adiabatic passage) pulse sequences. Our results open a route to coupling valence excitations and core-hole excitations in molecules and aggregates that locally address specific atoms and represent an initial step towards realization of multidimensional spectroscopy in the xuv and x-ray regimes.

  20. Real-time visualization of the vibrational wavepacket dynamics in electronically excited pyrimidine via femtosecond time-resolved photoelectron imaging

    Science.gov (United States)

    Li, Shuai; Long, Jinyou; Ling, Fengzi; Wang, Yanmei; Song, Xinli; Zhang, Song; Zhang, Bing

    2017-07-01

    The vibrational wavepacket dynamics at the very early stages of the S1-T1 intersystem crossing in photoexcited pyrimidine is visualized in real time by femtosecond time-resolved photoelectron imaging and time-resolved mass spectroscopy. A coherent superposition of the vibrational states is prepared by the femtosecond pump pulse at 315.3 nm, resulting in a vibrational wavepacket. The composition of the prepared wavepacket is directly identified by a sustained quantum beat superimposed on the parent-ion transient, possessing a frequency in accord with the energy separation between the 6a1 and 6b2 states. The dephasing time of the vibrational wavepacket is determined to be 82 ps. More importantly, the variable Franck-Condon factors between the wavepacket components and the dispersed cation vibrational levels are experimentally illustrated to identify the dark state and follow the energy-flow dynamics on the femtosecond time scale. The time-dependent intensities of the photoelectron peaks originated from the 6a1 vibrational state exhibit a clear quantum beating pattern with similar periodicity but a phase shift of π rad with respect to those from the 6b2 state, offering an unambiguous picture of the restricted intramolecular vibrational energy redistribution dynamics in the 6a1/6b2 Fermi resonance.

  1. Estimating side-chain order in methyl-protonated, perdeuterated proteins via multiple-quantum relaxation violated coherence transfer NMR spectroscopy

    International Nuclear Information System (INIS)

    Sun Hechao; Godoy-Ruiz, Raquel; Tugarinov, Vitali

    2012-01-01

    Relaxation violated coherence transfer NMR spectroscopy (Tugarinov et al. in J Am Chem Soc 129:1743–1750, 2007) is an established experimental tool for quantitative estimation of the amplitudes of side-chain motions in methyl-protonated, highly deuterated proteins. Relaxation violated coherence transfer experiments monitor the build-up of methyl proton multiple-quantum coherences that can be created in magnetically equivalent spin-systems as long as their transverse magnetization components relax with substantially different rates. The rate of this build-up is a reporter of the methyl-bearing side-chain mobility. Although the build-up of multiple-quantum 1 H coherences is monitored in these experiments, the decay of the methyl signal during relaxation delays occurs when methyl proton magnetization is in a single-quantum state. We describe a relaxation violated coherence transfer approach where the relaxation of multiple-quantum 1 H– 13 C methyl coherences during the relaxation delay period is quantified. The NMR experiment and the associated fitting procedure that models the time-dependence of the signal build-up, are applicable to the characterization of side-chain order in [ 13 CH 3 ]-methyl-labeled, highly deuterated protein systems up to ∼100 kDa in molecular weight. The feasibility of extracting reliable measures of side-chain order is experimentally verified on methyl-protonated, perdeuterated samples of an 8.5-kDa ubiquitin at 10°C and an 82-kDa Malate Synthase G at 37°C.

  2. The dependence of the ultrafast relaxation kinetics of the S2 and S1 states in β-carotene homologs and lycopene on conjugation length studied by femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies

    Science.gov (United States)

    Kosumi, Daisuke; Fujiwara, Masazumi; Fujii, Ritsuko; Cogdell, Richard J.; Hashimoto, Hideki; Yoshizawa, Masayuki

    2009-06-01

    The ultrafast relaxation kinetics of all-trans-β-carotene homologs with varying numbers of conjugated double bonds n(n =7-15) and lycopene (n =11) has been investigated using femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies, both carried out under identical excitation conditions. The nonradiative relaxation rates of the optically allowed S2(1Bu+1) state were precisely determined by the time-resolved fluorescence. The kinetics of the optically forbidden S1(2Ag-1) state were observed by the time-resolved absorption measurements. The dependence of the S1 relaxation rates upon the conjugation length is adequately described by application of the energy gap law. In contrast to this, the nonradiative relaxation rates of S2 have a minimum at n =9 and show a reverse energy gap law dependence for values of n above 11. This anomalous behavior of the S2 relaxation rates can be explained by the presence of an intermediate state (here called the Sx state) located between the S2 and S1 states at large values of n (such as n =11). The presence of such an intermediate state would then result in the following sequential relaxation pathway S2→Sx→S1→S0. A model based on conical intersections between the potential energy curves of these excited singlet states can readily explain the measured relationships between the decay rates and the energy gaps.

  3. Extended ABCD matrix formalism for the description of femtosecond diffraction patterns; application to femtosecond digital in-line holography with anamorphic optical systems.

    Science.gov (United States)

    Brunel, Marc; Shen, Huanhuan; Coetmellec, Sebastien; Lebrun, Denis

    2012-03-10

    We present a new model to predict diffraction patterns of femtosecond pulses through complex optical systems. The model is based on the extension of an ABCD matrix formalism combined with generalized Huygens-Fresnel transforms (already used in the CW regime) to the femtosecond regime. The model is tested to describe femtosecond digital in-line holography experiments realized in situ through a cylindrical Plexiglas pipe. The model allows us to establish analytical relations that link the holographic reconstruction process to the experimental parameters of the pipe and of the incident beam itself. Simulations and experimental results are in good concordance. Femtosecond digital in-line holography is shown to allow significant coherent noise reduction, and this model will be particularly efficient to describe a wide range of optical geometries. More generally, the model developed can be easily used in any experiment where the knowledge of the precise evolution of femtosecond transverse patterns is required.

  4. Excited-State Dynamics of a DNA Duplex in a Deep Eutectic Solvent Probed by Femtosecond Time-Resolved IR Spectroscopy.

    Science.gov (United States)

    de La Harpe, Kimberly; Kohl, Forrest R; Zhang, Yuyuan; Kohler, Bern

    2018-03-08

    To better understand how the solvent influences excited-state deactivation in DNA strands, femtosecond time-resolved IR (fs-TRIR) pump-probe measurements were performed on a d(AT) 9 ·d(AT) 9 duplex dissolved in a deep eutectic solvent (DES) made from choline chloride and ethylene glycol in a 1:2 mol ratio. This solvent, known as ethaline, is a member of a class of ionic liquids capable of solubilizing DNA with minimal disruption to its secondary structure. UV melting analysis reveals that the duplex studied here melts at 18 °C in ethaline compared to 50 °C in aqueous solution. Ethaline has an excellent transparency window that facilitates TRIR measurements in the double-bond stretching region. Transient spectra recorded in deuterated ethaline at room temperature indicate that photoinduced intrastrand charge transfer occurs from A to T, yielding the same exciplex state previously detected in aqueous solution. This state decays via charge recombination with a lifetime of 380 ± 10 ps compared to the 300 ± 10 ps lifetime measured earlier in D 2 O solution. The TRIR data strongly suggest that the long-lived exciplex forms exclusively in the solvated duplex, and not in the denatured single strands, which appear to have little, if any, base stacking. The longer lifetime of the exciplex state in the DES compared to aqueous solution is suggested to arise from reduced stabilization of the charge transfer state, resulting in slower charge recombination on account of Marcus inverted behavior.

  5. Femtosecond laser ablation of bovine cortical bone

    Science.gov (United States)

    Cangueiro, Liliana T.; Vilar, Rui; Botelho do Rego, Ana M.; Muralha, Vania S. F.

    2012-12-01

    We study the surface topographical, structural, and compositional modifications induced in bovine cortical bone by femtosecond laser ablation. The tests are performed in air, with a Yb:KYW chirped-pulse-regenerative amplification laser system (500 fs, 1030 nm) at fluences ranging from 0.55 to 2.24 J/cm2. The ablation process is monitored by acoustic emission measurements. The topography of the laser-treated surfaces is studied by scanning electron microscopy, and their constitution is characterized by glancing incidence x-ray diffraction, x-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and micro-Raman spectroscopy. The results show that femtosecond laser ablation allows removing bone without melting, carbonization, or cracking. The structure and composition of the remaining tissue are essentially preserved, the only constitutional changes observed being a reduction of the organic material content and a partial recrystallization of hydroxyapatite in the most superficial region of samples. The results suggest that, within this fluence range, ablation occurs by a combination of thermal and electrostatic mechanisms, with the first type of mechanism predominating at lower fluences. The associated thermal effects explain the constitutional changes observed. We show that femtosecond lasers are a promising tool for delicate orthopaedic surgeries, where small amounts of bone must be cut with negligible damage, thus minimizing surgical trauma.

  6. Femtosecond Synchronization of Laser Systems for the LCLS

    International Nuclear Information System (INIS)

    Byrd, John; Doolittle, Lawrence; Huang, Gang; Staples, John; Wilcox, Russell; Arthur, John; Frisch, Josef; White, William

    2012-01-01

    The scientific potential of femtosecond x-ray pulses at linac-driven free-electron lasers such as the Linac Coherent Light Source is tremendous. Time-resolved pump-probe experiments require a measure of the relative arrival time of each x-ray pulse with respect to the experimental pump laser. An optical timing system based on stabilized fiber links has been developed for the LCLS to provide this synchronization. Preliminary results show synchronization of the installed stabilized links at the sub-20-femtosecond level. We present details of the implementation at LCLS and potential for future development.

  7. Modern spectroscopy

    CERN Document Server

    Hollas, J Michael

    2013-01-01

    The latest edition of this highly acclaimed title introduces the reader to a wide range of spectroscopies, and includes both the background theory and applications to structure determination and chemical analysis.  It covers rotational, vibrational, electronic, photoelectron and Auger spectroscopy, as well as EXAFs and the theory of lasers and laser spectroscopy. A  revised and updated edition of a successful, clearly written book Includes the latest developments in modern laser techniques, such as cavity ring-down spectroscopy and femtosecond lasers Provides numerous worked examples, calculations and questions at the end of chapters.

  8. Third-harmonic generation and scattering in combustion flames using a femtosecond laser filament.

    Science.gov (United States)

    Zang, Hong-Wei; Li, He-Long; Su, Yue; Fu, Yao; Hou, Meng-Yao; Baltuška, Andrius; Yamanouchi, Kaoru; Xu, Huailiang

    2018-02-01

    Coherent radiation in the ultraviolent (UV) range has high potential applicability to the diagnosis of the formation processes of soot in combustion because of the high scattering efficiency in the UV wavelength region, even though the UV light is lost largely by the absorption within the combustion flames. We show that the third harmonic (TH) of a Ti:sapphire 800 nm femtosecond laser is generated in a laser-induced filament in a combustion flame and that the conversion efficiency of the TH varies sensitively by the ellipticity of the driver laser pulse but does not vary so much by the choice of alkanol species introduced as fuel for the combustion flames. We also find that the TH recorded from the side direction of the filament is the Rayleigh scattering of the TH by soot nanoparticles within the flame and that the intensity of the TH varies depending on the fuel species as well as on the position of the laser filament within the flame. Our results show that a remote and in situ measurement of distributions of soot nanoparticles in a combustion flame can be achieved by Rayleigh scattering spectroscopy of the TH generated by a femtosecond-laser-induced filament in the combustion flame.

  9. Femtosecond electron bunches, source and characterization

    International Nuclear Information System (INIS)

    Thongbai, C.; Kusoljariyakul, K.; Rimjaem, S.; Rhodes, M.W.; Saisut, J.; Thamboon, P.; Wichaisirimongkol, P.; Vilaithong, T.

    2008-01-01

    A femtosecond electron source has been developed at the Fast Neutron Research Facility (FNRF), Chiang Mai University, Thailand. So far, it has produced electron bunches as short as σ z ∼180 fs with (1-6)x10 8 electrons per microbunch. The system consists of an RF-gun with a thermionic cathode, an alpha-magnet as a magnetic bunch compressor, and a linear accelerator as a post acceleration section. Coherent transition radiation emitted at wavelengths equal to and longer than the bunch length is used in a Michelson interferometer to determine the bunch length by autocorrelation technique. The experimental setup and results of the bunch length measurement are described

  10. Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Hellman, Hal

    1968-01-01

    This booklet discusses spectroscopy, the study of absorption of radiation by matter, including X-ray, gamma-ray, microwave, mass spectroscopy, as well as others. Spectroscopy has produced more fundamental information to the study of the detailed structure of matter than any other tools.

  11. Direct measurement of exciton valley coherence in monolayer WSe2

    KAUST Repository

    Hao, Kai

    2016-02-29

    In crystals, energy band extrema in momentum space can be identified by a valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier, analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides. However, the valley coherence time—a crucial quantity for valley pseudospin manipulation—is difficult to directly probe. In this work, we use two-dimensional coherent spectroscopy to resonantly generate and detect valley coherence of excitons (Coulomb-bound electron–hole pairs) in monolayer WSe2 (refs ,). The imposed valley coherence persists for approximately one hundred femtoseconds. We propose that the electron–hole exchange interaction provides an important decoherence mechanism in addition to exciton population recombination. This work provides critical insight into the requirements and strategies for optical manipulation of the valley pseudospin for future valleytronics applications.

  12. What are the intensities and line-shapes of the twenty four polarization terms in coherent anti-Stokes Raman spectroscopy?

    International Nuclear Information System (INIS)

    Niu, Kai; Lee, Soo-Y.

    2015-01-01

    Coherent anti-Stokes Raman spectroscopy (CARS) is conventionally described by just one diagram/term where the three electric field interactions act on the ket side in a Feynman dual time-line diagram in a specific time order of pump, Stokes and probe pulses. In theory, however, any third-order nonlinear spectroscopy with three different electric fields interacting with a molecule can be described by forty eight diagrams/terms. They reduce to just 24 diagrams/terms if we treat the time ordering of the electric field interactions on the ket independently of those on the bra, i.e. the ket and bra wave packets evolve independently. The twenty four polarization terms can be calculated in the multidimensional, separable harmonic oscillator model to obtain the intensities and line-shapes. It is shown that in fs/ps CARS, for the two cases of off-resonance CARS in toluene and resonance CARS in rhodamine 6G, where we use a fs pump pulse, a fs Stokes pulse and a ps probe pulse, we obtain sharp vibrational lines in four of the polarization terms where the pump and Stokes pulses can create a vibrational coherence on the ground electronic state, while the spectral line-shapes of the other twenty terms are broad and featureless. The conventional CARS term with sharp vibrational lines is the dominant term, with intensity at least one order of magnitude larger than the other terms

  13. What are the intensities and line-shapes of the twenty four polarization terms in coherent anti-Stokes Raman spectroscopy?

    Energy Technology Data Exchange (ETDEWEB)

    Niu, Kai [School of Science, Tianjin University of Technology and Education, Tianjin, 300222 (China); Lee, Soo-Y., E-mail: sooying@ntu.edu.sg [Division of Physics & Applied Physics, and Division of Chemistry & Biological Chemistry, School of Physical & Mathematical Sciences, Nanyang Technological University, Singapore 637371 (Singapore)

    2015-12-15

    Coherent anti-Stokes Raman spectroscopy (CARS) is conventionally described by just one diagram/term where the three electric field interactions act on the ket side in a Feynman dual time-line diagram in a specific time order of pump, Stokes and probe pulses. In theory, however, any third-order nonlinear spectroscopy with three different electric fields interacting with a molecule can be described by forty eight diagrams/terms. They reduce to just 24 diagrams/terms if we treat the time ordering of the electric field interactions on the ket independently of those on the bra, i.e. the ket and bra wave packets evolve independently. The twenty four polarization terms can be calculated in the multidimensional, separable harmonic oscillator model to obtain the intensities and line-shapes. It is shown that in fs/ps CARS, for the two cases of off-resonance CARS in toluene and resonance CARS in rhodamine 6G, where we use a fs pump pulse, a fs Stokes pulse and a ps probe pulse, we obtain sharp vibrational lines in four of the polarization terms where the pump and Stokes pulses can create a vibrational coherence on the ground electronic state, while the spectral line-shapes of the other twenty terms are broad and featureless. The conventional CARS term with sharp vibrational lines is the dominant term, with intensity at least one order of magnitude larger than the other terms.

  14. What are the intensities and line-shapes of the twenty four polarization terms in coherent anti-Stokes Raman spectroscopy?

    Science.gov (United States)

    Niu, Kai; Lee, Soo-Y.

    2015-12-01

    Coherent anti-Stokes Raman spectroscopy (CARS) is conventionally described by just one diagram/term where the three electric field interactions act on the ket side in a Feynman dual time-line diagram in a specific time order of pump, Stokes and probe pulses. In theory, however, any third-order nonlinear spectroscopy with three different electric fields interacting with a molecule can be described by forty eight diagrams/terms. They reduce to just 24 diagrams/terms if we treat the time ordering of the electric field interactions on the ket independently of those on the bra, i.e. the ket and bra wave packets evolve independently. The twenty four polarization terms can be calculated in the multidimensional, separable harmonic oscillator model to obtain the intensities and line-shapes. It is shown that in fs/ps CARS, for the two cases of off-resonance CARS in toluene and resonance CARS in rhodamine 6G, where we use a fs pump pulse, a fs Stokes pulse and a ps probe pulse, we obtain sharp vibrational lines in four of the polarization terms where the pump and Stokes pulses can create a vibrational coherence on the ground electronic state, while the spectral line-shapes of the other twenty terms are broad and featureless. The conventional CARS term with sharp vibrational lines is the dominant term, with intensity at least one order of magnitude larger than the other terms.

  15. Spectroscopy

    CERN Document Server

    Walker, S

    1976-01-01

    The three volumes of Spectroscopy constitute the one comprehensive text available on the principles, practice and applications of spectroscopy. By giving full accounts of those spectroscopic techniques only recently introduced into student courses - such as Mössbauer spectroscopy and photoelectron spectroscopy - in addition to those techniques long recognised as being essential in chemistry teaching - sucha as e.s.r. and infrared spectroscopy - the book caters for the complete requirements of undergraduate students and at the same time provides a sound introduction to special topics for graduate students.

  16. Femtosecond Laser Filamentation

    CERN Document Server

    Chin, See Leang

    2010-01-01

    Femtosecond Laser Filamentation gives a comprehensive review of the physics of propagation of intense femtosecond laser pulses in optical media (principally air) and the applications and challenges of this new technique. This book presents the modern understanding of the physics of femtosecond laser pulse propagation, including unusual new effects such as the self-transformation of the pulse into a white light laser pulse, intensity clamping, the physics of multiple filamentation and competition, and how filaments’ ability to melt glass leads to wave guide writing. The potential applications of laser filamentation in atmospheric sensing and the generation of other electromagnetic pulses from the UV to the radio frequency are treated, together with possible future challenges in the excitation of super-excited states of molecules. Exciting new phenomena such as filament induced ultrafast birefringence and the excitation of molecular rotational wave packets and their multiple revivals in air (gases) will also ...

  17. Two-dimensional spectroscopy of a molecular dimer unveils the effects of vibronic coupling on exciton coherences

    NARCIS (Netherlands)

    Halpin, Alexei; Johnson, Philip J. M.; Tempelaar, Roel; Murphy, R. Scott; Knoester, Jasper; Jansen, Thomas L. C.; Miller, R. J. Dwayne

    The observation of persistent oscillatory signals in multidimensional spectra of protein-pigment complexes has spurred a debate on the role of coherence-assisted electronic energy transfer as a key operating principle in photosynthesis. Vibronic coupling has recently been proposed as an explanation

  18. Anomalous Phase Change in [(GeTe)2/(Sb2Te3)]20 Superlattice Observed by Coherent Phonon Spectroscopy

    Science.gov (United States)

    Makino, K.; Saito, Y.; Mitrofanov, K.; Tominaga, J.; Kolobov, A. V.; Nakano, T.; Fons, P.; Hase, M.

    The temperature-dependent ultrafast coherent phonon dynamics of topological (GeTe)2/(Sb2Te3) super lattice phase change memory material was investigated. By comparing with Ge-Sb-Te alloy, a clear contrast suggesting the unique phase change behavior was found.

  19. Generation of continuous coherent radiation at Lyman-alpha and 1S-2P Spectroscopy of atomic hydrogen

    NARCIS (Netherlands)

    Pahl, A.; Fendel, P.; Henrich, B.R.; Walz, J.; Hansch, T.W.; Eikema, K.S.E.

    2005-01-01

    Continuous coherent radiation from wavelengths from 121 to 123 nm in the vacuum ultraviolet (VUV) was generated by four-wave sum-frequency mixing in mercury vapor. A yield of 20 nW at Lyman-alpha (121.57 nm) was achieved. We describe the experimental setup in detail and present a calculation of the

  20. New ultrafast X-ray sources and their applications. Coherent ultrashort X UV emission by harmonic generation

    International Nuclear Information System (INIS)

    Salieres, P.; Le deroff, L.; Hergott, J.F.; Merdji, H.; Carre, B.

    2000-01-01

    By focusing an intense short-pulse laser into a rare gas jet, high-order harmonics of the laser frequency are generated. Considerable progress have been made in the last few years, with the observation of harmonic orders higher that 200, extending the emission down to 3 nm. Besides its fundamental interest, this XUV emission represents a new source with unique properties of coherence and ultrashort (femtosecond) duration. A growing number of applications are reported, ranging from atomic and molecular spectroscopy to solid-state and plasma physics. (authors)

  1. Coherent Control of Multiphoton Transitions in the Gas and Condensed Phases with Shaped Ultrashort Pulses

    International Nuclear Information System (INIS)

    Dantus, Marcos

    2008-01-01

    Controlling laser-molecule interactions has become an integral part of developing devices and applications in spectroscopy, microscopy, optical switching, micromachining and photochemistry. Coherent control of multiphoton transitions could bring a significant improvement of these methods. In microscopy, multi-photon transitions are used to activate different contrast agents and suppress background fluorescence; coherent control could generate selective probe excitation. In photochemistry, different dissociative states are accessed through two, three, or more photon transitions; coherent control could be used to select the reaction pathway and therefore the yield-specific products. For micromachining and processing a wide variety of materials, femtosecond lasers are now used routinely. Understanding the interactions between the intense femtosecond pulse and the material could lead to technologically important advances. Pulse shaping could then be used to optimize the desired outcome. The scope of our research program is to develop robust and efficient strategies to control nonlinear laser-matter interactions using ultrashort shaped pulses in gas and condensed phases. Our systematic research has led to significant developments in a number of areas relevant to the AMO Physics group at DOE, among them: generation of ultrashort phase shaped pulses, coherent control and manipulation of quantum mechanical states in gas and condensed phases, behavior of isolated molecules under intense laser fields, behavior of condensed phase matter under intense laser field and implications on micromachining with ultrashort pulses, coherent control of nanoparticles their surface plasmon waves and their nonlinear optical behavior, and observation of coherent Coulomb explosion processes at 10 16 W/cm 2 . In all, the research has resulted in 36 publications (five journal covers) and nine invention disclosures, five of which have continued on to patenting

  2. Enhancement of coherent acoustic phonons in InGaN multiple quantum wells

    Science.gov (United States)

    Hafiz, Shopan D.; Zhang, Fan; Monavarian, Morteza; Avrutin, Vitaliy; Morkoç, Hadis; Özgür, Ümit

    2015-03-01

    Enhancement of coherent zone folded longitudinal acoustic phonon (ZFLAP) oscillations at terahertz frequencies was demonstrated in InGaN multiple quantum wells (MQWs) by using wavelength degenerate time resolved differential transmission spectroscopy. Screening of the piezoelectric field in InGaN MQWs by photogenerated carriers upon femtosecond pulse excitation gave rise to terahertz ZFLAPs, which were monitored at the Brillouin zone center in the transmission geometry. MQWs composed of 10 pairs InxGa1-xN wells and In0.03Ga0.97N barriers provided coherent phonon frequencies of 0.69-0.80 THz depending on the period of MQWs. Dependences of ZFLAP amplitude on excitation density and wavelength were also investigated. Possibility of achieving phonon cavity, incorporating a MQW placed between two AlN/GaN phonon mirrors designed to exhibit large acoustic gaps at the zone center, was also explored.

  3. Femtosecond laser materials processing

    International Nuclear Information System (INIS)

    Stuart, B.C.

    1997-01-01

    The use femtosecond pulses for materials processing results in very precise cutting and drilling with high efficiency. Energy deposited in the electrons is not coupled into the bulk during the pulse, resulting in negligible shock or thermal loading to adjacent areas

  4. Femtosecond carotenoid to retinal energy transfer in xanthorhodopsin

    Czech Academy of Sciences Publication Activity Database

    Polívka, Tomáš; Balashov, S.P.; Chábera, P.; Imasheva, E.S.; Yartsev, A.; Sundström, V.; Lanyi, J.K.

    2009-01-01

    Roč. 96, č. 6 (2009), s. 2268-2277 ISSN 0006-3495 R&D Projects: GA AV ČR IAA608170604 Institutional research plan: CEZ:AV0Z50510513 Keywords : energy transfer * carotenoids * femtosecond spectroscopy Subject RIV: BO - Biophysics Impact factor: 4.390, year: 2009

  5. Spectroscopy

    DEFF Research Database (Denmark)

    Berg, Rolf W.

    This introductory booklet covers the basics of molecular spectroscopy, infrared and Raman methods, instrumental considerations, symmetry analysis of molecules, group theory and selection rules, as well as assignments of fundamental vibrational modes in molecules.......This introductory booklet covers the basics of molecular spectroscopy, infrared and Raman methods, instrumental considerations, symmetry analysis of molecules, group theory and selection rules, as well as assignments of fundamental vibrational modes in molecules....

  6. Quantum coherent control of the vibrational dynamics of a ...

    Indian Academy of Sciences (India)

    2014-02-12

    Feb 12, 2014 ... c Indian Academy of Sciences. Vol. 82, No ... Abstract. We simulate adaptive feedback control to coherently shape a femtosecond infrared laser ... it was shown that different coherent control schemes are unified on a fundamental level. ... A 150 fs pulse with a fluence of 600 J/m2 was used as an initial pulse.

  7. Development of fiber lasers and devices for coherent Raman scattering microscopy

    Science.gov (United States)

    Lamb, Erin Stranford

    As ultrafast laser technology has found expanding application in machining, spectroscopy, microscopy, surgery, and numerous other areas, the desire for inexpensive and robust laser sources has grown. Until recently, nonlinear effects in fiber systems due to the tight confinement of the light in the core have limited their performance. However, with advances in managing nonlinearity through pulse propagation physics and the use of large core fibers, the performance of fiber lasers can compete with that of their solid-state counterparts. As specific applications, such as coherent Raman scattering microscopy, emerge that stand to benefit from fiber technology, new performance challenges in areas such as laser noise are anticipated. This thesis studies nonlinear pulse propagation in fiber lasers and fiber parametric devices. Applications of dissipative solitons and self-similar pulse propagation to low-repetition rate oscillators that have the potential to simplify short-pulse amplification schemes will be examined. The rest of this thesis focuses on topics relevant to fiber laser development for coherent Raman scattering microscopy sources. Coherent pulse division and recombination inside the laser cavity will be introduced as an energy-scaling mechanism and demonstrated for a fiber soliton laser. The relative intensity noise properties of mode-locked fiber lasers, with a particular emphasis on normal dispersion lasers, will be explored in simulation and experiment. A fiber optical parametric oscillator will be studied in detail for low noise frequency conversion of picosecond pulses, and its utility for coherent Raman imaging will be demonstrated. Spectral compression of femtosecond pulses is used to generate picosecond pulses to pump this device, and this technique provides a route to future noise reduction in the system. Furthermore, this device forms a multimodal source capable of providing the picosecond pulses for coherent Raman scattering microscopy and the

  8. Tunable femtosecond Cherenkov fiber laser

    DEFF Research Database (Denmark)

    Liu, Xiaomin; Svane, Ask Sebastian; Lægsgaard, Jesper

    2014-01-01

    We demonstrate electrically-tunable femtosecond Cherenkov fiber laser output at the visible range. Using an all-fiber, self-starting femtosecond Yb-doped fiber laser as the pump source and nonlinear photonic crystal fiber link as the wave-conversion medium, ultrafast, milliwatt-level, tunable...... and spectral isolated Cherenkov radiation at visible wavelengths are reported. Such a femtosecond Cherenkov laser source is promising for practical biophotonics applications....

  9. Coherent imaging using SACLA

    International Nuclear Information System (INIS)

    Nishino, Yoshinori; Kimura, Takashi; Suzuki, Akihiro; Joti, Yasumasa; Bessho, Yoshitaka

    2017-01-01

    X-ray free-electron lasers (XFELs) with femtosecond pulse duration offer an innovative solution to transcend the spatial resolution limitation in conventional X-ray imaging for biological samples and soft matters by clearing up the radiation damage problem using the “diffraction-before-destruction” strategy. Building on this strategy, the authors are developing a method to image solution sample under controlled environment, pulsed coherent X-ray solution scattering (PCXSS), using XFELs and phase retrieval algorithms in coherent diffractive imaging (CDI). This article describes the basics of PCXSS and examples of PCXSS measurement, for a living cell and self-assemblies of gold nanoparticles, performed by the authors using SACLA. An attempt toward the industrial application of PCXSS is also described. (author)

  10. Optimization of a coherent synchrotron radiation source in the Tera-hertz range for high-resolution spectroscopy of molecules of astrophysical interest

    International Nuclear Information System (INIS)

    Barros, J.

    2012-01-01

    Fourier Transform spectroscopy is the most used multiplex tool for high-resolution measurements in the infrared range. Its extension to the Tera-hertz domain is of great interest for spectroscopic studies of interstellar molecules. This application is however hampered by the lack of dedicated, broadband sources with a sufficient intensity and stability. In this work, Coherent Synchrotron Radiation (CSR) was used as a source for molecular spectroscopy at high resolution on the AILES infrared and Tera-hertz beamline of SOLEIL synchrotron. The beamline being optimized for far-infrared, we could characterize the properties of CSR and compare them to the incoherent synchrotron radiation. A double detection system allowed to correct the effect of the source-related instabilities, hence to significantly increase the signal-to-noise ratio. Pure rotational spectra were measured using these developments. The case of the propynal molecule, for which a refined set of rotational and centrifugal distortion constants was calculated, proves the complementarity between CSR and the classical microwave or infrared sources. (author)

  11. High-resolution 1H NMR spectroscopy of fish muscle, eggs and small whole fish via Hadamard-encoded intermolecular multiple-quantum coherence.

    Directory of Open Access Journals (Sweden)

    Honghao Cai

    Full Text Available BACKGROUND AND PURPOSE: Nuclear magnetic resonance (NMR spectroscopy has become an important technique for tissue studies. Since tissues are in semisolid-state, their high-resolution (HR spectra cannot be obtained by conventional NMR spectroscopy. Because of this restriction, extraction and high-resolution magic angle spinning (HR MAS are widely applied for HR NMR spectra of tissues. However, both of the methods are subject to limitations. In this study, the feasibility of HR (1H NMR spectroscopy based on intermolecular multiple-quantum coherence (iMQC technique is explored using fish muscle, fish eggs, and a whole fish as examples. MATERIALS AND METHODS: Intact salmon muscle tissues, intact eggs from shishamo smelt and a whole fish (Siamese algae eater are studied by using conventional 1D one-pulse sequence, Hadamard-encoded iMQC sequence, and HR MAS. RESULTS: When we use the conventional 1D one-pulse sequence, hardly any useful spectral information can be obtained due to the severe field inhomogeneity. By contrast, HR NMR spectra can be obtained in a short period of time by using the Hadamard-encoded iMQC method without shimming. Most signals from fatty acids and small metabolites can be observed. Compared to HR MAS, the iMQC method is non-invasive, but the resolution and the sensitivity of resulting spectra are not as high as those of HR MAS spectra. CONCLUSION: Due to the immunity to field inhomogeneity, the iMQC technique can be a proper supplement to HR MAS, and it provides an alternative for the investigation in cases with field distortions and with samples unsuitable for spinning. The acquisition time of the proposed method is greatly reduced by introduction of the Hadamard-encoded technique, in comparison with that of conventional iMQC method.

  12. Femtosecond Optical Frequency Comb Technology Principle, Operation and Application

    CERN Document Server

    Ye, Jun

    2005-01-01

    Over the last few years, there has been a remarkable convergence among the fields of ultrafast optics, optical frequency metrology, and precision laser spectroscopy. This convergence has enabled unprecedented advances in control of the electric field of the pulses produced by femtosecond mode-locked lasers. The resulting spectrum consists of a comb of sharp spectral lines with well-defined frequencies. These new techniques and capabilities are generally known as "femtosecond comb technology." They have had dramatic impact on the diverse fields of precision measurement and extreme nonlinear optical physics. This book provides an introductory description of mode-locked lasers, the connection between time and frequency descriptions of their output and the physical origins of the electric field dynamics, together with an overview of applications of femtosecond comb technology. Individual chapters go into more detail on mode-locked laser development, spectral broadening in microstructure fiber, optical parametric ...

  13. Femtosecond laser irradiation-induced infrared absorption on silicon surfaces

    Directory of Open Access Journals (Sweden)

    Qinghua Zhu

    2015-04-01

    Full Text Available The near-infrared (NIR absorption below band gap energy of crystalline silicon is significantly increased after the silicon is irradiated with femtosecond laser pulses at a simple experimental condition. The absorption increase in the NIR range primarily depends on the femtosecond laser pulse energy, pulse number, and pulse duration. The Raman spectroscopy analysis shows that after the laser irradiation, the silicon surface consists of silicon nanostructure and amorphous silicon. The femtosecond laser irradiation leads to the formation of a composite of nanocrystalline, amorphous, and the crystal silicon substrate surface with microstructures. The composite has an optical absorption enhancement at visible wavelengths as well as at NIR wavelength. The composite may be useful for an NIR detector, for example, for gas sensing because of its large surface area.

  14. spectroscopy

    African Journals Online (AJOL)

    Aghomotsegin

    2015-10-14

    Oct 14, 2015 ... characterized by using phenotypic, API and Fourier transform infrared (FTIR) spectroscopy methods. One hundred and fifty-seven (157) strains were isolated from 13 cheese samples, and identification test was performed for 83 strains. At the end of the study, a total of 22 Lactococcus sp., 36 Enterecoccus ...

  15. Femtosecond lasers for countermeasure applications

    NARCIS (Netherlands)

    Franssen, G.C.; Schleijpen, H.M.A.; Heuvel, J.C. van den; Buersing, H.; Eberle, B.; Walter, D.

    2009-01-01

    In recent years, much advance in the field of high-power femtosecond laser technology has been made. The high pulse power of femtosecond laser systems leads to various interesting phenomena, such as a very high power density and the formation of a plasma in the propagation medium, which is usually

  16. Ultrahigh-Resolution Magnetic Resonance in Inhomogeneous Magnetic Fields: Two-Dimensional Long-Lived-Coherence Correlation Spectroscopy

    Science.gov (United States)

    Chinthalapalli, Srinivas; Bornet, Aurélien; Segawa, Takuya F.; Sarkar, Riddhiman; Jannin, Sami; Bodenhausen, Geoffrey

    2012-07-01

    A half-century quest for improving resolution in Nuclear Magnetic Resonance (NMR) and Magnetic Resonance Imaging (MRI) has enabled the study of molecular structures, biological interactions, and fine details of anatomy. This progress largely relied on the advent of sophisticated superconducting magnets that can provide stable and homogeneous fields with temporal and spatial variations below ΔB0/B0LLC-COSY) opens the way to overcome both inhomogeneous and homogeneous broadening, which arise from local variations in static fields and fluctuating dipole-dipole interactions, respectively. LLC-COSY makes it possible to obtain ultrahigh resolution two-dimensional spectra, with linewidths on the order of Δν=0.1 to 1 Hz, even in very inhomogeneous fields (ΔB0/B0>10ppm or 5000 Hz at 9.7 T), and can improve resolution by a factor up to 9 when the homogeneous linewidths are determined by dipole-dipole interactions. The resulting LLC-COSY spectra display chemical shift differences and scalar couplings in two orthogonal dimensions, like in “J spectroscopy.” LLC-COSY does not require any sophisticated gradient switching or frequency-modulated pulses. Applications to in-cell NMR and to magnetic resonance spectroscopy (MRS) of selected volume elements in MRI appear promising, particularly when susceptibility variations tend to preclude high resolution.

  17. Femtosecond laser ablation of enamel

    Science.gov (United States)

    Le, Quang-Tri; Bertrand, Caroline; Vilar, Rui

    2016-06-01

    The surface topographical, compositional, and structural modifications induced in human enamel by femtosecond laser ablation is studied. The laser treatments were performed using a Yb:KYW chirped-pulse-regenerative amplification laser system (560 fs and 1030 nm) and fluences up to 14 J/cm2. The ablation surfaces were studied by scanning electron microscopy, grazing incidence x-ray diffraction, and micro-Raman spectroscopy. Regardless of the fluence, the ablation surfaces were covered by a layer of resolidified material, indicating that ablation is accompanied by melting of hydroxyapatite. This layer presented pores and exploded gas bubbles, created by the release of gaseous decomposition products of hydroxyapatite (CO2 and H2O) within the liquid phase. In the specimen treated with 1-kHz repetition frequency and 14 J/cm2, thickness of the resolidified material is in the range of 300 to 900 nm. The micro-Raman analysis revealed that the resolidified material contains amorphous calcium phosphate, while grazing incidence x-ray diffraction analysis allowed detecting traces of a calcium phosphate other than hydroxyapatite, probably β-tricalcium phosphate Ca3), at the surface of this specimen. The present results show that the ablation of enamel involves melting of enamel's hydroxyapatite, but the thickness of the altered layer is very small and thermal damage of the remaining material is negligible.

  18. Can Excited State Electronic Coherence Be Tuned via Molecular Structural Modification? A First-Principles Quantum Electronic Dynamics Study of Pyrazolate-Bridged Pt(II) Dimers

    Energy Technology Data Exchange (ETDEWEB)

    Lingerfelt, David B.; Lestrange, Patrick J.; Radler, Joseph J.; Brown-Xu, Samantha E.; Kim, Pyosang; Castellano, Felix N.; Chen, Lin X.; Li, Xiaosong

    2017-02-24

    Materials and molecular systems exhibiting long-lived electronic coherence can facilitate coherent transport, opening the door to efficient charge and energy transport beyond traditional methods. Recently, signatures of a possible coherent, recurrent electronic motion were identified in femtosecond pump-probe spectroscopy experiments on a binuclear platinum complex, where a persistent periodic beating in the transient absorption signal’s anisotropy was observed. In this study, we investigate the excitonic dynamics that underlie the suspected electronic coherence for a series of binuclear platinum complexes exhibiting a range of interplatinum distances. Results suggest that the long-lived coherence can only result when competitive electronic couplings are in balance. At longer Pt-Pt distances, the electronic couplings between the two halves of the binuclear system weaken, and exciton localization and recombination is favored on short time scales. For short Pt-Pt distances, electronic couplings between the states in the coherent superposition are stronger than the coupling with other excitonic states, leading to long-lived coherence.

  19. Coherent evolution of parahydrogen induced polarisation using laser pump, NMR probe spectroscopy: Theoretical framework and experimental observation.

    Science.gov (United States)

    Halse, Meghan E; Procacci, Barbara; Henshaw, Sarah-Louise; Perutz, Robin N; Duckett, Simon B

    2017-05-01

    We recently reported a pump-probe method that uses a single laser pulse to introduce parahydrogen (p-H 2 ) into a metal dihydride complex and then follows the time-evolution of the p-H 2 -derived nuclear spin states by NMR. We present here a theoretical framework to describe the oscillatory behaviour of the resultant hyperpolarised NMR signals using a product operator formalism. We consider the cases where the p-H 2 -derived protons form part of an AX, AXY, AXYZ or AA'XX' spin system in the product molecule. We use this framework to predict the patterns for 2D pump-probe NMR spectra, where the indirect dimension represents the evolution during the pump-probe delay and the positions of the cross-peaks depend on the difference in chemical shift of the p-H 2 -derived protons and the difference in their couplings to other nuclei. The evolution of the NMR signals of the p-H 2 -derived protons, as well as the transfer of hyperpolarisation to other NMR-active nuclei in the product, is described. The theoretical framework is tested experimentally for a set of ruthenium dihydride complexes representing the different spin systems. Theoretical predictions and experimental results agree to within experimental error for all features of the hyperpolarised 1 H and 31 P pump-probe NMR spectra. Thus we establish the laser pump, NMR probe approach as a robust way to directly observe and quantitatively analyse the coherent evolution of p-H 2 -derived spin order over micro-to-millisecond timescales. Copyright © 2017 The Authors. Published by Elsevier Inc. All rights reserved.

  20. Toward a High-Stability Coherent Population Trapping Cs Vapor-Cell Atomic Clock Using Autobalanced Ramsey Spectroscopy

    Science.gov (United States)

    Abdel Hafiz, Moustafa; Coget, Grégoire; Petersen, Michael; Rocher, Cyrus; Guérandel, Stéphane; Zanon-Willette, Thomas; de Clercq, Emeric; Boudot, Rodolphe

    2018-06-01

    Vapor-cell atomic clocks are widely appreciated for their excellent short-term fractional frequency stability and their compactness. However, they are known to suffer on medium and long time scales from significant frequency instabilities, generally attributed to light-induced frequency-shift effects. In order to tackle this limitation, we investigate the application of the recently proposed autobalanced Ramsey (ABR) interrogation protocol onto a pulsed hot-vapor Cs vapor-cell clock based on coherent population trapping (CPT). We demonstrate that the ABR protocol, developed initially to probe the one-photon resonance of quantum optical clocks, can be successfully applied to a two-photon CPT resonance. The applied method, based on the alternation of two successive Ramsey-CPT sequences with unequal free-evolution times and the subsequent management of two interconnected phase and frequency servo loops, is found to allow a relevant reduction of the clock-frequency sensitivity to laser-power variations. This original ABR-CPT approach, combined with the implementation of advanced electronics laser-power stabilization systems, yields the demonstration of a CPT-based Cs vapor-cell clock with a short-term fractional frequency stability at the level of 3.1×10 -13τ-1 /2 , averaging down to the level of 6 ×10-15 at 2000-s integration time. These encouraging performances demonstrate that the use of the ABR interrogation protocol is a promising option towards the development of high-stability CPT-based frequency standards. Such clocks could be attractive candidates in numerous applications including next-generation satellite-based navigation systems, secure communications, instrumentation, or defense systems.

  1. Femtosecond laser ablation of dentin

    International Nuclear Information System (INIS)

    Alves, S; Vilar, R; Oliveira, V

    2012-01-01

    The surface morphology, structure and composition of human dentin treated with a femtosecond infrared laser (pulse duration 500 fs, wavelength 1030 nm, fluences ranging from 1 to 3 J cm -2 ) was studied by scanning electron microscopy, x-ray diffraction, x-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy. The average dentin ablation threshold under these conditions was 0.6 ± 0.2 J cm -2 and the ablation rate achieved in the range 1 to 2 µm/pulse for an average fluence of 3 J cm -2 . The ablation surfaces present an irregular and rugged appearance, with no significant traces of melting, deformation, cracking or carbonization. The smear layer was entirely removed by the laser treatment. For fluences only slightly higher than the ablation threshold the morphology of the laser-treated surfaces was very similar to the dentin fracture surfaces and the dentinal tubules remained open. For higher fluences, the surface was more porous and the dentin structure was partially concealed by ablation debris and a few resolidified droplets. Independently on the laser processing parameters and laser processing method used no sub-superficial cracking was observed. The dentin constitution and chemical composition was not significantly modified by the laser treatment in the processing parameter range used. In particular, the organic matter is not preferentially removed from the surface and no traces of high temperature phosphates, such as the β-tricalcium phosphate, were observed. The achieved results are compatible with an electrostatic ablation mechanism. In conclusion, the high beam quality and short pulse duration of the ultrafast laser used should allow the accurate preparation of cavities, with negligible damage of the underlying material. (paper)

  2. Polarization control of multi-photon absorption under intermediate femtosecond laser field

    International Nuclear Information System (INIS)

    Cheng Wenjing; Liang Guo; Wu Ping; Liu Pei; Jia Tianqing; Sun Zhenrong; Zhang Shian

    2017-01-01

    It has been shown that the femtosecond laser polarization modulation is a very simple and well-established method to control the multi-photon absorption process by the light–matter interaction. Previous studies mainly focused on the multi-photon absorption control in the weak field. In this paper, we further explore the polarization control behavior of multi-photon absorption process in the intermediate femtosecond laser field. In the weak femtosecond laser field, the second-order perturbation theory can well describe the non-resonant two-photon absorption process. However, the higher order nonlinear effect (e.g., four-photon absorption) can occur in the intermediate femtosecond laser field, and thus it is necessary to establish new theoretical model to describe the multi-photon absorption process, which includes the two-photon and four-photon transitions. Here, we construct a fourth-order perturbation theory to study the polarization control behavior of this multi-photon absorption under the intermediate femtosecond laser field excitation, and our theoretical results show that the two-photon and four-photon excitation pathways can induce a coherent interference, while the coherent interference is constructive or destructive that depends on the femtosecond laser center frequency. Moreover, the two-photon and four-photon transitions have the different polarization control efficiency, and the four-photon absorption can obtain the higher polarization control efficiency. Thus, the polarization control efficiency of the whole excitation process can be increased or decreased by properly designing the femtosecond laser field intensity and laser center frequency. These studies can provide a clear physical picture for understanding and controlling the multi-photon absorption process in the intermediate femtosecond laser field, and also can provide a theoretical guidance for the future experimental realization. (paper)

  3. Editorial: Focus on X-ray Beams with High Coherence

    Science.gov (United States)

    Robinson, Ian; Gruebel, Gerhard; Mochrie, Simon

    2010-03-01

    This editorial serves as the preface to a special issue of New Journal of Physics, which collects together solicited papers on a common subject, x-ray beams with high coherence. We summarize the issue's content, and explain why there is so much current interest both in the sources themselves and in the applications to the study of the structure of matter and its fluctuations (both spontaneous and driven). As this collection demonstrates, the field brings together accelerator physics in the design of new sources, particle physics in the design of detectors, and chemical and materials scientists who make use of the coherent beams produced. Focus on X-ray Beams with High Coherence Contents Femtosecond pulse x-ray imaging with a large field of view B Pfau, C M Günther, S Schaffert, R Mitzner, B Siemer, S Roling, H Zacharias, O Kutz, I Rudolph, R Treusch and S Eisebitt The FERMI@Elettra free-electron-laser source for coherent x-ray physics: photon properties, beam transport system and applications E Allaria, C Callegari, D Cocco, W M Fawley, M Kiskinova, C Masciovecchio and F Parmigiani Beyond simple exponential correlation functions and equilibrium dynamics in x-ray photon correlation spectroscopy Anders Madsen, Robert L Leheny, Hongyu Guo, Michael Sprung and Orsolya Czakkel The Coherent X-ray Imaging (CXI) instrument at the Linac Coherent Light Source (LCLS) Sébastien Boutet and Garth J Williams Dynamics and rheology under continuous shear flow studied by x-ray photon correlation spectroscopy Andrei Fluerasu, Pawel Kwasniewski, Chiara Caronna, Fanny Destremaut, Jean-Baptiste Salmon and Anders Madsen Exploration of crystal strains using coherent x-ray diffraction Wonsuk Cha, Sanghoon Song, Nak Cheon Jeong, Ross Harder, Kyung Byung Yoon, Ian K Robinson and Hyunjung Kim Coherence properties of the European XFEL G Geloni, E Saldin, L Samoylova, E Schneidmiller, H Sinn, Th Tschentscher and M Yurkov Fresnel coherent diffractive imaging: treatment and analysis of data G J

  4. Real-time dual-comb spectroscopy with a free-running bidirectionally mode-locked fiber laser

    Science.gov (United States)

    Mehravar, S.; Norwood, R. A.; Peyghambarian, N.; Kieu, K.

    2016-06-01

    Dual-comb technique has enabled exciting applications in high resolution spectroscopy, precision distance measurements, and 3D imaging. Major advantages over traditional methods can be achieved with dual-comb technique. For example, dual-comb spectroscopy provides orders of magnitude improvement in acquisition speed over standard Fourier-transform spectroscopy while still preserving the high resolution capability. Wider adoption of the technique has, however, been hindered by the need for complex and expensive ultrafast laser systems. Here, we present a simple and robust dual-comb system that employs a free-running bidirectionally mode-locked fiber laser operating at telecommunication wavelength. Two femtosecond frequency combs (with a small difference in repetition rates) are generated from a single laser cavity to ensure mutual coherent properties and common noise cancellation. As the result, we have achieved real-time absorption spectroscopy measurements without the need for complex servo locking with accurate frequency referencing, and relatively high signal-to-noise ratio.

  5. Determining the Effect of Calculus, Hypocalcification, and Stain on Using Optical Coherence Tomography and Polarized Raman Spectroscopy for Detecting White Spot Lesions

    Directory of Open Access Journals (Sweden)

    Amanda Huminicki

    2010-01-01

    Full Text Available Optical coherence tomography (OCT and polarized Raman spectroscopy (PRS have been shown as useful methods for distinguishing sound enamel from carious lesions ex vivo. However, factors in the oral environment such as calculus, hypocalcification, and stain could lead to false-positive results. OCT and PRS were used to investigate extracted human teeth clinically examined for sound enamel, white spot lesion (WSL, calculus, hypocalcification, and stain to determine whether these factors would confound WSL detection with these optical methods. Results indicate that OCT allowed differentiating caries from sound enamel, hypocalcification, and stain, with calculus deposits recognizable on OCT images. ANOVA and post-hoc unequal N HSD analyses to compare the mean Raman depolarization ratios from the various groups showed that the mean values were statistically significant at P<.05, except for several comparison pairs. With the current PRS analysis method, the mean depolarization ratios of stained enamel and caries are not significantly different due to the sloping background in the stained enamel spectra. Overall, calculus and hypocalcification are not confounding factors affecting WSL detection using OCT and PRS. Stain does not influence WSL detection with OCT. Improved PRS analysis methods are needed to differentiate carious from stained enamel.

  6. Depth-resolved multilayer pigment identification in paintings: combined use of laser-induced breakdown spectroscopy (LIBS) and optical coherence tomography (OCT).

    Science.gov (United States)

    Kaszewska, Ewa A; Sylwestrzak, Marcin; Marczak, Jan; Skrzeczanowski, Wojciech; Iwanicka, Magdalena; Szmit-Naud, Elżbieta; Anglos, Demetrios; Targowski, Piotr

    2013-08-01

    A detailed feasibility study on the combined use of laser-induced breakdown spectroscopy with optical coherence tomography (LIBS/OCT), aiming at a realistic depth-resolved elemental analysis of multilayer stratigraphies in paintings, is presented. Merging a high spectral resolution LIBS system with a high spatial resolution spectral OCT instrument significantly enhances the quality and accuracy of stratigraphic analysis. First, OCT mapping is employed prior to LIBS analysis in order to assist the selection of specific areas of interest on the painting surface to be examined in detail. Then, intertwined with LIBS, the OCT instrument is used as a precise profilometer for the online determination of the depth of the ablation crater formed by individual laser pulses during LIBS depth-profile analysis. This approach is novel and enables (i) the precise in-depth scaling of elemental concentration profiles, and (ii) the recognition of layer boundaries by estimating the corresponding differences in material ablation rate. Additionally, the latter is supported, within the transparency of the object, by analysis of the OCT cross-sectional views. The potential of this method is illustrated by presenting results on the detailed analysis of the structure of an historic painting on canvas performed to aid planned restoration of the artwork.

  7. Etude d'un continuum de lumière en régime femtoseconde. Applications au domaine biologique : microscopies et spectroscopie en temps résolu.

    OpenAIRE

    Courvoisier , Céline

    2006-01-01

    For few years, a new type of source, called "continuum of light", has been developed. It presents many advantages like a wideband spectrum, a huge brilliancy, a pulsed nature. The aim of this work is to perform a complete characterization of a continuum generated by the injection of femtosecond pulses into a microstructured fiber, and to consider the use of this continuum as optical source for biomedical applications.With acousto-optic filters, the continuum has been successfully employed as ...

  8. Observation and investigation of narrow optical transitions of 167Er3+ ions in femtosecond laser printed waveguides in 7LiYF4 crystal

    Science.gov (United States)

    Minnegaliev, M. M.; Dyakonov, I. V.; Gerasimov, K. I.; Kalinkin, A. A.; Kulik, S. P.; Moiseev, S. A.; Saygin, M. Yu; Urmancheev, R. V.

    2018-04-01

    We produced optical waveguides in the 167Er3+:7 LiYF4 crystal with diameters ranging from 30 to 100 μm by using the depressed-cladding approach with femtosecond laser. Stationary and coherent spectroscopy was performed on the 809 nm optical transitions between the hyperfine sublevels of 4I15/2 and 4I9/2 multiplets of 167Er3+ ions both inside and outside of waveguides. It was found that the spectra of 167Er3+ were slightly broadened and shifted inside the waveguides compared to the bulk crystal spectra. We managed to observe a two-pulse photon echo on this transition and determined phase relaxation times for each waveguide. The experimental results show that the created crystal waveguides doped by rare-earth ions can be used in optical quantum memory and integrated quantum schemes.

  9. International workshop on phase retrieval and coherent scattering. Coherence 2005

    International Nuclear Information System (INIS)

    Nugent, K.A.; Fienup, J.R.; Van Dyck, D.; Van Aert, S.; Weitkamp, T.; Diaz, A.; Pfeiffer, F.; Cloetens, P.; Stampanoni, M.; Bunk, O.; David, C.; Bronnikov, A.V.; Shen, Q.; Xiao, X.; Gureyev, T.E.; Nesterets, Ya.I.; Paganin, D.M.; Wilkins, S.W.; Mokso, R.; Cloetens, P.; Ludwig, W.; Hignette, O.; Maire, E.; Faulkner, H.M.L.; Rodenburg, J.M.; Wu, X.; Liu, H.; Grubel, G.; Ludwig, K.F.; Livet, F.; Bley, F.; Simon, J.P.; Caudron, R.; Le Bolloc'h, D.; Moussaid, A.; Gutt, C.; Sprung, M.; Madsen, A.; Tolan, M.; Sinha, S.K.; Scheffold, F.; Schurtenberger, P.; Robert, A.; Madsen, A.; Falus, P.; Borthwick, M.A.; Mochrie, S.G.J.; Livet, F.; Sutton, M.D.; Ehrburger-Dolle, F.; Bley, F.; Geissler, E.; Sikharulidze, I.; Jeu, W.H. de; Lurio, L.B.; Hu, X.; Jiao, X.; Jiang, Z.; Lurio, L.B.; Hu, X.; Jiao, X.; Jiang, Z.; Naryanan, S.; Sinha, S.K.; Lal, J.; Naryanan, S.; Sinha, S.K.; Lal, J.; Robinson, I.K.; Chapman, H.N.; Barty, A.; Beetz, T.; Cui, C.; Hajdu, J.; Hau-Riege, S.P.; He, H.; Stadler, L.M.; Sepiol, B.; Harder, R.; Robinson, I.K.; Zontone, F.; Vogl, G.; Howells, M.; London, R.; Marchesini, S.; Shapiro, D.; Spence, J.C.H.; Weierstall, U.; Eisebitt, S.; Shapiro, D.; Lima, E.; Elser, V.; Howells, M.R.; Huang, X.; Jacobsen, C.; Kirz, J.; Miao, H.; Neiman, A.; Sayre, D.; Thibault, P.; Vartanyants, I.A.; Robinson, I.K.; Onken, J.D.; Pfeifer, M.A.; Williams, G.J.; Pfeiffer, F.; Metzger, H.; Zhong, Z.; Bauer, G.; Nishino, Y.; Miao, J.; Kohmura, Y.; Yamamoto, M.; Takahashi, Y.; Koike, K.; Ebisuzaki, T.; Ishikawa, T.; Spence, J.C.H.; Doak, B.

    2005-01-01

    The contributions of the participants have been organized into 3 topics: 1) phase retrieval methods, 2) X-ray photon correlation spectroscopy, and 3) coherent diffraction imaging. This document gathers the abstracts of the presentations and of the posters

  10. International workshop on phase retrieval and coherent scattering. Coherence 2005

    Energy Technology Data Exchange (ETDEWEB)

    Nugent, K.A.; Fienup, J.R.; Van Dyck, D.; Van Aert, S.; Weitkamp, T.; Diaz, A.; Pfeiffer, F.; Cloetens, P.; Stampanoni, M.; Bunk, O.; David, C.; Bronnikov, A.V.; Shen, Q.; Xiao, X.; Gureyev, T.E.; Nesterets, Ya.I.; Paganin, D.M.; Wilkins, S.W.; Mokso, R.; Cloetens, P.; Ludwig, W.; Hignette, O.; Maire, E.; Faulkner, H.M.L.; Rodenburg, J.M.; Wu, X.; Liu, H.; Grubel, G.; Ludwig, K.F.; Livet, F.; Bley, F.; Simon, J.P.; Caudron, R.; Le Bolloc' h, D.; Moussaid, A.; Gutt, C.; Sprung, M.; Madsen, A.; Tolan, M.; Sinha, S.K.; Scheffold, F.; Schurtenberger, P.; Robert, A.; Madsen, A.; Falus, P.; Borthwick, M.A.; Mochrie, S.G.J.; Livet, F.; Sutton, M.D.; Ehrburger-Dolle, F.; Bley, F.; Geissler, E.; Sikharulidze, I.; Jeu, W.H. de; Lurio, L.B.; Hu, X.; Jiao, X.; Jiang, Z.; Lurio, L.B.; Hu, X.; Jiao, X.; Jiang, Z.; Naryanan, S.; Sinha, S.K.; Lal, J.; Naryanan, S.; Sinha, S.K.; Lal, J.; Robinson, I.K.; Chapman, H.N.; Barty, A.; Beetz, T.; Cui, C.; Hajdu, J.; Hau-Riege, S.P.; He, H.; Stadler, L.M.; Sepiol, B.; Harder, R.; Robinson, I.K.; Zontone, F.; Vogl, G.; Howells, M.; London, R.; Marchesini, S.; Shapiro, D.; Spence, J.C.H.; Weierstall, U.; Eisebitt, S.; Shapiro, D.; Lima, E.; Elser, V.; Howells, M.R.; Huang, X.; Jacobsen, C.; Kirz, J.; Miao, H.; Neiman, A.; Sayre, D.; Thibault, P.; Vartanyants, I.A.; Robinson, I.K.; Onken, J.D.; Pfeifer, M.A.; Williams, G.J.; Pfeiffer, F.; Metzger, H.; Zhong, Z.; Bauer, G.; Nishino, Y.; Miao, J.; Kohmura, Y.; Yamamoto, M.; Takahashi, Y.; Koike, K.; Ebisuzaki, T.; Ishikawa, T.; Spence, J.C.H.; Doak, B

    2005-07-01

    The contributions of the participants have been organized into 3 topics: 1) phase retrieval methods, 2) X-ray photon correlation spectroscopy, and 3) coherent diffraction imaging. This document gathers the abstracts of the presentations and of the posters.

  11. Coherent anti-Stokes Raman scattering (CARS) spectroscopy in Caenorhabditis elegans and Globodera pallida: evidence for an ivermectin-activated decrease in lipid stores.

    Science.gov (United States)

    Smus, Justyna P; Ludlow, Elizabeth; Dallière, Nicolas; Luedtke, Sarah; Monfort, Tual; Lilley, Catherine; Urwin, Peter; Walker, Robert J; O'Connor, Vincent; Holden-Dye, Lindy; Mahajan, Sumeet

    2017-12-01

    Macrocyclic lactones are arguably the most successful chemical class with efficacy against parasitic nematodes. Here we investigated the effect of the macrocyclic lactone ivermectin on lipid homeostasis in the plant parasitic nematode Globodera pallida and provide new insight into its mode of action. A non-invasive, non-destructive, label-free and chemically selective technique called Coherent anti-Stokes Raman scattering (CARS) spectroscopy was used to study lipid stores in G. pallida. We optimised the protocol using the free-living nematode Caenorhabditis elegans and then used CARS to quantify lipid stores in the pre-parasitic, non-feeding J2 stage of G. pallida. This revealed a concentration of lipid stores in the posterior region of J2 s within 24 h of hatching which decreased to undetectable levels over the course of 28 days. We tested the effect of ivermectin on J2 viability and lipid stores. Within 24 h, ivermectin paralysed J2 s. Counterintuitively, over the same time-course ivermectin increased the rate of depletion of J2 lipid, suggesting that in ivermectin-treated J2 s there is a disconnection between the energy requirements for motility and metabolic rate. This decrease in lipid stores would be predicted to negatively impact on J2 infective potential. These data suggest that the benefit of macrocyclic lactones as seed treatments may be underpinned by a multilevel effect involving both neuromuscular inhibition and acceleration of lipid metabolism. © 2017 The Authors. Pest Management Science published by John Wiley & Sons Ltd on behalf of Society of Chemical Industry. © 2017 The Authors. Pest Management Science published by John Wiley & Sons Ltd on behalf of Society of Chemical Industry.

  12. Spectroscopic analysis of femtosecond laser-induced gas breakdown

    International Nuclear Information System (INIS)

    Hermann, J.; Bruneau, S.; Sentis, M.

    2004-01-01

    The plasma generated by the interaction of a femtosecond laser pulse with gas has been analyzed using time- and space-resolved emission spectroscopy. The laser beam has been focused with a microscope objective into different gases (air, Ar, He) at pressures ranging from 10 2 to 10 5 Pa. From the analysis of spectral line emission from ions and neutral atoms, the plasma parameters and the plasma composition have been determined as a function of time and space. Furthermore, the generation of fast electrons and/or VUV radiation by the femtosecond laser interaction with the gas was brought to the fore. From the time- and space-evolution of the plasma parameters, a rough estimation of initial values of electron density and refraction index in the focal volume has been performed. These results are compared to analysis of the laser beam transmitted by the plasma. The latter show that only a small fraction of the laser energy is absorbed by the plasma while the spatial distribution of the transmitted laser beam is strongly perturbed by the plasma, which acts like a defocusing lens. However, in ambient helium, the plasma defocusing is weak due to the high ionization potential of helium. The understanding of femtosecond laser-induced gas breakdown is useful for process optimization in femtosecond laser applications like micromachining or surface microanalysis, etc

  13. Two-Dimensional Resonance Raman Signatures of Vibronic Coherence Transfer in Chemical Reactions.

    Science.gov (United States)

    Guo, Zhenkun; Molesky, Brian P; Cheshire, Thomas P; Moran, Andrew M

    2017-11-02

    Two-dimensional resonance Raman (2DRR) spectroscopy has been developed for studies of photochemical reaction mechanisms and structural heterogeneity in condensed phase systems. 2DRR spectroscopy is motivated by knowledge of non-equilibrium effects that cannot be detected with traditional resonance Raman spectroscopy. For example, 2DRR spectra may reveal correlated distributions of reactant and product geometries in systems that undergo chemical reactions on the femtosecond time scale. Structural heterogeneity in an ensemble may also be reflected in the 2D spectroscopic line shapes of both reactive and non-reactive systems. In this chapter, these capabilities of 2DRR spectroscopy are discussed in the context of recent applications to the photodissociation reactions of triiodide. We show that signatures of "vibronic coherence transfer" in the photodissociation process can be targeted with particular 2DRR pulse sequences. Key differences between the signal generation mechanisms for 2DRR and off-resonant 2D Raman spectroscopy techniques are also addressed. Overall, recent experimental developments and applications of the 2DRR method suggest that it will be a valuable tool for elucidating ultrafast chemical reaction mechanisms.

  14. Manipulating femtosecond spin-orbit torques with laser pulse sequences to control magnetic memory states and ringing

    Science.gov (United States)

    Lingos, P. C.; Wang, J.; Perakis, I. E.

    2015-05-01

    Femtosecond (fs) coherent control of collective order parameters is important for nonequilibrium phase dynamics in correlated materials. Here, we propose such control of ferromagnetic order based on using nonadiabatic optical manipulation of electron-hole (e -h ) photoexcitations to create fs carrier-spin pulses with controllable direction and time profile. These spin pulses are generated due to the time-reversal symmetry breaking arising from nonperturbative spin-orbit and magnetic exchange couplings of coherent photocarriers. By tuning the nonthermal populations of exchange-split, spin-orbit-coupled semiconductor band states, we can excite fs spin-orbit torques that control complex magnetization pathways between multiple magnetic memory states. We calculate the laser-induced fs magnetic anisotropy in the time domain by using density matrix equations of motion rather than the quasiequilibrium free energy. By comparing to pump-probe experiments, we identify a "sudden" out-of-plane magnetization canting displaying fs magnetic hysteresis, which agrees with switchings measured by the static Hall magnetoresistivity. This fs transverse spin-canting switches direction with magnetic state and laser frequency, which distinguishes it from the longitudinal nonlinear optical and demagnetization effects. We propose that sequences of clockwise or counterclockwise fs spin-orbit torques, photoexcited by shaping two-color laser-pulse sequences analogous to multidimensional nuclear magnetic resonance (NMR) spectroscopy, can be used to timely suppress or enhance magnetic ringing and switching rotation in magnetic memories.

  15. Quantum Femtosecond Magnetism: Phase Transition in Step with Light in a Strongly Correlated Manganese Oxide

    Science.gov (United States)

    Wang, Jigang

    2014-03-01

    Research of non-equilibrium phase transitions of strongly correlated electrons is built around addressing an outstanding challenge: how to achieve ultrafast manipulation of competing magnetic/electronic phases and reveal thermodynamically hidden orders at highly non-thermal, femtosecond timescales? Recently we reveal a new paradigm called quantum femtosecond magnetism-photoinduced femtosecond magnetic phase transitions driven by quantum spin flip fluctuations correlated with laser-excited inter-atomic coherent bonding. We demonstrate an antiferromagnetic (AFM) to ferromagnetic (FM) switching during about 100 fs laser pulses in a colossal magneto-resistive manganese oxide. Our results show a huge photoinduced femtosecond spin generation, measured by magnetic circular dichroism, with photo-excitation threshold behavior absent in the picosecond dynamics. This reveals an initial quantum coherent regime of magnetism, while the optical polarization/coherence still interacts with the spins to initiate local FM correlations that compete with the surrounding AFM matrix. Our results thus provide a framework that explores quantum non-equilibrium kinetics to drive phase transitions between exotic ground states in strongly correlated elecrons, and raise fundamental questions regarding some accepted rules, such as free energy and adiabatic potential surface. This work is in collaboration with Tianqi Li, Aaron Patz, Leonidas Mouchliadis, Jiaqiang Yan, Thomas A. Lograsso, Ilias E. Perakis. This work was supported by the National Science Foundation (contract no. DMR-1055352). Material synthesis at the Ames Laboratory was supported by the US Department of Energy-Basic Energy Sciences (contract no. DE-AC02-7CH11358).

  16. Manipulation of Squeezed Two-Phonon Bound States using Femtosecond Laser Pulses

    Directory of Open Access Journals (Sweden)

    Nakamura Kazutaka G.

    2013-03-01

    Full Text Available Two-phonon bound states have been excited exclusively in ZnTe(110 via impulsive stimulated second-order Raman scattering, essentially being squeezed states due to phase coherent excitation of two identical components anticorrelated in the wave vector. By using coherent control technique with a pair of femtosecond laser pulses, the manipulation of squeezed states has been demonstrated in which both the amplitude and lifetime of coherent oscillations of squeezed states are modulated, indicating the feasibility to control the quantum noise and the quantum nature of phonon squeezed states, respectively.

  17. Spatially periodic structures, under femtosecond pulsed excitation of crystals

    International Nuclear Information System (INIS)

    Martynovitch, Evgueni F.; Petite, Guillaume; Dresvianski, Vladimir P.; Starchenko, Anton A.

    2004-01-01

    Measuring the luminescence intensity of specially prepared irradiation defects induced in crystals, we observe that the longitudinal structure of quasi-interferences induced by two orthogonally polarized femtosecond pulses propagating together with different velocities is insensitive to the spatial broadening due to velocity dispersion in the crystals. On the contrary, it does depend on the pulse duration when it is changed by varying the spectral width of the radiation. It thus allows a direct measurement of the coherence time of such pulses. Stability of the axial selectivity is a good sign, taking away a number of serious limitations concerning possible applications

  18. Visible to Infrared Diamond Photonics Enabled by Focused Femtosecond Laser Pulses

    Directory of Open Access Journals (Sweden)

    Belén Sotillo

    2017-02-01

    Full Text Available Diamond’s nitrogen-vacancy (NV centers show great promise in sensing applications and quantum computing due to their long electron spin coherence time and because they can be found, manipulated, and read out optically. An important step forward for diamond photonics would be connecting multiple diamond NVs together using optical waveguides. However, the inertness of diamond is a significant hurdle for the fabrication of integrated optics similar to those that revolutionized silicon photonics. In this work, we show the fabrication of optical waveguides in diamond, enabled by focused femtosecond high repetition rate laser pulses. By optimizing the geometry of the waveguide, we obtain single mode waveguides from the visible to the infrared. Additionally, we show the laser writing of individual NV centers within the bulk of diamond. We use µ-Raman spectroscopy to gain better insight on the stress and the refractive index profile of the optical waveguides. Using optically detected magnetic resonance and confocal photoluminescence characterization, high quality NV properties are observed in waveguides formed in various grades of diamond, making them promising for applications such as magnetometry, quantum information systems, and evanescent field sensors.

  19. Longitudinal profile monitors using Coherent Smith–Purcell radiation

    International Nuclear Information System (INIS)

    Andrews, H.L.; Bakkali Taheri, F.; Barros, J.; Bartolini, R.; Cassinari, L.; Clarke, C.; Le Corre, S.; Delerue, N.; Doucas, G.; Fuster-Martinez, N.; Konoplev, I.; Labat, M.; Perry, C.; Reichold, A.; Stevenson, S.; Vieille Grosjean, M.

    2014-01-01

    Coherent Smith–Purcell radiation has the potential of providing information on the longitudinal profile of an electron bunch. The E-203 experiment at the FACET User Facility measures bunch profiles from the SLAC linac in the hundreds of femtoseconds range and the SPESO collaboration at Synchrotron SOLEIL is planning to make an accurate 2D map of the Coherent Smith–Purcell Radiation emission. - Highlights: • Coherent Smith–Purcell radiation can be used to measure longitudinal profiles in the hundred femtoseconds range. • The current setup used by the E-203 collaboration require integration over several shots and gratings. • Reducing the integration over a single shot and a single grating still yields a meaning full result. • The SPESO experiment at SOLEIL will make a systematic study of Coherent Smith–Purcell radiation

  20. Linear and Nonlinear Molecular Spectroscopy with Laser Frequency Combs

    Science.gov (United States)

    Picque, Nathalie

    2013-06-01

    The regular pulse train of a mode-locked femtosecond laser can give rise to a comb spectrum of millions of laser modes with a spacing precisely equal to the pulse repetition frequency. Laser frequency combs were conceived a decade ago as tools for the precision spectroscopy of atomic hydrogen. They are now becoming enabling tools for an increasing number of applications, including molecular spectroscopy. Recent experiments of multi-heterodyne frequency comb Fourier transform spectroscopy (also called dual-comb spectroscopy) have demonstrated that the precisely spaced spectral lines of a laser frequency comb can be harnessed for new techniques of linear absorption spectroscopy. The first proof-of-principle experiments have demonstrated a very exciting potential of dual-comb spectroscopy without moving parts for ultra-rapid and ultra-sensitive recording of complex broad spectral bandwidth molecular spectra. Compared to conventional Michelson-based Fourier transform spectroscopy, recording times could be shortened from seconds to microseconds, with intriguing prospects for spectroscopy of short lived transient species. The resolution improves proportionally to the measurement time. Therefore longer recordings allow high resolution spectroscopy of molecules with extreme precision, since the absolute frequency of each laser comb line can be known with the accuracy of an atomic clock. Moreover, since laser frequency combs involve intense ultrashort laser pulses, nonlinear interactions can be harnessed. Broad spectral bandwidth ultra-rapid nonlinear molecular spectroscopy and imaging with two laser frequency combs is demonstrated with coherent Raman effects and two-photon excitation. Real-time multiplex accessing of hyperspectral images may dramatically expand the range of applications of nonlinear microscopy. B. Bernhardt et al., Nature Photonics 4, 55-57 (2010); A. Schliesser et al. Nature Photonics 6, 440-449 (2012); T. Ideguchi et al. arXiv:1201.4177 (2012) T

  1. Serial Femtosecond Crystallography

    OpenAIRE

    Chapman, Henry N.

    2015-01-01

    X-ray free-electron lasers produce brief flashes of X-rays that are of about a billion times higher peak brightness than achievable from storage ring sources. Such a tremendous jump in X-ray source capabilities, which came in 2009 when the Linac Coherent Light Source began operations, was unprecedented in the history of X-ray science. Protein structure determination through the method of macromolecular crystallography has consistently benefited from the many increases in source performance fr...

  2. Vigilance task-related change in brain functional connectivity as revealed by wavelet phase coherence analysis of near-infrared spectroscopy signals

    Directory of Open Access Journals (Sweden)

    Wang Wei

    2016-08-01

    Full Text Available This study aims to assess the vigilance task-related change in connectivity in healthy adults using wavelet phase coherence (WPCO analysis of near-infrared spectroscopy signals (NIRS. NIRS is a non-invasive neuroimaging technique for assessing brain activity. Continuous recordings of the NIRS signals were obtained from the prefrontal cortex (PFC and sensorimotor cortical areas of 20 young healthy adults (24.9±3.3 years during a 10-min resting state and a 20-min vigilance task state. The vigilance task was used to simulate driving mental load by judging three random numbers (i.e., whether odd numbers. The task was divided into two sessions: the first 10 minutes (Task t1 and the second 10 minutes (Task t2. The WPCO of six channel pairs were calculated in five frequency intervals: 0.6–2 Hz (I, 0.145–0.6 Hz (II, 0.052–0.145 Hz (III, 0.021–0.052 Hz (IV, and 0.0095–0.021 Hz (V. The significant WPCO formed global connectivity (GC maps in intervals I and II and functional connectivity (FC maps in intervals III to V. Results show that the GC levels in interval I and FC levels in interval III were significantly lower in the Task t2 than in the resting state (p < 0.05, particularly between the left PFC and bilateral sensorimotor regions. Also, the reaction time shows an increase in Task t2 compared with that in Task t1. However, no significant difference in WPCO was found between Task t1 and resting state. The results showed that the change in FC at the range of 0.6-2 Hz was not attributed to the vigilance task pe se, but the interaction effect of vigilance task and time factors. The findings suggest that the decreased attention level might be partly attributed to the reduced GC levels between the left prefrontal region and sensorimotor area. The present results provide a new insight into the vigilance task-related brain activity.

  3. On interaction of femtosecond laser pulses with cluster targets

    International Nuclear Information System (INIS)

    Skobelev, I.Yu.; Faenov, A.Ya.; Magunov, A.I.

    2002-01-01

    The clusters heating through the femtosecond laser pulses is theoretically and experimentally studied. Both the process of the cluster target formation and results of the cluster plasma experimental studies through the emission X-ray spectroscopy methods are considered. The numerical model of clusters formation in the supersonic gaseous jet is proposed. It is shown that detailed studies on the two-phase gas-dynamic processes in the nozzle, forming the jet, make it possible to obtain spatial distributions of all cluster parameters, necessary for correct calculations of the clusters. The simple physical model of the plasma formation through the femtosecond laser method is proposed. It is shown that comparison of the observed X-ray spectra with the results of the detailed ion kinetics calculations, make it possible to determine the basic parameters of the formed plasma [ru

  4. Femtosecond Fiber Lasers

    Science.gov (United States)

    Bock, Katherine J.

    This thesis focuses on research I have done on ytterbium-doped femtosecond fiber lasers. These lasers operate in the near infrared region, lasing at 1030 nm. This wavelength is particularly important in biomedical applications, which includes but is not limited to confocal microscopy and ablation for surgical incisions. Furthermore, fiber lasers are advantageous compared to solid state lasers in terms of their cost, form factor, and ease of use. Solid state lasers still dominate the market due to their comparatively high energy pulses. High energy pulse generation in fiber lasers is hindered by either optical wave breaking or by multipulsing. One of the main challenges for fiber lasers is to overcome these limitations to achieve high energy pulses. The motivation for the work done in this thesis is increasing the output pulse peak power and energy. The main idea of the work is that decreasing the nonlinearity that acts on the pulse inside the cavity will prevent optical wave breaking, and thus will generate higher energy pulses. By increasing the output energy, ytterbium-doped femtosecond fiber lasers can be competitive with solid state lasers which are used commonly in research. Although fiber lasers tend to lack the wavelength tuning ability of solid state lasers, many biomedical applications take advantage of the 1030 microm central wavelength of ytterbium-doped fiber lasers, so the major limiting factor of fiber lasers in this field is simply the output power. By increasing the output energy without resorting to external amplification, the cavity is optimized and cost can remain low and economical. During verification of the main idea, the cavity was examined for possible back-reflections and for components with narrow spectral bandwidths which may have contributed to the presence of multipulsing. Distinct cases of multipulsing, bound pulse and harmonic mode-locking, were observed and recorded as they may be of more interest in the future. The third

  5. Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers

    Science.gov (United States)

    Harmand, M.; Coffee, R.; Bionta, M. R.; Chollet, M.; French, D.; Zhu, D.; Fritz, D. M.; Lemke, H. T.; Medvedev, N.; Ziaja, B.; Toleikis, S.; Cammarata, M.

    2013-03-01

    Recently, few-femtosecond pulses have become available at hard X-ray free-electron lasers. Coupled with the available sub-10 fs optical pulses, investigations into few-femtosecond dynamics are not far off. However, achieving sufficient synchronization between optical lasers and X-ray pulses continues to be challenging. We report a `measure-and-sort' approach, which achieves sub-10 fs root-mean-squared (r.m.s.) error measurement at hard X-ray FELs, far beyond the 100-200 fs r.m.s. jitter limitations. This timing diagnostic, now routinely available at the Linac Coherent Light Source (LCLS), is based on ultrafast free-carrier generation in optically transparent materials. Correlation between two independent measurements enables unambiguous demonstration of ~6 fs r.m.s. error in reporting the optical/X-ray delay, with single shot error suggesting the possibility of reaching few-femtosecond resolution.

  6. Optical coherence tomography characterization of femtosecond laser manufactured microfluidic circuits

    Science.gov (United States)

    De Pretto, Lucas Ramos; Samad, Ricardo Elgul; de Rossi, Wagner; de Freitas, Anderson Zanardi

    2018-02-01

    Dimensional characterization of microfluidic circuits were performed using three-dimensional models constructed from OCT images of such circuits. Were fabricated microchannels on the same BK7 glass plate, under different laser ablation conditions and substrate displacement velocity in relation to laser beam. Were used the following combination of energy, from 30 μJ to 60 μJ and velocity from 588 mm/min to 1176 mm/min, at 1 kHz laser repetition rate and 40 fs of pulse duration (FWHM). For OCT imaging we used an OCP930SR (Thorlabs System Inc) with 930 nm central wavelength, 6 μm of lateral and axial resolution, and image of 500 x 512 pixel corresponding to 2.0 mm x 1.6 mm of lateral and axial scans respectively at 8 frames per second. We also characterized devices like, micropumps, microvalves and microreactors. It was possible register the micropumps and valves in action in real time. Using the OCT images analyses was possible to select the best combination of laser pulse energy and substrate velocity. All the devices were made in raster protocol, where laser beam pass through the same path in a controlled number of times, and with each iteration more material is removed and deeper the channels remain. We found a deformation at the edge of fabricated structures, due to velocity reduction of substrate in relation to laser beam, which causes more laser pulses superposition in these regions, and more material is ablated. The technique was thus evaluated as a potential tool to aid in the inspection of microchannels.

  7. Ultraviolet-resonance femtosecond stimulated Raman study of the initial events in photoreceptor chromophore

    Directory of Open Access Journals (Sweden)

    Tahara T.

    2013-03-01

    Full Text Available Newly-developed ultraviolet-resonance femtosecond stimulated-Raman spectroscopy was utilized to study the initial structural evolution of photoactive yellow protein chromophore in solution. The obtained spectra changed drastically within 1 ps, demonstrating rapid in-plane deformations of the chromophore.

  8. Generation of polyyne and methylpolyyne molecules from toluene by intense femtosecond laser pulse irradiation

    International Nuclear Information System (INIS)

    Ramadhan, Ali; Wesolowski, Michal; Duley, Walter; Sanderson, Joseph; Wakabayashi, Tomonari; Shiromaru, Haruo; Fujino, Tatsuya; Kodama, Takeshi

    2015-01-01

    Hydrogen-capped and methyl-capped carbon chains (polyynes) have been generated by intense femtosecond laser irradiation of pure liquid toluene. UV-Vis and Raman spectroscopy were used to confirm the presence of polyynes in the irradiated samples, and high performance liquid chromatography (HPLC) was used to separate polyynes up to C 18 H 2 and HC 13 CH 3 . (paper)

  9. Femtosecond study of self-trapped vibrational excitons in crystalline acetanilide

    DEFF Research Database (Denmark)

    Edler, J.; Hamm, Peter; Scott, Alwyn C.

    2002-01-01

    Femtosecond IR spectroscopy of delocalized NH excitations of crystalline acetanilide confirms that self-trapping in hydrogen-bonded peptide units exists and does stabilize the excitation. Two phonons with frequencies of 48 and 76 cm(-1) are identified as the major degrees of freedom that mediate...

  10. Femtosecond pulse shaping using plasmonic snowflake nanoantennas

    Energy Technology Data Exchange (ETDEWEB)

    Tok, Ruestue Umut; Sendur, Kuersat [Sabanci University, Orhanli-Tuzla, 34956, Istanbul (Turkey)

    2011-09-15

    We have theoretically demonstrated femtosecond pulse manipulation at the nanoscale using the plasmonic snowflake antenna's ability to localize light over a broad spectrum. To analyze the interaction of the incident femtosecond pulse with the plasmonic nanoantenna, we first decompose the diffraction limited incident femtosecond pulse into its spectral components. The interaction of each spectral component with the nanoantenna is analyzed using finite element technique. The time domain response of the plasmonic antenna is obtained using inverse Fourier transformation. It is shown that the rich spectral characteristics of the plasmonic snowflake nanoantenna allow manipulation of the femtosecond pulses over a wide spectrum. Light localization around the gap region of the nanoantenna is shown for femtosecond pulses. As the alignment of incident light polarization is varied, different antenna elements oscillate, which in turn creates a different spectrum and a distinct femtosecond response.

  11. Mercury Amalgam Diffusion in Human Teeth Probed Using Femtosecond LIBS.

    Science.gov (United States)

    Bello, Liciane Toledo; da Ana, Patricia Aparecida; Santos, Dário; Krug, Francisco José; Zezell, Denise Maria; Vieira, Nilson Dias; Samad, Ricardo Elgul

    2017-04-01

    In this work the diffusion of mercury and other elements from amalgam tooth restorations through the surrounding dental tissue (dentin) was evaluated using femtosecond laser-induced breakdown spectroscopy (fs-LIBS). To achieve this, seven deciduous and eight permanent extracted human molar teeth with occlusal amalgam restorations were half-sectioned and analyzed using pulses from a femtosecond laser. The measurements were performed from the amalgam restoration along the amalgam/dentin interface to the apical direction. It was possible to observe the presence of metallic elements (silver, mercury, copper and tin) emission lines, as well as dental constituent ones, providing fingerprints of each material and comparable data for checking the consistence of the results. It was also shown that the elements penetration depth values in each tooth are usually similar and consistent, for both deciduous and permanent teeth, indicating that all the metals diffuse into the dentin by the same mechanism. We propose that this diffusion mechanism is mainly through liquid dragging inside the dentin tubules. The mercury diffused further in permanent teeth than in deciduous teeth, probably due to the longer diffusion times due to the age of the restorations. It was possible to conclude that the proposed femtosecond-LIBS system can detect the presence of metals in the dental tissue, among the tooth constituent elements, and map the distribution of endogenous and exogenous chemical elements, with a spatial resolution that can be brought under 100 µm.

  12. Coherent Exciton Dynamics in GaAs-Based Semiconductor Structures

    Science.gov (United States)

    Colocci, M.; Bogani, F.; Ceccherini, S.; Gurioli, M.

    We show that a very powerful tool in the investigation of the coherent exciton dynamics in semiconductors is provided by the study of the emitted light after resonant excitation from pairs of phase-locked femtosecond pulses. Under these conditions, not only the full dynamics of the coherent transients (dephasing times, quantum beat periods, etc.) can be obtained from linear experiments, but it can also be obtained a straightforward discrimination between the coherent or incoherent character of the emission by means of spectral filtering.

  13. Femtosecond Photon-Counting Receiver

    Science.gov (United States)

    Krainak, Michael A.; Rambo, Timothy M.; Yang, Guangning; Lu, Wei; Numata, Kenji

    2016-01-01

    An optical correlation receiver is described that provides ultra-precise distance and/or time/pulse-width measurements even for weak (single photons) and short (femtosecond) optical signals. A new type of optical correlation receiver uses a fourth-order (intensity) interferometer to provide micron distance measurements even for weak (single photons) and short (femtosecond) optical signals. The optical correlator uses a low-noise-integrating detector that can resolve photon number. The correlation (range as a function of path delay) is calculated from the variance of the photon number of the difference of the optical signals on the two detectors. Our preliminary proof-of principle data (using a short-pulse diode laser transmitter) demonstrates tens of microns precision.

  14. Femtosecond few-cycle mid-infrared laser pulses

    DEFF Research Database (Denmark)

    Liu, Xing

    The few-cycle pulses of mid-infrared (mid-IR, wavelength 2-10 microns) have attracted increasing attention owing to their great potentials for high order harmonic generation, time-resolved spectroscopy, precision of cutting and biomedical science.In this thesis, mid-IR frequency conversion.......2 - 5.5 μm with only one fixed pump wavelength, a feature absent in Kerr media. Finally, we experimentally observe supercontinuum generation spanning 1.5 octaves, generated in a 10 mm long silicon-rich nitride waveguide pumped by 100 pJ femtosecond pulses from an erbium fiber laser. The waveguide has...

  15. Coherent detectors

    International Nuclear Information System (INIS)

    Lawrence, C R; Church, S; Gaier, T; Lai, R; Ruf, C; Wollack, E

    2009-01-01

    Coherent systems offer significant advantages in simplicity, testability, control of systematics, and cost. Although quantum noise sets the fundamental limit to their performance at high frequencies, recent breakthroughs suggest that near-quantum-limited noise up to 150 or even 200 GHz could be realized within a few years. If the demands of component separation can be met with frequencies below 200 GHz, coherent systems will be strong competitors for a space CMB polarization mission. The rapid development of digital correlator capability now makes space interferometers with many hundreds of elements possible. Given the advantages of coherent interferometers in suppressing systematic effects, such systems deserve serious study.

  16. Coherent detectors

    Energy Technology Data Exchange (ETDEWEB)

    Lawrence, C R [M/C 169-327, Jet Propulsion Laboratory, 4800 Oak Grove Drive, Pasadena, CA 91109 (United States); Church, S [Room 324 Varian Physics Bldg, 382 Via Pueblo Mall, Stanford, CA 94305-4060 (United States); Gaier, T [M/C 168-314, Jet Propulsion Laboratory, 4800 Oak Grove Drive, Pasadena, CA 91109 (United States); Lai, R [Northrop Grumman Corporation, Redondo Beach, CA 90278 (United States); Ruf, C [1533 Space Research Building, The University of Michigan, Ann Arbor, MI 48109-2143 (United States); Wollack, E, E-mail: charles.lawrence@jpl.nasa.go [NASA/GSFC, Code 665, Observational Cosmology Laboratory, Greenbelt, MD 20771 (United States)

    2009-03-01

    Coherent systems offer significant advantages in simplicity, testability, control of systematics, and cost. Although quantum noise sets the fundamental limit to their performance at high frequencies, recent breakthroughs suggest that near-quantum-limited noise up to 150 or even 200 GHz could be realized within a few years. If the demands of component separation can be met with frequencies below 200 GHz, coherent systems will be strong competitors for a space CMB polarization mission. The rapid development of digital correlator capability now makes space interferometers with many hundreds of elements possible. Given the advantages of coherent interferometers in suppressing systematic effects, such systems deserve serious study.

  17. Femtosecond laser pulses for fast 3-D surface profilometry of microelectronic step-structures.

    Science.gov (United States)

    Joo, Woo-Deok; Kim, Seungman; Park, Jiyong; Lee, Keunwoo; Lee, Joohyung; Kim, Seungchul; Kim, Young-Jin; Kim, Seung-Woo

    2013-07-01

    Fast, precise 3-D measurement of discontinuous step-structures fabricated on microelectronic products is essential for quality assurance of semiconductor chips, flat panel displays, and photovoltaic cells. Optical surface profilers of low-coherence interferometry have long been used for the purpose, but the vertical scanning range and speed are limited by the micro-actuators available today. Besides, the lateral field-of-view extendable for a single measurement is restricted by the low spatial coherence of broadband light sources. Here, we cope with the limitations of the conventional low-coherence interferometer by exploiting unique characteristics of femtosecond laser pulses, i.e., low temporal but high spatial coherence. By scanning the pulse repetition rate with direct reference to the Rb atomic clock, step heights of ~69.6 μm are determined with a repeatability of 10.3 nm. The spatial coherence of femtosecond pulses provides a large field-of-view with superior visibility, allowing for a high volume measurement rate of ~24,000 mm3/s.

  18. Coherent wavepackets in the Fenna-Matthews-Olson complex are robust to excitonic-structure perturbations caused by mutagenesis

    Science.gov (United States)

    Maiuri, Margherita; Ostroumov, Evgeny E.; Saer, Rafael G.; Blankenship, Robert E.; Scholes, Gregory D.

    2018-02-01

    Femtosecond pulsed excitation of light-harvesting complexes creates oscillatory features in their response. This phenomenon has inspired a large body of work aimed at uncovering the origin of the coherent beatings and possible implications for function. Here we exploit site-directed mutagenesis to change the excitonic level structure in Fenna-Matthews-Olson (FMO) complexes and compare the coherences using broadband pump-probe spectroscopy. Our experiments detect two oscillation frequencies with dephasing on a picosecond timescale—both at 77 K and at room temperature. By studying these coherences with selective excitation pump-probe experiments, where pump excitation is in resonance only with the lowest excitonic state, we show that the key contributions to these oscillations stem from ground-state vibrational wavepackets. These experiments explicitly show that the coherences—although in the ground electronic state—can be probed at the absorption resonances of other bacteriochlorophyll molecules because of delocalization of the electronic excitation over several chromophores.

  19. Coherent anti-Stokes Raman scattering microscopy with a photonic crystal fiber based light source

    DEFF Research Database (Denmark)

    Paulsen, H.N.; Hilligsøe, Karen Marie; Thøgersen, J.

    2003-01-01

    A coherent anti-Stokes Raman scattering microscope based on a Ti:sapphire femtosecond oscillator and a photonic crystal fiber is demonstrated. The nonlinear response of the fiber is used to generate the additional wavelength needed in the Raman process. The applicability of the setup is demonstra......A coherent anti-Stokes Raman scattering microscope based on a Ti:sapphire femtosecond oscillator and a photonic crystal fiber is demonstrated. The nonlinear response of the fiber is used to generate the additional wavelength needed in the Raman process. The applicability of the setup...

  20. Nanosecond retinal structure changes in K-590 during the room-temperature bacteriorhodopsin photocycle: picosecond time-resolved coherent anti-stokes Raman spectroscopy

    OpenAIRE

    Weidlich, O.; Ujj, L.; Jäger, F.; Atkinson, G.H.

    1997-01-01

    Time-resolved vibrational spectra are used to elucidate the structural changes in the retinal chromophore within the K-590 intermediate that precedes the formation of the L-550 intermediate in the room-temperature (RT) bacteriorhodopsin (BR) photocycle. Measured by picosecond time-resolved coherent anti-Stokes Raman scattering (PTR/CARS), these vibrational data are recorded within the 750 cm-1 to 1720 cm-1 spectral region and with time delays of 50-260 ns after the RT/BR photocycle is optical...

  1. Femtosecond laser ablation of gold interdigitated electrodes for electronic tongues

    Science.gov (United States)

    Manzoli, Alexandra; de Almeida, Gustavo F. B.; Filho, José A.; Mattoso, Luiz H. C.; Riul, Antonio; Mendonca, Cleber R.; Correa, Daniel S.

    2015-06-01

    Electronic tongue (e-tongue) sensors based on impedance spectroscopy have emerged as a potential technology to evaluate the quality and chemical composition of food, beverages, and pharmaceuticals. E-tongues usually employ transducers based on metal interdigitated electrodes (IDEs) coated with a thin layer of an active material, which is capable of interacting chemically with several types of analytes. IDEs are usually produced by photolithographic methods, which are time-consuming and costly, therefore, new fabrication technologies are required to make it more affordable. Here, we employed femtosecond laser ablation with pulse duration of 50 fs to microfabricate gold IDEs having finger width from 2.3 μm up to 3.2 μm. The parameters used in the laser ablation technique, such as light intensity, scan speed and beam spot size have been optimized to achieve uniform IDEs, which were characterized by optical and scanning electron microscopy. The electrical properties of gold IDEs fabricated by laser ablation were evaluated by impedance spectroscopy, and compared to those produced by conventional photolithography. The results show that femtosecond laser ablation is a promising alternative to conventional photolithography for fabricating metal IDEs for e-tongue systems.

  2. Characterization of temporal coherence of hard X-ray free-electron laser pulses with single-shot interferograms

    Directory of Open Access Journals (Sweden)

    Taito Osaka

    2017-11-01

    Full Text Available Temporal coherence is one of the most fundamental characteristics of light, connecting to spectral information through the Fourier transform relationship between time and frequency. Interferometers with a variable path-length difference (PLD between the two branches have widely been employed to characterize temporal coherence properties for broad spectral regimes. Hard X-ray interferometers reported previously, however, have strict limitations in their operational photon energies, due to the specific optical layouts utilized to satisfy the stringent requirement for extreme stability of the PLD at sub-ångström scales. The work presented here characterizes the temporal coherence of hard X-ray free-electron laser (XFEL pulses by capturing single-shot interferograms. Since the stability requirement is drastically relieved with this approach, it was possible to build a versatile hard X-ray interferometer composed of six separate optical elements to cover a wide photon energy range from 6.5 to 11.5 keV while providing a large variable delay time of up to 47 ps at 10 keV. A high visibility of up to 0.55 was observed at a photon energy of 10 keV. The visibility measurement as a function of time delay reveals a mean coherence time of 5.9 ± 0.7 fs, which agrees with that expected from the single-shot spectral information. This is the first result of characterizing the temporal coherence of XFEL pulses in the hard X-ray regime and is an important milestone towards ultra-high energy resolutions at micro-electronvolt levels in time-domain X-ray spectroscopy, which will open up new opportunities for revealing dynamic properties in diverse systems on timescales from femtoseconds to nanoseconds, associated with fluctuations from ångström to nanometre spatial scales.

  3. Femtosecond Timekeeping: Slip-Free Clockwork for Optical Timescales

    Science.gov (United States)

    Herman, D.; Droste, S.; Baumann, E.; Roslund, J.; Churin, D.; Cingoz, A.; Deschênes, J.-D.; Khader, I. H.; Swann, W. C.; Nelson, C.; Newbury, N. R.; Coddington, I.

    2018-04-01

    The generation of true optical time standards will require the conversion of the highly stable optical-frequency output of an optical atomic clock to a high-fidelity time output. We demonstrate a comb-based clockwork that phase-coherently integrates ˜7 ×1020 optical cycles of an input optical frequency to create a coherent time output. We verify the underlying stability of the optical timing system by comparing two comb-based clockworks with a common input optical frequency and show time drift over the 37-day measurement period. Both clockworks also generate traditional timing signals including an optical pulse per second and a 10-MHz rf reference. The optical pulse-per-second time outputs remain synchronized to 240 attoseconds (240 as) at 1000 s. The phase-coherent 10-MHz rf outputs are stable to near a part in 1019 . Fault-free timekeeping from an optical clock to femtosecond level over months is an important step in replacing the current microwave time standard by an optical standard.

  4. High-coherence mid-infrared dual-comb spectroscopy spanning 2.6 to 5.2 μm

    Science.gov (United States)

    Ycas, Gabriel; Giorgetta, Fabrizio R.; Baumann, Esther; Coddington, Ian; Herman, Daniel; Diddams, Scott A.; Newbury, Nathan R.

    2018-04-01

    Mid-infrared dual-comb spectroscopy has the potential to supplant conventional Fourier-transform spectroscopy in applications requiring high resolution, accuracy, signal-to-noise ratio and speed. Until now, mid-infrared dual-comb spectroscopy has been limited to narrow optical bandwidths or low signal-to-noise ratios. Using digital signal processing and broadband frequency conversion in waveguides, we demonstrate a mid-infrared dual-comb spectrometer covering 2.6 to 5.2 µm with comb-tooth resolution, sub-MHz frequency precision and accuracy, and a spectral signal-to-noise ratio as high as 6,500. As a demonstration, we measure the highly structured, broadband cross-section of propane from 2,840 to 3,040 cm-1, the complex phase/amplitude spectra of carbonyl sulfide from 2,000 to 2,100 cm-1, and of a methane, acetylene and ethane mixture from 2,860 to 3,400 cm-1. The combination of broad bandwidth, comb-mode resolution and high brightness will enable accurate mid-infrared spectroscopy in precision laboratory experiments and non-laboratory applications including open-path atmospheric gas sensing, process monitoring and combustion.

  5. Nanoflow electrospinning serial femtosecond crystallography

    Science.gov (United States)

    Sierra, Raymond G.; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W.; Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W.; Sellberg, Jonas; McQueen, Trevor A.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H.; Glatzel, Pieter; Milathianaki, Despina; White, William E.; Adams, Paul D.; Williams, Garth J.; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K.; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K.; Bogan, Michael J.

    2012-01-01

    An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min−1 to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min−1 and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption. PMID:23090408

  6. Generating femtosecond X-ray pulses using an emittance-spoiling foil in free-electron lasers

    Energy Technology Data Exchange (ETDEWEB)

    Ding, Y., E-mail: ding@slac.stanford.edu; Coffee, R.; Decker, F.-J.; Emma, P.; Field, C.; Huang, Z.; Krejcik, P.; Krzywinski, J.; Loos, H.; Lutman, A.; Marinelli, A.; Maxwell, T. J.; Turner, J. [SLAC National Accelerator Laboratory, Menlo Park, California 94025 (United States); Behrens, C. [Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg (Germany); Helml, W. [Technische Universität München, James-Franck-Straße 1, 85748 Garching (Germany)

    2015-11-09

    Generation of femtosecond to sub-femtosecond pulses is attracting much attention in X-ray free-electron laser user community. One method is to use a slotted, emittance-spoiling foil which was proposed before (P. Emma et al., Phys. Rev. Lett. 92, 074801 (2004)) and has been widely used at the Linac Coherent Light Source. Direct experimental characterization of the slotted-foil performance was previously unfeasible due to a lack of appropriate diagnostics. With a recently installed X-band radio-frequency transverse deflector, we are able to characterize the electron bunch spoiling effect and X-ray pulse when using the slotted foil. We show that few-femtosecond X-ray pulses are generated with flexible control of the single-pulse duration or double-pulse separation with comparison to the theoretical model.

  7. Communication: The electronic structure of matter probed with a single femtosecond hard x-ray pulse

    Directory of Open Access Journals (Sweden)

    J. Szlachetko

    2014-03-01

    Full Text Available Physical, biological, and chemical transformations are initiated by changes in the electronic configuration of the species involved. These electronic changes occur on the timescales of attoseconds (10−18 s to femtoseconds (10−15 s and drive all subsequent electronic reorganization as the system moves to a new equilibrium or quasi-equilibrium state. The ability to detect the dynamics of these electronic changes is crucial for understanding the potential energy surfaces upon which chemical and biological reactions take place. Here, we report on the determination of the electronic structure of matter using a single self-seeded femtosecond x-ray pulse from the Linac Coherent Light Source hard x-ray free electron laser. By measuring the high energy resolution off-resonant spectrum (HEROS, we were able to obtain information about the electronic density of states with a single femtosecond x-ray pulse. We show that the unoccupied electronic states of the scattering atom may be determined on a shot-to-shot basis and that the measured spectral shape is independent of the large intensity fluctuations of the incoming x-ray beam. Moreover, we demonstrate the chemical sensitivity and single-shot capability and limitations of HEROS, which enables the technique to track the electronic structural dynamics in matter on femtosecond time scales, making it an ideal probe technique for time-resolved X-ray experiments.

  8. Coherent dynamics in semiconductors

    DEFF Research Database (Denmark)

    Hvam, Jørn Märcher

    1998-01-01

    enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic......Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further...... and molecular systems are found and studied in the exciton-biexciton system of semiconductors. At densities where strong exciton interactions, or many-body effects, become dominant, the semiconductor Bloch equations present a more rigorous treatment of the phenomena Ultrafast degenerate four-wave mixing is used...

  9. Electronic resonances in broadband stimulated Raman spectroscopy

    Science.gov (United States)

    Batignani, G.; Pontecorvo, E.; Giovannetti, G.; Ferrante, C.; Fumero, G.; Scopigno, T.

    2016-01-01

    Spontaneous Raman spectroscopy is a formidable tool to probe molecular vibrations. Under electronic resonance conditions, the cross section can be selectively enhanced enabling structural sensitivity to specific chromophores and reaction centers. The addition of an ultrashort, broadband femtosecond pulse to the excitation field allows for coherent stimulation of diverse molecular vibrations. Within such a scheme, vibrational spectra are engraved onto a highly directional field, and can be heterodyne detected overwhelming fluorescence and other incoherent signals. At variance with spontaneous resonance Raman, however, interpreting the spectral information is not straightforward, due to the manifold of field interactions concurring to the third order nonlinear response. Taking as an example vibrational spectra of heme proteins excited in the Soret band, we introduce a general approach to extract the stimulated Raman excitation profiles from complex spectral lineshapes. Specifically, by a quantum treatment of the matter through density matrix description of the third order nonlinear polarization, we identify the contributions which generate the Raman bands, by taking into account for the cross section of each process.

  10. Femtosecond versus nanosecond laser machining: comparison of induced stresses and structural changes in silicon wafers

    International Nuclear Information System (INIS)

    Amer, M.S.; El-Ashry, M.A.; Dosser, L.R.; Hix, K.E.; Maguire, J.F.; Irwin, Bryan

    2005-01-01

    Laser micromachining has proven to be a very successful tool for precision machining and microfabrication with applications in microelectronics, MEMS, medical device, aerospace, biomedical, and defense applications. Femtosecond (FS) laser micromachining is usually thought to be of minimal heat-affected zone (HAZ) local to the micromachined feature. The assumption of reduced HAZ is attributed to the absence of direct coupling of the laser energy into the thermal modes of the material during irradiation. However, a substantial HAZ is thought to exist when machining with lasers having pulse durations in the nanosecond (NS) regime. In this paper, we compare the results of micromachining a single crystal silicon wafer using a 150-femtosecond and a 30-nanosecond lasers. Induced stress and amorphization of the silicon single crystal were monitored using micro-Raman spectroscopy as a function of the fluence and pulse duration of the incident laser. The onset of average induced stress occurs at lower fluence when machining with the femtosecond pulse laser. Induced stresses were found to maximize at fluence of 44 J cm -2 and 8 J cm -2 for nanosecond and femtosecond pulsed lasers, respectively. In both laser pulse regimes, a maximum induced stress is observed at which point the induced stress begins to decrease as the fluence is increased. The maximum induced stress was comparable at 2.0 GPa and 1.5 GPa for the two lasers. For the nanosecond pulse laser, the induced amorphization reached a plateau of approximately 20% for fluence exceeding 22 J cm -2 . For the femtosecond pulse laser, however, induced amorphization was approximately 17% independent of the laser fluence within the experimental range. These two values can be considered nominally the same within experimental error. For femtosecond laser machining, some effect of the laser polarization on the amount of induced stress and amorphization was also observed

  11. Correction for the time dependent inner filter effect caused by transient absorption in femtosecond stimulated Raman experiment

    NARCIS (Netherlands)

    Kloz, M.; van Grondelle, R.; Kennis, J.T.M.

    2012-01-01

    Femtosecond stimulated Raman spectroscopy (FSRS) is a promising multiple-pulse ultrafast spectroscopic tool whose simplest form utilizes an actinic pump, a Raman pump and a continuum probe. Here, we report that the transient absorption generated by the actinic pulse modulates the overall magnitude

  12. [The Detection of Ultra-Broadband Terahertz Spectroscopy of InP Wafer by Using Coherent Heterodyne Time-Domain Spectrometer].

    Science.gov (United States)

    Zhang, Liang-liang; Zhang, Rui; Xu, Xiao-yan; Zhang, Cun-lin

    2016-02-01

    Indium Phosphide (InP) has attracted great physical interest because of its unique characteristics and is indispensable to both optical and electronic devices. However, the optical property of InP in the terahertz range (0. 110 THz) has not yet been fully characterized and systematically studied. The former researches about the properties of InP concentrated on the terahertz frequency between 0.1 and 4 THz. The terahertz optical properties of the InP in the range of 4-10 THz are still missing. It is fairly necessary to fully understand its properties in the entire terahertz range, which results in a better utilization as efficient terahertz devices. In this paper, we study the optical properties of undoped (100) InP wafer in the ultra-broad terahertz frequency range (0.5-18 THz) by using air-biased-coherent-detection (ABCD) system, enabling the coherent detection of terahertz wave in gases, which leads to a significant improvement on the dynamic range and sensitivity of the system. The advantage of this method is broad frequency bandwidth from 0.2 up to 18 THz which is only mainly limited by laser pulse duration since it uses ionized air as terahertz emitter and detector instead of using an electric optical crystal or photoconductive antenna. The terahertz pulse passing through the InP wafer is delayed regarding to the reference pulse and has much lower amplitude. In addition, the frequency spectrum amplitude of the terahertz sample signal drops to the noise floor level from 6.7 to 12.1 THz. At the same time InP wafer is opaque at the frequencies spanning from 6.7 to 12.1 THz. In the frequency regions of 0.8-6.7 and 12.1-18 THz it has relativemy low absorption coefficient. Meanwhile, the refractive index increases monotonously in the 0.8-6.7 THz region and 12.1-18 THz region. These findings will contribute to the design of InP based on nonlinear terahertz devices.

  13. Effects of emittance and space-charge in femtosecond bunch compression

    International Nuclear Information System (INIS)

    Kan, K.; Yang, J.; Kondoh, T.; Norizawa, K.; Yoshida, Y.

    2008-01-01

    Ultrashort electron bunches of the order of <100fs are essential for the study of ultrafast reactions and phenomena by means of time-resolved pump-probe experiments. In order to generate such an electron bunch, the effects of emittance, space-charge (SC) and coherent synchrotron radiation (CSR) on the bunch length in a femtosecond magnetic bunch compressor were studied theoretically. It was observed that the bunch length is dominated by the emittance, SC and CSR effects when the electron bunch is compressed into a femtosecond electron bunch. The increases in bunch length due to the transverse emittance, SC and CSR effects in the bunch compressor were 1.7 fs/mm mrad, 107 fs/nC and 72 fs/nC, respectively. Finally, the simulated bunch length was compared with the experimental results.

  14. Femtosecond Time-Resolved Resonance-Enhanced CARS of Gaseous Iodine at Room Temperature

    International Nuclear Information System (INIS)

    He Ping; Fan Rong-Wei; Xia Yuan-Qin; Yu Xin; Chen De-Ying; Yao Yong

    2011-01-01

    Time-resolved resonance-enhanced coherent anti-Stokes Raman scattering (CARS) is applied to investigate molecular dynamics in gaseous iodine. 40 fs laser pulses are applied to create and monitor the high vibrational states of iodine at room temperature (corresponding to a vapor pressure as low as about 35 Pa) by femtosecond time-resolved CARS. Depending on the time delay between the probe pulse and the pump/Stokes pulse pairs, the high vibrational states both on the electronically ground states and the excited states can be detected as oscillations in the CARS transient signal. It is proved that the femtosecond time-resolved CARS technique is a promising candidate for investigating the molecular dynamics of a low concentration system and can be applied to environmental and atmospheric monitoring measurements. (condensed matter: electronic structure, electrical, magnetic, and optical properties)

  15. The art of femtosecond laser writing

    OpenAIRE

    Kazansky, Peter G.; Yang, Weijia; Shimotsuma, Yasuhiko; Hirao, Kazuyuki; Arai, Alan; Svirko, Yuri P.

    2009-01-01

    Common beliefs that laser writing does not change when reversing beam scan or propagation direction are challenged. Recently discovered phenomena of quill and non-reciprocal femtosecond laser writing in glasses and crystals are reviewed

  16. Avant-garde femtosecond laser writing

    OpenAIRE

    Kazansky, Peter G.; Beresna, Martynas; Shimotsuma, Yasuhiko; Hirao, Kazuyuki; Svirko, Yuri P.; Aktürk, Selcuk

    2010-01-01

    Recently discovered phenomena of quill and non-reciprocal femtosecond laser writing in glasses and crystals are reviewed. Common beliefs that laser writing does not change when reversing beam scan or propagation direction are challenged.

  17. Programmable femtosecond laser pulses in the ultraviolet

    International Nuclear Information System (INIS)

    Hacker, M.; Feurer, T.; Sauerbrey, R.; Lucza, T.; Szabo, G.

    2001-01-01

    Using a combination of a zero-dispersion compressor and spectrally compensated sum-frequency generation, we have produced amplitude-modulated femtosecond pulses in the UV at 200 nm. [copyright] 2001 Optical Society of America

  18. Coherence and Sense of Coherence

    DEFF Research Database (Denmark)

    Dau, Susanne

    2014-01-01

    Constraints in the implementation of models of blended learning can be explained by several causes, but in this paper, it is illustrated that lack of sense of coherence is a major factor of these constraints along with the referential whole of the perceived learning environments. The question exa...

  19. Multidimensional high harmonic spectroscopy

    International Nuclear Information System (INIS)

    Bruner, Barry D; Soifer, Hadas; Shafir, Dror; Dudovich, Nirit; Serbinenko, Valeria; Smirnova, Olga

    2015-01-01

    High harmonic generation (HHG) has opened up a new frontier in ultrafast science where attosecond time resolution and Angstrom spatial resolution are accessible in a single measurement. However, reconstructing the dynamics under study is limited by the multiple degrees of freedom involved in strong field interactions. In this paper we describe a new class of measurement schemes for resolving attosecond dynamics, integrating perturbative nonlinear optics with strong-field physics. These approaches serve as a basis for multidimensional high harmonic spectroscopy. Specifically, we show that multidimensional high harmonic spectroscopy can measure tunnel ionization dynamics with high precision, and resolves the interference between multiple ionization channels. In addition, we show how multidimensional HHG can function as a type of lock-in amplifier measurement. Similar to multi-dimensional approaches in nonlinear optical spectroscopy that have resolved correlated femtosecond dynamics, multi-dimensional high harmonic spectroscopy reveals the underlying complex dynamics behind attosecond scale phenomena. (paper)

  20. Femtosecond laser-induced herringbone patterns

    Science.gov (United States)

    Garcell, Erik M.; Lam, Billy; Guo, Chunlei

    2018-06-01

    Femtosecond laser-induced herringbone patterns are formed on copper (Cu). These novel periodic structures are created following s-polarized, large incident angle, femtosecond laser pulses. Forming as slanted and axially symmetric laser-induced periodic surface structures along the side walls of ablated channels, the result is a series of v-shaped structures that resemble a herringbone pattern. Fluence mapping, incident angle studies, as well as polarization studies have been conducted and provide a clear understanding of this new structure.

  1. Electron Bunch Length Diagnostic With Coherent Smith-Purcell Radiation

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, D.C.

    1997-05-12

    The authors have designed a new technique for measuring subpicosecond electron bunch lengths using coherent Smith-Purcell radiation. This new diagnostic technique involves passing the electron beam in close proximity of a grating with a period comparable to the electron bunch length. The emitted Smith-Purcell radiation will have a coherent component whose angular position and distribution are directly related to the electron bunch length and longitudinal profile, respectively. This new diagnostic technique is inherently simple, inexpensive and non-intercepting. The authors show that the new technique is also scaleable to femtosecond regime.

  2. Electron Bunch Length Diagnostic With Coherent Smith-Purcell Radiation

    International Nuclear Information System (INIS)

    Nguyen, D.C.

    1997-01-01

    The authors have designed a new technique for measuring subpicosecond electron bunch lengths using coherent Smith-Purcell radiation. This new diagnostic technique involves passing the electron beam in close proximity of a grating with a period comparable to the electron bunch length. The emitted Smith-Purcell radiation will have a coherent component whose angular position and distribution are directly related to the electron bunch length and longitudinal profile, respectively. This new diagnostic technique is inherently simple, inexpensive and non-intercepting. The authors show that the new technique is also scaleable to femtosecond regime

  3. Transient grating spectroscopy in photosynthetic purple bacteria Rhodobacter sphaeroides 2.4.1

    Energy Technology Data Exchange (ETDEWEB)

    Sugisaki, Mitsuru, E-mail: mitsuru@sci.osaka-cu.ac.j [CREST-JST and Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi, Osaka 558-8585 (Japan); Fujiwara, Masazumi; Fujii, Ritsuko [CREST-JST and Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi, Osaka 558-8585 (Japan); Nakagawa, Katsunori; Nango, Mamoru [CREST-JST and Graduate School of Engineering, Nagoya Institute of Technology, Gokiso, Showa, Nagoya 466-8555 (Japan); Cogdell, Richard J. [Glasgow Biomedical Research Centre, IBLS, University of Glasgow, 126 University Place, Glasgow G12 8TA, Scotland (United Kingdom); Hashimoto, Hideki [CREST-JST and Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi, Osaka 558-8585 (Japan)

    2009-12-15

    The vibronic coherence of photosynthetic pigment-protein complexes has been investigated by means of transient grating spectroscopy using sub 20 fs optical pulses. In the present work, we focus our attention on the LH2 antenna complexes from Rhodobacter sphaeroides 2.4.1 because the information about their structure investigated by the electron and atomic force microscopy is available and the electric levels of pigments are well resolved, resulting in clear absorption spectrum. The vibronic coherent oscillations with a period of a few tens of femtoseconds have been clearly observed. We found that the temporal change of the coherent oscillations reflects the vibrational relaxation in the ground state. Calculations based on the Brownian oscillator model were performed under the impulsive excitation limit. The spectral density has been determined from the Raman measurement of spheroidene. Good agreement between the calculation and the experimental results has been achieved in the linear absorption spectrum and transient grating signal, which strongly supports the validity of our model.

  4. Photoemission using femtosecond laser pulses

    International Nuclear Information System (INIS)

    Srinivasan-Rao, T.; Tsang, T.; Fischer, J.

    1991-10-01

    Successful operation of short wavelength FEL requires an electron bunch of current >100 A and normalized emittance < 1 mm-mrad. Recent experiments show that RF guns with photocathodes as the electron source may be the ideal candidate for achieving these parameters. To reduce the emittance growth due to space charge and RF dynamics effects, the gun may have to operate at high field gradient (hence at high RF frequency) and a spot size small compared to the aperture. This may necessitate the laser pulse duration to be in the subpicosecond regime to reduce the energy spread. We will present the behavior of metal photocathodes upon irradiation with femtosecond laser beams, comparison of linear and nonlinear photoemission, and scalability to high currents. Theoretical estimate of the intrinsic emittance at the photocathode in the presence of the anomalous heating of the electrons, and the tolerance on the surface roughness of the cathode material will be discussed

  5. 2 micron femtosecond fiber laser

    Science.gov (United States)

    Liu, Jian; Wan, Peng; Yang, Lihmei

    2014-07-29

    Methods and systems for generating femtosecond fiber laser pulses are disclose, including generating a signal laser pulse from a seed laser oscillator; using a first amplifier stage comprising an input and an output, wherein the signal laser pulse is coupled into the input of the first stage amplifier and the output of the first amplifier stage emits an amplified and stretched signal laser pulse; using an amplifier chain comprising an input and an output, wherein the amplified and stretched signal laser pulse from the output of the first amplifier stage is coupled into the input of the amplifier chain and the output of the amplifier chain emits a further amplified, stretched signal laser pulse. Other embodiments are described and claimed.

  6. Fabrication of polycrystalline diamond refractive X-ray lens by femtosecond laser processing

    Energy Technology Data Exchange (ETDEWEB)

    Kononenko, T.V.; Ralchenko, V.G.; Ashkinazi, E.E.; Konov, V.I. [General Physics Institute of Russian Academy of Sciences, Moscow (Russian Federation); National Research Nuclear University ' ' MEPhI' ' , Moscow (Russian Federation); Polikarpov, M.; Ershov, P. [Immanuel Kant Baltic Federal University, Functional Nanomaterials, Kaliningrad (Russian Federation); Kuznetsov, S.; Yunkin, V. [Institute of Microelectronics Technology RAS, Chernogolovka, Moscow region (Russian Federation); Snigireva, I. [European Synchrotron Radiation Facility, Grenoble (France)

    2016-03-15

    X-ray planar compound refractive lenses were fabricated from a polycrystalline diamond plate grown by chemical vapor deposition, by precise through cutting with femtosecond laser pulses. The lens geometry and the surface morphology were investigated with optical and scanning electron microscopy, while the material structure modification was analyzed by Raman spectroscopy. The results of the preliminary lens test at 9.25-keV X-rays are presented. (orig.)

  7. Fabrication of polycrystalline diamond refractive X-ray lens by femtosecond laser processing

    International Nuclear Information System (INIS)

    Kononenko, T.V.; Ralchenko, V.G.; Ashkinazi, E.E.; Konov, V.I.; Polikarpov, M.; Ershov, P.; Kuznetsov, S.; Yunkin, V.; Snigireva, I.

    2016-01-01

    X-ray planar compound refractive lenses were fabricated from a polycrystalline diamond plate grown by chemical vapor deposition, by precise through cutting with femtosecond laser pulses. The lens geometry and the surface morphology were investigated with optical and scanning electron microscopy, while the material structure modification was analyzed by Raman spectroscopy. The results of the preliminary lens test at 9.25-keV X-rays are presented. (orig.)

  8. Coherent combination of ultrafast fiber amplifiers

    International Nuclear Information System (INIS)

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

    2016-01-01

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

  9. Contrasting organic aerosol particles from boreal and tropical forests during HUMPPA-COPEC-2010 and AMAZE-08 using coherent vibrational spectroscopy

    Directory of Open Access Journals (Sweden)

    C. J. Ebben

    2011-10-01

    Full Text Available We present the vibrational sum frequency generation spectra of organic particles collected in a boreal forest in Finland and a tropical forest in Brazil. These spectra are compared to those of secondary organic material produced in the Harvard Environmental Chamber. By comparing coherent vibrational spectra of a variety of terpene and olefin reference compounds, along with the secondary organic material synthesized in the environmental chamber, we show that submicron aerosol particles sampled in Southern Finland during HUMPPA-COPEC-2010 are composed to a large degree of material similar in chemical composition to synthetic α-pinene-derived material. For material collected in Brazil as part of AMAZE-08, the organic component is found to be chemically complex in the coarse mode but highly uniform in the fine mode. When combined with histogram analyses of the isoprene and monoterpene abundance recorded during the HUMPPA-COPEC-2010 and AMAZE-08 campaigns, the findings presented here indicate that if air is rich in monoterpenes, submicron-sized secondary aerosol particles that form under normal OH and O3 concentration levels can be described in terms of their hydrocarbon content as being similar to α-pinene-derived model secondary organic aerosol particles. If the isoprene concentration dominates the chemical composition of organic compounds in forest air, then the hydrocarbon component of secondary organic material in the submicron size range is not simply well-represented by that of isoprene-derived model secondary organic aerosol particles but is more complex. Throughout the climate-relevant size range of the fine mode, however, we find that the chemical composition of the secondary organic particle material from such air is invariant with size, suggesting that the particle growth does not change the chemical composition of the hydrocarbon component of the particles in a significant way.

  10. Vibrational spectrum of the K-590 intermediate in the bacteriorhodopsin photocycle at room temperature: picosecond time-resolved resonance coherent anti-Raman spectroscopy

    Science.gov (United States)

    Ujj, L.; Jäger, F.; Popp, A.; Atkinson, G. H.

    1996-12-01

    The vibrational spectrum of the K-590 intermediate, thought to contribute significantly to the energy storage and transduction mechanism in the bacteriorhodopsin (BR) photocycle, is measured at room temperature using picosecond time-resolved resonance coherent anti-Stokes Raman scattering (PTR/CARS). The room-temperature BR photocycle is initiated by the 3 ps, 570 nm excitation of the ground-state species, BR-570, prepared in both H 2O and D 2O suspensions of BR. PTR/CARS data, recorded 50 ps after BR-570 excitation, at which time only BR-570 and K-590 are present, have an excellent S/N which provides a significantly more detailed view of the K-590 vibrational degrees of freedom than previously available. Two picosecond (6 ps FWHM) laser pulses, ω1 (633.4 nm) and ωS (675-700 nm), are used to record PTR/CARS data via electronic resonance enhancement in both BR-570 and K-590, each of which contains a distinct retinal structure (assigned as 13- rans, 15- anti, 13- cis, respectively). To obtain the vibrational spectrum of K-590 separately, the PTR/CARS spectra from the mixture of isomeric retinals is quantitatively analyzed in terms of third-order susceptibility ( η(3)) relationships. PTR/CARS spectra of K-590 recorded from both H 2O and D 2O suspensions of BR are compared with the analogous vibrational data obtained via spontaneous resonance Raman (RR) scattering at both low (77 K) and room temperature. Analyses of these vibrational spectra identify temperature-dependent effects and changes assignable to the substitution of deuterium at the Schiff-base nitrogen not previously reported.

  11. 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

  12. 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.

  13. Pump pulse duration dependence of coherent phonon amplitudes in antimony

    Energy Technology Data Exchange (ETDEWEB)

    Misochko, O. V., E-mail: misochko@issp.ac.ru [Russian Academy of Sciences, Institute of Solid State Physics (Russian Federation)

    2016-08-15

    Coherent optical phonons of A{sub 1k} and E{sub k} symmetry in antimony have been studied using the femtosecond pump–probe technique. By varying the pump-pulse duration and keeping the probe duration constant, it was shown that the amplitude of coherent phonons of both symmetries exponentially decreases with increasing pulse width. It was found that the amplitude decay rate for the fully symmetric phonons with larger frequency is greater than that of the doubly degenerate phonons, whereas the frequency and lifetime for coherent phonons of both symmetries do not depend on the pump-pulse duration. Based on this data, the possibility of separation between dynamic and kinematic contributions to the generation mechanism of coherent phonons is discussed.

  14. Two-dimensional vibrational-electronic spectroscopy

    Science.gov (United States)

    Courtney, Trevor L.; Fox, Zachary W.; Slenkamp, Karla M.; Khalil, Munira

    2015-10-01

    Two-dimensional vibrational-electronic (2D VE) spectroscopy is a femtosecond Fourier transform (FT) third-order nonlinear technique that creates a link between existing 2D FT spectroscopies in the vibrational and electronic regions of the spectrum. 2D VE spectroscopy enables a direct measurement of infrared (IR) and electronic dipole moment cross terms by utilizing mid-IR pump and optical probe fields that are resonant with vibrational and electronic transitions, respectively, in a sample of interest. We detail this newly developed 2D VE spectroscopy experiment and outline the information contained in a 2D VE spectrum. We then use this technique and its single-pump counterpart (1D VE) to probe the vibrational-electronic couplings between high frequency cyanide stretching vibrations (νCN) and either a ligand-to-metal charge transfer transition ([FeIII(CN)6]3- dissolved in formamide) or a metal-to-metal charge transfer (MMCT) transition ([(CN)5FeIICNRuIII(NH3)5]- dissolved in formamide). The 2D VE spectra of both molecules reveal peaks resulting from coupled high- and low-frequency vibrational modes to the charge transfer transition. The time-evolving amplitudes and positions of the peaks in the 2D VE spectra report on coherent and incoherent vibrational energy transfer dynamics among the coupled vibrational modes and the charge transfer transition. The selectivity of 2D VE spectroscopy to vibronic processes is evidenced from the selective coupling of specific νCN modes to the MMCT transition in the mixed valence complex. The lineshapes in 2D VE spectra report on the correlation of the frequency fluctuations between the coupled vibrational and electronic frequencies in the mixed valence complex which has a time scale of 1 ps. The details and results of this study confirm the versatility of 2D VE spectroscopy and its applicability to probe how vibrations modulate charge and energy transfer in a wide range of complex molecular, material, and biological systems.

  15. Two-dimensional vibrational-electronic spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Courtney, Trevor L.; Fox, Zachary W.; Slenkamp, Karla M.; Khalil, Munira, E-mail: mkhalil@uw.edu [Department of Chemistry, University of Washington, Box 351700, Seattle, Washington 98195 (United States)

    2015-10-21

    Two-dimensional vibrational-electronic (2D VE) spectroscopy is a femtosecond Fourier transform (FT) third-order nonlinear technique that creates a link between existing 2D FT spectroscopies in the vibrational and electronic regions of the spectrum. 2D VE spectroscopy enables a direct measurement of infrared (IR) and electronic dipole moment cross terms by utilizing mid-IR pump and optical probe fields that are resonant with vibrational and electronic transitions, respectively, in a sample of interest. We detail this newly developed 2D VE spectroscopy experiment and outline the information contained in a 2D VE spectrum. We then use this technique and its single-pump counterpart (1D VE) to probe the vibrational-electronic couplings between high frequency cyanide stretching vibrations (ν{sub CN}) and either a ligand-to-metal charge transfer transition ([Fe{sup III}(CN){sub 6}]{sup 3−} dissolved in formamide) or a metal-to-metal charge transfer (MMCT) transition ([(CN){sub 5}Fe{sup II}CNRu{sup III}(NH{sub 3}){sub 5}]{sup −} dissolved in formamide). The 2D VE spectra of both molecules reveal peaks resulting from coupled high- and low-frequency vibrational modes to the charge transfer transition. The time-evolving amplitudes and positions of the peaks in the 2D VE spectra report on coherent and incoherent vibrational energy transfer dynamics among the coupled vibrational modes and the charge transfer transition. The selectivity of 2D VE spectroscopy to vibronic processes is evidenced from the selective coupling of specific ν{sub CN} modes to the MMCT transition in the mixed valence complex. The lineshapes in 2D VE spectra report on the correlation of the frequency fluctuations between the coupled vibrational and electronic frequencies in the mixed valence complex which has a time scale of 1 ps. The details and results of this study confirm the versatility of 2D VE spectroscopy and its applicability to probe how vibrations modulate charge and energy transfer in a

  16. Experimental investigation on the spiral trepanning of K24 superalloy with femtosecond laser

    Science.gov (United States)

    Wang, Maolu; Yang, Lijun; Zhang, Shuai; Wang, Yang

    2018-05-01

    Film cooling holes are crucial for improving the performance of the aviation engine. In the paper, the processing of the film cooling holes on K24 superalloy by femtosecond laser is investigated. By comparing the three different drilling methods, the spiral trepanning method is chosen, and all the drilling experiments are carried out in this way. The experimental results show that the drilling of femtosecond laser pulses has distinct merits against that of the traditional long pulse laser, which can realize the "cold" processing with less recasting layer and less crack. The influence of each process parameter on roundness and taper, which are the important parameters to measure the quality of holes, is analyzed in detail, and the method to decrease it is proposed. To further reduce the recasting layer, the processing quality of the inner wall of the micro hole is investigated by scanning electron microscopy (SEM) equipped with energy disperse spectroscopy (EDS), the mechanism of the femtosecond laser interaction with K24 superalloy is further revealed. The investigation to the film hole machining by femtosecond laser has important practical significance.

  17. Coherent Baryogenesis

    CERN Document Server

    Garbrecht, B; Schmidt, M G; Garbrecht, Bjorn; Prokopec, Tomislav; Schmidt, Michael G.

    2004-01-01

    We propose a new baryogenesis scenario based on coherent production and mixing of different fermionic species. The mechanism is operative during phase transitions, at which the fermions acquire masses via Yukawa couplings to scalar fields. Baryon production is efficient when the mass matrix is nonadiabatically varying, nonsymmetric and when it violates CP and B-L directly, or some other charges that are eventually converted to B-L. We first consider a toy model, which involves two mixing fermionic species, and then a hybrid inflationary scenario embedded in a supersymmetric Pati-Salam GUT. We show that, quite generically, a baryon excess in accordance with observation can result.

  18. Long distance measurement with a femtosecond laser based frequency comb

    Science.gov (United States)

    Bhattacharya, N.; Cui, M.; Zeitouny, M. G.; Urbach, H. P.; van den Berg, S. A.

    2017-11-01

    Recent advances in the field of ultra-short pulse lasers have led to the development of reliable sources of carrier envelope phase stabilized femtosecond pulses. The pulse train generated by such a source has a frequency spectrum that consists of discrete, regularly spaced lines known as a frequency comb. In this case both the frequency repetition and the carrier-envelope-offset frequency are referenced to a frequency standard, like an atomic clock. As a result the accuracy of the frequency standard is transferred to the optical domain, with the frequency comb as transfer oscillator. These unique properties allow the frequency comb to be applied as a versatile tool, not only for time and frequency metrology, but also in fundamental physics, high-precision spectroscopy, and laser noise characterization. The pulse-to-pulse phase relationship of the light emitted by the frequency comb has opened up new directions for long range highly accurate distance measurement.

  19. Femtosecond laser generated gold nanoparticles and their plasmonic properties

    International Nuclear Information System (INIS)

    Das, Rupali; Navas, M. P.; Soni, R. K.

    2016-01-01

    The pulsed laser ablation in liquid medium is now commonly used to generate stable colloidal nanoparticles (NPs) in absence of any chemical additives or stabilizer with diverse applications. In this paper, we report generation of gold NPs (Au NPs) by ultra-short laser pulses. Femtosecond (fs) laser radiation (λ = 800 nm) has been used to ablate a gold target in pure de-ionized water to produce gold colloids with smallsize distribution. The average size of the particles can be further controlled by subjecting to laser-induced post-irradiation providing a versatile physical method of size-selected gold nanoparticles. The optical extinction and morphological dimensions were investigated with UV-Vis spectroscopy and Transmission Electron Microscopy measurements, respectively. Finite difference time domain (FDTD) method is employed to calculate localized surface plasmon (LSPR) wavelength and the near-field generated by Au NPs and their hybrids.

  20. Novel concepts for terahertz waveguide spectroscopy

    DEFF Research Database (Denmark)

    Jepsen, Peter Uhd

    2009-01-01

    . With such waveguides we demonstrate that it is possible to perform quantitative spectroscopy on very small volumes of sample material inside the PPWG. Using continuous-wave as well as femtosecond excitation we inject carriers into semiconductor material in the transparent PPWG, and perform static as well as transient...

  1. Femtosecond lasers for microsurgery of cornea

    International Nuclear Information System (INIS)

    Vartapetov, Sergei K; Khudyakov, D V; Lapshin, Konstantin E; Obidin, Aleksei Z; Shcherbakov, Ivan A

    2012-01-01

    The review of femtosecond laser installations for medical applications is given and a new femtosecond ophthalmologic system for creation of a flap of corneal tissue during the LASIK operation is described. An all-fibre femtosecond laser emitting ∼400-fs pulses at 1067 nm is used. The pulse repetition rate can vary from 200 kHz up to 1 MHz. The output energy of the femtosecond system does not exceed 1 μJ. A specially developed objective with small spherical and chromatic aberrations is applied to focus laser radiation to an area of an eye cornea. The size of the focusing spot does not exceed 3 μm. To process the required area, scanning by a laser beam is applied with a speed no less than 5 m s -1 . At a stage of preliminary tests of the system, the Κ8 glass, organic PMMA glass and specially prepared agarose gels are used as a phantom of an eye. The femtosecond system is successfully clinically tested on a plenty of eyes of a pig and on several human eyes. The duration of the procedure of creation of a corneal flap does not exceed 20 s.

  2. Femtosecond lasers for microsurgery of cornea

    Energy Technology Data Exchange (ETDEWEB)

    Vartapetov, Sergei K; Khudyakov, D V; Lapshin, Konstantin E; Obidin, Aleksei Z; Shcherbakov, Ivan A

    2012-03-31

    The review of femtosecond laser installations for medical applications is given and a new femtosecond ophthalmologic system for creation of a flap of corneal tissue during the LASIK operation is described. An all-fibre femtosecond laser emitting {approx}400-fs pulses at 1067 nm is used. The pulse repetition rate can vary from 200 kHz up to 1 MHz. The output energy of the femtosecond system does not exceed 1 {mu}J. A specially developed objective with small spherical and chromatic aberrations is applied to focus laser radiation to an area of an eye cornea. The size of the focusing spot does not exceed 3 {mu}m. To process the required area, scanning by a laser beam is applied with a speed no less than 5 m s{sup -1}. At a stage of preliminary tests of the system, the {Kappa}8 glass, organic PMMA glass and specially prepared agarose gels are used as a phantom of an eye. The femtosecond system is successfully clinically tested on a plenty of eyes of a pig and on several human eyes. The duration of the procedure of creation of a corneal flap does not exceed 20 s.

  3. Femtosecond phacoemulsification: the business and the medicine.

    Science.gov (United States)

    Uy, Harvey S; Edwards, Keith; Curtis, Nick

    2012-01-01

    PURPOSE FOR REVIEW: Phacoemulsification is the preferred method for cataract surgery in the developed world. The number of phacoemulsification procedures performed annually is expected to increase as the population ages. Femtosecond cataract surgery offers several surgical advantages over conventional phacoemulsification and has already attained commercial application in some countries. The purpose of this review is to outline the benefits, risks and commercial issues of femtosecond lasers as applied to cataract surgery. Cataract surgeons are adopting femtosecond technology to perform laser capsulotomy, lens fragmentation, clear cornea incisions and limbal relaxing incisions. Femtosecond lasers clearly perform these surgical steps with greater precision and reproducibility. Further benefits such as improved postoperative refractive results and reduced complication rates are being investigated. Commercial issues have invariably arisen such as cost of installation and operation, value proposition and return on investment. Femtosecond cataract surgery is an evolving procedure that can potentially lead to better and safer surgical outcomes. This review presents the currently available scientific evidence and discusses some of the relevant financial issues concerning this technology.

  4. Terahertz Spectroscopy and Imaging

    CERN Document Server

    Zeitler, Axel; Kuwata-Gonokami, Makoto

    2013-01-01

    "This book presents the current state of knowledge in the field of terahertz spectroscopy, providing a comprehensive source of information for beginners and experienced researchers alike whose interests lie in this area. The book aims to explain the fundamental physics that underpins terahertz  technology and to describe its key applications. Highlights of scientific research in the field of terahertz science are also outlined in some chapters, providing an overview as well as giving an insight into future directions for research.  Over the past decade terahertz spectroscopy has developed into one of the most rapidly growing areas of its kind, gaining an important impact across a wide range of scientific disciplines. Due to substantial advances in femtosecond laser technology, terahertz time-domain spectroscopy (THz-TDS) has established itself as the dominant spectroscopic technique for experimental scientists interested in measurements at this frequency range. In solids and liquids THz radiation is in reso...

  5. High-speed asynchronous optical sampling for high-sensitivity detection of coherent phonons

    International Nuclear Information System (INIS)

    Dekorsy, T; Taubert, R; Hudert, F; Schrenk, G; Bartels, A; Cerna, R; Kotaidis, V; Plech, A; Koehler, K; Schmitz, J; Wagner, J

    2007-01-01

    A new optical pump-probe technique is implemented for the investigation of coherent acoustic phonon dynamics in the GHz to THz frequency range which is based on two asynchronously linked femtosecond lasers. Asynchronous optical sampling (ASOPS) provides the performance of on all-optical oscilloscope and allows us to record optically induced lattice dynamics over nanosecond times with femtosecond resolution at scan rates of 10 kHz without any moving part in the set-up. Within 1 minute of data acquisition time signal-to-noise ratios better than 10 7 are achieved. We present examples of the high-sensitivity detection of coherent phonons in superlattices and of the coherent acoustic vibration of metallic nanoparticles

  6. Construction of a femtosecond laser microsurgery system.

    Science.gov (United States)

    Steinmeyer, Joseph D; Gilleland, Cody L; Pardo-Martin, Carlos; Angel, Matthew; Rohde, Christopher B; Scott, Mark A; Yanik, Mehmet Fatih

    2010-03-01

    Femtosecond laser microsurgery is a powerful method for studying cellular function, neural circuits, neuronal injury and neuronal regeneration because of its capability to selectively ablate sub-micron targets in vitro and in vivo with minimal damage to the surrounding tissue. Here, we present a step-by-step protocol for constructing a femtosecond laser microsurgery setup for use with a widely available compound fluorescence microscope. The protocol begins with the assembly and alignment of beam-conditioning optics at the output of a femtosecond laser. Then a dichroic mount is assembled and installed to direct the laser beam into the objective lens of a standard inverted microscope. Finally, the laser is focused on the image plane of the microscope to allow simultaneous surgery and fluorescence imaging. We illustrate the use of this setup by presenting axotomy in Caenorhabditis elegans as an example. This protocol can be completed in 2 d.

  7. Influence of the Chemical Design on the Coherent Photoisomerization of Biomimetic Molecular Switches

    Directory of Open Access Journals (Sweden)

    Olivucci Massimo

    2013-03-01

    Full Text Available Ultrafast transient absorption spectroscopy reveals the effect of chemical substitutions on the photoreaction kinetics of biomimetic photoswitches displaying coherent dynamics. Ground state vibrational coherences are no longer observed when the excited state lifetime exceeds 300fs.

  8. Control of the kerf size and microstructure in Inconel 738 superalloy by femtosecond laser beam cutting

    Energy Technology Data Exchange (ETDEWEB)

    Wei, J.; Ye, Y.; Sun, Z. [Department of Mechanical Engineering, Tsinghua University, Beijing (China); Liu, L., E-mail: liulei@tsinghua.edu.cn [The State Key Laboratory of Tribology, Tsinghua University, Beijing (China); Zou, G., E-mail: sunzhg@tsinghua.edu.cn [Department of Mechanical Engineering, Tsinghua University, Beijing (China)

    2016-05-01

    Highlights: • Effects of processing parameters on the kerf size in Inconel 738 are investigated. • Defocus is a key parameter affecting the kerf width due to the intensity clamping. • The internal surface microstructures with different scanning speed are presented. • The material removal mechanism contains normal vaporization and phase explosion. • Oxidation mechanism is attributed to the trapping effect of the dangling bonds. - Abstract: Femtosecond laser beam cutting is becoming widely used to meet demands for increasing accuracy in micro-machining. In this paper, the effects of processing parameters in femtosecond laser beam cutting on the kerf size and microstructure in Inconel 738 have been investigated. The defocus, pulse width and scanning speed were selected to study the controllability of the cutting process. Adjusting and matching the processing parameters was a basic enhancement method to acquire well defined kerf size and the high-quality ablation of microstructures, which has contributed to the intensity clamping effect. The morphology and chemical compositions of these microstructures on the cut surface have been characterized by a scanning electron microscopy equipped with an energy dispersive X-ray spectroscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Additionally, the material removal mechanism and oxidation mechanism on the Inconel 738 cut surface have also been discussed on the basis of the femtosecond laser induced normal vaporization or phase explosion, and trapping effect of the dangling bonds.

  9. Selective ablation of dental enamel and dentin using femtosecond laser pulses

    International Nuclear Information System (INIS)

    Lizarelli, R F Z; Costa, M M; Carvalho-Filho, E; Bagnato, V S; Nunes, F D

    2008-01-01

    The study of the interaction of intense laser light with matter, as well as transient response of atoms and molecules is very appropriated because of the laser energy concentration in a femtosecond optical pulses. The fundamental problem to be solved is to find tools and techniques which allow us to observe and manipulate on a femtosecond time scale the photonics events on and into the matter. Six third human extracted molars were exposed to a femtosecond Ti:Sapphire Q-switched and mode locked laser (Libra-S, Coherent, Palo Alto, CA, USA), emitting pulses with 70 fs width, radiation wavelength of 801 nm, at a constant pulse repetition rate of 1 KHz. The laser was operated at different power levels (70 to 400 mW) with constant exposition time of 10 seconds, at focused and defocused mode. Enamel and dentin surfaces were evaluated concerned ablation rate and morphological aspects under scanning electron microscopic. The results in this present experiment suggest that at the focused mode and under higher average power, enamel tissues present microcavities with higher depth and very precise edges, but, while dentin shows a larger melt-flushing, lower depth and melting and solidification aspect. In conclusion, it is possible to choose hard or soft ablation, under lower and higher average power, respectively, revealing different aspects of dental enamel and dentin, depending on the average power, fluence and distance from the focal point of the ultra-short pulse laser on the tooth surface

  10. Traveling wave deflector design for femtosecond streak camera

    International Nuclear Information System (INIS)

    Pei, Chengquan; Wu, Shengli; Luo, Duan; Wen, Wenlong; Xu, Junkai; Tian, Jinshou; Zhang, Minrui; Chen, Pin; Chen, Jianzhong; Liu, Rong

    2017-01-01

    In this paper, a traveling wave deflection deflector (TWD) with a slow-wave property induced by a microstrip transmission line is proposed for femtosecond streak cameras. The pass width and dispersion properties were simulated. In addition, the dynamic temporal resolution of the femtosecond camera was simulated by CST software. The results showed that with the proposed TWD a femtosecond streak camera can achieve a dynamic temporal resolution of less than 600 fs. Experiments were done to test the femtosecond streak camera, and an 800 fs dynamic temporal resolution was obtained. Guidance is provided for optimizing a femtosecond streak camera to obtain higher temporal resolution.

  11. Traveling wave deflector design for femtosecond streak camera

    Energy Technology Data Exchange (ETDEWEB)

    Pei, Chengquan; Wu, Shengli [Key Laboratory for Physical Electronics and Devices of the Ministry of Education, Xi' an Jiaotong University, Xi’an 710049 (China); Luo, Duan [Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi' an 710119 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Wen, Wenlong [Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi' an 710119 (China); Xu, Junkai [Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi' an 710119 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Tian, Jinshou, E-mail: tianjs@opt.ac.cn [Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi' an 710119 (China); Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, Shanxi 030006 (China); Zhang, Minrui; Chen, Pin [Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi' an 710119 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Chen, Jianzhong [Key Laboratory for Physical Electronics and Devices of the Ministry of Education, Xi' an Jiaotong University, Xi’an 710049 (China); Liu, Rong [Xi' an Technological University, Xi' an 710021 (China)

    2017-05-21

    In this paper, a traveling wave deflection deflector (TWD) with a slow-wave property induced by a microstrip transmission line is proposed for femtosecond streak cameras. The pass width and dispersion properties were simulated. In addition, the dynamic temporal resolution of the femtosecond camera was simulated by CST software. The results showed that with the proposed TWD a femtosecond streak camera can achieve a dynamic temporal resolution of less than 600 fs. Experiments were done to test the femtosecond streak camera, and an 800 fs dynamic temporal resolution was obtained. Guidance is provided for optimizing a femtosecond streak camera to obtain higher temporal resolution.

  12. Femto-second pulses of synchrotron radiation

    International Nuclear Information System (INIS)

    Zholents, A.A.; Zolotorev, M.S.

    1995-07-01

    A method capable of producing femto-second pulses of synchrotron radiation is proposed. It is based on the interaction of femto-second light pulses with electrons in a storage ring. The application of the method to the generation of ultra-short x-ray pulses at the Advance Light Source of Lawrence Berkeley National Laboratory has been considered. The same method can also be used for extraction of electrons from a storage ring in ultra-short series of microbunches spaced by the periodicity of light wavelength

  13. Amorphization of silicon by femtosecond laser pulses

    International Nuclear Information System (INIS)

    Jia, Jimmy; Li Ming; Thompson, Carl V.

    2004-01-01

    We have used femtosecond laser pulses to drill submicron holes in single crystal silicon films in silicon-on-insulator structures. Cross-sectional transmission electron microscopy and energy dispersive x-ray analysis of material adjacent to the ablated holes indicates the formation of a layer of amorphous Si. This demonstrates that even when material is ablated using femtosecond pulses near the single pulse ablation threshold, sufficient heating of the surrounding material occurs to create a molten zone which solidifies so rapidly that crystallization is bypassed

  14. Laser-Induced Damage with Femtosecond Pulses

    Science.gov (United States)

    Kafka, Kyle R. P.

    The strong electric fields of focused femtosecond laser pulses lead to non-equilibrium dynamics in materials, which, beyond a threshold intensity, causes laser-induced damage (LID). Such a strongly non-linear and non-perturbative process renders important LID observables like fluence and intensity thresholds and damage morphology (crater) extremely difficult to predict quantitatively. However, femtosecond LID carries a high degree of precision, which has been exploited in various micro/nano-machining and surface engineering applications, such as human eye surgery and super-hydrophobic surfaces. This dissertation presents an array of experimental studies which have measured the damage behavior of various materials under femtosecond irradiation. Precision experiments were performed to produce extreme spatio-temporal confinement of the femtosecond laser-solid damage interaction on monocrystalline Cu, which made possible the first successful direct-benchmarking of LID simulation with realistic damage craters. A technique was developed to produce laser-induced periodic surface structures (LIPSS) in a single pulse (typically a multi-pulse phenomenon), and was used to perform a pump-probe study which revealed asynchronous LIPSS formation on copper. Combined with 1-D calculations, this new experimental result suggests more drastic electron heating than expected. Few-cycle pulses were used to study the LID performance and morphology of commercial ultra-broadband optics, which had not been systematically studied before. With extensive surface analysis, various morphologies were observed, including LIPSS, swelling (blisters), simple craters, and even ring-shaped structures, which varied depending on the coating design, number of pulses, and air/vacuum test environment. Mechanisms leading to these morphologies are discussed, many of which are ultrafast in nature. The applied damage behavior of multi-layer dielectric mirrors was measured and compared between long pulse (150 ps

  15. Size-controllable synthesis of bare gold nanoparticles by femtosecond laser fragmentation in water

    International Nuclear Information System (INIS)

    Maximova, Ksenia; Aristov, Andrei; Sentis, Marc; Kabashin, Andrei V

    2015-01-01

    We report a size-controllable synthesis of stable aqueous solutions of ultrapure low-size-dispersed Au nanoparticles by methods of femtosecond laser fragmentation from preliminary formed colloids. Such approach makes possible the tuning of mean nanoparticle size between a few nm and several tens of nm under the size dispersion lower than 70% by varying the fluence of pumping radiation during the fragmentation procedure. The efficient size control is explained by 3D geometry of laser fragmentation by femtosecond laser-induced white light super-continuum and plasma-related phenomena. Despite the absence of any protective ligands, the nanoparticle solutions demonstrate exceptional stability due to electric repulsion effect associated with strong negative charging of formed nanoparticles. Stable aqueous solutions of bare gold nanoparticles present a unique object with a variety of potential applications in catalysis, surface-enhanced Raman spectroscopy, photovoltaics, biosensing and biomedicine. (paper)

  16. Femtosecond laser ablation of polymeric substrates for the fabrication of microfluidic channels

    International Nuclear Information System (INIS)

    Suriano, Raffaella; Kuznetsov, Arseniy; Eaton, Shane M.; Kiyan, Roman; Cerullo, Giulio; Osellame, Roberto; Chichkov, Boris N.; Levi, Marinella; Turri, Stefano

    2011-01-01

    This manuscript presents a study of physical and chemical properties of microchannels fabricated by femtosecond laser processing technology in thermoplastic polymeric materials, including poly(methyl methacrylate) (PMMA), polystyrene (PS) and cyclic olefin polymer (COP). By surface electron microscopy and optical profilometry, the dimensions of microchannels in the polymers were found to be easily tunable, with surface roughness values comparable to those obtained by standard prototyping techniques such as micromilling. Through colorimetric analysis and optical microscopy, PMMA was found to remain nearly transparent after ablation while COP and PS darkened significantly. Using infrared spectroscopy, the darkening in PS and COP was attributed to significant oxidation and dehydrogenation during laser ablation, unlike PMMA, which was found to degrade by a thermal depolymerization process. The more stable molecular structure of PMMA makes it the most viable thermoplastic polymer for femtosecond laser fabrication of microfluidic channels.

  17. Clocking femtosecond collisional dynamics via resonant X-ray spectroscopy

    Czech Academy of Sciences Publication Activity Database

    van den Berg, Q.Y.; Fernandez-Tello, E.V.; Burian, Tomáš; Chalupský, Jaromír; Chung, H.-K.; Ciricosta, O.; Dakovski, G.L.; Hájková, Věra; Hollebon, P.; Juha, Libor; Krzywinski, J.; Lee, R. W.; Minitti, M.P.; Preston, T.R.; de la Varga, A.G.; Vozda, Vojtěch; Zastrau, U.; Wark, J. S.; Velarde, P.; Vinko, S.M.

    2018-01-01

    Roč. 120, č. 5 (2018), s. 1-6, č. článku 055002. ISSN 0031-9007 R&D Projects: GA ČR(CZ) GA17-05167s; GA MŠk LG15013 Institutional support: RVO:68378271 Keywords : hot dense matter * highly-charged ions * electron-impact-ionization * laser * plasma s Subject RIV: BL - Plasma and Gas Discharge Physics OBOR OECD: Fluids and plasma physics (including surface physics) Impact factor: 8.462, year: 2016

  18. Femtosecond time-resolved transient absorption spectroscopy of xanthophylls.

    Science.gov (United States)

    Niedzwiedzki, Dariusz M; Sullivan, James O; Polívka, Tomás; Birge, Robert R; Frank, Harry A

    2006-11-16

    Xanthophylls are a major class of photosynthetic pigments that participate in an adaptation mechanism by which higher plants protect themselves from high light stress. In the present work, an ultrafast time-resolved spectroscopic investigation of all the major xanthophyll pigments from spinach has been performed. The molecules are zeaxanthin, lutein, violaxanthin, and neoxanthin. beta-Carotene was also studied. The experimental data reveal the inherent spectral properties and ultrafast dynamics including the S(1) state lifetimes of each of the pigments. In conjunction with quantum mechanical computations the results address the molecular features of xanthophylls that control the formation and decay of the S* state in solution. The findings provide compelling evidence that S* is an excited state with a conformational geometry twisted relative to the ground state. The data indicate that S* is formed via a branched pathway from higher excited singlet states and that its yield depends critically on the presence of beta-ionylidene rings in the polyene system of pi-electron conjugated double bonds. The data are expected to be beneficial to researchers employing ultrafast time-resolved spectroscopic methods to investigate the mechanisms of both energy transfer and nonphotochemical quenching in higher plant preparations.

  19. Ultrafast optical generation of squeezed magnon states and long lifetime coherent LO phonons

    Science.gov (United States)

    Zhao, Jimin

    2005-12-01

    Ultrafast optical pulses have been used to generate, probe, and control low-energy elementary excitations in crystals. In particular, we report the first experimental demonstration of the generation of quantum squeezed states of magnons (collective spin-wave excitations) in a magnetic material, and new progress in experimental investigation of anharmonic interactions in a semiconductor. The mechanism for the magnon squeezing is two-magnon impulsive stimulated Raman scattering (ISRS). Femtosecond laser pulses have been used to coherently correlate degenerate counter-propagating magnons in the antiferromagnetic insulator MnF2. In the squeezed state, fluctuations of the magnetization of a crystallographic unit cell vary periodically in time and are reduced below that of the ground-state quantum noise. Similar experiments were also performed in another antiferromagnetic insulator, FeF2, for which the squeezing effect is one order of magnitude larger. We have also investigated the anharmonic interaction of the low-frequency E2 phonon in ZnO through ISRS. Temperature dependence of the linewidth and frequency indicates that the two-phonon up-conversion process is the dominant decay channel and isotopic disorder may be the main limit on the lifetime at low temperature. We have observed the longest lifetime of an optical phonon mode in a solid (211 ps at 5 K). And we have found that pump-probe experiments, compared with spontaneous Raman spectroscopy, have extremely high accuracy in determining the frequency of a low-lying excitation.

  20. Mid-infrared frequency comb via coherent dispersive wave generation in silicon nitride nanophotonic waveguides

    Science.gov (United States)

    Guo, Hairun; Herkommer, Clemens; Billat, Adrien; Grassani, Davide; Zhang, Chuankun; Pfeiffer, Martin H. P.; Weng, Wenle; Brès, Camille-Sophie; Kippenberg, Tobias J.

    2018-06-01

    Mid-infrared optical frequency combs are of significant interest for molecular spectroscopy due to the large absorption of molecular vibrational modes on the one hand, and the ability to implement superior comb-based spectroscopic modalities with increased speed, sensitivity and precision on the other hand. Here, we demonstrate a simple, yet effective, method for the direct generation of mid-infrared optical frequency combs in the region from 2.5 to 4.0 μm (that is, 2,500-4,000 cm-1), covering a large fraction of the functional group region, from a conventional and compact erbium-fibre-based femtosecond laser in the telecommunication band (that is, 1.55 μm). The wavelength conversion is based on dispersive wave generation within the supercontinuum process in an unprecedented large-cross-section silicon nitride (Si3N4) waveguide with the dispersion lithographically engineered. The long-wavelength dispersive wave can perform as a mid-infrared frequency comb, whose coherence is demonstrated via optical heterodyne measurements. Such an approach can be considered as an alternative option to mid-infrared frequency comb generation. Moreover, it has the potential to realize compact dual-comb spectrometers. The generated combs also have a fine teeth-spacing, making them suitable for gas-phase analysis.

  1. Coherent anti-Stokes Raman scattering and spontaneous Raman scattering diagnostics of nonequilibrium plasmas and flows

    Science.gov (United States)

    Lempert, Walter R.; Adamovich, Igor V.

    2014-10-01

    The paper provides an overview of the use of coherent anti-Stokes Raman scattering (CARS) and spontaneous Raman scattering for diagnostics of low-temperature nonequilibrium plasmas and nonequilibrium high-enthalpy flows. A brief review of the theoretical background of CARS, four-wave mixing and Raman scattering, as well as a discussion of experimental techniques and data reduction, are included. The experimental results reviewed include measurements of vibrational level populations, rotational/translational temperature, electric fields in a quasi-steady-state and transient molecular plasmas and afterglow, in nonequilibrium expansion flows, and behind strong shock waves. Insight into the kinetics of vibrational energy transfer, energy thermalization mechanisms and dynamics of the pulse discharge development, provided by these experiments, is discussed. Availability of short pulse duration, high peak power lasers, as well as broadband dye lasers, makes possible the use of these diagnostics at relatively low pressures, potentially with a sub-nanosecond time resolution, as well as obtaining single laser shot, high signal-to-noise spectra at higher pressures. Possibilities for the development of single-shot 2D CARS imaging and spectroscopy, using picosecond and femtosecond lasers, as well as novel phase matching and detection techniques, are discussed.

  2. Polarization Sensitive Coherent Raman Measurements of DCVJ

    Science.gov (United States)

    Anderson, Josiah; Cooper, Nathan; Lawhead, Carlos; Shiver, Tegan; Ujj, Laszlo

    2014-03-01

    Coherent Raman spectroscopy which recently developed into coherent Raman microscopy has been used to produce label free imaging of thin layers of material and find the spatial distributions of certain chemicals within samples, e.g. cancer cells.(1) Not all aspects of coherent scattering have been used for imaging. Among those for example are special polarization sensitive measurements. Therefore we have investigated the properties of polarization sensitive CARS spectra of a highly fluorescent molecule, DCVJ.(2) Spectra has been recorded by using parallel polarized and perpendicular polarized excitations. A special polarization arrangement was developed to suppress the non-resonant background scattering from the sample. These results can be used to improve the imaging properties of a coherent Raman microscope in the future. This is the first time coherent Raman polarization sensitive measurements have been used to characterize the vibrational modes of DCVJ. 1: K. I. Gutkowski, et al., ``Fluorescence of dicyanovinyl julolidine in a room temperature ionic liquid '' Chemical Physics Letters 426 (2006) 329 - 333 2: Fouad El-Diasty, ``Coherent anti-Stokes Raman scattering: Spectroscopy and microscopy'' Vibrational Spectroscopy 55 (2011) 1-37

  3. Coherent control of plasma dynamics

    Science.gov (United States)

    He, Zhaohan

    2014-10-01

    The concept of coherent control - precise measurement or determination of a process through control of the phase of an applied oscillating field - has been applied to numerous systems with great success. Here, we demonstrate the use of coherent control on plasma dynamics in a laser wakefield electron acceleration experiment. A tightly focused femtosecond laser pulse (10 mJ, 35 fs) was used to generate electron beams by plasma wakefield acceleration in the density down ramp. The technique is based on optimization of the electron beam using a deformable mirror adaptive optical system with an iterative evolutionary genetic algorithm. The image of the electrons on a scintillator screen was processed and used in a fitness function as direct feedback for the optimization algorithm. This coherent manipulation of the laser wavefront leads to orders of magnitude improvement to the electron beam properties such as the peak charge and beam divergence. The laser beam optimized to generate the best electron beam was not the one with the ``best'' focal spot. When a particular wavefront of laser light interacts with plasma, it can affect the plasma wave structures and trapping conditions of the electrons in a complex way. For example, Raman forward scattering, envelope self-modulation, relativistic self-focusing, and relativistic self-phase modulation and many other nonlinear interactions modify both the pulse envelope and phase as the pulse propagates, in a way that cannot be easily predicted and that subsequently dictates the formation of plasma waves. The optimal wavefront could be successfully determined via the heuristic search under laser-plasma conditions that were not known a priori. Control and shaping of the electron energy distribution was found to be less effective, but was still possible. Particle-in-cell simulations were performed to show that the mode structure of the laser beam can affect the plasma wave structure and trapping conditions of electrons, which

  4. Development of a high power femtosecond laser

    CSIR Research Space (South Africa)

    Neethling, PH

    2010-10-01

    Full Text Available The Laser Research Institute and the CSIR National Laser Centre are developing a high power femtosecond laser system in a joint project with a phased approach. The laser system consists of an fs oscillator and a regenerative amplifier. An OPCPA...

  5. Femtosecond laser pulse written Volume Bragg Gratings

    Directory of Open Access Journals (Sweden)

    Richter Daniel

    2013-11-01

    Full Text Available Femtosecond laser pulses can be applied for structuring a wide range of ransparent materials. Here we want to show how to use this ability to realize Volume-Bragg-Gratings in various- mainly non-photosensitive - glasses. We will further present the characteristics of the realized gratings and a few elected applications that have been realized.

  6. Femtosecond laser control of chemical reactions

    CSIR Research Space (South Africa)

    Du Plessis, A

    2010-08-31

    Full Text Available Femtosecond laser control of chemical reactions is made possible through the use of pulse-shaping techniques coupled to a learning algorithm feedback loop – teaching the laser pulse to control the chemical reaction. This can result in controllable...

  7. Bending diamonds by femtosecond laser ablation

    DEFF Research Database (Denmark)

    Balling, Peter; Esberg, Jakob; Kirsebom, Kim

    2009-01-01

    We present a new method based on femtosecond laser ablation for the fabrication of statically bent diamond crystals. Using this method, curvature radii of 1 m can easily be achieved, and the curvature obtained is very uniform. Since diamond is extremely tolerant to high radiation doses, partly due...

  8. Plasmon-enhanced terahertz emission in self-assembled quantum dots by femtosecond pulses

    Energy Technology Data Exchange (ETDEWEB)

    Carreño, F., E-mail: ferpo@fis.ucm.es; Antón, M. A., E-mail: antonm@fis.ucm.es; Melle, Sonia, E-mail: smelle@fis.ucm.es; Calderón, Oscar G., E-mail: oscargc@fis.ucm.es; Cabrera-Granado, E., E-mail: ecabrera@fis.ucm.es [Facultad de Óptica y Optometría, Universidad Complutense de Madrid, C/ Arcos de Jalón 118, 28037 Madrid (Spain); Cox, Joel, E-mail: jcox27@uwo.ca; Singh, Mahi R., E-mail: msingh@uwo.ca [Department of Physics and Astronomy, The University of Western Ontario, London N6A 3K7 (Canada); Egatz-Gómez, A., E-mail: Ana.Egatz-Gomez.1@nd.edu [Department of Chemical and Biomolecular Engineering, University of Notre Dame, South Bend, Indiana 46556 (United States)

    2014-02-14

    A scheme for terahertz (THz) generation from intraband transition in a self-assembled quantum dot (QD) molecule coupled to a metallic nanoparticle (MNP) is analyzed. The QD structure is described as a three-level atom-like system using the density matrix formalism. The MNP with spherical geometry is considered in the quasistatic approximation. A femtosecond laser pulse creates a coherent superposition of two subbands in the quantum dots and produces localized surface plasmons in the nanoparticle which act back upon the QD molecule via dipole-dipole interaction. As a result, coherent THz radiation with a frequency corresponding to the interlevel spacing can be obtained, which is strongly modified by the presence of the MNP. The peak value of the terahertz signal is analyzed as a function of nanoparticle's size, the MNP to QD distance, and the area of the applied laser field. In addition, we theoretically demonstrate that the terahertz pulse generation can be effectively controlled by making use of a train of femtosecond laser pulses. We show that by a proper choice of the parameters characterizing the pulse train a huge enhancement of the terahertz signal is obtained.

  9. Recording of interference fringe structure by femtosecond laser pulses in samples of silver-containing porous glass and thick slabs of dichromated gelatin

    Science.gov (United States)

    Andreeva, Olga V.; Dement'ev, Dmitry A.; Chekalin, Sergey V.; Kompanets, V. O.; Matveets, Yu. A.; Serov, Oleg B.; Smolovich, Anatoly M.

    2002-05-01

    The recording geometry and recording media for the method of achromatic wavefront reconstruction are discussed. The femtosecond recording on the thick slabs of dichromated gelatin and the samples of silver-containing porous glass was obtained. The applications of the method to ultrafast laser spectroscopy and to phase conjugation were suggested.

  10. Dye lasers in atomic spectroscopy

    International Nuclear Information System (INIS)

    Lange, W.; Luther, J.; Steudel, A.

    1974-01-01

    The properties of dye lasers which are relevant to atomic spectroscopy are discussed. Several experiments made possible by tunable dye lasers are discussed. Applications of high spectral density dye lasers are covered in areas such as absorption spectroscopy, fluorescence spectroscopy, photoionization and photodetachment, and two- and multi-photon processes. Applications which take advantage of the narrow bandwidth of tunable dye lasers are discussed, including saturation spectroscopy, fluorescence line narrowing, classic absorption and fluorescence spectroscopy, nonoptical detection of optical resonances, heterodyne spectroscopy, and nonlinear coherent resonant phenomena. (26 figures, 180 references) (U.S.)

  11. Optical coherence techniques for plasma doppler spectroscopy

    International Nuclear Information System (INIS)

    Howard, J.; Michael, C.; Glass, F.; Cheetham, A.D.

    2000-01-01

    A new electro-optically Modulated Optical Solid-State (MOSS) interferometer has been constructed for measurement of the low order spectral moments of line emission from optically thin radiant media. The instrument, which is based on the principle of the Fourier transform spectrometer, has high etendue and is rugged, compact and inexpensive. By employing electro-optical path-length modulation techniques, the spectral information is transferred to the temporal frequency domain and can be obtained using a single photodetector. Specifically, the zeroth moment (brightness) is given by the average signal level, the first moment (shift) by the modulation phase and the second moment (line width) by the modulation amplitude. (author)

  12. Coherent Quantum Control of Multidimensional Vibrational Spectroscopy

    National Research Council Canada - National Science Library

    Mukamel, Shaul; Sanda, Frantisek; Harbola, Upendra; Venkatramani, Ravi; Varonine, Dmitri

    2006-01-01

    .... Factorial moments of photon counting statistics from a single molecule coupled to a quantum bath were expressed in terms of multipoint quantum correlation functions and represented by double-sided Feynman diagrams...

  13. Femtosecond electron bunches from an RF-gun

    International Nuclear Information System (INIS)

    Rimjaem, Sakhorn; Farias, Ruy; Thongbai, Chitrlada; Vilaithong, Thiraphat; Wiedemann, Helmut

    2004-01-01

    Sub-picosecond electron pulses become a tool of increasing importance to study dynamics at an atomic level. Such electron pulses can be used directly or be converted into intense coherent far infrared radiation or equally short X-ray pulses. In principle, sub-picosecond electron pulses can be obtained in large, high-energy electron linear accelerator systems by repeatedly applying an energy slew and magnetic compression. Another process is the production of short electron pulses at low energies from an RF-gun with a thermionic cathode together with a bunch compressing α-magnet. In this paper, we present a systematic analysis of capabilities and limits of sub-picosecond electron pulses from such a source. We discuss particular parameter choices as well as the impact of geometric and electric specifications on the 6-dimensional phase space electron distribution. Numerical beam simulations with the computer code PARMELA are performed including effects and limitations due to space charge forces. While the production of femtosecond electron bunches is of primary concern, we also consider the preservation of such short bunches along a beam transport line

  14. Coherent Smith-Purcell radiation as a diagnostic for sub-picosecond electron bunch length

    International Nuclear Information System (INIS)

    Nguyen, D.C.

    1996-01-01

    We suggest a novel technique of measuring sub-picosecond electron bunch length base on coherent Smith-Purcell radiation (SPR) emitted when electrons pass close to the surface of a metal grating. With electron bunch lengths comparable to the grating period, we predict that coherent SPR will be emitted at large angles with respect to direction of beam propagation. As the bunch length shortens, the coherent SPR will be enhanced over the incoherent component that is normally observed at small angles. Furthermore, the angular distribution of the coherent SPR will be shifted toward smaller angles as the bunch length becomes much smaller than the grating period. By measuring the angular distribution of the coherent SPR, one can determine the bunch length of sub-picosecond electron pulses. This new technique is easy to implement and appears capable of measuring femtosecond electron bunch lengths

  15. Femtosecond laser micromachining of polylactic acid/graphene composites for designing interdigitated microelectrodes for sensor applications

    Science.gov (United States)

    Paula, Kelly T.; Gaál, Gabriel; Almeida, G. F. B.; Andrade, M. B.; Facure, Murilo H. M.; Correa, Daniel S.; Riul, Antonio; Rodrigues, Varlei; Mendonça, Cleber R.

    2018-05-01

    There is an increasing interest in the last years towards electronic applications of graphene-based materials and devices fabricated from patterning techniques, with the ultimate goal of high performance and temporal resolution. Laser micromachining using femtosecond pulses is an attractive methodology to integrate graphene-based materials into functional devices as it allows changes to the focal volume with a submicrometer spatial resolution due to the efficient nonlinear nature of the absorption, yielding rapid prototyping for innovative applications. We present here the patterning of PLA-graphene films spin-coated on a glass substrate using a fs-laser at moderate pulse energies to fabricate interdigitated electrodes having a minimum spatial resolution of 5 μm. Raman spectroscopy of the PLA-graphene films indicated the presence of multilayered graphene fibers. Subsequently, the PLA-graphene films were micromachined using a femtosecond laser oscillator delivering 50-fs pulses and 800 nm, where the pulse energy and scanning speed was varied in order to determine the optimum irradiation parameters (16 nJ and 100 μm/s) to the fabrication of microstructures. The micromachined patterns were characterized by optical microscopy and submitted to electrical measurements in liquid samples, clearly distinguishing all tastes tested. Our results confirm the femtosecond laser micromachining technique as an interesting approach to efficiently pattern PLA-graphene filaments with high precision and minimal mechanical defects, allowing the easy fabrication of interdigitated structures and an alternative method to those produced by conventional photolithography.

  16. Single-shot femtosecond laser ablation of gold surface in air and isopropyl alcohol

    Science.gov (United States)

    Kudryashov, S. I.; Saraeva, I. N.; Lednev, V. N.; Pershin, S. M.; Rudenko, A. A.; Ionin, A. A.

    2018-05-01

    Single-shot IR femtosecond-laser ablation of gold surfaces in ambient air and liquid isopropyl alcohol was studied by scanning electron microscopy characterization of crater topographies and time-resolved optical emission spectroscopy of ablative plumes in regimes, typical for non-filamentary and non-fragmentation laser production of nanoparticle sols. Despite one order of magnitude shorter (few nanoseconds) lifetimes and almost two orders of magnitude lower intensities of the quenched ablative plume emission in the alcohol ambient at the same peak laser fluence, craters for the dry and wet conditions appeared with rather similar nanofoam-like spallative topographies and the same thresholds. These facts envision the underlying surface spallation as one of the basic ablation mechanisms relevant for both dry and wet advanced femtosecond laser surface nano/micro-machining and texturing, as well as for high-throughput femtosecond laser ablative production of colloidal nanoparticles by MHz laser-pulse trains via their direct nanoscale jetting from the nanofoam in air and fluid environments.

  17. Characteristics and Applications of Spatiotemporally Focused Femtosecond Laser Pulses

    Directory of Open Access Journals (Sweden)

    Chenrui Jing

    2016-12-01

    Full Text Available Simultaneous spatial and temporal focusing (SSTF of femtosecond laser pulses gives rise to strong suppression of nonlinear self-focusing during the propagation of the femtosecond laser beam. In this paper, we begin with an introduction of the principle of SSTF, followed by a review of our recent experimental results on the characterization and application of the spatiotemporally focused pulses for femtosecond laser micromachining. Finally, we summarize all of the results and give a future perspective of this technique.

  18. Effects of femtosecond laser radiation on the skin

    International Nuclear Information System (INIS)

    Rogov, P Yu; Bespalov, V G

    2016-01-01

    A mathematical model of linear and nonlinear processes is presented occurring under the influence of femtosecond laser radiation on the skin. There was held an analysis and the numerical solution of an equation system describing the dynamics of the electron and phonon subsystems were received. The results can be used to determine the maximum permissible levels of energy generated by femtosecond laser systems and the establishment of Russian laser safety standards for femtosecond laser systems. (paper)

  19. Speckles generated by skewed, short-coherence light beams

    International Nuclear Information System (INIS)

    Brogioli, D; Salerno, D; Ziano, R; Mantegazza, F; Croccolo, F

    2011-01-01

    When a coherent laser beam impinges on a random sample (e.g. a colloidal suspension), the scattered light exhibits characteristic speckles. If the temporal coherence of the light source is too short, then the speckles disappear, along with the possibility of performing homodyne or heterodyne scattering detection or photon correlation spectroscopy. Here we investigate the scattering of a so-called ‘skewed coherence beam’, i.e. a short-coherence beam modified such that the field is coherent within slabs that are skewed with respect to the wave fronts. We show that such a beam generates speckles and can be used for heterodyne scattering detection, despite its short temporal coherence. Moreover, we show that the heterodyne signal is not affected by multiple scattering. We suggest that the phenomenon presented here can be used as a means of carrying out heterodyne scattering measurement with any short-coherence radiation, including x-rays. (paper)

  20. Current status of femtosecond triplet Linacs 2000

    International Nuclear Information System (INIS)

    Uesaka, M.; Watanabe, T.; Kobayashi, T.

    2000-01-01

    Femtosecond Ultrafast Quantum Phenomenon Research Facility has been commissioned in 2000. It consists the femtosecond linac-laser synchronization system, the 12 TW 50 fs laser system and the analyzing system. Laser photocathode RF gun produced l kA = 7 nC / 7 ps for 250 μJ 267 nm laser irradiation, synchronization of 300 fs (rms) for minutes and l.9 ps (rms) for hours was established. Efforts to avoid such long-term drift are under way. This system is applied to subpico- and picosecond pulseradiolysis for radiation chemistry of water and supercritical water. Laser plasma linac works are under way to generate 20 MeV 10 fs electron bunch and ps ion beam using the 12 TW 50 fs laser. Further, the time-resolved X-ray diffraction is close to dynamic visualization of atomic motions. (author)

  1. Preliminary Design of a Femtosecond Oscilloscope

    CERN Document Server

    Gazazyan, Edmond D; Kalantaryan, Davit K; Laziev, Edouard; Margaryan, Amour

    2005-01-01

    The calculations on motion of electrons in a finite length electromagnetic field of linearly and circularly polarized laser beams have shown that one can use the transversal deflection of electrons on a screen at a certain distance after the interaction region for the measurement of the length and longitudinal particle distribution of femtosecond bunches. In this work the construction and preliminary parameters of various parts of a device that may be called femtosecond oscilloscope are considered. The influence of various factors, such as the energy spread and size of the electron bunches, are taken into account. For CO2 laser intensity 1016 W/cm2 and field free drift length 1m the deflection is 5.3 and 0.06 cm, while the few centimeters long interaction length between 2 mirrors requires assembling accuracy 6 mm and 1.3 micron for 20 MeV to 50 keV, respectively.

  2. Use of the Femtosecond Lasers in Ophthalmology

    Directory of Open Access Journals (Sweden)

    Roszkowska Anna M

    2018-01-01

    Full Text Available Femtosecond laser (FSL is an infrared laser with a wavelength of 1053 nm. FS laser works producing photodisruption or photoionization of the optically transparent tissue such as cornea. Currently FS lasers have a wide range of applications in ophthalmic surgery. They are used above all in corneal surgery in refractive procedures and keratoplasty, and recently in cataract surgery. The use of the FSL in corneal refractive surgery includes LASIK flap creation, astigmatic keratotomy, Femtosecond Lenticule Extraction (FLEx, Small Incision Lenticule Extraction (SMILE and channels creation for implantation of the intrastromal corneal rings. As to the corneal grafting, the FS lasers are used in laser-assisted anterior and posterior lamellar keratoplasty and customized trephination in the penetrating keratoplasty. FS Laser Assisted Cataract Surgery (FLACS includes capsulorrhexis and nuclear fragmentation that enhance safety and efficacy of the procedure.

  3. Use of the Femtosecond Lasers in Ophthalmology

    Science.gov (United States)

    Roszkowska, Anna M.; Urso, Mario; Signorino, Alberto; Aragona, Pasquale

    2018-01-01

    Femtosecond laser (FSL) is an infrared laser with a wavelength of 1053 nm. FS laser works producing photodisruption or photoionization of the optically transparent tissue such as cornea. Currently FS lasers have a wide range of applications in ophthalmic surgery. They are used above all in corneal surgery in refractive procedures and keratoplasty, and recently in cataract surgery. The use of the FSL in corneal refractive surgery includes LASIK flap creation, astigmatic keratotomy, Femtosecond Lenticule Extraction (FLEx), Small Incision Lenticule Extraction (SMILE) and channels creation for implantation of the intrastromal corneal rings. As to the corneal grafting, the FS lasers are used in laser-assisted anterior and posterior lamellar keratoplasty and customized trephination in the penetrating keratoplasty. FS Laser Assisted Cataract Surgery (FLACS) includes capsulorrhexis and nuclear fragmentation that enhance safety and efficacy of the procedure.

  4. Cutting NiTi with Femtosecond Laser

    Directory of Open Access Journals (Sweden)

    L. Quintino

    2013-01-01

    Full Text Available Superelastic shape memory alloys are difficult to machine by thermal processes due to the facility for Ti oxidation and by mechanical processes due to their superelastic behavior. In this study, femtosecond lasers were tested to analyze the potential for machining NiTi since femtosecond lasers allow nonthermal processing of materials by ablation. The effect of processing parameters on machining depth was studied, and material removal rates were computed. Surfaces produced were analyzed under SEM which shows a resolidified thin layer with minimal heat affected zones. However, for high cutting speeds, that is, for short interaction times, this layer was not observed. A depletion of Ni was seen which may be beneficial in biomedical applications since Ni is known to produce human tissue reactions in biophysical environments.

  5. Progress in Cherenkov femtosecond fiber lasers

    DEFF Research Database (Denmark)

    Liu, Xiaomin; Svane, Ask Sebastian; Lægsgaard, Jesper

    2016-01-01

    systems are highlighted—dependent on the realization scheme, the Cherenkov lasers can generate the femtosecond output tunable across the entire visible and even the UV range, and for certain designs more than 40% conversion efficiency from the pump to Cherenkov signal can be achieved. The femtosecond......We review the recent developments in the field of ultrafast Cherenkov fiber lasers. Two essential properties of such laser systems—broad wavelength tunability and high efficiency of Cherenkov radiation wavelength conversion are discussed. The exceptional performance of the Cherenkov fiber laser...... Cherenkov laser with all-fiber architecture is presented and discussed. Operating in the visible range, it delivers 100–200 fs wavelength-tunable pulses with multimilliwatt output power and exceptionally low noise figure an order of magnitude lower than the traditional wavelength tunable supercontinuumbased...

  6. Femtosecond laser ablation of single-wall carbon nanotube-based material

    International Nuclear Information System (INIS)

    Danilov, Pavel A; Ionin, Andrey A; Kudryashov, Sergey I; Makarov, Sergey V; Mel’nik, Nikolay N; Rudenko, Andrey A; Yurovskikh, Vladislav I; Zayarny, Dmitry V; Lednev, Vasily N; Obraztsova, Elena D; Pershin, Sergey M; Bunkin, Alexey F

    2014-01-01

    Single- and multi-shot femtosecond laser surface ablation of a single-wall carbon nanotube-based substrate at 515- and 1030 nm wavelengths was studied by scanning electron microscopy and micro-Raman spectroscopy. The laser ablation proceeds in two ways: as the low-fluence mesoscopic shallow disintegration of the surface nanotube packing, preserving the individual integrity and the semiconducting character of the nanotubes or as the high-fluence deep material removal apparently triggered by the strong intrinsic or impurity-mediated ablation of the individual carbon nanotubes on the substrate surface. (letter)

  7. Femtosecond Study of Self-Trapped Vibrational Excitons in Crystalline Acetanilide

    Science.gov (United States)

    Edler, J.; Hamm, P.; Scott, A. C.

    2002-02-01

    Femtosecond IR spectroscopy of delocalized NH excitations of crystalline acetanilide confirms that self-trapping in hydrogen-bonded peptide units exists and does stabilize the excitation. Two phonons with frequencies of 48 and 76 cm -1 are identified as the major degrees of freedom that mediate self-trapping. After selective excitation of the free exciton, self-trapping occurs within a few 100 fs. Excitation of the self-trapped states disappears from the spectral window of this investigation on a 1 ps time scale, followed by a slow ground state recovery of the hot ground state within 18 ps.

  8. Femtosecond laser-ablated Fresnel zone plate fiber probe and sensing applications

    Science.gov (United States)

    Tan, Xiaoling; Geng, Youfu; Chen, Yan; Li, Shiguo; Wang, Xinzhong

    2018-02-01

    We investigate the Fresnel zone plate (FZP) inscribed on multimode fiber endface using femtosecond laser ablation and its application in sensing. The mode transmission through fiber tips with FZP is investigated both by the beam propagation method theoretically and by measuring the beam images with a charge-coupled device camera experimentally, which show a good agreement. Such devices are tested for surface-enhanced Raman scattering (SERS) using the aqueous solution of rhodamine 6G under a Raman spectroscopy. The experimental results demonstrate that the SERS signal is enhanced benefiting from focal ability of FZP, which is a promising method for the particular biochemical spectra sensing applications.

  9. Prospects of third-generation femtosecond laser technology in biological spectromicroscopy

    Science.gov (United States)

    Fattahi, Hanieh; Fattahi, Zohreh; Ghorbani, Asghar

    2018-05-01

    The next generation of biological imaging modalities will be a movement towards super-resolution, label-free approaches to realize subcellular images in a nonperturbative, non-invasive manner and towards new detection metrologies to reach a higher sensitivity and dynamic range. In this paper, we discuss how the third generation femtosecond laser technology in combination with the already existing concepts in time-resolved spectroscopy could fulfill the requirements of these exciting prospects. The expected enhanced specificity and sensitivity of the envisioned super-resolution microscope could lead us to a better understanding of the inter- and intra-cellular molecular transport and DNA-protein interaction.

  10. Femtosecond laser additive manufacturing of YSZ

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Jian; Bai, Shuang [PolarOnyx, Inc., San Jose, CA (United States)

    2017-04-15

    Laser additive manufacturing (LAM) of Yttria-Stabilized Zirconia (YSZ) is investigated using femtosecond (fs) fiber lasers. Various processing conditions are studied, which leads to desired characteristics in terms of morphology, porosity, hardness, microstructural and mechanical properties of the processed components. High-density (>99%) YSZ part with refined grain and increased hardness was obtained. Microstructure features of fabricated specimens were studied with SEM, EDX, the measured micro hardness is achieved as high as 18.84 GPa. (orig.)

  11. Probing chirality with a femtosecond reaction microscope

    Directory of Open Access Journals (Sweden)

    Janssen M. H. M.

    2013-03-01

    Full Text Available Detection of molecular chirality with high sensitivity and selectivity is important for many analytical and practical applications. Photoionization has emerged as a very sensitive probe of chirality in molecules. We show here that a table top setup with a femtosecond laser and a single imaging detector for both photoelectrons and photoions enables detection of chirality up to 3 orders of magnitude better than the existing conventional absorption based techniques.

  12. Proton radiography using highpower femtosecond laser

    International Nuclear Information System (INIS)

    Choi, Chang Il

    2010-08-01

    A femtosecond laser emits pulses whose width is between few and few hundreds femtoseconds (10 -15 s). The production mechanism of the high energy protons generated by the femtosecond laser is not clear so far, but the technologies have been improving. The applications using the generated protons are the proton therapy, proton radiography, nuclear physics, security inspection, and so on. Especially in the radiography, the laser-generated protons are very useful to obtain high quality images of thin objects, because protons are able to penetrate an object following an almost straight path and give a depth distribution information of various elements in a subject. Since the laser-driven protons require lower cost and smaller facility than accelerator-based protons, the radiography using laser-driven protons have been of interest. In this research, we have performed the radiography experiments by using protons generated by the 100 TW titanium sapphire femtosecond laser facility of Advanced Photonics Research Institute (APRI) of Gwangju Institute of Science Technology (GIST). A CR-39 Solid State Nuclear Track Detector (SSNTD) has been used as radiography screen. The radiography digital images have been obtained by using an optical microscope and a CCD camera. Modulation Transfer Function (MTF) has been derived from analyzing the obtained images, and the spatial resolution of the images have been evaluated. And, we have performed the radiography experiments of monoenergetic proton from the Tandem Van de Graaff accelerator of Korea Institute of Geoscience and Mineral Resources (KIGAM). We have obtained and compared the radiography images from other proton production methods which are the laser and the accelerator, respectively. And also, we have found out the optimized chemical etching condition, in order to improve the spatial resolution of the radiography images. Finally, the evaluated maximum spatial resolution of the images are 2.09 μm

  13. Beam Characterizations at Femtosecond Electron Beam Facility

    CERN Document Server

    Rimjaem, Sakhorn; Kangrang, Nopadol; Kusoljariyakul, Keerati; Rhodes, Michael W; Saisut, Jatuporn; Thongbai, Chitrlada; Vilaithong, Thiraphat; Wichaisirimongkol, Pathom; Wiedemann, Helmut

    2005-01-01

    The SURIYA project at the Fast Neutron Research Facility (FNRF) has been established and is being commissioning to generate femtosecond electron pulses. Theses short pulses are produced by a system consisting of an S-band thermionic cathode RF-gun, an alpha magnet as a magnetic bunch compressor, and a linear accelerator. The characteristics of its major components and the beam characterizations as well as the preliminary experimental results will be presented and discussed.

  14. Cohering power of quantum operations

    Energy Technology Data Exchange (ETDEWEB)

    Bu, Kaifeng, E-mail: bkf@zju.edu.cn [School of Mathematical Sciences, Zhejiang University, Hangzhou 310027 (China); Kumar, Asutosh, E-mail: asukumar@hri.res.in [Harish-Chandra Research Institute, Chhatnag Road, Jhunsi, Allahabad 211019 (India); Homi Bhabha National Institute, Anushaktinagar, Mumbai 400094 (India); Zhang, Lin, E-mail: linyz@zju.edu.cn [Institute of Mathematics, Hangzhou Dianzi University, Hangzhou 310018 (China); Wu, Junde, E-mail: wjd@zju.edu.cn [School of Mathematical Sciences, Zhejiang University, Hangzhou 310027 (China)

    2017-05-18

    Highlights: • Quantum coherence. • Cohering power: production of quantum coherence by quantum operations. • Study of cohering power and generalized cohering power, and their comparison for differentmeasures of quantum coherence. • Operational interpretation of cohering power. • Bound on cohering power of a generic quantum operation. - Abstract: Quantum coherence and entanglement, which play a crucial role in quantum information processing tasks, are usually fragile under decoherence. Therefore, the production of quantum coherence by quantum operations is important to preserve quantum correlations including entanglement. In this paper, we study cohering power–the ability of quantum operations to produce coherence. First, we provide an operational interpretation of cohering power. Then, we decompose a generic quantum operation into three basic operations, namely, unitary, appending and dismissal operations, and show that the cohering power of any quantum operation is upper bounded by the corresponding unitary operation. Furthermore, we compare cohering power and generalized cohering power of quantum operations for different measures of coherence.

  15. Long-lived coherence in carotenoids

    Energy Technology Data Exchange (ETDEWEB)

    Davis, J A; Cannon, E; Van Dao, L; Hannaford, P [ARC Centre of Excellence for Coherent X-ray Science, Centre for Atom Optics and Ultrafast Spectroscopy, Swinburne University of Technology, Victoria 3122 (Australia); Quiney, H M; Nugent, K A, E-mail: jdavis@swin.edu.a [ARC Centre of Excellence for Coherent X-ray Science, School of Physics, University of Melbourne, Victoria 3010 (Australia)

    2010-08-15

    We use two-colour vibronic coherence spectroscopy to observe long-lived vibrational coherences in the ground electronic state of carotenoid molecules, with decoherence times in excess of 1 ps. Lycopene and spheroidene were studied isolated in solution, and within the LH2 light-harvesting complex extracted from purple bacteria. The vibrational coherence time is shown to increase significantly for the carotenoid in the complex, providing further support to previous assertions that long-lived electronic coherences in light-harvesting complexes are facilitated by in-phase motion of the chromophores and surrounding proteins. Using this technique, we are also able to follow the evolution of excited state coherences and find that for carotenoids in the light-harvesting complex the (S{sub 2}|S{sub 0}) superposition remains coherent for more than 70 fs. In addition to the implications of this long electronic decoherence time, the extended coherence allows us to observe the evolution of the excited state wavepacket. These experiments reveal an enhancement of the vibronic coupling to the first vibrational level of the C-C stretching mode and/or methyl-rocking mode in the ground electronic state 70 fs after the initial excitation. These observations open the door to future experiments and modelling that may be able to resolve the relaxation dynamics of carotenoids in solution and in natural light-harvesting systems.

  16. Long-lived coherence in carotenoids

    International Nuclear Information System (INIS)

    Davis, J A; Cannon, E; Van Dao, L; Hannaford, P; Quiney, H M; Nugent, K A

    2010-01-01

    We use two-colour vibronic coherence spectroscopy to observe long-lived vibrational coherences in the ground electronic state of carotenoid molecules, with decoherence times in excess of 1 ps. Lycopene and spheroidene were studied isolated in solution, and within the LH2 light-harvesting complex extracted from purple bacteria. The vibrational coherence time is shown to increase significantly for the carotenoid in the complex, providing further support to previous assertions that long-lived electronic coherences in light-harvesting complexes are facilitated by in-phase motion of the chromophores and surrounding proteins. Using this technique, we are also able to follow the evolution of excited state coherences and find that for carotenoids in the light-harvesting complex the (S 2 |S 0 ) superposition remains coherent for more than 70 fs. In addition to the implications of this long electronic decoherence time, the extended coherence allows us to observe the evolution of the excited state wavepacket. These experiments reveal an enhancement of the vibronic coupling to the first vibrational level of the C-C stretching mode and/or methyl-rocking mode in the ground electronic state 70 fs after the initial excitation. These observations open the door to future experiments and modelling that may be able to resolve the relaxation dynamics of carotenoids in solution and in natural light-harvesting systems.

  17. Partially coherent imaging and spatial coherence wavelets

    International Nuclear Information System (INIS)

    Castaneda, Roman

    2003-03-01

    A description of spatially partially coherent imaging based on the propagation of second order spatial coherence wavelets and marginal power spectra (Wigner distribution functions) is presented. In this dynamics, the spatial coherence wavelets will be affected by the system through its elementary transfer function. The consistency of the model with the both extreme cases of full coherent and incoherent imaging was proved. In the last case we obtained the classical concept of optical transfer function as a simple integral of the elementary transfer function. Furthermore, the elementary incoherent response function was introduced as the Fourier transform of the elementary transfer function. It describes the propagation of spatial coherence wavelets form each object point to each image point through a specific point on the pupil planes. The point spread function of the system was obtained by a simple integral of the elementary incoherent response function. (author)

  18. On-chip nanostructuring and impedance trimming of transparent and flexible ITO electrodes by laser induced coherent sub-20 nm cuts

    Energy Technology Data Exchange (ETDEWEB)

    Afshar, Maziar, E-mail: m.afshar@lmm.uni-saarland.de [Lab for Micromechanics, Microfluidics, and Microactuators, Saarland University, Saarbrücken D-66123 (Germany); Leber, Moritz [Lab for Micromechanics, Microfluidics, and Microactuators, Saarland University, Saarbrücken D-66123 (Germany); Poppendieck, Wigand [Department of Medical Engineering & Neuroprosthetics, Fraunhofer Institute for Biomedical Engineering, St. Ingbert D-66386 (Germany); König, Karsten [Lab for Biophotonics and Laser Technology, Saarland University, Saarbrücken D-66123 (Germany); Seidel, Helmut; Feili, Dara [Lab for Micromechanics, Microfluidics, and Microactuators, Saarland University, Saarbrücken D-66123 (Germany)

    2016-01-01

    Graphical abstract: - Highlights: • A novel method to make sub-20 nm nanopatterning in ITO thin films by laser writing. • A novel way to functionalize ITO bio-electrodes to yield near-field polarizing feature. • A basic characterization of ITO electrodes was performed by impedance spectroscopy. • Presentation of simulations and possible theoretical approaches to explain the results. - Abstract: In this work, the effect of laser-induced nanostructuring of transparent indium tin oxide (ITO) electrodes on flexible glass is investigated. Multi-electrode arrays (MEA) for electrical and optical characterization of biological cells were fabricated using standard MEMS technologies. Optimal sputter parameters concerning oxygen flow, sputter power and ambient pressure for ITO layers with both good optical and electrical properties were determined. Afterwards, coherent sub-20 nm wide and 150 nm deep nanocuts of many micrometers in length were generated within the ITO electrodes by a sub-15 femtosecond (fs) pulsed laser. The influence of laser processing on the electrical and optical properties of electrodes was investigated. The electrochemical impedance of the manufactured electrodes was measured before and after laser modification using electrochemical impedance spectroscopy. A small reduction in electrode impedance was observed. These nanostructured electrodes show also polarizing effects by the visible spectrum.

  19. EDITORIAL: Coherent Control

    Science.gov (United States)

    Fielding, Helen; Shapiro, Moshe; Baumert, Thomas

    2008-04-01

    Quantum mechanics, though a probabilistic theory, gives a 'deterministic' answer to the question of how the present determines the future. In essence, in order to predict future probabilities, we need to (numerically) propagate the time-dependent Schrödinger equation from the present to the future. It is interesting to note that classical mechanics of macroscopic bodies, though reputed to be a deterministic theory, does not allow, due to chaos (which unfortunately is more prevalent than integrability), such clear insights into the future. In contrast, small (e.g., atomic, molecular and photonic) systems which are best understood using the tools of quantum mechanics, do not suffer from chaos, rendering the prediction of the probability-distributions of future events possible. The field of quantum control deals with an important modification of this task, namely, it asks: given a wave function in the present, what dynamics, i.e. what Hamiltonian, guarantees a desired outcome or 'objective' in the future? In practice one may achieve this goal of modifying and finding the desired Hamiltonian by introducing external fields, e.g. laser light. It is then possible to reach the objective in a 'trial-and-error' fashion, performed either numerically or in the laboratory. We can guess or build a Hamiltonian, do an experiment, or propagate the initial wave function to the future, compare the result with the desirable objective, and correct the guess for the Hamiltonian until satisfactory agreement with the objective is reached. A systematic way of executing this procedure is the sub-field called 'optimal control'. The trial-and-error method is often very time consuming and rarely provides mechanistic insight. There are situations where analytical solutions exist, rendering the control strategies more transparent. This is especially so when one can identify quantum interferences as the heart of quantum control, the essence of the field called 'coherent control'. The experience

  20. On Longitudinal Spectral Coherence

    DEFF Research Database (Denmark)

    Kristensen, Leif

    1979-01-01

    It is demonstrated that the longitudinal spectral coherence differs significantly from the transversal spectral coherence in its dependence on displacement and frequency. An expression for the longitudinal coherence is derived and it is shown how the scale of turbulence, the displacement between ...... observation sites and the turbulence intensity influence the results. The limitations of the theory are discussed....

  1. Femtosecond structural dynamics on the atomic length scale

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Dongfang

    2014-03-15

    This thesis reports on the development and application of two different but complementary ultrafast electron diffraction setups built at the Max Planck Research Department for Structural Dynamics. One is an ultra-compact femtosecond electron diffraction (FED) setup (Egun300), which is currently operational (with a maximum electron energy of 150 keV) and provides ultrashort (∝300 fs) and bright (∝10 e/μm{sup 2}) electron bunches. The other one, named as Relativistic Electron Gun for Atomic Exploration (REGAE) is a radio frequency driven 2 to 5 MeV FED setup built in collaboration with different groups from DESY. REGAE was developed as a facility that will provide high quality diffraction with sufficient coherence to even address structural protein dynamics and with electron pulses as short as 20 fs (FWHM). As one of the first students in Prof. R.J. Dwayne Miller's group, I led the femtosecond (fs) laser sub-group at REGAE being responsible for the construction of different key optical elements required to drive both of aforementioned FED systems. A third harmonic generation (THG) and a nonlinear optical parametric amplifier (NOPA) have been used for the photo-generation of ultrashort electron bursts as well as sample laser excitation. Different diagnostic tools have been constructed to monitor the performance of the fs optical system. A fast autocorrelator was developed to provide on the fly pulse duration correction. A transient-grating frequency-resolved optical gating (TG-FROG) was built to obtain detail information about the characteristics of fs optical pulse, i.e. phase and amplitude of its spectral components. In addition to these optical setups, I developed a fs optical pump-probe system, which supports broadband probe pulses. This setup was successfully applied to investigate the semiconductor-to-metal photoinduced phase transition in VO{sub 2} and the ultrafast photo-reduction mechanism of graphene oxide. In regard to FED setups, I have been

  2. Femtosecond structural dynamics on the atomic length scale

    International Nuclear Information System (INIS)

    Zhang, Dongfang

    2014-03-01

    This thesis reports on the development and application of two different but complementary ultrafast electron diffraction setups built at the Max Planck Research Department for Structural Dynamics. One is an ultra-compact femtosecond electron diffraction (FED) setup (Egun300), which is currently operational (with a maximum electron energy of 150 keV) and provides ultrashort (∝300 fs) and bright (∝10 e/μm 2 ) electron bunches. The other one, named as Relativistic Electron Gun for Atomic Exploration (REGAE) is a radio frequency driven 2 to 5 MeV FED setup built in collaboration with different groups from DESY. REGAE was developed as a facility that will provide high quality diffraction with sufficient coherence to even address structural protein dynamics and with electron pulses as short as 20 fs (FWHM). As one of the first students in Prof. R.J. Dwayne Miller's group, I led the femtosecond (fs) laser sub-group at REGAE being responsible for the construction of different key optical elements required to drive both of aforementioned FED systems. A third harmonic generation (THG) and a nonlinear optical parametric amplifier (NOPA) have been used for the photo-generation of ultrashort electron bursts as well as sample laser excitation. Different diagnostic tools have been constructed to monitor the performance of the fs optical system. A fast autocorrelator was developed to provide on the fly pulse duration correction. A transient-grating frequency-resolved optical gating (TG-FROG) was built to obtain detail information about the characteristics of fs optical pulse, i.e. phase and amplitude of its spectral components. In addition to these optical setups, I developed a fs optical pump-probe system, which supports broadband probe pulses. This setup was successfully applied to investigate the semiconductor-to-metal photoinduced phase transition in VO 2 and the ultrafast photo-reduction mechanism of graphene oxide. In regard to FED setups, I have been deeply involved in

  3. Thickness-dependent coherent phonon frequency in ultrathin FeSe/SrTiO3 films

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Shuolong [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Sobota, Jonathan A. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Leuenberger, Dominik [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Kemper, Alexander F. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lee, James J. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Schmitt, Felix T. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Li, Wei [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Moore, Rob G. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States); Kirchmann, Patrick S. [SLAC National Accelerator Lab., Menlo Park, CA (United States); Shen, Zhi -Xun [SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)

    2015-06-01

    Ultrathin FeSe films grown on SrTiO3 substrates are a recent milestone in atomic material engineering due to their important role in understanding unconventional superconductivity in Fe-based materials. By using femtosecond time- and angle-resolved photoelectron spectroscopy, we study phonon frequencies in ultrathin FeSe/SrTiO3 films grown by molecular beam epitaxy. After optical excitation, we observe periodic modulations of the photoelectron spectrum as a function of pump–probe delay for 1-unit-cell, 3-unit-cell, and 60-unit-cell thick FeSe films. The frequencies of the coherent intensity oscillations increase from 5.00 ± 0.02 to 5.25 ± 0.02 THz with increasing film thickness. By comparing with previous works, we attribute this mode to the Se A1g phonon. The dominant mechanism for the phonon softening in 1-unit-cell thick FeSe films is a substrate-induced lattice strain. Results demonstrate an abrupt phonon renormalization due to a lattice mismatch between the ultrathin film and the substrate.

  4. Coherence and relaxation in energy transfer processes in condensed phases

    International Nuclear Information System (INIS)

    Shelby, R.M.

    1978-03-01

    Investigations of electronic triplet and vibrational energy transfer dynamics and relaxation processes are presented. Emphasis is placed on understanding the role of coherence and interactions which tend to destroy the coherence. In the case of triplet excitons at low temperatures, the importance of coherence in energy migration can be established, and the average coherence parameters can be experimentally determined. In the case of vibrational excitations, both picosecond spectroscopic studies of vibrational relaxation and spontaneous Raman spectroscopy are used to characterize the dynamics and give increased insight into the nature of the mechanisms responsible for vibrational dephasing. The design and operation of the picosecond apparatus used in these experiments is also described

  5. Time-resolved Femtosecond Photon Echo Probes Bimodal Solvent Dynamics

    NARCIS (Netherlands)

    Pshenichnikov, M.S; Duppen, K.; Wiersma, D. A.

    1995-01-01

    We report on time-resolved femtosecond photon echo experiments of a dye molecule in a polar solution. The photon echo is time resolved by mixing the echo with a femtosecond gate pulse in a nonlinear crystal. It is shown that the temporal profile of the photon echo allows separation of the

  6. Femtosecond Non-Markovian Optical Dynamics in Solution

    NARCIS (Netherlands)

    Nibbering, Erik T.J.; Wiersma, Douwe A.; Duppen, Koos

    1991-01-01

    Femtosecond photon-echo experiments on sodium resorufin in dimethylsulfoxide at room temperature show that optical dephasing in solution is of non-Markovian character. A single Gauss-Markov stochastic modulation process is used to interpret both the femtosecond light-scattering results and the

  7. Novel techniques in VUV high-resolution spectroscopy

    NARCIS (Netherlands)

    Ubachs, W.M.G.; Salumbides, E.J.; Eikema, K.S.E.; de Oliveira, N.; Nahon, L.

    2014-01-01

    Novel VUV sources and techniques for VUV spectroscopy are reviewed. Laser-based VUV sources have been developed via non-linear upconversion of laser pulses in the nanosecond (ns), the picosecond (ps), and femtosecond (fs) domain, and are applied in high-resolution gas phase spectroscopic studies.

  8. Recent advances in femtosecond laser-assisted cataract surgery

    Directory of Open Access Journals (Sweden)

    Zhao-Jie Chu

    2013-07-01

    Full Text Available Perfect vision and fewer complications is our goal in cataract surgery, femtosecond laser-assisted cataract surgery hold the promise. Applications of femtosecond laser technology for capsulotomy, nuclear fragmentation and corneal incision in cataract surgery bring a new level of accuracy, reproducibility and predictability over the current cataract surgery. The femtosecond laser produces capsulotomies that are more precise, accurate, reproducible, and stronger than those created with the conventional manual technique, and further helps maintain proper positioning of the IOL. Femtosecond laser in nuclear fragmentation lead to a lower effective phacoemulsification time, and the corneal incision is more stable. But currently there are some complications and a clear learning curve associated with the use of femtosecond lasers for cataract surgery. The long-term safety and visual outcomes still need further investigation.

  9. Spatially resolved nanostructural transformation in graphite under femtosecond laser irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Marcu, A., E-mail: aurelian.marcu@inflpr.ro [National Institute for Laser, Plasma and Radiation Physics, 077125 Bucharest (Romania); Avotina, L. [Institute of Chemical Physics, University of Latvia, Kronvalda 4, LV 1010 Riga (Latvia); Porosnicu, C. [National Institute for Laser, Plasma and Radiation Physics, 077125 Bucharest (Romania); Marin, A. [Ilie Murgulescu” Institute of Physical Chemistry, 202 Splaiul Independentei 060021, Bucharest (Romania); Grigorescu, C.E.A. [National Institute R& D for Optoelectronics INOE 2000, 077125 Bucharest (Romania); Ursescu, D. [National Institute for Laser, Plasma and Radiation Physics, 077125 Bucharest (Romania); Lungu, M. [National Institute of Materials Physics Atomistilor Str., 105 bis, 077125, Magurele (Romania); Demitri, N. [Hard X-ray Beamline and Structural Biology, Elettra-Sincrotrone Trieste, Strada Statale 14 - km 163,5 in AREA Science Park, 34149 Basovizza TS Italy (Italy); Lungu, C.P. [National Institute for Laser, Plasma and Radiation Physics, 077125 Bucharest (Romania)

    2015-11-15

    Graphical abstract: - Highlights: • Polycrystalline graphite was irradiated with a high power fs (IR) laser. • Presence of a diamond peak was detected by synchrotron XRD. • XPS and Raman showed in-depth sp{sup 3}% increase at tens of nm below the surface. • sp{sup 3}% is increasing with laser power density but it is independent of photon absorption rate. • Graphite crystallite size locally increase at tens of nanometers below the irradiated spots. - Abstract: A polycrystalline graphite target was irradiated using infrared (800 nm) femtosecond (120 fs) laser pulses of different energies. Increase of sp{sup 3} bonds percentage and possible diamond crystal formation were investigated ‘in-depth’ and on the irradiated surfaces. Synchrotron X-ray diffraction pattern have shown the presence of a diamond peak in one of the irradiated zones while X-ray photoelectron spectroscopy investigations have shown an increasing tendency of the sp{sup 3} percent in the low power irradiated areas and similarly ‘in the depth’ of the higher power irradiated zones. Multiple wavelength Micro-Raman investigations have confirmed this trend along with an ‘in-depth’ (but not on the surface) increase of the crystallite size. Based on the wavelength dependent photon absorption into graphite, the observed effects are correlated with high density photon per atom and attributed to the melting and recrystallization processes taking place tens of nanometers below the target surface.

  10. Spatially resolved nanostructural transformation in graphite under femtosecond laser irradiation

    International Nuclear Information System (INIS)

    Marcu, A.; Avotina, L.; Porosnicu, C.; Marin, A.; Grigorescu, C.E.A.; Ursescu, D.; Lungu, M.; Demitri, N.; Lungu, C.P.

    2015-01-01

    Graphical abstract: - Highlights: • Polycrystalline graphite was irradiated with a high power fs (IR) laser. • Presence of a diamond peak was detected by synchrotron XRD. • XPS and Raman showed in-depth sp 3 % increase at tens of nm below the surface. • sp 3 % is increasing with laser power density but it is independent of photon absorption rate. • Graphite crystallite size locally increase at tens of nanometers below the irradiated spots. - Abstract: A polycrystalline graphite target was irradiated using infrared (800 nm) femtosecond (120 fs) laser pulses of different energies. Increase of sp 3 bonds percentage and possible diamond crystal formation were investigated ‘in-depth’ and on the irradiated surfaces. Synchrotron X-ray diffraction pattern have shown the presence of a diamond peak in one of the irradiated zones while X-ray photoelectron spectroscopy investigations have shown an increasing tendency of the sp 3 percent in the low power irradiated areas and similarly ‘in the depth’ of the higher power irradiated zones. Multiple wavelength Micro-Raman investigations have confirmed this trend along with an ‘in-depth’ (but not on the surface) increase of the crystallite size. Based on the wavelength dependent photon absorption into graphite, the observed effects are correlated with high density photon per atom and attributed to the melting and recrystallization processes taking place tens of nanometers below the target surface.

  11. Femtosecond laser surface structuring of molybdenum thin films

    Energy Technology Data Exchange (ETDEWEB)

    Kotsedi, L., E-mail: Kotsedi@tlabs.ac.za [UNESCO-UNISA Africa Chair in Nanosciences-Nanotechnology, College of Graduate Studies, University of South Africa, Muckleneuk ridge, PO Box 392, Pretoria (South Africa); Nanosciences African Network (NANOAFNET), iThemba LABS-National Research Foundation, 1 Old Faure Road, Somerset West 7129, PO Box 722, Somerset West, Western Cape Province (South Africa); Mthunzi, P. [Council for Scientific and Industrial Research (CSIR), Biophotonics Lab: National Laser Centre Pretoria, 0001 (South Africa); Nuru, Z.Y. [UNESCO-UNISA Africa Chair in Nanosciences-Nanotechnology, College of Graduate Studies, University of South Africa, Muckleneuk ridge, PO Box 392, Pretoria (South Africa); Nanosciences African Network (NANOAFNET), iThemba LABS-National Research Foundation, 1 Old Faure Road, Somerset West 7129, PO Box 722, Somerset West, Western Cape Province (South Africa); Eaton, S.M. [Physics Department, Politecnico di Milano, Piazza Leonardo Da Vinci, 32, 20133 Milano (Italy); Center for Nano Science and Technology, Istituto Italiano di Tecnologia, Via Pascoli 70/3, 20133 Milano, Itala (Italy); Sechoghela, P.; Mongwaketsi, N. [UNESCO-UNISA Africa Chair in Nanosciences-Nanotechnology, College of Graduate Studies, University of South Africa, Muckleneuk ridge, PO Box 392, Pretoria (South Africa); Nanosciences African Network (NANOAFNET), iThemba LABS-National Research Foundation, 1 Old Faure Road, Somerset West 7129, PO Box 722, Somerset West, Western Cape Province (South Africa); Ramponi, R. [Institute for Photonics and Nanotechnologies (IFN)–CNR, Piazza Leanardo Da Vinci, 32, 20133 Milano (Italy); Maaza, M. [UNESCO-UNISA Africa Chair in Nanosciences-Nanotechnology, College of Graduate Studies, University of South Africa, Muckleneuk ridge, PO Box 392, Pretoria (South Africa); Nanosciences African Network (NANOAFNET), iThemba LABS-National Research Foundation, 1 Old Faure Road, Somerset West 7129, PO Box 722, Somerset West, Western Cape Province (South Africa)

    2015-10-30

    Highlights: • Color change of the molybdenum thin film from shinny to violet–yellowish color after laser irradiation at various laser powers. • Formation of the molybdenum dioxide coating after laser exposure, as confirmed by the X-ray diffraction spectrometry. • Selective solar absorbing nature of the laser exposed films. • Study of the binding energies is presented in this contribution using the XPS spectrometry. - Abstract: This contribution reports on the femtosecond surface structuring of molybdenum thin coatings deposited by electron beam evaporation onto Corning glass substrates. The 1-D type periodic grating lines created by such an ablation showed that the widths of the shallow grooves followed a logarithmic dependence with the laser energy incident on the molybdenum film. The electronic valence “x” of the created oxide surface layer MoO{sub x} was found to be incident laser power dependent via Rutherford backscattering spectrometry, X-ray photoelectron spectroscopy and X-ray diffraction investigations. Such a photo-induced MoO{sub x}–Mo nanocomposite exhibited effective selective solar absorption in the UV–vis–IR spectral range.

  12. Femtosecond laser-induced surface wettability modification of polystyrene surface

    Science.gov (United States)

    Wang, Bing; Wang, XinCai; Zheng, HongYu; Lam, YeeCheong

    2016-12-01

    In this paper, we demonstrated a simple method to create either a hydrophilic or hydrophobic surface. With femtosecond laser irradiation at different laser parameters, the water contact angle (WCA) on polystyrene's surface can be modified to either 12.7° or 156.2° from its original WCA of 88.2°. With properly spaced micro-pits created, the surface became hydrophilic probably due to the spread of the water droplets into the micro-pits. While with properly spaced micro-grooves created, the surface became rough and more hydrophobic. We investigated the effect of laser parameters on WCAs and analyzed the laser-treated surface roughness, profiles and chemical bonds by surface profilometer, scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). For the laser-treated surface with low roughness, the polar (such as C—O, C=O, and O—C=O bonds) and non-polar (such as C—C or C—H bonds) groups were found to be responsible for the wettability changes. While for a rough surface, the surface roughness or the surface topography structure played a more significant role in the changes of the surface WCA. The mechanisms involved in the laser surface wettability modification process were discussed.

  13. Theoretical femtosecond physics atoms and molecules in strong laser fields

    CERN Document Server

    Grossmann, Frank

    2018-01-01

    This textbook extends from the basics of femtosecond physics all the way to some of the latest developments in the field. In this updated edition, the chapter on laser-driven atoms is augmented by the discussion of two-electron atoms interacting with strong and short laser pulses, as well as by a review of ATI rings and low energy structures in photo-electron spectra. In the chapter on laser-driven molecules a discussion of 2D infrared spectroscopy is incorporated. Theoretical investigations of atoms and molecules interacting with pulsed lasers up to atomic field strengths on the order of 10^16 W/cm² are leading to an understanding of many challenging experimental discoveries. The presentation starts with a brief introduction to pulsed laser physics. The basis for the non-perturbative treatment of laser-matter interaction in the book is the time-dependent Schrödinger equation. Its analytical as well as numerical solution are laid out in some detail. The light field is treated classically and different possi...

  14. Coherent fiber supercontinuum laser for nonlinear biomedical imaging

    DEFF Research Database (Denmark)

    Tu, Haohua; Liu, Yuan; Liu, Xiaomin

    2012-01-01

    Nonlinear biomedical imaging has not benefited from the well-known techniques of fiber supercontinuum generation for reasons such as poor coherence (or high noise), insufficient controllability, low spectral power intensity, and inadequate portability. Fortunately, a few techniques involving...... nonlinear fiber optics and femtosecond fiber laser development have emerged to overcome these critical limitations. These techniques pave the way for conducting point-of-care nonlinear biomedical imaging by a low-maintenance cost-effective coherent fiber supercontinuum laser, which covers a broad emission...... wavelength of 350-1700 nm. A prototype of this laser has been demonstrated in label-free multimodal nonlinear imaging of cell and tissue samples.© (2012) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only....

  15. CIRCE, the Coherent Infrared Center at the ALS

    International Nuclear Information System (INIS)

    Byrd, John M.; De Santis, Stefano; Jung, Jin-Young; Li, Derun; Martin, Michael C.; McKinney, W.; Munson, Dawn; Nishimura, Hiroshi; Robin, David S.; Sannibale, Fernando; Schlueter, Ross; Venturini, Marco; Wan, Weishi; Zolotorev, Max

    2004-01-01

    CIRCE (Coherent InfraRed CEnter) is a proposal for a new electron storage ring to be built at the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory (LBNL). The ring design is optimized for the generation of coherent synchrotron radiation (CSR) in the terahertz frequency range. Among others, CIRCE operation includes three interesting CSR modes: ultra stable, femtosecond laser slicing and broadband bursting. CSR allows CIRCE to generate an extremely high flux in the terahertz frequency region. The many orders of magnitude increase in the intensity over that presently achievable by conventional sources, has the potential to enable new science experiments. The characteristics of CIRCE and of the different modes of operation are described in this paper

  16. High level harmonic radiation: atto-second impulse generation, application to coherent radiation

    International Nuclear Information System (INIS)

    Kovacev, Milutin

    2003-01-01

    The work presented in this thesis is dedicated to the characterization and optimization of the unique properties of high order harmonic generation in a rare gas: high brilliance, short pulse duration (femtosecond to atto-second, 1 as = 10"-"1"8 s and good mutual coherence. In the first part of this work, we concentrate on the exploitation of a scaling law using a high-energy laser loosely focused inside an extended gaseous medium. For the first time, the generated harmonic energy exceeds the 1 μJ level per laser pulse using the fifteenth harmonic order at a wavelength of 53 nm. The conversion efficiency reaches 4.10"-"5, which results from the combination of a strong dipolar response and a good phase matching within a generating volume that is extended by self guiding of the generating laser pulse. In the second part, our interest is devoted to the temporal profile of the harmonic emission and its atto-second structure. We first demonstrate the feasibility of a spatial/spectral selection of the contributions associated to the two main electronic trajectories, allowing thereby the generation of regular atto-second pulse trains. We then characterize such a pulse train by the measurement of the relative phases of consecutive harmonics. Finally, we describe an original technique for the temporal confinement of the harmonic emission by manipulating the ellipticity of the generating laser beam. In the third part, our interest is dedicated to the mutual coherence properties of the harmonic emission. We first demonstrate the precise control of the relative phase of the harmonic pulses by multiple beam interference in the XUV. This frequency-domain interferometry using four phase-locked temporally separated pulses shows an extreme sensitivity to the relative phase of the pulses on an atto-second time scale. We then measure the first order autocorrelation trace of the harmonic beam thanks to the generation of two harmonic sources mutually coherent and spatially separated

  17. Microstructure and chemical bond evolution of diamond-like carbon films machined by femtosecond laser

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Jing; Wang, Chunhui [Science and Technology on Thermostructure Composite Materials Laboratory, Northwestern Polytechnical University, Xi’an 710072 (China); Liu, Yongsheng, E-mail: yongshengliu@nwpu.edu.cn [Science and Technology on Thermostructure Composite Materials Laboratory, Northwestern Polytechnical University, Xi’an 710072 (China); Cheng, Laifei [Science and Technology on Thermostructure Composite Materials Laboratory, Northwestern Polytechnical University, Xi’an 710072 (China); Li, Weinan [State Key Laboratory of Transient Optics and Photonics, Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi’an 10068 (China); Zhang, Qing [Science and Technology on Thermostructure Composite Materials Laboratory, Northwestern Polytechnical University, Xi’an 710072 (China); Yang, Xiaojun [State Key Laboratory of Transient Optics and Photonics, Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences, Xi’an 10068 (China)

    2015-06-15

    Highlights: • The machining depth was essentially proportional to the laser power. • The well patterned microgrooves and ripple structures with nanoparticles were formed distinctly in the channels. And the number of nanoparticles increased with the processing power as well. • It revealed a conversion from amorphous carbon to nanocrystalline graphite after laser treated with increasing laser power. • It showed that a great decrease of sp{sup 3}/sp{sup 2} after laser treatment. - Abstract: Femtosecond laser is of great interest for machining high melting point and hardness materials such as diamond-like carbon, SiC ceramic, et al. In present work, the microstructural and chemical bond evolution of diamond-like carbon films were investigated using electron microscopy and spectroscopy techniques after machined by diverse femtosecond laser power in air. The results showed the machining depth was essentially proportional to the laser power. The well patterned microgrooves and ripple structures with nanoparticles were formed distinctly in the channels. Considering the D and G Raman band parameters on the laser irradiation, it revealed a conversion from amorphous carbon to nanocrystalline graphite after laser treated with increasing laser power. X-ray photoelectron spectroscopy analysis showed a great decrease of sp{sup 3}/sp{sup 2} after laser treatment.

  18. Spatially and temporally resolved diagnostics of dense sprays using gated, femtosecond, digital holography

    Science.gov (United States)

    Trolinger, James D.; Dioumaev, Andrei K.; Ziaee, Ali; Minniti, Marco; Dunn-Rankin, Derek

    2017-08-01

    This paper describes research that demonstrated gated, femtosecond, digital holography, enabling 3D microscopic viewing inside dense, almost opaque sprays, and providing a new and powerful diagnostics capability for viewing fuel atomization processes never seen before. The method works by exploiting the extremely short coherence and pulse length (approximately 30 micrometers in this implementation) provided by a femtosecond laser combined with digital holography to eliminate multiple and wide angle scattered light from particles surrounding the injection region, which normally obscures the image of interest. Photons that follow a path that differs in length by more than 30 micrometers from a straight path through the field to the sensor do not contribute to the holographic recording of photons that travel in a near straight path (ballistic and "snake" photons). To further enhance the method, off-axis digital holography was incorporated to enhance signal to noise ratio and image processing capability in reconstructed images by separating the conjugate images, which overlap and interfere in conventional in-line holography. This also enables digital holographic interferometry. Fundamental relationships and limitations were also examined. The project is a continuing collaboration between MetroLaser and the University of California, Irvine.

  19. Fast pulses and slow atoms: making microKelvin molecules using femtosecond lasers

    Science.gov (United States)

    Walmsley, Ian

    2008-05-01

    We discuss a general approach to the formation of ultracold ground state molecules by synthesis from pairs of cold atoms using shaped ultrashort optical pulses. This method combines an effective and widely applicable control technology to the problem of preparing molecules is the ground state of all their degrees of freedom. The broad bandwidth of femtosecond pulses provides and number of options for removing energy from a pair of colliding atoms, and binding them with little or no vibrational energy. We shall give examples of possible strategies, and report on experiments demonstrating photoassocation using coherent control, and measuring wavepacket dynamics by femtosecond pump probe molecular ionization. Prospects for stabilizing the molecules by protecting them from further collisions, and for increasing the range of internuclear separations that can be associated will be pointed out. This work is funded by the UK EPSRC, and has contributions from J. Petrovic, A. Wyatt, A. Dicks, D. McCabe, D. England, M. Friedman, H. Martay, T. Koehler, C. Foot and collaborations with F. Masnou-Seeuws and J. Mur-Petit.

  20. Analysis of Femtosecond Timing Noise and Stability in Microwave Components

    International Nuclear Information System (INIS)

    2011-01-01

    To probe chemical dynamics, X-ray pump-probe experiments trigger a change in a sample with an optical laser pulse, followed by an X-ray probe. At the Linac Coherent Light Source, LCLS, timing differences between the optical pulse and x-ray probe have been observed with an accuracy as low as 50 femtoseconds. This sets a lower bound on the number of frames one can arrange over a time scale to recreate a 'movie' of the chemical reaction. The timing system is based on phase measurements from signals corresponding to the two laser pulses; these measurements are done by using a double-balanced mixer for detection. To increase the accuracy of the system, this paper studies parameters affecting phase detection systems based on mixers, such as signal input power, noise levels, temperature drift, and the effect these parameters have on components such as the mixers, splitters, amplifiers, and phase shifters. Noise data taken with a spectrum analyzer show that splitters based on ferrite cores perform with less noise than strip-line splitters. The data also shows that noise in specific mixers does not correspond with the changes in sensitivity per input power level. Temperature drift is seen to exist on a scale between 1 and 27 fs/ o C for all of the components tested. Results show that any components using more metallic conductor tend to exhibit more noise as well as more temperature drift. The scale of these effects is large enough that specific care should be given when choosing components and designing the housing of high precision microwave mixing systems for use in detection systems such as the LCLS. With these improvements, the timing accuracy can be improved to lower than currently possible.

  1. Coherent control of interfering wave packets in dissociating HD+ molecules: the role of phase and delay time

    International Nuclear Information System (INIS)

    Qin, Chaochao; Zhang, Lili; Zhang, Xianzhou; Liu, Yufang; Qiu, Xuejun

    2016-01-01

    The coherent control of interference between dissociating wave packets of the HD + molecules generated by a pair of time-delayed and phase-locked femtosecond laser pulses is theoretically studied by using the time-dependent quantum wave packet method. The density function in both coordinate and momentum representation are presented and discussed. It is demonstrated that the interference pattern is observed in both coordinate and momentum density functions. The interference undergoes a π-phase shift when the delay time between the two phase-locked femtosecond laser pulses is changed by half an optical period. In particular, the number of interference fringes, the fringe spacing in the R-dependent density distribution |ψ(R)| 2 , and the modulation period of the energy-dependent distribution of the fragments P(E) can be tuned by two phase-locked femtosecond pulses. (paper)

  2. Colorizing metals with femtosecond laser pulses

    International Nuclear Information System (INIS)

    Vorobyev, A. Y.; Guo Chunlei

    2008-01-01

    For centuries, it had been the dream of alchemists to turn inexpensive metals into gold. Certainly, it is not enough from an alchemist's point of view to transfer only the appearance of a metal to gold. However, the possibility of rendering a certain metal to a completely different color without coating can be very interesting in its own right. In this work, we demonstrate a femtosecond laser processing technique that allows us to create a variety of colors on a metal that ultimately leads us to control its optical properties from UV to terahertz

  3. Optofluidic Microlasers based on Femtosecond Micromachining Technology

    Directory of Open Access Journals (Sweden)

    Simoni F.

    2017-08-01

    Full Text Available We present the different optofluidic lasers which have been realized using the Femtosecond Micromachining technique to fabricate the monolithic optofluidic structures in glass chips. We show how the great flexibility of this 3D technique allows getting different kind of optical cavities. The most recent devices fabricated by this technique as ring shaped and Fabry-Perot resonators show excellent emission performances.We also point out how the addition of the inkjet printing technique provides further opportunities in realizing optofluidic chips.

  4. Femtosecond technology for science, industry and medicine

    International Nuclear Information System (INIS)

    Stingl, A.; Teraoka, Hiroshi

    2000-01-01

    Five years after introduction of the first ever prism less sub-20 Femtosecond oscillator, inventor of the chirped mirror technology are ranging from 10-fs-high power Oscillators with peak power levels up to MW regime, to ultra fast amplifier system in the GW regime, which became commercially available now. Advances in the optical and mechanical design yield highly compact and reliable laser systems ready to serve for scientific application as well as for real world application in diagnostics, medicine and micro-machining. (author)

  5. 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.

  6. Generation of dual-wavelength, synchronized, tunable, high energy, femtosecond laser pulses with nearly perfect gaussian spatial profile

    Science.gov (United States)

    Wang, J.-K.; Siegal, Y.; Lü, C.; Mazur, E.

    1992-07-01

    We use self-phase modulation in a single-mode fiber to produce broadband femtosecond laser pulses. Subsequent amplification through two Bethune cells yields high-energy, tunable, pulses synchronized with the output of an amplified colliding-pulse-modelocked (CPM) laser. We routinely obtain tunable 200 μJ pulses of 42 fs (fwhm) duration with a nearly perfect gaussian spatial profile. Although self-phase modulation in a single-mode fiber is widely used in femtosecond laser systems, amplification of a fiber-generated supercontinuum in a Bethune cell amplifier is a new feature which maintains the high-quality spatial profile while providing high gain. This laser system is particularly well suited for high energy dual-wavelength pump=probe experiments and time-resolved four-wave mixing spectroscopy.

  7. Vibrational Spectroscopy of Laser Cooled CaH

    Science.gov (United States)

    2015-10-28

    commercially available titanium -sapphire laser without any modification as explained in detail in subsection 4.2. Because these are higher-order...Briefly, a diode laser operates by emitting photons when current is run through the active region of between a n-type and p-type cladding layers. This...address all the rotational levels. We use a mode-locked femtosecond Titanium -Sapphire (Ti:Sapph) laser . For our experiments, we used a Coherent Mira

  8. Femtosecond X-ray Pulses from a Spatially Chirped Electron Bunch in a SASE FEL

    Energy Technology Data Exchange (ETDEWEB)

    Emma, P.

    2003-01-14

    We propose a simple method to produce short x-ray pulses using a spatially chirped electron bunch in a SASE FEL. The spatial chirp is generated using an rf deflector which produces a transverse offset (in y and/or y') correlated with the longitudinal bunch position. Since the FEL gain is very sensitive to an initial offset in the transverse phase space at the entrance of the undulator, only a small portion of the electron bunch with relatively small transverse offset will interact significantly with the radiation, resulting in an x-ray pulse length much shorter than the electron bunch length. The x-ray pulse is also naturally phase locked to the rf deflector and so allows high precision timing synchronization. We discuss the generation and transport of such a spatially chirped electron beam and show that tens of femtosecond long pulse can be generated for the linac coherent light source (LCLS).

  9. Fixed target matrix for femtosecond time-resolved and in situ serial micro-crystallography

    Directory of Open Access Journals (Sweden)

    C. Mueller

    2015-09-01

    Full Text Available We present a crystallography chip enabling in situ room temperature crystallography at microfocus synchrotron beamlines and X-ray free-electron laser (X-FEL sources. Compared to other in situ approaches, we observe extremely low background and high diffraction data quality. The chip design is robust and allows fast and efficient loading of thousands of small crystals. The ability to load a large number of protein crystals, at room temperature and with high efficiency, into prescribed positions enables high throughput automated serial crystallography with microfocus synchrotron beamlines. In addition, we demonstrate the application of this chip for femtosecond time-resolved serial crystallography at the Linac Coherent Light Source (LCLS, Menlo Park, California, USA. The chip concept enables multiple images to be acquired from each crystal, allowing differential detection of changes in diffraction intensities in order to obtain high signal-to-noise and fully exploit the time resolution capabilities of XFELs.

  10. Coupled wave equations theory of surface-enhanced femtosecond stimulated Raman scattering.

    Science.gov (United States)

    McAnally, Michael O; McMahon, Jeffrey M; Van Duyne, Richard P; Schatz, George C

    2016-09-07

    We present a coupled wave semiclassical theory to describe plasmonic enhancement effects in surface-enhanced femtosecond stimulated Raman scattering (SE-FSRS). A key result is that the plasmon enhanced fields which drive the vibrational equation of motion for each normal mode results in dispersive lineshapes in the SE-FSRS spectrum. This result, which reproduces experimental lineshapes, demonstrates that plasmon-enhanced stimulated Raman methods provide unique sensitivity to a plasmonic response. Our derived SE-FSRS theory shows a plasmonic enhancement of |gpu|(2)ImχR(ω)gst (2)/ImχR(ω), where |gpu|(2) is the absolute square of the plasmonic enhancement from the Raman pump, χR(ω) is the Raman susceptibility, and gst is the plasmonic enhancement of the Stokes field in SE-FSRS. We conclude with a discussion on potential future experimental and theoretical directions for the field of plasmonically enhanced coherent Raman scattering.

  11. In Situ Monitoring of Chemical Reactions at a Solid-Water Interface by Femtosecond Acoustics.

    Science.gov (United States)

    Shen, Chih-Chiang; Weng, Meng-Yu; Sheu, Jinn-Kong; Yao, Yi-Ting; Sun, Chi-Kuang

    2017-11-02

    Chemical reactions at a solid-liquid interface are of fundamental importance. Interfacial chemical reactions occur not only at the very interface but also in the subsurface area, while existing monitoring techniques either provide limited spatial resolution or are applicable only for the outmost atomic layer. Here, with the aid of the time-domain analysis with femtosecond acoustics, we demonstrate a subatomic-level-resolution technique to longitudinally monitor chemical reactions at solid-water interfaces, capable of in situ monitoring even the subsurface area under atmospheric conditions. Our work was proven by monitoring the already-known anode oxidation process occurring during photoelectrochemical water splitting. Furthermore, whenever the oxide layer thickness equals an integer  number of the effective atomic layer thickness, the measured acoustic echo will show higher signal-to-noise ratios with reduced speckle noise, indicating the quantum-like behavior of this coherent-phonon-based technique.

  12. 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

  13. Visible/IR light and x-rays in femtosecond synchronism from an x-ray free-electron laser

    International Nuclear Information System (INIS)

    Adams, B. A.; Experimental Facilities Division

    2005-01-01

    A way is proposed to obtain pulses of visible/infrared light in femtosecond synchronism with x-rays from an x-ray free-electron laser (XFEL), using the recently proposed emittance-slicing technique. In an XFEL undulator, only the short section of an electron bunch whose emittance is left unchanged by the slicing will emit intense coherent x-rays in the XFEL undulator. At the same time, the bunch emits highly collimated transition undulator radiation (TUR) into a cone whose opening angle is the reciprocal relativisticity parameter gamma. Due to the variation of the transverse momentum induced by the emittance slicing, the effective number of charges contributing to the TUR varies along the bunch, and is higher in the sliced-out part that emits the coherent x-rays. As with coherent synchrotron radiation (CSR), the TUR is thus coherently enhanced (CTUR) at near-infrared wavelengths. Coming from the same part of the bunch the CTUR and the coherent x-rays are perfectly synchronized to each other. Because both types of radiation are generated in the long straight XFEL undulator, there are no dispersion effects that might induce a timing jitter. With typical XFEL parameters, the energy content of the single optical cycle of near-IR CTUR light is about 100 Nano-Joule, which is quite sufficient for most pump-probe experiments

  14. Femtosecond laser surface texturing of titanium as a method to reduce the adhesion of Staphylococcus aureus and biofilm formation

    Energy Technology Data Exchange (ETDEWEB)

    Cunha, Alexandre [Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais 1, 1049-001 Lisboa (Portugal); Bordeaux University, Institute of Chemistry & Biology of Membranes & Nanoobjects (CBMN UMR 5248, CNRS), European Institute of Chemistry and Biology, 2 Rue Robert Escarpit, 33607 Pessac (France); Elie, Anne-Marie [Bordeaux University, CBMN UMR 5248, CNRS, Bordeaux Science Agro, 1 Rue du G. de Gaulle, 33170 Gradignan (France); Plawinski, Laurent [Bordeaux University, Institute of Chemistry & Biology of Membranes & Nanoobjects (CBMN UMR 5248, CNRS), European Institute of Chemistry and Biology, 2 Rue Robert Escarpit, 33607 Pessac (France); Serro, Ana Paula [Instituto Superior Técnico, Universidade de Lisboa, CQE-Centro de Química Estrutural, Av. Rovisco Pais 1, 1049-001 Lisbon (Portugal); Botelho do Rego, Ana Maria [Instituto Superior Técnico, Universidade de Lisboa, CQFM-Centro de Química-Física Molecular and Institute of Nanoscience and Nanotechnology - IN, Av. Rovisco Pais 1, 1049-001 Lisbon (Portugal); Almeida, Amélia [Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais 1, 1049-001 Lisboa (Portugal); Urdaci, Maria C. [Bordeaux University, CBMN UMR 5248, CNRS, Bordeaux Science Agro, 1 Rue du G. de Gaulle, 33170 Gradignan (France); Durrieu, Marie-Christine [Bordeaux University, Institute of Chemistry & Biology of Membranes & Nanoobjects (CBMN UMR 5248, CNRS), European Institute of Chemistry and Biology, 2 Rue Robert Escarpit, 33607 Pessac (France); Vilar, Rui, E-mail: rui.vilar@tecnico.ulisboa.pt [Instituto Superior Técnico, Universidade de Lisboa, Av. Rovisco Pais 1, 1049-001 Lisboa (Portugal)

    2016-01-01

    Graphical abstract: - Highlights: • The short-term adhesion of Staphylococcus aureus onto femtosecond laser textured surfaces of titanium was investigated. • The laser textured surfaces consist of laser-induced periodic surface structures (LIPSS) and nanopillars. • The laser treatment enhances the hydrophilicity and the surface free energy of the material. • The laser treatment reduces significantly the adhesion of S. aureus and biofilm formation. • Femtosecond laser surface texturing of titanium is a simple and promising method for endowing dental and orthopedic implants with antibacterial properties. - Abstract: The aim of the present work was to investigate the possibility of using femtosecond laser surface texturing as a method to reduce the colonization of Grade 2 Titanium alloy surfaces by Staphylococcus aureus and the subsequent formation of biofilm. The laser treatments were carried out with a Yb:KYW chirped-pulse-regenerative amplification laser system with a central wavelength of 1030 nm and a pulse duration of 500 fs. Two types of surface textures, consisting of laser-induced periodic surface structures (LIPSS) and nanopillars, were produced. The topography, chemical composition and phase constitution of these surfaces were investigated by atomic force microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, micro-Raman spectroscopy, and X-ray diffraction. Surface wettability was assessed by the sessile drop method using water and diiodomethane as testing liquids. The response of S. aureus put into contact with the laser treated surfaces in controlled conditions was investigated by epifluorescence microscopy and scanning electron microscopy 48 h after cell seeding. The results achieved show that the laser treatment reduces significantly the bacterial adhesion to the surface as well as biofilm formation as compared to a reference polished surfaces and suggest that femtosecond laser texturing is a simple and promising method

  15. Overall comparison of subpicosecond electron beam diagnostics by the polychromator, the interferometer and the femtosecond streak camera

    CERN Document Server

    Watanabe, T; Yoshimatsu, T; Sasaki, S; Sugiyama, Y; Ishi, K; Shibata, Y; Kondo, Y; Yoshii, K; Ueda, T; Uesaka, M

    2002-01-01

    Measurements of longitudinal bunch length of subpicosecond and picosecond electron beams have been performed by three methods with three radiation sources at the 35 MeV S-band twin liner accelerators at Nuclear Engineering Research Laboratory, University of Tokyo. The methods we adopt are the femtosecond streak camera with a nondispersive reflective optics, the coherent transition radiation (CTR) Michelson interferometer and the 10 ch polychromator that detects the spectrum of CTR and coherent diffraction radiation (CDR). The measurements by the two CTR methods were independently done with the streak camera and their results were consistent with one another. As a result, the reliability of the polychromator for the diagnostics of less than picosecond electron bunch and the usefulness of the diagnostics for the single shot measurement were verified. Furthermore, perfect nondestructive diagnostics for subpicosecond bunches was performed utilizing CDR interferometry. Then the good agreement between CDR interfero...

  16. Irregularity of the posterior corneal surface during applanation using a curved femtosecond laser interface and microkeratome cutting head.

    Science.gov (United States)

    Vetter, Jan M; Holtz, Carsten; Vossmerbaeumer, Urs; Pfeiffer, Norbert

    2012-03-01

    To evaluate the irregularity of the posterior corneal surface and intrastromal dissection during the preparation of donor tissue for Descemet stripping automated endothelial keratoplasty (DSAEK) using a curved interface femtosecond laser and microkeratome. Sixteen human donor corneas unsuitable for transplantation were divided into two groups: a femtosecond (FS) laser group (n=7) using the VisuMax femtosecond laser (Carl Zeiss Meditec) and a microkeratome group (n=9) using the Amadeus II microkeratome (Ziemer Ophthalmic Group). The corneas were fixed on artificial anterior chambers. Horizontal cross-sections were obtained using spectral-domain optical coherence tomography prior to applanation, during applanation, as well as during and after intrastromal dissection at 450-μm corneal depth. The posterior surface and the dissection line were evaluated for irregularity by fitting a second-order polynomial curve using regression analysis and obtaining the root-mean-square error (RMSE). Groups were compared using analysis of variance. The RMSE of the posterior surface prior to applanation was 9.7 ± 3.1 μm in the FS laser group and 10.2 ± 2.3 μm in the microkeratome group. The RMSE increased to 50.7 ± 9.4 μm and 20.9 ± 6.1 μm during applanation and decreased again to 10.6 ± 1.4 μm and 8.1 ± 1.8 μm after applanation in the FS laser and microkeratome groups, respectively. The RMSE of the intrastromal cut was 19.5 ± 5.7 μm in the FS laser group and 7.7 ± 3.0 μm in the microkeratome group (P<.001). Our results show significantly greater irregularity with the curved interface femtosecond laser-assisted cleavage compared to microkeratome-assisted corneal dissection, possibly due to applanation-derived deformation of the posterior cornea. Copyright 2012, SLACK Incorporated.

  17. Femtosecond pulse radiolysis based on photocathode electron accelerator

    International Nuclear Information System (INIS)

    Yoshida, Y.; Yang, Jinfeng; Kondoh, T.; Kozawa, T.; Tagawa, S.

    2006-01-01

    Pulse radiolysis is a powerful tool for studying chemical kinetics and primary processes or reactions of radiation chemistry. In the pulse radiolysis, a short electron beam, which is almost produced by radio-frequency (RF) electron linear accelerator with energy from a few MeV to a few tens MeV, is used as an irradiative source. The electron-induced reactions or phenomena in matter are analyzed by a short-pulse analyzing light (e.g. synchronized lasers) with the time-resolved stroboscopic technique. The time resolution of pulse radiolysis is not only dependent on the electron bunch length, the analyzing light pulse width, the time jitter between the electron bunch and the analyzing light, but also determined by degradation due to the velocity difference between light and the electron in the sample because of the refractive index. In order to improve the time resolution into femtosecond time region, we have develop a new pulse radiolysis based on a concept of 'Equivalent Velocity Spectroscopy (EVS)' to avoid the degradation of the time resolution caused by the velocity difference between the light and the electron beam in sample. In EVS as shown in Fig.1, a femtosecond electron beam produced by a photocathode electron linear accelerator was used, and a synchronized femtosecond laser was used as the analyzing light source. The electron beam and the laser light were injected into sample with an angle (θ), which is determined by the refractive index (n) of the sample. The electron bunch was also rotated with a same angle to make an overlap of the electron bunch with the laser pulse. The degradation of the time resolution caused by the velocity difference between the light and the electron beam can be calculated as g(L)=L[n/c-1/(vcos θ)], where L is the optical path length and v is the velocity of the electron in sample (we can assume v=c for a few tens MeV electron beam).We can thus obtained g(L)=0 by adjusting the incident angle to cos θ=1/n. However, the rotation

  18. Preliminary observation of refractive cataract surgery assisted by femtosecond laser

    Directory of Open Access Journals (Sweden)

    Xiao-Li Wang

    2015-12-01

    Full Text Available AIM:To compare the differences of visual acuity and corneal astigmatism postoperatively between conventional refractive cataract surgery and that assisted by femtosecond laser.METHODS:Sixty patients(60 eyeswith age-related cataract and cornea astigmatism were divided into femtosecond group and conventional group randomly or voluntarily. The flat shaft, steep shaft and diopter of corneal astigmatism in patients in femtosecond group were inputted into the online vector calculators to get the location and width of the incision. Then femtosecond laser was used to make corneal releasing incision, the main and auxiliary incision. Phacoemulsification and aspheric multifocal intraocular lens implantation were undergone. Patients in conventional group received full-thickness relaxing incision by cornea paracentesis knife at the steepest meridian axis during phacoemulsification. Then aspheric multifocal intraocular lenses were implanted. Uncorrected distance visual acuity(UCDVA, uncorrected near visual acuity(UCNVAand cornea astigmatism were observed at 1d,1wk and 1mo postoperative. RESULTS:UCVA of patients in both groups was improved after the surgeries. UCDVA and UCNVA of femtosecond group were higher than those of conventional group, while the cornea astigmatism of femtosecond group was lower than that of conventional group.CONCLUSION:Refractile cataract surgery assisted by femtosecond laser canoffer better visual quality than conventional refractive cataract surgery because of lower cornea astigmatism and better visual acuity.

  19. Studying dense plasmas with coherent XUV pulses

    International Nuclear Information System (INIS)

    Stabile, H.

    2006-12-01

    The investigation of dense plasma dynamic requires the development of diagnostics able to ensure the measurement of electronic density with micro-metric space resolution and sub-nanosecond, or even subpicosecond, time resolution (indeed this must be at least comparable with the characteristic tune scale of plasma evolution). In contrast with low-density plasmas, dense plasmas cannot be studied using optical probes in the visible domain, the density range accessible being limited to the critical density (N c equals 1.1*10 21 λ -2 (μm) ∼ 10 21 cm -3 for infrared). In addition, light is reflected even at smaller densities if the medium exhibits sharp density gradients. Hence probing of dense plasmas, for instance those produced by laser irradiation of solids, requires using shorter wavelength radiation. Thanks to their physical properties, high order harmonics generated in rare gases are particularly adapted to the study of dense plasmas. Indeed, they can naturally be synchronized with the generating laser and their pulse duration is very short, which makes it possible to use them in pump-probe experiments. Moreover, they exhibit good spatial and temporal coherencies. Two types of diagnostics were developed during this thesis. The first one was used to study the instantaneous creation of hot-solid-density plasma generated by focusing a femtosecond high-contrast laser on an ultra-thin foil (100 nm) in the 10 18 W/cm 2 intensity regime. The use of high order harmonics, providing a probe beam of sufficiently short wavelengths to penetrate such a medium, enables the study of its dynamics on the 100 fs time scale. The second one uses the harmonics beam as probe beam (λ equals 32 nm) within an interferometric device. This diagnostic was designed to ensure a micro-metric spatial resolution and a temporal resolution in the femtosecond range. The first results in presence of plasma created by irradiation of an aluminum target underline the potentialities of this new

  20. Femtosecond laser's application in the corneal surgery

    Directory of Open Access Journals (Sweden)

    Shu-Liang Wang

    2015-10-01

    Full Text Available With the rapid development over the past two decades,femtosecond(10-15slasers(FShas become a new application in ophthalmic surgery. As laser power is defined as energy delivered per unit time, decreasing the pulse duration to femtosecond level(100fsnot only increases the power delivered but also decreases the fluence threshold for laser induced optical breakdown. In ablating tissue, FS has an edge over nanosecond lasers as there is minimal collateral damage from shock waves and heat conduction during surgical ablation. Thus, application of FS has been widely spread, from flap creation for laser-assisted in situ keratomileusis(LASIKsurgery, cutting of donor and recipient corneas in keratoplasty, creation of pockets for intracorneal ring implantation. FS applied in keratoplasty is mainly used in making graft and recipient bed, and can exactly cut different tissue of keratopathy. FS can also cut partial tissue of cornea, even if it is under the moderate corneal macula and corneal edema condition.

  1. Femtosecond-laser assisted cell reprogramming

    Science.gov (United States)

    Breunig, Hans Georg; Uchugonova, Aisada; Batista, Ana; König, Karsten

    2017-02-01

    Femtosecond-laser pulses can assist to transfect cells by creating transient holes in the cell membrane, thus making them temporarily permeable for extraneous genetic material. This procedure offers the advantage of being completely "virus free" since no viruses are used for the delivery and integration of gene factors into the host genome and, thereby, avoiding serious side effects which so far prevent clinical application. Unfortunately, focusing of the laser radiation onto individual cell membranes is quite elaborate and time consuming. Regarding these obstacles, we briefly review two optical setups for fast, efficient and high throughput laser-assisted cell transfection based on femtosecond laser pulse excitation. The first setup aims at assisting the transfection of adherent cells. It comprises of a modified laser-scanning microscope with beamshaping optics as well as home-made software to automate the detection, targeting and laser-irradiation process. The second setup aims at laser-assisted transfection of non-adherent cells in suspension which move in a continuous flow through the laser focus region. The setup allows to address a large number of cells, however, with much lower transfection efficiency than the individual-cell targeting approach.

  2. Femtosecond Time-resolved Optical Polarigraphy (FTOP)

    International Nuclear Information System (INIS)

    Aoshima, S.; Fujimoto, M.; Hosoda, M.; Tsuchiya, Y.

    2000-01-01

    A novel time-resolved imaging technique named FTOP (Femtosecond Time-resolved Optical Polarigraphy) for visualizing the ultrafast propagation dynamics of intense light pulses in a medium has been proposed and demonstrated. Femtosecond snapshot images can be created with a high spatial resolution by imaging only the polarization components of the probe pulse; these polarization components change due to the instantaneous birefringence induced by the pump pulse in the medium. Ultrafast temporal changes in the two-dimensional spatial distribution of the optical pulse intensity were clearly visualized in consecutive images by changing the delay between the pump and probe. We observe that several filaments appear and then come together before the vacuum focus due to nonlinear effects in air. We also prove that filamentation dynamics such as the formation position and the propagation behavior are complex and are strongly affected by the pump energy. The results collected clearly show that this method FTOP succeeds for the first time in directly visualizing the ultrafast dynamics of the self-modulated nonlinear propagation of light. (author)

  3. Electromagnetic spatial coherence wavelets

    International Nuclear Information System (INIS)

    Castaneda, R.; Garcia-Sucerquia, J.

    2005-10-01

    The recently introduced concept of spatial coherence wavelets is generalized for describing the propagation of electromagnetic fields in the free space. For this aim, the spatial coherence wavelet tensor is introduced as an elementary amount, in terms of which the formerly known quantities for this domain can be expressed. It allows analyzing the relationship between the spatial coherence properties and the polarization state of the electromagnetic wave. This approach is completely consistent with the recently introduced unified theory of coherence and polarization for random electromagnetic beams, but it provides a further insight about the causal relationship between the polarization states at different planes along the propagation path. (author)

  4. Imaging femtosecond laser-induced electronic excitation in glass

    International Nuclear Information System (INIS)

    Mao Xianglei; Mao, Samuel S.; Russo, Richard E.

    2003-01-01

    While substantial progress has been achieved in understanding laser ablation on the nanosecond and picosecond time scales, it remains a considerable challenge to elucidate the underlying mechanisms during femtosecond laser material interactions. We present experimental observations of electronic excitation inside a wide band gap glass during single femtosecond laser pulse (100 fs, 800 nm) irradiation. Using a femtosecond time-resolved imaging technique, we measured the evolution of a laser-induced electronic plasma inside the glass and calculated the electron number density to be on the order of 10 19 cm -3

  5. Pico-femtosecond image-tube photography in quantum electronics

    International Nuclear Information System (INIS)

    Schelev, M Ya

    2001-01-01

    The possibility of experimental achievement of the time resolution of image-converter tubes (ICTs) corresponding to the theoretical limit of 10 fs is considered as applied to quantum electronics problems. A new generation of ICTs with a temporal resolution of 200 - 500 fs has been developed for recording femtosecond laser radiation. The entirely new devices based on time-analysing ICTs such as femtosecond photoelectronic diffractometers, have been created for studying the dynamics of phase transitions in substances using diffrac-tion of electrons with energies ranging from 20 to 40 keV. (femtosecond technologies)

  6. Femtosecond laser 3D micromachining for microfluidic and optofluidic applications

    CERN Document Server

    Sugioka, Koji

    2013-01-01

    Femtosecond lasers opened up new avenue in materials processing due to its unique features of ultrashort pulse width and extremely high peak intensity. One of the most important features of femtosecond laser processing is that strong absorption can be induced even by materials which are transparent to the femtosecond laser beam due to nonlinear multiphoton absorption. The multiphoton absorption allows us to perform not only surface but also three-dimensionally internal microfabrication of transparent materials such as glass. This capability makes it possible to directly fabricate three-dimensi

  7. Native sulfur/chlorine SAD phasing for serial femtosecond crystallography

    International Nuclear Information System (INIS)

    Nakane, Takanori; Song, Changyong; Suzuki, Mamoru; Nango, Eriko; Kobayashi, Jun; Masuda, Tetsuya; Inoue, Shigeyuki; Mizohata, Eiichi; Nakatsu, Toru; Tanaka, Tomoyuki; Tanaka, Rie; Shimamura, Tatsuro; Tono, Kensuke; Joti, Yasumasa; Kameshima, Takashi; Hatsui, Takaki; Yabashi, Makina; Nureki, Osamu; Iwata, So; Sugahara, Michihiro

    2015-01-01

    Sulfur SAD phasing facilitates the structure determination of diverse native proteins using femtosecond X-rays from free-electron lasers via serial femtosecond crystallography. Serial femtosecond crystallography (SFX) allows structures to be determined with minimal radiation damage. However, phasing native crystals in SFX is not very common. Here, the structure determination of native lysozyme from single-wavelength anomalous diffraction (SAD) by utilizing the anomalous signal of sulfur and chlorine at a wavelength of 1.77 Å is successfully demonstrated. This sulfur SAD method can be applied to a wide range of proteins, which will improve the determination of native crystal structures

  8. Coherent active polarization control without loss

    Science.gov (United States)

    Ye, Yuqian; Hay, Darrick; Shi, Zhimin

    2017-11-01

    We propose a lossless active polarization control mechanism utilizing an anisotropic dielectric medium with two coherent inputs. Using scattering matrix analysis, we derive analytically the required optical properties of the anisotropic medium that can behave as a switchable polarizing beam splitter. We also show that such a designed anisotropic medium can produce linearly polarized light at any azimuthal direction through coherent control of two inputs with a specific polarization state. Furthermore, we present a straightforward design-on-demand procedure of a subwavelength-thick metastructure that can possess the desired optical anisotropy at a flexible working wavelength. Our lossless coherent polarization control technique may lead to fast, broadband and integrated polarization control elements for applications in imaging, spectroscopy, and telecommunication.

  9. Coherent active polarization control without loss

    Directory of Open Access Journals (Sweden)

    Yuqian Ye

    2017-11-01

    Full Text Available We propose a lossless active polarization control mechanism utilizing an anisotropic dielectric medium with two coherent inputs. Using scattering matrix analysis, we derive analytically the required optical properties of the anisotropic medium that can behave as a switchable polarizing beam splitter. We also show that such a designed anisotropic medium can produce linearly polarized light at any azimuthal direction through coherent control of two inputs with a specific polarization state. Furthermore, we present a straightforward design-on-demand procedure of a subwavelength-thick metastructure that can possess the desired optical anisotropy at a flexible working wavelength. Our lossless coherent polarization control technique may lead to fast, broadband and integrated polarization control elements for applications in imaging, spectroscopy, and telecommunication.

  10. The Development, Commercialization, and Impact of Optical Coherence Tomography

    Science.gov (United States)

    Fujimoto, James; Swanson, Eric

    2016-01-01

    This review was written for the special issue of IOVS to describe the history of optical coherence tomography (OCT) and its evolution from a nonscientific, historic perspective. Optical coherence tomography has become a standard of care in ophthalmology, providing real-time information on structure and function – diagnosing disease, evaluating progression, and assessing response to therapy, as well as helping to understand disease pathogenesis and create new therapies. Optical coherence tomography also has applications in multiple clinical specialties, fundamental research, and manufacturing. We review the early history of OCT describing how research and development evolves and the important role of multidisciplinary collaboration and expertise. Optical coherence tomography had its origin in femtosecond optics, but used optical communications technologies and required advanced engineering for early OCT prototypes, clinical feasibility studies, entrepreneurship, and corporate development in order to achieve clinical acceptance and clinical impact. Critical advances were made by early career researchers, clinician scientists, engineering experts, and business leaders, which enabled OCT to have a worldwide impact on health care. We introduce the concept of an “ecosystem” consisting of research, government funding, collaboration and competition, clinical studies, innovation, entrepreneurship and industry, and impact – all of which must work synergistically. The process that we recount is long and challenging, but it is our hope that it might inspire early career professionals in science, engineering, and medicine, and that the clinical and research community will find this review of interest. PMID:27409459

  11. The Development, Commercialization, and Impact of Optical Coherence Tomography.

    Science.gov (United States)

    Fujimoto, James; Swanson, Eric

    2016-07-01

    This review was written for the special issue of IOVS to describe the history of optical coherence tomography (OCT) and its evolution from a nonscientific, historic perspective. Optical coherence tomography has become a standard of care in ophthalmology, providing real-time information on structure and function - diagnosing disease, evaluating progression, and assessing response to therapy, as well as helping to understand disease pathogenesis and create new therapies. Optical coherence tomography also has applications in multiple clinical specialties, fundamental research, and manufacturing. We review the early history of OCT describing how research and development evolves and the important role of multidisciplinary collaboration and expertise. Optical coherence tomography had its origin in femtosecond optics, but used optical communications technologies and required advanced engineering for early OCT prototypes, clinical feasibility studies, entrepreneurship, and corporate development in order to achieve clinical acceptance and clinical impact. Critical advances were made by early career researchers, clinician scientists, engineering experts, and business leaders, which enabled OCT to have a worldwide impact on health care. We introduce the concept of an "ecosystem" consisting of research, government funding, collaboration and competition, clinical studies, innovation, entrepreneurship and industry, and impact - all of which must work synergistically. The process that we recount is long and challenging, but it is our hope that it might inspire early career professionals in science, engineering, and medicine, and that the clinical and research community will find this review of interest.

  12. Femtosecond laser refractive surgery: small-incision lenticule extraction vs. femtosecond laser-assisted LASIK.

    Science.gov (United States)

    Lee, Jimmy K; Chuck, Roy S; Park, Choul Yong

    2015-07-01

    Small-incision lenticule extraction (SMILE) is a novel technique devised to correct refractive errors. SMILE circumvents excimer laser photoablation of cornea, as the stromal lenticule cut by femtosecond laser is removed manually. Smaller incisions and preservation of anterior corneal biomechanical strength have been suggested as some of the advantages of SMILE over femtosecond laser-assisted LASIK (FS-LASIK). In this review, we compared previous published results of SMILE and FS-LASIK. The advantage, efficacy and safety of SMILE are compared with FS-LASIK. SMILE achieved similar efficacy, predictability and safety as FS-LASIK. Greater preservations of corneal biomechanical strength and corneal nerves were observed in SMILE when compared with LASIK or PRK. Additionally, the incidence of postoperative dry eye syndrome was found to be less problematic in SMILE than in FS-LASIK. SMILE is a promising new surgery for refractive error correction. Prospective and retrospective studies of SMILE have shown that results of SMILE are similar to FS-LASIK. With advances in femtosecond laser technology, SMILE may gain greater acceptance in the future.

  13. Text Coherence in Translation

    Science.gov (United States)

    Zheng, Yanping

    2009-01-01

    In the thesis a coherent text is defined as a continuity of senses of the outcome of combining concepts and relations into a network composed of knowledge space centered around main topics. And the author maintains that in order to obtain the coherence of a target language text from a source text during the process of translation, a translator can…

  14. Coherent Multistatic ISAR Imaging

    NARCIS (Netherlands)

    Dorp, Ph. van; Otten, M.P.G.; Verzeilberg, J.M.M.

    2012-01-01

    This paper presents methods for Coherent Multistatic Radar Imaging for Non Cooperative Target Recognition (NCTR) with a network of radar sensors. Coherent Multistatic Radar Imaging is based on an extension of existing monostatic ISAR algorithms to the multistatic environment. The paper describes the

  15. VCSEL Based Coherent PONs

    DEFF Research Database (Denmark)

    Jensen, Jesper Bevensee; Rodes, Roberto; Caballero Jambrina, Antonio

    2014-01-01

    We present a review of research performed in the area of coherent access technologies employing vertical cavity surface emitting lasers (VCSELs). Experimental demonstrations of optical transmission over a passive fiber link with coherent detection using VCSEL local oscillators and directly modula...

  16. Narrow titanium oxide nanowires induced by femtosecond laser pulses on a titanium surface

    Energy Technology Data Exchange (ETDEWEB)

    Li, Hui; Li, Xian-Feng [Laboratory of Nanophotonic Functional Materials and Devices, School of Information and Optoelectronic Science and Engineering, South China Normal University, Guangzhou 510006 (China); Zhang, Cheng-Yun [School of Physics and Electronic Engineering, Guangzhou University, Guangzhou 510006 (China); Tie, Shao-Long [School of Chemistry and Environment, South China Normal University, Guangzhou 510006 (China); Lan, Sheng, E-mail: slan@scnu.edu.cn [Laboratory of Nanophotonic Functional Materials and Devices, School of Information and Optoelectronic Science and Engineering, South China Normal University, Guangzhou 510006 (China)

    2017-02-28

    Highlights: • Titanium oxide nanowires with a feature width as narrow as ∼20 nm were induced on a titanium surface by using femtosecond laser pulses at 400 nm. • An evolution of the surface structure from a high spatial frequency laser-induced periodic structure parallel to the laser polarization to a low spatial frequency one perpendicular to the laser polarization was observed with increasing irradiation pulse number. • The formation of the titanium oxide nanowires was confirmed by the energy dispersive spectroscopy measurements and the evolution of the surface structure was successfully interpreted by using the efficacy factor theory. - Abstract: The evolution of the nanostructure induced on a titanium (Ti) surface with increasing irradiation pulse number by using a 400-nm femtosecond laser was examined by using scanning electron microscopy. High spatial frequency periodic structures of TiO{sub 2} parallel to the laser polarization were initially observed because of the laser-induced oxidation of the Ti surface and the larger efficacy factor of TiO{sub 2} in this direction. Periodically aligned TiO{sub 2} nanowires with featured width as small as 20 nm were obtained. With increasing pulse number, however, low spatial frequency periodic structures of Ti perpendicular to the laser polarization became dominant because Ti possesses a larger efficacy factor in this direction. The competition between the high- and low-spatial frequency periodic structures is in good agreement with the prediction of the efficacy factor theory and it should also be observed in the femtosecond laser ablation of other metals which are easily oxidized in air.

  17. Multi-Parameter Measurement in Unseeded Flows using Femtosecond Lasers

    Data.gov (United States)

    National Aeronautics and Space Administration — Our approach is to use new turn-key femtosecond laser technology along with new high-speed CMOS camera technology to build a multi-parameter measurement system based...

  18. Femtosecond laser induced phenomena in transparent solid materials

    DEFF Research Database (Denmark)

    Tan, D.Z.; Sharafudeen, K.N.; Yue, Yuanzheng

    2016-01-01

    solved, especially concerning the interaction of strong, ultra-short electromagnetic pulses with matter, and also because potential advanced technologies will emerge due to the impressive capability of the intense femtosecond laser to create new material structures and hence functionalities. When......The interaction of intense femtosecond laser pulses with transparent materials is a topic that has caused great interest of scientists over the past two decades. It will continue to be a fascinating field in the coming years. This is because many challenging fundamental problems have not been......–matter interaction, and fabricate various integrated micro-devices. In recent years we have witnessed exciting development in understanding and applying femtosecond laser induced phenomena in transparent materials. The interaction of femtosecond laser pulses with transparent materials relies on non...

  19. Innovative applications of femtosecond laser induced self-organized nanostructure

    International Nuclear Information System (INIS)

    Shimotsuma, Yasuhiko; Miura, Kiyotaka; Sakakura, Masaaki

    2015-01-01

    The nanostructure induced by the direct-writing of femtosecond-laser pulses can open a new opportunity to develop avant-garde devices such as a 5D optical storage, polarization imaging sensor, thermoelectric conversion elements. (author)

  20. All-optical femtosecond switch using two-photon absorption

    International Nuclear Information System (INIS)

    Yavuz, D. D.

    2006-01-01

    Utilizing a two-photon absorption scheme in an alkali-metal vapor cell, we suggest a technique where a strong laser beam switches off another laser beam of different wavelength in femtosecond time scales

  1. Scalable coherent interface

    International Nuclear Information System (INIS)

    Alnaes, K.; Kristiansen, E.H.; Gustavson, D.B.; James, D.V.

    1990-01-01

    The Scalable Coherent Interface (IEEE P1596) is establishing an interface standard for very high performance multiprocessors, supporting a cache-coherent-memory model scalable to systems with up to 64K nodes. This Scalable Coherent Interface (SCI) will supply a peak bandwidth per node of 1 GigaByte/second. The SCI standard should facilitate assembly of processor, memory, I/O and bus bridge cards from multiple vendors into massively parallel systems with throughput far above what is possible today. The SCI standard encompasses two levels of interface, a physical level and a logical level. The physical level specifies electrical, mechanical and thermal characteristics of connectors and cards that meet the standard. The logical level describes the address space, data transfer protocols, cache coherence mechanisms, synchronization primitives and error recovery. In this paper we address logical level issues such as packet formats, packet transmission, transaction handshake, flow control, and cache coherence. 11 refs., 10 figs

  2. Measuring coherence with entanglement concurrence

    Science.gov (United States)

    Qi, Xianfei; Gao, Ting; Yan, Fengli

    2017-07-01

    Quantum coherence is a fundamental manifestation of the quantum superposition principle. Recently, Baumgratz et al (2014 Phys. Rev. Lett. 113 140401) presented a rigorous framework to quantify coherence from the view of theory of physical resource. Here we propose a new valid quantum coherence measure which is a convex roof measure, for a quantum system of arbitrary dimension, essentially using the generalized Gell-Mann matrices. Rigorous proof shows that the proposed coherence measure, coherence concurrence, fulfills all the requirements dictated by the resource theory of quantum coherence measures. Moreover, strong links between the resource frameworks of coherence concurrence and entanglement concurrence is derived, which shows that any degree of coherence with respect to some reference basis can be converted to entanglement via incoherent operations. Our work provides a clear quantitative and operational connection between coherence and entanglement based on two kinds of concurrence. This new coherence measure, coherence concurrence, may also be beneficial to the study of quantum coherence.

  3. Structural changes in femtosecond laser modified regions inside fused silica

    International Nuclear Information System (INIS)

    Juodkazis, Saulius; Kohara, Shinji; Ohishi, Yasuo; Hirao, Norihisa; Vailionis, Arturas; Mizeikis, Vygantas; Saito, Akira; Rode, Andrei

    2010-01-01

    Structural characterization of photomodified microvolumes formed by tightly focused femtosecond laser pulses inside silica glass was carried out using synchrotron x-ray diffraction. The observed distinct separation between the O–O and Si–Si pair correlation peaks can be interpreted as a phase separation induced by microexplosions at the focal volume. The mechanisms of structural transitions induced by femtosecond laser pulses inside dielectrics are discussed

  4. Penetrating and Intrastromal Corneal Arcuate Incisions in Rabbit and Human Cadaver Eyes: Manual Diamond Blade and Femtosecond Laser-Created Incisions.

    Science.gov (United States)

    Gray, Brad; Binder, Perry S; Huang, Ling C; Hill, Jim; Salvador-Silva, Mercedes; Gwon, Arlene

    2016-07-01

    To compare morphologic differences between freehand diamond or femtosecond laser-assisted penetrating and intrastromal arcuate incisions. Freehand diamond blade, corneal arcuate incisions (180° apart, 60° arc lengths) and 150 kHz femtosecond laser (80% scheimpflug pachymetry depth corneal thickness) arcuate incisions were performed in rabbits. Intrastromal arcuate incisions (100 μm above Descemet's membrane, 100 μm below epithelium) were performed in rabbit corneas (energy 1.2 μJ, spot line separation 3 × 3 μm, 90° side cut angle). Eyes were examined by slit lamp and light microscopy up to 47 days post-procedure. Freehand diamond blade penetrating incisions, and femtosecond laser penetrating and intrastromal arcuate incisions (energy 1.8 μJ, spot line separation 2 × 2 μm) were performed in cadaver eyes. Optical coherence tomography was performed immediately after surgery and the corneas were fixed for light scanning and transmission electron microscopy. The rabbit model showed anterior stromal inflammation with epithelial hyperplasia in penetrating blade and laser penetrating wounds. The laser intrastromal and penetrating incisions showed localized constriction of the stromal layers of the cornea near the wound. In cadaver eyes, penetrating wound morphology was similar between blade and laser whereas intrastromal wounds did not affect the cornea above or below incisions. Penetrating femtosecond laser arcuate incisions have more predictable and controlled outcomes shown by less post-operative scarring than incisions performed with a diamond blade. Intrastromal incisions do not affect uncut corneal layers as demonstrated by histopathology. The femtosecond laser has significant advantages in its ability to make intrastromal incisions which are not achievable by traditional freehand or mechanical diamond blades.

  5. Compact laser-diode-based femtosecond sources

    International Nuclear Information System (INIS)

    Brown, C T A; Cataluna, M A; Lagatsky, A A; Rafailov, E U; Agate, M B; Leburn, C G; Sibbett, W

    2004-01-01

    This paper describes the development of compact femtosecond laser systems that are capable of being directly pumped by laser diodes or are based directly on laser diodes. The paper demonstrates the latest results in a highly efficient vibronic based gain medium and a diode-pumped Yb:KYW laser is reported that has a wall plug efficiency >14%. A Cr 4+ :YAG oscillator is described that generates transform-limited pulses of 81 fs duration at a pulse repetition frequency of >4 GHz. The development of Cr 3+ :LiSAF lasers that can be operated using power supplies based on batteries is briefly discussed. We also present a summary of work being carried out on the generation of fs-pulses from laser diodes and discuss the important issues in this area. Finally, we outline results obtained on the generation of pulses as short as 550 fs directly from a two-section quantum dot laser without any external pulse compression

  6. Optical reprogramming with ultrashort femtosecond laser pulses

    Science.gov (United States)

    Uchugonova, Aisada; Breunig, Hans G.; Batista, Ana; König, Karsten

    2015-03-01

    The use of sub-15 femtosecond laser pulses in stem cell research is explored with particular emphasis on the optical reprogramming of somatic cells. The reprogramming of somatic cells into induced pluripotent stem (iPS) cells can be evoked through the ectopic expression of defined transcription factors. Conventional approaches utilize retro/lenti-viruses to deliver genes/transcription factors as well as to facilitate the integration of transcription factors into that of the host genome. However, the use of viruses may result in insertional mutations caused by the random integration of genes and as a result, this may limit the use within clinical applications due to the risk of the formation of cancer. In this study, a new approach is demonstrated in realizing non-viral reprogramming through the use of ultrashort laser pulses, to introduce transcription factors into the cell so as to generate iPS cells.

  7. Thin film femtosecond laser damage competition

    Science.gov (United States)

    Stolz, Christopher J.; Ristau, Detlev; Turowski, Marcus; Blaschke, Holger

    2009-10-01

    In order to determine the current status of thin film laser resistance within the private, academic, and government sectors, a damage competition was started at the 2008 Boulder Damage Symposium. This damage competition allows a direct comparison of the current state of the art of high laser resistance coatings since they are tested using the same damage test setup and the same protocol. In 2009 a high reflector coating was selected at a wavelength of 786 nm at normal incidence at a pulse length of 180 femtoseconds. A double blind test assured sample and submitter anonymity so only a summary of the results are presented here. In addition to the laser resistance results, details of deposition processes, coating materials and layer count, and spectral results will also be shared.

  8. Femtosecond laser enabled keratoplasty for advanced keratoconus

    Directory of Open Access Journals (Sweden)

    Yathish Shivanna

    2013-01-01

    Full Text Available Purpose : To assess the efficacy and advantages of femtosecond laser enabled keratoplasty (FLEK over conventional penetrating keratoplasty (PKP in advanced keratoconus. Materials and Methods: Detailed review of literature of published randomized controlled trials of operative techniques in PKP and FLEK. Results: Fifteen studies were identified, analyzed, and compared with our outcome. FLEK was found to have better outcome in view of better and earlier stabilization uncorrected visual acuity (UCVA, best corrected visual acuity (BCVA, and better refractive outcomes with low astigmatism as compared with conventional PKP. Wound healing also was noticed to be earlier, enabling early suture removal in FLEK. Conclusions: Studies relating to FLEK have shown better results than conventional PKP, however further studies are needed to assess the safety and intraoperative complications of the procedure.

  9. Femtosecond photoionization of atoms under noise

    International Nuclear Information System (INIS)

    Singh, Kamal P.; Rost, Jan M.

    2007-01-01

    We investigate the effect of incoherent perturbations on atomic photoionization due to a femtosecond midinfrared laser pulse by solving the time-dependent stochastic Schroedinger equation. For a weak laser pulse which causes almost no ionization, an addition of a Gaussian white noise to the pulse leads to a significantly enhanced ionization probability. Tuning the noise level, a stochastic resonancelike curve is observed showing the existence of an optimum noise for a given laser pulse. Besides studying the sensitivity of the obtained enhancement curve on the pulse parameters, such as the pulse duration and peak amplitude, we suggest that experimentally realizable broadband chaotic light can also be used instead of the white noise to observe similar features. The underlying enhancement mechanism is analyzed in the frequency domain by computing a frequency-resolved atomic gain profile, as well as in the time domain by controlling the relative delay between the action of the laser pulse and noise

  10. Femtosecond optical characterization and applications in cadmium(manganese) telluride diluted magnetic semiconductors

    Science.gov (United States)

    Wang, Daozhi

    This thesis is devoted to the optical characterization of Cd(Mn)Te single crystals. I present the studies of free-carrier dynamics and generation and detection of coherent acoustic phonons (CAPS) using time-resolved femtosecond pump-probe spectroscopy. The giant Faraday effect and ultrafast responsivity of Cd(Mn)Te to sub-picosecond electromagnetic transients are also demonstrated and discussed in detail. The first, few-picosecond-long electronic process after the initial optical excitation exhibits very distinct characteristic dependence on the excitation condition, and in case of Cd(Mn)Te, it has been attributed to the collective effects of band filling, band renormalization, and two-photon absorption. A closed-form, analytic expression for the differential reflectivity induced by the CAPs is derived based on the propagating-strain-pulse model and it accounts very well for our experimental observations. The accurate values of the Mn concentration and longitudinal sound velocity nu s in Cd(Mn)Te were obtained by fitting the data of the refractive index dependence on the probe wavelength to the Schubert model. In Cd 0.91Mn0.09Te, nus was found to be 3.6x103 m/s. Our comparison studies from the one-color and two-color experiments reveal that the intrinsic phonon lifetime in Cd(Mn)Te was at least on the order of nanoseconds, and the observed exponential damping of the CAP oscillations was due to the finite absorption depth of the probe light. Optically-induced electronic stress has been demonstrated to be the main generation mechanism of CAPs. We also present the giant Faraday effect in the Cd(Mn)Te and the spectra of the Verdet constant, which is mainly due to the exchange interaction between the Mn ions and band electrons. The spectral characteristics of the Verdet constant in Cd(Mn)Te exhibit very unique features compared to that in pure semiconductors. In our time-resolved sampling experiments at the room temperature, the response of the Cd(Mn)Te, particularly

  11. Surface modification of UHMWPE with infrared femtosecond laser

    Energy Technology Data Exchange (ETDEWEB)

    Fernandez-Pradas, J.M., E-mail: jmfernandez@ub.edu [Departament de Fisica Aplicada i Optica, Universitat de Barcelona Marti i Franques 1, E-08028 Barcelona (Spain); Naranjo-Leon, S.; Morenza, J.L.; Serra, P. [Departament de Fisica Aplicada i Optica, Universitat de Barcelona Marti i Franques 1, E-08028 Barcelona (Spain)

    2012-09-15

    Highlights: Black-Right-Pointing-Pointer Ultra High Molecular Weight Polyethylene surface was modified with femtosecond laser pulses at 1027 nm wavelength. Black-Right-Pointing-Pointer Surface roughness is increased. Black-Right-Pointing-Pointer Ablation efficiency is maximum for 6 {mu}J pulses. Black-Right-Pointing-Pointer Irradiated surfaces remain almost chemically unaltered. - Abstract: Ultra-high-molecular-weight polyethylene (UHMWPE) is a polymer with mechanical and corrosion properties, which make it appropriate for using in biomedical devices such as hip and knee prostheses. The surface morphology and chemistry of UHMWPE influence its biocompatibility. A laser with wavelength at 1027 nm delivering 450 fs pulses at a repetition rate of 1 kHz is used to modify the surface of UHMWPE samples with 0.45 {mu}m root mean square surface roughness. Micrometric resolution is achieved with the use of a focusing lens of 0.25 NA and pulse energies of few microjoules. The study focuses in the influence of different pulse energies and pulse overlaps on the laser-induced surface roughness and ablation yield. Confocal microscopy is used to characterize changes in the morphology of the irradiated surfaces, and their chemical structure is analyzed by attenuated total reflectance infrared and Raman spectroscopies. The roughness increases as the pulse energy increases until it reaches a maximum. The ablation yield increases with the pulse energy and pulse overlap. However, the ablation yield per pulse is lower for higher pulse overlap. Pulses of 6 {mu}J have the highest ablation efficiency. Infrared and Raman spectra of samples irradiated with low energy pulses are similar to those of the pristine sample. However, some C=C and C=O bonds can be detected after irradiation with the highest pulse energies.

  12. Study and realisation of a femtosecond dye laser operating at different wavelengths. Ultrashort pulses compression and amplification

    International Nuclear Information System (INIS)

    Georges, Patrick

    1989-01-01

    We present the study and the realization of a passively mode-locked dye laser producing pulses shorter than 100 femto-seconds (10 -13 s). In a ring cavity with an amplifier medium (Rhodamine 60) and a saturable absorber (DODCI), a sequence of four prisms controls the group velocity dispersion and allows the generation of very short pulses. Then we have studied the production of femtosecond pulses at other wavelengths directly from the femtosecond dye laser. For the first rime, 60 fs pulses at 685 nm and pulses shorter than 50 fs between 775 nm and 800 nm have been produced by passive mode locking. These near infrared pulses have been used to study the absorption saturation kinetics in semiconductors multiple quantum wells GaAs/GaAlAs. We have observed a singular behavior of the laser operating at 685 nm and analyzed the produced pulses in terms of optical solitons. To perform time resolved spectroscopy with shortest pulses, we have studied a pulse compressor and a multipass amplifier to increase the pulses energy. Pulses of 20 fs and 10 micro-joules (peak power: 0.5 GW) have been obtained at low repetition rate (10 Hz) and pulses of 16 fs and 0.6 micro-joules pulses have been generated at high repetition rate (11 kHz) using a copper vapor laser. These pulses have been used to study the absorption saturation kinetics of an organic dye (the Malachite Green). (author) [fr

  13. Towards laser spectroscopy of antihydrogen

    NARCIS (Netherlands)

    Walz, J.; Pahl, A.; Eikema, K.S.E.; Hansch, T.W.

    2000-01-01

    The development of the first continuous coherent source at 121.56 nm is described. Radiation at this wavelength of Lyman-alpha can be used for laser-cooling of antihydrogen on the strong 1S-2P transition. It also opens up a possibility for precision spectroscopy that requires just a few antihydrogen

  14. 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

  15. Electron spectroscopy

    International Nuclear Information System (INIS)

    Hegde, M.S.

    1979-01-01

    An introduction to the various techniques in electron spectroscopy is presented. These techniques include: (1) UV Photoelectron spectroscopy, (2) X-ray Photoelectron spectroscopy, (3) Auger electron spectroscopy, (4) Electron energy loss spectroscopy, (5) Penning ionization spectroscopy and (6) Ion neutralization spectroscopy. The radiations used in each technique, the basis of the technique and the special information obtained in structure determination in atoms and molecules by each technique are summarised. (A.K.)

  16. Determination of ablation threshold for composite resins and amalgam irradiated with femtosecond laser pulses

    International Nuclear Information System (INIS)

    Freitas, A Z; Samad, R E; Zezell, D M; Vieira Jr, N D; Freschi, L R; Gouw-Soares, S C

    2010-01-01

    The use of laser for caries removal and cavity preparation is already a reality in the dental clinic. The objective of the present study was to consider the viability of ultrashort laser pulses for restorative material selective removal, by determining the ablation threshold fluence for composite resins and amalgam irradiated with femtosecond laser pulses. Lasers pulses centered at 830 nm with 50 fs of duration and 1 kHz of repetition rate, with energies in the range of 300 to 770 μJ were used to irradiate the samples. The samples were irradiated using two different geometrical methods for ablation threshold fluence determinations and the volume ablation was measured by optical coherence tomography. The shape of the ablated surfaces were analyzed by optical microscopy and scanning electron microscopy. The determined ablation threshold fluence is 0.35 J/cm 2 for the composite resins Z-100 and Z-350, and 0.25 J/cm 2 for the amalgam. These values are half of the value for enamel in this temporal regime. Thermal damages were not observed in the samples. Using the OCT technique (optical coherence tomography) was possible to determine the ablated volume and the total mass removed

  17. Sequencing of Isotope-Labeled Small RNA Using Femtosecond Laser Ablation Time-of-Flight Mass Spectrometry

    Science.gov (United States)

    Kurata-Nishimura, Mizuki; Ando, Yoshinari; Kobayashi, Tohru; Matsuo, Yukari; Suzuki, Harukazu; Hayashizaki, Yoshihide; Kawai, Jun

    2010-04-01

    A novel method for the analysis of sequences of small RNAs using nucleotide triphosphates labeled with stable isotopes has been developed using time-of-flight mass spectroscopy combined with femtosecond laser ablation (fsLA-TOF-MS). Small RNAs synthesized with nucleotides enriched in 13C and 15N were efficiently atomized and ionized by single-shot fsLA and the isotope ratios 13C/12C and 15N/14N were evaluated using the TOF-MS method. By comparing the isotope ratios among four different configurations, the number of nucleotide contents of the control RNA sample were successfully reproduced.

  18. Femtosecond Single-Shot Imaging of Nanoscale Ferromagnetic Order in Co/Pd Multilayers using Resonant X-ray Holography

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Tianhan; Zhu, Diling; Benny Wu,; Graves, Catherine; Schaffert, Stefan; Rander, Torbjorn; Muller, leonard; Vodungbo, Boris; Baumier, Cedric; Bernstein, David P.; Brauer, Bjorn; Cros, Vincent; Jong, Sanne de; Delaunay, Renaud; Fognini, Andreas; Kukreja, Roopali; Lee, Sooheyong; Lopez-Flores, Victor; Mohanty, Jyoti; Pfau, Bastian; Popescu, 5 Horia

    2012-05-15

    We present the first single-shot images of ferromagnetic, nanoscale spin order taken with femtosecond x-ray pulses. X-ray-induced electron and spin dynamics can be outrun with pulses shorter than 80 fs in the investigated fluence regime, and no permanent aftereffects in the samples are observed below a fluence of 25 mJ/cm{sup 2}. Employing resonant spatially-muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm{sup 2}. Our results open new ways to combine ultrafast laser spectroscopy with sequential snapshot imaging on a single sample, generating a movie of excited state dynamics.

  19. Nanosecond and femtosecond mass spectroscopic analysis of a molecular beam produced by the spray-jet technique

    International Nuclear Information System (INIS)

    Yamada, Toshiki; Shinohara, Hidenori; Kamikado, Toshiya; Okuno, Yoshishige; Suzuki, Hitoshi; Mashiko, Shinro; Yokoyama, Shiyoshi

    2008-01-01

    The spray-jet molecular beam apparatus enabled us to produce a molecular beam of non-volatile molecules under high vacuum from a sprayed mist of sample solutions. The apparatus has been used in spectroscopic studies and as a means of molecular beam deposition. We analyzed the molecular beam, consisting of non-volatile, solvent, and carrier-gas molecules, by using femtosecond- and nanosecond- laser mass spectroscopy. The information thus obtained provided insight into the molecular beam produced by the spray-jet technique

  20. Intracoronary optical coherence tomography

    DEFF Research Database (Denmark)

    Tenekecioglu, Erhan; Albuquerque, Felipe N; Sotomi, Yohei

    2017-01-01

    By providing valuable information about the coronary artery wall and lumen, intravascular imaging may aid in optimizing interventional procedure results and thereby could improve clinical outcomes following percutaneous coronary intervention (PCI). Intravascular optical coherence tomography (OCT...

  1. Coherence in Industrial Transformation

    DEFF Research Database (Denmark)

    Jørgensen, Ulrik; Lauridsen, Erik Hagelskjær

    2003-01-01

    The notion of coherence is used to illustrate the general finding, that the impact of environmental management systems and environmental policy is highly dependent of the context and interrelatedness of the systems, procedures and regimes established in society....

  2. Optical Coherence Tomography

    DEFF Research Database (Denmark)

    Fercher, A.F.; Andersen, Peter E.

    2017-01-01

    Optical coherence tomography (OCT) is a technique that is used to peer inside a body noninvasively. Tissue structure defined by tissue absorption and scattering coefficients, and the speed of blood flow, are derived from the characteristics of light remitted by the body. Singly backscattered light...... detected by partial coherence interferometry (PCI) is used to synthesize the tomographic image coded in false colors. A prerequisite of this technique is a low time-coherent but high space-coherent light source, for example, a superluminescent diode or a supercontinuum source. Alternatively, the imaging...... technique can be realized by using ultrafast wavelength scanning light sources. For tissue imaging, the light source wavelengths are restricted to the red and near-infrared (NIR) region from about 600 to 1300 nm, the so-called therapeutic window, where absorption (μa ≈ 0.01 mm−1) is small enough. Transverse...

  3. Development of an X-ray delay unit for correlation spectroscopy and pump-probe experiments

    Energy Technology Data Exchange (ETDEWEB)

    Roseker, Wojciech

    2008-07-15

    Probing condensed matter on time scales ranging from femtoseconds to nanoseconds will be one of the key topics for future X-ray Free Electron Laser (XFEL) sources. The accessible time windows are, however, compromised by the intrinsic time structure of the sources. One way to overcome this limitation is the usage of a time delay unit. A prototype device capable of splitting an X-ray pulse into two adjustable fractions, delaying one of them with the aim to perform X-ray Photon Correlation Spectroscopy and pump-probe type studies was designed and manufactured. The device utilizes eight perfect crystals in vertical 90 scattering geometry. Its performance has been verified with 8.39 keV and 12.4 keV Xrays at various synchrotron sources. The measured throughput of the device with a Si(333) monochromator at 8.39 keV under ambient conditions is 0.6%. The stability was verified at 12.4 keV and operation without realignment and feedback was possible for more than 30 minutes. Time delays up to 2.95 ns have been achieved. The highest resolution achieved in an experiment was 15.4 ps, a value entirely determined by the diagnostics system. The influence of the delay unit optics on the coherence properties of the beam was investigated by means of Fraunhofer diffraction and static speckle analysis. The obtained high fringe visibility and contrast values larger than 23% indicate the feasibility of performing coherence based experiments with the delay line. (orig.)

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

    DEFF Research Database (Denmark)

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

    1996-01-01

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

  5. Coherent imaging at FLASH

    International Nuclear Information System (INIS)

    Chapman, H N; Bajt, S; Duesterer, S; Treusch, R; Barty, A; Benner, W H; Bogan, M J; Frank, M; Hau-Riege, S P; Woods, B W; Boutet, S; Cavalleri, A; Hajdu, J; Iwan, B; Seibert, M M; Timneanu, N; Marchesini, S; Sakdinawat, A; Sokolowski-Tinten, K

    2009-01-01

    We have carried out high-resolution single-pulse coherent diffractive imaging at the FLASH free-electron laser. The intense focused FEL pulse gives a high-resolution low-noise coherent diffraction pattern of an object before that object turns into a plasma and explodes. In particular we are developing imaging of biological specimens beyond conventional radiation damage resolution limits, developing imaging of ultrafast processes, and testing methods to characterize and perform single-particle imaging.

  6. Comparative study of ornamental granite cleaning using femtosecond and nanosecond pulsed lasers

    Energy Technology Data Exchange (ETDEWEB)

    Rivas, T., E-mail: trivas@uvigo.es [Dpto. Ingeniería de los Recursos Naturales y Medioambiente. E.T.S. Ingeniería de Minas, Universidad de Vigo, 36200 Vigo Spain (Spain); Lopez, A.J.; Ramil, A. [Centro de Investigaciones Tecnológicas. Campus de Esteiro. Universidad de A Coruña 15403 Ferrol Spain (Spain); Pozo, S. [Dpto. Ingeniería de los Recursos Naturales y Medioambiente. E.T.S. Ingeniería de Minas, Universidad de Vigo, 36200 Vigo Spain (Spain); Fiorucci, M.P. [Centro de Investigaciones Tecnológicas. Campus de Esteiro. Universidad de A Coruña 15403 Ferrol Spain (Spain); Silanes, M.E. López de [Dpto. Ingeniería de los Recursos Naturales y Medioambiente. E.I. Forestales. Universidad de Vigo, Campus Pontevedra. 36005 Pontevedra Spain (Spain); García, A.; Aldana, J. R. Vazquez de; Romero, C.; Moreno, P. [Grupo de Investigación en Microprocesado de Materiales con Laser. Facultad de Ciencias, Universidad de Salamanca, 37008 Salamanca Spain (Spain)

    2013-08-01

    Granite has been widely used as a structural and ornamental element in public works and buildings. In damp climates it is almost permanently humid and its exterior surfaces are consequently biologically colonized and blackened We describe a comparative analysis of the performance of two different laser sources in removing biological crusts from granite surfaces: nanosecond Nd:YVO{sub 4} laser (355 nm) and femtosecond Ti:Sapphire laser at its fundamental wavelength (790 nm) and second harmonic (395 nm). The granite surface was analyzed using scanning electron microscopy, attenuated total reflection – Fourier transform infrared spectroscopy and profilometry, in order to assess the degree of cleaning and to characterize possible morphological and chemical changes caused by the laser sources.

  7. Two-photon transitions driven by a combination of diode and femtosecond lasers.

    Science.gov (United States)

    Moreno, Marco P; Nogueira, Giovana T; Felinto, Daniel; Vianna, Sandra S

    2012-10-15

    We report on the combined action of a cw diode laser and a train of ultrashort pulses when each of them drives one step of the 5S-5P-5D two-photon transition in rubidium vapor. The fluorescence from the 6P(3/2) state is detected for a fixed repetition rate of the femtosecond laser while the cw-laser frequency is scanned over the rubidium D(2) lines. This scheme allows for a velocity selective spectroscopy in a large spectral range including the 5D(3/2) and 5D(5/2) states. The results are well described in a simplified frequency domain picture, considering the interaction of each velocity group with the cw laser and a single mode of the frequency comb.

  8. Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra

    Directory of Open Access Journals (Sweden)

    Thomas J. A. Wolf

    2017-07-01

    Full Text Available Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine′s neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.

  9. Optical fiber link for transmission of 1-nJ femtosecond laser pulses at 1550 nm

    DEFF Research Database (Denmark)

    Eichhorn, Finn; Olsson, Rasmus Kjelsmark; Buron, Jonas Christian Due

    2010-01-01

    We report on numerical and experimental characterization of the performance of a fiber link optimized for the delivery of sub-100-fs laser pulses at 1550 nm over several meters of fiber. We investigate the power handling capacity of the link, and demonstrate all-fiber delivery of 1-nJ pulses over...... a distance of 5.3 m. The fiber link consists of dispersion-compensating fiber (DCF) and standard single-mode fiber. The optical pulses at different positions in the fiber link are measured using frequency-resolved optical gating (FROG). The results are compared with numerical simulations of the pulse...... propagation based on the generalized nonlinear Schrödinger equation. The high input power capacity of the fiber link allows the splitting and distribution of femtosecond pulses to an array of fibers with applications in multi-channel fiber-coupled terahertz time-domain spectroscopy and imaging systems. We...

  10. Comparative study of ornamental granite cleaning using femtosecond and nanosecond pulsed lasers

    International Nuclear Information System (INIS)

    Rivas, T.; Lopez, A.J.; Ramil, A.; Pozo, S.; Fiorucci, M.P.; Silanes, M.E. López de; García, A.; Aldana, J. R. Vazquez de; Romero, C.; Moreno, P.

    2013-01-01

    Granite has been widely used as a structural and ornamental element in public works and buildings. In damp climates it is almost permanently humid and its exterior surfaces are consequently biologically colonized and blackened We describe a comparative analysis of the performance of two different laser sources in removing biological crusts from granite surfaces: nanosecond Nd:YVO 4 laser (355 nm) and femtosecond Ti:Sapphire laser at its fundamental wavelength (790 nm) and second harmonic (395 nm). The granite surface was analyzed using scanning electron microscopy, attenuated total reflection – Fourier transform infrared spectroscopy and profilometry, in order to assess the degree of cleaning and to characterize possible morphological and chemical changes caused by the laser sources.

  11. Development of a tunable femtosecond stimulated raman apparatus and its application to beta-carotene.

    Science.gov (United States)

    Shim, Sangdeok; Mathies, Richard A

    2008-04-17

    We have developed a tunable femtosecond stimulated Raman spectroscopy (FSRS) apparatus and used it to perform time-resolved resonance Raman experiments with Raman excitation, the resonant S1 state modes are enhanced by a factor of approximately 200 compared with 800 nm FSRS experiments. The improved signal-to-noise ratios facilitate the measurement of definitive time constants for beta-carotene dynamics including the 180 fs appearance of the S1 vibrational features due to direct internal conversion from S2 and their characteristic 9 ps decay to S0. By tuning the FSRS system to 590 nm Raman excitation, we are able to selectively enhance vibrational features of the hot ground state S hot 0 and monitor its approximately 5 ps cooling dynamics. This tunable FSRS system is valuable because it facilitates the direct observation of structural changes of selected resonantly enhanced states and intermediates during photochemical and photobiological reactions.

  12. Femtosecond time-resolved hot carrier energy distributions of photoexcited semiconductor quantum dots

    International Nuclear Information System (INIS)

    Chuang, Chi-Hung; Burda, Clemens; Chen, Xiaobo

    2013-01-01

    Using femtosecond transient absorption spectroscopy, we investigated hot carrier distributions in semiconductor cadmium selenide quantum dots. The relaxation processes represent the behavior of an ensemble of QDs. This concept is applied for analysis with the Fermi-Dirac distribution and relaxation processes among different electron-hole pair states. By extracting the experimental hot carrier distribution and fitting with the Fermi-Dirac function, we resolved the rapid thermalization processes, such as carrier-carrier and carrier-phonon interactions was resolved within one picosecond upon photoexcitation. The analysis, using the Fermi-Dirac distribution modulated by the density of states, provides a general route to understanding the carrier cooling and heat dissipation processes in quantum dot-based systems. (copyright 2012 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  13. Femtosecond stimulated Raman evidence for charge-transfer character in pentacene singlet fission.

    Science.gov (United States)

    Hart, Stephanie M; Silva, W Ruchira; Frontiera, Renee R

    2018-02-07

    Singlet fission is a spin-allowed process in which an excited singlet state evolves into two triplet states. We use femtosecond stimulated Raman spectroscopy, an ultrafast vibrational technique, to follow the molecular structural evolution during singlet fission in order to determine the mechanism of this process. In crystalline pentacene, we observe the formation of an intermediate characterized by pairs of excited state peaks that are red- and blue-shifted relative to the ground state features. We hypothesize that these features arise from the formation of cationic and anionic species due to partial transfer of electron density from one pentacene molecule to a neighboring molecule. These observations provide experimental evidence for the role of states with significant charge-transfer character which facilitate the singlet fission process in pentacene. Our work both provides new insight into the singlet fission mechanism in pentacene and demonstrates the utility of structurally-sensitive time-resolved spectroscopic techniques in monitoring ultrafast processes.

  14. Structural features of silver-doped phosphate glasses in zone of femtosecond laser-induced modification

    Science.gov (United States)

    Vasileva, A. A.; Nazarov, I. A.; Olshin, P. K.; Povolotskiy, A. V.; Sokolov, I. A.; Manshina, A. A.

    2015-10-01

    Femtosecond (fs) laser writing of two-dimensional microstructures (waveguides) is demonstrated in bulk phosphate glasses doped with silver ions. Silver-content phosphate and silver-content niobium-phosphate glasses with high concentration of silver oxide 55 mol% were used as samples for fs laser writing. The chemical network structure of the synthesized samples is analyzed through Raman spectroscopy and was found to be strongly sensitive to Nb incorporation. It was found that the direct laser writing process enables not only reorganization of glass network, but also formation of color centers and silver nanoparticles that are revealed in appearance of luminescence signal and plasmon absorption. The process of NPs' formation is more efficient for Nb-phosphate glass, while color centers are preferably formed in phosphate glass.

  15. Handbook of Coherent-Domain Optical Methods Biomedical Diagnostics, Environmental Monitoring, and Materials Science

    CERN Document Server

    2013-01-01

    This Handbook provides comprehensive coverage of laser and coherent-domain methods as applied to biomedicine, environmental monitoring, and materials science. Worldwide leaders in these fields describe the fundamentals of light interaction with random media and present an overview of basic research. The latest results on coherent and polarization properties of light scattered by random media, including tissues and blood, speckles formation in multiple scattering media, and other non-destructive interactions of coherent light with rough surfaces and tissues, allow the reader to understand the principles and applications of coherent diagnostic techniques. The expanded second edition has been thoroughly updated with particular emphasis on novel coherent-domain techniques and their applications in medicine and environmental science. Volume 1 describes state-of-the-art methods of coherent and polarization optical imaging, tomography and spectroscopy; diffusion wave spectroscopy; elastic, quasi-elastic and inelasti...

  16. Gamma Spectroscopy

    NARCIS (Netherlands)

    Niemantsverdriet, J.W.; Butz, Tilman; Ertl, G.; Knözinger, H.; Schüth, F.

    2008-01-01

    No abstract. The sections in this article are 1 Introduction 2 Mössbauer Spectroscopy 3 Time-Differential Perturbed Angular Correlations (TDPAC) 4 Conclusions and Outlook Keywords: Mössbauer spectroscopy; gamma spectroscopy; perturbed angular correlation; TDPAC

  17. Enhancement of peak intensity in a filament core with spatiotemporally focused femtosecond laser pulses

    Energy Technology Data Exchange (ETDEWEB)

    Zeng Bin; Chu Wei; Li Guihua; Zhang Haisu; Ni Jielei [State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800 (China); Graduate School of Chinese Academy of Sciences, Beijing 100080 (China); Gao Hui; Liu Weiwei [Institute of Modern Optics, Nankai University, Tianjin, 300071 (China); Yao Jinping; Cheng Ya; Xu Zhizhan [State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800 (China); Chin, See Leang [Center for Optics, Photonics and Laser (COPL) and Department of Physics, Engineering Physics and Optics, Universite Laval, Quebec City, QC, G1V 0A6 (Canada)

    2011-12-15

    We demonstrate that the peak intensity in the filament core, which is inherently limited by the intensity clamping effect during femtosecond laser filamentation, can be significantly enhanced using spatiotemporally focused femtosecond laser pulses. In addition, the filament length obtained by spatiotemporally focused femtosecond laser pulses is {approx}25 times shorter than that obtained by a conventional focusing scheme, resulting in improved high spatial resolution.

  18. Interaction of femtosecond X-ray pulses with periodical multilayer structures

    International Nuclear Information System (INIS)

    Ksenzov, Dmitry

    2010-01-01

    The VUV Free Electron Laser FLASH operates in soft X-ray range and produces high-intensive pulse trains with few tens femtoseconds duration. The transversely fully coherent beam will open new experiments in solid state physics which can not be studied with present radiation sources. The study of the time dependent response of the multilayer to the X-ray pulse can provide insights into the process of interaction of highly intense FEL radiation with matter. To test the influence of electron excitation on the optical properties of boron carbide, the refractive index of B 4 C was measured near B K-edge by energy-resolved photon-in-photon-out method probing a Bragg reflection from periodical multilayers. The measured data clearly show that the variation of the fine structure of the Kabsorption edges due to the chemical nature of the absorber element. The knowledge obtained from experiments with continuous radiation was used to design the respective experiments with pulse from the FEL. In my thesis, it is proposed that the geometrical setup, where the incident pulse arrives from the FEL under the angle close to the 1st order ML Bragg peak, provides the most valuable information. Preliminary simulation considering form factors of neutral and ionized boron showed that due to ionization, pronounced changes in the reflectivity curve are expected. The proposed scheme can be the powerful tool to study the various processes within the electronic subsystem of the FEL pulse interaction with matter. This type of investigations gives a deep understanding of the nature of the electronic excitation and the recombination at the femtosecond scale. (orig.)

  19. Electron acceleration by femtosecond laser interaction with micro-structured plasmas

    Science.gov (United States)

    Goers, Andy James

    Laser-driven accelerators are a promising and compact alternative to RF accelerator technology for generating relativistic electron bunches for medical, scientific, and security applications. This dissertation presents three experiments using structured plasmas designed to advance the state of the art in laser-based electron accelerators, with the goal of reducing the energy of the drive laser pulse and enabling higher repetition rate operation with current laser technology. First, electron acceleration by intense femtosecond laser pulses in He-like nitrogen plasma waveguides is demonstrated. Second, significant progress toward a proof of concept realization of quasi-phasematched direct acceleration (QPM-DLA) is presented. Finally, a laser wakefield accelerator at very high plasma density is studied, enabling relativistic electron beam generation with ˜10 mJ pulse energies. Major results from these experiments include: • Acceleration of electrons up to 120 MeV from an ionization injected wakefield accelerator driven in a 1.5 mm long He-like nitrogen plasma waveguide • Guiding of an intense, quasi-radially polarized femtosecond laser pulse in a 1 cm plasma waveguide. This pulse provides a strong drive field for the QPM-DLA concept. • Wakefield acceleration of electrons up to ˜10 MeV with sub-terawatt, ˜10 mJ pulses interacting with a thin (˜200 mum), high density (>1020 cm-3) plasma. • Observation of an intense, coherent, broadband wave breaking radiation flash from a high plasma density laser wakefield accelerator. The flash radiates > 1% of the drive laser pulse energy in a bandwidth consistent with half-cycle (˜1 fs) emission from violent unidirectional acceleration of electron bunches from rest. These results open the way to high repetition rate (>˜kHz) laser-driven generation of relativistic electron beams with existing laser technology.

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

    Science.gov (United States)

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

    2016-11-01

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