Time-resolved structural dynamics of thin metal films heated with femtosecond optical pulses.

PubMed

Chen, Jie; Chen, Wei-Kan; Tang, Jau; Rentzepis, Peter M

2011-11-22

We utilize 100 fs optical pulses to induce ultrafast disorder of 35- to 150-nm thick single Au(111) crystals and observe the subsequent structural evolution using 0.6-ps, 8.04-keV X-ray pulses. Monitoring the picosecond time-dependent modulation of the X-ray diffraction intensity, width, and shift, we have measured directly electron/phonon coupling, phonon/lattice interaction, and a histogram of the lattice disorder evolution, such as lattice breath due to a pressure wave propagating at sonic velocity, lattice melting, and recrystallization, including mosaic formation. Results of theoretical simulations agree and support the experimental data of the lattice/liquid phase transition process. These time-resolved X-ray diffraction data provide a detailed description of all the significant processes induced by ultrafast laser pulses impinging on thin metallic single crystals.

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

PubMed Central

Picón, A.; Lehmann, C. S.; Bostedt, C.; Rudenko, A.; Marinelli, A.; Osipov, T.; Rolles, D.; Berrah, N.; Bomme, C.; Bucher, M.; Doumy, G.; Erk, B.; Ferguson, K. R.; Gorkhover, T.; Ho, P. J.; Kanter, E. P.; Krässig, B.; Krzywinski, J.; Lutman, A. A.; March, A. M.; Moonshiram, D.; Ray, D.; Young, L.; Pratt, S. T.; Southworth, S. H.

2016-01-01

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site. PMID:27212390

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics.

PubMed

Picón, A; Lehmann, C S; Bostedt, C; Rudenko, A; Marinelli, A; Osipov, T; Rolles, D; Berrah, N; Bomme, C; Bucher, M; Doumy, G; Erk, B; Ferguson, K R; Gorkhover, T; Ho, P J; Kanter, E P; Krässig, B; Krzywinski, J; Lutman, A A; March, A M; Moonshiram, D; Ray, D; Young, L; Pratt, S T; Southworth, S H

2016-05-23

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.

Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eckert, Sebastian; Norell, Jesper; Miedema, Piter S.

Here, the femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort timescale.

Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering

DOE PAGES

Eckert, Sebastian; Norell, Jesper; Miedema, Piter S.; ...

2017-04-04

Here, the femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort timescale.

Temporal cross-correlation of x-ray free electron and optical lasers using soft x-ray pulse induced transient reflectivity.

PubMed

Krupin, O; Trigo, M; Schlotter, W F; Beye, M; Sorgenfrei, F; Turner, J J; Reis, D A; Gerken, N; Lee, S; Lee, W S; Hays, G; Acremann, Y; Abbey, B; Coffee, R; Messerschmidt, M; Hau-Riege, S P; Lapertot, G; Lüning, J; Heimann, P; Soufli, R; Fernández-Perea, M; Rowen, M; Holmes, M; Molodtsov, S L; Föhlisch, A; Wurth, W

2012-05-07

The recent development of x-ray free electron lasers providing coherent, femtosecond-long pulses of high brilliance and variable energy opens new areas of scientific research in a variety of disciplines such as physics, chemistry, and biology. Pump-probe experimental techniques which observe the temporal evolution of systems after optical or x-ray pulse excitation are one of the main experimental schemes currently in use for ultrafast studies. The key challenge in these experiments is to reliably achieve temporal and spatial overlap of the x-ray and optical pulses. Here we present measurements of the x-ray pulse induced transient change of optical reflectivity from a variety of materials covering the soft x-ray photon energy range from 500eV to 2000eV and outline the use of this technique to establish and characterize temporal synchronization of the optical-laser and FEL x-ray pulses.

Ultrafast nonthermal heating of water initiated by an X-ray Free-Electron Laser.

PubMed

Beyerlein, Kenneth R; Jönsson, H Olof; Alonso-Mori, Roberto; Aquila, Andrew; Bajt, Saša; Barty, Anton; Bean, Richard; Koglin, Jason E; Messerschmidt, Marc; Ragazzon, Davide; Sokaras, Dimosthenis; Williams, Garth J; Hau-Riege, Stefan; Boutet, Sébastien; Chapman, Henry N; Tîmneanu, Nicuşor; Caleman, Carl

2018-05-29

The bright ultrafast pulses of X-ray Free-Electron Lasers allow investigation into the structure of matter under extreme conditions. We have used single pulses to ionize and probe water as it undergoes a phase transition from liquid to plasma. We report changes in the structure of liquid water on a femtosecond time scale when irradiated by single 6.86 keV X-ray pulses of more than 10 6 J/cm 2 These observations are supported by simulations based on molecular dynamics and plasma dynamics of a water system that is rapidly ionized and driven out of equilibrium. This exotic ionic and disordered state with the density of a liquid is suggested to be structurally different from a neutral thermally disordered state.

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

DOE PAGES

Picón, A.; Lehmann, C. S.; Bostedt, C.; ...

2016-05-23

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Specifically, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. In this paper, we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ionsmore » during the fragmentation of XeF 2 molecules following X-ray absorption at the Xe site.« less

High-average-power 2-kHz laser for generation of ultrashort x-ray pulses.

PubMed

Jiang, Yan; Lee, Taewoo; Li, Wei; Ketwaroo, Gyanprakash; Rose-Petruck, Christoph G

2002-06-01

We describe a Ti:sapphire-based laser-x-ray system specifically designed for generation of ultrafast x-ray pulses in the tenths-of-nanometers spectral range at a 2-kHz repetition rate. To obtain high-contrast laser pulses we divide the laser system into a section for generation of microjoule, high-contrast pulses with pulse cleaning and a subsequent section for chirped-pulse amplification and pulse compression. This laser section operates in conjunction with an x-ray-generation section based on a moving copper wire in a He atmosphere. The high reliability of the entire system permits maintenance-free production of x-ray pulses over tens of hours. Average x-ray fluxes of 10(13) photons/(s 4pi sr 1 keV) at 3 keV and 10(9) photons/(s 4pi sr) above 5 keV of photon energy are produced.

Local terahertz field enhancement for time-resolved x-ray diffraction

DOE PAGES

Kozina, M.; Pancaldi, M.; Bernhard, C.; ...

2017-02-20

We report local field strength enhancement of single-cycle terahertz (THz) pulses in an ultrafast time-resolved x-ray diffraction experiment. We show that patterning the sample with gold microstructures increases the THz field without changing the THz pulse shape or drastically affecting the quality of the x-ray diffraction pattern. Lastly, we find a five-fold increase in THz-induced x-ray diffraction intensity change in the presence of microstructures on a SrTiO 3 thin-film sample.

Local terahertz field enhancement for time-resolved x-ray diffraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kozina, M.; Pancaldi, M.; Bernhard, C.

We report local field strength enhancement of single-cycle terahertz (THz) pulses in an ultrafast time-resolved x-ray diffraction experiment. We show that patterning the sample with gold microstructures increases the THz field without changing the THz pulse shape or drastically affecting the quality of the x-ray diffraction pattern. Lastly, we find a five-fold increase in THz-induced x-ray diffraction intensity change in the presence of microstructures on a SrTiO 3 thin-film sample.

Fresh-slice multicolour X-ray free-electron lasers

DOE PAGES

Lutman, Alberto A.; Maxwell, Timothy J.; MacArthur, James P.; ...

2016-10-24

X-ray free-electron lasers (XFELs) provide femtosecond X-ray pulses with a narrow energy bandwidth and unprecedented brightness. Ultrafast physical and chemical dynamics, initiated with a site-specific X-ray pulse, can be explored using XFELs with a second ultrashort X-ray probe pulse. However, existing double-pulse schemes are complicated, difficult to customize or provide only low-intensity pulses. Here we present the novel fresh-slice technique for multicolour pulse production, wherein different temporal slices of an electron bunch lase to saturation in separate undulator sections. This method combines electron bunch tailoring from a passive wakefield device with trajectory control to provide multicolour pulses. The fresh-slice schememore » outperforms existing techniques at soft X-ray wavelengths. It produces femtosecond pulses with a power of tens of gigawatts and flexible colour separation. The pulse delay can be varied from temporal overlap to almost one picosecond. As a result, we also demonstrate the first three-colour XFEL and variably polarized two-colour pulses.« less

Ultrafast X-Ray Coherent Control

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reis, David

2009-05-01

This main purpose of this grant was to develop the nascent eld of ultrafast x-ray science using accelerator-based sources, and originally developed from an idea that a laser could modulate the di racting properties of a x-ray di racting crystal on a fast enough time scale to switch out in time a shorter slice from the already short x-ray pulses from a synchrotron. The research was carried out primarily at the Advanced Photon Source (APS) sector 7 at Argonne National Laboratory and the Sub-Picosecond Pulse Source (SPPS) at SLAC; in anticipation of the Linac Coherent Light Source (LCLS) x-ray freemore » electron laser that became operational in 2009 at SLAC (all National User Facilities operated by BES). The research centered on the generation, control and measurement of atomic-scale dynamics in atomic, molecular optical and condensed matter systems with temporal and spatial resolution . It helped develop the ultrafast physics, techniques and scienti c case for using the unprecedented characteristics of the LCLS. The project has been very successful with results have been disseminated widely and in top journals, have been well cited in the eld, and have laid the foundation for many experiments being performed on the LCLS, the world's rst hard x-ray free electron laser.« less

Ultrashort x-ray backlighters and applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Umstadter, D., University of Michigan

Previously, using ultrashort laser pulses focused onto solid targets, we have experimentally studied a controllable ultrafast broadband radiation source in the extreme ultraviolet for time-resolved dynamical studies in ultrafast science [J. Workman, A. Maksimchuk, X. Llu, U. Ellenberger, J. S. Coe, C.-Y. Chien, and D. Umstadter, ``Control of Bright Picosecond X-Ray Emission from Intense Sub- Picosecond Laser-Plasma Interactions,`` Phys. Rev. Lett. 75, 2324 (1995)]. Once armed with a bright ultrafast broadband continuum x-ray source and appropriate detectors, we used the source as a backlighter to study a remotely produced plasma. The application of the source to a problem relevant tomore » high-density matter completes the triad: creating and controlling, efficiently detecting, and applying the source. This work represented the first use of an ultrafast laser- produced x-ray source as a time-resolving probe in an application relevant to atomic, plasma and high-energy-density matter physics. Using the x-ray source as a backlighter, we adopted a pump-probe geometry to investigate the dynamic changes in electronic structure of a thin metallic film as it is perturbed by an ultrashort laser pulse. Because the laser deposits its energy in a skin depth of about 100 {Angstrom} before expansion occurs, up to gigabar pressure shock waves lasting picosecond in duration have been predicted to form in these novel plasmas. This raises the possibility of studying high- energy-density matter relevant to inertial confinement fusion (ICF) and astrophysics in small-scale laboratory experiments. In the past, time-resolved measurements of K-edge shifts in plasmas driven by nanosecond pulses have been used to infer conditions in highly compressed materials. In this study, we used 100-fs laser pulses to impulsively drive shocks into a sample (an untamped 1000 {Angstrom} aluminum film on 2000 {Angstrom} of parylene-n), measuring L-edge shifts.« less

Following the dynamics of matter with femtosecond precision using the X-ray streaking method

DOE PAGES

David, C.; Karvinen, P.; Sikorski, M.; ...

2015-01-06

X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide amore » time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes.« less

Lattice-level measurement of material strength with LCLS during ultrafast dynamic compression

NASA Astrophysics Data System (ADS)

Milathianaki, Despina; Boutet, Sebastien; Ratner, Daniel; White, William; Williams, Garth; Gleason, Arianna; Swift, Damian; Higginbotham, Andrew; Wark, Justin

2013-10-01

An in-depth understanding of the stress-strain behavior of materials during ultrafast dynamic compression requires experiments that offer in-situ observation of the lattice at the pertinent temporal and spatial scales. To date, the lattice response under extreme strain-rate conditions (>108 s-1) has been inferred predominantly from continuum-level measurements and multi-million atom molecular dynamics simulations. Several time-resolved x-ray diffraction experiments have captured important information on plasticity kinetics, while limited to nanosecond timescales due to the lack of high brilliance ultrafast x-ray sources. Here we present experiments at LCLS combining ultrafast laser-shocks and serial femtosecond x-ray diffraction. The high spectral brightness (~1012 photons per pulse, ΔE/E = 0.2%) and subpicosecond temporal resolution (<100 fs pulsewidth) of the LCLS x-ray free electron laser allow investigations that link simulations and experiments at the fundamental temporal and spatial scales for the first time. We present movies of the lattice undergoing rapid shock-compression, composed by a series of single femtosecond x-ray snapshots, demonstrating the transient behavior while successfully decoupling the elastic and plastic response in polycrystalline Cu.

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

NASA Astrophysics Data System (ADS)

Fahy, Stephen; Murray, Eamonn

2015-03-01

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

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources

PubMed Central

Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

2017-01-01

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today’s ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources. PMID:28067288

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources

NASA Astrophysics Data System (ADS)

Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

2017-01-01

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today’s ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources.

10-fs-level synchronization of photocathode laser with RF-oscillator for ultrafast electron and X-ray sources.

PubMed

Yang, Heewon; Han, Byungheon; Shin, Junho; Hou, Dong; Chung, Hayun; Baek, In Hyung; Jeong, Young Uk; Kim, Jungwon

2017-01-09

Ultrafast electron-based coherent radiation sources, such as free-electron lasers (FELs), ultrafast electron diffraction (UED) and Thomson-scattering sources, are becoming more important sources in today's ultrafast science. Photocathode laser is an indispensable common subsystem in these sources that generates ultrafast electron pulses. To fully exploit the potentials of these sources, especially for pump-probe experiments, it is important to achieve high-precision synchronization between the photocathode laser and radio-frequency (RF) sources that manipulate electron pulses. So far, most of precision laser-RF synchronization has been achieved by using specially designed low-noise Er-fibre lasers at telecommunication wavelength. Here we show a modular method that achieves long-term (>1 day) stable 10-fs-level synchronization between a commercial 79.33-MHz Ti:sapphire laser oscillator and an S-band (2.856-GHz) RF oscillator. This is an important first step toward a photocathode laser-based femtosecond RF timing and synchronization system that is suitable for various small- to mid-scale ultrafast X-ray and electron sources.

Towards shot-noise limited diffraction experiments with table-top femtosecond hard x-ray sources.

PubMed

Holtz, Marcel; Hauf, Christoph; Weisshaupt, Jannick; Salvador, Antonio-Andres Hernandez; Woerner, Michael; Elsaesser, Thomas

2017-09-01

Table-top laser-driven hard x-ray sources with kilohertz repetition rates are an attractive alternative to large-scale accelerator-based systems and have found widespread applications in x-ray studies of ultrafast structural dynamics. Hard x-ray pulses of 100 fs duration have been generated at the Cu K α wavelength with a photon flux of up to 10 9 photons per pulse into the full solid angle, perfectly synchronized to the sub-100-fs optical pulses from the driving laser system. Based on spontaneous x-ray emission, such sources display a particular noise behavior which impacts the sensitivity of x-ray diffraction experiments. We present a detailed analysis of the photon statistics and temporal fluctuations of the x-ray flux, together with experimental strategies to optimize the sensitivity of optical pump/x-ray probe experiments. We demonstrate measurements close to the shot-noise limit of the x-ray source.

Towards shot-noise limited diffraction experiments with table-top femtosecond hard x-ray sources

PubMed Central

Holtz, Marcel; Hauf, Christoph; Weisshaupt, Jannick; Salvador, Antonio-Andres Hernandez; Woerner, Michael; Elsaesser, Thomas

2017-01-01

Table-top laser-driven hard x-ray sources with kilohertz repetition rates are an attractive alternative to large-scale accelerator-based systems and have found widespread applications in x-ray studies of ultrafast structural dynamics. Hard x-ray pulses of 100 fs duration have been generated at the Cu Kα wavelength with a photon flux of up to 109 photons per pulse into the full solid angle, perfectly synchronized to the sub-100-fs optical pulses from the driving laser system. Based on spontaneous x-ray emission, such sources display a particular noise behavior which impacts the sensitivity of x-ray diffraction experiments. We present a detailed analysis of the photon statistics and temporal fluctuations of the x-ray flux, together with experimental strategies to optimize the sensitivity of optical pump/x-ray probe experiments. We demonstrate measurements close to the shot-noise limit of the x-ray source. PMID:28795079

Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction

NASA Astrophysics Data System (ADS)

Minitti, M. P.; Budarz, J. M.; Kirrander, A.; Robinson, J. S.; Ratner, D.; Lane, T. J.; Zhu, D.; Glownia, J. M.; Kozina, M.; Lemke, H. T.; Sikorski, M.; Feng, Y.; Nelson, S.; Saita, K.; Stankus, B.; Northey, T.; Hastings, J. B.; Weber, P. M.

2015-06-01

Structural rearrangements within single molecules occur on ultrafast time scales. Many aspects of molecular dynamics, such as the energy flow through excited states, have been studied using spectroscopic techniques, yet the goal to watch molecules evolve their geometrical structure in real time remains challenging. By mapping nuclear motions using femtosecond x-ray pulses, we have created real-space representations of the evolving dynamics during a well-known chemical reaction and show a series of time-sorted structural snapshots produced by ultrafast time-resolved hard x-ray scattering. A computational analysis optimally matches the series of scattering patterns produced by the x rays to a multitude of potential reaction paths. In so doing, we have made a critical step toward the goal of viewing chemical reactions on femtosecond time scales, opening a new direction in studies of ultrafast chemical reactions in the gas phase.

Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction.

PubMed

Minitti, M P; Budarz, J M; Kirrander, A; Robinson, J S; Ratner, D; Lane, T J; Zhu, D; Glownia, J M; Kozina, M; Lemke, H T; Sikorski, M; Feng, Y; Nelson, S; Saita, K; Stankus, B; Northey, T; Hastings, J B; Weber, P M

2015-06-26

Structural rearrangements within single molecules occur on ultrafast time scales. Many aspects of molecular dynamics, such as the energy flow through excited states, have been studied using spectroscopic techniques, yet the goal to watch molecules evolve their geometrical structure in real time remains challenging. By mapping nuclear motions using femtosecond x-ray pulses, we have created real-space representations of the evolving dynamics during a well-known chemical reaction and show a series of time-sorted structural snapshots produced by ultrafast time-resolved hard x-ray scattering. A computational analysis optimally matches the series of scattering patterns produced by the x rays to a multitude of potential reaction paths. In so doing, we have made a critical step toward the goal of viewing chemical reactions on femtosecond time scales, opening a new direction in studies of ultrafast chemical reactions in the gas phase.

Femtosecond Optical and X-Ray Measurement of the Semiconductor-to-Metal Transition in VO2

NASA Astrophysics Data System (ADS)

Cavalleri, Andrea; Toth, Csaba; Squier, Jeff; Siders, Craig; Raksi, Ferenc; Forget, Patrick; Kieffer, Jean-Claude

2001-03-01

While the use of ultrashort visible pulses allows access to ultrafast changes in the optical properties during phase transitions, measurement of the correlation between atomic movement and electronic rearrangement has proven more elusive. Here, we report on the conjunct measurement of ultrafast electronic and structural dynamics during a semiconductor-to-metal phase transition in VO2. Rearrangement of the unit cell from monoclinic to rutile (measured by ultrafast x-ray diffraction) is accompanied by a sharp increase in the electrical conductivity and perturbation of the optical properties (measured with ultrafast visible spectroscopy). Ultrafast x-ray diffraction experiments were performed using femtosecond bursts of Cu-Ka from a laser generated plasma source. A clear rise of the diffraction signal originating from the impulsively generated metallic phase was observable on the sub-picosecond timescale. Optical experiments were performed using time-resolved microscopy, providing temporally and spatially resolved measurements of the optical reflectivity at 800 nm. The data indicate that the reflectivity of the low-temperature semiconducting solid is driven to that of the equilibrium, high-temperature metallic phase within 400 fs after irradiation with a 50-fs laser pulse at fluences in excess of 10 mJ/cm2. In conclusion, the data presented in this contribution suggest that the semiconductor-to-metal transition in VO2 occurs within 500 fs after laser-irradiation. A nonthermal physical mechanism governs the re-arrangement.

Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy

DOE PAGES

Mara, Michael W.; Hadt, Ryan G.; Reinhard, Marco Eli; ...

2017-06-23

The multifunctional protein cytochrome c (cyt c) plays key roles in electron transport and apoptosis, switching function by modulating bonding between a heme iron and the sulfur in a methionine residue. This Fe–S(Met) bond is too weak to persist in the absence of protein constraints. We ruptured the bond in ferrous cyt c using an optical laser pulse and monitored the bond reformation within the protein active site using ultrafast x-ray pulses from an x-ray free-electron laser, determining that the Fe–S(Met) bond enthalpy is ~4 kcal/mol stronger than in the absence of protein constraints. As a result, the 4 kcal/molmore » is comparable with calculations of stabilization effects in other systems, demonstrating how biological systems use an entatic state for modest yet accessible energetics to modulate chemical function.« less

Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mara, Michael W.; Hadt, Ryan G.; Reinhard, Marco Eli

The multifunctional protein cytochrome c (cyt c) plays key roles in electron transport and apoptosis, switching function by modulating bonding between a heme iron and the sulfur in a methionine residue. This Fe–S(Met) bond is too weak to persist in the absence of protein constraints. We ruptured the bond in ferrous cyt c using an optical laser pulse and monitored the bond reformation within the protein active site using ultrafast x-ray pulses from an x-ray free-electron laser, determining that the Fe–S(Met) bond enthalpy is ~4 kcal/mol stronger than in the absence of protein constraints. As a result, the 4 kcal/molmore » is comparable with calculations of stabilization effects in other systems, demonstrating how biological systems use an entatic state for modest yet accessible energetics to modulate chemical function.« less

Gas gun shock experiments with single-pulse x-ray phase contrast imaging and diffraction at the Advanced Photon Source

NASA Astrophysics Data System (ADS)

Luo, S. N.; Jensen, B. J.; Hooks, D. E.; Fezzaa, K.; Ramos, K. J.; Yeager, J. D.; Kwiatkowski, K.; Shimada, T.

2012-07-01

The highly transient nature of shock loading and pronounced microstructure effects on dynamic materials response call for in situ, temporally and spatially resolved, x-ray-based diagnostics. Third-generation synchrotron x-ray sources are advantageous for x-ray phase contrast imaging (PCI) and diffraction under dynamic loading, due to their high photon fluxes, high coherency, and high pulse repetition rates. The feasibility of bulk-scale gas gun shock experiments with dynamic x-ray PCI and diffraction measurements was investigated at the beamline 32ID-B of the Advanced Photon Source. The x-ray beam characteristics, experimental setup, x-ray diagnostics, and static and dynamic test results are described. We demonstrate ultrafast, multiframe, single-pulse PCI measurements with unprecedented temporal (<100 ps) and spatial (˜2 μm) resolutions for bulk-scale shock experiments, as well as single-pulse dynamic Laue diffraction. The results not only substantiate the potential of synchrotron-based experiments for addressing a variety of shock physics problems, but also allow us to identify the technical challenges related to image detection, x-ray source, and dynamic loading.

Laser-driven powerful kHz hard x-ray source

NASA Astrophysics Data System (ADS)

Li, Minghua; Huang, Kai; Chen, Liming; Yan, Wenchao; Tao, Mengze; Zhao, Jiarui; Ma, Yong; Li, Yifei; Zhang, Jie

2017-08-01

A powerful hard x-ray source based on laser plasma interaction is developed. By introducing the kHz, 800 nm pulses onto a rotating molybdenum (Mo) disk target, intense Mo Kα x-rays are emitted with suppressed bremsstrahlung background. Results obtained with different laser intensities suggest that the dominant absorption mechanism responsible for the high conversion efficiency is vacuum heating (VH). The high degree of spatial coherence is verified. With the high average flux and a source size comparable to the laser focus spot, absorption contrast imaging and phase contrast imaging are carried out to test the imaging capability of the source. Not only useful for imaging application, this compact x-ray source is also holding great potential for ultrafast x-ray diffraction (XRD) due to the intrinsic merits such as femtosecond pulse duration and natural synchronization with the driving laser pulses.

Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO 3

DOE PAGES

Kozina, M.; van Driel, T.; Chollet, M.; ...

2017-05-03

We use ultrafast x-ray pulses to characterize the lattice response of SrTiO 3 when driven by strong terahertz (THz) fields. We observe transient changes in the diffraction intensity with a delayed onset with respect to the driving field. Fourier analysis reveals two frequency components corresponding to the two lowest energy zone-center optical modes in SrTiO 3. Lastly, the lower frequency mode exhibits clear softening as the temperature is decreased while the higher frequency mode shows slight temperature dependence.

Using Lasers and X-rays to Reveal the Motion of Atoms and Electrons (LBNL Summer Lecture Series)

ScienceCinema

Schoenlein, Robert [Deputy Director, Advanced Light Source

2017-12-09

Summer Lecture Series 2009: The ultrafast motion of atoms and electrons lies at the heart of chemical reactions, advanced materials with exotic properties, and biological processes such as the first event in vision. Bob Schoenlein, Deputy Director for Science at the Advanced Light Source, will discuss how such processes are revealed by using laser pulses spanning a millionth of a billionth of a second, and how a new generation of light sources will bring the penetrating power of x-rays to the world of ultrafast science.

Using Lasers and X-rays to Reveal the Motion of Atoms and Electrons (LBNL Summer Lecture Series)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schoenlein, Robert

2009-07-07

Summer Lecture Series 2009: The ultrafast motion of atoms and electrons lies at the heart of chemical reactions, advanced materials with exotic properties, and biological processes such as the first event in vision. Bob Schoenlein, Deputy Director for Science at the Advanced Light Source, will discuss how such processes are revealed by using laser pulses spanning a millionth of a billionth of a second, and how a new generation of light sources will bring the penetrating power of x-rays to the world of ultrafast science.

Ultrafast X-ray diffraction probe of terahertz field-driven soft mode dynamics in SrTiO 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kozina, M.; van Driel, T.; Chollet, M.

We use ultrafast x-ray pulses to characterize the lattice response of SrTiO 3 when driven by strong terahertz (THz) fields. We observe transient changes in the diffraction intensity with a delayed onset with respect to the driving field. Fourier analysis reveals two frequency components corresponding to the two lowest energy zone-center optical modes in SrTiO 3. Lastly, the lower frequency mode exhibits clear softening as the temperature is decreased while the higher frequency mode shows slight temperature dependence.

Using Lasers and X-rays to Reveal the Motion of Atoms and Electrons (LBNL Summer Lecture Series)

ScienceCinema

Schoenlein, Robert [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS), Materials Sciences Division and Chemical Sciences Division

2018-05-07

Summer Lecture Series 2009: The ultrafast motion of atoms and electrons lies at the heart of chemical reactions, advanced materials with exotic properties, and biological processes such as the first event in vision. Bob Schoenlein, Deputy Director for Science at the Advanced Light Source, will discuss how such processes are revealed by using laser pulses spanning a millionth of a billionth of a second, and how a new generation of light sources will bring the penetrating power of x-rays to the world of ultrafast science.

Overview of options for generating high-brightness attosecond x-ray pulses at free-electron lasers and applications at the European XFEL

NASA Astrophysics Data System (ADS)

Serkez, S.; Geloni, G.; Tomin, S.; Feng, G.; Gryzlova, E. V.; Grum-Grzhimailo, A. N.; Meyer, M.

2018-02-01

The generation of attosecond, highbrightness x-ray pulses is a matter of great interest given their applications in the study of ultra-fast processes. In recent years, the production of x-ray pulses of high brightness, both in the soft and in the hard x-ray range, has been enabled by x-ray free-electron lasers (XFELs). In contrast to conventional quantum lasers, XFELs are based on the use of an ultra-relativistic electron beam as gain medium. They often work in the self-amplified spontaneous emission (SASE) regime, which provides pulses of duration down to a few femtoseconds, composed of several longitudinal modes. In order to further decrease the duration of these pulses, special methods need to be implemented. In this paper we review available methods, with particular focus on the x-ray laser-enhanced attosecond pulse generation, which is one of the most promising techniques. We illustrate the method using the SASE3 soft x-ray undulator of the European XFEL facility as a case study, emphasizing the importance of high-repetition rate attosecond x-ray pulses. The expected attosecond-level radiation output is used for simulations of sequential ionization processes in atoms in the case of ionization in the soft x-ray regime, demonstrating the importance of this opportunity for the user community.

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

NASA Astrophysics Data System (ADS)

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

2013-06-01

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

X-ray phase contrast imaging of biological specimens with femtosecond pulses of betatron radiation from a compact laser plasma wakefield accelerator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kneip, S.; Center for Ultrafast Optical Science, University of Michigan, Ann Arbor 48109; McGuffey, C.

2011-08-29

We show that x-rays from a recently demonstrated table top source of bright, ultrafast, coherent synchrotron radiation [Kneip et al., Nat. Phys. 6, 980 (2010)] can be applied to phase contrast imaging of biological specimens. Our scheme is based on focusing a high power short pulse laser in a tenuous gas jet, setting up a plasma wakefield accelerator that accelerates and wiggles electrons analogously to a conventional synchrotron, but on the centimeter rather than tens of meter scale. We use the scheme to record absorption and phase contrast images of a tetra fish, damselfly and yellow jacket, in particular highlightingmore » the contrast enhancement achievable with the simple propagation technique of phase contrast imaging. Coherence and ultrafast pulse duration will allow for the study of various aspects of biomechanics.« less

Investigating radiation induced damage processes with femtosecond x-ray pulses (Conference Presentation)

NASA Astrophysics Data System (ADS)

Song, Changyong

2017-05-01

Interest in high-resolution structure investigation has been zealous, especially with the advent of X-ray free electron lasers (XFELs). The intense and ultra-short X-ray laser pulses ( 10 GW) pave new routes to explore structures and dynamics of single macromolecules, functional nanomaterials and complex electronic materials. In the last several years, we have developed XFEL single-shot diffraction imaging by probing ultrafast phase changes directly. Pump-probe single-shot imaging was realized by synchronizing femtosecond (<10 fs in FWHM) X-ray laser (probe) with femtosecond (50 fs) IR laser (pump) at better than 1 ps resolution. Nanoparticles under intense fs-laser pulses were investigated with fs XFEL pulses to provide insight into the irreversible particle damage processes with nanoscale resolution. Research effort, introduced, aims to extend the current spatio-temporal resolution beyond the present limit. We expect this single-shot dynamic imaging to open new science opportunity with XFELs.

Full characterization of an attosecond pulse generated using an infrared driver

PubMed Central

Zhang, Chunmei; Brown, Graham G.; Kim, Kyung Taec; Villeneuve, D. M.; Corkum, P. B.

2016-01-01

The physics of attosecond pulse generation requires using infrared driving wavelength to reach the soft X-rays. However, with longer driving wavelength, the harmonic conversion efficiency drops significantly. It makes the conventional attosecond pulse measurement using streaking very difficult due to the low photoionization cross section in the soft X-rays region. In-situ measurement was developed for precisely this purpose. We use in-situ measurement to characterize, in both space and time, an attosecond pulse produced by ultrafast wavefront rotation of a 1.8 μm fundamental beam. We confirm what models suggest – that each beamlet is an isolated attosecond pulse in the time domain. We get almost constant flat wavefront curvature through the whole photon energy range. The measurement method is scalable to the soft X-ray spectral region. PMID:27230961

Generation of High Brightness X-rays with the PLEIADES Thomson X-ray Source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, W J; Anderson, S G; Barty, C P J

2003-05-28

The use of short laser pulses to generate high peak intensity, ultra-short x-ray pulses enables exciting new experimental capabilities, such as femtosecond pump-probe experiments used to temporally resolve material structural dynamics on atomic time scales. PLEIADES (Picosecond Laser Electron InterAction for Dynamic Evaluation of Structures) is a next generation Thomson scattering x-ray source being developed at Lawrence Livermore National Laboratory (LLNL). Ultra-fast picosecond x-rays (10-200 keV) are generated by colliding an energetic electron beam (20-100 MeV) with a high intensity, sub-ps, 800 nm laser pulse. The peak brightness of the source is expected to exceed 10{sup 20} photons/s/0.1% bandwidth/mm2/mrad2. Simulationsmore » of the electron beam production, transport, and final focus are presented. Electron beam measurements, including emittance and final focus spot size are also presented and compared to simulation results. Measurements of x-ray production are also reported and compared to theoretical calculations.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cammarata, Marco; Eybert, Laurent; Ewald, Friederike

A chopper system for time resolved pump-probe experiments with x-ray beams from a synchrotron is described. The system has three parts: a water-cooled heatload chopper, a high-speed chopper, and a millisecond shutter. The chopper system, which is installed in beamline ID09B at the European Synchrotron Radiation Facility, provides short x-ray pulses for pump-probe experiments with ultrafast lasers. The chopper system can produce x-ray pulses as short as 200 ns in a continuous beam and repeat at frequencies from 0 to 3 kHz. For bunch filling patterns of the synchrotron with pulse separations greater than 100 ns, the high-speed chopper canmore » isolate single 100 ps x-ray pulses that are used for the highest time resolution. A new rotor in the high-speed chopper is presented with a single pulse (100 ps) and long pulse (10 {mu}s) option. In white beam experiments, the heatload of the (noncooled) high-speed chopper is lowered by a heatload chopper, which absorbs 95% of the incoming power without affecting the pulses selected by the high speed chopper.« less

The Linac Coherent Light Source: Recent Developments and Future Plans

DOE PAGES

Schoenlein, R. W.; Boutet, S.; Minitti, M. P.; ...

2017-08-18

The development of X-ray free-electron lasers (XFELs) has launched a new era in X-ray science by providing ultrafast coherent X-ray pulses with a peak brightness that is approximately one billion times higher than previous X-ray sources. The Linac Coherent Light Source (LCLS) facility at the SLAC National Accelerator Laboratory, the world’s first hard X-ray FEL, has already demonstrated a tremendous scientific impact across broad areas of science. Here in this paper, a few of the more recent representative highlights from LCLS are presented in the areas of atomic, molecular, and optical science; chemistry; condensed matter physics; matter in extreme conditions;more » and biology. This paper also outlines the near term upgrade (LCLS-II) and motivating science opportunities for ultrafast X-rays in the 0.25–5 keV range at repetition rates up to 1 MHz. Future plans to extend the X-ray energy reach to beyond 13 keV (<1 Å) at high repetition rate (LCLS-II-HE) are envisioned, motivated by compelling new science of structural dynamics at the atomic scale.« less

Time delay measurement in the frequency domain

DOE PAGES

Durbin, Stephen M.; Liu, Shih -Chieh; Dufresne, Eric M.; ...

2015-08-06

Pump–probe studies at synchrotrons using X-ray and laser pulses require accurate determination of the time delay between pulses. This becomes especially important when observing ultrafast responses with lifetimes approaching or even less than the X-ray pulse duration (~100 ps). The standard approach of inspecting the time response of a detector sensitive to both types of pulses can have limitations due to dissimilar pulse profiles and other experimental factors. Here, a simple alternative is presented, where the frequency response of the detector is monitored versus time delay. Measurements readily demonstrate a time resolution of ~1 ps. Improved precision is possible bymore » simply extending the data acquisition time.« less

Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

PubMed Central

Canton, Sophie E.; Kjær, Kasper S.; Vankó, György; van Driel, Tim B.; Adachi, Shin-ichi; Bordage, Amélie; Bressler, Christian; Chabera, Pavel; Christensen, Morten; Dohn, Asmus O.; Galler, Andreas; Gawelda, Wojciech; Gosztola, David; Haldrup, Kristoffer; Harlang, Tobias; Liu, Yizhu; Møller, Klaus B.; Németh, Zoltán; Nozawa, Shunsuke; Pápai, Mátyás; Sato, Tokushi; Sato, Takahiro; Suarez-Alcantara, Karina; Togashi, Tadashi; Tono, Kensuke; Uhlig, Jens; Vithanage, Dimali A.; Wärnmark, Kenneth; Yabashi, Makina; Zhang, Jianxin; Sundström, Villy; Nielsen, Martin M.

2015-01-01

Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined. PMID:25727920

Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

DOE PAGES

Canton, Sophie E.; Kjær, Kasper S.; Vankó, György; ...

2015-03-02

Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances.more » Thus experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.« less

Ultrafast X-ray Auger probing of photoexcited molecular dynamics

DOE PAGES

McFarland, B. K.; Farrell, J. P.; Miyabe, S.; ...

2014-06-23

Here, molecules can efficiently and selectively convert light energy into other degrees of freedom. Disentangling the underlying ultrafast motion of electrons and nuclei of the photoexcited molecule presents a challenge to current spectroscopic approaches. Here we explore the photoexcited dynamics of molecules by an interaction with an ultrafast X-ray pulse creating a highly localized core hole that decays via Auger emission. We discover that the Auger spectrum as a function of photoexcitation—X-ray-probe delay contains valuable information about the nuclear and electronic degrees of freedom from an element-specific point of view. For the nucleobase thymine, the oxygen Auger spectrum shifts towardsmore » high kinetic energies, resulting from a particular C–O bond stretch in the ππ* photoexcited state. A subsequent shift of the Auger spectrum towards lower kinetic energies displays the electronic relaxation of the initial photoexcited state within 200 fs. Ab-initio simulations reinforce our interpretation and indicate an electronic decay to the nπ* state.« less

Large-scale atomistic calculations of clusters in intense x-ray pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ho, Phay J.; Knight, Chris

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that leadmore » to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.« less

Large-scale atomistic calculations of clusters in intense x-ray pulses

DOE PAGES

Ho, Phay J.; Knight, Chris

2017-04-28

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that leadmore » to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.« less

Single shot speckle and coherence analysis of the hard X-ray free electron laser LCLS

DOE PAGES

Lee, Sooheyong; Roseker, W.; Gutt, C.; ...

2013-10-08

The single shot based coherence properties of hard x-ray pulses from the Linac Coherent Light Source (LCLS) were measured by analyzing coherent diffraction patterns from nano-particles and gold nanopowder. The intensity histogram of the small angle x-ray scattering ring from nano-particles reveals the fully transversely coherent nature of the LCLS beam with a number of transverse modemore » $$\\langle$$M s$$\\rangle$$ = 1.1. On the other hand, the speckle contrasts measured at a large wavevector yields information about the longitudinal coherence of the LCLS radiation after a silicon (111) monochromator. The quantitative agreement between our data and the simulation confirms a mean coherence time of 2.2 fs and a x-ray pulse duration of 29 fs. Lastly the observed reduction of the speckle contrast generated by x-rays with pulse duration longer than 30 fs indicates ultrafast dynamics taking place at an atomic length scale prior to the permanent sample damage.« less

Proposed imaging of the ultrafast electronic motion in samples using x-ray phase contrast.

PubMed

Dixit, Gopal; Slowik, Jan Malte; Santra, Robin

2013-03-29

Tracing the motion of electrons has enormous relevance to understanding ubiquitous phenomena in ultrafast science, such as the dynamical evolution of the electron density during complex chemical and biological processes. Scattering of ultrashort x-ray pulses from an electronic wave packet would appear to be the most obvious approach to image the electronic motion in real time and real space with the notion that such scattering patterns, in the far-field regime, encode the instantaneous electron density of the wave packet. However, recent results by Dixit et al. [Proc. Natl. Acad. Sci. U.S.A. 109, 11636 (2012)] have put this notion into question and have shown that the scattering in the far-field regime probes spatiotemporal density-density correlations. Here, we propose a possible way to image the instantaneous electron density of the wave packet via ultrafast x-ray phase contrast imaging. Moreover, we show that inelastic scattering processes, which plague ultrafast scattering in the far-field regime, do not contribute in ultrafast x-ray phase contrast imaging as a consequence of an interference effect. We illustrate our general findings by means of a wave packet that lies in the time and energy range of the dynamics of valence electrons in complex molecular and biological systems. This present work offers a potential to image not only instantaneous snapshots of nonstationary electron dynamics, but also the laplacian of these snapshots which provide information about the complex bonding and topology of the charge distributions in the systems.

Proposed Imaging of the Ultrafast Electronic Motion in Samples using X-Ray Phase Contrast

NASA Astrophysics Data System (ADS)

Dixit, Gopal; Slowik, Jan Malte; Santra, Robin

2013-03-01

Tracing the motion of electrons has enormous relevance to understanding ubiquitous phenomena in ultrafast science, such as the dynamical evolution of the electron density during complex chemical and biological processes. Scattering of ultrashort x-ray pulses from an electronic wave packet would appear to be the most obvious approach to image the electronic motion in real time and real space with the notion that such scattering patterns, in the far-field regime, encode the instantaneous electron density of the wave packet. However, recent results by Dixit et al. [Proc. Natl. Acad. Sci. U.S.A. 109, 11 636 (2012)] have put this notion into question and have shown that the scattering in the far-field regime probes spatiotemporal density-density correlations. Here, we propose a possible way to image the instantaneous electron density of the wave packet via ultrafast x-ray phase contrast imaging. Moreover, we show that inelastic scattering processes, which plague ultrafast scattering in the far-field regime, do not contribute in ultrafast x-ray phase contrast imaging as a consequence of an interference effect. We illustrate our general findings by means of a wave packet that lies in the time and energy range of the dynamics of valence electrons in complex molecular and biological systems. This present work offers a potential to image not only instantaneous snapshots of nonstationary electron dynamics, but also the Laplacian of these snapshots which provide information about the complex bonding and topology of the charge distributions in the systems.

Photon-assisted electron energy loss spectroscopy and ultrafast imaging.

PubMed

Howie, Archie

2009-08-01

A variety of ways is described in which photons can be used not only for ultrafast electron microscopy but also to enormously widen the energy range of spatially-resolved electron spectroscopy. Periodic chains of femtosecond laser pulses are a particularly important and accurately timed source for single-shot imaging and diffraction as well as for several forms of pump-probe microscopy at even higher spatial resolution and sub-picosecond timing. Many exciting new fields are opened up for study by these developments. Ultrafast, single shot diffraction with intense pulses of X-rays supplemented by phase retrieval techniques may eventually offer a challenging alternative and purely photon-based route to dynamic imaging at high spatial resolution.

On the properties of synchrotron-like X-ray emission from laser wakefield accelerated electron beams

NASA Astrophysics Data System (ADS)

McGuffey, C.; Schumaker, W.; Matsuoka, T.; Chvykov, V.; Dollar, F.; Kalintchenko, G.; Kneip, S.; Najmudin, Z.; Mangles, S. P. D.; Vargas, M.; Yanovsky, V.; Maksimchuk, A.; Thomas, A. G. R.; Krushelnick, K.

2018-04-01

The electric and magnetic fields responsible for electron acceleration in a Laser Wakefield Accelerator (LWFA) also cause electrons to radiate x-ray photons. Such x-ray pulses have several desirable properties including short duration and being well collimated with tunable high energy. We measure the scaling of this x-ray source experimentally up to laser powers greater than 100 TW. An increase in laser power allows electron trapping at a lower density as well as with an increased trapped charge. These effects resulted in an x-ray fluence that was measured to increase non-linearly with laser power. The fluence of x-rays was also compared with that produced from K-α emission resulting from a solid target interaction for the same energy laser pulse. The flux was shown to be comparable, but the LWFA x-rays had a significantly smaller source size. This indicates that such a source may be useful as a backlighter for probing high energy density plasmas with ultrafast temporal resolution.

Coherent Multidimensional Core Spectroscopy of Molecules with Multiple X-ray pulses

NASA Astrophysics Data System (ADS)

Mukamel, Shaul

2017-04-01

Multidimensional spectroscopy uses sequences of optical pulses to study dynamical processes in complex molecules through correlation plots involving several time delay periods. Extensions of these techniques to the x-ray regime will be discussed. Ultrafast nonlinear x-ray spectroscopy is made possible by newly developed free electron laser and high harmonic generation sources. The attosecond duration of X-ray pulses and the atomic selectivity of core X-ray excitations offer a uniquely high spatial and temporal resolution. We demonstrate how stimulated Raman detection of an X-ray probe may be used to monitor the phase and dynamics of the nonequilibrium valence electronic state wavepacket created by e.g. photoexcitation, photoionization and Auger processes. Spectroscopy of multiplecore excitations provides a new window into electron correlations. Applications will be presented to long-range charge transfer in proteins and to excitation energy transfer in porphyrin arrays. Conical intersections (CoIn) dominate the pathways and outcomes of virtually all photophysical and photochemical molecular processes. Despite extensive experimental and theoretical effort CoIns have not been directly observed yet and the experimental evidence is being inferred from fast reaction rates and some vibrational signatures. Novel ultrafast X ray probes for these processes will be presented. Short X-ray pulses can directly detect the passage through a CoIn with the adequate temporal and spectral sensitivity. The technique is based on a coherent Raman process that employs a composite femtosecond/attosecond X-ray pulse to directly detect the electronic coherences (rather than populations) that are generated as the system passes through the CoIn. Streaking of time-resolved photoelectron spectroscopy (TRPES) signals offers another powerful window into the joint electronic/vibrational dynamics at concial intersections. Strong coupling of molecules to the vacuum field of micro cavities can modify the potential energy surfaces thereby manipulating the photophysical and photochemical reaction pathways. The photonic vacuum state of a localized cavity mode can be strongly mixed with the molecular degrees of freedom to create hybrid field-matter states known as polaritons. Simulations of the avoided crossing of sodium iodide in a cavity which incorporate the quantized cavity field into the nuclear wave packet dynamics will be presented. Numerical results show how the branching ratio between the covalent and ionic dissociation channels can be strongly manipulated by the optical cavity.

0.5-keV Soft X-ray attosecond continua

PubMed Central

Teichmann, S. M.; Silva, F.; Cousin, S. L.; Hemmer, M.; Biegert, J.

2016-01-01

Attosecond light pulses in the extreme ultraviolet have drawn a great deal of attention due to their ability to interrogate electronic dynamics in real time. Nevertheless, to follow charge dynamics and excitations in materials, element selectivity is a prerequisite, which demands such pulses in the soft X-ray region, above 200 eV, to simultaneously cover several fundamental absorption edges of the constituents of the materials. Here, we experimentally demonstrate the exploitation of a transient phase matching regime to generate carrier envelope controlled soft X-ray supercontinua with pulse energies up to 2.9±0.1 pJ and a flux of (7.3±0.1) × 107 photons per second across the entire water window and attosecond pulses with 13 as transform limit. Our results herald attosecond science at the fundamental absorption edges of matter by bridging the gap between ultrafast temporal resolution and element specific probing. PMID:27167525

Ultrafast visualization of the structural evolution of dense hydrogen towards warm dense matter

NASA Astrophysics Data System (ADS)

Fletcher, Luke

2016-10-01

Hot dense hydrogen far from equilibrium is ubiquitous in nature occurring during some of the most violent and least understood events in our universe such as during star formation, supernova explosions, and the creation of cosmic rays. It is also a state of matter important for applications in inertial confinement fusion research and in laser particle acceleration. Rapid progress occurred in recent years characterizing the high-pressure structural properties of dense hydrogen under static or dynamic compression. Here, we show that spectrally and angularly resolved x-ray scattering measure the thermodynamic properties of dense hydrogen and resolve the ultrafast evolution and relaxation towards thermodynamic equilibrium. These studies apply ultra-bright x-ray pulses from the Linac Coherent Light (LCLS) source. The interaction of rapidly heated cryogenic hydrogen with a high-peak power optical laser is visualized with intense LCLS x-ray pulses in a high-repetition rate pump-probe setting. We demonstrate that electron-ion coupling is affected by the small number of particles in the Debye screening cloud resulting in much slower ion temperature equilibration than predicted by standard theory. This work was supported by the DOE Office of Science, Fusion Energy Science under FWP 100182.

Observation of Reverse Saturable Absorption of an X-ray Laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cho, B. I.; Cho, M. S.; Kim, M.

A nonlinear absorber in which the excited state absorption is larger than the ground state can undergo a process called reverse saturable absorption. It is a well-known phenomenon in laser physics in the optical regime, but is more difficult to generate in the x-ray regime, where fast nonradiative core electron transitions typically dominate the population kinetics during light matter interactions. Here, we report the first observation of decreasing x-ray transmission in a solid target pumped by intense x-ray free electron laser pulses. The measurement has been made below the K-absorption edge of aluminum, and the x-ray intensity ranges are 10more » 16 –10 17 W=cm 2. It has been confirmed by collisional radiative population kinetic calculations, underscoring the fast spectral modulation of the x-ray pulses and charge states relevant to the absorption and transmission of x-ray photons. The processes shown through detailed simulations are consistent with reverse saturable absorption, which would be the first observation of this phenomena in the x-ray regime. These light matter interactions provide a unique opportunity to investigate optical transport properties in the extreme state of matters, as well as affording the potential to regulate ultrafast x-ray freeelectron laser pulses.« less

Observation of Reverse Saturable Absorption of an X-ray Laser

DOE PAGES

Cho, B. I.; Cho, M. S.; Kim, M.; ...

2017-08-16

A nonlinear absorber in which the excited state absorption is larger than the ground state can undergo a process called reverse saturable absorption. It is a well-known phenomenon in laser physics in the optical regime, but is more difficult to generate in the x-ray regime, where fast nonradiative core electron transitions typically dominate the population kinetics during light matter interactions. Here, we report the first observation of decreasing x-ray transmission in a solid target pumped by intense x-ray free electron laser pulses. The measurement has been made below the K-absorption edge of aluminum, and the x-ray intensity ranges are 10more » 16 –10 17 W=cm 2. It has been confirmed by collisional radiative population kinetic calculations, underscoring the fast spectral modulation of the x-ray pulses and charge states relevant to the absorption and transmission of x-ray photons. The processes shown through detailed simulations are consistent with reverse saturable absorption, which would be the first observation of this phenomena in the x-ray regime. These light matter interactions provide a unique opportunity to investigate optical transport properties in the extreme state of matters, as well as affording the potential to regulate ultrafast x-ray freeelectron laser pulses.« less

Transient lattice contraction in the solid-to-plasma transition

PubMed Central

Ferguson, Ken R.; Bucher, Maximilian; Gorkhover, Tais; Boutet, Sébastien; Fukuzawa, Hironobu; Koglin, Jason E.; Kumagai, Yoshiaki; Lutman, Alberto; Marinelli, Agostino; Messerschmidt, Marc; Nagaya, Kiyonobu; Turner, Jim; Ueda, Kiyoshi; Williams, Garth J.; Bucksbaum, Philip H.; Bostedt, Christoph

2016-01-01

In condensed matter systems, strong optical excitations can induce phonon-driven processes that alter their mechanical properties. We report on a new phenomenon where a massive electronic excitation induces a collective change in the bond character that leads to transient lattice contraction. Single large van der Waals clusters were isochorically heated to a nanoplasma state with an intense 10-fs x-ray (pump) pulse. The structural evolution of the nanoplasma was probed with a second intense x-ray (probe) pulse, showing systematic contraction stemming from electron delocalization during the solid-to-plasma transition. These findings are relevant for any material in extreme conditions ranging from the time evolution of warm or hot dense matter to ultrafast imaging with intense x-ray pulses or, more generally, any situation that involves a condensed matter-to-plasma transition. PMID:27152323

Ultrafast High Harmonic, Soft X-Ray Probing of Molecular Dynamics

DTIC Science & Technology

2013-04-30

590 L/s scroll pump and a titanium sublimation pump . A TOF-PES has been designed and constructed to analyze the energy of the photoelectrons...are studied using the quasi-continuous vacuum ultraviolet light of the Advanced Light Source at Lawrence Berkeley National Laboratory. The molecular...34), the method of high order harmonic generation of ultrashort vacuum ultraviolet pulses was used to investigate molecular photodissociation, ultrafast

Spatially confined low-power optically pumped ultrafast synchrotron x-ray nanodiffraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, Joonkyu; Zhang, Qingteng; Chen, Pice

2015-08-27

The combination of ultrafast optical excitation and time-resolved synchrotron x-ray nanodiffraction provides unique insight into the photoinduced dynamics of materials, with the spatial resolution required to probe individual nanostructures or small volumes within heterogeneous materials. Optically excited x-ray nanobeam experiments are challenging because the high total optical power required for experimentally relevant optical fluences leads to mechanical instability due to heating. For a given fluence, tightly focusing the optical excitation reduces the average optical power by more than three orders of magnitude and thus ensures sufficient thermal stability for x-ray nanobeam studies. Delivering optical pulses via a scannable fiber-coupled opticalmore » objective provides a well-defined excitation geometry during rotation and translation of the sample and allows the selective excitation of isolated areas within the sample. Finally, experimental studies of the photoinduced lattice dynamics of a 35 nm BiFeO 3 thin film on a SrTiO 3 substrate demonstrate the potential to excite and probe nanoscale volumes.« less

Opportunities and challenges for time-resolved studies of protein structural dynamics at X-ray free-electron lasers.

PubMed

Neutze, Richard

2014-07-17

X-ray free-electron lasers (XFELs) are revolutionary X-ray sources. Their time structure, providing X-ray pulses of a few tens of femtoseconds in duration; and their extreme peak brilliance, delivering approximately 10(12) X-ray photons per pulse and facilitating sub-micrometre focusing, distinguish XFEL sources from synchrotron radiation. In this opinion piece, I argue that these properties of XFEL radiation will facilitate new discoveries in life science. I reason that time-resolved serial femtosecond crystallography and time-resolved wide angle X-ray scattering are promising areas of scientific investigation that will be advanced by XFEL capabilities, allowing new scientific questions to be addressed that are not accessible using established methods at storage ring facilities. These questions include visualizing ultrafast protein structural dynamics on the femtosecond to picosecond time-scale, as well as time-resolved diffraction studies of non-cyclic reactions. I argue that these emerging opportunities will stimulate a renaissance of interest in time-resolved structural biochemistry.

THz-pump and X-ray-probe sources based on an electron linac

NASA Astrophysics Data System (ADS)

Setiniyaz, Sadiq; Park, Seong Hee; Kim, Hyun Woo; Vinokurov, Nikolay A.; Jang, Kyu-Ha; Lee, Kitae; Baek, In Hyung; Jeong, Young Uk

2017-11-01

We describe a compact THz-pump and X-ray-probe beamline, based on an electron linac, for ultrafast time-resolved diffraction applications. Two high-energy electron (γ > 50) bunches, 5 ns apart, impinge upon a single-foil or multifoil radiator and generate THz radiation and X-rays simultaneously. The THz pulse from the first bunch is synchronized to the X-ray beam of the second bunch by using an adjustable optical delay of a THz pulse. The peak power of THz radiation from the multifoil radiator is estimated to be 0.14 GW for a 200 pC well-optimized electron bunch. GEANT4 simulations show that a carbon foil with a thickness of 0.5-1.0 mm has the highest yield of 10-20 keV hard X-rays for a 25 MeV beam, which is approximately 103 photons/(keV pC-electrons) within a few degrees of the polar angle. A carbon multifoil radiator with 35 foils (25 μm thick each) can generate close to 103 hard X-rays/(keV pC-electrons) within a 2° acceptance angle. With 200 pC charge and a 100 Hz repetition rate, we can generate 107 X-rays per 1 keV energy bin per second or 105 X-rays per 1 keV energy bin per pulse. The longitudinal time profile of an X-ray pulse ranges from 400 to 600 fs depending on the acceptance angle. The broadening of the time duration of an X-ray pulse is observed owing to its diverging effect. A double-crystal monochromator will be used to select and transport the desired X-rays to the sample. The heating of the radiators by an electron beam is negligible because of the low beam current.

Laser acceleration

NASA Astrophysics Data System (ADS)

Tajima, T.; Nakajima, K.; Mourou, G.

2017-02-01

The fundamental idea of Laser Wakefield Acceleration (LWFA) is reviewed. An ultrafast intense laser pulse drives coherent wakefield with a relativistic amplitude robustly supported by the plasma. While the large amplitude of wakefields involves collective resonant oscillations of the eigenmode of the entire plasma electrons, the wake phase velocity ˜ c and ultrafastness of the laser pulse introduce the wake stability and rigidity. A large number of worldwide experiments show a rapid progress of this concept realization toward both the high-energy accelerator prospect and broad applications. The strong interest in this has been spurring and stimulating novel laser technologies, including the Chirped Pulse Amplification, the Thin Film Compression, the Coherent Amplification Network, and the Relativistic Mirror Compression. These in turn have created a conglomerate of novel science and technology with LWFA to form a new genre of high field science with many parameters of merit in this field increasing exponentially lately. This science has triggered a number of worldwide research centers and initiatives. Associated physics of ion acceleration, X-ray generation, and astrophysical processes of ultrahigh energy cosmic rays are reviewed. Applications such as X-ray free electron laser, cancer therapy, and radioisotope production etc. are considered. A new avenue of LWFA using nanomaterials is also emerging.

Theory of time-resolved x-ray photoelectron diffraction from transient conformational molecules

NASA Astrophysics Data System (ADS)

Tsuru, Shota; Sako, Tokuei; Fujikawa, Takashi; Yagishita, Akira

2017-04-01

We formulate x-ray photoelectron diffraction (XPD) from molecules undergoing photochemical reactions induced by optical laser pulses, and then apply the formula to the simulation of time-dependent XPD profiles from both dissociating I2 molecules and bending C S2 molecules. The dependence of nuclear wave-packet motions on the intensity and shape of the optical laser pulses is examined. As a result, the XPD simulations based on such nuclear wave-packet calculations are observed to exhibit characteristic features, which are compared with the XPD profiles due to classical trajectories of nuclear motions. The present study provides a methodology toward creating "molecular movies" of ultrafast photochemical reactions by means of femtosecond XPD with x-ray free-electron lasers.

Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy

NASA Astrophysics Data System (ADS)

Priebe, Katharina E.; Rathje, Christopher; Yalunin, Sergey V.; Hohage, Thorsten; Feist, Armin; Schäfer, Sascha; Ropers, Claus

2017-12-01

Ultrafast electron and X-ray imaging and spectroscopy are the basis for an ongoing revolution in the understanding of dynamical atomic-scale processes in matter. The underlying technology relies heavily on laser science for the generation and characterization of ever shorter pulses. Recent findings suggest that ultrafast electron microscopy with attosecond-structured wavefunctions may be feasible. However, such future technologies call for means to both prepare and fully analyse the corresponding free-electron quantum states. Here, we introduce a framework for the preparation, coherent manipulation and characterization of free-electron quantum states, experimentally demonstrating attosecond electron pulse trains. Phase-locked optical fields coherently control the electron wavefunction along the beam direction. We establish a new variant of quantum state tomography—`SQUIRRELS'—for free-electron ensembles. The ability to tailor and quantitatively map electron quantum states will promote the nanoscale study of electron-matter entanglement and new forms of ultrafast electron microscopy down to the attosecond regime.

Analyzing the effect of slotted foil on radiation pulse profile in a mode locked afterburner X-ray free electron laser

NASA Astrophysics Data System (ADS)

Kumar, Sandeep; Hur, Min Sup; Chung, Moses

2017-06-01

Extremely short X-ray pulses in the attosecond (as) range are important tools for ultrafast dynamics, high resolution microscopy, and nuclear dynamics study. In this paper, we numerically examine the generation of gigawatt (GW) mode-locked (ML) multichromatic X-rays using the parameters of the Pohang Accelerator Laboratory (PAL)-X-ray free electron laser (XFEL), the Korean XFEL. In this vein, we analyze the ML-FEL [Thompson and McNeil, Phys. Rev. Lett. 100, 203901 (2008)] and mode-locked afterburner (MLAB) FEL [Dunning et al., Phys. Rev. Lett. 110, 104801 (2013)] schemes on the hard X-ray beamline of the PAL-XFEL. Using the ML scheme, we numerically demonstrate a train of radiation pulses in the hard X-ray (photon energy ˜12.4 keV) with 3.5 GW power and 16 as full-width half maximum (FWHM) pulse duration. On the other hand, using the MLAB scheme, a train of radiation pulses with 3 GW power and 1 as FWHM (900 zs in RMS) pulse duration has been obtained at 12.4 keV photon energy. Both schemes generate broadband, discrete, and coherent spectrum compared to the XFEL's narrowband spectrum. Furthermore, the effect of slotted foil is also studied first time on the MLAB-FEL output. Numerical comparisons show that the temporal structure of the MLAB-FEL output can be improved significantly by the use of the slotted foil. Such short X-ray pulses at XFEL facilities will allow the studies of electron-nuclear and nuclear dynamics in atoms or molecules, and the broadband radiation will substantially improve the efficiency of the experimental techniques such as X-ray crystallography and spectroscopy, paving the way for outstanding progress in biology and material science.

Roadmap of ultrafast x-ray atomic and molecular physics

NASA Astrophysics Data System (ADS)

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

2018-02-01

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ˜1 Ångstrom, and HHG provides unprecedented time resolution (˜50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ˜280 eV (44 Ångstroms) and the bond length in methane of ˜1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.

Roadmap of ultrafast x-ray atomic and molecular physics

DOE PAGES

Young, Linda; Ueda, Kiyoshi; Gühr, Markus; ...

2018-01-09

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10 20 W cm -2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scalesmore » can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here in this paper, we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.« less

Roadmap of ultrafast x-ray atomic and molecular physics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Young, Linda; Ueda, Kiyoshi; Gühr, Markus

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10 20 W cm -2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scalesmore » can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here in this paper, we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.« less

Analysis of a measurement scheme for ultrafast hole dynamics by few femtosecond resolution X-ray pump-probe Auger spectroscopy.

PubMed

Cooper, Bridgette; Kolorenč, Přemysl; Frasinski, Leszek J; Averbukh, Vitali; Marangos, Jon P

2014-01-01

Ultrafast hole dynamics created in molecular systems as a result of sudden ionisation is the focus of much attention in the field of attosecond science. Using the molecule glycine we show through ab initio simulations that the dynamics of a hole, arising from ionisation in the inner valence region, evolves with a timescale appropriate to be measured using X-ray pulses from the current generation of SASE free electron lasers. The examined pump-probe scheme uses X-rays with photon energy below the K edge of carbon (275-280 eV) that will ionise from the inner valence region. A second probe X-ray at the same energy can excite an electron from the core to fill the vacancy in the inner-valence region. The dynamics of the inner valence hole can be tracked by measuring the Auger electrons produced by the subsequent refilling of the core hole as a function of pump-probe delay. We consider the feasibility of the experiment and include numerical simulation to support this analysis. We discuss the potential for all X-ray pump-X-ray probe Auger spectroscopy measurements for tracking hole migration.

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

NASA Astrophysics Data System (ADS)

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

2007-03-01

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

Generation of sub-two-cycle millijoule infrared pulses in an optical parametric chirped-pulse amplifier and their application to soft x-ray absorption spectroscopy with high-flux high harmonics

NASA Astrophysics Data System (ADS)

Ishii, Nobuhisa; Kaneshima, Keisuke; Kanai, Teruto; Watanabe, Shuntaro; Itatani, Jiro

2018-01-01

An optical parametric chirped-pulse amplifier (OPCPA) based on bismuth triborate (BiB3O6, BIBO) crystals has been developed to deliver 1.5 mJ, 10.1 fs optical pulses around 1.6 μm with a repetition rate of 1 kHz and a stable carrier-envelope phase. The seed and pump pulses of the BIBO-based OPCPA are provided from two Ti:sapphire chirped-pulse amplification (CPA) systems. In both CPA systems, transmission gratings are used in the stretchers and compressors that result in a high throughput and robust operation without causing any thermal problem and optical damage. The seed pulses of the OPCPA are generated by intrapulse frequency mixing of a spectrally broadened continuum, temporally stretched to approximately 5 ps then, and amplified to more than 1.5 mJ. The amplified pulses are compressed in a fused silica block down to 10.1 fs. This BIBO-based OPCPA has been applied to high-flux high harmonic generation beyond the carbon K edge at 284 eV. The high-flux soft-x-ray continuum allows measuring the x-ray absorption near-edge structure of the carbon K edge within 2 min, which is shorter than a typical measurement time using synchrotron-based light sources. This laser-based table-top soft-x-ray source is a promising candidate for ultrafast soft x-ray spectroscopy with femtosecond to attosecond time resolution.

Pulse intensity characterization of the LCLS nanosecond double-bunch mode of operation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sun, Yanwen; Decker, Franz-Josef; Turner, James

The recent demonstration of the 'nanosecond double-bunch' operation mode,i.e.two X-ray pulses separated in time between 0.35 and hundreds of nanoseconds and by increments of 0.35 ns, offers new opportunities to investigate ultrafast dynamics in diverse systems of interest. However, in order to reach its full potential, this mode of operation requires the precise characterization of the intensity of each X-ray pulse within each pulse pair for any time separation. Here, a transmissive single-shot diagnostic that achieves this goal for time separations larger than 0.7 ns with a precision better than 5% is presented. Lastly, it also provides real-time monitoring feedbackmore » to help tune the accelerator parameters to deliver double pulse intensity distributions optimized for specific experimental goals.« less

Pulse intensity characterization of the LCLS nanosecond double-bunch mode of operation

DOE PAGES

Sun, Yanwen; Decker, Franz-Josef; Turner, James; ...

2018-03-27

The recent demonstration of the 'nanosecond double-bunch' operation mode,i.e.two X-ray pulses separated in time between 0.35 and hundreds of nanoseconds and by increments of 0.35 ns, offers new opportunities to investigate ultrafast dynamics in diverse systems of interest. However, in order to reach its full potential, this mode of operation requires the precise characterization of the intensity of each X-ray pulse within each pulse pair for any time separation. Here, a transmissive single-shot diagnostic that achieves this goal for time separations larger than 0.7 ns with a precision better than 5% is presented. Lastly, it also provides real-time monitoring feedbackmore » to help tune the accelerator parameters to deliver double pulse intensity distributions optimized for specific experimental goals.« less

Detailed transient heme structures of Mb-CO in solution after CO dissociation: an X-ray transient absorption spectroscopic study.

PubMed

Stickrath, Andrew B; Mara, Michael W; Lockard, Jenny V; Harpham, Michael R; Huang, Jier; Zhang, Xiaoyi; Attenkofer, Klaus; Chen, Lin X

2013-04-25

Although understanding the structural dynamics associated with ligand photodissociation is necessary in order to correlate structure and function in biological systems, few techniques are capable of measuring the ultrafast dynamics of these systems in solution-phase at room temperature. We present here a detailed X-ray transient absorption (XTA) study of the photodissociation of CO-bound myoglobin (Fe(II)CO-Mb) in room-temperature aqueous buffer solution with a time resolution of 80 ps, along with a general procedure for handling biological samples under the harsh experimental conditions that transient X-ray experiments entail. The XTA spectra of (Fe(II)CO-Mb) exhibit significant XANES and XAFS alterations following 527 nm excitation, which remain unchanged for >47 μs. These spectral changes indicate loss of the CO ligand, resulting in a five-coordinate, domed heme, and significant energetic reorganization of the 3d orbitals of the Fe center. With the current experimental setup, each X-ray pulse in the pulse train, separated by ~153 ns, can be separately discriminated, yielding snapshots of the myoglobin evolution over time. These methods can be easily applied to other biological systems, allowing for simultaneous structural and electronic measurements of any biological system with both ultrafast and slow time resolutions, effectively mapping out all of the samples' relevant physiological processes.

Direct longitudinal laser acceleration of electrons in free space

NASA Astrophysics Data System (ADS)

Carbajo, Sergio; Nanni, Emilio A.; Wong, Liang Jie; Moriena, Gustavo; Keathley, Phillip D.; Laurent, Guillaume; Miller, R. J. Dwayne; Kärtner, Franz X.

2016-02-01

Compact laser-driven accelerators are pursued heavily worldwide because they make novel methods and tools invented at national laboratories widely accessible in science, health, security, and technology [V. Malka et al., Principles and applications of compact laser-plasma accelerators, Nat. Phys. 4, 447 (2008)]. Current leading laser-based accelerator technologies [S. P. D. Mangles et al., Monoenergetic beams of relativistic electrons from intense laser-plasma interactions, Nature (London) 431, 535 (2004); T. Toncian et al., Ultrafast laser-driven microlens to focus and energy-select mega-electron volt protons, Science 312, 410 (2006); S. Tokita et al. Single-shot ultrafast electron diffraction with a laser-accelerated sub-MeV electron pulse, Appl. Phys. Lett. 95, 111911 (2009)] rely on a medium to assist the light to particle energy transfer. The medium imposes material limitations or may introduce inhomogeneous fields [J. R. Dwyer et al., Femtosecond electron diffraction: "Making the molecular movie,", Phil. Trans. R. Soc. A 364, 741 (2006)]. The advent of few cycle ultraintense radially polarized lasers [S. Carbajo et al., Efficient generation of ultraintense few-cycle radially polarized laser pulses, Opt. Lett. 39, 2487 (2014)] has ushered in a novel accelerator concept [L. J. Wong and F. X. Kärtner, Direct acceleration of an electron in infinite vacuum by a pulsed radially polarized laser beam, Opt. Express 18, 25035 (2010); F. Pierre-Louis et al. Direct-field electron acceleration with ultrafast radially polarized laser beams: Scaling laws and optimization, J. Phys. B 43, 025401 (2010); Y. I. Salamin, Electron acceleration from rest in vacuum by an axicon Gaussian laser beam, Phys. Rev. A 73, 043402 (2006); C. Varin and M. Piché, Relativistic attosecond electron pulses from a free-space laser-acceleration scheme, Phys. Rev. E 74, 045602 (2006); A. Sell and F. X. Kärtner, Attosecond electron bunches accelerated and compressed by radially polarized laser pulses and soft-x-ray pulses from optical undulators, J. Phys. B 47, 015601 (2014)] avoiding the need of a medium or guiding structure entirely to achieve strong longitudinal energy transfer. Here we present the first observation of direct longitudinal laser acceleration of nonrelativistic electrons that undergo highly directional multi-GeV /m accelerating gradients. This demonstration opens a new frontier for direct laser-driven particle acceleration capable of creating well collimated and relativistic attosecond electron bunches [C. Varin and M. Piché, Relativistic attosecond electron pulses from a free-space laser-acceleration scheme, Phys. Rev. E 74, 045602 (2006)] and x-ray pulses [A. Sell and F. X. Kärtner, Attosecond electron bunches accelerated and compressed by radially polarized laser pulses and soft-x-ray pulses from optical undulators, J. Phys. B 47, 015601 (2014)].

Hit detection in serial femtosecond crystallography using X-ray spectroscopy of plasma emission.

PubMed

Jönsson, H Olof; Caleman, Carl; Andreasson, Jakob; Tîmneanu, Nicuşor

2017-11-01

Serial femtosecond crystallography is an emerging and promising method for determining protein structures, making use of the ultrafast and bright X-ray pulses from X-ray free-electron lasers. The upcoming X-ray laser sources will produce well above 1000 pulses per second and will pose a new challenge: how to quickly determine successful crystal hits and avoid a high-rate data deluge. Proposed here is a hit-finding scheme based on detecting photons from plasma emission after the sample has been intercepted by the X-ray laser. Plasma emission spectra are simulated for systems exposed to high-intensity femtosecond pulses, for both protein crystals and the liquid carrier systems that are used for sample delivery. The thermal radiation from the glowing plasma gives a strong background in the XUV region that depends on the intensity of the pulse, around the emission lines from light elements (carbon, nitrogen, oxygen). Sample hits can be reliably distinguished from the carrier liquid based on the characteristic emission lines from heavier elements present only in the sample, such as sulfur. For buffer systems with sulfur present, selenomethionine substitution is suggested, where the selenium emission lines could be used both as an indication of a hit and as an aid in phasing and structural reconstruction of the protein.

Experimental characterization of an ultra-fast Thomson scattering x-ray source with three-dimensional time and frequency-domain analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuba, J; Slaughter, D R; Fittinghoff, D N

We present a detailed comparison of the measured characteristics of Thomson backscattered x-rays produced at the PLEIADES (Picosecond Laser-Electron Interaction for the Dynamic Evaluation of Structures) facility at Lawrence Livermore National Laboratory to predicted results from a newly developed, fully three-dimensional time and frequency-domain code. Based on the relativistic differential cross section, this code has the capability to calculate time and space dependent spectra of the x-ray photons produced from linear Thomson scattering for both bandwidth-limited and chirped incident laser pulses. Spectral broadening of the scattered x-ray pulse resulting from the incident laser bandwidth, perpendicular wave vector components in themore » laser focus, and the transverse and longitudinal phase space of the electron beam are included. Electron beam energy, energy spread, and transverse phase space measurements of the electron beam at the interaction point are presented, and the corresponding predicted x-ray characteristics are determined. In addition, time-integrated measurements of the x-rays produced from the interaction are presented, and shown to agree well with the simulations.« less

X-ray phase-contrast imaging: the quantum perspective

NASA Astrophysics Data System (ADS)

Slowik, J. M.; Santra, R.

2013-08-01

Time-resolved phase-contrast imaging using ultrafast x-ray sources is an emerging method to investigate ultrafast dynamical processes in matter. Schemes to generate attosecond x-ray pulses have been proposed, bringing electronic timescales into reach and emphasizing the demand for a quantum description. In this paper, we present a method to describe propagation-based x-ray phase-contrast imaging in nonrelativistic quantum electrodynamics. We explain why the standard scattering treatment via Fermi’s golden rule cannot be applied. Instead, the quantum electrodynamical treatment of phase-contrast imaging must be based on a different approach. It turns out that it is essential to select a suitable observable. Here, we choose the quantum-mechanical Poynting operator. We determine the expectation value of our observable and demonstrate that the leading order term describes phase-contrast imaging. It recovers the classical expression of phase-contrast imaging. Thus, it makes the instantaneous electron density of non-stationary electronic states accessible to time-resolved imaging. Interestingly, inelastic (Compton) scattering does automatically not contribute in leading order, explaining the success of the semiclassical description.

Measurement of high-dynamic range x-ray Thomson scattering spectra for the characterization of nano-plasmas at LCLS

DOE PAGES

MacDonald, M. J.; Gorkhover, T.; Bachmann, B.; ...

2016-08-08

Atomic clusters can serve as ideal model systems for exploring ultrafast (~100 fs) laser-driven ionization dynamics of dense matter on the nanometer scale. Resonant absorption of optical laser pulses enables heating to temperatures on the order of 1 keV at near solid density conditions. To date, direct probing of transient states of such nano plasmas was limited to coherent x-ray imaging. Here we present the first measurement of spectrally-resolved incoherent x-ray scattering from clusters, enabling measurements of transient temperature, densities and ionization. Single shot x-ray Thomson scatterings signals were recorded at 120 Hz using a crystal spectrometer in combination withmore » a single-photon counting and energy-dispersive pnCCD. A precise pump laser collimation scheme enabled recording near background-free scattering spectra from Ar clusters with an unprecedented dynamic range of more than 3 orders of magnitude. As a result, such measurements are important for understanding collective effects in laser-matter interactions on femtosecond timescales, opening new routes for the development of schemes for their ultrafast control.« less

Measurement of high-dynamic range x-ray Thomson scattering spectra for the characterization of nano-plasmas at LCLS

DOE Office of Scientific and Technical Information (OSTI.GOV)

MacDonald, M. J., E-mail: macdonm@umich.edu; SLAC National Accelerator Laboratory, Menlo Park, California 94025; Gorkhover, T.

2016-11-15

Atomic clusters can serve as ideal model systems for exploring ultrafast (∼100 fs) laser-driven ionization dynamics of dense matter on the nanometer scale. Resonant absorption of optical laser pulses enables heating to temperatures on the order of 1 keV at near solid density conditions. To date, direct probing of transient states of such nano-plasmas was limited to coherent x-ray imaging. Here we present the first measurement of spectrally resolved incoherent x-ray scattering from clusters, enabling measurements of transient temperature, densities, and ionization. Single shot x-ray Thomson scattering signals were recorded at 120 Hz using a crystal spectrometer in combination withmore » a single-photon counting and energy-dispersive pnCCD. A precise pump laser collimation scheme enabled recording near background-free scattering spectra from Ar clusters with an unprecedented dynamic range of more than 3 orders of magnitude. Such measurements are important for understanding collective effects in laser-matter interactions on femtosecond time scales, opening new routes for the development of schemes for their ultrafast control.« less

X-ray Diffuse Scattering from Ultrafast Laser Excited Solids

NASA Astrophysics Data System (ADS)

Trigo, Mariano; Sheu, Yu-Miin; Chen, Jian; Reis, David; Fahy, Stephen; Murray, Eamonn; Graber, Timothy; Henning, Robert

2009-03-01

Intense, ultrashort laser pulses can be used to excite and detect coherent phonons in solids. However, optical experiments can only probe a reduced fraction of the Brillouin zone and hence most of the decay channels of such coherent phonons become invisible. In contrast, time-resolved x-ray diffuse scattering (TRXDS) has the potential to be the ultimate tool to study these phonon decay processes throughout the Brillouin-zone of the crystal. In our work, performed at the BioCARS beamline at the Advanced Photon Source, we use synchrotron time-resolved diffuse x-ray scattering to study Si and Bi under intense laser excitation with 100 ps resolution. We show that reasonable signal levels can be achieved with incident flux of 10^12 photons comparable to the flux that will be available at future 4th generation sources such as the LCLS in a single pulse. These sources will also provide three orders of magnitude shorter pulses; thus, this experiment serves as a test of the feasibility of time-resolved X-ray diffuse scattering as a tool for studying nonequilibrium phonon dynamics in solids.

THz-pump and X-ray-probe sources based on an electron linac.

PubMed

Setiniyaz, Sadiq; Park, Seong Hee; Kim, Hyun Woo; Vinokurov, Nikolay A; Jang, Kyu-Ha; Lee, Kitae; Baek, In Hyung; Jeong, Young Uk

2017-11-01

We describe a compact THz-pump and X-ray-probe beamline, based on an electron linac, for ultrafast time-resolved diffraction applications. Two high-energy electron (γ > 50) bunches, 5 ns apart, impinge upon a single-foil or multifoil radiator and generate THz radiation and X-rays simultaneously. The THz pulse from the first bunch is synchronized to the X-ray beam of the second bunch by using an adjustable optical delay of a THz pulse. The peak power of THz radiation from the multifoil radiator is estimated to be 0.14 GW for a 200 pC well-optimized electron bunch. GEANT4 simulations show that a carbon foil with a thickness of 0.5-1.0 mm has the highest yield of 10-20 keV hard X-rays for a 25 MeV beam, which is approximately 10 3 photons/(keV pC-electrons) within a few degrees of the polar angle. A carbon multifoil radiator with 35 foils (25 μm thick each) can generate close to 10 3 hard X-rays/(keV pC-electrons) within a 2° acceptance angle. With 200 pC charge and a 100 Hz repetition rate, we can generate 10 7 X-rays per 1 keV energy bin per second or 10 5 X-rays per 1 keV energy bin per pulse. The longitudinal time profile of an X-ray pulse ranges from 400 to 600 fs depending on the acceptance angle. The broadening of the time duration of an X-ray pulse is observed owing to its diverging effect. A double-crystal monochromator will be used to select and transport the desired X-rays to the sample. The heating of the radiators by an electron beam is negligible because of the low beam current.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dixit, Gopal; Santra, Robin; Department of Physics, University of Hamburg, D-20355 Hamburg

2013-04-07

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

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

NASA Astrophysics Data System (ADS)

Dixit, Gopal; Santra, Robin

2013-04-01

Ultrafast time-resolved x-ray scattering is an emerging approach to image the dynamical evolution of the electronic charge distribution during complex chemical and biological processes in real-space and real-time. Recently, the differences between semiclassical and quantum-electrodynamical (QED) theory of light-matter interaction for scattering of ultrashort x-ray pulses from the electronic wavepacket were formally demonstrated and visually illustrated by scattering patterns calculated for an electronic wavepacket in atomic hydrogen [G. Dixit, O. Vendrell, and R. Santra, Proc. Natl. Acad. Sci. U.S.A. 109, 11636 (2012)], 10.1073/pnas.1202226109. In this work, we present a detailed analysis of time-resolved x-ray scattering from a sample containing a mixture of non-stationary and stationary electrons within both the theories. In a many-electron system, the role of scattering interference between a non-stationary and several stationary electrons to the total scattering signal is investigated. In general, QED and semiclassical theory provide different results for the contribution from the scattering interference, which depends on the energy resolution of the detector and the x-ray pulse duration. The present findings are demonstrated by means of a numerical example of x-ray time-resolved imaging for an electronic wavepacket in helium. It is shown that the time-dependent scattering interference vanishes within semiclassical theory and the corresponding patterns are dominated by the scattering contribution from the time-independent interference, whereas the time-dependent scattering interference contribution do not vanish in the QED theory and the patterns are dominated by the scattering contribution from the non-stationary electron scattering.

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

PubMed

Dixit, Gopal; Santra, Robin

2013-04-07

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

Direct-write maskless lithography using patterned oxidation of Si-substrate Induced by femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Kiani, Amirkianoosh; Venkatakrishnan, Krishnan; Tan, Bo

2013-03-01

In this study we report a new method for direct-write maskless lithography using oxidized silicon layer induced by high repetition (MHz) ultrafast (femtosecond) laser pulses under ambient condition. The induced thin layer of predetermined pattern can act as an etch stop during etching process in alkaline etchants such as KOH. The proposed method can be leading to promising solutions for direct-write maskless lithography technique since the proposed method offers a higher degree of flexibility and reduced time and cost of fabrication which makes it particularly appropriate for rapid prototyping and custom scale manufacturing. A Scanning Electron Microscope (SEM), Micro-Raman, Energy Dispersive X-ray (EDX), optical microscope and X-ray diffraction spectroscopy (XRD) were used to evaluate the quality of oxidized layer induced by laser pulses.

Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses

PubMed Central

Boll, Rebecca; Erk, Benjamin; Coffee, Ryan; Trippel, Sebastian; Kierspel, Thomas; Bomme, Cédric; Bozek, John D.; Burkett, Mitchell; Carron, Sebastian; Ferguson, Ken R.; Foucar, Lutz; Küpper, Jochen; Marchenko, Tatiana; Miron, Catalin; Patanen, Minna; Osipov, Timur; Schorb, Sebastian; Simon, Marc; Swiggers, Michelle; Techert, Simone; Ueda, Kiyoshi; Bostedt, Christoph; Rolles, Daniel; Rudenko, Artem

2016-01-01

Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse. PMID:27051675

Time-resolved structural studies at synchrotrons and X-ray free electron lasers: opportunities and challenges

PubMed Central

Neutze, Richard; Moffat, Keith

2012-01-01

X-ray free electron lasers (XFELs) are potentially revolutionary X-ray sources because of their very short pulse duration, extreme peak brilliance and high spatial coherence, features that distinguish them from today’s synchrotron sources. We review recent time-resolved Laue diffraction and time-resolved wide angle X-ray scattering (WAXS) studies at synchrotron sources, and initial static studies at XFELs. XFELs have the potential to transform the field of time-resolved structural biology, yet many challenges arise in devising and adapting hardware, experimental design and data analysis strategies to exploit their unusual properties. Despite these challenges, we are confident that XFEL sources are poised to shed new light on ultrafast protein reaction dynamics. PMID:23021004

Ultrafast isomerization initiated by X-ray core ionization

NASA Astrophysics Data System (ADS)

Liekhus-Schmaltz, Chelsea E.; Tenney, Ian; Osipov, Timur; Sanchez-Gonzalez, Alvaro; Berrah, Nora; Boll, Rebecca; Bomme, Cedric; Bostedt, Christoph; Bozek, John D.; Carron, Sebastian; Coffee, Ryan; Devin, Julien; Erk, Benjamin; Ferguson, Ken R.; Field, Robert W.; Foucar, Lutz; Frasinski, Leszek J.; Glownia, James M.; Gühr, Markus; Kamalov, Andrei; Krzywinski, Jacek; Li, Heng; Marangos, Jonathan P.; Martinez, Todd J.; McFarland, Brian K.; Miyabe, Shungo; Murphy, Brendan; Natan, Adi; Rolles, Daniel; Rudenko, Artem; Siano, Marco; Simpson, Emma R.; Spector, Limor; Swiggers, Michele; Walke, Daniel; Wang, Song; Weber, Thorsten; Bucksbaum, Philip H.; Petrovic, Vladimir S.

2015-09-01

Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a `molecular movie' of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.

Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Ji -Cai; Berrah, Nora; Cederbaum, Lorenz S.

Here, we study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength ofmore » $$1.1\\;{\\rm{nm}}$$ ($$1100\\;{\\rm{eV}}$$ photon energy) from the Linac Coherent Light Source (LCLS) free electron laser. Molecular rate equations are derived to describe the intertwined photoionization, decay, and dissociation processes occurring for N2. This model complements our earlier phenomenological approaches, the single-atom, symmetric-sharing, and fragmentation-matrix models of 2012 (J. Chem. Phys. 136 214310). Our rate-equations are used to obtain the effective pulse energy at the sample and the time scale for the dissociation of the metastable dication $${{\\rm{N}}}_{2}^{2+}$$. This leads to a very good agreement between the theoretically and experimentally determined ion yields and, consequently, the average charge states. The effective pulse energy is found to decrease with shortening pulse duration. This variation together with a change in the molecular fragmentation pattern and frustrated absorption—an effect that reduces absorption of x-rays due to (double) core hole formation—are the causes for the drop of the average charge state with shortening LCLS pulse duration discovered previously.« less

Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses

DOE PAGES

Liu, Ji -Cai; Berrah, Nora; Cederbaum, Lorenz S.; ...

2016-03-16

Here, we study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength ofmore » $$1.1\\;{\\rm{nm}}$$ ($$1100\\;{\\rm{eV}}$$ photon energy) from the Linac Coherent Light Source (LCLS) free electron laser. Molecular rate equations are derived to describe the intertwined photoionization, decay, and dissociation processes occurring for N2. This model complements our earlier phenomenological approaches, the single-atom, symmetric-sharing, and fragmentation-matrix models of 2012 (J. Chem. Phys. 136 214310). Our rate-equations are used to obtain the effective pulse energy at the sample and the time scale for the dissociation of the metastable dication $${{\\rm{N}}}_{2}^{2+}$$. This leads to a very good agreement between the theoretically and experimentally determined ion yields and, consequently, the average charge states. The effective pulse energy is found to decrease with shortening pulse duration. This variation together with a change in the molecular fragmentation pattern and frustrated absorption—an effect that reduces absorption of x-rays due to (double) core hole formation—are the causes for the drop of the average charge state with shortening LCLS pulse duration discovered previously.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weathersby, S. P.; Brown, G.; Chase, T. F.

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

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

PubMed

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

2015-07-01

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

Single-particle coherent diffractive imaging with a soft x-ray free electron laser: towards soot aerosol morphology

NASA Astrophysics Data System (ADS)

Bogan, Michael J.; Starodub, Dmitri; Hampton, Christina Y.; Sierra, Raymond G.

2010-10-01

The first of its kind, the Free electron LASer facility in Hamburg, FLASH, produces soft x-ray pulses with unprecedented properties (10 fs, 6.8-47 nm, 1012 photons per pulse, 20 µm diameter). One of the seminal FLASH experiments is single-pulse coherent x-ray diffractive imaging (CXDI). CXDI utilizes the ultrafast and ultrabright pulses to overcome resolution limitations in x-ray microscopy imposed by x-ray-induced damage to the sample by 'diffracting before destroying' the sample on sub-picosecond timescales. For many lensless imaging algorithms used for CXDI it is convenient when the data satisfy an oversampling constraint that requires the sample to be an isolated object, i.e. an individual 'free-standing' portion of disordered matter delivered to the centre of the x-ray focus. By definition, this type of matter is an aerosol. This paper will describe the role of aerosol science methodologies used for the validation of the 'diffract before destroy' hypothesis and the execution of the first single-particle CXDI experiments being developed for biological imaging. FLASH CXDI now enables the highest resolution imaging of single micron-sized or smaller airborne particulate matter to date while preserving the native substrate-free state of the aerosol. Electron microscopy offers higher resolution for single-particle analysis but the aerosol must be captured on a substrate, potentially modifying the particle morphology. Thus, FLASH is poised to contribute significant advancements in our knowledge of aerosol morphology and dynamics. As an example, we simulate CXDI of combustion particle (soot) morphology and introduce the concept of extracting radius of gyration of fractal aggregates from single-pulse x-ray diffraction data. Future upgrades to FLASH will enable higher spatially and temporally resolved single-particle aerosol dynamics studies, filling a critical technological need in aerosol science and nanotechnology. Many of the methodologies described for FLASH will directly translate to use at hard x-ray free electron lasers.

Isolated elliptically polarized attosecond soft X-ray with high-brilliance using polarization gating of harmonics from relativistic plasmas at oblique incidence.

PubMed

Chen, Zi-Yu; Li, Xiao-Ya; Li, Bo-Yuan; Chen, Min; Liu, Feng

2018-02-19

The production of intense isolated attosecond pulse is a major goal in ultrafast research. Recent advances in high harmonic generation from relativistic plasma mirrors under oblique incidence interactions gave rise to photon-rich attosecond pulses with circular or elliptical polarization. However, to achieve an isolated elliptical attosecond pulse via polarization gating using currently available long driving pulses remains a challenge, because polarization gating of high harmonics from relativistic plasmas is assumed only possible at normal or near-normal incidence. Here we numerically demonstrate a scheme around this problem. We show that via control of plasma dynamics by managing laser polarization, it is possible to gate an intense single attosecond pulse with high ellipticity extending to the soft X-ray regime at oblique incidence. This approach thus paves the way towards a powerful tool enabling high-time-resolution probe of dynamics of chiral systems and magnetic materials with current laser technology.

Ultrafast High Harmonic, Soft X-Ray Probing of Molecular Dynamics

DTIC Science & Technology

2009-12-16

12. D. G. Lappas and A. L’Huillier, "Generation of attosecond XUV pulses in strong laser-atom interactions," Phys. Rev. A 58, 4140 (1998). 13...presentation at the 37 th AIAA/ASME/ SAE /ASEE Joint Propulsion Conference and Exhibition, Salt Lake City, UT, p. 3937 (2001). 36. A. Bultel, B. G

Harmonium: An Ultrafast Vacuum Ultraviolet Facility.

PubMed

Arrell, Christopher A; Ojeda, José; Longetti, Luca; Crepaldi, Alberto; Roth, Silvan; Gatti, Gianmarco; Clark, Andrew; van Mourik, Frank; Drabbels, Marcel; Grioni, Marco; Chergui, Majed

2017-05-31

Harmonium is a vacuum ultraviolet (VUV) photon source built within the Lausanne Centre for Ultrafast Science (LACUS). Utilising high harmonic generation, photons from 20-110 eV are available to conduct steady-state or ultrafast photoelectron and photoion spectroscopies (PES and PIS). A pulse preserving monochromator provides either high energy resolution (70 meV) or high temporal resolution (40 fs). Three endstations have been commissioned for: a) PES of liquids; b) angular resolved PES (ARPES) of solids and; c) coincidence PES and PIS of gas phase molecules or clusters. The source has several key advantages: high repetition rate (up to 15 kHz) and high photon flux (1011 photons per second at 38 eV). The capabilities of the facility complement the Swiss ultrafast and X-ray community (SwissFEL, SLS, NCCR MUST, etc.) helping to maintain Switzerland's leading role in ultrafast science in the world.

X-Ray Sum Frequency Diffraction for Direct Imaging of Ultrafast Electron Dynamics

NASA Astrophysics Data System (ADS)

Rouxel, Jérémy R.; Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

2018-06-01

X-ray diffraction from molecules in the ground state produces an image of their charge density, and time-resolved x-ray diffraction can thus monitor the motion of the nuclei. However, the density change of excited valence electrons upon optical excitation can barely be monitored with regular diffraction techniques due to the overwhelming background contribution of the core electrons. We present a nonlinear x-ray technique made possible by novel free electron laser sources, which provides a spatial electron density image of valence electron excitations. The technique, sum frequency generation carried out with a visible pump and a broadband x-ray diffraction pulse, yields snapshots of the transition charge densities, which represent the electron density variations upon optical excitation. The technique is illustrated by ab initio simulations of transition charge density imaging for the optically induced electronic dynamics in a donor or acceptor substituted stilbene.

Massively parallel X-ray holography

NASA Astrophysics Data System (ADS)

Marchesini, Stefano; Boutet, Sébastien; Sakdinawat, Anne E.; Bogan, Michael J.; Bajt, Saša; Barty, Anton; Chapman, Henry N.; Frank, Matthias; Hau-Riege, Stefan P.; Szöke, Abraham; Cui, Congwu; Shapiro, David A.; Howells, Malcolm R.; Spence, John C. H.; Shaevitz, Joshua W.; Lee, Joanna Y.; Hajdu, Janos; Seibert, Marvin M.

2008-09-01

Advances in the development of free-electron lasers offer the realistic prospect of nanoscale imaging on the timescale of atomic motions. We identify X-ray Fourier-transform holography as a promising but, so far, inefficient scheme to do this. We show that a uniformly redundant array placed next to the sample, multiplies the efficiency of X-ray Fourier transform holography by more than three orders of magnitude, approaching that of a perfect lens, and provides holographic images with both amplitude- and phase-contrast information. The experiments reported here demonstrate this concept by imaging a nano-fabricated object at a synchrotron source, and a bacterial cell with a soft-X-ray free-electron laser, where illumination by a single 15-fs pulse was successfully used in producing the holographic image. As X-ray lasers move to shorter wavelengths we expect to obtain higher spatial resolution ultrafast movies of transient states of matter.

Generation of Gigawatt Circularly Polarized Attosecond-Pulse Pairs

NASA Astrophysics Data System (ADS)

Hu, K.; Wu, H.-C.

2017-12-01

A novel scheme for generating a pair of gigawatt attosecond pulses by coherent Thomson scattering from relativistic electron sheets is proposed. With a circularly polarized relativistic laser pulse, the scattered x-ray signal can have a saddlelike temporal profile, where the lower electromagnetic frequencies are found mostly in the center region of this saddlelike profile. By filtering out the latter, we can obtain two few-attosecond pulses separated by a subfemtosecond interval, which is tunable by controlling the energy of the sheet electrons. Such a pulse pair can be useful for an attosecond pump probe at an unprecedented time resolution and for ultrafast chiral studies in molecules and materials.

Simulation studies of a XUV/soft X-ray harmonic-cascade FEL for the proposed LBNL recirculating linac*

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fawley, W.M.; Barletta, W.A.; Corlett, J.N.

Presently there is significant interest at LBNL in designing and building a facility for ultrafast (i.e. femtosecond time scale) x-ray science based upon a superconducting, recirculating RF linac (see Corlett et al. for more details). In addition to producing synchrotron radiation pulses in the 1-15 keV energy range, we are also considering adding one or more free-electron laser (FEL) beamlines using a harmonic cascade approach to produce coherent XUV soft X-ray emission beginning with a strong input seed at {approx}200 nm wavelength obtained from a ''conventional'' laser. Each cascade is composed of a radiator together with a modulator section, separatedmore » by a magnetic chicane. The chicane temporally delays the electron beam pulse in order that a ''virgin'' pulse region (with undegraded energy spread) be brought into synchronism with the radiation pulse, which together then undergo FEL action in the modulator. We present various results obtained with the GINGER simulation code examining final output sensitivity to initial electron beam parameters. We also discuss the effects of spontaneous emission and shot noise upon this particular cascade approach which can limit the final output coherence.« less

PLEIADES: High Peak Brightness, Subpicosecond Thomson Hard-X-ray source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kuba, J; Anderson, S G; Barty, C J

2003-12-15

The Picosecond Laser-Electron Inter-Action for the Dynamic Evaluation of Structures (PLEIADES) facility, is a unique, novel, tunable (10-200 keV), ultrafast (ps-fs), hard x-ray source that greatly extends the parameter range reached by existing 3rd generation sources, both in terms of x-ray energy range, pulse duration, and peak brightness at high energies. First light was observed at 70 keV early in 2003, and the experimental data agrees with 3D codes developed at LLNL. The x-rays are generated by the interaction of a 50 fs Fourier-transform-limited laser pulse produced by the TW-class FALCON CPA laser and a highly focused, relativistic (20-100 MeV),more » high brightness (1 nC, 0.3-5 ps, 5 mm.mrad, 0.2% energy spread) photo-electron bunch. The resulting x-ray brightness is expected to exceed 10{sup 20} ph/mm{sup 2}/s/mrad{sup 2}/0.1% BW. The beam is well-collimated (10 mrad divergence over the full spectrum, 1 mrad for a single color), and the source is a unique tool for time-resolved dynamic measurements in matter, including high-Z materials.« less

AXSIS: Exploring the frontiers in attosecond X-ray science, imaging and spectroscopy.

PubMed

Kärtner, F X; Ahr, F; Calendron, A-L; Çankaya, H; Carbajo, S; Chang, G; Cirmi, G; Dörner, K; Dorda, U; Fallahi, A; Hartin, A; Hemmer, M; Hobbs, R; Hua, Y; Huang, W R; Letrun, R; Matlis, N; Mazalova, V; Mücke, O D; Nanni, E; Putnam, W; Ravi, K; Reichert, F; Sarrou, I; Wu, X; Yahaghi, A; Ye, H; Zapata, L; Zhang, D; Zhou, C; Miller, R J D; Berggren, K K; Graafsma, H; Meents, A; Assmann, R W; Chapman, H N; Fromme, P

2016-09-01

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser-, accelerator,- X-ray scientists as well as spectroscopists and biochemists optimizes X-ray pulse parameters, in tandem with sample delivery, crystal size, and advanced X-ray detectors. Ultimately, the new capability, attosecond serial X-ray crystallography and spectroscopy, will be applied to one of the most important problems in structural biology, which is to elucidate the dynamics of light reactions, electron transfer and protein structure in photosynthesis.

An ultrafast X-ray scintillating detector made of ZnO(Ga)

NASA Astrophysics Data System (ADS)

Zhang, Qingmin; Yan, Jun; Deng, Bangjie; Zhang, Jingwen; Lv, Jinge; Wen, Xin; Gao, Keqing

2017-12-01

Owing to its ultrafast scintillation, quite high light yield, strong radiation resistance, and non-deliquescence, ZnO(Ga) is a highly promising choice for an ultrafast X-ray detector. Because of its high deposition rate, good production repeatability and strong adhesive force, reactive magnetron sputtering was used to produce a ZnO(Ga) crystal on a quartz glass substrate, after the production conditions were optimized. The fluorescence lifetime of the sample was 173 ps. An ultrafast X-ray scintillating detector, equipped with a fast microchannel plate (MCP) photomultiplier tube (PMT), was developed and the X-ray tests show a signal full width at half maximum (FWHM) of only 385.5 ps. Moreover, derivation from the previous measurement shows the ZnO(Ga) has an ultrafast time response (FWHM = 355.1 ps) and a high light yield (14740 photons/MeV).

Intense γ ray generated by refocusing laser pulse on wakefield accelerated electrons

NASA Astrophysics Data System (ADS)

Feng, Jie; Wang, Jinguang; Li, Yifei; Zhu, Changqing; Li, Minghua; He, Yuhang; Li, Dazhang; Wang, Weimin; Chen, Liming

2017-09-01

Ultrafast x/γ ray emission from the combination of laser wake-field acceleration and plasma mirror has been investigated as a promising Thomson scattering source. However, the photon energy and yield of radiation are limited to the intensity of reflected laser pulses. We use the 2D particle in cell simulation to demonstrate that a 75TW driven laser pulse can be refocused on the accelerated electron bunches through a hemispherical plasma mirror with a small f number of 0.25. The energetic electrons with the maximum energy about 350 MeV collide with the reflected laser pulse of a0 = 3.82 at the focal spot, producing high order multi-photon Thomson scattering, and resulting in the scattering spectrum which extends up to 21.2 MeV. Such a high energy γ ray source could be applied to photonuclear reaction and materials science.

A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography

DOE Office of Scientific and Technical Information (OSTI.GOV)

van Thor, Jasper J.; Madsen, Anders

In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or “probe-pump-probe”) which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF,more » in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse.« less

A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography

DOE PAGES

van Thor, Jasper J.; Madsen, Anders

2015-01-01

In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or “probe-pump-probe”) which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF,more » in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse.« less

A split-beam probe-pump-probe scheme for femtosecond time resolved protein X-ray crystallography

PubMed Central

van Thor, Jasper J.; Madsen, Anders

2015-01-01

In order to exploit the femtosecond pulse duration of X-ray Free-Electron Lasers (XFEL) operating in the hard X-ray regime for ultrafast time-resolved protein crystallography experiments, critical parameters that determine the crystallographic signal-to-noise (I/σI) must be addressed. For single-crystal studies under low absorbed dose conditions, it has been shown that the intrinsic pulse intensity stability as well as mode structure and jitter of this structure, significantly affect the crystallographic signal-to-noise. Here, geometrical parameters are theoretically explored for a three-beam scheme: X-ray probe, optical pump, X-ray probe (or “probe-pump-probe”) which will allow experimental determination of the photo-induced structure factor amplitude differences, ΔF, in a ratiometric manner, thereby internally referencing the intensity noise of the XFEL source. In addition to a non-collinear split-beam geometry which separates un-pumped and pumped diffraction patterns on an area detector, applying an additional convergence angle to both beams by focusing leads to integration over mosaic blocks in the case of well-ordered stationary protein crystals. Ray-tracing X-ray diffraction simulations are performed for an example using photoactive yellow protein crystals in order to explore the geometrical design parameters which would be needed. The specifications for an X-ray split and delay instrument that implements both an offset angle and focused beams are discussed, for implementation of a probe-pump-probe scheme at the European XFEL. We discuss possible extension of single crystal studies to serial femtosecond crystallography, particularly in view of the expected X-ray damage and ablation due to the first probe pulse. PMID:26798786

Anisotropy enhanced X-ray scattering from solvated transition metal complexes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Biasin, Elisa; van Driel, Tim B.; Levi, Gianluca

Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolvedmore » X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. Here it is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute,i.e.the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.« less

Anisotropy enhanced X-ray scattering from solvated transition metal complexes

DOE PAGES

Biasin, Elisa; van Driel, Tim B.; Levi, Gianluca; ...

2018-02-13

Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolvedmore » X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. Here it is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute,i.e.the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.« less

Femtosecond X-ray Diffraction From Two-Dimensional Protein Crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frank, Matthias; Carlson, David B.; Hunter, Mark

2014-02-28

Here we present femtosecond x-ray diffraction patterns from two-dimensional (2-D) protein crystals using an x-ray free electron laser (XFEL). To date it has not been possible to acquire x-ray diffraction from individual 2-D protein crystals due to radiation damage. However, the intense and ultrafast pulses generated by an XFEL permits a new method of collecting diffraction data before the sample is destroyed. Utilizing a diffract-before-destroy methodology at the Linac Coherent Light Source, we observed Bragg diffraction to better than 8.5 Å resolution for two different 2-D protein crystal samples that were maintained at room temperature. These proof-of-principle results show promisemore » for structural analysis of both soluble and membrane proteins arranged as 2-D crystals without requiring cryogenic conditions or the formation of three-dimensional crystals.« less

Science at the Time-scale of the Electron

NASA Astrophysics Data System (ADS)

Murnane, Margaret

2010-03-01

Replace this text with your abstract Ever since the invention of the laser 50 years ago and its application in nonlinear optics, scientists have been striving to extend coherent laser beams into the x-ray region of the spectrum. Very recently however, the prospects for tabletop coherent sources, with attosecond pulse durations, at very short wavelengths even in the hard x-ray region of the spectrum at wavelengths < 1nm, have brightened considerably. These advances are possible by taking nonlinear optics techniques to an extreme, and are the direct result of a new ability to manipulate electrons on the fastest, attosecond, time-scales of our natural world. My talk will discuss new experimental data that demonstrates high harmonic generation of laser-like, fully coherent, 10 attosecond duration, soft x-ray beams at photon energies around 0.5keV. Several applications will also be discussed, including making a movie of how electron orbitals in a molecule change shape as a molecule breaks apart, following how fast a magnetic material can flip orientation, understanding how fast heat flows in a nanocircuit, or building a microscope without lenses. [4pt] [1] T. Popmintchev et al., ``Phase matched upconversion of coherent ultrafast laser light into the soft and hard x-ray regions of the spectrum'', PNAS 106, 10516 (2009). [0pt] [2] C. LaOVorakiat et al., ``Ultrafast Soft X-Ray Magneto-Optics at the M-edge Using a Tabletop High-Harmonic Source'', Physical Review Letters 103, 257402 (2009). [0pt] [3] M. Siemens et al. ``Measurement of quasi-ballistic heat transport across nanoscale interfaces using ultrafast coherent soft x-ray beams'', Nature Materials 9, 26 (2010). [0pt] [4] K. Raines et al., ``Three-dimensional structure determination from a single view,'' Nature 463, 214 (2010). [0pt] [5] W. Li et al., ``Time-resolved Probing of Dynamics in Polyatomic Molecules using High Harmonic Generation'', Science 322, 1207 (2008).

Advanced Instrumentation for Ultrafast Science at the LCLS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berrah, Nora

2015-10-13

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

Photoinduced coherent acoustic phonon dynamics inside Mott insulator Sr2IrO4 films observed by femtosecond X-ray pulses

NASA Astrophysics Data System (ADS)

Zhang, Bing-Bing; Liu, Jian; Wei, Xu; Sun, Da-Rui; Jia, Quan-Jie; Li, Yuelin; Tao, Ye

2017-04-01

We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 film by femtosecond X-ray diffraction using a laser plasma-based X-ray source. The ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of (0012) Bragg diffraction after excitation by 1.5 eV and 3.0 eV pump photons for films with different thicknesses. The observed transient lattice response can be well interpreted as a distinct three-step dynamics due to the propagation of coherent acoustic phonons generated by photoinduced quasiparticles (QPs). Employing a normalized phonon propagation model, we found that the photoinduced angular shifts of the Bragg peak collapse into a universal curve after introducing normalized coordinates to account for different thicknesses and pump photon energies, pinpointing the origin of the lattice distortion and its early evolution. In addition, a transient photocurrent measurement indicates that the photoinduced QPs are charge neutral excitons. Mapping the phonon propagation and correlating its dynamics with the QP by ultrafast X-ray diffraction (UXRD) establish a powerful way to study electron-phonon coupling and uncover the exotic physics in strongly correlated systems under nonequilibrium conditions.

High flux table-top ultrafast soft X-ray source generated by high harmonic generation

NASA Astrophysics Data System (ADS)

Thiré, Nicolas; Schmidt, Bruno E.; Fourmeaux, Sylvain; Beaulieu, Samuel; Cardin, Vincent; Negro, Matteo; Kieffer, Jean-Claude; Vozzi, Caterina; Legare, François

2014-05-01

Generation of ultrafast soft X-ray pulses is a major challenge for conventional laboratories. Using the process of HHG enables generation of such short wavelength photons. Intense laser sources in the infrared are necessary to reach the soft X-ray spectral range as the HHG cut-off scales with Iλ2. However, in the limit of the single atom response, increasing the laser wavelength leads to a significant decrease of the HHG flux. To compensate, one has to increase the number of emitters with high ionization potential. At the Advanced Laser Light Source, we have addressed this challenge by using a new gas cell design and developing a 10 mJ - 30 fs source at 1.8 μm. Using this setup, we have been able to generate harmonics in the water window spectral range for neon and helium with short time duration (<30 fs) in a conventional laboratory. A flux measurement has been performed showing ~ 2 × 105 photons/shot between 280 and 540 eV, making it possible to see the carbon k-edge at 280eV in a single shot manner. This soft X-ray beam is also extremely well collimated (0.1 mrad) making it this table-top beamline ideal for a number of applications.

kW picosecond thin-disk regenerative amplifier

NASA Astrophysics Data System (ADS)

Michel, Knut; Wandt, Christoph; Klingebiel, Sandro; Schultze, Marcel; Prinz, Stephan; Teisset, Catherine Y.; Stark, Sebastian; Grebing, Christian; Bessing, Robert; Herzig, Tobias; Häfner, Matthias; Budnicki, Aleksander; Sutter, Dirk; Metzger, Thomas

2018-02-01

TRUMPF Scientific Lasers provides ultrafast laser sources for the scientific community with high pulse energies and high average power. All systems are based on the industrialized TRUMPF thin-disk technology. Regenerative amplifiers systems with multi-millijoule pulses, kilohertz repetition rates and picosecond pulse durations are available. Record values of 220mJ at 1kHz could be demonstrated originally developed for pumping optical parametric amplifiers. The ultimate goal is to combine high energies, <100mJ per pulse, with average powers of several hundred watts to a kilowatt. Based on a regenerative amplifier containing two Ytterbium doped thin-disks operated at ambient temperature pulses with picosecond duration and more than 100mJ could be generated at a repetition rate of 10kHz reaching 1kW of average output power. This system is designed to operate at different repetition rates from 100kHz down to 5kHz so that even higher pulse energies can be reached. This type of ultrafast sources uncover new application fields in science. Laser based lightning rods, X-ray lasers and Compton backscatter sources are among them.

Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source

DOE PAGES

Alonso-Mori, Roberto; Sokaras, Dimosthenis; Zhu, Diling; ...

2015-04-15

X-ray free-electron lasers (FELs) have opened unprecedented possibilities to study the structure and dynamics of matter at an atomic level and ultra-fast timescale. Many of the techniques routinely used at storage ring facilities are being adapted for experiments conducted at FELs. In order to take full advantage of these new sources several challenges have to be overcome. They are related to the very different source characteristics and its resulting impact on sample delivery, X-ray optics, X-ray detection and data acquisition. Here it is described how photon-in photon-out hard X-ray spectroscopy techniques can be applied to study the electronic structure andmore » its dynamics of transition metal systems with ultra-bright and ultra-short FEL X-ray pulses. In particular, some of the experimental details that are different compared with synchrotron-based setups are discussed and illustrated by recent measurements performed at the Linac Coherent Light Source.« less

Ultrahigh resolution and brilliance laser wakefield accelerator betatron x-ray source for rapid in vivo tomographic microvasculature imaging in small animal models

NASA Astrophysics Data System (ADS)

Fourmaux, Sylvain; Kieffer, Jean-Claude; Krol, Andrzej

2017-03-01

We are developing ultrahigh spatial resolution (FWHM < 2 μm) high-brilliance x-ray source for rapid in vivo tomographic microvasculature imaging micro-CT angiography (μCTA) in small animal models using optimized contrast agent. It exploits Laser Wakefield Accelerator (LWFA) betatron x-ray emission phenomenon. Ultrashort high-intensity laser pulse interacting with a supersonic gas jet produces an ion cavity ("bubble") in the plasma in the wake of the laser pulse. Electrons that are injected into this bubble gain energy, perform wiggler-like oscillations and generate burst of incoherent x-rays with characteristic duration time comparable to the laser pulse duration, continuous synchrotron-like spectral distribution that might extend to hundreds keV, very high brilliance, very small focal spot and highly directional emission in the cone-beam geometry. Such LWFA betatron x-ray source created in our lab produced 1021 -1023 photonsṡ shot-1ṡmrad-2ṡmm-2/0.1%bw with mean critical energy in the12-30 keV range. X-ray source size for a single laser shot was FWHM=1.7 μm x-ray beam divergence 20-30 mrad, and effective focal spot size for multiple shots FWHM= 2 μm. Projection images of simple phantoms and complex biological objects including insects and mice were obtained in single laser shots. We conclude that ultrahigh spatial resolution μCTA (FWHM 2 μm) requiring thousands of projection images could be accomplished using LWFA betatron x-ray radiation in approximately 40 s with our existing 220 TW laser and sub seconds with next generation of ultrafast lasers and x-ray detectors, as opposed to several hours required using conventional microfocal x-ray tubes. Thus, sub second ultrahigh resolution in vivo microtomographic microvasculature imaging (in both absorption and phase contrast mode) in small animal models of cancer and vascular diseases will be feasible with LWFA betatron x-ray source.

Strong-Field Driven Dynamics of Metal and Dielectric Nanoparticles

NASA Astrophysics Data System (ADS)

Powell, Jeffrey

The motion of electrons in atoms, molecules, and solids in the presence of intense electromagnetic radiation is an important research topic in physics and physical chemistry because of its fundamental nature and numerous practical applications, ranging from precise machining of materials to optical control of chemical reactions and light-driven electronic devices. Mechanisms of light-matter interactions critically depend on the dimensions of the irradiated system and evolve significantly from single atoms or molecules to the macroscopic bulk. Nanoparticles provide the link between these two extremes. In this thesis, I take advantage of this bridge to study light-matter interactions as a function of nanoparticle size, shape, and composition. I present here three discrete, but interconnected, experiments contributing to our knowledge of nanoparticle properties and their response to intense, short-pulsed light fields. First, I investigate how individual nanoparticles interact with each other in solution, studying their temperature-dependent solubility. The interaction potential between 5.5nm gold nanoparticles, ligated by an alkanethiol was found to be -0.165eV, in reasonable agreement with a phenomenological model. The other two experiments explore ultrafast dynamics driven by intense femtosecond lasers in isolated, gas-phase metallic and dielectric nanoparticles. Photoelectron momentum imaging is applied to study the response of gold, silica, and gold-shell/silica-core nanoparticles (ranging from single to several hundred nanometers in size) with near-infrared (NIR), 25 fs laser pulses in the intensity range of 1011 - 1014 W/cm2. These measurements, which constitute the bulk of my graduate work, reveal the complex interplay between the external optical field and the induced near-field of the nanoparticle, resulting in the emission of very energetic electrons that are much faster than those emitted from isolated atoms or molecules exposed to the same light pulses. The highest photoelectron energies ("cutoffs") were measured as a function of laser intensity, nanoparticle material and size. We found that the energy cutoffs increase monotonically with laser intensity and nanoparticle size, except for the gold/silica hybrid where the plasmon resonance response modifies this behavior at low intensities. The measured photoelectron spectra for metallic nanoparticles display a large energy enhancement over silica. Finally, the last part of this thesis explores the possibility to apply time-resolved x-ray scattering as a probe of the ultrafast dynamics in isolated nanoparticles driven by very intense ( 1015 W/cm2) NIR laser radiation. To do this, I developed and built a nanoparticle source capable of injecting single, gas-phase nanoparticles with a narrow size distribution into the laser focus. We used femtosecond x-ray pulses from an x-ray free electron laser (XFEL) to map the evolution of the laser-irradiated nanoparticle. The ultrafast dynamics were observed in the single-shot x-ray diffraction patterns measured as a function of delay between the NIR and x-ray pulses, which allows for femtosecond temporal and nanometer spatial resolution. We found that the intense IR laser pulse rapidly ionizes the nanoparticle, effectively turning it into a nanoplasma within less than a picosecond, and observed signatures of the nanoparticle surface softening on a few hundred-femtosecond time scale.

Time zero determination for FEL pump-probe studies based on ultrafast melting of bismuth.

PubMed

Epp, S W; Hada, M; Zhong, Y; Kumagai, Y; Motomura, K; Mizote, S; Ono, T; Owada, S; Axford, D; Bakhtiarzadeh, S; Fukuzawa, H; Hayashi, Y; Katayama, T; Marx, A; Müller-Werkmeister, H M; Owen, R L; Sherrell, D A; Tono, K; Ueda, K; Westermeier, F; Miller, R J D

2017-09-01

A common challenge for pump-probe studies of structural dynamics at X-ray free-electron lasers (XFELs) is the determination of time zero (T 0 )-the time an optical pulse (e.g., an optical laser) arrives coincidently with the probe pulse (e.g., a XFEL pulse) at the sample position. In some cases, T 0 might be extracted from the structural dynamics of the sample's observed response itself, but generally, an independent robust method is required or would be superior to the inferred determination of T 0 . In this paper, we present how the structural dynamics in ultrafast melting of bismuth can be exploited for a quickly performed, reliable and accurate determination of T 0 with a precision below 20 fs and an overall experimental accuracy of 50 fs to 150 fs (estimated). Our approach is potentially useful and applicable for fixed-target XFEL experiments, such as serial femtosecond crystallography, utilizing an optical pump pulse in the ultraviolet to near infrared spectral range and a pixelated 2D photon detector for recording crystallographic diffraction patterns in transmission geometry. In comparison to many other suitable approaches, our method is fairly independent of the pumping wavelength (UV-IR) as well as of the X-ray energy and offers a favorable signal contrast. The technique is exploitable not only for the determination of temporal characteristics of the experiment at the interaction point but also for investigating important conditions affecting experimental control such as spatial overlap and beam spot sizes.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua

NASA Astrophysics Data System (ADS)

Popmintchev, Dimitar; Galloway, Benjamin R.; Chen, Ming-Chang; Dollar, Franklin; Mancuso, Christopher A.; Hankla, Amelia; Miaja-Avila, Luis; O'Neil, Galen; Shaw, Justin M.; Fan, Guangyu; Ališauskas, Skirmantas; Andriukaitis, Giedrius; Balčiunas, Tadas; Mücke, Oliver D.; Pugzlys, Audrius; Baltuška, Andrius; Kapteyn, Henry C.; Popmintchev, Tenio; Murnane, Margaret M.

2018-03-01

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV . Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K - and L -absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 109 photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 1026 photons/s /mrad2/mm2/1 % bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

Ultrafast X-Ray Absorption Spectroscopy of Isochorically Heated Warm Dense Matter

NASA Astrophysics Data System (ADS)

Engelhorn, Kyle Craig

This dissertation will present a series of new tools, together with new techniques, focused on the understanding of warm and dense matter. We report on the development of a high time resolution and high detection efficiency x-ray camera. The camera is integrated with a short pulse laser and an x-ray beamline at the Advanced Light Source synchrotron. This provides an instrument for single shot, broadband x-ray absorption spectroscopy of warm and dense matter with 2 picosecond time resolution. Warm and dense matter is created by isochorically heating samples of known density with an ultrafast optical laser pulse, and X-ray absorption spectroscopy probes the unoccupied electronic density of states before the onset of hydrodynamic expansion and electron-ion equilibrium is reached. Measured spectra from a variety of materials are compared with first principle molecular dynamics and density functional theory calculations. In heated silicon dioxide spectra, two novel pre-edge features are observed, a peak below the band gap and absorption within the band gap, while a reduction was observed in the features above the edge. From consideration of the calculated spectra, the peak below the gap is attributed to valence electrons that have been promoted to the conduction band, the absorption within the gap is attributed to broken Si-O bonds, and the reduction above the edge is attributed to an elevated ionic temperature. In heated copper spectra, a time-dependent shift and broadening of the absorption edge are observed, consistent with and elevated electron temperature. The temporal evolution of the electronic temperature is accurately determined by fitting the measured spectra with calculated spectra. The electron-ion equilibration is studied with a two-temperature model. In heated nickel spectra, a shift of the absorption edge is observed. This shift is found to be inconsistent with calculated spectra and independent of incident laser fluence. A shift of the chemical potential is applied to the calculated spectra to obtain satisfactory agreement with measured spectra.

Simulations of ultrafast x-ray laser experiments

NASA Astrophysics Data System (ADS)

Fortmann-Grote, C.; Andreev, A. A.; Appel, K.; Branco, J.; Briggs, R.; Bussmann, M.; Buzmakov, A.; Garten, M.; Grund, A.; Huebl, A.; Jurek, Z.; Loh, N. D.; Nakatsutsumi, M.; Samoylova, L.; Santra, R.; Schneidmiller, E. A.; Sharma, A.; Steiniger, K.; Yakubov, S.; Yoon, C. H.; Yurkov, M. V.; Zastrau, U.; Ziaja-Motyka, B.; Mancuso, A. P.

2017-06-01

Simulations of experiments at modern light sources, such as optical laser laboratories, synchrotrons, and free electron lasers, become increasingly important for the successful preparation, execution, and analysis of these experiments investigating ever more complex physical systems, e.g. biomolecules, complex materials, and ultra-short lived states of matter at extreme conditions. We have implemented a platform for complete start-to-end simulations of various types of photon science experiments, tracking the radiation from the source through the beam transport optics to the sample or target under investigation, its interaction with and scattering from the sample, and registration in a photon detector. This tool allows researchers and facility operators to simulate their experiments and instruments under real life conditions, identify promising and unattainable regions of the parameter space and ultimately make better use of valuable beamtime. In this paper, we present an overview about status and future development of the simulation platform and discuss three applications: 1.) Single-particle imaging of biomolecules using x-ray free electron lasers and optimization of x-ray pulse properties, 2.) x-ray scattering diagnostics of hot dense plasmas in high power laser-matter interaction and identification of plasma instabilities, and 3.) x-ray absorption spectroscopy in warm dense matter created by high energy laser-matter interaction and pulse shape optimization for low-isentrope dynamic compression.

Attosecond Thomson-scattering x-ray source driven by laser-based electron acceleration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Luo, W.; College of Science, National University of Defense Technology, Changsha 410073; Zhuo, H. B.

2013-10-21

The possibility of producing attosecond x-rays through Thomson scattering of laser light off laser-driven relativistic electron beams is investigated. For a ≤200-as, tens-MeV electron bunch produced with laser ponderomotive-force acceleration in a plasma wire, exceeding 10{sup 6} photons/s in the form of ∼160 as pulses in the range of 3–300 keV are predicted, with a peak brightness of ≥5 × 10{sup 20} photons/(s mm{sup 2} mrad{sup 2} 0.1% bandwidth). Our study suggests that the physical scheme discussed in this work can be used for an ultrafast (attosecond) x-ray source, which is the most beneficial for time-resolved atomic physics, dubbed “attosecondmore » physics.”.« less

Imaging single cells in a beam of live cyanobacteria with an X-ray laser.

PubMed

van der Schot, Gijs; Svenda, Martin; Maia, Filipe R N C; Hantke, Max; DePonte, Daniel P; Seibert, M Marvin; Aquila, Andrew; Schulz, Joachim; Kirian, Richard; Liang, Mengning; Stellato, Francesco; Iwan, Bianca; Andreasson, Jakob; Timneanu, Nicusor; Westphal, Daniel; Almeida, F Nunes; Odic, Dusko; Hasse, Dirk; Carlsson, Gunilla H; Larsson, Daniel S D; Barty, Anton; Martin, Andrew V; Schorb, Sebastian; Bostedt, Christoph; Bozek, John D; Rolles, Daniel; Rudenko, Artem; Epp, Sascha; Foucar, Lutz; Rudek, Benedikt; Hartmann, Robert; Kimmel, Nils; Holl, Peter; Englert, Lars; Duane Loh, Ne-Te; Chapman, Henry N; Andersson, Inger; Hajdu, Janos; Ekeberg, Tomas

2015-02-11

There exists a conspicuous gap of knowledge about the organization of life at mesoscopic levels. Ultra-fast coherent diffractive imaging with X-ray free-electron lasers can probe structures at the relevant length scales and may reach sub-nanometer resolution on micron-sized living cells. Here we show that we can introduce a beam of aerosolised cyanobacteria into the focus of the Linac Coherent Light Source and record diffraction patterns from individual living cells at very low noise levels and at high hit ratios. We obtain two-dimensional projection images directly from the diffraction patterns, and present the results as synthetic X-ray Nomarski images calculated from the complex-valued reconstructions. We further demonstrate that it is possible to record diffraction data to nanometer resolution on live cells with X-ray lasers. Extension to sub-nanometer resolution is within reach, although improvements in pulse parameters and X-ray area detectors will be necessary to unlock this potential.

Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL

PubMed Central

Obara, Yuki; Ito, Hironori; Ito, Terumasa; Kurahashi, Naoya; Thürmer, Stephan; Tanaka, Hiroki; Katayama, Tetsuo; Togashi, Tadashi; Owada, Shigeki; Yamamoto, Yo-ichi; Karashima, Shutaro; Nishitani, Junichi; Yabashi, Makina; Suzuki, Toshinori; Misawa, Kazuhiko

2017-01-01

The charge-carrier dynamics of anatase TiO2 nanoparticles in an aqueous solution were studied by femtosecond time-resolved X-ray absorption spectroscopy using an X-ray free electron laser in combination with a synchronized ultraviolet femtosecond laser (268 nm). Using an arrival time monitor for the X-ray pulses, we obtained a temporal resolution of 170 fs. The transient X-ray absorption spectra revealed an ultrafast Ti K-edge shift and a subsequent growth of a pre-edge structure. The edge shift occurred in ca. 100 fs and is ascribed to reduction of Ti by localization of generated conduction band electrons into shallow traps of self-trapped polarons or deep traps at penta-coordinate Ti sites. Growth of the pre-edge feature and reduction of the above-edge peak intensity occur with similar time constants of 300–400 fs, which we assign to the structural distortion dynamics near the surface. PMID:28713842

A high-resolving-power x-ray spectrometer for the OMEGA EP Laser (invited)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nilson, P. M., E-mail: pnil@lle.rochester.edu; Ehrne, F.; Mileham, C.

A high-resolving-power x-ray spectrometer has been developed for the OMEGA EP Laser System based on a spherically bent Si [220] crystal with a radius of curvature of 330 mm and a Spectral Instruments (SI) 800 Series charge-coupled device. The instrument measures time-integrated x-ray emission spectra in the 7.97- to 8.11-keV range, centered on the Cu K{sub α1} line. To demonstrate the performance of the spectrometer under high-power conditions, K{sub α1,2} emission spectra were measured from Cu foils irradiated by the OMEGA EP laser with 100-J, 1-ps pulses at focused intensities above 10{sup 18} W/cm{sup 2}. The ultimate goal is tomore » couple the spectrometer to a picosecond x-ray streak camera and measure temperature-equilibration dynamics inside rapidly heated materials. The plan for these ultrafast streaked x-ray spectroscopy studies is discussed.« less

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE PAGES

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung; ...

2017-05-24

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Characteristics of soft x-ray spectra from ultra-fast micro-capillary discharge plasmas

NASA Astrophysics Data System (ADS)

Li, Jing; Avaria, Gonzalo; Shlyaptsev, Vyacheslav; Tomasel, Fernando; Grisham, Michael; Dawson, Quincy; Rocca, Jorge; NSF CenterExtreme Ultraviolet Science; Technology Collaboration

2013-10-01

The efficient generation of high aspect ratio (e.g. 300:1) plasma columns ionized to very high degrees of ionization (e.g. Ni-like Xenon) by an ultrafast current pulses of moderate amplitude in micro-capillary channels is of interest for fundamental plasma studies and for applications such as the generation of discharge-pumped soft x-ray lasers. Spectra and simulations for plasmas generated in 500 um alumina capillary discharges driven by 35-40 kA current pulses with 4 ns rise time were obtained in Xenon and Neon discharges. The first shows the presence of lines corresponding to ionization stages up to Fe-like Xe. The latter show that Al impurities from the walls and Si (from injected SiH4) are ionized to the H-like and He-like stages. He-like spectra containing the resonance line significantly broaden by opacity, the intercombination line, and Li-like satellites are analyzed and modeled. For Xenon discharges, the spectral lines from the Ni-like transitions the 3d94d(3/2, 3/2)J=0 to the 3d94p(5/2, 3/2)J=1 and to 3d94p(3/2, 1/2)J=1 are observed at gas pressures up to 2.0 Torr. Work supported by NSF Award PHY-1004295.

600 eV falcon-linac thomson x-ray source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crane, J K; LeSage, G P; Ditmire, T

2000-12-15

The advent of 3rd generation light sources such as the Advanced Light Source (ALS) at LBL, and the Advanced Photon Source at Argonne, have produced a revolution in x-ray probing of dense matter during the past decade. These machines use electron-synchrotrons in conjunction with undulator stages to produce 100 psec x-ray pulses with photon energies of several kiloelectronvolts (keV). The applications for x-ray probing of matter are numerous and diverse with experiments in medicine and biology, semiconductors and materials science, and plasma and solid state physics. In spite of the success of the 3rd generation light sources there is strongmore » motivation to push the capabilities of x-ray probing into new realms, requiring shorter pulses, higher brightness and harder x-rays. A 4th generation light source, the Linac Coherent Light Source (LCLS), is being considered at the Stanford Linear Accelerator [1]. The LCLS will produce multi-kilovolt x-rays of subpicosecond duration that are 10 orders of magnitude brighter than today's 3rd generation light sources.[1] Although the LCLS will provide unprecedented capability for performing time-resolved x-ray probing of ultrafast phenomena at solid densities, this machine will not be completed for many years. In the meantime there is a serious need for an ultrashort-pulse, high-brightness, hard x-ray source that is capable of probing deep into high-Z solid materials to measure dynamic effects that occur on picosecond time scales. Such an instrument would be ideal for probing the effects of shock propagation in solids using Bragg and Laue diffraction. These techniques can be used to look at phase transitions, melting and recrystallization, and the propagation of defects and dislocations well below the surface in solid materials. [2] These types of dynamic phenomena undermine the mechanical properties of metals and are of general interest in solid state physics, materials science, metallurgy, and have specific relevance to stockpile stewardship. Another x-ray diagnostic technique, extended x-ray absorption fine structure (EXAFS) spectroscopy, can be used to measure small-scale structural changes to understand the underlying atomic physics associated with the formation of defects. [2]« less

Stochastic stimulated electronic x-ray Raman spectroscopy

PubMed Central

Kimberg, Victor; Rohringer, Nina

2016-01-01

Resonant inelastic x-ray scattering (RIXS) is a well-established tool for studying electronic, nuclear, and collective dynamics of excited atoms, molecules, and solids. An extension of this powerful method to a time-resolved probe technique at x-ray free electron lasers (XFELs) to ultimately unravel ultrafast chemical and structural changes on a femtosecond time scale is often challenging, due to the small signal rate in conventional implementations at XFELs that rely on the usage of a monochromator setup to select a small frequency band of the broadband, spectrally incoherent XFEL radiation. Here, we suggest an alternative approach, based on stochastic spectroscopy, which uses the full bandwidth of the incoming XFEL pulses. Our proposed method is relying on stimulated resonant inelastic x-ray scattering, where in addition to a pump pulse that resonantly excites the system a probe pulse on a specific electronic inelastic transition is provided, which serves as a seed in the stimulated scattering process. The limited spectral coherence of the XFEL radiation defines the energy resolution in this process and stimulated RIXS spectra of high resolution can be obtained by covariance analysis of the transmitted spectra. We present a detailed feasibility study and predict signal strengths for realistic XFEL parameters for the CO molecule resonantly pumped at the O1s→π* transition. Our theoretical model describes the evolution of the spectral and temporal characteristics of the transmitted x-ray radiation, by solving the equation of motion for the electronic and vibrational degrees of freedom of the system self consistently with the propagation by Maxwell equations. PMID:26958585

High-yield, ultrafast, surface plasmon-enhanced, Au nanorod optical field electron emitter arrays.

PubMed

Hobbs, Richard G; Yang, Yujia; Fallahi, Arya; Keathley, Philip D; De Leo, Eva; Kärtner, Franz X; Graves, William S; Berggren, Karl K

2014-11-25

Here we demonstrate the design, fabrication, and characterization of ultrafast, surface-plasmon enhanced Au nanorod optical field emitter arrays. We present a quantitative study of electron emission from Au nanorod arrays fabricated by high-resolution electron-beam lithography and excited by 35 fs pulses of 800 nm light. We present accurate models for both the optical field enhancement of Au nanorods within high-density arrays, and electron emission from those nanorods. We have also studied the effects of surface plasmon damping induced by metallic interface layers at the substrate/nanorod interface on near-field enhancement and electron emission. We have identified the peak optical field at which the electron emission mechanism transitions from a 3-photon absorption mechanism to strong-field tunneling emission. Moreover, we have investigated the effects of nanorod array density on nanorod charge yield, including measurement of space-charge effects. The Au nanorod photocathodes presented in this work display 100-1000 times higher conversion efficiency relative to previously reported UV triggered emission from planar Au photocathodes. Consequently, the Au nanorod arrays triggered by ultrafast pulses of 800 nm light in this work may outperform equivalent UV-triggered Au photocathodes, while also offering nanostructuring of the electron pulse produced from such a cathode, which is of interest for X-ray free-electron laser (XFEL) development where nanostructured electron pulses may facilitate more efficient and brighter XFEL radiation.

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays.

PubMed

Rudenko, A; Inhester, L; Hanasaki, K; Li, X; Robatjazi, S J; Erk, B; Boll, R; Toyota, K; Hao, Y; Vendrell, O; Bomme, C; Savelyev, E; Rudek, B; Foucar, L; Southworth, S H; Lehmann, C S; Kraessig, B; Marchenko, T; Simon, M; Ueda, K; Ferguson, K R; Bucher, M; Gorkhover, T; Carron, S; Alonso-Mori, R; Koglin, J E; Correa, J; Williams, G J; Boutet, S; Young, L; Bostedt, C; Son, S-K; Santra, R; Rolles, D

2017-06-01

X-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecular system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects-an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure-the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

DOE PAGES

Rudenko, A.; Inhester, L.; Hanasaki, K.; ...

2017-05-31

We report x-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecularmore » system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects—an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure—the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Fnally, our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.« less

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rudenko, A.; Inhester, L.; Hanasaki, K.

We report x-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 10 20 watts per square centimetre). However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption, which in a heteronuclear molecularmore » system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge. In serial femtosecond crystallography of biological objects—an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure—the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects and has been suggested as a way of phasing the diffraction data. On the basis of experiments using either soft or less-intense hard X-rays, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 10 20 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Fnally, our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.« less

RELATIVISTIC THOMSON SCATTERING EXPERIMENT AT BNL - STATUS REPORT.

DOE Office of Scientific and Technical Information (OSTI.GOV)

POGORELSKY,I.V.; BEN ZVI,I.; KUSCHE,K.

2001-12-03

1.7 x 10{sup 8} x-ray photons per 3.5 ps pulse have been produced in Thomson scattering by focusing CO{sub 2} laser pulse on counter-propagating relativistic electron beam. We explore a possibility of further enhancement of process efficiency by propagating both beams in a plasma capillary. Conventional synchrotron light sources based on using giga-electron-volt electron synchrotron accelerators and magnetic wigglers generate x-ray radiation for versatile application in multi-disciplinary research. An intense laser beam causes relativistic electron oscillations similar to a wiggler. However, because the laser wavelength is thousand times shorter than a wiggler period, very moderate electron energy is needed tomore » produce hard x-rays via Thomson scattering. This allows using relatively compact mega-electron-volt linear accelerators instead of giga-electron-volt synchrotrons. Another important advantage of Thomson sources is a possibility to generate femtosecond x-ray pulses whereas conventional synchrotron sources have typically {approx}300 ps pulse duration. This promises to revolutionize x-ray research in chemistry, physics, and biology expanding it to ultra-fast processes. Thomson sources do not compete in repetition rate and average intensity with conventional light sources that operate at the megahertz frequency. However, Thomson sources have a potential to produce much higher photon numbers per pulse. This may allow developing a single shot exposure important for structural analysis of live biological objects. The BNL Thomson source is a user's experiment conducted at the Accelerator Test Facility since 1998 by an international collaboration in High Energy Physics. Since inception, the ATF source produces the record peak x-ray yield, intensity and brightness among other similar proof-of-principle demonstrations attempted elsewhere. Note that this result is achieved with a moderate laser power of 15 GW. A key to this achievement is in choosing right apparatus and efficient interaction geometry. We use a CO{sub 2} laser that delivers 10 times more photons per unit energy than the 1-{micro}m laser, a high-brightness linac, and the most energy-efficient backscattering interaction geometry. The purpose of this report is to give an update on new results obtained during this year and our near-term plans.« less

Roadmap on ultrafast optics

NASA Astrophysics Data System (ADS)

Reid, Derryck T.; Heyl, Christoph M.; Thomson, Robert R.; Trebino, Rick; Steinmeyer, Günter; Fielding, Helen H.; Holzwarth, Ronald; Zhang, Zhigang; Del'Haye, Pascal; Südmeyer, Thomas; Mourou, Gérard; Tajima, Toshiki; Faccio, Daniele; Harren, Frans J. M.; Cerullo, Giulio

2016-09-01

The year 2015 marked the 25th anniversary of modern ultrafast optics, since the demonstration of the first Kerr lens modelocked Ti:sapphire laser in 1990 (Spence et al 1990 Conf. on Lasers and Electro-Optics, CLEO, pp 619-20) heralded an explosion of scientific and engineering innovation. The impact of this disruptive technology extended well beyond the previous discipline boundaries of lasers, reaching into biology labs, manufacturing facilities, and even consumer healthcare and electronics. In recognition of such a milestone, this roadmap on Ultrafast Optics draws together articles from some of the key opinion leaders in the field to provide a freeze-frame of the state-of-the-art, while also attempting to forecast the technical and scientific paradigms which will define the field over the next 25 years. While no roadmap can be fully comprehensive, the thirteen articles here reflect the most exciting technical opportunities presented at the current time in Ultrafast Optics. Several articles examine the future landscape for ultrafast light sources, from practical solid-state/fiber lasers and Raman microresonators to exotic attosecond extreme ultraviolet and possibly even zeptosecond x-ray pulses. Others address the control and measurement challenges, requiring radical approaches to harness nonlinear effects such as filamentation and parametric generation, coupled with the question of how to most accurately characterise the field of ultrafast pulses simultaneously in space and time. Applications of ultrafast sources in materials processing, spectroscopy and time-resolved chemistry are also discussed, highlighting the improvements in performance possible by using lasers of higher peak power and repetition rate, or by exploiting the phase stability of emerging new frequency comb sources.

Ultrahigh-speed X-ray imaging of hypervelocity projectiles

NASA Astrophysics Data System (ADS)

Miller, Stuart; Singh, Bipin; Cool, Steven; Entine, Gerald; Campbell, Larry; Bishel, Ron; Rushing, Rick; Nagarkar, Vivek V.

2011-08-01

High-speed X-ray imaging is an extremely important modality for healthcare, industrial, military and research applications such as medical computed tomography, non-destructive testing, imaging in-flight projectiles, characterizing exploding ordnance, and analyzing ballistic impacts. We report on the development of a modular, ultrahigh-speed, high-resolution digital X-ray imaging system with large active imaging area and microsecond time resolution, capable of acquiring at a rate of up to 150,000 frames per second. The system is based on a high-resolution, high-efficiency, and fast-decay scintillator screen optically coupled to an ultra-fast image-intensified CCD camera designed for ballistic impact studies and hypervelocity projectile imaging. A specially designed multi-anode, high-fluence X-ray source with 50 ns pulse duration provides a sequence of blur-free images of hypervelocity projectiles traveling at speeds exceeding 8 km/s (18,000 miles/h). This paper will discuss the design, performance, and high frame rate imaging capability of the system.

Imaging at an x-ray absorption edge using free electron laser pulses for interface dynamics in high energy density systems [Resonant phase contrast imaging for interface physics

DOE PAGES

Beckwith, M. A.; Jiang, S.; Schropp, A.; ...

2017-05-01

Tuning the energy of an x-ray probe to an absorption line or edge can provide material-specific measurements that are particularly useful for interfaces. Simulated hard x-ray images above the Fe K-edge are presented to examine ion diffusion across an interface between Fe 2O 3 and SiO 2 aerogel foam materials. The simulations demonstrate the feasibility of such a technique for measurements of density scale lengths near the interface with submicron spatial resolution. A proof-of-principle experiment is designed and performed at the Linac coherent light source facility. Preliminary data show the change of the interface after shock compression and heating withmore » simultaneous fluorescence spectra for temperature determination. Here, the results provide the first demonstration of using x-ray imaging at an absorption edge as a diagnostic to detect ultrafast phenomena for interface physics in high-energy-density systems.« less

Nano-structuring of multi-layer material by single x-ray vortex pulse with femtosecond duration

NASA Astrophysics Data System (ADS)

Kohmura, Yoshiki; Zhakhovsky, Vasily; Takei, Dai; Suzuki, Yoshio; Takeuchi, Akihisa; Inoue, Ichiro; Inubushi, Yuichi; Inogamov, Nail; Ishikawa, Tetsuya; Yabashi, Makina

2018-03-01

A narrow zero-intensity spot arising from an x-ray vortex has huge potential for future applications such as nanoscopy and nanofabrication. We here present an X-ray Free Electron Laser (XFEL) experiment with a focused vortex wavefront which generated high aspect ratio nanoneedles on a Cr/Au multi-layer (ML) specimen. A sharp needle with a typical width and height of 310 and 600 nm was formed with a high occurrence rate at the center of a 7.71 keV x-ray vortex on this ML specimen, respectively. The observed width exceeds the diffraction limit, and the smallest structures ever reported using an intense-XFEL ablation were fabricated. We found that the elemental composition of the nanoneedles shows a significant difference from that of the unaffected area of Cr/Au ML. All these results are well explained by the molecular dynamics simulations, leading to the elucidation of the needle formation mechanism on an ultra-fast timescale.

Structure determination of molecules in an alignment laser field by femtosecond photoelectron diffraction using an X-ray free-electron laser

PubMed Central

Minemoto, Shinichirou; Teramoto, Takahiro; Akagi, Hiroshi; Fujikawa, Takashi; Majima, Takuya; Nakajima, Kyo; Niki, Kaori; Owada, Shigeki; Sakai, Hirofumi; Togashi, Tadashi; Tono, Kensuke; Tsuru, Shota; Wada, Ken; Yabashi, Makina; Yoshida, Shintaro; Yagishita, Akira

2016-01-01

We have successfully determined the internuclear distance of I2 molecules in an alignment laser field by applying our molecular structure determination methodology to an I 2p X-ray photoelectron diffraction profile observed with femtosecond X-ray free electron laser pulses. Using this methodology, we have found that the internuclear distance of the sample I2 molecules in an alignment Nd:YAG laser field of 6 × 1011 W/cm2 is elongated by from 0.18 to 0.30 Å “in average” relatively to the equilibrium internuclear distance of 2.666 Å. Thus, the present experiment constitutes a critical step towards the goal of femtosecond imaging of chemical reactions and opens a new direction for the study of ultrafast chemical reaction in the gas phase. PMID:27934891

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fang, Li; Xiong, Hui; Kukk, Edwin

Molecular dynamics is of fundamental interest in natural science research. The capability of investigating molecular dynamics is one of the various motivations for ultrafast optics. Here, we present our investigation of photoionization and nuclear dynamics in methyl iodine (CH 3I) molecule with an X-ray pump X-ray probe scheme. The pump–probe experiment was realized with a two-mirror X-ray split and delay apparatus. Time-of-flight mass spectra at various pump–probe delay times were recorded to obtain the time profile for the creation of high charge states via sequential ionization and for molecular dissociation. We observed high charge states of atomic iodine up tomore » 29+, and visualized the evolution of creating these high atomic ion charge states, including their population suppression and enhancement as the arrival time of the second X-ray pulse was varied. We also show the evolution of the kinetics of the high charge states upon the timing of their creation during the ionization-dissociation coupled dynamics. We demonstrate the implementation of X-ray pump–probe methodology for investigating X-ray induced molecular dynamics with femtosecond temporal resolution. The results indicate the footprints of ionization that lead to high charge states, probing the long-range potential curves of the high charge states.« less

Coherent diffractive imaging of single helium nanodroplets with a high harmonic generation source.

PubMed

Rupp, Daniela; Monserud, Nils; Langbehn, Bruno; Sauppe, Mario; Zimmermann, Julian; Ovcharenko, Yevheniy; Möller, Thomas; Frassetto, Fabio; Poletto, Luca; Trabattoni, Andrea; Calegari, Francesca; Nisoli, Mauro; Sander, Katharina; Peltz, Christian; J Vrakking, Marc; Fennel, Thomas; Rouzée, Arnaud

2017-09-08

Coherent diffractive imaging of individual free nanoparticles has opened routes for the in situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using extreme ultraviolet pulses from a femtosecond-laser-driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely identify hitherto unresolved prolate shapes of superfluid helium droplets. Our results mark the advent of single-shot gas-phase nanoscopy with lab-based short-wavelength pulses and pave the way to ultrafast coherent diffractive imaging with phase-controlled multicolor fields and attosecond pulses.Diffraction imaging studies of free individual nanoparticles have so far been restricted to XUV and X-ray free - electron laser facilities. Here the authors demonstrate the possibility of using table-top XUV laser sources to image prolate shapes of superfluid helium droplets.

Ultrafast X-Ray Spectroscopy of Conical Intersections

NASA Astrophysics Data System (ADS)

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

2018-06-01

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

Current Status of Single Particle Imaging with X-ray Lasers

DOE PAGES

Sun, Zhibin; Fan, Jiadong; Li, Haoyuan; ...

2018-01-22

The advent of ultrafast X-ray free-electron lasers (XFELs) opens the tantalizing possibility of the atomic-resolution imaging of reproducible objects such as viruses, nanoparticles, single molecules, clusters, and perhaps biological cells, achieving a resolution for single particle imaging better than a few tens of nanometers. Improving upon this is a significant challenge which has been the focus of a global single particle imaging (SPI) initiative launched in December 2014 at the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, USA. A roadmap was outlined, and significant multi-disciplinary effort has since been devoted to work on the technical challenges of SPImore » such as radiation damage, beam characterization, beamline instrumentation and optics, sample preparation and delivery and algorithm development at multiple institutions involved in the SPI initiative. Currently, the SPI initiative has achieved 3D imaging of rice dwarf virus (RDV) and coliphage PR772 viruses at ~10 nm resolution by using soft X-ray FEL pulses at the Atomic Molecular and Optical (AMO) instrument of LCLS. Meanwhile, diffraction patterns with signal above noise up to the corner of the detector with a resolution of ~6 Ångström (Å) were also recorded with hard X-rays at the Coherent X-ray Imaging (CXI) instrument, also at LCLS. Achieving atomic resolution is truly a grand challenge and there is still a long way to go in light of recent developments in electron microscopy. However, the potential for studying dynamics at physiological conditions and capturing ultrafast biological, chemical and physical processes represents a tremendous potential application, attracting continued interest in pursuing further method development. In this paper, we give a brief introduction of SPI developments and look ahead to further method development.« less

Current Status of Single Particle Imaging with X-ray Lasers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sun, Zhibin; Fan, Jiadong; Li, Haoyuan

The advent of ultrafast X-ray free-electron lasers (XFELs) opens the tantalizing possibility of the atomic-resolution imaging of reproducible objects such as viruses, nanoparticles, single molecules, clusters, and perhaps biological cells, achieving a resolution for single particle imaging better than a few tens of nanometers. Improving upon this is a significant challenge which has been the focus of a global single particle imaging (SPI) initiative launched in December 2014 at the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, USA. A roadmap was outlined, and significant multi-disciplinary effort has since been devoted to work on the technical challenges of SPImore » such as radiation damage, beam characterization, beamline instrumentation and optics, sample preparation and delivery and algorithm development at multiple institutions involved in the SPI initiative. Currently, the SPI initiative has achieved 3D imaging of rice dwarf virus (RDV) and coliphage PR772 viruses at ~10 nm resolution by using soft X-ray FEL pulses at the Atomic Molecular and Optical (AMO) instrument of LCLS. Meanwhile, diffraction patterns with signal above noise up to the corner of the detector with a resolution of ~6 Ångström (Å) were also recorded with hard X-rays at the Coherent X-ray Imaging (CXI) instrument, also at LCLS. Achieving atomic resolution is truly a grand challenge and there is still a long way to go in light of recent developments in electron microscopy. However, the potential for studying dynamics at physiological conditions and capturing ultrafast biological, chemical and physical processes represents a tremendous potential application, attracting continued interest in pursuing further method development. In this paper, we give a brief introduction of SPI developments and look ahead to further method development.« less

Tracking the ultrafast XUV optical properties of x-ray free-electron-laser heated matter with high-order harmonics

NASA Astrophysics Data System (ADS)

Williams, Gareth O.; Künzel, S.; Daboussi, S.; Iwan, B.; Gonzalez, A. I.; Boutu, W.; Hilbert, V.; Zastrau, U.; Lee, H. J.; Nagler, B.; Granados, E.; Galtier, E.; Heimann, P.; Barbrel, B.; Dovillaire, G.; Lee, R. W.; Dunn, J.; Recoules, V.; Blancard, C.; Renaudin, P.; de la Varga, A. G.; Velarde, P.; Audebert, P.; Merdji, H.; Zeitoun, Ph.; Fajardo, M.

2018-02-01

We present measurements of photon absorption by free electrons as a solid is transformed to plasma. A femtosecond x-ray free-electron laser is used to heat a solid, which separates the electron and ion heating time scales. The changes in absorption are measured with an independent probe pulse created through high-order-harmonic generation. We find an increase in electron temperature to have a relatively small impact on absorption, contrary to several predictions, whereas ion heating increases absorption. We compare the data to current theoretical and numerical approaches and find that a smoother electronic structure yields a better fit to the data, suggestive of a temperature-dependent electronic structure in warm dense matter.

X-ray Pump–Probe Investigation of Charge and Dissociation Dynamics in Methyl Iodine Molecule

DOE PAGES

Fang, Li; Xiong, Hui; Kukk, Edwin; ...

2017-05-19

Molecular dynamics is of fundamental interest in natural science research. The capability of investigating molecular dynamics is one of the various motivations for ultrafast optics. Here, we present our investigation of photoionization and nuclear dynamics in methyl iodine (CH 3I) molecule with an X-ray pump X-ray probe scheme. The pump–probe experiment was realized with a two-mirror X-ray split and delay apparatus. Time-of-flight mass spectra at various pump–probe delay times were recorded to obtain the time profile for the creation of high charge states via sequential ionization and for molecular dissociation. We observed high charge states of atomic iodine up tomore » 29+, and visualized the evolution of creating these high atomic ion charge states, including their population suppression and enhancement as the arrival time of the second X-ray pulse was varied. We also show the evolution of the kinetics of the high charge states upon the timing of their creation during the ionization-dissociation coupled dynamics. We demonstrate the implementation of X-ray pump–probe methodology for investigating X-ray induced molecular dynamics with femtosecond temporal resolution. The results indicate the footprints of ionization that lead to high charge states, probing the long-range potential curves of the high charge states.« less

Practical application of cross correlation technique to measure jitter of master-oscillator-power-amplifier laser system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Młyńczak, J.; Sawicz-Kryniger, K.; Fry, A. R.

2014-01-01

The Linac coherent light source (LCLS) at the SLAC National Accelerator Laboratory (SLAC) is the world’s first hard X-ray free electron laser (XFEL) and is capable of producing high-energy, femtosecond duration X-ray pulses. A common technique to study fast timescale physical phenomena, various “pump/probe” techniques are used. In these techniques there are two lasers, one optical and one X-ray, that work as a pump and as a probe to study dynamic processes in atoms and molecules. In order to resolve phenomena that occur on femtosecond timescales, it is imperative to have very precise timing between the optical lasers and X-raysmore » (on the order of ~ 20 fs or better). The lasers are synchronized to the same RF source that drives the accelerator and produces the X-ray laser. However, elements in the lasers cause some drift and time jitter, thereby de-synchronizing the system. This paper considers cross-correlation technique as a way to quantify the drift and jitter caused by the regenerative amplifier of the ultrafast optical laser.« less

Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array

DOE PAGES

O’Neil, Galen C.; Miaja-Avila, Luis; Joe, Young Il; ...

2017-02-17

The detailed pathways of photoactivity on ultrafast time scales are a topic of contemporary interest. Using a tabletop apparatus based on a laser plasma X-ray source and an array of cryogenic microcalorimeter X-ray detectors, we measured a transient X-ray absorption spectrum during the ferrioxalate photoreduction reaction. With these high-efficiency detectors, we observe the Fe K edge move to lower energies and the amplitude of the extended X-ray absorption fine structure reduce, consistent with a photoreduction mechanism in which electron transfer precedes disassociation. We provide quantitative limits on the Fe–O bond length change. Lastly, we review potential improvements to our measurementmore » technique, highlighting the future potential of tabletop X-ray science using microcalorimeter sensors.« less

Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array

DOE Office of Scientific and Technical Information (OSTI.GOV)

O’Neil, Galen C.; Miaja-Avila, Luis; Joe, Young Il

The detailed pathways of photoactivity on ultrafast time scales are a topic of contemporary interest. Using a tabletop apparatus based on a laser plasma X-ray source and an array of cryogenic microcalorimeter X-ray detectors, we measured a transient X-ray absorption spectrum during the ferrioxalate photoreduction reaction. With these high-efficiency detectors, we observe the Fe K edge move to lower energies and the amplitude of the extended X-ray absorption fine structure reduce, consistent with a photoreduction mechanism in which electron transfer precedes disassociation. We provide quantitative limits on the Fe–O bond length change. Lastly, we review potential improvements to our measurementmore » technique, highlighting the future potential of tabletop X-ray science using microcalorimeter sensors.« less

Higgs amplitude mode in the BCS superconductors Nb1-xTi(x)N induced by terahertz pulse excitation.

PubMed

Matsunaga, Ryusuke; Hamada, Yuki I; Makise, Kazumasa; Uzawa, Yoshinori; Terai, Hirotaka; Wang, Zhen; Shimano, Ryo

2013-08-02

Ultrafast responses of BCS superconductor Nb(1-x)Ti(x)N films in a nonadiabatic excitation regime were investigated by using terahertz (THz) pump-THz probe spectroscopy. After an instantaneous excitation with the monocycle THz pump pulse, a transient oscillation emerges in the electromagnetic response in the BCS gap energy region. The oscillation frequency coincides with the asymptotic value of the BCS gap energy, indicating the appearance of the theoretically anticipated collective amplitude mode of the order parameter, namely the Higgs amplitude mode. Our result opens a new pathway to the ultrafast manipulation of the superconducting order parameter by optical means.

Ultrafast Coulomb explosion of a diiodomethane molecule induced by an X-ray free-electron laser pulse.

PubMed

Takanashi, Tsukasa; Nakamura, Kosuke; Kukk, Edwin; Motomura, Koji; Fukuzawa, Hironobu; Nagaya, Kiyonobu; Wada, Shin-Ichi; Kumagai, Yoshiaki; Iablonskyi, Denys; Ito, Yuta; Sakakibara, Yuta; You, Daehyun; Nishiyama, Toshiyuki; Asa, Kazuki; Sato, Yuhiro; Umemoto, Takayuki; Kariyazono, Kango; Ochiai, Kohei; Kanno, Manabu; Yamazaki, Kaoru; Kooser, Kuno; Nicolas, Christophe; Miron, Catalin; Asavei, Theodor; Neagu, Liviu; Schöffler, Markus; Kastirke, Gregor; Liu, Xiao-Jing; Rudenko, Artem; Owada, Shigeki; Katayama, Tetsuo; Togashi, Tadashi; Tono, Kensuke; Yabashi, Makina; Kono, Hirohiko; Ueda, Kiyoshi

2017-08-02

Coulomb explosion of diiodomethane CH 2 I 2 molecules irradiated by ultrashort and intense X-ray pulses from SACLA, the Japanese X-ray free electron laser facility, was investigated by multi-ion coincidence measurements and self-consistent charge density-functional-based tight-binding (SCC-DFTB) simulations. The diiodomethane molecule, containing two heavy-atom X-ray absorbing sites, exhibits a rather different charge generation and nuclear motion dynamics compared to iodomethane CH 3 I with only a single heavy atom, as studied earlier. We focus on charge creation and distribution in CH 2 I 2 in comparison to CH 3 I. The release of kinetic energy into atomic ion fragments is also studied by comparing SCC-DFTB simulations with the experiment. Compared to earlier simulations, several key enhancements are made, such as the introduction of a bond axis recoil model, where vibrational energy generated during charge creation processes induces only bond stretching or shrinking. We also propose an analytical Coulomb energy partition model to extract the essential mechanism of Coulomb explosion of molecules from the computed and the experimentally measured kinetic energies of fragment atomic ions by partitioning each pair Coulomb interaction energy into two ions of the pair under the constraint of momentum conservation. Effective internuclear distances assigned to individual fragment ions at the critical moment of the Coulomb explosion are then estimated from the average kinetic energies of the ions. We demonstrate, with good agreement between the experiment and the SCC-DFTB simulation, how the more heavily charged iodine fragments and their interplay define the characteristic features of the Coulomb explosion of CH 2 I 2 . The present study also confirms earlier findings concerning the magnitude of bond elongation in the ultrashort X-ray pulse duration, showing that structural damage to all but C-H bonds does not develop to a noticeable degree in the pulse length of ∼10 fs.

Ultrafast Magnetization Manipulation Using Single Femtosecond Light and Hot-Electron Pulses.

PubMed

Xu, Yong; Deb, Marwan; Malinowski, Grégory; Hehn, Michel; Zhao, Weisheng; Mangin, Stéphane

2017-11-01

Current-induced magnetization manipulation is a key issue for spintronic applications. This manipulation must be fast, deterministic, and nondestructive in order to function in device applications. Therefore, single- electronic-pulse-driven deterministic switching of the magnetization on the picosecond timescale represents a major step toward future developments of ultrafast spintronic systems. Here, the ultrafast magnetization dynamics in engineered Gd x [FeCo] 1- x -based structures are studied to compare the effect of femtosecond laser and hot-electron pulses. It is demonstrated that a single femtosecond hot-electron pulse causes deterministic magnetization reversal in either Gd-rich and FeCo-rich alloys similarly to a femtosecond laser pulse. In addition, it is shown that the limiting factor of such manipulation for perpendicular magnetized films arises from the formation of a multidomain state due to dipolar interactions. By performing time-resolved measurements under various magnetic fields, it is demonstrated that the same magnetization dynamics are observed for both light and hot-electron excitation, and that the full magnetization reversal takes place within 40 ps. The efficiency of the ultrafast current-induced magnetization manipulation is enhanced due to the ballistic transport of hot electrons before reaching the GdFeCo magnetic layer. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Irreversible transformation of ferromagnetic ordered stripe domains in single-shot infrared-pump/resonant-x-ray-scattering-probe experiments

NASA Astrophysics Data System (ADS)

Bergeard, Nicolas; Schaffert, Stefan; López-Flores, Víctor; Jaouen, Nicolas; Geilhufe, Jan; Günther, Christian M.; Schneider, Michael; Graves, Catherine; Wang, Tianhan; Wu, Benny; Scherz, Andreas; Baumier, Cédric; Delaunay, Renaud; Fortuna, Franck; Tortarolo, Marina; Tudu, Bharati; Krupin, Oleg; Minitti, Michael P.; Robinson, Joe; Schlotter, William F.; Turner, Joshua J.; Lüning, Jan; Eisebitt, Stefan; Boeglin, Christine

2015-02-01

The evolution of a magnetic domain structure upon excitation by an intense, femtosecond infrared (IR) laser pulse has been investigated using single-shot based time-resolved resonant x-ray scattering at the x-ray free electron laser LCLS. A well-ordered stripe domain pattern as present in a thin CoPd alloy film has been used as a prototype magnetic domain structure for this study. The fluence of the IR laser pump pulse was sufficient to lead to an almost complete quenching of the magnetization within the ultrafast demagnetization process taking place within the first few hundreds of femtoseconds following the IR laser pump pulse excitation. On longer time scales this excitation gave rise to subsequent irreversible transformations of the magnetic domain structure. Under our specific experimental conditions, it took about 2 ns before the magnetization started to recover. After about 5 ns the previously ordered stripe domain structure had evolved into a disordered labyrinth domain structure. Surprisingly, we observe after about 7 ns the occurrence of a partially ordered stripe domain structure reoriented into a novel direction. It is this domain structure in which the sample's magnetization stabilizes as revealed by scattering patterns recorded long after the initial pump-probe cycle. Using micromagnetic simulations we can explain this observation based on changes of the magnetic anisotropy going along with heat dissipation in the film.

Development of extreme ultraviolet and soft x-ray multilayer optics for scientific studies with femtosecond/attosecond sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aquila, Andrew Lee

The development of multilayer optics for extreme ultraviolet (EUV) radiation has led to advancements in many areas of science and technology, including materials studies, EUV lithography, water window microscopy, plasma imaging, and orbiting solar physics imaging. Recent developments in femtosecond and attosecond EUV pulse generation from sources such as high harmonic generation lasers, combined with the elemental and chemical specificity provided by EUV radiation, are opening new opportunities to study fundamental dynamic processes in materials. Critical to these efforts is the design and fabrication of multilayer optics to transport, focus, shape and image these ultra-fast pulses This thesis describes themore » design, fabrication, characterization, and application of multilayer optics for EUV femtosecond and attosecond scientific studies. Multilayer mirrors for bandwidth control, pulse shaping and compression, tri-material multilayers, and multilayers for polarization control are described. Characterization of multilayer optics, including measurement of material optical constants, reflectivity of multilayer mirrors, and metrology of reflected phases of the multilayer, which is critical to maintaining pulse size and shape, were performed. Two applications of these multilayer mirrors are detailed in the thesis. In the first application, broad bandwidth multilayers were used to characterize and measure sub-100 attosecond pulses from a high harmonic generation source and was performed in collaboration with the Max-Planck institute for Quantum Optics and Ludwig- Maximilians University in Garching, Germany, with Professors Krausz and Kleineberg. In the second application, multilayer mirrors with polarization control are useful to study femtosecond spin dynamics in an ongoing collaboration with the T-REX group of Professor Parmigiani at Elettra in Trieste, Italy. As new ultrafast x-ray sources become available, for example free electron lasers, the multilayer designs described in this thesis can be extended to higher photon energies, and such designs can be used with those sources to enable new scientific studies, such as molecular bonding, phonon, and spin dynamics.« less

Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop

NASA Astrophysics Data System (ADS)

Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young I.; Alpert, Bradley K.; Damrauer, Niels H.; Doriese, William B.; Fatur, Steven M.; Fowler, Joseph W.; Hilton, Gene C.; Jimenez, Ralph; Reintsema, Carl D.; Schmidt, Daniel R.; Silverman, Kevin L.; Swetz, Daniel S.; Tatsuno, Hideyuki; Ullom, Joel N.

2016-07-01

Experimental tools capable of monitoring both atomic and electronic structure on ultrafast (femtosecond to picosecond) time scales are needed for investigating photophysical processes fundamental to light harvesting, photocatalysis, energy and data storage, and optical display technologies. Time-resolved hard x-ray (>3 keV ) spectroscopies have proven valuable for these measurements due to their elemental specificity and sensitivity to geometric and electronic structures. Here, we present the first tabletop apparatus capable of performing time-resolved x-ray emission spectroscopy. The time resolution of the apparatus is better than 6 ps. By combining a compact laser-driven plasma source with a highly efficient array of microcalorimeter x-ray detectors, we are able to observe photoinduced spin changes in an archetypal polypyridyl iron complex [Fe (2 ,2'-bipyridine)3]2 + and accurately measure the lifetime of the quintet spin state. Our results demonstrate that ultrafast hard x-ray emission spectroscopy is no longer confined to large facilities and now can be performed in conventional laboratories with 10 times better time resolution than at synchrotrons. Our results are enabled, in part, by a 100- to 1000-fold increase in x-ray collection efficiency compared to current techniques.

Batch crystallization of rhodopsin for structural dynamics using an X-ray free-electron laser

DOE PAGES

Wu, Wenting; Nogly, Przemyslaw; Rheinberger, Jan; ...

2015-06-27

Rhodopsin is a membrane protein from the G protein-coupled receptor family. Together with its ligand retinal, it forms the visual pigment responsible for night vision. In order to perform ultrafast dynamics studies, a time-resolved serial femtosecond crystallography method is required owing to the nonreversible activation of rhodopsin. In such an approach, microcrystals in suspension are delivered into the X-ray pulses of an X-ray free-electron laser (XFEL) after a precise photoactivation delay. Here in this study, a millilitre batch production of high-density microcrystals was developed by four methodical conversion steps starting from known vapour-diffusion crystallization protocols: (i) screening the low-salt crystallizationmore » conditions preferred for serial crystallography by vapour diffusion, (ii) optimization of batch crystallization, (iii) testing the crystal size and quality using second-harmonic generation (SHG) imaging and X-ray powder diffraction and (iv) production of millilitres of rhodopsin crystal suspension in batches for serial crystallography tests; these crystals diffracted at an XFEL at the Linac Coherent Light Source using a liquid-jet setup.« less

Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals.

PubMed

Cherukara, Mathew J; Sasikumar, Kiran; Cha, Wonsuk; Narayanan, Badri; Leake, Steven J; Dufresne, Eric M; Peterka, Tom; McNulty, Ian; Wen, Haidan; Sankaranarayanan, Subramanian K R S; Harder, Ross J

2017-02-08

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behavior is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use X-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic "hard" or inhomogeneous and "soft" or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystal structure obtained from the ultrafast X-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.

Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cherukara, Mathew J.; Sasikumar, Kiran; Cha, Wonsuk

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behaviour is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use x-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic ‘hard’ or inhomogeneous and ‘soft’ or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystalmore » structure obtained from the ultrafast x-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Furthermore, understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.« less

Ultrafast Three-Dimensional X-ray Imaging of Deformation Modes in ZnO Nanocrystals

DOE PAGES

Cherukara, Mathew J.; Sasikumar, Kiran; Cha, Wonsuk; ...

2016-12-27

Imaging the dynamical response of materials following ultrafast excitation can reveal energy transduction mechanisms and their dissipation pathways, as well as material stability under conditions far from equilibrium. Such dynamical behaviour is challenging to characterize, especially operando at nanoscopic spatiotemporal scales. In this letter, we use x-ray coherent diffractive imaging to show that ultrafast laser excitation of a ZnO nanocrystal induces a rich set of deformation dynamics including characteristic ‘hard’ or inhomogeneous and ‘soft’ or homogeneous modes at different time scales, corresponding respectively to the propagation of acoustic phonons and resonant oscillation of the crystal. By integrating the 3D nanocrystalmore » structure obtained from the ultrafast x-ray measurements with a continuum thermo-electro-mechanical finite element model, we elucidate the deformation mechanisms following laser excitation, in particular, a torsional mode that generates a 50% greater electric potential gradient than that resulting from the flexural mode. Furthermore, understanding of the time-dependence of these mechanisms on ultrafast scales has significant implications for development of new materials for nanoscale power generation.« less

The Evolution of Surface Symmetry in Femtosecond Laser-Induced Transient States of Matter

NASA Astrophysics Data System (ADS)

Garnett, Joy Carleen

Gallium arsenide and other III-V materials are well known for their excellent optical and electronic properties and have led to the development of high-performance photovoltaic cells1,2, photoelectrochemical water splitting3,4, and light emitting diodes (LEDs)5. Several combinations of III-V semiconductors are now being considered as potentially attractive alternatives to silicon for these applications. However, further development requires fundamental understanding of processes that govern light-matter interactions. Specifically, surface strain and ultrafast dynamics are of great interest to the optoelectronic industry. Strained semiconductor surfaces dominate the design of optoelectronics and III-V semiconductor-based LEDs. Currently, the structures of strained surfaces are well characterized with x-ray diffraction (XRD)6 and electron crystallography7-9. However, optically-induced electronic behavior at these interfaces are not fully understood. This has the been one of the stimulants for the research in this dissertation. To further explore opticallyinduced electronic behavior at strained interfaces, I have asked the following questions: 1. How does static optoelectronic behavior change as a function of strain? 2. How does surface symmetry and electronic motion change with respect to strain? 3. How do atomic bonds change as a function of strain? Another main research goal of this work is to understand ultrafast subpicosecond processes after pulsed laser excitation. The knowledge of ultrafast processes dominates the design of devices in industries that require high temporal and spectral resolution. Ultrafast atomic motion has been the major focus of subpicosecond structural dynamics. Currently, these dynamics upon photoexcitation are well characterized with experimental methods such as ultrafast x-ray diffraction (U-XRD), ultrafast electron diffraction (UED), and ultrafast electron crystallography (UEC). However, ultrafast atomic motion does not occur alone. The bonds connecting these moving atoms are also affected during this process. The correlation between structural and electronic dynamics is not well understood. To further explore correlated structural and electronic behavior upon ultrafast laser excitation, I have asked the following questions: 1. How does subpicosecond optoelectronic behavior change as a function of time after femtosecond pulse photoexcitation? 2. How does subpicosecond surface symmetry and electronic motion change with respect to time after femtosecond pulse photoexcitation? 3. How do atomic bonds change as a function of time after femtosecond pulse photoexcitation? To address these questions, I used experimental methods sensitive to both atomic motions and electronic responses: polarization-resolved second harmonic generation (PRSHG) and timeresolved, polarization-resolved second harmonic generation (TRPRSHG). The dissertation covers application of these techniques to III-V semiconductors: gallium arsenide (GaAs), gallium antimonide (GaSb), and aluminum gallium arsenide (AlGaAs). This dissertation is organized as follows. Chapter 2 presents the background of electronic band structures, ultrafast relaxation processes, and the origin of nonlinear optics from the perspectives of classical and quantum mechanics. It thus provides a framework for the static and transient nonlinear optical processes observed in III-V semiconductors under ultrafast pulse excitation. Next, Chapter 3 motivates the use of the experimental and analytical methods as applied to the experimental and theoretical studies outlined in Chapters 4 and 5. Chapter 4 is devoted to the understanding of polarization-resolved second-order nonlinear optical responses of various strained III-V semiconductor heterostructures resulting from defect-conducive growth conditions. Simplified phenomenological expressions for the polarization-resolved second harmonic generation (PRSHG) are first derived using tensor analysis. Afterwards, these expressions are used to fit experimental data. The developed formalism is tested under different conditions to gauge the fit robustness and sensitivity to mechanical and electronic changes in strained IIIV semiconductors. Along that same vein, Chapter 5 extends this analytical fit to describe ultrafast PRSHG responses of GaAs (100) as a function of transient changes in the interatomic potential within the first picosecond after photoexcitation. Finally, the dissertation concludes with Chapter 6 addressing possible directions for future work. The chapter begins with a description of studies to further test the sensitivity and robustness of the PRSHG phenomenological fit and how it can be used to characterize more classes of materials.

Coulomb-Driven Relativistic Electron Beam Compression

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

Coulomb-Driven Relativistic Electron Beam Compression.

PubMed

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

2018-01-26

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

Tracking the ultrafast XUV optical properties of x-ray free-electron-laser heated matter with high-order harmonics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Williams, Gareth O.; Künzel, S.; Daboussi, S.

We present measurements of photon absorption by free electrons as a solid is transformed to plasma. A femtosecond x-ray free-electron laser is used to heat a solid, which separates the electron and ion heating time scales. The changes in absorption are measured with an independent probe pulse created through high-order-harmonic generation. We find an increase in electron temperature to have a relatively small impact on absorption, contrary to several predictions, whereas ion heating increases absorption. Here, we compare the data to current theoretical and numerical approaches and find that a smoother electronic structure yields a better fit to the data,more » suggestive of a temperature-dependent electronic structure in warm dense matter.« less

Tracking the ultrafast XUV optical properties of x-ray free-electron-laser heated matter with high-order harmonics

DOE PAGES

Williams, Gareth O.; Künzel, S.; Daboussi, S.; ...

2018-02-14

We present measurements of photon absorption by free electrons as a solid is transformed to plasma. A femtosecond x-ray free-electron laser is used to heat a solid, which separates the electron and ion heating time scales. The changes in absorption are measured with an independent probe pulse created through high-order-harmonic generation. We find an increase in electron temperature to have a relatively small impact on absorption, contrary to several predictions, whereas ion heating increases absorption. Here, we compare the data to current theoretical and numerical approaches and find that a smoother electronic structure yields a better fit to the data,more » suggestive of a temperature-dependent electronic structure in warm dense matter.« less

Perspective: Opportunities for ultrafast science at SwissFEL

PubMed Central

Abela, Rafael; Beaud, Paul; van Bokhoven, Jeroen A.; Chergui, Majed; Feurer, Thomas; Haase, Johannes; Ingold, Gerhard; Johnson, Steven L.; Knopp, Gregor; Lemke, Henrik; Milne, Chris J.; Pedrini, Bill; Radi, Peter; Schertler, Gebhard; Standfuss, Jörg; Staub, Urs; Patthey, Luc

2018-01-01

We present the main specifications of the newly constructed Swiss Free Electron Laser, SwissFEL, and explore its potential impact on ultrafast science. In light of recent achievements at current X-ray free electron lasers, we discuss the potential territory for new scientific breakthroughs offered by SwissFEL in Chemistry, Biology, and Materials Science, as well as nonlinear X-ray science. PMID:29376109

Directly probing spin dynamics in insulating antiferromagnets using ultrashort terahertz pulses

DOE PAGES

Bowlan, Pamela Renee; Trugman, Stuart Alan; Wang, X.; ...

2016-11-22

We investigate spin dynamics in the antiferromagnetic (AFM) multiferroic TbMnO3 using opticalpump, terahertz (THz)-probe spectroscopy. Photoexcitation results in a broadband THz transmission change, with an onset time of 25 ps at 6 K that becomes faster at higher temperatures. We attribute this time constant to spin-lattice thermalization. The excellent agreement between our measurements and previous ultrafast resonant x-ray diffraction measurements on the same material confirms that our THz pulse directly probes spin order. We suggest that this could be the case in general for insulating AFM materials, if the origin of the static absorption in the THz spectral range ismore » magnetic.« less

Vibrational cross-angles in condensed molecules: a structural tool.

PubMed

Chen, Hailong; Zhang, Yufan; Li, Jiebo; Liu, Hongjun; Jiang, De-En; Zheng, Junrong

2013-09-05

The fluctuations of three-dimensional molecular conformations of a molecule in different environments play critical roles in many important chemical and biological processes. X-ray diffraction (XRD) techniques and nuclear magnetic resonance (NMR) methods are routinely applied to monitor the molecular conformations in condensed phases. However, some special requirements of the methods have prevented them from exploring many molecular phenomena at the current stage. Here, we introduce another method to resolve molecular conformations based on an ultrafast MIR/T-Hz multiple-dimensional vibrational spectroscopic technique. The model molecule (4'-methyl-2'-nitroacetanilide, MNA) is prepared in two of its crystalline forms and liquid samples. Two polarized ultrafast infrared pulses are then used to determine the cross-angles of vibrational transition moment directions by exciting one vibrational band and detecting the induced response on another vibrational band of the molecule. The vibrational cross-angles are then converted into molecular conformations with the aid of calculations. The molecular conformations determined by the method are supported by X-ray diffraction and molecular dynamics simulation results. The experimental results suggest that thermodynamic interactions with solvent molecules are not altering the molecular conformations of MNA in the solutions to control their ultimate conformations in the crystals.

Direct characterization of photoinduced lattice dynamics in BaFe 2As 2

DOE PAGES

Gerber, S.; Kim, K. W.; Zhang, Y.; ...

2015-06-08

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe 2As 2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent latticemore » dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands.« less

Direct characterization of photoinduced lattice dynamics in BaFe2As2

PubMed Central

Gerber, S.; Kim, K. W.; Zhang, Y.; Zhu, D.; Plonka, N.; Yi, M.; Dakovski, G. L.; Leuenberger, D.; Kirchmann, P.S.; Moore, R. G.; Chollet, M.; Glownia, J. M.; Feng, Y.; Lee, J.-S.; Mehta, A.; Kemper, A. F.; Wolf, T.; Chuang, Y.-D.; Hussain, Z.; Kao, C.-C.; Moritz, B.; Shen, Z.-X.; Devereaux, T. P.; Lee, W.-S.

2015-01-01

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe2As2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands. PMID:26051704

Capturing Structural Dynamics in Crystalline Silicon Using Chirped Electrons from a Laser Wakefield Accelerator

PubMed Central

He, Z.-H.; Beaurepaire, B.; Nees, J. A.; Gallé, G.; Scott, S. A.; Pérez, J. R. Sánchez; Lagally, M. G.; Krushelnick, K.; Thomas, A. G. R.; Faure, J.

2016-01-01

Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scale by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes. PMID:27824086

Capturing Structural Dynamics in Crystalline Silicon Using Chirped Electrons from a Laser Wakefield Accelerator

DOE PAGES

He, Z. -H.; Beaurepaire, B.; Nees, J. A.; ...

2016-11-08

Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here in this paper, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scalemore » by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes.« less

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken

Ultrafast X-ray imaging on individual fragile specimens such as aerosols, metastable particles, superfluid quantum systems and live biospecimens provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined. Here in this paper, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolutionmore » so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.« less

Time-dependent nonequilibrium soft x-ray response during a spin crossover

NASA Astrophysics Data System (ADS)

van Veenendaal, Michel

2018-03-01

A theoretical framework is developed for better understanding the time-dependent soft-x-ray response of dissipative quantum many-body systems. It is shown how x-ray absorption and resonant inelastic x-ray scattering (RIXS) at transition-metal L edges can provide insight into ultrafast intersystem crossings of importance for energy conversion, ultrafast magnetism, and catalysis. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogs is used as a model system to demonstrate how the x-ray response is affected by the nonequilibrium dynamics on a femtosecond time scale. Changes in local spin and symmetry and the underlying mechanism are reflected in strong broadenings, a collapse of clear selection rules during the intersystem crossing, fluctuations in the isotropic branching ratio in x-ray absorption, crystal-field collapse and/or oscillations, and time-dependent anti-Stokes processes in RIXS.

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

NASA Astrophysics Data System (ADS)

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken; Bucher, Max; Maia, Filipe R. N. C.; Bielecki, Johan; Ekeberg, Tomas; Hantke, Max F.; Daurer, Benedikt J.; Nettelblad, Carl; Andreasson, Jakob; Barty, Anton; Bruza, Petr; Carron, Sebastian; Hasse, Dirk; Krzywinski, Jacek; Larsson, Daniel S. D.; Morgan, Andrew; Mühlig, Kerstin; Müller, Maria; Okamoto, Kenta; Pietrini, Alberto; Rupp, Daniela; Sauppe, Mario; van der Schot, Gijs; Seibert, Marvin; Sellberg, Jonas A.; Svenda, Martin; Swiggers, Michelle; Timneanu, Nicusor; Westphal, Daniel; Williams, Garth; Zani, Alessandro; Chapman, Henry N.; Faigel, Gyula; Möller, Thomas; Hajdu, Janos; Bostedt, Christoph

2018-03-01

Ultrafast X-ray imaging on individual fragile specimens such as aerosols1, metastable particles2, superfluid quantum systems3 and live biospecimens4 provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined4,5. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolution so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

DOE PAGES

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken; ...

2018-02-26

Ultrafast X-ray imaging on individual fragile specimens such as aerosols, metastable particles, superfluid quantum systems and live biospecimens provides high-resolution information that is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely defined. Here in this paper, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lateral resolutionmore » so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond timescale.« less

Hard-X-Ray-Induced Multistep Ultrafast Dissociation

NASA Astrophysics Data System (ADS)

Travnikova, Oksana; Marchenko, Tatiana; Goldsztejn, Gildas; Jänkälä, Kari; Sisourat, Nicolas; Carniato, Stéphane; Guillemin, Renaud; Journel, Loïc; Céolin, Denis; Püttner, Ralph; Iwayama, Hiroshi; Shigemasa, Eiji; Piancastelli, Maria Novella; Simon, Marc

2016-05-01

Creation of deep core holes with very short (τ ≤1 fs ) lifetimes triggers a chain of relaxation events leading to extensive nuclear dynamics on a few-femtosecond time scale. Here we demonstrate a general multistep ultrafast dissociation on an example of HCl following Cl 1 s →σ* excitation. Intermediate states with one or multiple holes in the shallower core electron shells are generated in the course of the decay cascades. The repulsive character and large gradients of the potential energy surfaces of these intermediates enable ultrafast fragmentation after the absorption of a hard x-ray photon.

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

PubMed

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

2009-12-11

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

Ultrafast secondary emission X-ray imaging detectors: A possible application to TRD

NASA Astrophysics Data System (ADS)

Akkerman, A.; Breskin, A.; Chechik, R.; Elkind, V.; Gibrekhterman, A.; Majewski, S.

1992-05-01

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

R&D 100, 2016: Ultrafast X-ray Imager

ScienceCinema

Porter, John; Claus, Liam; Sanchez, Marcos; Robertson, Gideon; Riley, Nathan; Rochau, Greg

2018-06-13

The Ultrafast X-ray Imager is a solid-state camera capable of capturing a sequence of images with user-selectable exposure times as short as 2 billionths of a second. Using 3D semiconductor integration techniques to form a hybrid chip, this camera was developed to enable scientists to study the heating and compression of fusion targets in the quest to harness the energy process that powers the stars.

R&D 100, 2016: Ultrafast X-ray Imager

DOE Office of Scientific and Technical Information (OSTI.GOV)

Porter, John; Claus, Liam; Sanchez, Marcos

The Ultrafast X-ray Imager is a solid-state camera capable of capturing a sequence of images with user-selectable exposure times as short as 2 billionths of a second. Using 3D semiconductor integration techniques to form a hybrid chip, this camera was developed to enable scientists to study the heating and compression of fusion targets in the quest to harness the energy process that powers the stars.

Ultrafast photo-induced hidden phases in strained manganite thin films

NASA Astrophysics Data System (ADS)

Zhang, Jingdi; McLeod, A. S.; Zhang, Gu-Feng; Stoica, Vladimir; Jin, Feng; Gu, Mingqiang; Gopalan, Venkatraman; Freeland, John W.; Wu, Wenbin; Rondinelli, James; Wen, Haidan; Basov, D. N.; Averitt, R. D.

Correlated transition metal oxides (TMOs) are particularly sensitive to external control because of energy degeneracy in a complex energy landscape that promote a plethora of metastable states. However, it remains a grand challenge to actively control and fully explore the rich landscape of TMOs. Dynamic control with pulsed photons can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible. In the past, we have demonstrated that mode-selective single-laser-pulse excitation of a strained manganite thin film La2/3Ca1/3MnO3 initiates a persistent phase transition from an emergent antiferromagnetic insulating ground state to a ferromagnetic metallic metastable state. Beyond the photo-induced insulator to metal transition, we recently discovered a new peculiar photo-induced hidden phase, identified by an experimental approach that combines ultrafast pump-probe spectroscopy, THz spectroscopy, X-ray diffraction, cryogenic near-field spectroscopy and SHG probe. This work is funded by the DOE, Office of Science, Office of Basic Energy Science under Award Numbers DE-SC0012375 and DE-SC0012592.

A Search for H I Lyα Counterparts to Ultrafast X-Ray Outflows

NASA Astrophysics Data System (ADS)

Kriss, Gerard A.; Lee, Julia C.; Danehkar, Ashkbiz

2018-06-01

Prompted by the H I Lyα absorption associated with the X-ray ultrafast outflow at ‑17,300 km s‑1 in the quasar PG 1211+143, we have searched archival UV spectra at the expected locations of H I Lyα absorption for a large sample of ultrafast outflows identified in XMM-Newton and Suzaku observations. Sixteen of the X-ray outflows have predicted H I Lyα wavelengths falling within the bandpass of spectra from either the Far Ultraviolet Spectroscopic Explorer or the Hubble Space Telescope, although none of the archival observations were simultaneous with the X-ray observations in which ultrafast X-ray outflows (UFOs) were detected. In our spectra broad features with FWHM of 1000 km s‑1 have 2σ upper limits on the H I column density of generally ≲2 × 1013 cm‑2. Using grids of photoionization models covering a broad range of spectral energy distributions (SEDs), we find that producing Fe XXVI Lyα X-ray absorption with equivalent widths >30 eV and associated H I Lyα absorption with {N}{{H}{{I}}}< 2× {10}13 {cm}}-2 requires total absorbing column densities {N}{{H}}> 5× {10}22 {cm}}-2 and ionization parameters log ξ ≳ 3.7. Nevertheless, a wide range of SEDs would predict observable H I Lyα absorption if ionization parameters are only slightly below peak ionization fractions for Fe XXV and Fe XXVI. The lack of Lyα features in the archival UV spectra indicates that the UFOs have very high ionization parameters, that they have very hard UV-ionizing spectra, or that they were not present at the time of the UV spectral observations owing to variability.

Homepage P. Fischer, LBNL, Berkeley CA | UC Santa Cruz CA

Science.gov Websites

mesoscale magnetic x-ray microscopy and spectroscopy (ultra-)fast spin dynamics soft x-ray tomography of condensed matter x-ray optics publications presentations invited talks conference contributions curriculum

X-ray Emission Characteristics of Ultra-High Energy Density Relativistic Plasmas Created by Ultrafast Laser Irradiation of Nanowire Arrays

NASA Astrophysics Data System (ADS)

Hollinger, R. C.; Bargsten, C.; Shlyaptsev, V. N.; Pukhov, A.; Purvis, M. A.; Townsend, A.; Keiss, D.; Wang, Y.; Wang, S.; Prieto, A.; Rocca, J. J.

2014-10-01

Irradiation of ordered nanowire arrays with high contrast femtosecond laser pulses of relativistic intensity creates volumetrically heated near solid density plasmas characterized by multi-KeV temperatures and extreme degrees of ionization. The large hydrodynamic-to-radiative lifetime ratio of these plasmas results in very efficient X-ray generation. Au nanowire array plasmas irradiated at I 5×1018 Wcm-2 are measured to convert ~ 5 percent of the laser energy into h ν > 0.9 KeV X-rays, and >1 × 10-4 into h ν > 9 KeV photons, creating bright picosecond X-ray sources. The angular distribution of the higher energy photons is measured to change from isotropic into annular as the intensity increases, while softer X-ray emission (h ν >1 KeV) remains isotropic and nearly unchanged. Model simulations suggest the unexpected annular distribution of the hard X-rays might result from bremsstrahlung of fast electrons confined in a high aspect ratio near solid density plasma in which the electron-ion collision mean free-path is of the order of the plasma thickness. Work supported by the U.S Department of Energy, Fusion Energy Sciences and the Defense Threat Reduction Agency Grant HDTRA-1-10-1-0079. A.P was supported by of DFG-funded project TR18.

Attosecond electron bunches from a nanofiber driven by Laguerre-Gaussian laser pulses.

PubMed

Hu, Li-Xiang; Yu, Tong-Pu; Sheng, Zheng-Ming; Vieira, Jorge; Zou, De-Bin; Yin, Yan; McKenna, Paul; Shao, Fu-Qiu

2018-05-08

Generation of attosecond bunches of energetic electrons offers significant potential from ultrafast physics to novel radiation sources. However, it is still a great challenge to stably produce such electron beams with lasers, since the typical subfemtosecond electron bunches from laser-plasma interactions either carry low beam charge, or propagate for only several tens of femtoseconds. Here we propose an all-optical scheme for generating dense attosecond electron bunches via the interaction of an intense Laguerre-Gaussian (LG) laser pulse with a nanofiber. The dense bunch train results from the unique field structure of a circularly polarized LG laser pulse, enabling each bunch to be phase-locked and accelerated forward with low divergence, high beam charge and large beam-angular-momentum. This paves the way for wide applications in various fields, e.g., ultrabrilliant attosecond x/γ-ray emission.

Morphological and chemical evolution on InP(1 0 0) surface irradiated with femtosecond laser

NASA Astrophysics Data System (ADS)

Qian, H. X.; Zhou, W.; Zheng, H. Y.; Lim, G. C.

2005-12-01

Single crystalline InP was ablated in air with p-polarized Ti:sapphire femtosecond laser at a fixed laser fluence of 82 mJ/cm 2. Ripples parallel to the laser polarization direction were found by scanning electron microscopy and atomic force microscopy to form for laser pulses ranging from 50 to 1000, whereas flower-like structures appeared for laser pulses of 10 4 and above. Analysis by X-ray photoelectron spectroscopy showed formation of indium and phosphorus oxides on the irradiated surface and the amounts of oxides increased with increasing number of laser pulses. The oxide formation is attributed to chemical reaction between the ultrafast laser ablation plume and oxygen in air, and formation of the flower-like structures is shown to be related to deposition of the oxides on the irradiated surface.

The LAMP instrument at the Linac Coherent Light Source free-electron laser

NASA Astrophysics Data System (ADS)

Osipov, Timur; Bostedt, Christoph; Castagna, J.-C.; Ferguson, Ken R.; Bucher, Maximilian; Montero, Sebastian C.; Swiggers, Michele L.; Obaid, Razib; Rolles, Daniel; Rudenko, Artem; Bozek, John D.; Berrah, Nora

2018-03-01

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusive metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.

Ultrafast cavitation induced by an X-ray laser in water drops

NASA Astrophysics Data System (ADS)

Stan, Claudiu; Willmott, Philip; Stone, Howard; Koglin, Jason; Liang, Mengning; Aquila, Andrew; Robinson, Joseph; Gumerlock, Karl; Blaj, Gabriel; Sierra, Raymond; Boutet, Sebastien; Guillet, Serge; Curtis, Robin; Vetter, Sharon; Loos, Henrik; Turner, James; Decker, Franz-Josef

2016-11-01

Cavitation in pure water is determined by an intrinsic heterogeneous cavitation mechanism, which prevents in general the experimental generation of large tensions (negative pressures) in bulk liquid water. We developed an ultrafast decompression technique, based on the reflection of shock waves generated by an X-ray laser inside liquid drops, to stretch liquids to large negative pressures in a few nanoseconds. Using this method, we observed cavitation in liquid water at pressures below -100 MPa. These large tensions exceed significantly those achieved previously, mainly due to the ultrafast decompression. The decompression induced by shock waves generated by an X-ray laser is rapid enough to continue to stretch the liquid phase after the heterogeneous cavitation occurs in water, despite the rapid growth of cavitation nanobubbles. We developed a nucleation-and-growth hydrodynamic cavitation model that explains our results and estimates the concentration of heterogeneous cavitation nuclei in water.

Dynamic x-ray imaging of laser-driven nanoplasmas

NASA Astrophysics Data System (ADS)

Fennel, Thomas

2016-05-01

A major promise of current x-ray science at free electron lasers is the realization of unprecedented imaging capabilities for resolving the structure and ultrafast dynamics of matter with nanometer spatial and femtosecond temporal resolution or even below via single-shot x-ray diffraction. Laser-driven atomic clusters and nanoparticles provide an ideal platform for developing and demonstrating the required technology to extract the ultrafast transient spatiotemporal dynamics from the diffraction images. In this talk, the perspectives and challenges of dynamic x-ray imaging will be discussed using complete self-consistent microscopic electromagnetic simulations of IR pump x-ray probe imaging for the example of clusters. The results of the microscopic particle-in-cell simulations (MicPIC) enable the simulation-assisted reconstruction of corresponding experimental data. This capability is demonstrated by converting recently measured LCLS data into a ultrahigh resolution movie of laser-induced plasma expansion. Finally, routes towards reaching attosecond time resolution in the visualization of complex dynamical processes in matter by x-ray diffraction will be discussed.

Femtosecond X-ray Fourier holography imaging of freeflying nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gorkhover, Tais; Ulmer, Anatoli; Ferguson, Ken R.

Ultrafast X-ray imaging on individual fragile specimens such as aerosols1, metastable particles2, superfluid quantum systems3 and live biospecimen4 provides high resolution information, which is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imag- 2 ing, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely-defined4, 5. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers in order to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highestmore » lateral resolution so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond time scale.« less

Watching proteins function with time-resolved x-ray crystallography

NASA Astrophysics Data System (ADS)

Šrajer, Vukica; Schmidt, Marius

2017-09-01

Macromolecular crystallography was immensely successful in the last two decades. To a large degree this success resulted from use of powerful third generation synchrotron x-ray sources. An expansive database of more than 100 000 protein structures, of which many were determined at resolution better than 2 Å, is available today. With this achievement, the spotlight in structural biology is shifting from determination of static structures to elucidating dynamic aspects of protein function. A powerful tool for addressing these aspects is time-resolved crystallography, where a genuine biological function is triggered in the crystal with a goal of capturing molecules in action and determining protein kinetics and structures of intermediates (Schmidt et al 2005a Methods Mol. Biol. 305 115-54, Schmidt 2008 Ultrashort Laser Pulses in Biology and Medicine (Berlin: Springer) pp 201-41, Neutze and Moffat 2012 Curr. Opin. Struct. Biol. 22 651-9, Šrajer 2014 The Future of Dynamic Structural Science (Berlin: Springer) pp 237-51). In this approach, short and intense x-ray pulses are used to probe intermediates in real time and at room temperature, in an ongoing reaction that is initiated synchronously and rapidly in the crystal. Time-resolved macromolecular crystallography with 100 ps time resolution at synchrotron x-ray sources is in its mature phase today, particularly for studies of reversible, light-initiated reactions. The advent of the new free electron lasers for hard x-rays (XFELs; 5-20 keV), which provide exceptionally intense, femtosecond x-ray pulses, marks a new frontier for time-resolved crystallography. The exploration of ultra-fast events becomes possible in high-resolution structural detail, on sub-picosecond time scales (Tenboer et al 2014 Science 346 1242-6, Barends et al 2015 Science 350 445-50, Pande et al 2016 Science 352 725-9). We review here state-of-the-art time-resolved crystallographic experiments both at synchrotrons and XFELs. We also outline challenges and further developments necessary to broaden the application of these methods to many important proteins and enzymes of biomedical relevance.

Watching proteins function with time-resolved x-ray crystallography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Šrajer, Vukica; Schmidt, Marius

Macromolecular crystallography was immensely successful in the last two decades. To a large degree this success resulted from use of powerful third generation synchrotron x-ray sources. An expansive database of more than 100 000 protein structures, of which many were determined at resolution better than 2 Å, is available today. With this achievement, the spotlight in structural biology is shifting from determination of static structures to elucidating dynamic aspects of protein function. A powerful tool for addressing these aspects is time-resolved crystallography, where a genuine biological function is triggered in the crystal with a goal of capturing molecules in actionmore » and determining protein kinetics and structures of intermediates (Schmidt et al 2005a Methods Mol. Biol. 305 115–54, Schmidt 2008 Ultrashort Laser Pulses in Biology and Medicine (Berlin: Springer) pp 201–41, Neutze and Moffat 2012 Curr. Opin. Struct. Biol. 22 651–9, Šrajer 2014 The Future of Dynamic Structural Science (Berlin: Springer) pp 237–51). In this approach, short and intense x-ray pulses are used to probe intermediates in real time and at room temperature, in an ongoing reaction that is initiated synchronously and rapidly in the crystal. Time-resolved macromolecular crystallography with 100 ps time resolution at synchrotron x-ray sources is in its mature phase today, particularly for studies of reversible, light-initiated reactions. The advent of the new free electron lasers for hard x-rays (XFELs; 5–20 keV), which provide exceptionally intense, femtosecond x-ray pulses, marks a new frontier for time-resolved crystallography. The exploration of ultra-fast events becomes possible in high-resolution structural detail, on sub-picosecond time scales (Tenboer et al 2014 Science 346 1242–6, Barends et al 2015 Science 350 445–50, Pande et al 2016 Science 352 725–9). We review here state-of-the-art time-resolved crystallographic experiments both at synchrotrons and XFELs. We also outline challenges and further developments necessary to broaden the application of these methods to many important proteins and enzymes of biomedical relevance.« less

Toward a terahertz-driven electron gun

PubMed Central

Huang, W. Ronny; Nanni, Emilio A.; Ravi, Koustuban; Hong, Kyung-Han; Fallahi, Arya; Wong, Liang Jie; Keathley, Phillip D.; Zapata, Luis E.; Kärtner, Franz X.

2015-01-01

Femtosecond electron bunches with keV energies and eV energy spread are needed by condensed matter physicists to resolve state transitions in carbon nanotubes, molecular structures, organic salts, and charge density wave materials. These semirelativistic electron sources are not only of interest for ultrafast electron diffraction, but also for electron energy-loss spectroscopy and as a seed for x-ray FELs. Thus far, the output energy spread (hence pulse duration) of ultrafast electron guns has been limited by the achievable electric field at the surface of the emitter, which is 10 MV/m for DC guns and 200 MV/m for RF guns. A single-cycle THz electron gun provides a unique opportunity to not only achieve GV/m surface electric fields but also with relatively low THz pulse energies, since a single-cycle transform-limited waveform is the most efficient way to achieve intense electric fields. Here, electron bunches of 50 fC from a flat copper photocathode are accelerated from rest to tens of eV by a microjoule THz pulse with peak electric field of 72 MV/m at 1 kHz repetition rate. We show that scaling to the readily-available GV/m THz field regime would translate to monoenergetic electron beams of ~100 keV. PMID:26486697

Dynamic fracture of tantalum under extreme tensile stress.

PubMed

Albertazzi, Bruno; Ozaki, Norimasa; Zhakhovsky, Vasily; Faenov, Anatoly; Habara, Hideaki; Harmand, Marion; Hartley, Nicholas; Ilnitsky, Denis; Inogamov, Nail; Inubushi, Yuichi; Ishikawa, Tetsuya; Katayama, Tetsuo; Koyama, Takahisa; Koenig, Michel; Krygier, Andrew; Matsuoka, Takeshi; Matsuyama, Satoshi; McBride, Emma; Migdal, Kirill Petrovich; Morard, Guillaume; Ohashi, Haruhiko; Okuchi, Takuo; Pikuz, Tatiana; Purevjav, Narangoo; Sakata, Osami; Sano, Yasuhisa; Sato, Tomoko; Sekine, Toshimori; Seto, Yusuke; Takahashi, Kenjiro; Tanaka, Kazuo; Tange, Yoshinori; Togashi, Tadashi; Tono, Kensuke; Umeda, Yuhei; Vinci, Tommaso; Yabashi, Makina; Yabuuchi, Toshinori; Yamauchi, Kazuto; Yumoto, Hirokatsu; Kodama, Ryosuke

2017-06-01

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power optical laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of [Formula: see text] ~2 × 10 8 to 3.5 × 10 8 s -1 . A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions.

Dynamic fracture of tantalum under extreme tensile stress

PubMed Central

Albertazzi, Bruno; Ozaki, Norimasa; Zhakhovsky, Vasily; Faenov, Anatoly; Habara, Hideaki; Harmand, Marion; Hartley, Nicholas; Ilnitsky, Denis; Inogamov, Nail; Inubushi, Yuichi; Ishikawa, Tetsuya; Katayama, Tetsuo; Koyama, Takahisa; Koenig, Michel; Krygier, Andrew; Matsuoka, Takeshi; Matsuyama, Satoshi; McBride, Emma; Migdal, Kirill Petrovich; Morard, Guillaume; Ohashi, Haruhiko; Okuchi, Takuo; Pikuz, Tatiana; Purevjav, Narangoo; Sakata, Osami; Sano, Yasuhisa; Sato, Tomoko; Sekine, Toshimori; Seto, Yusuke; Takahashi, Kenjiro; Tanaka, Kazuo; Tange, Yoshinori; Togashi, Tadashi; Tono, Kensuke; Umeda, Yuhei; Vinci, Tommaso; Yabashi, Makina; Yabuuchi, Toshinori; Yamauchi, Kazuto; Yumoto, Hirokatsu; Kodama, Ryosuke

2017-01-01

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power optical laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of ε. ~2 × 108 to 3.5 × 108 s−1. A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions. PMID:28630909

DOE Office of Scientific and Technical Information (OSTI.GOV)

Albertazzi, Bruno; Ozaki, Norimasa; Zhakhovsky, Vasily

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power opticalmore » laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of Embedded Image ~2 × 10 8 to 3.5 × 10 8 s -1. A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions.« less

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, F.; Zhu, Y.; Liu, S.

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. Thismore » effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.« less

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, F.; Zhu, Y.; Liu, S.

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here in this paper we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent acrossmore » unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.« less

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

DOE PAGES

Chen, F.; Zhu, Y.; Liu, S.; ...

2016-11-22

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here in this paper we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent acrossmore » unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.« less

Diffraction leveraged modulation of X-ray pulses using MEMS-based X-ray optics

DOEpatents

Lopez, Daniel; Shenoy, Gopal; Wang, Jin; Walko, Donald A.; Jung, Il-Woong; Mukhopadhyay, Deepkishore

2016-08-09

A method and apparatus are provided for implementing Bragg-diffraction leveraged modulation of X-ray pulses using MicroElectroMechanical systems (MEMS) based diffractive optics. An oscillating crystalline MEMS device generates a controllable time-window for diffraction of the incident X-ray radiation. The Bragg-diffraction leveraged modulation of X-ray pulses includes isolating a particular pulse, spatially separating individual pulses, and spreading a single pulse from an X-ray pulse-train.

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

DOE PAGES

Rouxel, Jérémy R.; Kowalewski, Markus; Mukamel, Shaul

2017-07-01

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

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rouxel, Jérémy R.; Kowalewski, Markus; Mukamel, Shaul

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

Optical laser systems at the Linac Coherent Light Source

DOE PAGES

Minitti, Michael P.; Robinson, Joseph S.; Coffee, Ryan N.; ...

2015-04-22

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump–probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump–probe experiments to be performed at LCLS.

Space-Time Characterization of Laser Plasma Interactions in the Warm Dense Matter Regime

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cao, L F; Uschmann, I; Forster, E

2008-04-30

Laser plasma interaction experiments have been performed using a fs Titanium Sapphire laser. Plasmas have been generated from planar PMMA targets using single laser pulses with 3.3 mJ pulse energy, 50 fs pulse duration at 800 nm wavelength. The electron density distributions of the plasmas in different delay times have been characterized by means of Nomarski Interferometry. Experimental data were compared with hydrodynamic simulation. First results to characterize the plasma density and temperature as a function of space and time are obtained. This work aims to generate plasmas in the warm dense matter (WDM) regime at near solid-density in anmore » ultra-fast laser target interaction process. Plasmas under these conditions can serve as targets to develop x-ray Thomson scattering as a plasma diagnostic tool, e.g., using the VUV free-electron laser (FLASH) at DESY Hamburg.« less

An adjustable short-focal length, high-gradient PMQ electron-beam final-focus system for the PLEIADES ultra-fast x-ray Thomson source

NASA Astrophysics Data System (ADS)

Lim, Jae-Ku

In the span of a 100 year since the discovery of first x-rays by Roentgen that won him the first Nobel prize in physics, several types of radiation sources have been developed. Currently, radiations at extremely short wavelengths have only been accessed at synchrotron radiation sources. However, the current 3rd generation synchrotron sources can only produce x-rays of energy up to 60 keV and pulse lengths of several picoseconds long. But needs for shorter wavelength and shorter pulse duration radiations demanded by scientists to understand the nature of matter at atomic/molecular scale initiated the new scientific research for the production of sub-picosecond, hard x-rays. At the Lawrence Livermore National Laboratory, a Thomson x-ray source in the backscattering mode---a head-on collision between a high intensity Ti:Sapphire Chirped Pulse Amplification laser and a relativistic electron beam---called the PLEIADES (Picosecond Laser-Electron Inter-Action for the Dynamical Evaluation of Structures) laboratory has been developed. Early works demonstrated the production of quasi-monochromatic, femto-second long, hard x-rays. Initially reported x-ray flux was in the low range of 105--10 6 photons per shot. During the early stage of PLEIADES experiments, 15 T/m electromagnet final focusing quadrupoles (in a triplet lattice configuration) were employed to focus the beam to a 40-50 mum spot-size. A larger focal spot-size beam has a low-density of electron particles available at the interaction with incident photons, which leads to a low scattering probability. The current dissertation shows that by employing a 560 T/m PMQ (Permanent-Magnet Quadrupole) final focus system, an electron beam as small as 10-20 mum can be achieved. The implementation of this final focus system demonstrated the improvement of the total x-ray flux by two orders of magnitude. The PMQ final focus system also produced small electron beams consistently over 30-100 MeV electron beam energy, which enabled the production of x-ray energy over 40-140 keV. In this dissertation, the PLEIADES Thomson x-ray facility will be described in detail includes the 100 MeV linac and the FALCON laser system. Later, we will discuss the design, construction and implementation of the PMQ final focus system in the beamline. The measurement of electron beam parameters before and after the final focus system will be presented. The beam measurements at the interaction region were accomplished with the use of both OTR (Optical Transition Radiation) imaged by a CCD camera and the fast streak camera for respective spatial and temporal alignments. The theoretical analysis in "real beam" effects and spacetime beam jitter effects will be given to help understand the observations. A 3D simulation tool developed for x-ray data analysis was used to provide direct comparisons with the x-ray flux, spectrum distribution and transverse x-ray profile.

Broadband ultrafast nonlinear absorption and nonlinear refraction of layered molybdenum dichalcogenide semiconductors

NASA Astrophysics Data System (ADS)

Wang, Kangpeng; Feng, Yanyan; Chang, Chunxia; Zhan, Jingxin; Wang, Chengwei; Zhao, Quanzhong; Coleman, Jonathan N.; Zhang, Long; Blau, Werner J.; Wang, Jun

2014-08-01

A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS2 and MoSe2 dispersions after higher speed centrifugation (10 000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc.A series of layered molybdenum dichalcogenides, i.e., MoX2 (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX2 dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS2 and MoSe2 dispersions after higher speed centrifugation (10 000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc. Electronic supplementary information (ESI) available: Electron scattering patterns from TEM characterizations of MX2 nanosheets; CA Z-scan results of graphene dispersions in the ps region. See DOI: 10.1039/c4nr02634a

Impact of intense x-ray pulses on a NaI(Tl)-based gamma camera

NASA Astrophysics Data System (ADS)

Koppert, W. J. C.; van der Velden, S.; Steenbergen, J. H. L.; de Jong, H. W. A. M.

2018-03-01

In SPECT/CT systems x-ray and γ-ray imaging is performed sequentially. Simultaneous acquisition may have advantages, for instance in interventional settings. However, this may expose a gamma camera to relatively high x-ray doses and deteriorate its functioning. We studied the NaI(Tl) response to x-ray pulses with a photodiode, PMT and gamma camera, respectively. First, we exposed a NaI(Tl)-photodiode assembly to x-ray pulses to investigate potential crystal afterglow. Next, we exposed a NaI(Tl)-PMT assembly to 10 ms LED pulses (mimicking x-ray pulses) and measured the response to flashing LED probe-pulses (mimicking γ-pulses). We then exposed the assembly to x-ray pulses, with detector entrance doses of up to 9 nGy/pulse, and analysed the response for γ-pulse variations. Finally, we studied the response of a Siemens Diacam gamma camera to γ-rays while exposed to x-ray pulses. X-ray exposure of the crystal, read out with a photodiode, revealed 15% afterglow fraction after 3 ms. The NaI(Tl)-PMT assembly showed disturbances up to 10 ms after 10 ms LED exposure. After x-ray exposure however, responses showed elevated baselines, with 60 ms decay-time. Both for x-ray and LED exposure and after baseline subtraction, probe-pulse analysis revealed disturbed pulse height measurements shortly after exposure. X-ray exposure of the Diacam corroborated the elementary experiments. Up to 50 ms after an x-ray pulse, no events are registered, followed by apparent energy elevations up to 100 ms after exposure. Limiting the dose to 0.02 nGy/pulse prevents detrimental effects. Conventional gamma cameras exhibit substantial dead-time and mis-registration of photon energies up to 100 ms after intense x-ray pulses. This is due PMT limitations and due to afterglow in the crystal. Using PMTs with modified circuitry, we show that deteriorative afterglow effects can be reduced without noticeable effects on the PMT performance, up to x-ray pulse doses of 1 nGy.

Photosensitivity study of GeS2 chalcogenide glass under femtosecond laser pulses irradiation

NASA Astrophysics Data System (ADS)

Ayiriveetil, Arunbabu; Sabapathy, Tamilarasan; Kar, Ajoy K.; Asokan, Sundarrajan

2015-07-01

The present study discusses the photosensitivity of GeS2 chalcogenide glass in response to irradiation with femtosecond pulses at 1047 nm. Bulk GeS2 glasses are prepared by conventional melt quenching technique and the amorphous nature of the glass is confirmed using X-ray diffraction. Ultrafast laser inscription technique is used to fabricate the straight channel waveguides in the glass. Single scan and multi scan waveguides are inscribed in GeS2 glasses of length 0.65 cm using a master oscillator power amplifier Yb doped fiber laser (IMRA μjewel D400) with different pulse energy and translation speed. Diameters of the inscribed waveguides are measured and its dependence on the inscription parameters such as translation speed and pulse energy is studied. Butt coupling method is used to characterize the loss measurement of the inscribed optical waveguides. The mode field image of the waveguides is captured using CCD camera and compared with the mode field image of a standard SMF-28 fibers.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rosenzweig, James; Andonian, Gerard; Fukasawa, Atsushi

2012-06-22

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

The LAMP instrument at the Linac Coherent Light Source free-electron laser

DOE PAGES

Osipov, Timur; Bostedt, Christoph; Castagna, J. -C.; ...

2018-03-23

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusivemore » metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here in this paper we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.« less

The LAMP instrument at the Linac Coherent Light Source free-electron laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Osipov, Timur; Bostedt, Christoph; Castagna, J. -C.

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusivemore » metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here in this paper we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.« less

Nanoscale femtosecond imaging of transient hot solid density plasmas with elemental and charge state sensitivity using resonant coherent diffraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kluge, T., E-mail: t.kluge@hzdr.de; Bussmann, M.; Huang, L. G., E-mail: lingen.huang@hzdr.de

Here, we propose to exploit the low energy bandwidth, small wavelength, and penetration power of ultrashort pulses from XFELs for resonant Small Angle Scattering (SAXS) on plasma structures in laser excited plasmas. Small angle scattering allows to detect nanoscale density fluctuations in forward scattering direction. Typically, the SAXS signal from laser excited plasmas is expected to be dominated by the free electron distribution. We propose that the ionic scattering signal becomes visible when the X-ray energy is in resonance with an electron transition between two bound states (resonant coherent X-ray diffraction). In this case, the scattering cross-section dramatically increases somore » that the signal of X-ray scattering from ions silhouettes against the free electron scattering background which allows to measure the opacity and derived quantities with high spatial and temporal resolution, being fundamentally limited only by the X-ray wavelength and timing. Deriving quantities such as ion spatial distribution, charge state distribution, and plasma temperature with such high spatial and temporal resolution will make a vast number of processes in shortpulse laser-solid interaction accessible for direct experimental observation, e.g., hole-boring and shock propagation, filamentation and instability dynamics, electron transport, heating, and ultrafast ionization dynamics.« less

Ultrafast time scale X-rotation of cold atom storage qubit using Rubidium clock states

NASA Astrophysics Data System (ADS)

Song, Yunheung; Lee, Han-Gyeol; Kim, Hyosub; Jo, Hanlae; Ahn, Jaewook

2017-04-01

Ultrafast-time-scale optical interaction is a local operation on the electronic subspace of an atom, thus leaving its nuclear state intact. However, because atomic clock states are maximally entangled states of the electronic and nuclear degrees of freedom, their entire Hilbert space should be accessible only with local operations and classical communications (LOCC). Therefore, it may be possible to achieve hyperfine qubit gates only with electronic transitions. Here we show an experimental implementation of ultrafast X-rotation of atomic hyperfine qubits, in which an optical Rabi oscillation induces a geometric phase between the constituent fine-structure states, thus bringing about the X-rotation between the two ground hyperfine levels. In experiments, cold atoms in a magneto-optical trap were controlled with a femtosecond laser pulse from a Ti:sapphire laser amplifier. Absorption imaging of the as-controlled atoms initially in the ground hyperfine state manifested polarization dependence, strongly agreeing with the theory. The result indicates that single laser pulse implementations of THz clock speed qubit controls are feasible for atomic storage qubits. Samsung Science and Technology Foundation [SSTF-BA1301-12].

Bringing PW-class lasers to XFELs (Conference Presentation)

NASA Astrophysics Data System (ADS)

Tomizawa, Hiromitsu

2017-06-01

Experimental researches using high power optical lasers combined with free electron lasers (FELs) open new frontiers in high energy density (HED) sciences. Probing and pumping capabilities are dramatically improved due to the brightness of the XFEL pulses with ultrafast duration. Besides, the peak intensities of Ti:sapphire laser Chirped Pulse Amplification (CPA) systems reach petawatt (PW)-class with operating in few tens of fs and commercially available at a few Hz of repetition rate. We have been developing an experimental platform for HED sciences using high power, high intensity optical lasers at the XFEL facility, SACLA.Currently, an experimental platform with a dual 0.5 PW Ti:Sapphire laser system is under beam commissioning for experiments combined with the SACLA's x-ray beam for research objectives that require more peak power in the optical laser pulses with a few tens of fs. The optical laser system is designed to deliver two laser beams simultaneously with the maximum power of 0.5 PW in each into a target chamber located in an experimental hutch 6 (EH6) at BL2, which was recently commissioned as a SACLA's 2nd hard x-ray beamline. A focusing capability using sets of compound refractive lenses will be applied to increase the x-ray fluence on the target sample. One of the most key issues for the integrated experimental platform is development of diagnostics that meets requirements both from the high power laser (e.g. resistance to harsh environments) and from the XFEL (e.g. adaptation to the available data acquisition system). The status and future perspective of the development including automatic laser alignment systems will be reported in the presentation. We will discuss the most promising and important new physics experiments that will be enabled by the combination of PW-class lasers and the world-class FEL's x-ray beam.

Ultrafast magnetodynamics with free-electron lasers

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Ultrafast electron microscopy in materials science, biology, and chemistry

NASA Astrophysics Data System (ADS)

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

2005-06-01

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

Dynamic fracture of tantalum under extreme tensile stress

DOE PAGES

Albertazzi, Bruno; Ozaki, Norimasa; Zhakhovsky, Vasily; ...

2017-06-02

The understanding of fracture phenomena of a material at extremely high strain rates is a key issue for a wide variety of scientific research ranging from applied science and technological developments to fundamental science such as laser-matter interaction and geology. Despite its interest, its study relies on a fine multiscale description, in between the atomic scale and macroscopic processes, so far only achievable by large-scale atomic simulations. Direct ultrafast real-time monitoring of dynamic fracture (spallation) at the atomic lattice scale with picosecond time resolution was beyond the reach of experimental techniques. We show that the coupling between a high-power opticalmore » laser pump pulse and a femtosecond x-ray probe pulse generated by an x-ray free electron laser allows detection of the lattice dynamics in a tantalum foil at an ultrahigh strain rate of Embedded Image ~2 × 10 8 to 3.5 × 10 8 s -1. A maximal density drop of 8 to 10%, associated with the onset of spallation at a spall strength of ~17 GPa, was directly measured using x-ray diffraction. The experimental results of density evolution agree well with large-scale atomistic simulations of shock wave propagation and fracture of the sample. Our experimental technique opens a new pathway to the investigation of ultrahigh strain-rate phenomena in materials at the atomic scale, including high-speed crack dynamics and stress-induced solid-solid phase transitions.« less

Nanometer-scale characterization of laser-driven plasmas, compression, shocks and phase transitions, by coherent small angle x-ray scattering

NASA Astrophysics Data System (ADS)

Kluge, Thomas

2015-11-01

Combining ultra-intense short-pulse and high-energy long-pulse lasers, with brilliant coherent hard X-ray FELs, such as the Helmholtz International Beamline for Extreme Fields (HIBEF) under construction at the HED Instrument of European XFEL, or MEC at LCLS, holds the promise to revolutionize our understanding of many High Energy Density Physics phenomena. Examples include the relativistic electron generation, transport, and bulk plasma response, and ionization dynamics and heating in relativistic laser-matter interactions, or the dynamics of laser-driven shocks, quasi-isentropic compression, and the kinetics of phase transitions at high pressure. A particularly promising new technique is the use of coherent X-ray diffraction to characterize electron density correlations, and by resonant scattering to characterize the distribution of specific charge-state ions, either on the ultrafast time scale of the laser interaction, or associated with hydrodynamic motion. As well one can image slight density changes arising from phase transitions inside of shock-compressed high pressure matter. The feasibility of coherent diffraction techniques in laser-driven matter will be discussed. including recent results from demonstration experiments at MEC. Among other things, very sharp density changes from laser-driven compression are observed, having an effective step width of 10 nm or smaller. This compares to a resolution of several hundred nm achievedpreviously with phase contrast imaging. and on behalf of HIBEF User Consortium, for the Helmholtz International Beamline for Extreme Fields at the European XFEL.

EDITORIAL: Attosecond and x-ray free-electron laser physics Attosecond and x-ray free-electron laser physics

NASA Astrophysics Data System (ADS)

Moshammer, R.; Ullrich, J.

2009-07-01

Currently, we are witnessing a revolution in photon science, driven by the vision to time-resolve ultra-fast electronic motion in atoms, molecules, and solids as well as by the quest for the characterization of time-dependent structural changes in large molecules and solids. Quantum jumps in the development of light sources are the key technologies for this emerging field of research. Thus, high harmonic radiation bursts now penetrate the attosecond (10-18 s) regime and free-electron lasers (FELs) deliver ultra-brilliant femtosecond, coherent VUV and x-ray pulses. This special issue presents a snapshot of this ongoing revolution and brings together, for the first time, pioneering results in both of these fields that are expected to evolve synergetically in the future. The volume is based on the spirit of the International Conference on Multi-Photon Processes, ICOMP08, which was held at the Max Planck Institute for Nuclear Physics in Heidelberg in summer 2008. The first contributions include articles that envision tracing electronic motion on an attosecond time scale and its relation to nuclear motion. After more technical papers on the generation of attosecond pulses via high harmonic generation (HHG), molecular and two-electron atomic dynamics in strong optical fields at a typical wavelength of 800 nm are presented pointing to sub-cycle, attosecond features. Making the transition to shorter wavelengths, nonlinear dynamics in atoms and molecules is explored via experimental and theoretical methods, where the present measurements are nearly exclusively performed at FEL sources. A substantial number of articles focus on the investigation of the most simple many- (few-) photon two-electron processes in double ionization of helium at optical and VUV wavelengths, with the goal of characterizing this fundamental reaction, not yet consistently solved theoretically, in spite of huge efforts. Finally, the behaviour of more complex nanoscaled systems, i.e. clusters, is investigated bridging the gap from atoms and molecules to solids introduced to intense FEL radiation. Beyond the basic interest in many-particle dynamics in finite systems, these studies are of enormous practical relevance for upcoming research at X-ray FELs. Here, realizing the dream of coherent imaging of the structure of single bio-molecules in the gas phase with atomic resolution is critically dependent on ultra-fast dynamics initiated by the pulse. In other words, it is reduced to the simple question of whether the molecule is first imaged and then destroyed or vice versa! During the preparation of this Editorial, the first lasing at the Stanford Linac Coherent Light Source (LCLS) was achieved at a photon energy of about 8 keV - a further milestone in this exciting revolution in the science related to light.

Terahertz Streaking of Few-Femtosecond Relativistic Electron Beams

NASA Astrophysics Data System (ADS)

Zhao, Lingrong; Wang, Zhe; Lu, Chao; Wang, Rui; Hu, Cheng; Wang, Peng; Qi, Jia; Jiang, Tao; Liu, Shengguang; Ma, Zhuoran; Qi, Fengfeng; Zhu, Pengfei; Cheng, Ya; Shi, Zhiwen; Shi, Yanchao; Song, Wei; Zhu, Xiaoxin; Shi, Jiaru; Wang, Yingxin; Yan, Lixin; Zhu, Liguo; Xiang, Dao; Zhang, Jie

2018-04-01

Streaking of photoelectrons with optical lasers has been widely used for temporal characterization of attosecond extreme ultraviolet pulses. Recently, this technique has been adapted to characterize femtosecond x-ray pulses in free-electron lasers with the streaking imprinted by far-infrared and terahertz (THz) pulses. Here, we report successful implementation of THz streaking for time stamping of an ultrashort relativistic electron beam, whose energy is several orders of magnitude higher than photoelectrons. Such an ability is especially important for MeV ultrafast electron diffraction (UED) applications, where electron beams with a few femtosecond pulse width may be obtained with longitudinal compression, while the arrival time may fluctuate at a much larger timescale. Using this laser-driven THz streaking technique, the arrival time of an ultrashort electron beam with a 6-fs (rms) pulse width has been determined with 1.5-fs (rms) accuracy. Furthermore, we have proposed and demonstrated a noninvasive method for correction of the timing jitter with femtosecond accuracy through measurement of the compressed beam energy, which may allow one to advance UED towards a sub-10-fs frontier, far beyond the approximate 100-fs (rms) jitter.

Ultrafast nanoscale imaging using high order harmonic generation (Conference Presentation)

NASA Astrophysics Data System (ADS)

Merdji, Hamed

2017-05-01

Ultrafast coherent diffraction using soft and hard X-rays is actually revolutionizing imaging science thanks to new sources recently available. This powerful technique extends standard X-ray diffraction towards imaging of non-crystalline objects and leads actually to a strong impact in physics, chemistry and biology. New ultrashort pulses recently available hold the promise of watching matter evolving with unprecedented space and time resolution. Femtosecond coherent and intense radiation in the soft X-ray (λ = 10-40 nm) is currently produced in our laboratory, from highly non linear frequency conversion (high harmonic generation). A high intensity UV-X coherent beam is obtained using a loose focusing geometry, which allows coupling a very high amount of Ti:Sapphire laser system energy in the HHG process. Using a long gas cell and a long focal length lens, the emitting volume can be increased by orders of magnitude compared to standard HHG set-ups. This approach, allows reaching up to 1x1011 photons per shot for the 25th harmonic (λ=32nm). We have already demonstrated nanoscale imaging in a single shot mode reaching 70 nm spatial resolution and 20 femtoseconds snapshot [1]. We then implemented a recently proposed holographic technique using extended references. This technique, easy to implement, allows a direct non iterative image reconstruction. In the single shot regime, we demonstrated a spatial resolution of 110nm [2].This opens fascinating perspectives in imaging dynamical phenomena to be spread over a large scientific community. I will present recent results in the investigation of femtosecond phase spin-reversals of magnetic nano-domains [3]. Finally, I will report on recent development on noise sensitivity of the technique and perspectives in attosecond coherent imaging [4]. [1] A. Ravasio et al., Physical Review Letters 103, 028104 (2009). [2] D. Gauthier et al., Physical Review Letters 105, 093901 (2010). [3] Vodungbo et al., Nature Communications 3, 999 (2012) [4] Williams et al., Optics Letters 40 (13), 3205 (2015)

Temporal lenses for attosecond and femtosecond electron pulses

PubMed Central

Hilbert, Shawn A.; Uiterwaal, Cornelis; Barwick, Brett; Batelaan, Herman; Zewail, Ahmed H.

2009-01-01

Here, we describe the “temporal lens” concept that can be used for the focus and magnification of ultrashort electron packets in the time domain. The temporal lenses are created by appropriately synthesizing optical pulses that interact with electrons through the ponderomotive force. With such an arrangement, a temporal lens equation with a form identical to that of conventional light optics is derived. The analog of ray diagrams, but for electrons, are constructed to help the visualization of the process of compressing electron packets. It is shown that such temporal lenses not only compensate for electron pulse broadening due to velocity dispersion but also allow compression of the packets to durations much shorter than their initial widths. With these capabilities, ultrafast electron diffraction and microscopy can be extended to new domains,and, just as importantly, electron pulses can be delivered directly on an ultrafast techniques target specimen. PMID:19541639

Intensity correlation measurement system by picosecond single shot soft x-ray laser.

PubMed

Kishimoto, Maki; Namikawa, Kazumichi; Sukegawa, Kouta; Yamatani, Hiroshi; Hasegawa, Noboru; Tanaka, Momoko

2010-01-01

We developed a new soft x-ray speckle intensity correlation spectroscopy system by use of a single shot high brilliant plasma soft x-ray laser. The plasma soft x-ray laser is characterized by several picoseconds in pulse width, more than 90% special coherence, and 10(11) soft x-ray photons within a single pulse. We developed a Michelson type delay pulse generator using a soft x-ray beam splitter to measure the intensity correlation of x-ray speckles from materials and succeeded in generating double coherent x-ray pulses with picosecond delay times. Moreover, we employed a high-speed soft x-ray streak camera for the picosecond time-resolved measurement of x-ray speckles caused by double coherent x-ray pulse illumination. We performed the x-ray speckle intensity correlation measurements for probing the relaxation phenomena of polarizations in polarization clusters in the paraelectric phase of the ferroelectric material BaTiO(3) near its Curie temperature and verified its performance.

Method for spatially modulating X-ray pulses using MEMS-based X-ray optics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lopez, Daniel; Shenoy, Gopal; Wang, Jin

A method and apparatus are provided for spatially modulating X-rays or X-ray pulses using microelectromechanical systems (MEMS) based X-ray optics. A torsionally-oscillating MEMS micromirror and a method of leveraging the grazing-angle reflection property are provided to modulate X-ray pulses with a high-degree of controllability.

Physical mechanisms of SiN{sub x} layer structuring with ultrafast lasers by direct and confined laser ablation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rapp, S., E-mail: rapp@hm.edu; Erlangen Graduate School in Advanced Optical Technologies; Heinrich, G.

2015-03-14

In the production process of silicon microelectronic devices and high efficiency silicon solar cells, local contact openings in thin dielectric layers are required. Instead of photolithography, these openings can be selectively structured with ultra-short laser pulses by confined laser ablation in a fast and efficient lift off production step. Thereby, the ultrafast laser pulse is transmitted by the dielectric layer and absorbed at the substrate surface leading to a selective layer removal in the nanosecond time domain. Thermal damage in the substrate due to absorption is an unwanted side effect. The aim of this work is to obtain a deepermore » understanding of the physical laser-material interaction with the goal of finding a damage-free ablation mechanism. For this, thin silicon nitride (SiN{sub x}) layers on planar silicon (Si) wafers are processed with infrared fs-laser pulses. Two ablation types can be distinguished: The known confined ablation at fluences below 300 mJ/cm{sup 2} and a combined partial confined and partial direct ablation at higher fluences. The partial direct ablation process is caused by nonlinear absorption in the SiN{sub x} layer in the center of the applied Gaussian shaped laser pulses. Pump-probe investigations of the central area show ultra-fast reflectivity changes typical for direct laser ablation. Transmission electron microscopy results demonstrate that the Si surface under the remaining SiN{sub x} island is not damaged by the laser ablation process. At optimized process parameters, the method of direct laser ablation could be a good candidate for damage-free selective structuring of dielectric layers on absorbing substrates.« less

New Directions in X-Ray Light Sources

ScienceCinema

Falcone, Roger

2017-12-09

July 15, 2008 Berkeley Lab lecture: Molecular movies of chemical reactions and material phase transformations need a strobe of x-rays, the penetrating light that reveals how atoms and molecules assemble in chemical and biological systems and complex materials. Roger Falcone, Director of the Advanced Light Source,will discuss a new generation of x ray sources that will enable a new science of atomic dynamics on ultrafast timescales.

Application of MEMS-based x-ray optics as tuneable nanosecond choppers

NASA Astrophysics Data System (ADS)

Chen, Pice; Walko, Donald A.; Jung, Il Woong; Li, Zhilong; Gao, Ya; Shenoy, Gopal K.; Lopez, Daniel; Wang, Jin

2017-08-01

Time-resolved synchrotron x-ray measurements often rely on using a mechanical chopper to isolate a set of x-ray pulses. We have started the development of micro electromechanical systems (MEMS)-based x-ray optics, as an alternate method to manipulate x-ray beams. In the application of x-ray pulse isolation, we recently achieved a pulse-picking time window of half a nanosecond, which is more than 100 times faster than mechanical choppers can achieve. The MEMS device consists of a comb-drive silicon micromirror, designed for efficiently diffracting an x-ray beam during oscillation. The MEMS devices were operated in Bragg geometry and their oscillation was synchronized to x-ray pulses, with a frequency matching subharmonics of the cycling frequency of x-ray pulses. The microscale structure of the silicon mirror in terms of the curvature and the quality of crystallinity ensures a narrow angular spread of the Bragg reflection. With the discussion of factors determining the diffractive time window, this report showed our approaches to narrow down the time window to half a nanosecond. The short diffractive time window will allow us to select single x-ray pulse out of a train of pulses from synchrotron radiation facilities.

Beating Darwin-Bragg losses in lab-based ultrafast x-ray experiments

PubMed Central

Fullagar, Wilfred K.; Uhlig, Jens; Mandal, Ujjwal; Kurunthu, Dharmalingam; El Nahhas, Amal; Tatsuno, Hideyuki; Honarfar, Alireza; Parnefjord Gustafsson, Fredrik; Sundström, Villy; Palosaari, Mikko R. J.; Kinnunen, Kimmo M.; Maasilta, Ilari J.; Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young Il; Swetz, Daniel S.; Ullom, Joel N.

2017-01-01

The use of low temperature thermal detectors for avoiding Darwin-Bragg losses in lab-based ultrafast experiments has begun. An outline of the background of this new development is offered, showing the relevant history and initiative taken by this work. PMID:28396880

Watching ultrafast responses of structure and magnetism in condensed matter with momentum-resolved probes

PubMed Central

Johnson, S. L.; Savoini, M.; Beaud, P.; Ingold, G.; Staub, U.; Carbone, F.; Castiglioni, L.; Hengsberger, M.; Osterwalder, J.

2017-01-01

We present a non-comprehensive review of some representative experimental studies in crystalline condensed matter systems where the effects of intense ultrashort light pulses are probed using x-ray diffraction and photoelectron spectroscopy. On an ultrafast (sub-picosecond) time scale, conventional concepts derived from the assumption of thermodynamic equilibrium must often be modified in order to adequately describe the time-dependent changes in material properties. There are several commonly adopted approaches to this modification, appropriate in different experimental circumstances. One approach is to treat the material as a collection of quasi-thermal subsystems in thermal contact with each other in the so-called “N-temperature” models. On the other extreme, one can also treat the time-dependent changes as fully coherent dynamics of a sometimes complex network of excitations. Here, we present examples of experiments that fall into each of these categories, as well as experiments that partake of both models. We conclude with a discussion of the limitations and future potential of these concepts. PMID:29308418

The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering

PubMed Central

Barke, Ingo; Hartmann, Hannes; Rupp, Daniela; Flückiger, Leonie; Sauppe, Mario; Adolph, Marcus; Schorb, Sebastian; Bostedt, Christoph; Treusch, Rolf; Peltz, Christian; Bartling, Stephan; Fennel, Thomas; Meiwes-Broer, Karl-Heinz; Möller, Thomas

2015-01-01

The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncovered from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science. PMID:25650004

The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Barke, Ingo; Hartmann, Hannes; Rupp, Daniela

The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncoveredmore » from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science« less

Beyond a phenomenological description of magnetostriction

DOE PAGES

Reid, A. H.; Shen, X.; Maldonado, P.; ...

2018-01-26

Magnetostriction, the strain induced by a change in magnetization, is a universal effect in magnetic materials. Owing to the difficulty in unraveling its microscopic origin, it has been largely treated phenomenologically. Here in this paper, we show how the source of magnetostriction—the underlying magnetoelastic stress—can be separated in the time domain, opening the door for an atomistic understanding. X-ray and electron diffraction are used to separate the sub-picosecond spin and lattice responses of FePt nanoparticles. Following excitation with a 50-fs laser pulse, time-resolved X-ray diffraction demonstrates that magnetic order is lost within the nanoparticles with a time constant of 146more » fs. Ultrafast electron diffraction reveals that this demagnetization is followed by an anisotropic, three-dimensional lattice motion. Analysis of the size, speed, and symmetry of the lattice motion, together with ab initio calculations accounting for the stresses due to electrons and phonons, allow us to reveal the magnetoelastic stress generated by demagnetization.« less

Terahertz-driven linear electron acceleration

PubMed Central

Nanni, Emilio A.; Huang, Wenqian R.; Hong, Kyung-Han; Ravi, Koustuban; Fallahi, Arya; Moriena, Gustavo; Dwayne Miller, R. J.; Kärtner, Franz X.

2015-01-01

The cost, size and availability of electron accelerators are dominated by the achievable accelerating gradient. Conventional high-brightness radio-frequency accelerating structures operate with 30–50 MeV m−1 gradients. Electron accelerators driven with optical or infrared sources have demonstrated accelerating gradients orders of magnitude above that achievable with conventional radio-frequency structures. However, laser-driven wakefield accelerators require intense femtosecond sources and direct laser-driven accelerators suffer from low bunch charge, sub-micron tolerances and sub-femtosecond timing requirements due to the short wavelength of operation. Here we demonstrate linear acceleration of electrons with keV energy gain using optically generated terahertz pulses. Terahertz-driven accelerating structures enable high-gradient electron/proton accelerators with simple accelerating structures, high repetition rates and significant charge per bunch. These ultra-compact terahertz accelerators with extremely short electron bunches hold great potential to have a transformative impact for free electron lasers, linear colliders, ultrafast electron diffraction, X-ray science and medical therapy with X-rays and electron beams. PMID:26439410

Terahertz-driven linear electron acceleration

DOE PAGES

Nanni, Emilio A.; Huang, Wenqian R.; Hong, Kyung-Han; ...

2015-10-06

The cost, size and availability of electron accelerators are dominated by the achievable accelerating gradient. Conventional high-brightness radio-frequency accelerating structures operate with 30–50 MeVm -1 gradients. Electron accelerators driven with optical or infrared sources have demonstrated accelerating gradients orders of magnitude above that achievable with conventional radio-frequency structures. However, laser-driven wakefield accelerators require intense femtosecond sources and direct laser-driven accelerators suffer from low bunch charge, sub-micron tolerances and sub-femtosecond timing requirements due to the short wavelength of operation. Here we demonstrate linear acceleration of electrons with keV energy gain using optically generated terahertz pulses. Terahertz-driven accelerating structures enable high-gradient electron/protonmore » accelerators with simple accelerating structures, high repetition rates and significant charge per bunch. As a result, these ultra-compact terahertz accelerators with extremely short electron bunches hold great potential to have a transformative impact for free electron lasers, linear colliders, ultrafast electron diffraction, X-ray science and medical therapy with X-rays and electron beams.« less

The 3D-architecture of individual free silver nanoparticles captured by X-ray scattering

DOE PAGES

Barke, Ingo; Hartmann, Hannes; Rupp, Daniela; ...

2015-02-04

The diversity of nanoparticle shapes generated by condensation from gaseous matter reflects the fundamental competition between thermodynamic equilibration and the persistence of metastable configurations during growth. In the kinetically limited regime, intermediate geometries that are favoured only in early formation stages can be imprinted in the finally observed ensemble of differently structured specimens. Here we demonstrate that single-shot wide-angle scattering of femtosecond soft X-ray free-electron laser pulses allows three-dimensional characterization of the resulting metastable nanoparticle structures. For individual free silver particles, which can be considered frozen in space for the duration of photon exposure, both shape and orientation are uncoveredmore » from measured scattering images. We identify regular shapes, including species with fivefold symmetry and surprisingly large aspect ratio up to particle radii of the order of 100 nm. Our approach includes scattering effects beyond Born’s approximation and is remarkably efficient—opening up new routes in ultrafast nanophysics and free-electron laser science« less

Ultrafast Absorption Spectroscopy of Aluminum Plasmas Created by LCLS using Betatron X-Ray Radiation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Albert, Felicie

2016-10-12

This document summarizes the goals and accomplishments of a six month-long LDRD project, awarded through the LLNL director Early and Mid Career Recognition (EMCR) program. This project allowed us to support beamtime awarded at the Matter under Extreme Conditions (MEC) end station of the Linac Coherent Light Source (LCLS). The goal of the experiment was to heat metallic samples with the bright x-rays from the LCLS free electron laser. Then, we studied how they relaxed back to equilibrium by probing them with ultrafast x-ray absorption spectroscopy using laser-based betatron radiation. Our work enabled large collaborations between LLNL, SLAC, LBNL, andmore » institutions in France and in the UK, while providing training to undergraduate and graduate students during the experiment. Following this LDRD project, the PI was awarded a 5-year DOE early career research grant to further develop applications of laser-driven x-ray sources for high energy density science experiments and warm dense matter states.« less

New Directions in X-Ray Light Sources or Fiat Lux: what's under the dome and watching atoms with x-rays (LBNL Summer Lecture Series)

ScienceCinema

Falcone, Roger [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Berkeley, CA (United States). Dept. of Physics

2018-05-04

Summer Lecture Series 2008: Molecular movies of chemical reactions and material phase transformations need a strobe of x-rays, the penetrating light that reveals how atoms and molecules assemble in chemical and biological systems and complex materials. Roger Falcone, Director of the Advanced Light Source,will discuss a new generation of x ray sources that will enable a new science of atomic dynamics on ultrafast timescales.

Spin-vibronic quantum dynamics for ultrafast excited-state processes.

PubMed

Eng, Julien; Gourlaouen, Christophe; Gindensperger, Etienne; Daniel, Chantal

2015-03-17

Ultrafast intersystem crossing (ISC) processes coupled to nuclear relaxation and solvation dynamics play a central role in the photophysics and photochemistry of a wide range of transition metal complexes. These phenomena occurring within a few hundred femtoseconds are investigated experimentally by ultrafast picosecond and femtosecond transient absorption or luminescence spectroscopies, and optical laser pump-X-ray probe techniques using picosecond and femtosecond X-ray pulses. The interpretation of ultrafast structural changes, time-resolved spectra, quantum yields, and time scales of elementary processes or transient lifetimes needs robust theoretical tools combining state-of-the-art quantum chemistry and developments in quantum dynamics for solving the electronic and nuclear problems. Multimode molecular dynamics beyond the Born-Oppenheimer approximation has been successfully applied to many small polyatomic systems. Its application to large molecules containing a transition metal atom is still a challenge because of the nuclear dimensionality of the problem, the high density of electronic excited states, and the spin-orbit coupling effects. Rhenium(I) α-diimine carbonyl complexes, [Re(L)(CO)3(N,N)](n+) are thermally and photochemically robust and highly flexible synthetically. Structural variations of the N,N and L ligands affect the spectroscopy, the photophysics, and the photochemistry of these chromophores easily incorporated into a complex environment. Visible light absorption opens the route to a wide range of applications such as sensors, probes, or emissive labels for imaging biomolecules. Halide complexes [Re(X)(CO)3(bpy)] (X = Cl, Br, or I; bpy = 2,2'-bipyridine) exhibit complex electronic structure and large spin-orbit effects that do not correlate with the heavy atom effects. Indeed, the (1)MLCT → (3)MLCT intersystem crossing (ISC) kinetics is slower than in [Ru(bpy)3](2+) or [Fe(bpy)3](2+) despite the presence of a third-row transition metal. Counterintuitively, singlet excited-state lifetime increases on going from Cl (85 fs) to Br (128 fs) and to I (152 fs). Moreover, correlation between the Re-X stretching mode and the rate of ISC is observed. In this Account, we emphasize on the role of spin-vibronic coupling on the mechanism of ultrafast ISC put in evidence in [Re(Br)(CO)3(bpy)]. For this purpose, we have developed a model Hamiltonian for solving an 11 electronic excited states multimode problem including vibronic and SO coupling within the linear vibronic coupling (LVC) approximation and the assumption of harmonic potentials. The presence of a central metal atom coupled to rigid ligands, such as α-diimine, ensures nuclear motion of small amplitudes and a priori justifies the use of the LVC model. The simulation of the ultrafast dynamics by wavepacket propagations using the multiconfiguration time-dependent Hartree (MCTDH) method is based on density functional theory (DFT), and its time-dependent extension to excited states (TD-DFT) electronic structure data. We believe that the interplay between time-resolved experiments and these pioneering simulations covering the first picoseconds and including spin-vibronic coupling will promote a number of quantum dynamical studies that will contribute to a better understanding of ultrafast processes in a wide range of organic and inorganic chromophores easily incorporated in biosystems or supramolecular devices for specific functions.

Extreme degree of ionization in homogenous micro-capillary plasma columns heated by ultrafast current pulses.

PubMed

Avaria, G; Grisham, M; Li, J; Tomasel, F G; Shlyaptsev, V N; Busquet, M; Woolston, M; Rocca, J J

2015-03-06

Homogeneous plasma columns with ionization levels typical of megaampere discharges are created by rapidly heating gas-filled 520-μm-diameter channels with nanosecond rise time current pulses of 40 kA. Current densities of up to 0.3  GA cm^{-2} greatly increase Joule heating with respect to conventional capillary discharge Z pinches, reaching unprecedented degrees of ionization for a high-Z plasma column heated by a current pulse of remarkably low amplitude. Dense xenon plasmas are ionized to Xe^{28+}, while xenon impurities in hydrogen discharges reach Xe^{30+}. The unique characteristics of these hot, ∼300:1 length-to-diameter aspect ratio plasmas allow the observation of unexpected spectroscopic phenomena. Axial spectra show the unusual dominance of the intercombination line over the resonance line of He-like Al by nearly an order of magnitude, caused by differences in opacities in the axial and radial directions. These plasma columns could enable the development of sub-10-nm x-ray lasers.

Enhanced water window x-ray emission from in situ formed carbon clusters irradiated by intense ultra-short laser pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chakravarty, U.; Rao, B. S.; Arora, V.

Enhanced water window x-ray emission (23–44 Å) from carbon clusters, formed in situ using a pre-pulse, irradiated by intense (I > 10{sup 17} W/cm{sup 2}) ultra-short laser pulse, is demonstrated. An order of magnitude x-ray enhancement over planar graphite target is observed in carbon clusters, formed by a sub-ns pre-pulse, interacting with intense main pulse after a delay. The effect of the delay and the duration of the main pulse is studied for optimizing the x-ray emission in the water window region. This x-ray source has added advantages of being an efficient, high repetition rate, and low debris x-ray source.

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

DOE PAGES

Levantino, Matteo; Schirò, Giorgio; Lemke, Henrik Till; ...

2015-04-02

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

The X-ray Fluorescence Microscopy Beamline at the Australian Synchrotron

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paterson, D.; Jonge, M. D. de; Howard, D. L.

2011-09-09

A hard x-ray micro-nanoprobe has commenced operation at the Australian Synchrotron providing versatile x-ray fluorescence microscopy across an incident energy range from 4 to 25 keV. Two x-ray probes are used to collect {mu}-XRF and {mu}-XANES for elemental and chemical microanalysis: a Kirkpatrick-Baez mirror microprobe for micron resolution studies and a Fresnel zone plate nanoprobe capable of 60-nm resolution. Some unique aspects of the beamline design and operation are discussed. An advanced energy dispersive x-ray fluorescence detection scheme named Maia has been developed for the beamline, which enables ultrafast x-ray fluorescence microscopy.

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

NASA Astrophysics Data System (ADS)

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

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

Discovery of an Ultraviolet Counterpart to an Ultrafast X-Ray Outflow in the Quasar PG 1211+143

NASA Astrophysics Data System (ADS)

Kriss, Gerard A.; Lee, Julia C.; Danehkar, Ashkbiz; Nowak, Michael A.; Fang, Taotao; Hardcastle, Martin J.; Neilsen, Joseph; Young, Andrew

2018-02-01

We observed the quasar PG 1211+143 using the Cosmic Origins Spectrograph on the Hubble Space Telescope in 2015 April as part of a joint campaign with the Chandra X-ray Observatory and the Jansky Very Large Array. Our ultraviolet spectra cover the wavelength range 912–2100 Å. We find a broad absorption feature (∼ 1080 {km} {{{s}}}-1) at an observed wavelength of 1240 Å. Interpreting this as H I Lyα, in the rest frame of PG 1211+143 (z = 0.0809), this corresponds to an outflow velocity of ‑16,980 {km} {{{s}}}-1 (outflow redshift {z}{out}∼ -0.0551), matching the moderate ionization X-ray absorption system detected in our Chandra observation and reported previously by Pounds et al. With a minimum H I column density of {log} {N}{{H}{{I}}}> 14.5, and no absorption in other UV resonance lines, this Lyα absorber is consistent with arising in the same ultrafast outflow as the X-ray absorbing gas. The Lyα feature is weak or absent in archival ultraviolet spectra of PG 1211+143, strongly suggesting that this absorption is transient, and intrinsic to PG 1211+143. Such a simultaneous detection in two independent wavebands for the first time gives strong confirmation of the reality of an ultrafast outflow in an active galactic nucleus.

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources.

PubMed

Pincelli, T; Petrov, V N; Brajnik, G; Ciprian, R; Lollobrigida, V; Torelli, P; Krizmancic, D; Salvador, F; De Luisa, A; Sergo, R; Gubertini, A; Cautero, G; Carrato, S; Rossi, G; Panaccione, G

2016-03-01

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric and magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources

NASA Astrophysics Data System (ADS)

Pincelli, T.; Petrov, V. N.; Brajnik, G.; Ciprian, R.; Lollobrigida, V.; Torelli, P.; Krizmancic, D.; Salvador, F.; De Luisa, A.; Sergo, R.; Gubertini, A.; Cautero, G.; Carrato, S.; Rossi, G.; Panaccione, G.

2016-03-01

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric and magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pincelli, T., E-mail: pincelli@iom.cnr.it; Rossi, G.; Laboratorio TASC, IOM-CNR, S.S. 14 km 163.5, Basovizza, 34149 Trieste

2016-03-15

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric andmore » magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).« less

Broadband ultrafast nonlinear absorption and nonlinear refraction of layered molybdenum dichalcogenide semiconductors.

PubMed

Wang, Kangpeng; Feng, Yanyan; Chang, Chunxia; Zhan, Jingxin; Wang, Chengwei; Zhao, Quanzhong; Coleman, Jonathan N; Zhang, Long; Blau, Werner J; Wang, Jun

2014-09-21

A series of layered molybdenum dichalcogenides, i.e., MoX₂ (X = S, Se and Te), were prepared in cyclohexyl pyrrolidinone by a liquid-phase exfoliation technique. The high quality of the two-dimensional nanostructures was verified by transmission electron microscopy and absorption spectroscopy. Open- and closed-aperture Z-scans were employed to study the nonlinear absorption and nonlinear refraction of the MoX₂ dispersions, respectively. All the three-layered nanostructures exhibit prominent ultrafast saturable absorption (SA) for both femtosecond (fs) and picosecond (ps) laser pulses over a broad wavelength range from the visible to the near infrared. While the dispersions treated with low-speed centrifugation (1500 rpm) have an SA response, and the MoS₂ and MoSe₂ dispersions after higher speed centrifugation (10,000 rpm) possess two-photon absorption for fs pulses at 1030 nm, which is due to the significant reduction of the average thickness of the nanosheets; hence, the broadening of band gap. In addition, all dispersions show obvious nonlinear self-defocusing for ps pulses at both 1064 nm and 532 nm, resulting from the thermally-induced nonlinear refractive index. The versatile ultrafast nonlinear properties imply a huge potential of the layered MoX2 semiconductors in the development of nanophotonic devices, such as mode-lockers, optical limiters, optical switches, etc.

Generation of first hard X-ray pulse at Tsinghua Thomson Scattering X-ray Source.

PubMed

Du, Yingchao; Yan, Lixin; Hua, Jianfei; Du, Qiang; Zhang, Zhen; Li, Renkai; Qian, Houjun; Huang, Wenhui; Chen, Huaibi; Tang, Chuanxiang

2013-05-01

Tsinghua Thomson Scattering X-ray Source (TTX) is the first-of-its-kind dedicated hard X-ray source in China based on the Thomson scattering between a terawatt ultrashort laser and relativistic electron beams. In this paper, we report the experimental generation and characterization of the first hard X-ray pulses (51.7 keV) via head-on collision of an 800 nm laser and 46.7 MeV electron beams. The measured yield is 1.0 × 10(6) per pulse with an electron bunch charge of 200 pC and laser pulse energy of 300 mJ. The angular intensity distribution and energy spectra of the X-ray pulse are measured with an electron-multiplying charge-coupled device using a CsI scintillator and silicon attenuators. These measurements agree well with theoretical and simulation predictions. An imaging test using the X-ray pulse at the TTX is also presented.

Femtosecond profiling of shaped x-ray pulses

NASA Astrophysics Data System (ADS)

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.

Ultrafast compression of graphite observed with sub-ps time resolution diffraction on LCLS

NASA Astrophysics Data System (ADS)

Armstrong, Michael; Goncharov, A.; Crowhurst, J.; Zaug, J.; Radousky, H.; Grivickas, P.; Bastea, S.; Goldman, N.; Stavrou, E.; Belof, J.; Gleason, A.; Lee, H. J.; Nagler, R.; Holtgrewe, N.; Walter, P.; Pakaprenka, V.; Nam, I.; Granados, E.; Presher, C.; Koroglu, B.

2017-06-01

We will present ps time resolution pulsed x-ray diffraction measurements of rapidly compressed highly oriented pyrolytic graphite along its basal plane at the Materials under Extreme Conditions (MEC) sector of the Linac Coherent Light Source (LCLS). These experiments explore the possibility of rapid (<100 ps time scale) material transformations occurring under very highly anisotropic compression conditions. Under such conditions, non-equilibrium mechanisms may play a role in the transformation process. We will present experimental results and simulations which explore this possibility. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Security, LLC under Contract DE-AC52-07NA27344.

Ultrafast dynamics of localized magnetic moments in the unconventional Mott insulator Sr 2IrO 4

DOE PAGES

Krupin, O.; Dakovski, G. L.; Kim, B. J.; ...

2016-06-16

Here, we report a time-resolved study of the ultrafast dynamics of the magnetic moments formed by themore » $${{J}_{\\text{eff}}}=1/2$$ states in Sr 2IrO 4 by directly probing the localized iridium 5d magnetic state through resonant x-ray diffraction. Using optical pump–hard x-ray probe measurements, two relaxation time scales were determined: a fast fluence-independent relaxation is found to take place on a time scale of 1.5 ps, followed by a slower relaxation on a time scale of 500 ps–1.5 ns.« less

Optimal Pulse Processing, Pile-Up Decomposition, and Applications of Silicon Drift Detectors at LCLS

DOE PAGES

Blaj, G.; Kenney, C. J.; Dragone, A.; ...

2017-10-11

Silicon drift detectors (SDDs) revolutionized spectroscopy in fields as diverse as geology and dentistry. For a subset of experiments at ultrafast, X-ray free-electron lasers (FELs), SDDs can make substantial contributions. Often the unknown spectrum is interesting, carrying science data, or the background measurement is useful to identify unexpected signals. Many measurements involve only several discrete photon energies known a priori, allowing single-event decomposition of pile-up and spectroscopic photon counting. We designed a pulse function and demonstrated that the signal amplitude (i.e., proportional to the detected energy and obtained from fitting with the pulse function), rise time, and pulse height aremore » interrelated, and at short peaking times, the pulse height and pulse area are not optimal estimators for detected energy; instead, the signal amplitude and rise time are obtained for each pulse by fitting, thus removing the need for pulse shaping. By avoiding pulse shaping, rise times of tens of nanoseconds resulted in reduced pulse pile-up and allowed decomposition of remaining pulse pile-up at photon separation times down to hundreds of nanoseconds while yielding time-of-arrival information with the precision of 10 ns. Waveform fitting yields simultaneously high energy resolution and high counting rates (two orders of magnitude higher than current digital pulse processors). At pulsed sources or high photon rates, photon pile-up still occurs. We showed that pile-up spectrum fitting is relatively simple and preferable to pile-up spectrum deconvolution. We then developed a photon pile-up statistical model for constant intensity sources, extended it to variable intensity sources (typical for FELs), and used it to fit a complex pileup spectrum. We subsequently developed a Bayesian pile-up decomposition method that allows decomposing pile-up of single events with up to six photons from six monochromatic lines with 99% accuracy. The usefulness of SDDs will continue into the X-ray FEL era of science. Their successors, the ePixS hybrid pixel detectors, already offer hundreds of pixels, each with a similar performance to an SDD, in a compact, robust and affordable package.« less

Optimal Pulse Processing, Pile-Up Decomposition, and Applications of Silicon Drift Detectors at LCLS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Blaj, G.; Kenney, C. J.; Dragone, A.

Silicon drift detectors (SDDs) revolutionized spectroscopy in fields as diverse as geology and dentistry. For a subset of experiments at ultrafast, X-ray free-electron lasers (FELs), SDDs can make substantial contributions. Often the unknown spectrum is interesting, carrying science data, or the background measurement is useful to identify unexpected signals. Many measurements involve only several discrete photon energies known a priori, allowing single-event decomposition of pile-up and spectroscopic photon counting. We designed a pulse function and demonstrated that the signal amplitude (i.e., proportional to the detected energy and obtained from fitting with the pulse function), rise time, and pulse height aremore » interrelated, and at short peaking times, the pulse height and pulse area are not optimal estimators for detected energy; instead, the signal amplitude and rise time are obtained for each pulse by fitting, thus removing the need for pulse shaping. By avoiding pulse shaping, rise times of tens of nanoseconds resulted in reduced pulse pile-up and allowed decomposition of remaining pulse pile-up at photon separation times down to hundreds of nanoseconds while yielding time-of-arrival information with the precision of 10 ns. Waveform fitting yields simultaneously high energy resolution and high counting rates (two orders of magnitude higher than current digital pulse processors). At pulsed sources or high photon rates, photon pile-up still occurs. We showed that pile-up spectrum fitting is relatively simple and preferable to pile-up spectrum deconvolution. We then developed a photon pile-up statistical model for constant intensity sources, extended it to variable intensity sources (typical for FELs), and used it to fit a complex pileup spectrum. We subsequently developed a Bayesian pile-up decomposition method that allows decomposing pile-up of single events with up to six photons from six monochromatic lines with 99% accuracy. The usefulness of SDDs will continue into the X-ray FEL era of science. Their successors, the ePixS hybrid pixel detectors, already offer hundreds of pixels, each with a similar performance to an SDD, in a compact, robust and affordable package.« less

Macrophage and tumor cell responses to repetitive pulsed X-ray radiation

NASA Astrophysics Data System (ADS)

Buldakov, M. A.; Tretyakova, M. S.; Ryabov, V. B.; Klimov, I. A.; Kutenkov, O. P.; Kzhyshkowska, J.; Bol'shakov, M. A.; Rostov, V. V.; Cherdyntseva, N. V.

2017-05-01

To study a response of tumor cells and macrophages to the repetitive pulsed low-dose X-ray radiation. Methods. Tumor growth and lung metastasis of mice with an injected Lewis lung carcinoma were analysed, using C57Bl6. Monocytes were isolated from a human blood, using CD14+ magnetic beads. IL6, IL1-betta, and TNF-alpha were determined by ELISA. For macrophage phenotyping, a confocal microscopy was applied. “Sinus-150” was used for the generation of pulsed X-ray radiation (the absorbed dose was below 0.1 Gy, the pulse repetition frequency was 10 pulse/sec). The irradiation of mice by 0.1 Gy pulsed X-rays significantly inhibited the growth of primary tumor and reduced the number of metastatic colonies in the lung. Furthermore, the changes in macrophage phenotype and cytokine secretion were observed after repetitive pulsed X-ray radiation. Conclusion. Macrophages and tumor cells had a different response to a low-dose pulsed X-ray radiation. An activation of the immune system through changes of a macrophage phenotype can result in a significant antitumor effect of the low-dose repetitive pulsed X-ray radiation.

Single-pulse coherent diffraction imaging using soft x-ray laser.

PubMed

Kang, Hyon Chol; Kim, Hyung Taek; Kim, Sang Soo; Kim, Chan; Yu, Tae Jun; Lee, Seong Ku; Kim, Chul Min; Kim, I Jong; Sung, Jae Hee; Janulewicz, Karol A; Lee, Jongmin; Noh, Do Young

2012-05-15

We report a coherent diffraction imaging (CDI) using a single 8 ps soft x-ray laser pulse at a wavelength of 13.9 nm. The soft x-ray pulse was generated by a laboratory-scale intense pumping laser providing coherent x-ray pulses up to the level of 10(11) photons/pulse. A spatial resolution below 194 nm was achieved with a single pulse, and it was shown that a resolution below 55 nm is feasible with improved detector capability. The single-pulse CDI might provide a way to investigate dynamics of nanoscale molecules or particles.

Attosecond time-energy structure of X-ray free-electron laser pulses

NASA Astrophysics Data System (ADS)

Hartmann, N.; Hartmann, G.; Heider, R.; Wagner, M. S.; Ilchen, M.; Buck, J.; Lindahl, A. O.; Benko, C.; Grünert, J.; Krzywinski, J.; Liu, J.; Lutman, A. A.; Marinelli, A.; Maxwell, T.; Miahnahri, A. A.; Moeller, S. P.; Planas, M.; Robinson, J.; Kazansky, A. K.; Kabachnik, N. M.; Viefhaus, J.; Feurer, T.; Kienberger, R.; Coffee, R. N.; Helml, W.

2018-04-01

The time-energy information of ultrashort X-ray free-electron laser pulses generated by the Linac Coherent Light Source is measured with attosecond resolution via angular streaking of neon 1s photoelectrons. The X-ray pulses promote electrons from the neon core level into an ionization continuum, where they are dressed with the electric field of a circularly polarized infrared laser. This induces characteristic modulations of the resulting photoelectron energy and angular distribution. From these modulations we recover the single-shot attosecond intensity structure and chirp of arbitrary X-ray pulses based on self-amplified spontaneous emission, which have eluded direct measurement so far. We characterize individual attosecond pulses, including their instantaneous frequency, and identify double pulses with well-defined delays and spectral properties, thus paving the way for X-ray pump/X-ray probe attosecond free-electron laser science.

MeV electron acceleration at 1 kHz with <10 mJ laser pulses

NASA Astrophysics Data System (ADS)

Salehi, Fatholah; Goers, Andy; Hine, George; Feder, Linus; Kuk, Donghoon; Miao, Bo; Woodbury, Daniel; Kim, Ki-Yong; Milchberg, Howard

2017-01-01

We demonstrate laser driven acceleration of electrons to MeV-scale energies at 1 kHz repetition rate using <10 mJ pulses focused on near-critical density He and H2 gas jets. Using the H2 gas jet, electron acceleration to 0.5 MeV in 10 fC bunches was observed with laser pulse energy as low as 1.3 mJ. Increasing the pulse energy to 10 mJ, we measure 1pC charge bunches with >1 MeV energy for both He and H gas jets. Such a high repetition rate, high flux ultrafast source has immediate application to time resolved probing of matter for scientific, medical, or security applications, either using the electrons directly or using a high-Z foil converter to generate ultrafast γ-rays. This work is supported by the US Department of Energy, the National Science Foundation, and the Air Force Office of Scientific Research.

Molecular electron recollision dynamics in intense circularly polarized laser pulses

NASA Astrophysics Data System (ADS)

Bandrauk, André D.; Yuan, Kai-Jun

2018-04-01

Extreme UV and x-ray table top light sources based on high-order harmonic generation (HHG) are focused now on circular polarization for the generation of circularly polarized attosecond pulses as new tools for controlling electron dynamics, such as charge transfer and migration and the generation of attosecond quantum electron currents for ultrafast magneto-optics. A fundamental electron dynamical process in HHG is laser induced electron recollision with the parent ion, well established theoretically and experimentally for linear polarization. We discuss molecular electron recollision dynamics in circular polarization by theoretical analysis and numerical simulation. The control of the polarization of HHG with circularly polarized ionizing pulses is examined and it is shown that bichromatic circularly polarized pulses enhance recollision dynamics, rendering HHG more efficient, especially in molecules because of their nonspherical symmetry. The polarization of the harmonics is found to be dependent on the compatibility of the rotational symmetry of the net electric field created by combinations of bichromatic circularly polarized pulses with the dynamical symmetry of molecules. We show how the field and molecule symmetry influences the electron recollision trajectories by a time-frequency analysis of harmonics. The results, in principle, offer new unique controllable tools in the study of attosecond molecular electron dynamics.

Femtosecond profiling of shaped x-ray pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoffmann, M. C.; Grguras, I.; Behrens, C.

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 fullymore » 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. Furthermore, this achievement completes an important step toward future x-ray pulse shaping techniques.« less

Femtosecond profiling of shaped x-ray pulses

DOE PAGES

Hoffmann, M. C.; Grguras, I.; Behrens, C.; ...

2018-03-26

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 fullymore » 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. Furthermore, this achievement completes an important step toward future x-ray pulse shaping techniques.« less

THz pulse doubler at FLASH: double pulses for pump–probe experiments at X-ray FELs

PubMed Central

Zapolnova, Ekaterina; Golz, Torsten; Pan, Rui; Klose, Karsten; Stojanovic, Nikola

2018-01-01

FLASH, the X-ray free-electron laser in Hamburg, Germany, employs a narrowband high-field accelerator THz source for unique THz pump X-ray probe experiments. However, the large difference in optical paths of the THz and X-ray beamlines prevents utilization of the machine’s full potential (e.g. extreme pulse energies in the soft X-ray range). To solve this issue, lasing of double electron bunches, separated by 28 periods of the driving radiofrequency (at 1.3 GHz), timed for the temporal overlap of THz and X-ray pulses at the experimental station has been employed. In order to optimize conditions for a typical THz pump X-ray probe experiment, X-ray lasing of the first bunch to one-sixth of that of the second has been suppressed. Finally, synchronization of THz radiation pulses was measured to be ∼20 fs (r.m.s.), and a solution for monitoring the arrival time for achieving higher temporal resolution is presented. PMID:29271749

THz pulse doubler at FLASH: double pulses for pump-probe experiments at X-ray FELs.

PubMed

Zapolnova, Ekaterina; Golz, Torsten; Pan, Rui; Klose, Karsten; Schreiber, Siegfried; Stojanovic, Nikola

2018-01-01

FLASH, the X-ray free-electron laser in Hamburg, Germany, employs a narrowband high-field accelerator THz source for unique THz pump X-ray probe experiments. However, the large difference in optical paths of the THz and X-ray beamlines prevents utilization of the machine's full potential (e.g. extreme pulse energies in the soft X-ray range). To solve this issue, lasing of double electron bunches, separated by 28 periods of the driving radiofrequency (at 1.3 GHz), timed for the temporal overlap of THz and X-ray pulses at the experimental station has been employed. In order to optimize conditions for a typical THz pump X-ray probe experiment, X-ray lasing of the first bunch to one-sixth of that of the second has been suppressed. Finally, synchronization of THz radiation pulses was measured to be ∼20 fs (r.m.s.), and a solution for monitoring the arrival time for achieving higher temporal resolution is presented.

Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales

DOE PAGES

Ulvestad, A.; Cherukara, M. J.; Harder, R.; ...

2017-08-29

Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4Dmore » evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. Lastly, we find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.« less

Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ulvestad, A.; Cherukara, M. J.; Harder, R.

Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4Dmore » evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. Lastly, we find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.« less

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

NASA Astrophysics Data System (ADS)

Karasawa, Naoki

2018-04-01

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

PAL-XFEL soft X-ray scientific instruments and X-ray optics: First commissioning results

NASA Astrophysics Data System (ADS)

Park, Sang Han; Kim, Minseok; Min, Changi-Ki; Eom, Intae; Nam, Inhyuk; Lee, Heung-Soo; Kang, Heung-Sik; Kim, Hyeong-Do; Jang, Ho Young; Kim, Seonghan; Hwang, Sun-min; Park, Gi-Soo; Park, Jaehun; Koo, Tae-Yeong; Kwon, Soonnam

2018-05-01

We report an overview of soft X-ray scientific instruments and X-ray optics at the free electron laser (FEL) of the Pohang Accelerator Laboratory, with selected first-commissioning results. The FEL exhibited a pulse energy of 200 μJ/pulse, a pulse width of <50 fs full width at half maximum, and an energy bandwidth of 0.44% at a photon energy of 850 eV. Monochromator resolving power of 10 500 was achieved. The estimated total time resolution between optical laser and X-ray pulses was <270 fs. A resonant inelastic X-ray scattering spectrometer was set up; its commissioning results are also reported.

Method and apparatus for producing durationally short ultraviolet or x-ray laser pulses

DOEpatents

MacGowan, B.J.; Matthews, D.L.; Trebes, J.E.

1987-05-05

A method and apparatus is disclosed for producing ultraviolet or x- ray laser pulses of short duration. An ultraviolet or x-ray laser pulse of long duration is progressively refracted, across the surface of an opaque barrier, by a streaming plasma that is produced by illuminating a solid target with a pulse of conventional line focused high power laser radiation. The short pulse of ultraviolet or x-ray laser radiation, which may be amplified to high power, is separated out by passage through a slit aperture in the opaque barrier.

Simple and robust generation of ultrafast laser pulse trains using polarization-independent parallel-aligned thin films

NASA Astrophysics Data System (ADS)

Wang, Andong; Jiang, Lan; Li, Xiaowei; Wang, Zhi; Du, Kun; Lu, Yongfeng

2018-05-01

Ultrafast laser pulse temporal shaping has been widely applied in various important applications such as laser materials processing, coherent control of chemical reactions, and ultrafast imaging. However, temporal pulse shaping has been limited to only-in-lab technique due to the high cost, low damage threshold, and polarization dependence. Herein we propose a novel design of ultrafast laser pulse train generation device, which consists of multiple polarization-independent parallel-aligned thin films. Various pulse trains with controllable temporal profile can be generated flexibly by multi-reflections within the splitting films. Compared with other pulse train generation techniques, this method has advantages of compact structure, low cost, high damage threshold and polarization independence. These advantages endow it with high potential for broad utilization in ultrafast applications.

Single-pulse x-ray diffraction using polycapillary optics for in situ dynamic diffraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maddox, B. R., E-mail: maddox3@llnl.gov; Akin, M. C., E-mail: akin1@llnl.gov; Teruya, A.

2016-08-15

Diagnostic use of single-pulse x-ray diffraction (XRD) at pulsed power facilities can be challenging due to factors such as the high flux and brightness requirements for diffraction and the geometric constraints of experimental platforms. By necessity, the x-ray source is usually positioned very close, within a few inches of the sample. On dynamic compression platforms, this puts the x-ray source in the debris field. We coupled x-ray polycapillary optics to a single-shot needle-and-washer x-ray diode source using a laser-based alignment scheme to obtain high-quality x-ray diffraction using a single 16 ns x-ray pulse with the source >1 m from themore » sample. The system was tested on a Mo sample in reflection geometry using 17 keV x-rays from a Mo anode. We also identified an anode conditioning effect that increased the x-ray intensity by 180%. Quantitative measurements of the x-ray focal spot produced by the polycapillary yielded a total x-ray flux on the sample of 3.3 ± 0.5 × 10{sup 7} molybdenum Kα photons.« less

Construction of a magnetic bottle spectrometer and its application to pulse duration measurement of X-ray laser using a pump-probe method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Namba, S., E-mail: namba@hiroshima-u.ac.jp; Hasegawa, N.; Kishimoto, M.

To characterize the temporal evolution of ultrashort X-ray pulses emitted by laser plasmas using a pump-probe method, a magnetic bottle time-of-flight electron spectrometer is constructed. The design is determined by numerical calculations of a mirror magnetic field and of the electron trajectory in a flight tube. The performance of the spectrometer is characterized by measuring the electron spectra of xenon atoms irradiated with a laser-driven plasma X-ray pulse. In addition, two-color above-threshold ionization (ATI) experiment is conducted for measurement of the X-ray laser pulse duration, in which xenon atoms are simultaneously irradiated with an X-ray laser pump and an IRmore » laser probe. The correlation in the intensity of the sideband spectra of the 4d inner-shell photoelectrons and in the time delay of the two laser pulses yields an X-ray pulse width of 5.7 ps, in good agreement with the value obtained using an X-ray streak camera.« less

Tamper to delay motion and decrease ionization of a sample during short pulse x-ray imaging

DOEpatents

London, Richard A [Orinda, CA; Szoke,; Abraham, Hau-Riege [Fremont, CA; Stefan P. , Chapman; Henry, N [Livermore, CA

2007-06-26

A system for x-ray imaging of a small sample comprising positioning a tamper so that it is operatively connected to the sample, directing short intense x-ray pulses onto the tamper and the sample, and detecting an image from the sample. The tamper delays the explosive motion of the sample during irradiation by the short intense x-ray pulses, thereby extending the time to obtain an x-ray image of the original structure of the sample.

Domain wall remote pinning in magnetic nano wires

NASA Astrophysics Data System (ADS)

Read, Dan; Miguel, Jorge; Maccherozzi, Francesco; Cavill, Stuart; Dhesi, Sarnjeet; Cardiff University Collaboration; Diamond Light Source Collaboration

2013-03-01

In the current race for information storage media with ever increasing density the position of magnetic domain walls, the region in a magnetic system where the local magnetization continually rotates its direction between adjacent magnetic domains, is one of the most promising routes for future storage media devices. Information storage requires ultrafast read-out and writing operations, but domain walls need to be pinned so that the information is safely stored in the long term. Here we investigate the use of remote magnetostatic charges to trap domain walls. By using X-ray photoelectron emission microscopy we have followed the position of domain walls of opposite charge being pinned or repelled by pinning potentials of increasing strength. Micromagnetic simulations show an excellent agreement with the experimental results. We demonstrate the attractive or repulsive character of the interaction between domain wall and trap depending upon the sign of their magnetic charges. These quasi-static experiments are the antecedent to ultrafast time-resolved XMCD-PEEM experiments where the spin-transfer torque effect will be studied dynamically by applying picosecond-long current pulses across the magnetic nanowire.

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

In Situ Synchrotron X-ray Study of Ultrasound Cavitation and Its Effect on Solidification Microstructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mi, Jiawei; Tan, Dongyue; Lee, Tung Lik

2014-12-11

Considerable progress has been made in studying the mechanism and effectiveness of using ultrasound waves to manipulate the solidification microstructures of metallic alloys. However, uncertainties remain in both the underlying physics of how microstructures evolve under ultrasonic waves, and the best technological approach to control the final microstructures and properties. We used the ultrafast synchrotron X-ray phase contrast imaging facility housed at the Advanced Photon Source, Argonne National Laboratory, US to study in situ the highly transient and dynamic interactions between the liquid metal and ultrasonic waves/bubbles. The dynamics of ultrasonic bubbles in liquid metal and their interactions with themore » solidifying phases in a transparent alloy were captured in situ. The experiments were complemented by the simulations of the acoustic pressure field, the pulsing of the bubbles, and the associated forces acting onto the solidifying dendrites. The study provides more quantitative understanding on how ultrasonic waves/bubbles influence the growth of dendritic grains and promote the grain multiplication effect for grain refinement.« less

Femtosecond Structural Dynamics Drives the Trans/Cis Isomerization in Photoactive Yellow Protein

PubMed Central

Pande, Kanupriya; Hutchison, Christopher D. M.; Groenhof, Gerrit; Aquila, Andy; Robinson, Josef S.; Tenboer, Jason; Basu, Shibom; Boutet, Sébastien; DePonte, Daniel P.; Liang, Mengning; White, Thomas A.; Zatsepin, Nadia A.; Yefanov, Oleksandr; Morozov, Dmitry; Oberthuer, Dominik; Gati, Cornelius; Subramanian, Ganesh; James, Daniel; Zhao, Yun; Koralek, Jake; Brayshaw, Jennifer; Kupitz, Christopher; Conrad, Chelsie; Roy-Chowdhury, Shatabdi; Coe, Jesse D.; Metz, Markus; Xavier, Paulraj Lourdu; Grant, Thomas D.; Koglin, Jason E.; Ketawala, Gihan; Fromme, Raimund; Šrajer, Vukica; Henning, Robert; Spence, John C. H.; Ourmazd, Abbas; Schwander, Peter; Weierstall, Uwe; Frank, Matthias; Fromme, Petra; Barty, Anton; Chapman, Henry N.; Moffat, Keith; van Thor, Jasper J.; Schmidt, Marius

2017-01-01

A variety of organisms have evolved mechanisms to detect and respond to light, in which the response is mediated by protein structural changes following photon absorption. The initial step is often the photo-isomerization of a conjugated chromophore. Isomerization occurs on ultrafast timescales, and is substantially influenced by the chromophore environment. Here we identify structural changes associated with the earliest steps in the trans to cis isomerization of the chromophore in photoactive yellow protein. Femtosecond, hard X-ray pulses emitted by the Linac Coherent Light Source were used to conduct time-resolved serial femtosecond crystallography on PYP microcrystals over the time range from 100 femtoseconds to 3 picoseconds to determine the structural dynamics of the photoisomerization reaction. PMID:27151871

Femtosecond all-optical synchronization of an X-ray free-electron laser

DOE PAGES

Schulz, S.; Grguraš, I.; Behrens, C.; ...

2015-01-20

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarilymore » by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses.« less

Femtosecond all-optical synchronization of an X-ray free-electron laser

PubMed Central

Schulz, S.; Grguraš, I.; Behrens, C.; Bromberger, H.; Costello, J. T.; Czwalinna, M. K.; Felber, M.; Hoffmann, M. C.; Ilchen, M.; Liu, H. Y.; Mazza, T.; Meyer, M.; Pfeiffer, S.; Prędki, P.; Schefer, S.; Schmidt, C.; Wegner, U.; Schlarb, H.; Cavalieri, A. L.

2015-01-01

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarily by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses. PMID:25600823

Femtosecond timing distribution and control for next generation accelerators and light sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Li -Jin

Femtosecond Timing Distribution At LCLS Free-electron-lasers (FEL) have the capability of producing high photon flux from the IR to the hard x-ray wavelength range and to emit femtosecond and eventually even attosecond pulses. This makes them an ideal tool for fundamental as well as applied re-search. Timing precision at the Stanford Linear Coherent Light Source (LCLS) between the x-ray FEL (XFEL) and ultrafast optical lasers is currently no better than 100 fs RMS. Ideally this precision should be much better and could be limited only by the x-ray pulse duration, which can be as short as a few femtoseconds. Anmore » increasing variety of science problems involving electron and nuclear dynamics in chemical and material systems will become accessible as the timing improves to a few femtoseconds. Advanced methods of electron beam conditioning or pulse injection could allow the FEL to achieve pulse durations less than one femtosecond. The objective of the work described in this proposal is to set up an optical timing distribution system based on mode locked Erbium doped fiber lasers at LCLS facility to improve the timing precision in the facility and allow time stamping with a 10 fs precision. The primary commercial applications for optical timing distributions systems are seen in the worldwide accelerator facilities and next generation light sources community. It is reasonable to expect that at least three major XFELs will be built in the next decade. In addition there will be up to 10 smaller machines, such as FERMI in Italy and Maxlab in Sweden, plus the market for upgrading already existing facilities like Jefferson Lab. The total market is estimated to be on the order of a 100 Million US Dollars. The company owns the exclusive rights to the IP covering the technology enabling sub-10 fs synchronization systems. Testing this technology, which has set records in a lab environment, at LCLS, hence in a real world scenario, is an important corner stone of bringing the technology to market.« less

3-D Ultrafast Doppler Imaging Applied to the Noninvasive and Quantitative Imaging of Blood Vessels in Vivo

PubMed Central

Provost, J.; Papadacci, C.; Demene, C.; Gennisson, J-L.; Tanter, M.; Pernot, M.

2016-01-01

Ultrafast Doppler Imaging was introduced as a technique to quantify blood flow in an entire 2-D field of view, expanding the field of application of ultrasound imaging to the highly sensitive anatomical and functional mapping of blood vessels. We have recently developed 3-D Ultrafast Ultrasound Imaging, a technique that can produce thousands of ultrasound volumes per second, based on three-dimensional plane and diverging wave emissions, and demonstrated its clinical feasibility in human subjects in vivo. In this study, we show that non-invasive 3-D Ultrafast Power Doppler, Pulsed Doppler, and Color Doppler Imaging can be used to perform quantitative imaging of blood vessels in humans when using coherent compounding of three-dimensional tilted plane waves. A customized, programmable, 1024-channel ultrasound system was designed to perform 3-D Ultrafast Imaging. Using a 32X32, 3-MHz matrix phased array (Vermon, France), volumes were beamformed by coherently compounding successive tilted plane wave emissions. Doppler processing was then applied in a voxel-wise fashion. 3-D Ultrafast Power Doppler Imaging was first validated by imaging Tygon tubes of varying diameter and its in vivo feasibility was demonstrated by imaging small vessels in the human thyroid. Simultaneous 3-D Color and Pulsed Doppler Imaging using compounded emissions were also applied in the carotid artery and the jugular vein in one healthy volunteer. PMID:26276956

Monochromatic x-ray radiography for areal-density measurement of inertial fusion energy fuel in fast ignition experiment.

PubMed

Fujioka, Shinsuke; Fujiwara, Takashi; Tanabe, Minoru; Nishimura, Hiroaki; Nagatomo, Hideo; Ohira, Shinji; Inubushi, Yuichi; Shiraga, Hiroyuki; Azechi, Hiroshi

2010-10-01

Ultrafast, two-dimensional x-ray imaging is an important diagnostics for the inertial fusion energy research, especially in investigating implosion dynamics at the final stage of the fuel compression. Although x-ray radiography was applied to observing the implosion dynamics, intense x-rays emitted from the high temperature and dense fuel core itself are often superimposed on the radiograph. This problem can be solved by coupling the x-ray radiography with monochromatic x-ray imaging technique. In the experiment, 2.8 or 5.2 keV backlight x-rays emitted from laser-irradiated polyvinyl chloride or vanadium foils were selectively imaged by spherically bent quartz crystals with discriminating the out-of-band emission from the fuel core. This x-ray radiography system achieved 24 μm and 100 ps of spatial and temporal resolutions, respectively.

Satellite Observations of Rapidly Varying Cosmic X-ray Sources. Ph.D. Thesis - Catholic Univ.

NASA Technical Reports Server (NTRS)

Maurer, G. S.

1979-01-01

The X-ray source data obtained with the high energy celestial X-ray detector on the Orbiting Solar Observatory -8 are presented. The results from the 1977 Crab observation show nonstatistical fluctuations in the pulsed emission and in the structure of the integrated pulse profile which cannot be attributed to any known systematic effect. The Hercules observations presented here provide information on three different aspects of the pulsed X-ray emission: the variation of pulsed flux as a function of the time from the beginning of the ON-state, the variation of pulsed flux as a function of binary phase, and the energy spectrum of the pulse emission.

Observation of femtosecond X-ray interactions with matter using an X-ray–X-ray pump–probe scheme

PubMed Central

Inoue, Ichiro; Inubushi, Yuichi; Sato, Takahiro; Tono, Kensuke; Katayama, Tetsuo; Kameshima, Takashi; Ogawa, Kanade; Togashi, Tadashi; Owada, Shigeki; Amemiya, Yoshiyuki; Tanaka, Takashi; Hara, Toru

2016-01-01

Resolution in the X-ray structure determination of noncrystalline samples has been limited to several tens of nanometers, because deep X-ray irradiation required for enhanced resolution causes radiation damage to samples. However, theoretical studies predict that the femtosecond (fs) durations of X-ray free-electron laser (XFEL) pulses make it possible to record scattering signals before the initiation of X-ray damage processes; thus, an ultraintense X-ray beam can be used beyond the conventional limit of radiation dose. Here, we verify this scenario by directly observing femtosecond X-ray damage processes in diamond irradiated with extraordinarily intense (∼1019 W/cm2) XFEL pulses. An X-ray pump–probe diffraction scheme was developed in this study; tightly focused double–5-fs XFEL pulses with time separations ranging from sub-fs to 80 fs were used to excite (i.e., pump) the diamond and characterize (i.e., probe) the temporal changes of the crystalline structures through Bragg reflection. It was found that the pump and probe diffraction intensities remain almost constant for shorter time separations of the double pulse, whereas the probe diffraction intensities decreased after 20 fs following pump pulse irradiation due to the X-ray–induced atomic displacement. This result indicates that sub-10-fs XFEL pulses enable conductions of damageless structural determinations and supports the validity of the theoretical predictions of ultraintense X-ray–matter interactions. The X-ray pump–probe scheme demonstrated here would be effective for understanding ultraintense X-ray–matter interactions, which will greatly stimulate advanced XFEL applications, such as atomic structure determination of a single molecule and generation of exotic matters with high energy densities. PMID:26811449

Ultrafast photoelectron spectroscopy of small molecule organic films

NASA Astrophysics Data System (ADS)

Read, Kendall Laine

As research in the field of ultrafast optics has produced shorter and shorter pulses, at an ever-widening range of frequencies, ultrafast spectroscopy has grown correspondingly. In particular, ultrafast photoelectron spectroscopy allows direct observation of electrons in transient or excited states, regardless of the eventual relaxation mechanisms. High-harmonic conversion of 800nm, femtosecond, Ti:sapphire laser pulses allows excite/probe spectroscopy down into atomic core level states. To this end, an ultrafast, X-UV photoelectron spectroscopic system is described, including design considerations for the high-harmonic generation line, the time of flight detector, and the subsequent data collection electronics. Using a similar experimental setup, I have performed several ultrafast, photoelectron excited state decay studies at the IBM, T. J. Watson Research Center. All of the observed materials were electroluminescent thin film organics, which have applications as the emitter layer in organic light emitting devices. The specific materials discussed are: Alq, BAlq, DPVBi, and Alq doped with DCM or DMQA. Alq:DCM is also known to lase at low photoexcitation thresholds. A detailed understanding of the involved relaxation mechanisms is beneficial to both applications. Using 3.14 eV excite, and 26.7 eV probe, 90 fs laser pulses, we have observed the lowest unoccupied molecular orbital (LUMO) decay rate over the first 200 picoseconds. During this time, diffusion is insignificant, and all dynamics occur in the absence of electron transport. With excitation intensities in the range of 100μJ/cm2, we have modeled the Alq, BAlq, and DPVBi decays via bimolecular singlet-singlet annihilation. At similar excitations, we have modeled the Alq:DCM decay via Förster transfer, stimulated emission, and excimeric formation. Furthermore, the Alq:DCM occupied to unoccupied molecular orbital energy gap was seen to shrink as a function of excite-to-probe delay, in accordance with the expected relaxation within the excited states. Stable, shorter pulses allow finer temporal resolution and more efficient high-harmonic generation. This work therefore concludes by discussing a method for further shortening 25 femtosecond pulses via self-phase modulation, using filamentation in air and subsequent fiber channeling.

Temporal characteristic analysis of laser-modulated pulsed X-ray source for space X-ray communication

NASA Astrophysics Data System (ADS)

Hang, Shuang; Liu, Yunpeng; Li, Huan; Tang, Xiaobin; Chen, Da

2018-04-01

X-ray communication (XCOM) is a new communication type and is expected to realize high-speed data transmission in some special communication scenarios, such as deep space communication and blackout communication. This study proposes a high-speed modulated X-ray source scheme based on the laser-to-X-ray conversion. The temporal characteristics of the essential components of the proposed laser-modulated pulsed X-ray source (LMPXS) were analyzed to evaluate its pulse emission performance. Results show that the LMPXS can provide a maximum modulation rate up to 100 Mbps which is expected to significantly improve the data rate of XCOM.

Nonequilibrium Phase Precursors during a Photoexcited Insulator-to-Metal Transition in V2O3

NASA Astrophysics Data System (ADS)

Singer, Andrej; Ramirez, Juan Gabriel; Valmianski, Ilya; Cela, Devin; Hua, Nelson; Kukreja, Roopali; Wingert, James; Kovalchuk, Olesya; Glownia, James M.; Sikorski, Marcin; Chollet, Matthieu; Holt, Martin; Schuller, Ivan K.; Shpyrko, Oleg G.

2018-05-01

Here, we photoinduce and directly observe with x-ray scattering an ultrafast enhancement of the structural long-range order in the archetypal Mott system V2O3 . Despite the ultrafast increase in crystal symmetry, the change of unit cell volume occurs an order of magnitude slower and coincides with the insulator-to-metal transition. The decoupling between the two structural responses in the time domain highlights the existence of a transient photoinduced precursor phase, which is distinct from the two structural phases present in equilibrium. X-ray nanoscopy reveals that acoustic phonons trapped in nanoscale twin domains govern the dynamics of the ultrafast transition into the precursor phase, while nucleation and growth of metallic domains dictate the duration of the slower transition into the metallic phase. The enhancement of the long-range order before completion of the electronic transition demonstrates the critical role the nonequilibrium structural phases play during electronic phase transitions in correlated electrons systems.

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

NASA Astrophysics Data System (ADS)

Sension, R. J.

2017-06-01

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

A photodiode amplifier system for pulse-by-pulse intensity measurement of an x-ray free electron laser.

PubMed

Kudo, Togo; Tono, Kensuke; Yabashi, Makina; Togashi, Tadashi; Sato, Takahiro; Inubushi, Yuichi; Omodani, Motohiko; Kirihara, Yoichi; Matsushita, Tomohiro; Kobayashi, Kazuo; Yamaga, Mitsuhiro; Uchiyama, Sadayuki; Hatsui, Takaki

2012-04-01

We have developed a single-shot intensity-measurement system using a silicon positive-intrinsic-negative (PIN) photodiode for x-ray pulses from an x-ray free electron laser. A wide dynamic range (10(3)-10(11) photons/pulse) and long distance signal transmission (>100 m) were required for this measurement system. For this purpose, we developed charge-sensitive and shaping amplifiers, which can process charge pulses with a wide dynamic range and variable durations (ns-μs) and charge levels (pC-μC). Output signals from the amplifiers were transmitted to a data acquisition system through a long cable in the form of a differential signal. The x-ray pulse intensities were calculated from the peak values of the signals by a waveform fitting procedure. This system can measure 10(3)-10(9) photons/pulse of ~10 keV x-rays by direct irradiation of a silicon PIN photodiode, and from 10(7)-10(11) photons/pulse by detecting the x-rays scattered by a diamond film using the silicon PIN photodiode. This system gives a relative accuracy of ~10(-3) with a proper gain setting of the amplifiers for each measurement. Using this system, we succeeded in detecting weak light at the developmental phase of the light source, as well as intense light during lasing of the x-ray free electron laser. © 2012 American Institute of Physics

Femtosecond laser-electron x-ray source

DOEpatents

Hartemann, Frederic V.; Baldis, Hector A.; Barty, Chris P.; Gibson, David J.; Rupp, Bernhard

2004-04-20

A femtosecond laser-electron X-ray source. A high-brightness relativistic electron injector produces an electron beam pulse train. A system accelerates the electron beam pulse train. The femtosecond laser-electron X-ray source includes a high intra-cavity power, mode-locked laser and an x-ray optics system.

Method and apparatus for producing durationally short ultraviolet or X-ray laser pulses

DOEpatents

MacGowan, Brian J.; Matthews, Dennis L.; Trebes, James E.

1988-01-01

A method and apparatus is disclosed for producing ultraviolet or X-ray laser pulses of short duration (32). An ultraviolet or X-ray laser pulse of long duration (12) is progressively refracted, across the surface of an opaque barrier (28), by a streaming plasma (22) that is produced by illuminating a solid target (16, 18) with a pulse of conventional line focused high power laser radiation (20). The short pulse of ultraviolet or X-ray laser radiation (32), which may be amplified to high power (40, 42), is separated out by passage through a slit aperture (30) in the opaque barrier (28).

HEAO 1 high-energy X-ray observations of Centaurus X-3

NASA Technical Reports Server (NTRS)

Howe, S. K.; Primini, F. A.; Bautz, M. W.; Lang, F. L.; Levine, A. M.; Lewin, W. H. G.

1983-01-01

Pulsations of 4.8 sec were detected up to energies above 38 keV by the present High Energy X-ray and Low Energy Gamma-Ray HEAO 1 satellite experiment observations of Cen X-3, and an analysis of the X-ray spectrum as a function of pulse phase indicates that the spectrum hardens during an interval of about 1.2 sec which lags the pulse peak by about 0.6 sec. The results of correlated observations of pulse period and X-ray intensity include (1) the detection of a high intensity state during which the pulse period is on the average increasing, (2) the measurement of comparable high intensities during episodes of both period increase and decrease, (3) the detection of X-ray pulsations at a much reduced level during a period of low intensity, and (4) the detection of a transition between spin-down, and spin-up episodes that coincides with a rapid decrease in X-ray intensity.

Small-Size High-Current Generators for X-Ray Backlighting

NASA Astrophysics Data System (ADS)

Chaikovsky, S. A.; Artyomov, A. P.; Zharova, N. V.; Zhigalin, A. S.; Lavrinovich, I. V.; Oreshkin, V. I.; Ratakhin, N. A.; Rousskikh, A. G.; Fedunin, A. V.; Fedushchak, V. F.; Erfort, A. A.

2017-12-01

The paper deals with the soft X-ray backlighting based on the X-pinch as a powerful tool for physical studies of fast processes. Proposed are the unique small-size pulsed power generators operating as a low-inductance capacitor bank. These pulse generators provide the X-pinch-based soft X-ray source (hν = 1-10 keV) of micron size at 2-3 ns pulse duration. The small size and weight of pulse generators allow them to be transported to any laboratory for conducting X-ray backlighting of test objects with micron space resolution and nanosecond exposure time. These generators also allow creating synchronized multi-frame radiographic complexes with frame delay variation in a broad range.

Circularly polarized attosecond pulse generation and applications to ultrafast magnetism

NASA Astrophysics Data System (ADS)

Bandrauk, André D.; Guo, Jing; Yuan, Kai-Jun

2017-12-01

Attosecond science is a growing new field of research and potential applications which relies on the development of attosecond light sources. Achievements in the generation and application of attosecond pulses enable to investigate electron dynamics in the nonlinear nonperturbative regime of laser-matter interactions on the electron’s natural time scale, the attosecond. In this review, we describe the generation of circularly polarized attosecond pulses and their applications to induce attosecond magnetic fields, new tools for ultrafast magnetism. Simulations are performed on aligned one-electron molecular ions by using nonperturbative nonlinear solutions of the time-dependent Schrödinger equation. We discuss how bichromatic circularly polarized laser pulses with co-rotating or counter-rotating components induce electron-parent ion recollisions, thus producing circularly polarized high-order harmonic generation, the source of circularly polarized attosecond pulses. Ultrafast quantum electron currents created by the generated attosecond pulses give rise to attosecond magnetic field pulses. The results provide a guiding principle for producing circularly polarized attosecond pulses and ultrafast magnetic fields in complex molecular systems for future research in ultrafast magneto-optics.

Noncollinear wave mixing of attosecond XUV and few-cycle optical laser pulses in gas-phase atoms: Toward multidimensional spectroscopy involving XUV excitations

NASA Astrophysics Data System (ADS)

Cao, Wei; Warrick, Erika R.; Fidler, Ashley; Neumark, Daniel M.; Leone, Stephen R.

2016-11-01

Ultrafast nonlinear spectroscopy, which records transient wave-mixing signals in a medium, is a powerful tool to access microscopic information using light sources in the radio-frequency and optical regimes. The extension of this technique towards the extreme ultraviolet (XUV) or even x-ray regimes holds the promise to uncover rich structural or dynamical information with even higher spatial or temporal resolution. Here, we demonstrate noncollinear wave mixing between weak XUV attosecond pulses and a strong near-infrared (NIR) few-cycle laser pulse in gas phase atoms (one photon of XUV and two photons of NIR). In the noncollinear geometry the attosecond and either one or two NIR pulses interact with argon atoms. Nonlinear XUV signals are generated in a spatially resolved fashion as required by phase matching. Different transition pathways can be identified from these background-free nonlinear signals according to the specific phase-matching conditions. Time-resolved measurements of the spatially gated XUV signals reveal electronic coherences of Rydberg wave packets prepared by a single XUV photon or XUV-NIR two-photon excitation, depending on the applied pulse sequences. These measurements open possible applications of tabletop multidimensional spectroscopy to the study of dynamics associated with valence or core excitation with XUV photons.

Burning plasmas with ultrashort soft-x-ray flashing

NASA Astrophysics Data System (ADS)

Hu, S. X.; Goncharov, V. N.; Skupsky, S.

2012-07-01

Fast ignition with narrow-band coherent x-ray pulses has been revisited for cryogenic deuterium-tritium (DT) plasma conditions achieved on the OMEGA Laser System. In contrast to using hard-x-rays (hv = 3-6 keV) proposed in the original x-ray fast-ignition proposal, we find that soft-x-ray sources with hv ≈ 500 eV photons can be suitable for igniting the dense DT-plasmas achieved on OMEGA. Two-dimensional radiation-hydrodynamics simulations have identified the break-even conditions for realizing such a "hybrid" ignition scheme (direct-drive compression with soft-x-ray heating) with 50-μm-offset targets: ˜10 ps soft-x-ray pulse (hv ≈ 500 eV) with a total energy of 500-1000 J to be focused into a 10 μm spot-size. A variety of x-ray pulse parameters have also been investigated for optimization. It is noted that an order of magnitude increase in neutron yield has been predicted even with x-ray energy as low as ˜50 J. Scaling this idea to a 1 MJ large-scale target, a gain above ˜30 can be reached with the same soft-x-ray pulse at 1.65 kJ energy. Even though such energetic x-ray sources do not currently exist, we hope that the proposed ignition scheme may stimulate efforts on generating powerful soft-x-ray sources in the near future.

Rapidly variable relatvistic absorption

NASA Astrophysics Data System (ADS)

Parker, M.; Pinto, C.; Fabian, A.; Lohfink, A.; Buisson, D.; Alston, W.; Jiang, J.

2017-10-01

I will present results from the 1.5Ms XMM-Newton observing campaign on the most X-ray variable AGN, IRAS 13224-3809. We find a series of nine absorption lines with a velocity of 0.24c from an ultra-fast outflow. For the first time, we are able to see extremely rapid variability of the UFO features, and can link this to the X-ray variability from the inner accretion disk. We find a clear flux dependence of the outflow features, suggesting that the wind is ionized by increasing X-ray emission.

The X-ray Pump–Probe instrument at the Linac Coherent Light Source

DOE PAGES

Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco; ...

2015-04-21

The X-ray Pump–Probe instrument achieves femtosecond time-resolution with hard X-ray methods using a free-electron laser source. It covers a photon energy range of 4–24 keV. A femtosecond optical laser system is available across a broad spectrum of wavelengths for generating transient states of matter. The instrument is designed to emphasize versatility and the scientific goals encompass ultrafast physical, chemical and biological processes involved in the transformation of matter and transfer of energy at the atomic scale.

Ultrafast table-top dynamic radiography of spontaneous or stimulated events

DOEpatents

Smilowitz, Laura; Henson, Bryan

2018-01-16

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

The X-ray Pump-Probe instrument at the Linac Coherent Light Source.

PubMed

Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco; Damiani, Daniel; Defever, Jim; Delor, James T; Feng, Yiping; Glownia, James M; Langton, J Brian; Nelson, Silke; Ramsey, Kelley; Robert, Aymeric; Sikorski, Marcin; Song, Sanghoon; Stefanescu, Daniel; Srinivasan, Venkat; Zhu, Diling; Lemke, Henrik T; Fritz, David M

2015-05-01

The X-ray Pump-Probe instrument achieves femtosecond time-resolution with hard X-ray methods using a free-electron laser source. It covers a photon energy range of 4-24 keV. A femtosecond optical laser system is available across a broad spectrum of wavelengths for generating transient states of matter. The instrument is designed to emphasize versatility and the scientific goals encompass ultrafast physical, chemical and biological processes involved in the transformation of matter and transfer of energy at the atomic scale.

In situ observation of high-pressure phase transition in silicon carbide under shock loading using ultrafast x-ray diffraction

NASA Astrophysics Data System (ADS)

Tracy, Sally June

2017-06-01

SiC is an important high-strength ceramic material used for a range of technological applications, including lightweight impact shielding and abrasives. SiC is also relevant to geology and planetary science. It may be a host of reduced carbon in the Earth's interior and also occurs in meteorites and impact sites. SiC has also been put forward as a possible major constituent in the proposed class of extra-solar planets known as carbon planets. Previous studies have used wave profile measurements to identify a phase transition under shock loading near 1 Mbar, but lattice-level structural information was not obtained. Here we present the behavior of silicon carbide under shock loading as investigated through a series of time-resolved pump-probe x-ray diffraction measurements up to 200 GPa. Our experiments were conducted at the Materials in Extreme Conditions beamline of the Linac Coherent Light Source. In situ x-ray diffraction data on shock-compressed SiC was collected using a free electron laser source combined with a pulsed high-energy laser. These measurements allow for the determination of time-dependent atomic arrangements, demonstrating that the wurtzite phase of SiC transforms directly to the B1 structure. Our measurements also reveal details of the material texture evolution under shock loading and release.

Pulsed x-ray imaging of high-density objects using a ten picosecond high-intensity laser driver

NASA Astrophysics Data System (ADS)

Rusby, D. R.; Brenner, C. M.; Armstrong, C.; Wilson, L. A.; Clarke, R.; Alejo, A.; Ahmed, H.; Butler, N. M. H.; Haddock, D.; Higginson, A.; McClymont, A.; Mirfayzi, S. R.; Murphy, C.; Notley, M.; Oliver, P.; Allott, R.; Hernandez-Gomez, C.; Kar, S.; McKenna, P.; Neely, D.

2016-10-01

Point-like sources of X-rays that are pulsed (sub nanosecond), high energy (up to several MeV) and bright are very promising for industrial and security applications where imaging through large and dense objects is required. Highly penetrating X-rays can be produced by electrons that have been accelerated by a high intensity laser pulse incident onto a thin solid target. We have used a pulse length of 10ps to accelerate electrons to create a bright x-ray source. The bremsstrahlung temperature was measured for a laser intensity from 8.5-12×1018 W/cm2. These x-rays have sequentially been used to image high density materials using image plate and a pixelated scintillator system.

Gain dynamics in a soft X-ray laser ampli er perturbed by a strong injected X-ray eld

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yong; Wang, Shoujun; Oliva, E

2014-01-01

Seeding soft X-ray plasma ampli ers with high harmonics has been demonstrated to generate high-brightness soft X-ray laser pulses with full spatial and temporal coherence. The interaction between the injected coherent eld and the swept-gain medium has been modelled. However, no exper- iment has been conducted to probe the gain dynamics when perturbed by a strong external seed eld. Here, we report the rst X-ray pump X-ray probe measurement of the nonlinear response of a plasma ampli er perturbed by a strong soft X-ray ultra-short pulse. We injected a sequence of two time-delayed high-harmonic pulses (l518.9 nm) into a collisionallymore » excited nickel-like molybdenum plasma to measure with femto-second resolution the gain depletion induced by the saturated ampli cation of the high-harmonic pump and its subsequent recovery. The measured fast gain recovery in 1.5 1.75 ps con rms the possibility to generate ultra-intense, fully phase-coherent soft X-ray lasers by chirped pulse ampli cation in plasma ampli ers.« less

Quantum simulation of ultrafast dynamics using trapped ultracold atoms.

PubMed

Senaratne, Ruwan; Rajagopal, Shankari V; Shimasaki, Toshihiko; Dotti, Peter E; Fujiwara, Kurt M; Singh, Kevin; Geiger, Zachary A; Weld, David M

2018-05-25

Ultrafast electronic dynamics are typically studied using pulsed lasers. Here we demonstrate a complementary experimental approach: quantum simulation of ultrafast dynamics using trapped ultracold atoms. Counter-intuitively, this technique emulates some of the fastest processes in atomic physics with some of the slowest, leading to a temporal magnification factor of up to 12 orders of magnitude. In these experiments, time-varying forces on neutral atoms in the ground state of a tunable optical trap emulate the electric fields of a pulsed laser acting on bound charged particles. We demonstrate the correspondence with ultrafast science by a sequence of experiments: nonlinear spectroscopy of a many-body bound state, control of the excitation spectrum by potential shaping, observation of sub-cycle unbinding dynamics during strong few-cycle pulses, and direct measurement of carrier-envelope phase dependence of the response to an ultrafast-equivalent pulse. These results establish cold-atom quantum simulation as a complementary tool for studying ultrafast dynamics.

New 'Molecular Movie' Reveals Ultrafast Chemistry in Motion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Minitti, Michael

2015-06-22

Scientists for the first time tracked ultrafast structural changes, captured in quadrillionths-of-a-second steps, as ring-shaped gas molecules burst open and unraveled. Ring-shaped molecules are abundant in biochemistry and also form the basis for many drug compounds. The study points the way to a wide range of real-time X-ray studies of gas-based chemical reactions that are vital to biological processes.

New 'Molecular Movie' Reveals Ultrafast Chemistry in Motion

ScienceCinema

Minitti, Michael

2018-02-14

Scientists for the first time tracked ultrafast structural changes, captured in quadrillionths-of-a-second steps, as ring-shaped gas molecules burst open and unraveled. Ring-shaped molecules are abundant in biochemistry and also form the basis for many drug compounds. The study points the way to a wide range of real-time X-ray studies of gas-based chemical reactions that are vital to biological processes.

Time-resolved molecular imaging

NASA Astrophysics Data System (ADS)

Xu, Junliang; Blaga, Cosmin I.; Agostini, Pierre; DiMauro, Louis F.

2016-06-01

Time-resolved molecular imaging is a frontier of ultrafast optical science and physical chemistry. In this article, we review present and future key spectroscopic and microscopic techniques for ultrafast imaging of molecular dynamics and show their differences and connections. The advent of femtosecond lasers and free electron x-ray lasers bring us closer to this goal, which eventually will extend our knowledge about molecular dynamics to the attosecond time domain.

X-ray emission as a potential hazard during ultrashort pulse laser material processing

NASA Astrophysics Data System (ADS)

Legall, Herbert; Schwanke, Christoph; Pentzien, Simone; Dittmar, Günter; Bonse, Jörn; Krüger, Jörg

2018-06-01

In laser machining with ultrashort laser pulses unwanted X-ray radiation in the keV range can be generated when a critical laser intensity is exceeded. Even if the emitted X-ray dose per pulse is low, high laser repetition rates can lead to an accumulation of X-ray doses beyond exposure safety limits. For 925 fs pulse duration at a center wavelength of 1030 nm, the X-ray emission was investigated up to an intensity of 2.6 × 1014 W/cm2. The experiments were performed in air with a thin disk laser at a repetition rate of 400 kHz. X-ray spectra and doses were measured for various planar target materials covering a wide range of the periodic table from aluminum to tungsten. Without radiation shielding, the measured radiation doses at this high repetition rate clearly exceed the regulatory limits. Estimations for an adequate radiation shielding are provided.

X-Ray Radiation Measurements With Photodiodes In Plasmas Generated By 1017 W/Cm2 Intensity Krf Excimer Laser Pulses

NASA Astrophysics Data System (ADS)

Rácz, E.; Földes, I. B.; Ryć, L.

2006-01-01

Experiments were carried out using a prepulse-free hybrid KrF excimer-dye laser system (700fs pulse duration, 248nm wavelength, 15mJ pulse energy). The intensity of the p-polarized, focused laser beam was 1.5ṡ1017 W/cm2. Vacuum ultraviolet (VUV) and x-rays from solid state laser plasmas were generated in the laser-plasma interaction of subpicosecond laser pulses of nonrelativistic laser intensities. An x-ray sensitive FLM photodiode (ITE, Warsaw) was used to detect x-rays between 1-19 keV in front of the targets. The diode was filtered by a 4μm Al foil. The dependence of the x-ray flux on laser intensity and the angular distribution of x-rays for aluminum and copper targets in the half space of the front side of the targets were investigated.

Dynamic absorption and scattering of water and hydrogel during high-repetition-rate (>100 MHz) burst-mode ultrafast-pulse laser ablation.

PubMed

Qian, Zuoming; Covarrubias, Andrés; Grindal, Alexander W; Akens, Margarete K; Lilge, Lothar; Marjoribanks, Robin S

2016-06-01

High-repetition-rate burst-mode ultrafast-laser ablation and disruption of biological tissues depends on interaction of each pulse with the sample, but under those particular conditions which persist from previous pulses. This work characterizes and compares the dynamics of absorption and scattering of a 133-MHz repetition-rate, burst-mode ultrafast-pulse laser, in agar hydrogel targets and distilled water. The differences in energy partition are quantified, pulse-by-pulse, using a time-resolving integrating-sphere-based device. These measurements reveal that high-repetition-rate burst-mode ultrafast-laser ablation is a highly dynamical process affected by the persistence of ionization, dissipation of plasma plume, neutral material flow, tissue tensile strength, and the hydrodynamic oscillation of cavitation bubbles.

Structural, optical and vibrational properties of self-assembled Pbn+1(Ti1−xFex)nO3n+1−δ Ruddlesden-Popper superstructures

PubMed Central

Doig, K. I.; Peters, J. J. P.; Nawaz, S.; Walker, D.; Walker, M.; Lees, M. R.; Beanland, R.; Sanchez, A. M.; McConville, C. F.; Palkar, V. R.; Lloyd-Hughes, J.

2015-01-01

Bulk crystals and thin films of PbTi1−xFexO3−δ (PTFO) are multiferroic, exhibiting ferroelectricity and ferromagnetism at room temperature. Here we report that the Ruddlesden-Popper phase Pbn+1(Ti1−xFex)nO3n+1−δ forms spontaneously during pulsed laser deposition of PTFO on LaAlO3 substrates. High-resolution transmission electron microscopy, x-ray diffraction and x-ray photoemission spectroscopy were utilised to perform a structural and compositional analysis, demonstrating that and . The complex dielectric function of the films was determined from far-infrared to ultraviolet energies using a combination of terahertz time-domain spectroscopy, Fourier transform spectroscopy, and spectroscopic ellipsometry. The simultaneous Raman and infrared activity of phonon modes and the observation of second harmonic generation establishes a non-centrosymmetric point group for Pbn+1(Ti0.5Fe0.5)nO3n+1−δ, a prerequisite for (but not proof of) ferroelectricity. No evidence of macroscopic ferromagnetism was found in SQUID magnetometry. The ultrafast optical response exhibited coherent magnon oscillations compatible with local magnetic order, and additionally was used to study photocarrier cooling on picosecond timescales. An optical gap smaller than that of BiFeO3 and long photocarrier lifetimes may make this system interesting as a ferroelectric photovoltaic. PMID:25591924

Distributed ultrafast fibre laser

PubMed Central

Liu, Xueming; Cui, Yudong; Han, Dongdong; Yao, Xiankun; Sun, Zhipei

2015-01-01

A traditional ultrafast fibre laser has a constant cavity length that is independent of the pulse wavelength. The investigation of distributed ultrafast (DUF) lasers is conceptually and technically challenging and of great interest because the laser cavity length and fundamental cavity frequency are changeable based on the wavelength. Here, we propose and demonstrate a DUF fibre laser based on a linearly chirped fibre Bragg grating, where the total cavity length is linearly changeable as a function of the pulse wavelength. The spectral sidebands in DUF lasers are enhanced greatly, including the continuous-wave (CW) and pulse components. We observe that all sidebands of the pulse experience the same round-trip time although they have different round-trip distances and refractive indices. The pulse-shaping of the DUF laser is dominated by the dissipative processes in addition to the phase modulations, which makes our ultrafast laser simple and stable. This laser provides a simple, stable, low-cost, ultrafast-pulsed source with controllable and changeable cavity frequency. PMID:25765454

Ultrafast molecular processes mapped by femtosecond x-ray diffraction

NASA Astrophysics Data System (ADS)

Elsaesser, Thomas

2012-02-01

X-ray diffraction with a femtosecond time resolution allows for mapping photoinduced structural dynamics on the length scale of a chemical bond and in the time domain of atomic and molecular motion. In a pump-probe approach, a femtosecond excitation pulse induces structural changes which are probed by diffracting a femtosecond hard x-ray pulse from the excited sample. The transient angular positions and intensities of diffraction peaks give insight into the momentary atomic or molecular positions and into the distribution of electronic charge density. The simultaneous measurement of changes on different diffraction peaks is essential for determining atom positions and charge density maps with high accuracy. Recent progress in the generation of ultrashort hard x-ray pulses (Cu Kα, wavelength λ=0.154 nm) in laser-driven plasma sources has led to the implementation of the powder diffraction and the rotating crystal method with a time resolution of 100 fs. In this contribution, we report new results from powder diffraction studies of molecular materials. A first series of experiments gives evidence of a so far unknown concerted transfer of electrons and protons in ammonium sulfate [(NH4)2SO4], a centrosymmetric structure. Charge transfer from the sulfate groups results in the sub-100 fs generation of a confined electron channel along the c-axis of the unit cell which is stabilized by transferring protons from the adjacent ammonium groups into the channel. Time-dependent charge density maps display a periodic modulation of the channel's charge density by low-frequency lattice motions with a concerted electron and proton motion between the channel and the initial proton binding site. A second study addresses atomic rearrangements and charge dislocations in the non-centrosymmetric potassium dihydrogen phosphate [KH2PO4, KDP]. Photoexcitation generates coherent low-frequency motions along the LO and TO phonon coordinates, leaving the average atomic positions unchanged. The time-dependent maps of electron density demonstrate a concomitant oscillatory relocation of electronic charge with a spatial amplitude of the order of a chemical bond length, two orders of magnitude larger than the vibrational amplitudes. The coherent phonon motions drive the charge relocation, similar to a soft mode driven phase transition between the ferro- and paraelectric phase of KDP.

Generation of High-Power High-Intensity Short X-Ray Free-Electron-Laser Pulses

DOE PAGES

Guetg, Marc W.; Lutman, Alberto A.; Ding, Yuantao; ...

2018-01-03

X-ray free-electron lasers combine a high pulse power, short pulse length, narrow bandwidth, and high degree of transverse coherence. Any increase in the photon pulse power, while shortening the pulse length, will further push the frontier on several key x-ray free-electron laser applications including single-molecule imaging and novel nonlinear x-ray methods. This Letter shows experimental results at the Linac Coherent Light Source raising its maximum power to more than 300% of the current limit while reducing the photon pulse length to 10 fs. As a result, this was achieved by minimizing residual transverse-longitudinal centroid beam offsets and beam yaw andmore » by correcting the dispersion when operating over 6 kA peak current with a longitudinally shaped beam.« less

Generation of High-Power High-Intensity Short X-Ray Free-Electron-Laser Pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guetg, Marc W.; Lutman, Alberto A.; Ding, Yuantao

X-ray free-electron lasers combine a high pulse power, short pulse length, narrow bandwidth, and high degree of transverse coherence. Any increase in the photon pulse power, while shortening the pulse length, will further push the frontier on several key x-ray free-electron laser applications including single-molecule imaging and novel nonlinear x-ray methods. This Letter shows experimental results at the Linac Coherent Light Source raising its maximum power to more than 300% of the current limit while reducing the photon pulse length to 10 fs. As a result, this was achieved by minimizing residual transverse-longitudinal centroid beam offsets and beam yaw andmore » by correcting the dispersion when operating over 6 kA peak current with a longitudinally shaped beam.« less

Acoustic Injectors for Drop-On-Demand Serial Femtosecond Crystallography.

PubMed

Roessler, Christian G; Agarwal, Rakhi; Allaire, Marc; Alonso-Mori, Roberto; Andi, Babak; Bachega, José F R; Bommer, Martin; Brewster, Aaron S; Browne, Michael C; Chatterjee, Ruchira; Cho, Eunsun; Cohen, Aina E; Cowan, Matthew; Datwani, Sammy; Davidson, Victor L; Defever, Jim; Eaton, Brent; Ellson, Richard; Feng, Yiping; Ghislain, Lucien P; Glownia, James M; Han, Guangye; Hattne, Johan; Hellmich, Julia; Héroux, Annie; Ibrahim, Mohamed; Kern, Jan; Kuczewski, Anthony; Lemke, Henrik T; Liu, Pinghua; Majlof, Lars; McClintock, William M; Myers, Stuart; Nelsen, Silke; Olechno, Joe; Orville, Allen M; Sauter, Nicholas K; Soares, Alexei S; Soltis, S Michael; Song, Heng; Stearns, Richard G; Tran, Rosalie; Tsai, Yingssu; Uervirojnangkoorn, Monarin; Wilmot, Carrie M; Yachandra, Vittal; Yano, Junko; Yukl, Erik T; Zhu, Diling; Zouni, Athina

2016-04-05

X-ray free-electron lasers (XFELs) provide very intense X-ray pulses suitable for macromolecular crystallography. Each X-ray pulse typically lasts for tens of femtoseconds and the interval between pulses is many orders of magnitude longer. Here we describe two novel acoustic injection systems that use focused sound waves to eject picoliter to nanoliter crystal-containing droplets out of microplates and into the X-ray pulse from which diffraction data are collected. The on-demand droplet delivery is synchronized to the XFEL pulse scheme, resulting in X-ray pulses intersecting up to 88% of the droplets. We tested several types of samples in a range of crystallization conditions, wherein the overall crystal hit ratio (e.g., fraction of images with observable diffraction patterns) is a function of the microcrystal slurry concentration. We report crystal structures from lysozyme, thermolysin, and stachydrine demethylase (Stc2). Additional samples were screened to demonstrate that these methods can be applied to rare samples. Copyright © 2016 Elsevier Ltd. All rights reserved.

Acoustic Injectors for Drop-On-Demand Serial Femtosecond Crystallography

DOE PAGES

Roessler, Christian G.; Agarwal, Rakhi; Allaire, Marc; ...

2016-03-17

X-ray free-electron lasers (XFELs) provide very intense X-ray pulses suitable for macromolecular crystallography. Each X-ray pulse typically lasts for tens of femtoseconds and the interval between pulses is many orders of magnitude longer. Here we describe two novel acoustic injection systems that use focused sound waves to eject picoliter to nanoliter crystal-containing droplets out of microplates and into the X-ray pulse from which diffraction data are collected. The on-demand droplet delivery is synchronized to the XFEL pulse scheme, resulting in X-ray pulses intersecting up to 88% of the droplets. We tested several types of samples in a range of crystallizationmore » conditions, wherein the overall crystal hit ratio (e.g., fraction of images with observable diffraction patterns) is a function of the microcrystal slurry concentration. Lastly, we report crystal structures from lysozyme, thermolysin, and stachydrine demethylase (Stc2). In addition, samples were screened to demonstrate that these methods can be applied to rare samples« less

Acoustic Injectors for Drop-On-Demand Serial Femtosecond Crystallography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roessler, Christian G.; Agarwal, Rakhi; Allaire, Marc

X-ray free-electron lasers (XFELs) provide very intense X-ray pulses suitable for macromolecular crystallography. Each X-ray pulse typically lasts for tens of femtoseconds and the interval between pulses is many orders of magnitude longer. Here we describe two novel acoustic injection systems that use focused sound waves to eject picoliter to nanoliter crystal-containing droplets out of microplates and into the X-ray pulse from which diffraction data are collected. The on-demand droplet delivery is synchronized to the XFEL pulse scheme, resulting in X-ray pulses intersecting up to 88% of the droplets. We tested several types of samples in a range of crystallizationmore » conditions, wherein the overall crystal hit ratio (e.g., fraction of images with observable diffraction patterns) is a function of the microcrystal slurry concentration. We report crystal structures from lysozyme, thermolysin, and stachydrine demethylase (Stc2). Additional samples were screened to demonstrate that these methods can be applied to rare samples.« less

Acoustic Injectors for Drop-On-Demand Serial Femtosecond Crystallography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roessler, Christian G.; Agarwal, Rakhi; Allaire, Marc

X-ray free-electron lasers (XFELs) provide very intense X-ray pulses suitable for macromolecular crystallography. Each X-ray pulse typically lasts for tens of femtoseconds and the interval between pulses is many orders of magnitude longer. Here we describe two novel acoustic injection systems that use focused sound waves to eject picoliter to nanoliter crystal-containing droplets out of microplates and into the X-ray pulse from which diffraction data are collected. The on-demand droplet delivery is synchronized to the XFEL pulse scheme, resulting in X-ray pulses intersecting up to 88% of the droplets. We tested several types of samples in a range of crystallizationmore » conditions, wherein the overall crystal hit ratio (e.g., fraction of images with observable diffraction patterns) is a function of the microcrystal slurry concentration. Lastly, we report crystal structures from lysozyme, thermolysin, and stachydrine demethylase (Stc2). In addition, samples were screened to demonstrate that these methods can be applied to rare samples« less

Numerical simulations of the hard X-ray pulse intensity distribution at the Linac Coherent Light Source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pardini, Tom; Aquila, Andrew; Boutet, Sebastien

Numerical simulations of the current and future pulse intensity distributions at selected locations along the Far Experimental Hall, the hard X-ray section of the Linac Coherent Light Source (LCLS), are provided. Estimates are given for the pulse fluence, energy and size in and out of focus, taking into account effects due to the experimentally measured divergence of the X-ray beam, and measured figure errors of all X-ray optics in the beam path. Out-of-focus results are validated by comparison with experimental data. Previous work is expanded on, providing quantitatively correct predictions of the pulse intensity distribution. Numerical estimates in focus aremore » particularly important given that the latter cannot be measured with direct imaging techniques due to detector damage. Finally, novel numerical estimates of improvements to the pulse intensity distribution expected as part of the on-going upgrade of the LCLS X-ray transport system are provided. As a result, we suggest how the new generation of X-ray optics to be installed would outperform the old one, satisfying the tight requirements imposed by X-ray free-electron laser facilities.« less

Numerical simulations of the hard X-ray pulse intensity distribution at the Linac Coherent Light Source

DOE PAGES

Pardini, Tom; Aquila, Andrew; Boutet, Sebastien; ...

2017-06-15

Numerical simulations of the current and future pulse intensity distributions at selected locations along the Far Experimental Hall, the hard X-ray section of the Linac Coherent Light Source (LCLS), are provided. Estimates are given for the pulse fluence, energy and size in and out of focus, taking into account effects due to the experimentally measured divergence of the X-ray beam, and measured figure errors of all X-ray optics in the beam path. Out-of-focus results are validated by comparison with experimental data. Previous work is expanded on, providing quantitatively correct predictions of the pulse intensity distribution. Numerical estimates in focus aremore » particularly important given that the latter cannot be measured with direct imaging techniques due to detector damage. Finally, novel numerical estimates of improvements to the pulse intensity distribution expected as part of the on-going upgrade of the LCLS X-ray transport system are provided. As a result, we suggest how the new generation of X-ray optics to be installed would outperform the old one, satisfying the tight requirements imposed by X-ray free-electron laser facilities.« less

THz pulses from 4th generation X-ray light sources: Perspectives for fully synchronized THz pump X-ray probe experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gensch, M.

2010-02-03

In this paper the prospects of terahertz (THz) pulses generated at 4th generation X-ray light sources are presented on the example of recent results from a prototype set-up at the soft X-ray FEL FLASH. It is shown, that the THz pulses from the relativistic ultra short electron bunches have unique properties, that at FLASH are utilized for novel THz pump X-ray probe experiments with a robust few fs resolution. Based on these experiences it is discussed, how future facilities can benefit from implementation of similar or further improved instrumentation.

Hercules X-1: Spectral Variability of an X-Ray Pulsar in a Stellar Binary System. Ph.D. Thesis

NASA Technical Reports Server (NTRS)

Pravdo, S. H.

1976-01-01

A cosmic X-ray spectroscopy experiment onboard the Orbiting Solar Observatory 8 (OSO-8), observed Her x-1 continuously for approximately 8 days. Spectral-temporal correlations of the X-ray emission were obtained. The major results concern observations of: (1) iron band emission, (2) spectral hardening (increase in effective x-ray temperature) within the X-ray pulse, and (3) a transition from an X-ray low state to a high state. The spectrum obtained prior to the high state can be interpreted as reflected emission from a hot coronal gas surrounding an accretion disk, which itself shields the primary X-ray source from the line of sight during the low state. The spectral hardening within the X-ray pulse was indicative of the beaming mechanism at the neutron star surface. The hardest spectrum by pulse phase was identified with the line of sight close to the Her x-1 magnetic dipole axis, and the X-ray pencil beam become harder with decreasing angle between the line of sight and the dipole axis.

Few-femtosecond time-resolved measurements of X-ray free-electron lasers.

PubMed

Behrens, C; Decker, F-J; Ding, Y; Dolgashev, V A; Frisch, J; Huang, Z; Krejcik, P; Loos, H; Lutman, A; Maxwell, T J; Turner, J; Wang, J; Wang, M-H; Welch, J; Wu, J

2014-04-30

X-ray free-electron lasers, with pulse durations ranging from a few to several hundred femtoseconds, are uniquely suited for studying atomic, molecular, chemical and biological systems. Characterizing the temporal profiles of these femtosecond X-ray pulses that vary from shot to shot is not only challenging but also important for data interpretation. Here we report the time-resolved measurements of X-ray free-electron lasers by using an X-band radiofrequency transverse deflector at the Linac Coherent Light Source. We demonstrate this method to be a simple, non-invasive technique with a large dynamic range for single-shot electron and X-ray temporal characterization. A resolution of less than 1 fs root mean square has been achieved for soft X-ray pulses. The lasing evolution along the undulator has been studied with the electron trapping being observed as the X-ray peak power approaches 100 GW.

Spectral and temporal properties of the X-ray pulsar SMC X-1 at hard X-rays

NASA Technical Reports Server (NTRS)

Kunz, M.; Gruber, D. E.; Kendziorra, E .; Kretschmar, P.; Maisack, M.; Mony, B.; Staubert, R.; Doebereiner, S.; Englhauser, J.; Pietsch, W.

1993-01-01

The binary X-ray pulsar SMC X- 1 has been observed at hard X-rays with the High Energy X-Ray Experiment (HEXE) on nine occasions between Nov. 1987 and March 1989. A thin thermal bremsstrahlung fit to the phase averaged spectrum yields a plasma temperature (14.4 +/- 1.3) keV and a luminosity above (1.1 +/- 0.1) x 10 exp 38 erg/s in the 20-80 keV band. Pulse period values have been established for three observations, confirming the remarkably stable spin-up trend of SMC X-1. In one of the three observations the pulse profile was seen to deviate from a dominant double pulsation, while at the same time the pulsed fraction was unusually large. For one observation we determined for the first time the pulsed fraction in narrow energy bands. It increases with photon energy from about 20 percent up to over 60 percent in the energy range from 20 to 80 keV.

Capturing local structure modulations of photoexcited BiVO4 by ultrafast transient XAFS.

PubMed

Uemura, Yohei; Kido, Daiki; Koide, Akihiro; Wakisaka, Yuki; Niwa, Yasuhiro; Nozawa, Shunsuke; Ichiyanagi, Kohei; Fukaya, Ryo; Adachi, Shin-Ichi; Katayama, Tetsuo; Togashi, Tadashi; Owada, Shigeki; Yabashi, Makina; Hatada, Keisuke; Iwase, Akihide; Kudo, Akihiko; Takakusagi, Satoru; Yokoyama, Toshihiko; Asakura, Kiyotaka

2017-06-29

Ultrafast excitation of photocatalytically active BiVO 4 was characterized by femto- and picosecond transient X-ray absorption fine structure spectroscopy. An initial photoexcited state (≪500 fs) changed to a metastable state accompanied by a structural change with a time constant of ∼14 ps. The structural change might stabilize holes on oxygen atoms since the interaction between Bi and O increases.

Apparatus and method to enhance X-ray production in laser produced plasmas

DOEpatents

Augustoni, Arnold L.; Gerardo, James B.; Raymond, Thomas D.

1992-01-01

Method and apparatus for generating x-rays for use in, for instance, x-ray photolithography. The method of generating x-rays includes the steps of providing a target and irradiating the target with a laser system which produces a train of sub-pulses to generate an x-ray producing plasma. The sub-pulses are of both high intensity and short duration. The apparatus for generating x-rays from a plasma includes a vacuum chamber, a target supported within the chamber and a laser system, including a short storage time laser.

Bright attosecond γ-ray pulses from nonlinear Compton scattering with laser-illuminated compound targets

NASA Astrophysics Data System (ADS)

Zhu, Xing-Long; Chen, Min; Yu, Tong-Pu; Weng, Su-Ming; Hu, Li-Xiang; McKenna, Paul; Sheng, Zheng-Ming

2018-04-01

Attosecond light sources have the potential to open up totally unexplored research avenues in ultrafast science. However, the photon energies achievable using existing generation schemes are limited to the keV range. Here, we propose and numerically demonstrate an all-optical mechanism for the generation of bright MeV attosecond γ-photon beams with desirable angular momentum. Using a circularly polarized Laguerre-Gaussian laser pulse focused onto a cone-foil target, dense attosecond bunches ( ≲ 170 as ) of electrons are produced. The electrons interact with the laser pulse which is reflected by a plasma mirror, producing ultra-brilliant (˜1023 photons/s/mm2/mrad2/0.1%BW) multi-MeV (Eγ,max > 30 MeV) isolated attosecond ( ≲ 260 as ) γ-ray pulse trains. Moreover, the angular momentum is transferred to γ-photon beams via nonlinear Compton scattering of ultra-intense tightly focused laser pulse by energetic electrons. Such a brilliant attosecond γ-photon source would provide the possibilities in attosecond nuclear science.

APS Science 2006.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gibson, J. M.; Fenner, R. B.; Long, G.

2007-05-24

In my five years as the Director of the Advanced Photon Source (APS), I have been fortunate to see major growth in the scientific impact from the APS. This year I am particularly enthusiastic about prospects for our longer-term future. Every scientific instrument must remain at the cutting edge to flourish. Our plans for the next generation of APS--an APS upgrade--got seriously in gear this year with strong encouragement from our users and sponsors. The most promising avenue that has emerged is the energy-recovery linac (ERL) (see article on page xx), for which we are beginning serious R&D. The ERL{at}APSmore » would offer revolutionary performance, especially for x-ray imaging and ultrafast science, while not seriously disrupting the existing user base. I am very proud of our accelerator physics and engineering staff, who not only keep the current APS at the forefront, but were able to greatly impress our international Machine Advisory Committee with the quality of their work on the possible upgrade option (see page xx). As we prepare for long-term major upgrades, our plans to develop and optimize all the sectors at APS in the near future are advancing. Several new beamlines saw first light this year, including a dedicated powder diffraction beamline (11-BM), two instruments for inelastic x-ray scattering at sector 30, and the Center for Nanoscale Materials (CNM) Nanoprobe beamline at sector 26. Our partnership in the first x-ray free-electron laser (LCLS) to be built at Stanford contributes to revolutionary growth in ultrafast science (see page xx), and we are developing a pulse chirping scheme to get ps pulses at sector 7 of the APS within a year or so. In this report, you will find selected highlights of scientific research at the APS from calendar year 2006. The highlighted work covers diverse disciplines, from fundamental to applied science. In the article on page xx you can see the direct impact of APS research on technology. Several new products have emerged from work at the APS, to complement the tremendous output of work in basic science, which often has payoff in technology but over decades rather than years. Highlights in this report also reflect the relevance of APS work to Department of Energy missions, for example a route to more efficient fuel cells (page xx mr-88-073113) addresses the energy challenge, and natural approaches to cleaning up the environment.« less

Relativistic electron diffraction at the UCLA Pegasus photoinjector laboratory.

PubMed

Musumeci, P; Moody, J T; Scoby, C M

2008-10-01

Electron diffraction holds the promise to yield real-time resolution of atomic motion in an easily accessible environment like a university laboratory at a fraction of the cost of fourth-generation X-ray sources. Currently the limit in time-resolution for conventional electron diffraction is set by how short an electron pulse can be made. A very promising solution to maintain the highest possible beam intensity without excessive pulse broadening from space charge effects is to increase the electron energy to the MeV level where relativistic effects significantly reduce the space charge forces. Rf photoinjectors can in principle deliver up to 10(7)-10(8) electrons packed in bunches of approximately 100-fs length, allowing an unprecedented time resolution and enabling the study of irreversible phenomena by single-shot diffraction patterns. The use of rf photoinjectors as sources for ultrafast electron diffraction has been recently at the center of various theoretical and experimental studies. The UCLA Pegasus laboratory, commissioned in early 2007 as an advanced photoinjector facility, is the only operating system in the country, which has recently demonstrated electron diffraction using a relativistic beam from an rf photoinjector. Due to the use of a state-of-the-art ultrashort photoinjector driver laser system, the beam has been measured to be sub-100-fs long, at least a factor of 5 better than what measured in previous relativistic electron diffraction setups. Moreover, diffraction patterns from various metal targets (titanium and aluminum) have been obtained using the Pegasus beam. One of the main laboratory goals in the near future is to fully develop the rf photoinjector-based ultrafast electron diffraction technique with particular attention to the optimization of the working point of the photoinjector in a low-charge ultrashort pulse regime, and to the development of suitable beam diagnostics.

Ultrafast X-ray Imaging of Fuel Sprays

NASA Astrophysics Data System (ADS)

Wang, Jin

2007-01-01

Detailed analysis of fuel sprays has been well recognized as an important step for optimizing the operation of internal combustion engines to improve efficiency and reduce emissions. Ultrafast radiographic and tomographic techniques have been developed for probing the fuel distribution close to the nozzles of direct-injection diesel and gasoline injectors. The measurement was made using x-ray absorption of monochromatic synchrotron-generated radiation, allowing quantitative determination of the fuel distribution in this optically impenetrable region with a time resolution on the order of 1 μs. Furthermore, an accurate 3-dimensional fuel-density distribution, in the form of fuel volume fraction, was obtained by the time-resolved computed tomography. These quantitative measurements constitute the most detailed near-nozzle study of a fuel spray to date. With high-energy and high-brilliance x-ray beams available at the Advanced Photon Source, propagation-based phase-enhanced imaging was developed as a unique metrology technique to visualize the interior of an injection nozzle through a 3-mm-thick steel with a 10-μs temporal resolution, which is virtually impossible by any other means.

Revealing the X-Ray Emission Processes of Old Rotation-Powered Pulsars: XMM-Newton Observations of PSR B0950+08, PSR B0823+26 and PSR J2043+2740

NASA Technical Reports Server (NTRS)

Becker, Werner; Weisskopf, Martin C.; Tenant, Allyn F.; Jessmer, Axel; Zhang, Shiang N.

2004-01-01

We have completed part of a program to study the X-ray emission properties of old rotation-powered pulsars with XMM-Newton in order to probe and identify the origin of their X radiation. The X-ray emission from these old pulsars is largely dominated by non-thermal processes. None of the observed spectra required adding a thermal component consisting of either a hot polar cap or surface cooling emission to model the data. The energy spectrum of PSR B0950+08 is best described by a single power law of photon-index alpha = 1.93(sup +0.14)(sub -0.12). Three-sigma temperature upper limits for possible contributions from a heated polar cap or the whole neutron star surface are T(sup infinity)(sub pc) < 0.87 x 10(exp 6) K and T(sup infinity)(sub s) < 0.48 x 10(exp 6) K, respectively. We also find that the X-ray emission from PSR B0950+08 is pulsed with two peaks per rotation period. The phase separation between the two X-ray peaks is approx. 144 deg (maximum to maximum) which is similar to the pulse peak separation observed in the radio band at 1.4 GHz. The fraction of X-ray pulsed photons is approx. 30%. A phase resolved spectral analysis confirms the nonthermal nature of the pulsed emission and finds power law slopes of alpha = 2.4(sup +0.52)(sub -0.42) and alpha = 1.93(sup +0.29)(sub -0.24) for the pulse peaks P1 and P2, respectively. The spectral emission properties observed for PSR B0823+26 are similar to those of PSR B0950+08. Its energy spectrum is very well described by a single power law with photon-index alpha = 2.5(sup +0.52)(sub -0.24. Three-sigma temperature upper limits for thermal contributions from a hot polar cap or from the entire neutron star surface are T(sup infinity)(sub pc) < 1.17 x 10(exp 6) K and T(sup infinity)(sub s) < 0.5 x 10(exp 6) K, respectively. There is evidence for pulsed X-ray emission at the - 97% confidence level with a pulsed fraction of 49 +/- 22%. For PSR 52043+2740 we report the first detection of X-ray emission. A power law spectrum, or a combination of a thermal and a power law spectrum all yield acceptable descriptions of its X-ray spectrum. No X-ray pulses are detected from PSR J2043+2740 but the sensitivity is low - the 2-sigma pulsed fraction upper limit is 57% assuming a sinusoidal pulse profile.

X-rays only when you want them: optimized pump–probe experiments using pseudo-single-bunch operation

PubMed Central

Hertlein, M. P.; Scholl, A.; Cordones, A. A.; Lee, J. H.; Engelhorn, K.; Glover, T. E.; Barbrel, B.; Sun, C.; Steier, C.; Portmann, G.; Robin, D. S.

2015-01-01

Laser pump–X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500 kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shot X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated. PMID:25931090

X-rays only when you want them: Optimized pump–probe experiments using pseudo-single-bunch operation

DOE PAGES

Hertlein, M. P.; Scholl, A.; Cordones, A. A.; ...

2015-04-02

Laser pump–X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500 kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shotmore » X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated.« less

Thomson-backscattered x rays from laser-accelerated electrons.

PubMed

Schwoerer, H; Liesfeld, B; Schlenvoigt, H-P; Amthor, K-U; Sauerbrey, R

2006-01-13

We present the first observation of Thomson-backscattered light from laser-accelerated electrons. In a compact, all-optical setup, the "photon collider," a high-intensity laser pulse is focused into a pulsed He gas jet and accelerates electrons to relativistic energies. A counterpropagating laser probe pulse is scattered from these high-energy electrons, and the backscattered x-ray photons are spectrally analyzed. This experiment demonstrates a novel source of directed ultrashort x-ray pulses and additionally allows for time-resolved spectroscopy of the laser acceleration of electrons.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, Chao; Jiang, Tao; Liu, Shengguang

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

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

DOE PAGES

Lu, Chao; Jiang, Tao; Liu, Shengguang; ...

2018-03-12

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

Magnetic switching in granular FePt layers promoted by near-field laser enhancement

DOE PAGES

Granitzka, Patrick W.; Jal, Emmanuelle; Le Guyader, Loic; ...

2017-03-08

Light-matter interaction at the nanoscale in magnetic materials is a topic of intense research in view of potential applications in next-generation high-density magnetic recording. Laser-assisted switching provides a pathway for overcoming the material constraints of high-anisotropy and high-packing density media, though much about the dynamics of the switching process remains unexplored. We use ultrafast small-angle X-ray scattering at an X-ray free-electron laser to probe the magnetic switching dynamics of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. We observe that the combination of laser excitation and applied static magnetic field, 1 order ofmore » magnitude smaller than the coercive field, can overcome the magnetic anisotropy barrier between “up” and “down” magnetization, enabling magnetization switching. This magnetic switching is found to be inhomogeneous throughout the material with some individual FePt nanoparticles neither switching nor demagnetizing. The origin of this behavior is identified as the near-field modification of the incident laser radiation around FePt nanoparticles. Furthermore, the fraction of not-switching nanoparticles is influenced by the heat flow between FePt and a heat-sink layer.« less

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

NASA Astrophysics Data System (ADS)

Schäfer, Julia M.; Inhester, Ludger; Son, Sang-Kil; Fink, Reinhold F.; Santra, Robin

2018-05-01

With the highly intense x-ray light generated by x-ray free-electron lasers (XFELs), molecular samples can be ionized many times in a single pulse. Here we report on a computational study of molecular spectroscopy at the high x-ray intensity provided by XFELs. Calculated photoelectron, Auger electron, and x-ray fluorescence spectra are presented for a single water molecule that reaches many electronic hole configurations through repeated ionization steps. The rich details shown in the spectra depend on the x-ray pulse parameters in a nonintuitive way. We discuss how the observed trends can be explained by the competition of microscopic electronic transition processes. A detailed comparison between spectra calculated within the independent-atom model and within the molecular-orbital framework highlights the chemical sensitivity of the spectral lines of multiple-hole configurations. Our results demonstrate how x-ray multiphoton ionization-related effects such as charge-rearrangement-enhanced x-ray ionization of molecules and frustrated absorption manifest themselves in the electron and fluorescence spectra.

The first search for X-ray polarization in the Centaurus X-3 and Hercules X-1 pulsars

NASA Technical Reports Server (NTRS)

Silver, E. H.; Weisskopf, M. C.; Kestenbaum, H. L.; Long, K. S.; Novick, R.; Wolff, R. S.

1979-01-01

The first search for X-ray polarization in the Cen X-3 and Her X-1 pulsars was performed by the OSO 8 polarimeters in 1975 July and 1975 August, respectively. Three-sigma upper limits to the polarization in Cen X-3 of 13.5% and 19% at 2.6 keV and 5.2 keV, respectively, were obtained when the data were averaged over the pulse and binary periods. The upper limit for Her X-1 at 2.6 keV is 60%. A search for pulse-phase dependent X-ray polarization from both objects was also performed. At the 91% confidence level, emission from Cen X-3 exhibits evidence for X-ray polarization at 2.6 keV that varies with pulse phase. Upper limits to polarization are presented for the leading and trailing edges and peak of the Her X-1 pulse at 2.6 keV.

Deconvolving the temporal response of photoelectric x-ray detectors for the diagnosis of pulsed radiations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zou, Shiyang; Song, Peng; Pei, Wenbing

2013-09-15

Based on the conjugate gradient method, a simple algorithm is presented for deconvolving the temporal response of photoelectric x-ray detectors (XRDs) to reconstruct the resolved time-dependent x-ray fluxes. With this algorithm, we have studied the impact of temporal response of XRD on the radiation diagnosis of hohlraum heated by a short intense laser pulse. It is found that the limiting temporal response of XRD not only postpones the rising edge and peak position of x-ray pulses but also smoothes the possible fluctuations of radiation fluxes. Without a proper consideration of the temporal response of XRD, the measured radiation flux canmore » be largely misinterpreted for radiation pulses of a hohlraum heated by short or shaped laser pulses.« less

Enhanced coherent Thomson scattering in the few-cycle regime.

PubMed

Hu, Ke; Wu, Hui-Chun

2016-10-01

We study x-ray production by coherent nonlinear Thomson scattering of few-cycle laser pulses from relativistic electron sheets. For an electron sheet thicker than the wavelength of the x-ray, the scattering efficiency is found to increase by two orders of magnitude for single-cycle laser pulses, as compared with longer pulses. This enhancement is attributed to the suppression of the destructive interference during the scattering process, as well as the frequency downshift related to the ultrabroad spectra of single-cycle pulses. The x-ray amplitude in this nonadiabatic regime is calculated and agrees with that from the particle-in-cell simulation. These results can be useful for designing more intense, shorter attosecond x-ray sources.

Performance summary on a high power dense plasma focus x-ray lithography point source producing 70 nm line features in AlGaAs microcircuits

NASA Astrophysics Data System (ADS)

Petr, Rodney; Bykanov, Alexander; Freshman, Jay; Reilly, Dennis; Mangano, Joseph; Roche, Maureen; Dickenson, Jason; Burte, Mitchell; Heaton, John

2004-08-01

A high average power dense plasma focus (DPF), x-ray point source has been used to produce ˜70 nm line features in AlGaAs-based monolithic millimeter-wave integrated circuits (MMICs). The DPF source has produced up to 12 J per pulse of x-ray energy into 4π steradians at ˜1 keV effective wavelength in ˜2 Torr neon at pulse repetition rates up to 60 Hz, with an effective x-ray yield efficiency of ˜0.8%. Plasma temperature and electron concentration are estimated from the x-ray spectrum to be ˜170 eV and ˜5.1019 cm-3, respectively. The x-ray point source utilizes solid-state pulse power technology to extend the operating lifetime of electrodes and insulators in the DPF discharge. By eliminating current reversals in the DPF head, an anode electrode has demonstrated a lifetime of more than 5 million shots. The x-ray point source has also been operated continuously for 8 h run times at 27 Hz average pulse recurrent frequency. Measurements of shock waves produced by the plasma discharge indicate that overpressure pulses must be attenuated before a collimator can be integrated with the DPF point source.

Pump–probe spectrometer for measuring x-ray induced strain

DOE PAGES

Loether, A.; Adams, B. W.; DiCharia, A.; ...

2016-04-20

A hard x-ray pump–probe spectrometer using a multi-crystal Bragg reflector is demonstrated at a third generation synchrotron source. This device derives both broadband pump and monochromatic probe pulses directly from a single intense, broadband x-ray pulse centered at 8.767 keV. In conclusion, we present a proof-of-concept experiment which directly measures x-ray induced crystalline lattice strain.

Influence of Xe and Kr impurities on x-ray yield from debris-free plasma x-ray sources with an Ar supersonic gas jet irradiated by femtosecond near-infrared-wavelength laser pulses

NASA Astrophysics Data System (ADS)

Kantsyrev, V. L.; Schultz, K. A.; Shlyaptseva, V. V.; Petrov, G. M.; Safronova, A. S.; Petkov, E. E.; Moschella, J. J.; Shrestha, I.; Cline, W.; Wiewior, P.; Chalyy, O.

2016-11-01

Many aspects of physical phenomena occurring when an intense laser pulse with subpicosecond duration and an intensity of 1018-1019W /cm2 heats an underdense plasma in a supersonic clustered gas jet are studied to determine the relative contribution of thermal and nonthermal processes to soft- and hard-x-ray emission from debris-free plasmas. Experiments were performed at the University of Nevada, Reno (UNR) Leopard laser operated with a 15-J, 350-fs pulse and different pulse contrasts (107 or 105). The supersonic linear (elongated) nozzle generated Xe cluster-monomer gas jets as well as jets with Kr-Ar or Xe-Kr-Ar mixtures with densities of 1018-1019cm-3 . Prior to laser heating experiments, all jets were probed with optical interferometry and Rayleigh scattering to measure jet density and cluster distribution parameters. The supersonic linear jet provides the capability to study the anisotropy of x-ray yield from laser plasma and also laser beam self-focusing in plasma, which leads to efficient x-ray generation. Plasma diagnostics included x-ray diodes, pinhole cameras, and spectrometers. Jet signatures of x-ray emission from pure Xe gas, as well as from a mixture with Ar and Kr, was found to be very different. The most intense x-ray emission in the 1-9 KeV spectral region was observed from gas mixtures rather than pure Xe. Also, this x-ray emission was strongly anisotropic with respect to the direction of laser beam polarization. Non-local thermodynamic equilibrium (Non-LTE) models have been implemented to analyze the x-ray spectra to determine the plasma temperature and election density. Evidence of electron beam generation in the supersonic jet plasma was found. The influence of the subpicosecond laser pulse contrast (a ratio between the laser peak intensity and pedestal pulse intensity) on the jets' x-ray emission characteristics is discussed. Surprisingly, it was found that the x-ray yield was not sensitive to the prepulse contrast ratio.

Generation of bright attosecond x-ray pulse trains via Thomson scattering from laser-plasma accelerators.

PubMed

Luo, W; Yu, T P; Chen, M; Song, Y M; Zhu, Z C; Ma, Y Y; Zhuo, H B

2014-12-29

Generation of attosecond x-ray pulse attracts more and more attention within the advanced light source user community due to its potentially wide applications. Here we propose an all-optical scheme to generate bright, attosecond hard x-ray pulse trains by Thomson backscattering of similarly structured electron beams produced in a vacuum channel by a tightly focused laser pulse. Design parameters for a proof-of-concept experiment are presented and demonstrated by using a particle-in-cell code and a four-dimensional laser-Compton scattering simulation code to model both the laser-based electron acceleration and Thomson scattering processes. Trains of 200 attosecond duration hard x-ray pulses holding stable longitudinal spacing with photon energies approaching 50 keV and maximum achievable peak brightness up to 10²⁰ photons/s/mm²/mrad²/0.1%BW for each micro-bunch are observed. The suggested physical scheme for attosecond x-ray pulse trains generation may directly access the fastest time scales relevant to electron dynamics in atoms, molecules and materials.

Growth of ferroelectric Ba{sub 0.8}Sr{sub 0.2}TiO{sub 3} epitaxial films by ultraviolet pulsed laser irradiation of chemical solution derived precursor layers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Queraltó, A.; Pérez del Pino, A., E-mail: aperez@icmab.es; Mata, M. de la

2015-06-29

Highly crystalline epitaxial Ba{sub 0.8}Sr{sub 0.2}TiO{sub 3} (BST) thin-films are grown on (001)-oriented LaNiO{sub 3}-buffered LaAlO{sub 3} substrates by pulsed laser irradiation of solution derived barium-zirconium-titanium precursor layers using a UV Nd:YAG laser source at atmospheric conditions. The structural analyses of the obtained films, studied by X-ray diffractometry and transmission electron microscopy, demonstrate that laser processing allows the growth of tens of nm-thick BST epitaxial films with crystalline structure similar to that of films obtained through conventional thermal annealing methods. However, the fast pulsed nature of the laser employed leads to crystallization kinetic evolution orders of magnitude faster than inmore » thermal treatments. The combination of specific photothermal and photochemical mechanisms is the main responsible for the ultrafast epitaxial laser-induced crystallization. Piezoresponse microscopy measurements demonstrate equivalent ferroelectric behavior in laser and thermally annealed films, being the piezoelectric constant ∼25 pm V{sup −1}.« less

Nonlinear resonance scattering of femtosecond X-ray pulses on atoms in plasmas

NASA Astrophysics Data System (ADS)

Rosmej, F. B.; Astapenko, V. A.; Lisitsa, V. S.; Moroz, N. N.

2017-11-01

It is shown that for sufficiently short pulses the resonance scattering probability becomes a nonlinear function of the pulse duration. For fs X-ray pulses scattered on atoms in plasmas maxima and minima develop in the nonlinear regime whereas in the limit of long pulses the probability becomes linear and turns over into the standard description of the electromagnetic pulse scattering. Numerical calculations are carried out in terms of a generalized scattering probability for the total time of pulse duration including fine structure splitting and ion Doppler broadening in hot plasmas. For projected X-ray monocycles, the generalized nonlinear approach differs by 1-2 orders of magnitude from the standard theory.

Short x-ray pulse generation using deflecting cavities at the Advanced Photon Source.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sajaev, V.; Borland, M.; Chae, Y.-C.

2007-11-11

Storage-ring-based third-generation light sources can provide intense radiation pulses with durations as short as 100 ps. However, there is growing interest within the synchrotron radiation user community in performing experiments with much shorter X-ray pulses. Zholents et al. [Nucl. Instr. and Meth. A 425 (1999) 385] recently proposed using RF orbit deflection to generate sub-ps X-ray pulses. In this scheme, two deflecting cavities are used to deliver a longitudinally dependent vertical kick to the beam. An optical slit can then be used to slice out a short part of the radiation pulse. Implementation of this scheme is planned for onemore » APS beamline in the near future. In this paper, we summarize our feasibility study of this method and the expected X-ray beam parameters. We find that a pulse length of less than two picoseconds can be achieved.« less

X-ray laser–induced electron dynamics observed by femtosecond diffraction from nanocrystals of Buckminsterfullerene

PubMed Central

Abbey, Brian; Dilanian, Ruben A.; Darmanin, Connie; Ryan, Rebecca A.; Putkunz, Corey T.; Martin, Andrew V.; Wood, David; Streltsov, Victor; Jones, Michael W. M.; Gaffney, Naylyn; Hofmann, Felix; Williams, Garth J.; Boutet, Sébastien; Messerschmidt, Marc; Seibert, M. Marvin; Williams, Sophie; Curwood, Evan; Balaur, Eugeniu; Peele, Andrew G.; Nugent, Keith A.; Quiney, Harry M.

2016-01-01

X-ray free-electron lasers (XFELs) deliver x-ray pulses with a coherent flux that is approximately eight orders of magnitude greater than that available from a modern third-generation synchrotron source. The power density of an XFEL pulse may be so high that it can modify the electronic properties of a sample on a femtosecond time scale. Exploration of the interaction of intense coherent x-ray pulses and matter is both of intrinsic scientific interest and of critical importance to the interpretation of experiments that probe the structures of materials using high-brightness femtosecond XFEL pulses. We report observations of the diffraction of extremely intense 32-fs nanofocused x-ray pulses by a powder sample of crystalline C60. We find that the diffraction pattern at the highest available incident power significantly differs from the one obtained using either third-generation synchrotron sources or XFEL sources operating at low output power and does not correspond to the diffraction pattern expected from any known phase of crystalline C60. We interpret these data as evidence of a long-range, coherent dynamic electronic distortion that is driven by the interaction of the periodic array of C60 molecular targets with intense x-ray pulses of femtosecond duration. PMID:27626076

Monitoring The Crab Pulsar

NASA Technical Reports Server (NTRS)

Rots, Arnold H.; Swank, Jean (Technical Monitor)

2001-01-01

The monitoring of the X-ray pulses from the Crab pulsar is still ongoing at the time of this writing, and we hope to be able to continue the campaign for the life of the XTE mission. We have established beyond all doubt that: (1) the X-ray main pulse leads the radio pulse by approximately 300 microseconds, (2) this phase lag is constant and not influenced by glitches, (3) this lag does not depend on X-ray energy, (4) the relative phase of the two X-ray pulses does not vary, and (5) the spectral indices of primary, secondary, and inter-pulse are distinct and constant. At this time we are investigating whether the radio timing ephemeris can be replaced by an x-ray ephemeris and whether any long-time timing ephemeris can be established. If so, it would enable use to study variations in pulse arrival times at a longer time scales. Such a study is easier in x-rays than at radio wavelengths since the dispersion measure plays no role. These results were reported at the 2000 HEAD Meeting in Honolulu, HI. Travel was paid partly out of this grant. The remainder was applied toward the acquisition of a laptop computer that allows independent and fast analysis of all monitoring observations.

Nonthermal ultrafast optical control of the magnetization in garnet films

NASA Astrophysics Data System (ADS)

Hansteen, Fredrik; Kimel, Alexey; Kirilyuk, Andrei; Rasing, Theo

2006-01-01

We demonstrate coherent optical control of the magnetization in ferrimagnetic garnet films on the femtosecond time scale through a combination of two different ultrafast and nonthermal photomagnetic effects and by employing multiple pump pulses. Linearly polarized laser pulses are shown to create a long-lived modification of the magnetocrystalline anisotropy via optically induced electron transfer between nonequivalent ion sites while circularly polarized pulses additionally act as strong transient magnetic field pulses originating from the nonabsorptive inverse Faraday effect. Due to the slow phonon-magnon interaction in these dielectrics, thermal effects of the laser excitation are clearly distinguished from the ultrafast nonthermal effects and can be seen only on the time scale of nanoseconds for sample temperatures near the Curie point. The reported effects open exciting possibilities for ultrafast manipulation of spins by light, and provide insight into the physics of magnetism on ultrafast time scales.

Characterization of the LCLS “nanosecond two-bunch” mode for x-ray speckle visibility spectroscopy experiments

DOE PAGES

Sun, Yanwen; Zhu, Diling; Song, Sanghoon; ...

2017-05-23

The generation of two X-ray pulses with tunable nanosecond scale time separations has recently been demonstrated at the Linac Coherent Light Source using an accelerator based technique. This approach offers the opportunity to extend X-ray Photon Correlation Spectroscopy techniques to the yet unexplored regime of nanosecond timescales by means of X-ray Speckle Visibility Spectroscopy. As the two pulses originate from two independent Spontaneous Amplified Stimulated Emission processes, the beam properties fluctuate from pulse pair to pulse pair, but as well between the individual pulses within a pair. However, two-pulse XSVS experiments require the intensity of the individual pulses to bemore » either identical in the ideal case, or with a accurately known intensity ratio. We present the design and performances of a non-destructive intensity diagnostic based on measurement of scattering from a transparent target using a high-speed photo-detector. Individual pulses within a pulse pair with time delays as short as 0.7 ns can be resolved. Moreover, using small angle coherent scattering, we characterize the averaged spatial overlap of the focused pulse pairs. Furthermore, the multi-shot average-speckle contrasts from individual pulses and pulse pairs are compared.« less

Study of 1–8 keV K-α x-ray emission from high intensity femtosecond laser produced plasma

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arora, V., E-mail: arora@rrcat.gov.in; Naik, P. A.; Chakera, J. A.

2014-04-15

We report an experimental study on the optimization of a laser plasma based x-ray source of ultra-short duration K-α line radiation. The interaction of pulses from a CPA based Ti:sapphire laser (10 TW, 45 fs, 10 Hz) system with magnesium, titanium, iron and copper solid target generates bright 1-8 keV K-α x-ray radiation. The x-ray yield was optimized with the laser pulse duration (at fixed fluence) which is varied in the range of 45 fs to 1.4 ps. It showed a maximum at laser pulse duration of ∼740 fs, 420 fs, 350 and 250 fs for Mg (1.3 keV), Timore » (4.5 keV), Fe (6.4 keV) and Cu (8.05 keV) respectively. The x-ray yield is observed to be independent of the sign of the chirp. The scaling of the K-α yield (I{sub x} ∝ I{sub L}{sup β}) for 45 fs and optimized pulse duration were measured for laser intensities in the region of 3 × 10{sup 14} – 8 × 10{sup 17}. The x-ray yield shows a much faster scaling exponent β = 1.5, 2.1, 2.4 and 2.6 for Mg, Ti, Fe and Cu respectively at optimized pulse duration compared to scaling exponent of 0.65, 1.3, 1.5, and 1.7 obtained for 45 fs duration laser pulses. The laser to x-ray energy conversion efficiencies obtained for different target materials are η{sub Mg} = 1.2 × 10{sup −5}, η{sub Ti} = 3.1 × 10{sup −5}, η{sub Fe} = 2.7 × 10{sup −5}, η{sub Cu} = 1.9 × 10{sup −5}. The results have been explained from the efficient generation of optimal energy hot electrons at longer laser pulse duration. The faster scaling observed at optimal pulse duration indicates that the x-ray source is generated at the target surface and saturation of x-ray emission would appear at larger laser fluence. An example of utilization of the source for measurement of shock-wave profiles in a silicon crystal by time resolved x-ray diffraction is also presented.« less

Retinal isomerization in bacteriorhodopsin captured by a femtosecond x-ray laser.

PubMed

Nogly, Przemyslaw; Weinert, Tobias; James, Daniel; Carbajo, Sergio; Ozerov, Dmitry; Furrer, Antonia; Gashi, Dardan; Borin, Veniamin; Skopintsev, Petr; Jaeger, Kathrin; Nass, Karol; Båth, Petra; Bosman, Robert; Koglin, Jason; Seaberg, Matthew; Lane, Thomas; Kekilli, Demet; Brünle, Steffen; Tanaka, Tomoyuki; Wu, Wenting; Milne, Christopher; White, Thomas; Barty, Anton; Weierstall, Uwe; Panneels, Valerie; Nango, Eriko; Iwata, So; Hunter, Mark; Schapiro, Igor; Schertler, Gebhard; Neutze, Richard; Standfuss, Jörg

2018-06-14

Ultrafast isomerization of retinal is the primary step in photoresponsive biological functions including vision in humans and ion-transport across bacterial membranes. We studied the sub-picosecond structural dynamics of retinal isomerization in the light-driven proton pump bacteriorhodopsin using an x-ray laser. A series of structural snapshots with near-atomic spatial and temporal resolution in the femtosecond regime show how the excited all- trans retinal samples conformational states within the protein binding pocket prior to passing through a twisted geometry and emerging in the 13 -cis conformation. Our findings suggest ultrafast collective motions of aspartic acid residues and functional water molecules in the proximity of the retinal Schiff base as a key ingredient for this stereo-selective and efficient photochemical reaction. Copyright © 2018, American Association for the Advancement of Science.

Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [ Co ( terpy ) 2 ] 2 +

DOE PAGES

Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S.; ...

2016-06-30

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

Ultrafast Structural Dynamics in Combustion Relevant Model Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weber, Peter M.

2014-03-31

The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energymore » of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or excited valence states is measured by inducing the dynamics using a near UV laser pulse, and employing a multi-photon ionization scheme via the Rydberg states as a probe process. Thus, the technique is capable of measuring the reaction dynamics in any electronic state of neutral molecules.« less

Apparatus and method to enhance X-ray production in laser produced plasmas

DOEpatents

Augustoni, A.L.; Gerardo, J.B.; Raymond, T.D.

1992-12-29

Method and apparatus for generating x-rays for use in, for instance, x-ray photolithography is disclosed. The method of generating x-rays includes the steps of providing a target and irradiating the target with a laser system which produces a train of sub-pulses to generate an x-ray producing plasma. The sub-pulses are of both high intensity and short duration. The apparatus for generating x-rays from a plasma includes a vacuum chamber, a target supported within the chamber and a laser system, including a short storage time laser. 8 figs.

X-ray analog pixel array detector for single synchrotron bunch time-resolved imaging.

PubMed

Koerner, Lucas J; Gruner, Sol M

2011-03-01

Dynamic X-ray studies can reach temporal resolutions limited by only the X-ray pulse duration if the detector is fast enough to segregate synchrotron pulses. An analog integrating pixel array detector with in-pixel storage and temporal resolution of around 150 ns, sufficient to isolate pulses, is presented. Analog integration minimizes count-rate limitations and in-pixel storage captures successive pulses. Fundamental tests of noise and linearity as well as high-speed laser measurements are shown. The detector resolved individual bunch trains at the Cornell High Energy Synchrotron Source at levels of up to 3.7 × 10(3) X-rays per pixel per train. When applied to turn-by-turn X-ray beam characterization, single-shot intensity measurements were made with a repeatability of 0.4% and horizontal oscillations of the positron cloud were detected.

X-ray analog pixel array detector for single synchrotron bunch time-resolved imaging

PubMed Central

Koerner, Lucas J.; Gruner, Sol M.

2011-01-01

Dynamic X-ray studies can reach temporal resolutions limited by only the X-ray pulse duration if the detector is fast enough to segregate synchrotron pulses. An analog integrating pixel array detector with in-pixel storage and temporal resolution of around 150 ns, sufficient to isolate pulses, is presented. Analog integration minimizes count-rate limitations and in-pixel storage captures successive pulses. Fundamental tests of noise and linearity as well as high-speed laser measurements are shown. The detector resolved individual bunch trains at the Cornell High Energy Synchrotron Source at levels of up to 3.7 × 103 X-rays per pixel per train. When applied to turn-by-turn X-ray beam characterization, single-shot intensity measurements were made with a repeatability of 0.4% and horizontal oscillations of the positron cloud were detected. PMID:21335901

Progress Towards Improved Analysis of TES X-ray Data Using Principal Component Analysis

NASA Technical Reports Server (NTRS)

Busch, S. E.; Adams, J. S.; Bandler, S. R.; Chervenak, J. A.; Eckart, M. E.; Finkbeiner, F. M.; Fixsen, D. J.; Kelley, R. L.; Kilbourne, C. A.; Lee, S.-J.;

Compact x-ray source based on burst-mode inverse Compton scattering at 100 kHz

DOE PAGES

Graves, W.  S.; Bessuille, J.; Brown, P.; ...

2014-12-01

A design for a compact x-ray light source (CXLS) with flux and brilliance orders of magnitude beyond existing laboratory scale sources is presented. The source is based on inverse Compton scattering of a high brightness electron bunch on a picosecond laser pulse. The accelerator is a novel high-efficiency standingwave linac and rf photoinjector powered by a single ultrastable rf transmitter at X-band rf frequency. The high efficiency permits operation at repetition rates up to 1 kHz, which is further boosted to 100 kHz by operating with trains of 100 bunches of 100 pC charge, each separated by 5 ns. Themore » entire accelerator is approximately 1 meter long and produces hard x rays tunable over a wide range of photon energies. The colliding laser is a Yb:YAG solid-state amplifier producing 1030 nm, 100 mJ pulses at the same 1 kHz repetition rate as the accelerator. The laser pulse is frequency-doubled and stored for many passes in a ringdown cavity to match the linac pulse structure. At a photon energy of 12.4 keV, the predicted x-ray flux is 5 × 10¹¹ photons/second in a 5% bandwidth and the brilliance is 2 × 10¹² photons/(sec mm² mrad² 0.1%) in pulses with rms pulse length of 490 fs. The nominal electron beam parameters are 18 MeV kinetic energy, 10 microamp average current, 0.5 microsecond macropulse length, resulting in average electron beam power of 180 W. Optimization of the x-ray output is presented along with design of the accelerator, laser, and x-ray optic components that are specific to the particular characteristics of the Compton scattered x-ray pulses.« less

Simulations of X-ray diffraction of shock-compressed single-crystal tantalum with synchrotron undulator sources.

PubMed

Tang, M X; Zhang, Y Y; E, J C; Luo, S N

2018-05-01

Polychromatic synchrotron undulator X-ray sources are useful for ultrafast single-crystal diffraction under shock compression. Here, simulations of X-ray diffraction of shock-compressed single-crystal tantalum with realistic undulator sources are reported, based on large-scale molecular dynamics simulations. Purely elastic deformation, elastic-plastic two-wave structure, and severe plastic deformation under different impact velocities are explored, as well as an edge release case. Transmission-mode diffraction simulations consider crystallographic orientation, loading direction, incident beam direction, X-ray spectrum bandwidth and realistic detector size. Diffraction patterns and reciprocal space nodes are obtained from atomic configurations for different loading (elastic and plastic) and detection conditions, and interpretation of the diffraction patterns is discussed.

Simulations of X-ray diffraction of shock-compressed single-crystal tantalum with synchrotron undulator sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tang, M. X.; Zhang, Y. Y.; E, J. C.

Polychromatic synchrotron undulator X-ray sources are useful for ultrafast single-crystal diffraction under shock compression. Here, simulations of X-ray diffraction of shock-compressed single-crystal tantalum with realistic undulator sources are reported, based on large-scale molecular dynamics simulations. Purely elastic deformation, elastic–plastic two-wave structure, and severe plastic deformation under different impact velocities are explored, as well as an edge release case. Transmission-mode diffraction simulations consider crystallographic orientation, loading direction, incident beam direction, X-ray spectrum bandwidth and realistic detector size. Diffraction patterns and reciprocal space nodes are obtained from atomic configurations for different loading (elastic and plastic) and detection conditions, and interpretation of themore » diffraction patterns is discussed.« less

X-Pinch And Its Applications In X-ray Radiograph

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zou Xiaobing; Wang Xinxin; Liu Rui

2009-07-07

An X-pinch device and the related diagnostics of x-ray emission from X-pinch were briefly described. The time-resolved x-ray measurements with photoconducting diodes show that the x-ray pulse usually consists of two subnanosecond peaks with a time interval of about 0.5 ns. Being consistent with these two peaks of the x-ray pulse, two point x-ray sources of size ranging from 100 mum to 5 mum and depending on cut-off x-ray photon energy were usually observed on the pinhole pictures. The x-pinch was used as x-ray source for backlighting of the electrical explosion of single wire and the evolution of X-pinch, andmore » for phase-contrast imaging of soft biological objects such as a small shrimp and a mosquito.« less

Proof of the Feasibility of Coherent and Incoherent Schemes for Pumping a Gamma-Ray Laser

DTIC Science & Technology

1990-03-01

systems, a dc power supply or a resonantly pulse a laboratory-swcled source of intense pulses of x rays deliv- charged sobirce. The latter configuration...GENERATOR. V 2 X- KRAY POWER tc o f- LM HA Tcs -0-50VOIC L SAYFir, 2. Resonant pulse power supply used TRIGGER to charge (he Blumlean in these expert- UNIT...primary The scaling of x-ray outputs to larger values with in- power supply to the pulse-charged system prevented the ac- creased system size is illustrated

Anomalous Behavior of the Homogeneous Ice Nucleation Rate in “No-Man’s Land”

PubMed Central

2015-01-01

We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit TH by cooling micrometer-sized droplets (microdroplets) evaporatively at 103–104 K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water’s diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at <227 K, but vitrify at cooling rates of 106–107 K/s. We also hypothesize that the slower increase in the nucleation rate is connected with the proposed “fragile-to-strong” transition anomaly in water. PMID:26207172

Real-time dynamics of Auger wave packets and decays in ultrafast charge migration processes

NASA Astrophysics Data System (ADS)

Covito, F.; Perfetto, E.; Rubio, A.; Stefanucci, G.

2018-06-01

The Auger decay is a relevant recombination channel during the first few femtoseconds of molecular targets impinged by attosecond XUV or soft x-ray pulses. Including this mechanism in time-dependent simulations of charge-migration processes is a difficult task, and Auger scatterings are often ignored altogether. In this work we present an advance of the current state-of-the-art by putting forward a real-time approach based on nonequilibrium Green's functions suitable for first-principles calculations of molecules with tens of active electrons. To demonstrate the accuracy of the method we report comparisons against accurate grid simulations of one-dimensional systems. We also predict a highly asymmetric profile of the Auger wave packet, with a long tail exhibiting ripples temporally spaced by the inverse of the Auger energy.

Optimization for Single-Spike X-Ray FELs at LCLS with a Low Charge Beam

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, L.; Ding, Y.; Huang, Z.

2011-12-14

The Linac Coherent Light Source is an x-ray free-electron laser at the SLAC National Accelerator Laboratory, which is operating at x-ray wavelengths of 20-1.2 Angstrom with peak brightness nearly ten orders of magnitude beyond conventional synchrotron radiation sources. At the low charge operation mode (20 pC), the x-ray pulse length can be <10 fs. In this paper we report our numerical optimization and simulations to produce even shorter x-ray pulses by optimizing the machine and undulator setup at 20 pC charge. In the soft x-ray regime, with combination of slotted-foil or undulator taper, a single spike x-ray pulse is achievablemore » with peak FEL power of a few 10s GW. Linac Coherent Light Source (LCLS), the world's first hard x-ray Free electron laser (FEL), has started operation since 2009. With nominal operation charge of 250 pC, the generated x-ray pulse length is from 70 fs to a few hundred fs. This marks the beginning of a new era of ultrashort x-ray sciences. In addition, a low charge (20pC) operation mode has also been established. Since the collective effects are reduced at the low charge mode, we can increase the compression factor and still achieve a few kA peak current. The expected electron beam and x-ray pulses are less than 10 fs. There are growing interests in even shorter x-ray pulses, such as fs to sub-fs regime. One of the simple solutions is going to even lower charge. As discussed, single-spike x-ray pulses can be generated using 1 pC charge. However, this charge level is out of the present LCLS diagnostic range. 20 pC is a reasonable operation charge at LCLS, based on the present diagnostic system. At 20 pC in the soft x-ray wavelength regime, we have experimentally demonstrated that FEL can work at undercompression or over-compression mode, such as 1 degree off the full-compression; at full-compression, however, there is almost no lasing. In hard x-ray wavelength regime, we observed that there are reasonable photons generated even at full-compression mode, although the photon number is less than that from under-compression or over-compression mode. Since we cannot measure the x-ray pulse length at this time scale, the machine is typically optimized for generating maximum photons, not minimum pulse length. In this paper, we study the methods of producing femtosecond (or single-spike) x-ray pulses at LCLS with 20 pC charge, based on start-to-end simulations. Figure 1 shows a layout of LCLS. The compression in the second bunch compressor (BC2) determines the final e-beam bunch length. However, the laser heater, dog-leg after the main linac (DL2) and collective effects also affect the final bunch length. To adjust BC2 compression, we can either change the L2 phase or BC2 R{sub 56}. In this paper we only tune L2 phase while keep BC2 R{sub 56} fixed. For the start-to-end simulations, we used IMPACT-T and ELEGANT tracking from the photocathode to the entrance of the undulator, after that the FEL radiation was simulated with GENESIS. IMPACT-T tracks about 10{sup 6} particles in the injector part until 135 MeV, including 3D space charge force. The output particles from IMPACT-T are smoothed and increased to 12 x 10{sup 6} to reduce high-frequency numerical noise for subsequent ELEGANT simulations, which include linear and nonlinear transport effects, a 1D transient model of CSR, and longitudinal space charge effects, as well as geometric and resistive wake fields in the accelerator. In GENESIS part, the longitudinal wake field from undulator chamber and longitudinal space field are also included.« less

Characteristics of light reflected from a dense ionization wave with a tunable velocity.

PubMed

Zhidkov, A; Esirkepov, T; Fujii, T; Nemoto, K; Koga, J; Bulanov, S V

2009-11-20

An optically dense ionization wave (IW) produced by two femtosecond (approximately 10/30 fs) laser pulses focused cylindrically and crossing each other may become an efficient coherent x-ray converter in accordance with the Semenova-Lampe theory. The resulting velocity of a quasiplane IW in the vicinity of pulse intersection changes with the angle between the pulses from the group velocity of ionizing pulses to infinity allowing a tuning of the wavelength of x rays and their bunching. The x-ray spectra after scattering of a lower frequency and long coherent light pulse change from the monochromatic to high order harmoniclike with the duration of the ionizing pulses.

Ultrafast photophysics of transition metal complexes.

PubMed

Chergui, Majed

2015-03-17

The properties of transition metal complexes are interesting not only for their potential applications in solar energy conversion, OLEDs, molecular electronics, biology, photochemistry, etc. but also for their fascinating photophysical properties that call for a rethinking of fundamental concepts. With the advent of ultrafast spectroscopy over 25 years ago and, more particularly, with improvements in the past 10-15 years, a new area of study was opened that has led to insightful observations of the intramolecular relaxation processes such as internal conversion (IC), intersystem crossing (ISC), and intramolecular vibrational redistribution (IVR). Indeed, ultrafast optical spectroscopic tools, such as fluorescence up-conversion, show that in many cases, intramolecular relaxation processes can be extremely fast and even shorter than time scales of vibrations. In addition, more and more examples are appearing showing that ultrafast ISC rates do not scale with the magnitude of the metal spin-orbit coupling constant, that is, that there is no heavy-atom effect on ultrafast time scales. It appears that the structural dynamics of the system and the density of states play a crucial role therein. While optical spectroscopy delivers an insightful picture of electronic relaxation processes involving valence orbitals, the photophysics of metal complexes involves excitations that may be centered on the metal (called metal-centered or MC) or the ligand (called ligand-centered or LC) or involve a transition from one to the other or vice versa (called MLCT or LMCT). These excitations call for an element-specific probe of the photophysics, which is achieved by X-ray absorption spectroscopy. In this case, transitions from core orbitals to valence orbitals or higher allow probing the electronic structure changes induced by the optical excitation of the valence orbitals, while also delivering information about the geometrical rearrangement of the neighbor atoms around the atom of interest. With the emergence of new instruments such as X-ray free electron lasers (XFELs), it is now possible to perform ultrafast laser pump/X-ray emission probe experiments. In this case, one probes the density of occupied states. These core-level spectroscopies and other emerging ones, such as photoelectron spectroscopy of solutions, are delivering a hitherto unseen degree of detail into the photophysics of metal-based molecular complexes. In this Account, we will give examples of applications of the various methods listed above to address specific photophysical processes.

Clean sub-8-fs pulses at 400 nm generated by a hollow fiber compressor for ultraviolet ultrafast pump-probe spectroscopy.

PubMed

Liu, Jun; Okamura, Kotaro; Kida, Yuichiro; Teramoto, Takahiro; Kobayashi, Takayoshi

2010-09-27

Clean 7.5 fs pulses at 400 nm with less than 3% energy in tiny satellite pulses were obtained by spectral broadening in a hollow fiber and dispersive compensating using a prism pair together with a deformable mirror system. As an example, this stable and clean pulse was used to study the ultrafast pump-probe spectroscopy of photoactive yellow protein. Moreover, the self-diffraction signal shows a smoothed and broadened laser spectrum and is expected to have a further clean laser pulse, which makes it more useful in the ultrafast pump-probe spectroscopy in the future.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, L. X.; Zhang, X.; Lockard, J. V.

Transient molecular structures along chemical reaction pathways are important for predicting molecular reactivity, understanding reaction mechanisms, as well as controlling reaction pathways. During the past decade, X-ray transient absorption spectroscopy (XTA, or LITR-XAS, laser-initiated X-ray absorption spectroscopy), analogous to the commonly used optical transient absorption spectroscopy, has been developed. XTA uses a laser pulse to trigger a fundamental chemical process, and an X-ray pulse(s) to probe transient structures as a function of the time delay between the pump and probe pulses. Using X-ray pulses with high photon flux from synchrotron sources, transient electronic and molecular structures of metal complexes havemore » been studied in disordered media from homogeneous solutions to heterogeneous solution-solid interfaces. Several examples from the studies at the Advanced Photon Source in Argonne National Laboratory are summarized, including excited-state metalloporphyrins, metal-to-ligand charge transfer (MLCT) states of transition metal complexes, and charge transfer states of metal complexes at the interface with semiconductor nanoparticles. Recent developments of the method are briefly described followed by a future prospective of XTA. It is envisioned that concurrent developments in X-ray free-electron lasers and synchrotron X-ray facilities as well as other table-top laser-driven femtosecond X-ray sources will make many breakthroughs and realise dreams of visualizing molecular movies and snapshots, which ultimately enable chemical reaction pathways to be controlled.« less

High-intensity double-pulse X-ray free-electron laser

DOE PAGES

Marinelli, A.; Ratner, D.; Lutman, A. A.; ...

2015-03-06

The X-ray free-electron laser has opened a new era for photon science, improving the X-ray brightness by ten orders of magnitude over previously available sources. Similar to an optical laser, the spectral and temporal structure of the radiation pulses can be tailored to the specific needs of many experiments by accurately manipulating the lasing medium, that is, the electron beam. Here we report the generation of mJ-level two-colour hard X-ray pulses of few femtoseconds duration with an XFEL driven by twin electron bunches at the Linac Coherent Light Source. This performance represents an improvement of over an order of magnitudemore » in peak power over state-of-the-art two-colour XFELs. The unprecedented intensity and temporal coherence of this new two-colour X-ray free-electron laser enable an entirely new set of scientific applications, ranging from X-ray pump/X-ray probe experiments to the imaging of complex biological samples with multiple wavelength anomalous dispersion.« less

Hitomi X-ray studies of giant radio pulses from the Crab pulsar

NASA Astrophysics Data System (ADS)

Hitomi Collaboration; Aharonian, Felix; Akamatsu, Hiroki; Akimoto, Fumie; Allen, Steven W.; Angelini, Lorella; Audard, Marc; Awaki, Hisamitsu; Axelsson, Magnus; Bamba, Aya; Bautz, Marshall W.; Blandford, Roger; Brenneman, Laura W.; Brown, Gregory V.; Bulbul, Esra; Cackett, Edward M.; Chernyakova, Maria; Chiao, Meng P.; Coppi, Paolo S.; Costantini, Elisa; de Plaa, Jelle; de Vries, Cor P.; den Herder, Jan-Willem; Done, Chris; Dotani, Tadayasu; Ebisawa, Ken; Eckart, Megan E.; Enoto, Teruaki; Ezoe, Yuichiro; Fabian, Andrew C.; Ferrigno, Carlo; Foster, Adam R.; Fujimoto, Ryuichi; Fukazawa, Yasushi; Furuzawa, Akihiro; Galeazzi, Massimiliano; Gallo, Luigi C.; Gandhi, Poshak; Giustini, Margherita; Goldwurm, Andrea; Gu, Liyi; Guainazzi, Matteo; Haba, Yoshito; Hagino, Kouichi; Hamaguchi, Kenji; Harrus, Ilana M.; Hatsukade, Isamu; Hayashi, Katsuhiro; Hayashi, Takayuki; Hayashida, Kiyoshi; Hiraga, Junko S.; Hornschemeier, Ann; Hoshino, Akio; Hughes, John P.; Ichinohe, Yuto; Iizuka, Ryo; Inoue, Hajime; Inoue, Yoshiyuki; Ishida, Manabu; Ishikawa, Kumi; Ishisaki, Yoshitaka; Iwai, Masachika; Kaastra, Jelle; Kallman, Tim; Kamae, Tsuneyoshi; Kataoka, Jun; Katsuda, Satoru; Kawai, Nobuyuki; Kelley, Richard L.; Kilbourne, Caroline A.; Kitaguchi, Takao; Kitamoto, Shunji; Kitayama, Tetsu; Kohmura, Takayoshi; Kokubun, Motohide; Koyama, Katsuji; Koyama, Shu; Kretschmar, Peter; Krimm, Hans A.; Kubota, Aya; Kunieda, Hideyo; Laurent, Philippe; Lee, Shiu-Hang; Leutenegger, Maurice A.; Limousin, Olivier O.; Loewenstein, Michael; Long, Knox S.; Lumb, David; Madejski, Greg; Maeda, Yoshitomo; Maier, Daniel; Makishima, Kazuo; Markevitch, Maxim; Matsumoto, Hironori; Matsushita, Kyoko; McCammon, Dan; McNamara, Brian R.; Mehdipour, Missagh; Miller, Eric D.; Miller, Jon M.; Mineshige, Shin; Mitsuda, Kazuhisa; Mitsuishi, Ikuyuki; Miyazawa, Takuya; Mizuno, Tsunefumi; Mori, Hideyuki; Mori, Koji; Mukai, Koji; Murakami, Hiroshi; Mushotzky, Richard F.; Nakagawa, Takao; Nakajima, Hiroshi; Nakamori, Takeshi; Nakashima, Shinya; Nakazawa, Kazuhiro; Nobukawa, Kumiko K.; Nobukawa, Masayoshi; Noda, Hirofumi; Odaka, Hirokazu; Ohashi, Takaya; Ohno, Masanori; Okajima, Takashi; Oshimizu, Kenya; Ota, Naomi; Ozaki, Masanobu; Paerels, Frits; Paltani, Stéphane; Petre, Robert; Pinto, Ciro; Porter, Frederick S.; Pottschmidt, Katja; Reynolds, Christopher S.; Safi-Harb, Samar; Saito, Shinya; Sakai, Kazuhiro; Sasaki, Toru; Sato, Goro; Sato, Kosuke; Sato, Rie; Sawada, Makoto; Schartel, Norbert; Serlemtsos, Peter J.; Seta, Hiromi; Shidatsu, Megumi; Simionescu, Aurora; Smith, Randall K.; Soong, Yang; Stawarz, Łukasz; Sugawara, Yasuharu; Sugita, Satoshi; Szymkowiak, Andrew; Tajima, Hiroyasu; Takahashi, Hiromitsu; Takahashi, Tadayuki; Takeda, Shiníchiro; Takei, Yoh; Tamagawa, Toru; Tamura, Takayuki; Tanaka, Takaaki; Tanaka, Yasuo; Tanaka, Yasuyuki T.; Tashiro, Makoto S.; Tawara, Yuzuru; Terada, Yukikatsu; Terashima, Yuichi; Tombesi, Francesco; Tomida, Hiroshi; Tsuboi, Yohko; Tsujimoto, Masahiro; Tsunemi, Hiroshi; Tsuru, Takeshi Go; Uchida, Hiroyuki; Uchiyama, Hideki; Uchiyama, Yasunobu; Ueda, Shutaro; Ueda, Yoshihiro; Uno, Shiníchiro; Urry, C. Megan; Ursino, Eugenio; Watanabe, Shin; Werner, Norbert; Wilkins, Dan R.; Williams, Brian J.; Yamada, Shinya; Yamaguchi, Hiroya; Yamaoka, Kazutaka; Yamasaki, Noriko Y.; Yamauchi, Makoto; Yamauchi, Shigeo; Yaqoob, Tahir; Yatsu, Yoichi; Yonetoku, Daisuke; Zhuravleva, Irina; Zoghbi, Abderahmen; Terasawa, Toshio; Sekido, Mamoru; Takefuji, Kazuhiro; Kawai, Eiji; Misawa, Hiroaki; Tsuchiya, Fuminori; Yamazaki, Ryo; Kobayashi, Eiji; Kisaka, Shota; Aoki, Takahiro

2018-03-01

To search for giant X-ray pulses correlated with the giant radio pulses (GRPs) from the Crab pulsar, we performed a simultaneous observation of the Crab pulsar with the X-ray satellite Hitomi in the 2-300 keV band and the Kashima NICT radio telescope in the 1.4-1.7 GHz band with a net exposure of about 2 ks on 2016 March 25, just before the loss of the Hitomi mission. The timing performance of the Hitomi instruments was confirmed to meet the timing requirement and about 1000 and 100 GRPs were simultaneously observed at the main pulse and inter-pulse phases, respectively, and we found no apparent correlation between the giant radio pulses and the X-ray emission in either the main pulse or inter-pulse phase. All variations are within the 2 σ fluctuations of the X-ray fluxes at the pulse peaks, and the 3 σ upper limits of variations of main pulse or inter-pulse GRPs are 22% or 80% of the peak flux in a 0.20 phase width, respectively, in the 2-300 keV band. The values for main pulse or inter-pulse GRPs become 25% or 110%, respectively, when the phase width is restricted to the 0.03 phase. Among the upper limits from the Hitomi satellite, those in the 4.5-10 keV and 70-300 keV bands are obtained for the first time, and those in other bands are consistent with previous reports. Numerically, the upper limits of the main pulse and inter-pulse GRPs in the 0.20 phase width are about (2.4 and 9.3) × 10-11 erg cm-2, respectively. No significant variability in pulse profiles implies that the GRPs originated from a local place within the magnetosphere. Although the number of photon-emitting particles should temporarily increase to account for the brightening of the radio emission, the results do not statistically rule out variations correlated with the GRPs, because the possible X-ray enhancement may appear due to a >0.02% brightening of the pulse-peak flux under such conditions.

Polarization control in an X-ray free-electron laser

DOE PAGES

Lutman, Alberto A.; MacArthur, James P.; Ilchen, Markus; ...

2016-05-09

X-ray free-electron lasers are unique sources of high-brightness coherent radiation. However, existing devices supply only linearly polarized light, precluding studies of chiral dynamics. A device called the Delta undulator has been installed at the Linac Coherent Light Source (LCLS) to provide tunable polarization. With a reverse tapered planar undulator line to pre-microbunch the beam and the novel technique of beam diverting, hundreds of microjoules of circularly polarized X-ray pulses are produced at 500–1,200 eV. These X-ray pulses are tens of femtoseconds long, have a degree of circular polarization of 0.98 –0.04 +0.02 at 707 eV and may be scanned inmore » energy. We also present a new two-colour X-ray pump–X-ray probe operating mode for the LCLS. As a result, energy differences of ΔE/E = 2.4% are supported, and the second pulse can be adjusted to any elliptical polarization. In this mode, the pointing, timing, intensity and wavelength of the two pulses can be modified.« less

Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers

PubMed Central

Chen, Ming-Chang; Mancuso, Christopher; Hernández-García, Carlos; Dollar, Franklin; Galloway, Ben; Popmintchev, Dimitar; Huang, Pei-Chi; Walker, Barry; Plaja, Luis; Jaroń-Becker, Agnieszka A.; Becker, Andreas; Murnane, Margaret M.; Kapteyn, Henry C.; Popmintchev, Tenio

2014-01-01

High harmonic generation driven by femtosecond lasers makes it possible to capture the fastest dynamics in molecules and materials. However, to date the shortest subfemtosecond (attosecond, 10−18 s) pulses have been produced only in the extreme UV region of the spectrum below 100 eV, which limits the range of materials and molecular systems that can be explored. Here we experimentally demonstrate a remarkable convergence of physics: when midinfrared lasers are used to drive high harmonic generation, the conditions for optimal bright, soft X-ray generation naturally coincide with the generation of isolated attosecond pulses. The temporal window over which phase matching occurs shrinks rapidly with increasing driving laser wavelength, to the extent that bright isolated attosecond pulses are the norm for 2-µm driving lasers. Harnessing this realization, we experimentally demonstrate the generation of isolated soft X-ray attosecond pulses at photon energies up to 180 eV for the first time, to our knowledge, with a transform limit of 35 attoseconds (as), and a predicted linear chirp of 300 as. Most surprisingly, advanced theory shows that in contrast with as pulse generation in the extreme UV, long-duration, 10-cycle, driving laser pulses are required to generate isolated soft X-ray bursts efficiently, to mitigate group velocity walk-off between the laser and the X-ray fields that otherwise limit the conversion efficiency. Our work demonstrates a clear and straightforward approach for robustly generating bright isolated attosecond pulses of electromagnetic radiation throughout the soft X-ray region of the spectrum. PMID:24850866

Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers.

PubMed

Chen, Ming-Chang; Mancuso, Christopher; Hernández-García, Carlos; Dollar, Franklin; Galloway, Ben; Popmintchev, Dimitar; Huang, Pei-Chi; Walker, Barry; Plaja, Luis; Jaroń-Becker, Agnieszka A; Becker, Andreas; Murnane, Margaret M; Kapteyn, Henry C; Popmintchev, Tenio

2014-06-10

High harmonic generation driven by femtosecond lasers makes it possible to capture the fastest dynamics in molecules and materials. However, to date the shortest subfemtosecond (attosecond, 10(-18) s) pulses have been produced only in the extreme UV region of the spectrum below 100 eV, which limits the range of materials and molecular systems that can be explored. Here we experimentally demonstrate a remarkable convergence of physics: when midinfrared lasers are used to drive high harmonic generation, the conditions for optimal bright, soft X-ray generation naturally coincide with the generation of isolated attosecond pulses. The temporal window over which phase matching occurs shrinks rapidly with increasing driving laser wavelength, to the extent that bright isolated attosecond pulses are the norm for 2-µm driving lasers. Harnessing this realization, we experimentally demonstrate the generation of isolated soft X-ray attosecond pulses at photon energies up to 180 eV for the first time, to our knowledge, with a transform limit of 35 attoseconds (as), and a predicted linear chirp of 300 as. Most surprisingly, advanced theory shows that in contrast with as pulse generation in the extreme UV, long-duration, 10-cycle, driving laser pulses are required to generate isolated soft X-ray bursts efficiently, to mitigate group velocity walk-off between the laser and the X-ray fields that otherwise limit the conversion efficiency. Our work demonstrates a clear and straightforward approach for robustly generating bright isolated attosecond pulses of electromagnetic radiation throughout the soft X-ray region of the spectrum.

Heterogeneity in Short Gamma-Ray Bursts

NASA Technical Reports Server (NTRS)

Norris, Jay P.; Gehrels Neil; Scargle, Jeffrey D.

2011-01-01

We analyze the Swift/BAT sample of short gamma-ray bursts, using an objective Bayesian Block procedure to extract temporal descriptors of the bursts' initial pulse complexes (IPCs). The sample comprises 12 and 41 bursts with and without extended emission (EE) components, respectively. IPCs of non-EE bursts are dominated by single pulse structures, while EE bursts tend to have two or more pulse structures. The medians of characteristic timescales - durations, pulse structure widths, and peak intervals - for EE bursts are factors of approx 2-3 longer than for non-EE bursts. A trend previously reported by Hakkila and colleagues unifying long and short bursts - the anti-correlation of pulse intensity and width - continues in the two short burst groups, with non-EE bursts extending to more intense, narrower pulses. In addition we find that preceding and succeeding pulse intensities are anti-correlated with pulse interval. We also examine the short burst X-ray afterglows as observed by the Swift/XRT. The median flux of the initial XRT detections for EE bursts (approx 6 X 10(exp -10) erg / sq cm/ s) is approx > 20 x brighter than for non-EE bursts, and the median X-ray afterglow duration for EE bursts (approx 60,000 s) is approx 30 x longer than for non-EE bursts. The tendency for EE bursts toward longer prompt-emission timescales and higher initial X-ray afterglow fluxes implies larger energy injections powering the afterglows. The longer-lasting X-ray afterglows of EE bursts may suggest that a significant fraction explode into more dense environments than non-EE bursts, or that the sometimes-dominant EE component efficiently p()wers the afterglow. Combined, these results favor different progenitors for EE and non-EE short bursts.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sperling, P.; Fletcher, L. B.; Chung, H. -K.

2016-03-29

We measure the highly-resolved inelastic x-ray scattering spectrum of isochorically ultrafast heated aluminum. In the x-ray forward scattering spectra the electron temperature could be measured from the down- and upshifted plasmon, where the electron density of ne = 1:8 1023 cm 3 is known a priori. We have studied the plasmon damping by applying electron-particle collision models beyond the Born approximation determining the electrical conductivity of warm dense aluminum.

Discovery of a 50 millisecond pulsar in the Large Magellanic Cloud

NASA Technical Reports Server (NTRS)

Seward, F. D.; Harnden, F. R., Jr.; Helfand, D. J.

1984-01-01

The present investigation is concerned with the discovery of a new pulsed X-ray source in the Large Magellanic Cloud (LMC) supernova remnant 0540 - 693. The SNR 0540 - 693 is one of three suspected Crab-like remnants in the LMC. The existing X-ray, optical, and radio observations of the remnant itself are discussed, and an analysis is conducted of the implications of the period, period derivative, and X-ray pulse shape of the new source. It is concluded that the pulsed X-ray source is almost certainly a young, isolated pulsar. Many of its properties are very similar to those of the Crab pulsar.

Clusters in intense x-ray pulses

NASA Astrophysics Data System (ADS)

Bostedt, Christoph

2012-06-01

Free-electron lasers can deliver extremely intense, coherent x-ray flashes with femtosecond pulse length, opening the door for imaging single nanoscale objects in a single shot. All matter irradiated by these intense x-ray pulses, however, will be transformed into a highly-excited non-equilibrium plasma within femtoseconds. During the x-ray pulse complex electron dynamics and the onset of atomic disorder will be induced, leading to a time-varying sample. We have performed first experiments about x-ray laser pulse -- cluster interaction with a combined spectroscopy and imaging approach at both, the FLASH free electron laser in Hamburg (Germany) and the LCLS x-ray free-electron laser in Stanford (California). Atomic clusters are ideal for investigating the light - matter interaction because their size can be tuned from the molecular to the bulk regime, thus allowing to distinguish between intra and inter atomic processes. Imaging experiments with xenon clusters show power-density dependent changes in the scattering patterns. Modeling the scattering data indicates that the optical constants of the clusters change during the femtosecond pulse due to the transient creation of high charge states. The results show that ultra fast scattering is a promising approach to study transient states of matter on a femtosecond time scale. Coincident recording of time-of-flight spectra and scattering patterns allows the deconvolution of focal volume and particle size distribution effects. Single-shot single-particle experiments with keV x-rays reveal that for the highest power densities an highly excited and hot cluster plasma is formed for which recombination is suppressed. Time resolved infrared pump -- x-ray probe experiments have started. Here, the clusters are pumped into a nanoplasma state and their time evolution is probed with femtosecond x-ray scattering. The data show strong variations in the scattering patterns stemming from electronic reconfigurations in the cluster plasma. The results will be compared to theoretical predictions and discussed in light of current developments at free-electron laser sources.

The fluid dynamics of microjet explosions caused by extremely intense X-ray pulses

NASA Astrophysics Data System (ADS)

Stan, Claudiu; Laksmono, Hartawan; Sierra, Raymond; Milathianaki, Despina; Koglin, Jason; Messerschmidt, Marc; Williams, Garth; Demirci, Hasan; Botha, Sabine; Nass, Karol; Stone, Howard; Schlichting, Ilme; Shoeman, Robert; Boutet, Sebastien

2014-11-01

Femtosecond X-ray scattering experiments at free-electron laser facilities typically requires liquid jet delivery methods to bring samples to the region of interaction with X-rays. We have imaged optically the damage process in water microjets due to intense hard X-ray pulses at the Linac Coherent Light Source (LCLS), using time-resolved imaging techniques to record movies at rates up to half a billion frames per second. For pulse energies larger than a few percent of the maximum pulse energy available at LCLS, the X-rays deposit energies much larger than the latent heat of vaporization in water, and induce a phase explosion that opens a gap in the jet. The LCLS pulses last a few tens of femtoseconds, but the full evolution of the broken jet is orders of magnitude slower - typically in the microsecond range - due to complex fluid dynamics processes triggered by the phase explosion. Although the explosion results in a complex sequence of phenomena, they lead to an approximately self-similar flow of the liquid in the jet.

Isolated terawatt attosecond hard X-ray pulse generated from single current spike.

PubMed

Shim, Chi Hyun; Parc, Yong Woon; Kumar, Sandeep; Ko, In Soo; Kim, Dong Eon

2018-05-10

Isolated terawatt (TW) attosecond (as) hard X-ray pulse is greatly desired for four-dimensional investigations of natural phenomena with picometer spatial and attosecond temporal resolutions. Since the demand for such sources is continuously increasing, the possibility of generating such pulse by a single current spike without the use of optical or electron delay units in an undulator line is addressed. The conditions of a current spike (width and height) and a modulation laser pulse (wavelength and power) is also discussed. We demonstrate that an isolated TW-level as a hard X-ray can be produced by a properly chosen single current spike in an electron bunch with simulation results. By using realistic specifications of an electron bunch of the Pohang Accelerator Laboratory X-ray Free-Electron Laser (PAL-XFEL), we show that an isolated, >1.0 TW and ~36 as X-ray pulse at 12.4 keV can be generated in an optimized-tapered undulator line. This result opens a new vista for current XFEL operation: the attosecond XFEL.

White light for the fast lane: supercontinuum generation in all-normal dispersion fibers for ultrafast photonics

NASA Astrophysics Data System (ADS)

Heidt, Alexander M.

2014-03-01

This talk will give an overview of the unique properties of supercontinuum generation (SCG) in all-normal dispersion (ANDi) fibers pumped by ultrashort pulses and the possibilities they offer for ultrafast photonics applications. In contrast to their anomalously pumped counterparts, the SCG process in ANDi fibers conserves a single ultrashort pulse in the time domain, completely suppresses soliton formation and decay, and avoids noise-amplifying nonlinear dynamics. The resulting spectra combine the best of both worlds - the broad, more than octave-spanning bandwidths usually associated with anomalous dispersion pumping with the high temporal coherence, pulse-to-pulse stability and well-defined temporal pulse characteristics known from the normal dispersion regime. These characteristics are ideally suited for ultrafast photonics, and I will present application examples including the generation of high quality single-cycle pulses and their amplification, as well as ultrafast spectroscopy. This talk will also explore the exciting new possibilities enabled by extending this approach into the mid-IR spectral region using novel soft glass fiber designs.

Condensation of collective charge ordering in chromium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singer, A.; Marsh, M. J.; Dietze, S. H.

2015-03-01

We report on the dynamics of the structural order parameter in a chromium film using synchrotron radiation in response to photoinduced ultrafast excitations. Following transient optical excitations the effective lattice temperature of the film rises close to the Neel temperature and the charge-density wave (CDW) amplitude is reduced but does not appear to ever be fully destroyed. The persistence of the CDW diffraction signal demonstrates that the CDW, if destroyed by the laser pulse, must be reestablished within the 100-ps time resolution of the synchrotron x-ray pulses. Furthermore, at all times after photoexcitation, the CDW retains its low-temperature periodicity, rathermore » than regenerating with its high-temperature period shortly after photoexcitation. The long-term evolution shows that the CDW reverts to its ground state on a time scale of 370 +/- 40 ps. We attribute the apparent persistence of the CDW to the long-lived periodic lattice displacement in chromium. This study highlights the fundamental role of the lattice distortion and its impact on the recondensation dynamics of the charge ordered state in strongly correlated materials.« less

Improving the efficiency of x-ray lasers

NASA Astrophysics Data System (ADS)

Tallents, Gregory J.; Zeitoun, Philippe; Behjat, A.; Demir, A.; Holden, M.; Krishnan, J.; Lewis, Ciaran L. S.; MacPhee, Andrew G.; Warwick, P. J.; Nantel, Marc; Jamelot, Gerard; Rus, Bedrich; Jaegle, Pierre; Klisnick, Annie; Goedtkindt, P.; Carillon, Antoine; Fill, Ernst E.; Li, Yuelin; Pretzler, Georg; Schloegl, Dieter; Steingruber, Juergen; Neely, David; Norreys, Peter A.; Key, Michael H.; Zhang, Jie; Pert, Geoffrey J.; Healy, S. B.; Plowes, J. A.

1995-09-01

Current successful approaches for achieving soft x-ray lasing typically require pumping laser pulses of duration approximately ns and energy approximately kJ (collisionally pumped schemes) or approximately ps pulses and powers of approximately several TW (recombination-pumped schemes). For applications, it is important to improve the efficiency of soft x-ray lasers and so reduce the required power of pumping lasers. The effect of pre- pulse on neon-like collisionally pumped lasers has been investigated using the LULI laser (Ecole Polytechnique, France). A small pre-pulse level approximately 10-3 of the main pulse energy was found to increase the J equals 0 minus 1 neon-like zinc laser output at 21 nm by an order-of-magnitude with a comparable increase in efficiency. A double pumping laser pulse on neon-like yttrium lasing output at 15 nm obtained with the VULCAN laser (Rutherford Appleton Laboratory, England) was also found to increase the x-ray lasing efficiency. With adiabatically cooled recombination lasing, it is shown that approximately 2 ps pulses are optimum for achieving the desired ionization balance for lasing output. The possibility of achieving recombination lasing at short wavelengths on lithium-like ions with longer pulse lasers has been investigated using the ASTERIX laser (Max-Planck Quantenoptik, Germany). These results are presented and interpreted to provide possible directions for improving the efficiency of x-ray lasers.

High-resolution ab initio three-dimensional x-ray diffraction microscopy

DOE PAGES

Chapman, Henry N.; Barty, Anton; Marchesini, Stefano; ...

2006-01-01

Coherent x-ray diffraction microscopy is a method of imaging nonperiodic isolated objects at resolutions limited, in principle, by only the wavelength and largest scattering angles recorded. We demonstrate x-ray diffraction imaging with high resolution in all three dimensions, as determined by a quantitative analysis of the reconstructed volume images. These images are retrieved from the three-dimensional diffraction data using no a priori knowledge about the shape or composition of the object, which has never before been demonstrated on a nonperiodic object. We also construct two-dimensional images of thick objects with greatly increased depth of focus (without loss of transverse spatialmore » resolution). These methods can be used to image biological and materials science samples at high resolution with x-ray undulator radiation and establishes the techniques to be used in atomic-resolution ultrafast imaging at x-ray free-electron laser sources.« less

Several new directions for ultrafast fiber lasers [Invited].

PubMed

Fu, Walter; Wright, Logan G; Sidorenko, Pavel; Backus, Sterling; Wise, Frank W

2018-04-16

Ultrafast fiber lasers have the potential to make applications of ultrashort pulses widespread - techniques not only for scientists, but also for doctors, manufacturing engineers, and more. Today, this potential is only realized in refractive surgery and some femtosecond micromachining. The existing market for ultrafast lasers remains dominated by solid-state lasers, primarily Ti:sapphire, due to their superior performance. Recent advances show routes to ultrafast fiber sources that provide performance and capabilities equal to, and in some cases beyond, those of Ti:sapphire, in compact, versatile, low-cost devices. In this paper, we discuss the prospects for future ultrafast fiber lasers built on new kinds of pulse generation that capitalize on nonlinear dynamics. We focus primarily on three promising directions: mode-locked oscillators that use nonlinearity to enhance performance; systems that use nonlinear pulse propagation to achieve ultrashort pulses without a mode-locked oscillator; and multimode fiber lasers that exploit nonlinearities in space and time to obtain unparalleled control over an electric field.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Loether, A.; Adams, B. W.; DiCharia, A.

A hard x-ray pump–probe spectrometer using a multi-crystal Bragg reflector is demonstrated at a third generation synchrotron source. This device derives both broadband pump and monochromatic probe pulses directly from a single intense, broadband x-ray pulse centered at 8.767 keV. In conclusion, we present a proof-of-concept experiment which directly measures x-ray induced crystalline lattice strain.

Ab initio studies of ultrafast x-ray scattering of the photodissociation of iodine

DOE Office of Scientific and Technical Information (OSTI.GOV)

Debnarova, Andrea; Techert, Simone; Schmatz, Stefan

2010-09-28

We computationally examine various aspects of the reaction dynamics of the photodissociation and recombination of molecular iodine. We use our recently proposed formalism to calculate time-dependent x-ray scattering signal changes from first principles. Different aspects of the dynamics of this prototypical reaction are studied, such as coherent and noncoherent processes, features of structural relaxation that are periodic in time versus nonperiodic dissociative processes, as well as small electron density changes caused by electronic excitation, all with respect to x-ray scattering. We can demonstrate that wide-angle x-ray scattering offers a possibility to study the changes in electron densities in nonperiodic systems,more » which render it a suitable technique for the investigation of chemical reactions from a structural dynamics point of view.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Bing-Bing; Liu, Jian; Wei, Xu

We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 film by femtosecond X-ray diffraction using a laser plasma-based X-ray source. The ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of (0012) Bragg diffraction after excitation by 1.5 eV and 3.0 eV pump photons for films with different thicknesses. The observed transient lattice response can be well interpreted as a distinct three-step dynamics due to the propagation of coherent acoustic phonons generated by photoinduced quasiparticles (QPs). Employing a normalized phonon propagation model, we found that the photoinduced angular shiftsmore » of the Bragg peak collapse into a universal curve after introducing normalizedn coordinates to account for different thicknesses and pump photon energies, pinpointing the origin of the lattice distortion and its early evolution. In addition, a transient photocurrent measurement indicates that the photoinduced QPs are charge neutral excitons. Mapping the phonon propagation and correlating its dynamics with the QP by ultrafast X-ray diffraction (UXRD) establish a powerful way to study electron-phonon coupling and uncover the exotic physics in strongly correlated systems under nonequilibrium conditions.« less

Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning

DOE PAGES

Sanchez-Gonzalez, A.; Micaelli, P.; Olivier, C.; ...

2017-06-05

Free-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy,more » we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. Lastly, this opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers.« less

Accurate prediction of X-ray pulse properties from a free-electron laser using machine learning

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sanchez-Gonzalez, A.; Micaelli, P.; Olivier, C.

Free-electron lasers providing ultra-short high-brightness pulses of X-ray radiation have great potential for a wide impact on science, and are a critical element for unravelling the structural dynamics of matter. To fully harness this potential, we must accurately know the X-ray properties: intensity, spectrum and temporal profile. Owing to the inherent fluctuations in free-electron lasers, this mandates a full characterization of the properties for each and every pulse. While diagnostics of these properties exist, they are often invasive and many cannot operate at a high-repetition rate. Here, we present a technique for circumventing this limitation. Employing a machine learning strategy,more » we can accurately predict X-ray properties for every shot using only parameters that are easily recorded at high-repetition rate, by training a model on a small set of fully diagnosed pulses. Lastly, this opens the door to fully realizing the promise of next-generation high-repetition rate X-ray lasers.« less

Counting-loss correction for X-ray spectroscopy using unit impulse pulse shaping.

PubMed

Hong, Xu; Zhou, Jianbin; Ni, Shijun; Ma, Yingjie; Yao, Jianfeng; Zhou, Wei; Liu, Yi; Wang, Min

2018-03-01

High-precision measurement of X-ray spectra is affected by the statistical fluctuation of the X-ray beam under low-counting-rate conditions. It is also limited by counting loss resulting from the dead-time of the system and pile-up pulse effects, especially in a high-counting-rate environment. In this paper a detection system based on a FAST-SDD detector and a new kind of unit impulse pulse-shaping method is presented, for counting-loss correction in X-ray spectroscopy. The unit impulse pulse-shaping method is evolved by inverse deviation of the pulse from a reset-type preamplifier and a C-R shaper. It is applied to obtain the true incoming rate of the system based on a general fast-slow channel processing model. The pulses in the fast channel are shaped to unit impulse pulse shape which possesses small width and no undershoot. The counting rate in the fast channel is corrected by evaluating the dead-time of the fast channel before it is used to correct the counting loss in the slow channel.

Focusing X-ray free-electron laser pulses using Kirkpatrick-Baez mirrors at the NCI hutch of the PAL-XFEL.

PubMed

Kim, Jangwoo; Kim, Hyo Yun; Park, Jaehyun; Kim, Sangsoo; Kim, Sunam; Rah, Seungyu; Lim, Jun; Nam, Ki Hyun

2018-01-01

The Pohang Accelerator Laboratory X-ray Free-Electron Laser (PAL-XFEL) is a recently commissioned X-ray free-electron laser (XFEL) facility that provides intense ultrashort X-ray pulses based on the self-amplified spontaneous emission process. The nano-crystallography and coherent imaging (NCI) hutch with forward-scattering geometry is located at the hard X-ray beamline of the PAL-XFEL and provides opportunities to perform serial femtosecond crystallography and coherent X-ray diffraction imaging. To produce intense high-density XFEL pulses at the interaction positions between the X-rays and various samples, a microfocusing Kirkpatrick-Baez (KB) mirror system that includes an ultra-precision manipulator has been developed. In this paper, the design of a KB mirror system that focuses the hard XFEL beam onto a fixed sample point of the NCI hutch, which is positioned along the hard XFEL beamline, is described. The focusing system produces a two-dimensional focusing beam at approximately 2 µm scale across the 2-11 keV photon energy range. XFEL pulses of 9.7 keV energy were successfully focused onto an area of size 1.94 µm × 2.08 µm FWHM.

Hard x ray observations of Vela X-1 and A0535+26 with HEXE: Discovery of cyclotron lines

NASA Technical Reports Server (NTRS)

Kendziorra, E.; Mony, B.; Kretschmar, P.; Maisack, M.; Staubert, R.; Doebereiner, S.; Englhauser, J.; Pietsch, W.; Reppin, C.; Truemper, J.

1992-01-01

The X ray pulsars Vela X-1 (4U 0900-40) and A0535+26) were observed with the High Energy X ray Experiment (HEXE) onboard the Mir space station at energies above 20 keV. The pulse profiles of Vela X-1 (P = 283.22 s for JD 244 7486) and A0535+26 (P = 103.27 s for JD 244 7626) were measured up to at least 100 keV. The time averaged pulse profiles of the two sources both show a clear double peak structure with an asymmetric main pulse and a more symmetric secondary pulse. The spectrum of the main pulse is significantly harder than that of the secondary. Pulse phase resolved spectra show absorption features at 54 keV and possibly 27 keV for Vela X-1 and around 100 keV for A0535+26. If these features are interpreted as second and first harmonic (fundamental) cyclotron absorption lines, lower limits are derived of 2.6 x 10(exp 12) and 4.3 x 10(exp 12) Gauss for the magnetic fields of the neutron stars in Vela X-1 and A0535+26, respectively.

Ablation experiment and threshold calculation of titanium alloy irradiated by ultra-fast pulse laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zheng, Buxiang; Jiang, Gedong; Wang, Wenjun, E-mail: wenjunwang@mail.xjtu.edu.cn

The interaction between an ultra-fast pulse laser and a material's surface has become a research hotspot in recent years. Micromachining of titanium alloy with an ultra-fast pulse laser is a very important research direction, and it has very important theoretical significance and application value in investigating the ablation threshold of titanium alloy irradiated by ultra-fast pulse lasers. Irradiated by a picosecond pulse laser with wavelengths of 1064 nm and 532 nm, the surface morphology and feature sizes, including ablation crater width (i.e. diameter), ablation depth, ablation area, ablation volume, single pulse ablation rate, and so forth, of the titanium alloymore » were studied, and their ablation distributions were obtained. The experimental results show that titanium alloy irradiated by a picosecond pulse infrared laser with a 1064 nm wavelength has better ablation morphology than that of the green picosecond pulse laser with a 532 nm wavelength. The feature sizes are approximately linearly dependent on the laser pulse energy density at low energy density and the monotonic increase in laser pulse energy density. With the increase in energy density, the ablation feature sizes are increased. The rate of increase in the feature sizes slows down gradually once the energy density reaches a certain value, and gradually saturated trends occur at a relatively high energy density. Based on the linear relation between the laser pulse energy density and the crater area of the titanium alloy surface, and the Gaussian distribution of the laser intensity on the cross section, the ablation threshold of titanium alloy irradiated by an ultra-fast pulse laser was calculated to be about 0.109 J/cm{sup 2}.« less

ZAP! The X-Ray Laser is Born

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ratner, Daniel

2009-11-17

SLAC has converted its giant particle accelerator into the world's first X-ray laser. By a billion fold the world's brightest X-ray source, the laser packs a trillion photons into pulses as short as a millionth of a billionth of a second. The ultra-bright, ultra-short X-ray pulses will drive a wide range of new experiments, as scientists strip electrons from atoms, photograph single molecules and make movies of chemical reactions. How has SLAC accomplished such feats of X-ray wizardry? Attend this public lecture to learn about the basics of an X-ray laser, the technologies at SLAC that make it possible, andmore » the exciting new experiments now underway.« less

Ultrafast Laser-Based Spectroscopy and Sensing: Applications in LIBS, CARS, and THz Spectroscopy

PubMed Central

Leahy-Hoppa, Megan R.; Miragliotta, Joseph; Osiander, Robert; Burnett, Jennifer; Dikmelik, Yamac; McEnnis, Caroline; Spicer, James B.

2010-01-01

Ultrafast pulsed lasers find application in a range of spectroscopy and sensing techniques including laser induced breakdown spectroscopy (LIBS), coherent Raman spectroscopy, and terahertz (THz) spectroscopy. Whether based on absorption or emission processes, the characteristics of these techniques are heavily influenced by the use of ultrafast pulses in the signal generation process. Depending on the energy of the pulses used, the essential laser interaction process can primarily involve lattice vibrations, molecular rotations, or a combination of excited states produced by laser heating. While some of these techniques are currently confined to sensing at close ranges, others can be implemented for remote spectroscopic sensing owing principally to the laser pulse duration. We present a review of ultrafast laser-based spectroscopy techniques and discuss the use of these techniques to current and potential chemical and environmental sensing applications. PMID:22399883

DOE Office of Scientific and Technical Information (OSTI.GOV)

LaRue, Jerry; Krejci, Ondrej; Yu, Liang

Here, the direct elucidation of the reaction pathways in heterogeneous catalysis has been challenging due the short-lived nature of reaction intermediates. Here, we directly measured on ultrafast timescales the initial hydrogenation steps of adsorbed CO on a Ru catalyst surface, which is known as the bottleneck reaction in syngas and CO 2 reforming processes. We initiated the hydrogenation of CO with an ultrafast laser temperature jump and probed transient changes in the electronic structure using real-time x-ray spectroscopy. In combination with theoretical simulations, we verified the formation of CHO during CO hydrogenation.

X-ray two-photon absorption with high fluence XFEL pulses

DOE PAGES

Hoszowska, Joanna; Szlachetko, J.; Dousse, J. -Cl.; ...

2015-09-07

Here, we report on nonlinear interaction of solid Fe with intense femtosecond hard x-ray free-electron laser (XFEL) pulses. The experiment was performed at the CXI end-station of the Linac Coherent Light Source (LCLS) by means of high- resolution x-ray emission spectroscopy. The focused x-ray beam provided extreme fluence of ~10 5 photons/Å 2. Two-photon absorption leading to K-shell hollow atom formation and to single K-shell ionization of solid Fe was investigated.

Time-Resolved Macromolecular Crystallography at Modern X-Ray Sources.

PubMed

Schmidt, Marius

2017-01-01

Time-resolved macromolecular crystallography unifies protein structure determination with chemical kinetics. With the advent of fourth generation X-ray sources the time-resolution can be on the order of 10-40 fs, which opens the ultrafast time scale to structure determination. Fundamental motions and transitions associated with chemical reactions in proteins can now be observed. Moreover, new experimental approaches at synchrotrons allow for the straightforward investigation of all kind of reactions in biological macromolecules. Here, recent developments in the field are reviewed.

Large-area tungsten disulfide for ultrafast photonics.

PubMed

Yan, Peiguang; Chen, Hao; Yin, Jinde; Xu, Zihan; Li, Jiarong; Jiang, Zike; Zhang, Wenfei; Wang, Jinzhang; Li, Irene Ling; Sun, Zhipei; Ruan, Shuangchen

2017-02-02

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have attracted significant interest in various optoelectronic applications due to their excellent nonlinear optical properties. One of the most important applications of TMDs is to be employed as an extraordinary optical modulation material (e.g., the saturable absorber (SA)) in ultrafast photonics. The main challenge arises while embedding TMDs into fiber laser systems to generate ultrafast pulse trains and thus constraints their practical applications. Herein, few-layered WS 2 with a large-area was directly transferred on the facet of the pigtail and acted as a SA for erbium-doped fiber laser (EDFL) systems. In our study, WS 2 SA exhibited remarkable nonlinear optical properties (e.g., modulation depth of 15.1% and saturable intensity of 157.6 MW cm -2 ) and was used for ultrafast pulse generation. The soliton pulses with remarkable performances (e.g., ultrashort pulse duration of 1.49 ps, high stability of 71.8 dB, and large pulse average output power of 62.5 mW) could be obtained in a telecommunication band. To the best of our knowledge, the average output power of the mode-locked pulse trains is the highest by employing TMD materials in fiber laser systems. These results indicate that atomically large-area WS 2 could be used as excellent optical modulation materials in ultrafast photonics.

Heterogeneity in Short Gamma-Ray Bursts

NASA Astrophysics Data System (ADS)

Norris, Jay P.; Gehrels, Neil; Scargle, Jeffrey D.

2011-07-01

We analyze the Swift/BAT sample of short gamma-ray bursts, using an objective Bayesian Block procedure to extract temporal descriptors of the bursts' initial pulse complexes (IPCs). The sample is comprised of 12 and 41 bursts with and without extended emission (EE) components, respectively. IPCs of non-EE bursts are dominated by single pulse structures, while EE bursts tend to have two or more pulse structures. The medians of characteristic timescales—durations, pulse structure widths, and peak intervals—for EE bursts are factors of ~2-3 longer than for non-EE bursts. A trend previously reported by Hakkila and colleagues unifying long and short bursts—the anti-correlation of pulse intensity and width—continues in the two short burst groups, with non-EE bursts extending to more intense, narrower pulses. In addition, we find that preceding and succeeding pulse intensities are anti-correlated with pulse interval. We also examine the short burst X-ray afterglows as observed by the Swift/X-Ray Telescope (XRT). The median flux of the initial XRT detections for EE bursts (~6×10-10 erg cm-2 s-1) is gsim20× brighter than for non-EE bursts, and the median X-ray afterglow duration for EE bursts (~60,000 s) is ~30× longer than for non-EE bursts. The tendency for EE bursts toward longer prompt-emission timescales and higher initial X-ray afterglow fluxes implies larger energy injections powering the afterglows. The longer-lasting X-ray afterglows of EE bursts may suggest that a significant fraction explode into denser environments than non-EE bursts, or that the sometimes-dominant EE component efficiently powers the afterglow. Combined, these results favor different progenitors for EE and non-EE short bursts.

Measurement of the effective energy of pulsed X-rays emitted from a Mather-type plasma focus device.

PubMed

Miremad, Seyed Milad; Shirani Bidabadi, Babak

2017-07-01

The current study examined the effective energy of pulsed x-rays emitted from a Mather-type plasma focus device with copper anodes at an energy range of 2-3kJ using x-ray transmission radiography. Aluminum filters of different thicknesses and dental x-ray film were used. When air gas was used at a constant voltage of 21kV at 0.3, 0.6, 0.9 and 1.2 mbar, the effective energy of pulsed the x-ray was 10.9, 10.7, 17.3 and 15.8keV, respectively. At 0.6 mbar of air, as the operating voltage increased to 19, 21 and 23kV, the effective energy of the x-ray radiation was 10.6, 10.7 and 12.4keV, respectively. Comprehensive investigation of the characteristics of x-ray emission from plasma focus devices makes it feasible to use this device as an intensive x-ray generator for medical and industrial purposes. The present study is a part of a program which is planned to realize these applications. Copyright © 2017 Elsevier Ltd. All rights reserved.

Probing molecular dynamics in solution with x-ray valence-to-core spectroscopy

NASA Astrophysics Data System (ADS)

Doumy, Gilles; March, Anne Marie; Tu, Ming-Feng; Al Haddad, Andre; Southworth, Stephen; Young, Linda; Walko, Donald; Bostedt, Christoph

2017-04-01

Hard X-ray spectroscopies are powerful tools for probing the electronic and geometric structure of molecules in complex or disordered systems and have been particularly useful for studying molecules in the solution phase. They are element specific, sensitive to the electronic structure and the local arrangements of surrounding atoms of the element being selectively probed. When combined in a pump-probe scheme with ultrafast lasers, X-ray spectroscopies can be used to track the evolution of structural changes that occur after photoexcitation. Efficient use of hard x-ray radiation coming from high brilliance synchrotrons and upcoming high repetition rate X-ray Free Electron Lasers requires MHz repetition rate lasers and data acquisition systems. High information content Valence-to-Core x-ray emission is directly sensitive to the molecular orbitals involved in photochemistry. We report on recent progress towards fully enabling this photon-hungry technique for the study of time-resolved molecular dynamics, including efficient detection and use of polychromatic x-ray micro-probe at the Advanced Photon Source. Work was supported by the U.S. Department of Energy, Office of Science, Chemical Sciences, Geosciences, and Biosciences Division.

High-flux soft x-ray harmonic generation from ionization-shaped few-cycle laser pulses

PubMed Central

Brahms, Christian; Gregory, Andrew; Tisch, John W. G.; Marangos, Jon P.

2018-01-01

Laser-driven high-harmonic generation provides the only demonstrated route to generating stable, tabletop attosecond x-ray pulses but has low flux compared to other x-ray technologies. We show that high-harmonic generation can produce higher photon energies and flux by using higher laser intensities than are typical, strongly ionizing the medium and creating plasma that reshapes the driving laser field. We obtain high harmonics capable of supporting attosecond pulses up to photon energies of 600 eV and a photon flux inside the water window (284 to 540 eV) 10 times higher than previous attosecond sources. We demonstrate that operating in this regime is key for attosecond pulse generation in the x-ray range and will become increasingly important as harmonic generation moves to fields that drive even longer wavelengths. PMID:29756033

Configuring and Characterizing X-Rays for Laser-Driven Compression Experiments at the Dynamic Compression Sector

NASA Astrophysics Data System (ADS)

Li, Y.; Capatina, D.; D'Amico, K.; Eng, P.; Hawreliak, J.; Graber, T.; Rickerson, D.; Klug, J.; Rigg, P. A.; Gupta, Y. M.

2017-06-01

Coupling laser-driven compression experiments to the x-ray beam at the Dynamic Compression Sector (DCS) at the Advanced Photon Source (APS) of Argonne National Laboratory requires state-of-the-art x-ray focusing, pulse isolation, and diagnostics capabilities. The 100J UV pulsed laser system can be fired once every 20 minutes so precise alignment and focusing of the x-rays on each new sample must be fast and reproducible. Multiple Kirkpatrick-Baez (KB) mirrors are used to achieve a focal spot size as small as 50 μm at the target, while the strategic placement of scintillating screens, cameras, and detectors allows for fast diagnosis of the beam shape, intensity, and alignment of the sample to the x-ray beam. In addition, a series of x-ray choppers and shutters are used to ensure that the sample is exposed to only a single x-ray pulse ( 80ps) during the dynamic compression event and require highly precise synchronization. Details of the technical requirements, layout, and performance of these instruments will be presented. Work supported by DOE/NNSA.

Characterization of Ultrafast Laser Pulses using a Low-dispersion Frequency Resolved Optical Grating Spectrometer

NASA Astrophysics Data System (ADS)

Whitelock, Hope; Bishop, Michael; Khosravi, Soroush; Obaid, Razib; Berrah, Nora

2016-05-01

A low dispersion frequency-resolved optical gating (FROG) spectrometer was designed to characterize ultrashort (<50 femtosecond) laser pulses from a commercial regenerative amplifier, optical parametric amplifier, and a home-built non-colinear optical parametric amplifier. This instrument splits a laser pulse into two replicas with a 90:10 intensity ratio using a thin pellicle beam-splitter and then recombines the pulses in a birefringent medium. The instrument detects a wavelength-sensitive change in polarization of the weak probe pulse in the presence of the stronger pump pulse inside the birefringent medium. Scanning the time delay between the two pulses and acquiring spectra allows for characterization of the frequency and time content of ultrafast laser pulses, that is needed for interpretation of experimental results obtained from these ultrafast laser systems. Funded by the DoE-BES, Grant No. DE-SC0012376.

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

PubMed

Gessner, Oliver; Gühr, Markus

2016-01-19

The directed flow of charge and energy is at the heart of all chemical processes. Extraordinary efforts are underway to monitor and understand the concerted motion of electrons and nuclei with ever increasing spatial and temporal sensitivity. The element specificity, chemical sensitivity, and temporal resolution of ultrafast X-ray spectroscopy techniques hold great promise to provide new insight into the fundamental interactions underlying chemical dynamics in systems ranging from isolated molecules to application-like devices. Here, we focus on the potential of ultrafast X-ray spectroscopy techniques based on the detection of photo- and Auger electrons to provide new fundamental insight into photochemical processes of systems with various degrees of complexity. Isolated nucleobases provide an excellent testing ground for our most fundamental understanding of intramolecular coupling between electrons and nuclei beyond the traditionally applied Born-Oppenheimer approximation. Ultrafast electronic relaxation dynamics enabled by the breakdown of this approximation is the major component of the nucleobase photoprotection mechanisms. Transient X-ray induced Auger electron spectroscopy on photoexcited thymine molecules provides atomic-site specific details of the extremely efficient coupling that converts potentially bond changing ultraviolet photon energy into benign heat. In particular, the time-dependent spectral shift of a specific Auger band is sensitive to the length of a single bond within the molecule. The X-ray induced Auger transients show evidence for an electronic transition out of the initially excited state within only ∼200 fs in contrast to theoretically predicted picosecond population trapping behind a reaction barrier. Photoinduced charge transfer dynamics between transition metal complexes and semiconductor nanostructures are of central importance for many emerging energy and climate relevant technologies. Numerous demonstrations of photovoltaic and photocatalytic activity have been performed based on the combination of strong light absorption in dye molecules with charge separation and transport in adjacent semiconductor nanostructures. However, a fundamental understanding of the enabling and limiting dynamics on critical atomic length- and time scales is often still lacking. Femtosecond time-resolved X-ray photoelectron spectroscopy is employed to gain a better understanding of a short-lived intermediate that may be linked to the unexpectedly limited performance of ZnO based dye-sensitized solar cells by delaying the generation of free charge carriers. The transient spectra strongly suggest that photoexcited dye molecules attached to ZnO nanocrystals inject their charges into the substrate within less than 1 ps but the electrons are then temporarily trapped at the surface of the semiconductor in direct vicinity of the injecting molecules. The experiments are extended to monitor the electronic response of the semiconductor substrate to the collective injection from a monolayer of dye molecules and the subsequent electron-ion recombination dynamics. The results indicate some qualitative similarities but quantitative differences between the recombination dynamics at molecule-semiconductor interfaces and previously studied bulk-surface electron-hole recombination dynamics in photoexcited semiconductors.

Proposed Laser-driven, Dielectric Microstructure Few-cm Long Undulator for Attosecond Coherent X-rays

DOE Office of Scientific and Technical Information (OSTI.GOV)

Plettner, T; Byer, R.L.; /Stanford U., Ginzton Lab.

This article presents the concept of an all-dielectric laser-driven undulator for the generation of coherent X-rays. The proposed laser-driven undulator is expected to produce internal deflection forces equivalent to a several-Tesla magnetic field acting on a speed-of-light particle. The key idea for this laser-driven undulator is its ability to provide phase synchronicity between the deflection force and the electron beam for a distance that is much greater than the laser wavelength. The potential advantage of this undulator is illustrated with a possible design example that assumes a small laser accelerator which delivers a 2 GeV, 1 pC, 1 kHz electronmore » bunch train to a 10 cm long, 1/2 mm period laser-driven undulator. Such an undulator could produce coherent X-ray pulses with {approx}10{sup 9} photons of 64 keV energy. The numerical modeling for the expected X-ray pulse shape was performed with GENESIS, which predicts X-ray pulse durations in the few-attosecond range. Possible applications for nonlinear electromagnetic effects from these X-ray pulses are briefly discussed.« less

Creation of X-Ray Transparency of Matter by Stimulated Elastic Forward Scattering.

PubMed

Stöhr, J; Scherz, A

2015-09-04

X-ray absorption by matter has long been described by the famous Beer-Lambert law. Here, we show how this fundamental law needs to be modified for high-intensity coherent x-ray pulses, now available at x-ray free electron lasers, due to the onset of stimulated elastic forward scattering. We present an analytical expression for the modified polarization-dependent Beer-Lambert law for the case of resonant core-to-valence electronic transitions and incident transform limited x-ray pulses. Upon transmission through a solid, the resonant absorption and dichroic contrasts are found to vanish with increasing x-ray intensity, with the stimulation threshold lowered by orders of magnitude through a resonant superradiantlike effect. Our results have broad implications for the study of matter with x-ray lasers.

Creation of X-Ray Transparency of Matter by Stimulated Elastic Forward Scattering

NASA Astrophysics Data System (ADS)

Stöhr, J.; Scherz, A.

2015-09-01

X-ray absorption by matter has long been described by the famous Beer-Lambert law. Here, we show how this fundamental law needs to be modified for high-intensity coherent x-ray pulses, now available at x-ray free electron lasers, due to the onset of stimulated elastic forward scattering. We present an analytical expression for the modified polarization-dependent Beer-Lambert law for the case of resonant core-to-valence electronic transitions and incident transform limited x-ray pulses. Upon transmission through a solid, the resonant absorption and dichroic contrasts are found to vanish with increasing x-ray intensity, with the stimulation threshold lowered by orders of magnitude through a resonant superradiantlike effect. Our results have broad implications for the study of matter with x-ray lasers.

Numerical optimization of a picosecond pulse driven Ni-like Nb x-ray laser at 20.3 nm

NASA Astrophysics Data System (ADS)

Lu, X.; Zhong, J. Y.; Li, Y. J.; Zhang, J.

2003-07-01

Detailed simulations of a Ni-like Nb x-ray laser pumped by a nanosecond prepulse followed by a picosecond main pulse are presented. The atomic physics data are obtained using the Cowan code [R. D. Cowan, The Theory of Atomic Structure and Spectra (University of California Press, Berkeley, CA, 1981)]. The optimization calculations are performed in terms of the intensity of prepulse and the time delay between the prepulse and the main pulse. A high gain over 150 cm-1 is obtained for the optimized drive pulse configuration. The ray-tracing calculations suggest that the total pump energy for a saturated x-ray laser can be reduced to less than 1 J.

Time-resolved single-shot terahertz time-domain spectroscopy for ultrafast irreversible processes

NASA Astrophysics Data System (ADS)

Zhai, Zhao-Hui; Zhong, Sen-Cheng; Li, Jun; Zhu, Li-Guo; Meng, Kun; Li, Jiang; Liu, Qiao; Peng, Qi-Xian; Li, Ze-Ren; Zhao, Jian-Heng

2016-09-01

Pulsed terahertz spectroscopy is suitable for spectroscopic diagnostics of ultrafast events. However, the study of irreversible or single shot ultrafast events requires ability to record transient properties at multiple time delays, i.e., time resolved at single shot level, which is not available currently. Here by angular multiplexing use of femtosecond laser pulses, we developed and demonstrated a time resolved, transient terahertz time domain spectroscopy technique, where burst mode THz pulses were generated and then detected in a single shot measurement manner. The burst mode THz pulses contain 2 sub-THz pulses, and the time gap between them is adjustable up to 1 ns with picosecond accuracy, thus it can be used to probe the single shot event at two different time delays. The system can detect the sub-THz pulses at 0.1 THz-2.5 THz range with signal to noise ratio (SNR) of ˜400 and spectrum resolution of 0.05 THz. System design was described here, and optimizations of single shot measurement of THz pulses were discussed in detail. Methods to improve SNR were also discussed in detail. A system application was demonstrated where pulsed THz signals at different time delays of the ultrafast process were successfully acquired within single shot measurement. This time resolved transient terahertz time domain spectroscopy technique provides a new diagnostic tool for irreversible or single shot ultrafast events where dynamic information can be extracted at terahertz range within one-shot experiment.

Time-resolved single-shot terahertz time-domain spectroscopy for ultrafast irreversible processes.

PubMed

Zhai, Zhao-Hui; Zhong, Sen-Cheng; Li, Jun; Zhu, Li-Guo; Meng, Kun; Li, Jiang; Liu, Qiao; Peng, Qi-Xian; Li, Ze-Ren; Zhao, Jian-Heng

2016-09-01

Pulsed terahertz spectroscopy is suitable for spectroscopic diagnostics of ultrafast events. However, the study of irreversible or single shot ultrafast events requires ability to record transient properties at multiple time delays, i.e., time resolved at single shot level, which is not available currently. Here by angular multiplexing use of femtosecond laser pulses, we developed and demonstrated a time resolved, transient terahertz time domain spectroscopy technique, where burst mode THz pulses were generated and then detected in a single shot measurement manner. The burst mode THz pulses contain 2 sub-THz pulses, and the time gap between them is adjustable up to 1 ns with picosecond accuracy, thus it can be used to probe the single shot event at two different time delays. The system can detect the sub-THz pulses at 0.1 THz-2.5 THz range with signal to noise ratio (SNR) of ∼400 and spectrum resolution of 0.05 THz. System design was described here, and optimizations of single shot measurement of THz pulses were discussed in detail. Methods to improve SNR were also discussed in detail. A system application was demonstrated where pulsed THz signals at different time delays of the ultrafast process were successfully acquired within single shot measurement. This time resolved transient terahertz time domain spectroscopy technique provides a new diagnostic tool for irreversible or single shot ultrafast events where dynamic information can be extracted at terahertz range within one-shot experiment.

Pulse-to-pulse variations in accreting X-ray pulsars

NASA Astrophysics Data System (ADS)

Kretschmar, Peter; Marcu, Diana; Kühnel, Matthias; Klochkov, Dmitry; Pottschmidt, Katja; Staubert, Rüdiger; Wilson-Hodge, Colleen A.; Jenke, Peter A.; Caballero, Isabel; Fürst, Felix

2014-01-01

In most accreting X-ray pulsars, the periodic signal is very clear and easily shows up as soon as data covering sufficient pulse periods (a few ten) are available. The mean pulse profile is often quite typical for a given source and with minor variations repeated and recognisable across observations done years or even decades apart. At the time scale of individual pulses, significant pulse-to-pulse variations are commonly observed. While at low energies some of these variations might be explained by absorption, in the hard X-rays they will reflect changes in the accretion and subsequent emission. The amount of these variations appears to be quite different between sources and contains information about the surrounding material as well ass possibly interactions at the magnetosphere. We investigate such variations for a sample of well-known sources.

High flux femtosecond x-ray emission from the electron-hose instability in laser wakefield accelerators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dong, C. F.; Zhao, T. Z.; Behm, K.

Here, bright and ultrashort duration x-ray pulses can be produced by through betatron oscillations of electrons during laser wakefield acceleration (LWFA). Our experimental measurements using the Hercules laser system demonstrate a dramatic increase in x-ray flux for interaction distances beyond the depletion/dephasing lengths, where the initial electron bunch injected into the first wake bucket catches up with the laser pulse front and the laser pulse depletes. A transition from an LWFA regime to a beam-driven plasma wakefield acceleration regime consequently occurs. The drive electron bunch is susceptible to the electron-hose instability and rapidly develops large amplitude oscillations in its tail,more » which leads to greatly enhanced x-ray radiation emission. We measure the x-ray flux as a function of acceleration length using a variable length gas cell. 3D particle-in-cell simulations using a Monte Carlo synchrotron x-ray emission algorithm elucidate the time-dependent variations in the radiation emission processes.« less

Intense Non-Linear Soft X-Ray Emission from a Hydride Target during Pulsed D Bombardment

NASA Astrophysics Data System (ADS)

Miley, George H.; Yang, Yang; Lipson, Andrei; Haque, Munima; Percel, Ian; Romer, Michael

Radiation emission from low-energy nuclear radiation (LENR) electrodes (both charged-particle and X-rays) represents an important feature of LENR in general. Here, calibration, measurement techniques, and soft X-ray emission results from deuterium bombardment of a Pd target (cathode) placed in a pulsed deuterium glow discharge (PGD) are described. An X-ray intensity of 13.4 mW/cm2 and a dose of 3.3 μJ/cm2 were calculated over a 0.5 ms pulse time from AXUV photodiode radiation detector measurements. A most striking feature is that X-ray energies >600 V are observed with a discharge voltage only about half of that value. To further investigate this phenomenon, emission during room temperature D-desorption from electrolytically loaded Pd:Dx cathodes was also studied. The X-ray emission energy observed was quite similar to the PGD case. However, the intensity in this case was almost 13 orders of magnitude lower due to the much lower deuterium fluxes involved.

High flux femtosecond x-ray emission from the electron-hose instability in laser wakefield accelerators

NASA Astrophysics Data System (ADS)

Dong, C. F.; Zhao, T. Z.; Behm, K.; Cummings, P. G.; Nees, J.; Maksimchuk, A.; Yanovsky, V.; Krushelnick, K.; Thomas, A. G. R.

2018-04-01

Bright and ultrashort duration x-ray pulses can be produced by through betatron oscillations of electrons during laser wakefield acceleration (LWFA). Our experimental measurements using the Hercules laser system demonstrate a dramatic increase in x-ray flux for interaction distances beyond the depletion/dephasing lengths, where the initial electron bunch injected into the first wake bucket catches up with the laser pulse front and the laser pulse depletes. A transition from an LWFA regime to a beam-driven plasma wakefield acceleration regime consequently occurs. The drive electron bunch is susceptible to the electron-hose instability and rapidly develops large amplitude oscillations in its tail, which leads to greatly enhanced x-ray radiation emission. We measure the x-ray flux as a function of acceleration length using a variable length gas cell. 3D particle-in-cell simulations using a Monte Carlo synchrotron x-ray emission algorithm elucidate the time-dependent variations in the radiation emission processes.

The use of short and wide x-ray pulses for time-of-flight x-ray Compton Scatter Imaging in cargo security

NASA Astrophysics Data System (ADS)

Calvert, Nick; Betcke, Marta M.; Cresswell, John R.; Deacon, Alick N.; Gleeson, Anthony J.; Judson, Daniel S.; Mason, Peter; McIntosh, Peter A.; Morton, Edward J.; Nolan, Paul J.; Ollier, James; Procter, Mark G.; Speller, Robert D.

2015-05-01

Using a short pulse width x-ray source and measuring the time-of-flight of photons that scatter from an object under inspection allows for the point of interaction to be determined, and a profile of the object to be sampled along the path of the beam. A three dimensional image can be formed by interrogating the entire object. Using high energy x rays enables the inspection of cargo containers with steel walls, in the search for concealed items. A longer pulse width x-ray source can also be used with deconvolution techniques to determine the points of interaction. We present time-of-flight results from both short (picosecond) width and long (hundreds of nanoseconds) width x-ray sources, and show that the position of scatter can be localised with a resolution of 2 ns, equivalent to 30 cm, for a 3 cm thick plastic test object.

High flux femtosecond x-ray emission from the electron-hose instability in laser wakefield accelerators

DOE PAGES

Dong, C. F.; Zhao, T. Z.; Behm, K.; ...

2018-04-24

Here, bright and ultrashort duration x-ray pulses can be produced by through betatron oscillations of electrons during laser wakefield acceleration (LWFA). Our experimental measurements using the Hercules laser system demonstrate a dramatic increase in x-ray flux for interaction distances beyond the depletion/dephasing lengths, where the initial electron bunch injected into the first wake bucket catches up with the laser pulse front and the laser pulse depletes. A transition from an LWFA regime to a beam-driven plasma wakefield acceleration regime consequently occurs. The drive electron bunch is susceptible to the electron-hose instability and rapidly develops large amplitude oscillations in its tail,more » which leads to greatly enhanced x-ray radiation emission. We measure the x-ray flux as a function of acceleration length using a variable length gas cell. 3D particle-in-cell simulations using a Monte Carlo synchrotron x-ray emission algorithm elucidate the time-dependent variations in the radiation emission processes.« less

Start-to-end simulation of single-particle imaging using ultra-short pulses at the European X-ray Free-Electron Laser

DOE PAGES

Fortmann-Grote, Carsten; Buzmakov, Alexey; Jurek, Zoltan; ...

2017-09-01

Single-particle imaging with X-ray free-electron lasers (XFELs) has the potential to provide structural information at atomic resolution for non-crystalline biomolecules. This potential exists because ultra-short intense pulses can produce interpretable diffraction data notwithstanding radiation damage. This paper explores the impact of pulse duration on the interpretability of diffraction data using comprehensive and realistic simulations of an imaging experiment at the European X-ray Free-Electron Laser. In conclusion, it is found that the optimal pulse duration for molecules with a few thousand atoms at 5 keV lies between 3 and 9 fs.

Start-to-end simulation of single-particle imaging using ultra-short pulses at the European X-ray Free-Electron Laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fortmann-Grote, Carsten; Buzmakov, Alexey; Jurek, Zoltan

Single-particle imaging with X-ray free-electron lasers (XFELs) has the potential to provide structural information at atomic resolution for non-crystalline biomolecules. This potential exists because ultra-short intense pulses can produce interpretable diffraction data notwithstanding radiation damage. This paper explores the impact of pulse duration on the interpretability of diffraction data using comprehensive and realistic simulations of an imaging experiment at the European X-ray Free-Electron Laser. In conclusion, it is found that the optimal pulse duration for molecules with a few thousand atoms at 5 keV lies between 3 and 9 fs.

Status of the laboratory infrastructure for detector calibration and characterization at the European XFEL

NASA Astrophysics Data System (ADS)

Raab, N.; Ballak, K.-E.; Dietze, T.; Ekmedzič, M.; Hauf, S.; Januschek, F.; Kaukher, A.; Kuster, M.; Lang, P. M.; Münnich, A.; Schmitt, R.; Sztuk-Dambietz, J.; Turcato, M.

2016-12-01

The European X-ray Free Electron Laser (XFEL.EU) will provide unprecedented peak brilliance and ultra-short and spatially coherent X-ray pulses in an energy range of 0.25 to 25 keV . The pulse timing structure is unique with a burst of 2700 pulses of 100 fs length at a temporal distance of 220 ns followed by a 99.4 ms gap. To make optimal use of this timing structure and energy range a great variety of detectors are being developed for use at XFEL.EU, including 2D X-ray imaging cameras that are able to detect images at a rate of 4.5 MHz, provide dynamic ranges up to 105 photons per pulse per pixel under different operating conditions and covering a large range of angular resolution \\cite{requirements,Markus}. In order to characterize, commission and calibrate this variety of detectors and for testing of detector prototypes the XFEL.EU detector group is building up an X-ray test laboratory that allows testing of detectors with X-ray photons under conditions that are as similar to the future beam line conditions at the XFEL.EU as is possible with laboratory sources [1]. A total of four test environments provide the infrastructure for detector tests and calibration: two portable setups that utilize low power X-ray sources and radioactive isotopes, a test environment where a commercial high power X-ray generator is in use, and a pulsed X-ray/electron source which will provide pulses as short as 25 ns in XFEL.EU burst mode combined with target anodes of different materials. The status of the test environments, three of which are already in use while one is in commissioning phase, will be presented as well as first results from performance tests and characterization of the sources.

X-ray pulsars in nearby irregular galaxies

NASA Astrophysics Data System (ADS)

Yang, Jun

2018-01-01

The Small Magellanic Cloud (SMC), Large Magellanic Cloud (LMC) and Irregular Galaxy IC 10 are valuable laboratories to study the physical, temporal and statistical properties of the X-ray pulsar population with multi-satellite observations, in order to probe fundamental physics. The known distance of these galaxies can help us easily categorize the luminosity of the pulsars and their age difference can be helpful for for studying the origin and evolution of compact objects. Therefore, a complete archive of 116 XMM-Newton PN, 151 Chandra (Advanced CCD Imaging Spectrometer) ACIS, and 952 RXTE PCA observations for the pulsars in the Small Magellanic Cloud (SMC) were collected and analyzed, along with 42 XMM-Newton and 30 Chandra observations for the Large Magellanic Cloud, spanning 1997-2014. From a sample of 67 SMC pulsars we generate a suite of products for each pulsar detection: spin period, flux, event list, high time-resolution light-curve, pulse-profile, periodogram, and X-ray spectrum. Combining all three satellites, I generated complete histories of the spin periods, pulse amplitudes, pulsed fractions and X-ray luminosities. Many of the pulsars show variations in pulse period due to the combination of orbital motion and accretion torques. Long-term spin-up/down trends are seen in 28/25 pulsars respectively, pointing to sustained transfer of mass and angular momentum to the neutron star on decadal timescales. The distributions of pulse detection and flux as functions of spin period provide interesting findings: mapping boundaries of accretion-driven X-ray luminosity, and showing that fast pulsars (P<10 s) are rarely detected, which yet are more prone to giant outbursts. In parallel we compare the observed pulse profiles to our general relativity (GR) model of X-ray emission in order to constrain the physical parameters of the pulsars.In addition, we conduct a search for optical counterparts to X-ray sources in the local dwarf galaxy IC 10 to form a comparison sample for Magellanic Cloud X-ray pulsars.

The effect of Se/Te ratio on transient absorption behavior and nonlinear absorption properties of CuIn0.7Ga0.3(Se1-xTex)2 (0 ≤ x ≤ 1) amorphous semiconductor thin films

NASA Astrophysics Data System (ADS)

Karatay, Ahmet; Küçüköz, Betül; Çankaya, Güven; Ates, Aytunc; Elmali, Ayhan

2017-11-01

The characterization of the CuInSe2 (CIS), CuInGaSe (CIGS) and CuGaSe2 (CGS) based semiconductor thin films are very important role for solar cell and various nonlinear optical applications. In this paper, the amorphous CuIn0.7Ga0.3(Se1-xTex)2 semiconductor thin films (0 ≤ x ≤ 1) were prepared with 60 nm thicknesses by using vacuum evaporation technique. The nonlinear absorption properties and ultrafast transient characteristics were investigated by using open aperture Z-scan and ultrafast pump-probe techniques. The energy bandgap values were calculated by using linear absorption spectra. The bandgap values are found to be varying from 0.67 eV to 1.25 eV for CuIn0.7Ga0.3Te2, CuIn0.7Ga0.3Se1.6Te0.4, CuIn0.7Ga0.3Se0.4Te1.6 and CuIn0.7Ga0.3Se2 thin films. The energy bandgap values decrease with increasing telluride (Te) doping ratio in mixed CuIn0.7Ga0.3(Se1-xTex)2 films. This affects nonlinear characteristics and ultrafast dynamics of amorphous thin films. Ultrafast pump-probe experiments indicated that decreasing of bandgap values with increasing the Te amount switches from the excited state absorption signals to ultrafast bleaching signals. Open aperture Z-scan experiments show that nonlinear absorption properties enhance with decreasing bandgaps values for 65 ps pulse duration at 1064 nm. Highest nonlinear absorption coefficient was found for CuIn0.7Ga0.3Te2 thin film due to having the smallest energy bandgap.

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

PubMed

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

2018-01-01

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

Resonantly Enhanced Betatron Hard X-rays from Ionization Injected Electrons in a Laser Plasma Accelerator

PubMed Central

Huang, K.; Li, Y. F.; Li, D. Z.; Chen, L. M.; Tao, M. Z.; Ma, Y.; Zhao, J. R.; Li, M. H.; Chen, M.; Mirzaie, M.; Hafz, N.; Sokollik, T.; Sheng, Z. M.; Zhang, J.

2016-01-01

Ultrafast betatron x-ray emission from electron oscillations in laser wakefield acceleration (LWFA) has been widely investigated as a promising source. Betatron x-rays are usually produced via self-injected electron beams, which are not controllable and are not optimized for x-ray yields. Here, we present a new method for bright hard x-ray emission via ionization injection from the K-shell electrons of nitrogen into the accelerating bucket. A total photon yield of 8 × 108/shot and 108 photons with energy greater than 110 keV is obtained. The yield is 10 times higher than that achieved with self-injection mode in helium under similar laser parameters. The simulation suggests that ionization-injected electrons are quickly accelerated to the driving laser region and are subsequently driven into betatron resonance. The present scheme enables the single-stage betatron radiation from LWFA to be extended to bright γ-ray radiation, which is beyond the capability of 3rd generation synchrotrons. PMID:27273170

Strong-field physics with mid-infrared lasers

NASA Astrophysics Data System (ADS)

Pogorelsky, I. V.

2002-04-01

Mid-infrared gas laser technology promises to become a unique tool for research in strong-field relativistic physics. The degree to which physics is relativistic is determined by a ponderomotive potential. At a given intensity, a 10 μm wavelength CO2 laser reaches a 100 times higher ponderomotive potential than the 1 μm wavelength solid state lasers. Thus, we can expect a proportional increase in the throughput of such processes as laser acceleration, x-ray production, etc. These arguments have been confirmed in proof-of-principle Thomson scattering and laser acceleration experiments conducted at BNL and UCLA where the first terawatt-class CO2 lasers are in operation. Further more, proposals for the 100 TW, 100 fs CO2 lasers based on frequency-chirped pulse amplification have been conceived. Such lasers can produce physical effects equivalent to a hypothetical multi-petawatt solid state laser. Ultra-fast mid-infrared lasers will open new routes to the next generation electron and ion accelerators, ultra-bright monochromatic femtosecond x-ray and gamma sources, allow to attempt the study of Hawking-Unruh radiation, and explore relativistic aspects of laser-matter interactions. We review the present status and experiments with terawatt-class CO2 lasers, sub-petawatt projects, and prospective applications in strong-field science. .

STRONG FIELD PHYSICS WITH MID INFRARED LASERS.

DOE Office of Scientific and Technical Information (OSTI.GOV)

POGORELSKY,I.V.

2001-08-27

Mid-infrared gas laser technology promises to become a unique tool for research in strong-field relativistic physics. The degree to which physics is relativistic is determined by a ponderomotive potential. At a given intensity, a 10 {micro}m wavelength CO{sub 2} laser reaches a 100 times higher ponderomotive potential than the 1 {micro}m wavelength solid state lasers. Thus, we can expect a proportional increase in the throughput of such processes as laser acceleration, x-ray production, etc. These arguments have been confirmed in proof-of-principle Thomson scattering and laser acceleration experiments conducted at BNL and UCLA where the first terawatt-class CO{sub 2} lasers aremore » in operation. Further more, proposals for the 100 TW, 100 fs CO{sub 2} lasers based on frequency-chirped pulse amplification have been conceived. Such lasers can produce physical effects equivalent to a hypothetical multi-petawatt solid state laser. Ultra-fast mid-infrared lasers will open new routes to the next generation electron and ion accelerators, ultra-bright monochromatic femtosecond x-ray and gamma sources, allow to attempt the study of Hawking-Unruh radiation, and explore relativistic aspects of laser-matter interactions. We review the present status and experiments with terawatt-class CO{sub 2} lasers, sub-petawatt projects, and prospective applications in strong-field science.« less

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

PubMed

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; Ropers, Claus

2017-05-01

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 9Å focused beam diameter, 200fs pulse duration and 0.6eV 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. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

Optical control of hard X-ray polarization by electron injection in a laser wakefield accelerator

PubMed Central

Schnell, Michael; Sävert, Alexander; Uschmann, Ingo; Reuter, Maria; Nicolai, Maria; Kämpfer, Tino; Landgraf, Björn; Jäckel, Oliver; Jansen, Oliver; Pukhov, Alexander; Kaluza, Malte Christoph; Spielmann, Christian

2013-01-01

Laser-plasma particle accelerators could provide more compact sources of high-energy radiation than conventional accelerators. Moreover, because they deliver radiation in femtosecond pulses, they could improve the time resolution of X-ray absorption techniques. Here we show that we can measure and control the polarization of ultra-short, broad-band keV photon pulses emitted from a laser-plasma-based betatron source. The electron trajectories and hence the polarization of the emitted X-rays are experimentally controlled by the pulse-front tilt of the driving laser pulses. Particle-in-cell simulations show that an asymmetric plasma wave can be driven by a tilted pulse front and a non-symmetric intensity distribution of the focal spot. Both lead to a notable off-axis electron injection followed by collective electron–betatron oscillations. We expect that our method for an all-optical steering is not only useful for plasma-based X-ray sources but also has significance for future laser-based particle accelerators. PMID:24026068

PF-AR NW14, a new time-resolved diffraction/scattering beamline

NASA Astrophysics Data System (ADS)

Nozawa, Shunsuke; Adachi, Shin-ichi; Tazaki, Ryoko; Takahashi, Jun-ichi; Itatani, Jiro; Daimon, Masahiro; Mori, Takeharu; Sawa, Hiroshi; Kawata, Hiroshi; Koshihara, Shin-ya

2005-01-01

NW14 is a new insertion device beamline at the Photon Factory Advanced Ring (PF-AR), which is a unique ring with full-time single-bunched operation, aiming for timeresolved x-ray diffraction/scattering and XAFS experiments. The primary scientific goal of this beamline is to observe the ultrafast dynamics of condensed matter systems such as organic and inorganic crystals, biological systems and liquids triggered by optical pulses. With the large photon fluxes derived from the undulator, it should become possible to take a snapshoot an atomic-scale image of the electron density distribution. By combining a series of images it is possible to produce a movie of the photo-induced dynamics with 50-ps resolution. The construction of the beamline is being funded by the ERATO Koshihara Non-equilibrium Dynamics Project of the Japan Science and Technology Agency (JST), and the beamline will be operational from autumn 2005.

Anomalous behavior of the homogeneous ice nucleation rate in “No-Man’s Land”

DOE PAGES

Laksmono, Hartawan; McQueen, Trevor A.; Sellberg, Jonas A.; ...

2015-07-02

We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit T H by cooling micrometer-sized droplets (microdroplets) evaporatively at 10³-10⁴ K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water's diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at <227 K, but vitrify at cooling rates of 10⁶–10⁷more » K/s. We also hypothesize that the slower increase in the nucleation rate is connected with the proposed "fragile-to-strong" transition anomaly in water.« less

Emerging opportunities in structural biology with X-ray free-electron lasers

PubMed Central

Schlichting, Ilme; Miao, Jianwei

2012-01-01

X-ray free-electron lasers (X-FELs) produce X-ray pulses with extremely brilliant peak intensity and ultrashort pulse duration. It has been proposed that radiation damage can be “outrun” by using an ultra intense and short X-FEL pulse that passes a biological sample before the onset of significant radiation damage. The concept of “diffraction-before-destruction” has been demonstrated recently at the Linac Coherent Light Source, the first operational hard X-ray FEL, for protein nanocrystals and giant virus particles. The continuous diffraction patterns from single particles allow solving the classical “phase problem” by the oversampling method with iterative algorithms. If enough data are collected from many identical copies of a (biological) particle, its three-dimensional structure can be reconstructed. We review the current status and future prospects of serial femtosecond crystallography (SFX) and single-particle coherent diffraction imaging (CDI) with X-FELs. PMID:22922042

Pulse X-ray device for stereo imaging and few-projection tomography of explosive and fast processes

NASA Astrophysics Data System (ADS)

Palchikov, E. I.; Dolgikh, A. V.; Klypin, V. V.; Krasnikov, I. Y.; Ryabchun, A. M.

2017-10-01

This paper describes the operation principles and design features of the device for single pulse X-raying of explosive and high-speed processes, developed on the basis of a Tesla transformer with lumped secondary capacitor bank. The circuit with the lumped capacitor bank allows transferring a greater amount of energy to the discharge circuit as compared with the Marks-surge generator for more effective operation with remote X-ray tubes connected by coaxial cables. The device equipped with multiple X-ray tubes provides simultaneous X-raying of extended or spaced objects, stereo imaging, or few-projection tomography.

Atomic and molecular dynamics triggered by ultrashort light pulses on the atto- to picosecond time scale

NASA Astrophysics Data System (ADS)

Pabst, Stefan

2013-04-01

Time-resolved investigations of ultrafast electronic and molecular dynamics were not possible until recently. The typical time scale of these processes is in the picosecond to attosecond realm. The tremendous technological progress in recent years made it possible to generate ultrashort pulses, which can be used to trigger, to watch, and to control atomic and molecular motion. This tutorial focuses on experimental and theoretical advances which are used to study the dynamics of electrons and molecules in the presence of ultrashort pulses. In the first part, the rotational dynamics of molecules, which happens on picosecond and femtosecond time scales, is reviewed. Well-aligned molecules are particularly suitable for angle-dependent investigations like x-ray diffraction or strong-field ionization experiments. In the second part, the ionization dynamics of atoms is studied. The characteristic time scale lies, here, in the attosecond to few-femtosecond regime. Although a one-particle picture has been successfully applied to many processes, many-body effects do constantly occur. After a broad overview of the main mechanisms and the most common tools in attosecond physics, examples of many-body dynamics in the attosecond world (e.g., in high-harmonic generation and attosecond transient absorption spectroscopy) are discussed.

Ionization of Xenon to the Nickel-Like Stage and Beyond in Micro-Capillary Plasma Columns Heated by Ultrafast Current Pulses

NASA Astrophysics Data System (ADS)

Avaria, G.; Grisham, M.; Li, J.; Tomasel, F. G.; Shlyapstsev, V. N.; Busquet, M.; Woolston, M.; Rocca, J. J.

Homogeneous plasma columns with ionization levels typical of MA discharges were created by rapidly heating gas-filled 520 µm diameter channels with ns rise-time current pulses of unusually low amplitude, 40 kA. These conditions allow the generation of high aspect ratio (eg. > 300:1) plasma columns with very high degrees of ionization (e.g. Ni-like Xenon) of interest for soft x-ray lasers below λ = 10 nm. Spectra and simulations of plasmas generated in 520 µm diameter alumina capillaries driven by 35-40 kA current pulses with 4 ns rise time were obtained for discharges in Xenon and Neon discharges. The first shows the presence of lines corresponding to ionization stages up to Fe-like Xe. The latter show that Al impurities from the walls are ionized to the H-like and He-like stages. He-like Al spectra containing the resonance line significantly broaden by opacity, the intercombination line, and Li-like satellites are analyzed. For Xenon discharges, the spectral lines from the Ni-like transitions the 3d94d (3/2, 3/2)J = 0 to the 3d94p(5/2, 3/2)J = 1 and to 3d94p(3/2, 1/2)J = 1 are observed.

Tuning ultrafast electron injection dynamics at organic-graphene/metal interfaces.

PubMed

Ravikumar, Abhilash; Kladnik, Gregor; Müller, Moritz; Cossaro, Albano; Bavdek, Gregor; Patera, Laerte L; Sánchez-Portal, Daniel; Venkataraman, Latha; Morgante, Alberto; Brivio, Gian Paolo; Cvetko, Dean; Fratesi, Guido

2018-05-03

We compare the ultrafast charge transfer dynamics of molecules on epitaxial graphene and bilayer graphene grown on Ni(111) interfaces through first principles calculations and X-ray resonant photoemission spectroscopy. We use 4,4'-bipyridine as a prototypical molecule for these explorations as the energy level alignment of core-excited molecular orbitals allows ultrafast injection of electrons from a substrate to a molecule on a femtosecond timescale. We show that the ultrafast injection of electrons from the substrate to the molecule is ∼4 times slower on weakly coupled bilayer graphene than on epitaxial graphene. Through our experiments and calculations, we can attribute this to a difference in the density of states close to the Fermi level between graphene and bilayer graphene. We therefore show how graphene coupling with the substrate influences charge transfer dynamics between organic molecules and graphene interfaces.

A Deep Pulse Search in 11 Low Mass X-Ray Binaries

NASA Astrophysics Data System (ADS)

Patruno, A.; Wette, K.; Messenger, C.

2018-06-01

We present a systematic coherent X-ray pulsation search in 11 low mass X-ray binaries (LMXBs). We select a relatively broad variety of LMXBs, including persistent and transient sources, spanning orbital periods between 0.3 and 17 hr. We use about 3.6 Ms of data collected by the Rossi X-Ray Timing Explorer and XMM-Newton and apply a semi-coherent search strategy to look for weak and persistent pulses in a wide spin frequency range. We find no evidence for X-ray pulsations in these systems and consequently set upper limits on the pulsed sinusoidal semi-amplitude below 1.6% for ten outbursting/persistent LMXBs and 6% for a quiescent system; the upper limits are further refined, by searching a narrower parameter space around the outliers, down to 0.14%–0.78% and 2.9%, respectively. These results suggest that weak pulsations might not form in (most) non pulsating LMXBs.

High-energy (>70 keV) x-ray conversion efficiency measurement on the ARC laser at the National Ignition Facility

NASA Astrophysics Data System (ADS)

Chen, Hui; Hermann, M. R.; Kalantar, D. H.; Martinez, D. A.; Di Nicola, P.; Tommasini, R.; Landen, O. L.; Alessi, D.; Bowers, M.; Browning, D.; Brunton, G.; Budge, T.; Crane, J.; Di Nicola, J.-M.; Döppner, T.; Dixit, S.; Erbert, G.; Fishler, B.; Halpin, J.; Hamamoto, M.; Heebner, J.; Hernandez, V. J.; Hohenberger, M.; Homoelle, D.; Honig, J.; Hsing, W.; Izumi, N.; Khan, S.; LaFortune, K.; Lawson, J.; Nagel, S. R.; Negres, R. A.; Novikova, L.; Orth, C.; Pelz, L.; Prantil, M.; Rushford, M.; Shaw, M.; Sherlock, M.; Sigurdsson, R.; Wegner, P.; Widmayer, C.; Williams, G. J.; Williams, W.; Whitman, P.; Yang, S.

2017-03-01

The Advanced Radiographic Capability (ARC) laser system at the National Ignition Facility (NIF) is designed to ultimately provide eight beamlets with a pulse duration adjustable from 1 to 30 ps, and energies up to 1.5 kJ per beamlet. Currently, four beamlets have been commissioned. In the first set of 6 commissioning target experiments, the individual beamlets were fired onto gold foil targets with energy up to 1 kJ per beamlet at 20-30 ps pulse length. The x-ray energy distribution and pulse duration were measured, yielding energy conversion efficiencies of 4-9 × 10-4 for x-rays with energies greater than 70 keV. With greater than 3 J of such x-rays, ARC provides a high-precision x-ray backlighting capability for upcoming inertial confinement fusion and high-energy-density physics experiments on NIF.

Ultrafast control and monitoring of material properties using terahertz pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bowlan, Pamela Renee

These are a set of slides on ultrafast control and monitoring of material properties using terahertz pulses. A few of the topics covered in these slides are: How fast is a femtosecond (fs), Different frequencies probe different properties of molecules or solids, What can a THz pulse do to a material, Ultrafast spectroscopy, Generating and measuring ultrashort THz pulses, Tracking ultrafast spin dynamics in antiferromagnets through spin wave resonances, Coherent two-dimensional THz spectroscopy, and Probing vibrational dynamics at a surface. Conclusions are: Coherent two-dimensional THz spectroscopy: a powerful approach for studying coherence and dynamics of low energy resonances. Applying thismore » to graphene we investigated the very strong THz light mater interaction which dominates over scattering. Useful for studying coupled excitations in multiferroics and monitoring chemical reactions. Also, THz-pump, SHG-probe spectoscopy: an ultrafast, surface sensitive probe of atomic-scale symmetry changes and nonlinear phonon dymanics. We are using this in Bi 2Se 3 to investigate the nonlinear surface phonon dynamics. This is potentially very useful for studying catalysis.« less

The Orbital Parameters and Nature of the X-ray Pulsar IGR J16393-4643 Using Pulse Timing Analysis

NASA Astrophysics Data System (ADS)

Pearlman, Aaron B.; Corbet, R. H. D.; Pottschmidt, K.; Skinner, G. K.

2011-09-01

A 3.7 day orbital period was previously suggested for the 910 s X-ray pulsar IGR J16393-4643 from a pulse timing study of widely separated X-ray observations (Thompson et al., 2006), placing the system in the supergiant wind-fed region of the Ppulse-Porb diagram. However, orbital periods of 50.2 and 8.1 days could not be excluded. Nespoli et al. (2010) refute this wind-accreting high-mass X-ray binary classification and suggest a symbiotic X-ray binary (SyXB) designation based on infrared spectroscopy of the proposed counterpart and the potential 50.2 day orbital solution. SyXBs are low-mass X-ray binaries in which a neutron star accretes from the inhomogeneous medium around an M-type giant companion. We find that two statistically independent light curves of IGR J16393-4643, from the Swift Burst Alert Telescope (15-50 keV) and the Rossi X-ray Timing Explorer (RXTE) Proportional Counter Array (PCA) Galactic bulge scans (2-10 keV), show highly significant orbital modulation near 4.24 days. Making use of this precise orbital period, we present the results from pulse arrival time analysis on IGR J16393-4643 using RXTE PCA observations. We provide significantly improved phase-connected pulse timing results using archival observations presented in Thompson et al. (2006) and additional pulse timing data not included in their study to determine the orbital parameters of the system. The derived 7.5 M⊙ mass function is inconsistent with a SyXB identification.

Ultrafast electron crystallography: Transient structures of molecules, surfaces, and phase transitions

PubMed Central

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

2004-01-01

The static structure of macromolecular assemblies can be mapped out with atomic-scale resolution by using electron diffraction and microscopy of crystals. For transient nonequilibrium structures, which are critical to the understanding of dynamics and mechanisms, both spatial and temporal resolutions are required; the shortest scales of length (0.1–1 nm) and time (10–13 to 10–12 s) represent the quantum limit, the nonstatistical regime of rates. Here, we report the development of ultrafast electron crystallography for direct determination of structures with submonolayer sensitivity. In these experiments, we use crystalline silicon as a template for different adsorbates: hydrogen, chlorine, and trifluoroiodomethane. We observe the coherent restructuring of the surface layers with subangstrom displacement of atoms after the ultrafast heat impulse. This nonequilibrium dynamics, which is monitored in steps of 2 ps (total change ≤10 ps), contrasts that of the nanometer substrate. The effect of adsorbates and the phase transition at higher fluences were also studied through the evolution of streaks of interferences, Bragg spots (and their rocking curves), and rings in the diffraction patterns. We compare these results with kinematical theory and those of x-ray diffraction developed to study bulk behaviors. The sensitivity achieved here, with the 6 orders of magnitude larger cross section than x-ray diffraction, and with the capabilities of combined spatial (≈0.01 Å) and temporal (300–600 fs) resolutions, promise diverse applications for this ultrafast electron crystallography tabletop methodology. PMID:14745037

High resolution x-ray Thomson scattering measurements from cryogenic hydrogen jets using the linac coherent light source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fletcher, L. B., E-mail: lbfletch@slac.stanford.edu; Galtier, E.; Gamboa, E. J.

2016-11-15

We present the first spectrally resolved measurements of x-rays scattered from cryogenic hydrogen jets in the single photon counting limit. The 120 Hz capabilities of the LCLS, together with a novel hydrogen jet design [J. B. Kim et al., Rev. Sci. Instrum. (these proceedings)], allow for the ability to record a near background free spectrum. Such high-dynamic-range x-ray scattering measurements enable a platform to study ultra-fast, laser-driven, heating dynamics of hydrogen plasmas. This measurement has been achieved using two highly annealed pyrolytic graphite crystal spectrometers to spectrally resolve 5.5 keV x-rays elastically and inelastically scattered from cryogenic hydrogen and focusedmore » on Cornell-SLAC pixel array detectors [S. Herrmann et al., Nucl. Instrum. Methods Phys. Res., Sect. A 718, 550 (2013)].« less

Ultra-fast LuI{sub 3}:Ce scintillators for hard x-ray imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marton, Zsolt, E-mail: zmarton@rmdinc.com; Miller, Stuart R.; Ovechkina, Elena

We have developed ultra-fast cerium-coped lutetium-iodide (LuI{sub 3}:Ce) films thermally evaporated as polycrystalline, structured scintillator using hot wall epitaxy (HWE) method. The films have shown a 13 ns decay compared to the 28 ns reported for crystals. The fast speed coupled with its high density (∼5.6 g/cm{sup 3}), high effective atomic number (59.7), and the fact that it can be vapor deposited in a columnar form makes LuI{sub 3}:Ce an attractive candidate for high frame rate, high-resolution, hard X-ray imaging. In crystal form, LuI{sub 3}:Ce has demonstrated bright (>100,000 photons/MeV) green (540 nm) emission, which is well matched to commercialmore » CCD/CMOS sensors and is critical for maintaining high signal to noise ratio in light starved applications. Here, we report on the scintillation properties of films and those for corresponding crystalline material. The vapor grown films were integrated into a high-speed CMOS imager to demonstrate high-speed radiography capability. The films were also tested at Advanced Photon Source, Argonne National Laboratory beamline 1-ID under hard X-ray irradiation. The data show a factor of four higher efficiency than the reference LuAG:Ce scintillators, high image quality, and linearity of scintillation response over a wide energy range. The films were employed to perform hard X-ray microtomography, the results of which will also be discussed.« less

X-ray lasers and methods utilizing two component driving illumination provided by optical laser means of relatively low energy and small physical size

DOEpatents

Rosen, Mordecai D.; Matthews, Dennis L.

1991-01-01

An X-ray laser (10), and related methodology, are disclosed wherein an X-ray laser target (12) is illuminated with a first pulse of optical laser radiation (14) of relatively long duration having scarcely enough energy to produce a narrow and linear cool plasma of uniform composition (38). A second, relatively short pulse of optical laser radiation (18) is uniformly swept across the length, from end to end, of the plasma (38), at about the speed of light, to consecutively illuminate continuously succeeding portions of the plasma (38) with optical laser radiation having scarcely enough energy to heat, ionize, and invert them into the continuously succeeding portions of an X-ray gain medium. This inventive double pulse technique results in a saving of more than two orders of magnitude in driving optical laser energy, when compared to the conventional single pulse approach.

The method of pulsed x-ray detection with a diode laser.

PubMed

Liu, Jun; Ouyang, Xiaoping; Zhang, Zhongbing; Sheng, Liang; Chen, Liang; Tan, Xinjian; Weng, Xiufeng

2016-12-01

A new class of pulsed X-ray detection methods by sensing carrier changes in a diode laser cavity has been presented and demonstrated. The proof-of-principle experiments on detecting pulsed X-ray temporal profile have been done through the diode laser with a multiple quantum well active layer. The result shows that our method can achieve the aim of detecting the temporal profile of a pulsed X-ray source. We predict that there is a minimum value for the pre-bias current of the diode laser by analyzing the carrier rate equation, which exists near the threshold current of the diode laser chip in experiments. This behaviour generally agrees with the characterizations of theoretical analysis. The relative sensitivity is estimated at about 3.3 × 10 -17 C ⋅ cm 2 . We have analyzed the time scale of about 10 ps response with both rate equation and Monte Carlo methods.

Software defined photon counting system for time resolved x-ray experiments.

PubMed

Acremann, Y; Chembrolu, V; Strachan, J P; Tyliszczak, T; Stöhr, J

2007-01-01

The time structure of synchrotron radiation allows time resolved experiments with sub-100 ps temporal resolution using a pump-probe approach. However, the relaxation time of the samples may require a lower repetition rate of the pump pulse compared to the full repetition rate of the x-ray pulses from the synchrotron. The use of only the x-ray pulse immediately following the pump pulse is not efficient and often requires special operation modes where only a few buckets of the storage ring are filled. We designed a novel software defined photon counting system that allows to implement a variety of pump-probe schemes at the full repetition rate. The high number of photon counters allows to detect the response of the sample at multiple time delays simultaneously, thus improving the efficiency of the experiment. The system has been successfully applied to time resolved scanning transmission x-ray microscopy. However, this technique is applicable more generally.

Magnetically Driven Accretion Disk Winds and Ultra-fast Outflows in PG 1211+143

NASA Astrophysics Data System (ADS)

Fukumura, Keigo; Tombesi, Francesco; Kazanas, Demosthenes; Shrader, Chris; Behar, Ehud; Contopoulos, Ioannis

2015-05-01

We present a study of X-ray ionization of MHD accretion-disk winds in an effort to constrain the physics underlying the highly ionized ultra-fast outflows (UFOs) inferred by X-ray absorbers often detected in various sub classes of Seyfert active galactic nuclei (AGNs). Our primary focus is to show that magnetically driven outflows are indeed physically plausible candidates for the observed outflows accounting for the AGN absorption properties of the present X-ray spectroscopic observations. Employing a stratified MHD wind launched across the entire AGN accretion disk, we calculate its X-ray ionization and the ensuing X-ray absorption-line spectra. Assuming an appropriate ionizing AGN spectrum, we apply our MHD winds to model the absorption features in an XMM-Newton/EPIC spectrum of the narrow-line Seyfert, PG 1211+143. We find, through identifying the detected features with Fe Kα transitions, that the absorber has a characteristic ionization parameter of log (ξc[erg cm s-1]) ≃ 5-6 and a column density on the order of NH ≃ 1023 cm-2 outflowing at a characteristic velocity of vc/c ≃ 0.1-0.2 (where c is the speed of light). The best-fit model favors its radial location at rc ≃ 200 Ro (Ro is the black hole’s innermost stable circular orbit), with an inner wind truncation radius at Rt ≃ 30 Ro. The overall K-shell feature in the data is suggested to be dominated by Fe xxv with very little contribution from Fe xxvi and weakly ionized iron, which is in good agreement with a series of earlier analyses of the UFOs in various AGNs, including PG 1211+143.

Generation of stable subfemtosecond hard x-ray pulses with optimized nonlinear bunch compression

DOE PAGES

Huang, Senlin; Ding, Yuantao; Huang, Zhirong; ...

2014-12-15

In this paper, we propose a simple scheme that leverages existing x-ray free-electron laser hardware to produce stable single-spike, subfemtosecond x-ray pulses. By optimizing a high-harmonic radio-frequency linearizer to achieve nonlinear compression of a low-charge (20 pC) electron beam, we obtain a sharp current profile possessing a few-femtosecond full width at half maximum temporal duration. A reverse undulator taper is applied to enable lasing only within the current spike, where longitudinal space charge forces induce an electron beam time-energy chirp. Simulations based on the Linac Coherent Light Source parameters show that stable single-spike x-ray pulses with a duration less thanmore » 200 attoseconds can be obtained.« less

Establishing nonlinearity thresholds with ultraintense X-ray pulses

NASA Astrophysics Data System (ADS)

Szlachetko, Jakub; Hoszowska, Joanna; Dousse, Jean-Claude; Nachtegaal, Maarten; Błachucki, Wojciech; Kayser, Yves; Sà, Jacinto; Messerschmidt, Marc; Boutet, Sebastien; Williams, Garth J.; David, Christian; Smolentsev, Grigory; van Bokhoven, Jeroen A.; Patterson, Bruce D.; Penfold, Thomas J.; Knopp, Gregor; Pajek, Marek; Abela, Rafael; Milne, Christopher J.

2016-09-01

X-ray techniques have evolved over decades to become highly refined tools for a broad range of investigations. Importantly, these approaches rely on X-ray measurements that depend linearly on the number of incident X-ray photons. The advent of X-ray free electron lasers (XFELs) is opening the ability to reach extremely high photon numbers within ultrashort X-ray pulse durations and is leading to a paradigm shift in our ability to explore nonlinear X-ray signals. However, the enormous increase in X-ray peak power is a double-edged sword with new and exciting methods being developed but at the same time well-established techniques proving unreliable. Consequently, accurate knowledge about the threshold for nonlinear X-ray signals is essential. Herein we report an X-ray spectroscopic study that reveals important details on the thresholds for nonlinear X-ray interactions. By varying both the incident X-ray intensity and photon energy, we establish the regimes at which the simplest nonlinear process, two-photon X-ray absorption (TPA), can be observed. From these measurements we can extract the probability of this process as a function of photon energy and confirm both the nature and sub-femtosecond lifetime of the virtual intermediate electronic state.

Generation and dose distribution measurement of flash x-ray in KALI-5000 system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Menon, Rakhee; Roy, Amitava; Mitra, S.

2008-10-15

Flash x-ray generation studies have been carried out in KALI-5000 Pulse power system. The intense relativistic electron beam has been bombarded on a tantalum target at anode to produce flash x-ray via bremsstrahlung conversion. The typical electron beam parameter was 360 kV, 18 kA, and 100 ns, with a few hundreds of A/cm{sup 2} current density. The x-ray dose has been measured with calcium sulfate:dysposium (CaSO{sub 4}:Dy) thermoluminescent dosimeter and the axial dose distribution has been characterized. It has been observed that the on axis dose falls of with distance {approx}1/x{sup n}, where n varies from 1.8 to 1.85. Amore » maximum on axis dose of 46 mrad has been measured at 1 m distance from the source. A plastic scintillator with optical fiber coupled to a photomultiplier tube has been developed to measure the x-ray pulse width. The typical x-ray pulse width varied from 50 to 80 ns.« less

Invited Article: Coherent imaging using seeded free-electron laser pulses with variable polarization: First results and research opportunities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Capotondi, F.; Pedersoli, E.; Mahne, N.

2013-05-15

FERMI-Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a 'seeded' scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline.more » The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20-32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump/FEL-probe with two color FEL pulses generated by the same electron bunch.« less

Intensity-Modulated Advanced X-ray Source (IMAXS) for Homeland Security Applications

NASA Astrophysics Data System (ADS)

Langeveld, Willem G. J.; Johnson, William A.; Owen, Roger D.; Schonberg, Russell G.

2009-03-01

X-ray cargo inspection systems for the detection and verification of threats and contraband require high x-ray energy and high x-ray intensity to penetrate dense cargo. On the other hand, low intensity is desirable to minimize the radiation footprint. A collaboration between HESCO/PTSE Inc., Schonberg Research Corporation and Rapiscan Laboratories, Inc. has been formed in order to design and build an Intensity-Modulated Advanced X-ray Source (IMAXS). Such a source would allow cargo inspection systems to achieve up to two inches greater imaging penetration capability, while retaining the same average radiation footprint as present fixed-intensity sources. Alternatively, the same penetration capability can be obtained as with conventional sources with a reduction of the average radiation footprint by about a factor of three. The key idea is to change the intensity of the source for each x-ray pulse based on the signal strengths in the inspection system detector array during the previous pulse. In this paper we describe methods to accomplish pulse-to-pulse intensity modulation in both S-band (2998 MHz) and X-band (9303 MHz) linac sources, with diode or triode (gridded) electron guns. The feasibility of these methods has been demonstrated. Additionally, we describe a study of a shielding design that would allow a 6 MV X-band source to be used in mobile applications.

A multi-MHz single-shot data acquisition scheme with high dynamic range: pump-probe X-ray experiments at synchrotrons.

PubMed

Britz, Alexander; Assefa, Tadesse A; Galler, Andreas; Gawelda, Wojciech; Diez, Michael; Zalden, Peter; Khakhulin, Dmitry; Fernandes, Bruno; Gessler, Patrick; Sotoudi Namin, Hamed; Beckmann, Andreas; Harder, Manuel; Yavaş, Hasan; Bressler, Christian

2016-11-01

The technical implementation of a multi-MHz data acquisition scheme for laser-X-ray pump-probe experiments with pulse limited temporal resolution (100 ps) is presented. Such techniques are very attractive to benefit from the high-repetition rates of X-ray pulses delivered from advanced synchrotron radiation sources. Exploiting a synchronized 3.9 MHz laser excitation source, experiments in 60-bunch mode (7.8 MHz) at beamline P01 of the PETRA III storage ring are performed. Hereby molecular systems in liquid solutions are excited by the pulsed laser source and the total X-ray fluorescence yield (TFY) from the sample is recorded using silicon avalanche photodiode detectors (APDs). The subsequent digitizer card samples the APD signal traces in 0.5 ns steps with 12-bit resolution. These traces are then processed to deliver an integrated value for each recorded single X-ray pulse intensity and sorted into bins according to whether the laser excited the sample or not. For each subgroup the recorded single-shot values are averaged over ∼10 7  pulses to deliver a mean TFY value with its standard error for each data point, e.g. at a given X-ray probe energy. The sensitivity reaches down to the shot-noise limit, and signal-to-noise ratios approaching 1000 are achievable in only a few seconds collection time per data point. The dynamic range covers 100 photons pulse -1 and is only technically limited by the utilized APD.

Ultrafast laser ablation for targeted atherosclerotic plaque removal

NASA Astrophysics Data System (ADS)

Lanvin, Thomas; Conkey, Donald B.; Descloux, Laurent; Frobert, Aurelien; Valentin, Jeremy; Goy, Jean-Jacques; Cook, Stéphane; Giraud, Marie-Noelle; Psaltis, Demetri

2015-07-01

Coronary artery disease, the main cause of heart disease, develops as immune cells and lipids accumulate into plaques within the coronary arterial wall. As a plaque grows, the tissue layer (fibrous cap) separating it from the blood flow becomes thinner and increasingly susceptible to rupturing and causing a potentially lethal thrombosis. The stabilization and/or treatment of atherosclerotic plaque is required to prevent rupturing and remains an unsolved medical problem. Here we show for the first time targeted, subsurface ablation of atherosclerotic plaque using ultrafast laser pulses. Excised atherosclerotic mouse aortas were ablated with ultrafast near-infrared (NIR) laser pulses. The physical damage was characterized with histological sections of the ablated atherosclerotic arteries from six different mice. The ultrafast ablation system was integrated with optical coherence tomography (OCT) imaging for plaque-specific targeting and monitoring of the resulting ablation volume. We find that ultrafast ablation of plaque just below the surface is possible without causing damage to the fibrous cap, which indicates the potential use of ultrafast ablation for subsurface atherosclerotic plaque removal. We further demonstrate ex vivo subsurface ablation of a plaque volume through a catheter device with the high-energy ultrafast pulse delivered via hollow-core photonic crystal fiber.

Femtosecond laser spectroscopy of the rhodopsin photochromic reaction: a concept for ultrafast optical molecular switch creation (ultrafast reversible photoreaction of rhodopsin).

PubMed

Smitienko, Olga; Nadtochenko, Victor; Feldman, Tatiana; Balatskaya, Maria; Shelaev, Ivan; Gostev, Fedor; Sarkisov, Oleg; Ostrovsky, Mikhail

2014-11-11

Ultrafast reverse photoreaction of visual pigment rhodopsin in the femtosecond time range at room temperature is demonstrated. Femtosecond two-pump probe experiments with a time resolution of 25 fs have been performed. The first рump pulse at 500 nm initiated cis-trans photoisomerization of rhodopsin chromophore, 11-cis retinal, which resulted in the formation of the primary ground-state photoproduct within a mere 200 fs. The second pump pulse at 620 nm with a varying delay of 200 to 3750 fs relative to the first рump pulse, initiated the reverse phototransition of the primary photoproduct to rhodopsin. The results of this photoconversion have been observed on the differential spectra obtained after the action of two pump pulses at a time delay of 100 ps. It was found that optical density decreased at 560 nm in the spectral region of bathorhodopsin absorption and increased at 480 nm, where rhodopsin absorbs. Rhodopsin photoswitching efficiency shows oscillations as a function of the time delay between two рump pulses. The quantum yield of reverse photoreaction initiated by the second pump pulse falls within the range 15%±1%. The molecular mechanism of the ultrafast reversible photoreaction of visual pigment rhodopsin may be used as a concept for the development of an ultrafast optical molecular switch.

Optoelectronic Picosecond Detection of Synchrotron X-rays

DOE Office of Scientific and Technical Information (OSTI.GOV)

Durbin, Stephen M.

2017-08-04

The goal of this research program was to develop a detector that would measure x-ray time profiles with picosecond resolution. This was specifically aimed for use at x-ray synchrotrons, where x-ray pulse profiles have Gaussian time spreads of 50-100 ps (FWHM), so the successful development of such a detector with picosecond resolution would permit x-ray synchrotron studies to break through the pulse width barrier. That is, synchrotron time-resolved studies are currently limited to pump-probe studies that cannot reveal dynamics faster than ~50 ps, whereas the proposed detector would push this into the physically important 1 ps domain. The results ofmore » this research effort, described in detail below, are twofold: 1) the original plan to rely on converting electronic signals from a semiconductor sensor into an optical signal proved to be insufficient for generating signals with the necessary time resolution and sensitivity to be widely applicable; and 2) an all-optical method was discovered whereby the x-rays are directly absorbed in an optoelectronic material, lithium tantalate, which can then be probed by laser pulses with the desired picosecond sensitivity for detection of synchrotron x-rays. This research program has also produced new fundamental understanding of the interaction of x-rays and optical lasers in materials that has now created a viable path for true picosecond detection of synchrotron x-rays.« less

TH-AB-209-07: High Resolution X-Ray-Induced Acoustic Computed Tomography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xiang, L; Tang, S; Ahmad, M

Purpose: X-ray radiographic absorption imaging is an invaluable tool in medical diagnostics, biology and materials science. However, the use of conventional CT is limited by two factors: the detection sensitivity to weak absorption material and the radiation dose from CT scanning. The purpose of this study is to explore X-ray induced acoustic computed tomography (XACT), a new imaging modality, which combines X-ray absorption contrast and high ultrasonic resolution to address these challenges. Methods: First, theoretical models was built to analyze the XACT sensitivity to X-ray absorption and calculate the minimal radiation dose in XACT imaging. Then, an XACT system comprisedmore » of an ultrashort X-ray pulse, a low noise ultrasound detector and a signal acquisition system was built to evaluate the X-ray induced acoustic signal generation. A piece of chicken bone and a phantom with two golden fiducial markers were exposed to 270 kVp X-ray source with 60 ns exposure time, and the X-ray induced acoustic signal was received by a 2.25MHz ultrasound transducer in 200 positions. XACT images were reconstructed by a filtered back-projection algorithm. Results: The theoretical analysis shows that X-ray induced acoustic signals have 100% relative sensitivity to X-ray absorption, but not to X-ray scattering. Applying this innovative technology to breast imaging, we can reduce radiation dose by a factor of 50 compared with newly FDA approved breast CT. The reconstructed images of chicken bone and golden fiducial marker phantom reveal that the spatial resolution of the built XACT system is 350µm. Conclusion: In XACT, the imaging sensitivity to X-ray absorption is improved and the imaging dose is dramatically reduced by using ultrashort pulsed X-ray. Taking advantage of the high ultrasonic resolution, we can also perform 3D imaging with a single X-ray pulse. This new modality has the potential to revolutionize x-ray imaging applications in medicine and biology.« less

Start-to-end simulation of single-particle imaging using ultra-short pulses at the European X-ray Free-Electron Laser

PubMed Central

Buzmakov, Alexey; Jurek, Zoltan; Loh, Ne-Te Duane; Samoylova, Liubov; Santra, Robin; Schneidmiller, Evgeny A.; Tschentscher, Thomas; Yakubov, Sergey; Yoon, Chun Hong; Yurkov, Michael V.; Ziaja-Motyka, Beata; Mancuso, Adrian P.

2017-01-01

Single-particle imaging with X-ray free-electron lasers (XFELs) has the potential to provide structural information at atomic resolution for non-crystalline biomolecules. This potential exists because ultra-short intense pulses can produce interpretable diffraction data notwithstanding radiation damage. This paper explores the impact of pulse duration on the interpretability of diffraction data using comprehensive and realistic simulations of an imaging experiment at the European X-ray Free-Electron Laser. It is found that the optimal pulse duration for molecules with a few thousand atoms at 5 keV lies between 3 and 9 fs. PMID:28989713

The period history of the X-ray pulsar in MSH 15-52

NASA Technical Reports Server (NTRS)

Weisskopf, M. C.; Elsner, R. F.; Darbo, W.; Leahy, D.; Naranan, S.; Harnden, F. R.; Seward, F. D.; Sutherland, P. G.; Grindlay, J. E.

1983-01-01

New and refined mesurements of the pulse period of the X-ray pulsar in the supernova remnant MSH 15-52 are presented. The data were obtained with the Monitor proportional Counter on board the HEAO 2 observatory. The period measurements were obtained by analyzing pulse arrival times determined by cross-correlating sample pulse profiles with a master template. The period history for the source and a representative 0.15 s X-ray light curve are shown. The X-ray measurements alone lead to a refined value of the period derivative of (1.5382 + or -0.0024) x 10 to the -12th s/s, while including the results of more recent radio observations leads to a value of (1.54029 + or -0.00095) x 10 to the -12th s/s. These results indicate a hard-point source surrounded by diffuse nebular emission.

Stimulated resonant x-ray Raman scattering with incoherent radiation

NASA Astrophysics Data System (ADS)

Weninger, Clemens; Rohringer, Nina

2013-11-01

We present a theoretical study on stimulated electronic Raman scattering in neon by resonant excitation with an x-ray free electron laser (XFEL). This study is in support of the recent experimental demonstration [C. Weninger , Phys. Rev. Lett. (to be published)] of stimulated x-ray Raman scattering. Focusing the broadband XFEL pulses into a cell of neon gas at atmospheric pressure a strong inelastic x-ray scattering signal in the forward direction was observed, as the x-ray energy was varied across the region of core-excited Rydberg states and the K edge. The broadband and intrinsically incoherent x-ray pulses from the XFEL lead to a rich, structured line shape of the scattered radiation. We present a generalized Maxwell-Liouville-von Neumann approach to self-consistently solve for the amplification of the scattered radiation along with the time evolution of the density matrix of the atomic and residual ionic system. An in-depth analysis of the evolution of the emission spectra as a function of the Raman gain is presented. Furthermore, we propose the use of statistical methods to obtain high-resolution scattering data beyond the lifetime broadening despite pumping with incoherent x-ray pulses.

Single mimivirus particles intercepted and imaged with an X-ray laser

PubMed Central

Seibert, M. Marvin; Ekeberg, Tomas; Maia, Filipe R. N. C.; Svenda, Martin; Andreasson, Jakob; Jönsson, Olof; Odić, Duško; Iwan, Bianca; Rocker, Andrea; Westphal, Daniel; Hantke, Max; DePonte, Daniel P.; Barty, Anton; Schulz, Joachim; Gumprecht, Lars; Coppola, Nicola; Aquila, Andrew; Liang, Mengning; White, Thomas A.; Martin, Andrew; Caleman, Carl; Stern, Stephan; Abergel, Chantal; Seltzer, Virginie; Claverie, Jean-Michel; Bostedt, Christoph; Bozek, John D.; Boutet, Sébastien; Miahnahri, A. Alan; Messerschmidt, Marc; Krzywinski, Jacek; Williams, Garth; Hodgson, Keith O.; Bogan, Michael J.; Hampton, Christina Y.; Sierra, Raymond G.; Starodub, Dmitri; Andersson, Inger; Bajt, Saša; Barthelmess, Miriam; Spence, John C. H.; Fromme, Petra; Weierstall, Uwe; Kirian, Richard; Hunter, Mark; Doak, R. Bruce; Marchesini, Stefano; Hau-Riege, Stefan P.; Frank, Matthias; Shoeman, Robert L.; Lomb, Lukas; Epp, Sascha W.; Hartmann, Robert; Rolles, Daniel; Rudenko, Artem; Schmidt, Carlo; Foucar, Lutz; Kimmel, Nils; Holl, Peter; Rudek, Benedikt; Erk, Benjamin; Hömke, André; Reich, Christian; Pietschner, Daniel; Weidenspointner, Georg; Strüder, Lothar; Hauser, Günter; Gorke, Hubert; Ullrich, Joachim; Schlichting, Ilme; Herrmann, Sven; Schaller, Gerhard; Schopper, Florian; Soltau, Heike; Kühnel, Kai-Uwe; Andritschke, Robert; Schröter, Claus-Dieter; Krasniqi, Faton; Bott, Mario; Schorb, Sebastian; Rupp, Daniela; Adolph, Marcus; Gorkhover, Tais; Hirsemann, Helmut; Potdevin, Guillaume; Graafsma, Heinz; Nilsson, Björn; Chapman, Henry N.; Hajdu, Janos

2014-01-01

X-ray lasers offer new capabilities in understanding the structure of biological systems, complex materials and matter under extreme conditions1–4. Very short and extremely bright, coherent X-ray pulses can be used to outrun key damage processes and obtain a single diffraction pattern from a large macromolecule, a virus or a cell before the sample explodes and turns into plasma1. The continuous diffraction pattern of non-crystalline objects permits oversampling and direct phase retrieval2. Here we show that high-quality diffraction data can be obtained with a single X-ray pulse from a non-crystalline biological sample, a single mimivirus particle, which was injected into the pulsed beam of a hard-X-ray free-electron laser, the Linac Coherent Light Source5. Calculations indicate that the energy deposited into the virus by the pulse heated the particle to over 100,000 K after the pulse had left the sample. The reconstructed exit wavefront (image) yielded 32-nm full-period resolution in a single exposure and showed no measurable damage. The reconstruction indicates inhomogeneous arrangement of dense material inside the virion. We expect that significantly higher resolutions will be achieved in such experiments with shorter and brighter photon pulses focused to a smaller area. The resolution in such experiments can be further extended for samples available in multiple identical copies. PMID:21293374

Experimental strategies for imaging bioparticles with femtosecond hard X-ray pulses

DOE Data Explorer

Daurer, Benedikt, J.

2016-12-09

Facilitating the very short and intense pulses from an X-ray laser for the purpose of imaging small bioparticles carries the potential for structure determination at atomic resolution without the need for crystallization. In this study, we explore experimental strategies for this idea based on data collected at the Linac Coherent Light Source from 40 nm virus particles injected into a hard X-ray beam.

A two-stage series diode for intense large-area moderate pulsed X rays production.

PubMed

Lai, Dingguo; Qiu, Mengtong; Xu, Qifu; Su, Zhaofeng; Li, Mo; Ren, Shuqing; Huang, Zhongliang

2017-01-01

This paper presents a method for moderate pulsed X rays produced by a series diode, which can be driven by high voltage pulse to generate intense large-area uniform sub-100-keV X rays. A two stage series diode was designed for Flash-II accelerator and experimentally investigated. A compact support system of floating converter/cathode was invented, the extra cathode is floating electrically and mechanically, by withdrawing three support pins several milliseconds before a diode electrical pulse. A double ring cathode was developed to improve the surface electric field and emission stability. The cathode radii and diode separation gap were optimized to enhance the uniformity of X rays and coincidence of the two diode voltages based on the simulation and theoretical calculation. The experimental results show that the two stage series diode can work stably under 700 kV and 300 kA, the average energy of X rays is 86 keV, and the dose is about 296 rad(Si) over 615 cm 2 area with uniformity 2:1 at 5 cm from the last converter. Compared with the single diode, the average X rays' energy reduces from 132 keV to 88 keV, and the proportion of sub-100-keV photons increases from 39% to 69%.

Ultrafast Carrier dynamics of InxGa1-xN nanostructures grown directly on Si(111)

NASA Astrophysics Data System (ADS)

Kumar, Praveen; Devi, Pooja; Rodriguez⁠, P. E. D. S.; Kumar, Manish; Shivling, V. D.; Noetzel, Richard; Sharma, Chhavi; Sinha, R. K.; Kumar, Mahesh

2018-05-01

We show a flux dependence changes in structural, optical and electronic properties of InxGa1-xN nanostructures (NSs) namely nanocolumns (NCs), nanoflakes (NFs) and nanowall network (NWN) grown directly on Si(111) surface. Field emission scanning electron microscopy (FESEM) images were recorded to see morphological changes from NFs to NCs and NWNc etc, while high-resolution X-ray diffraction (HRXRD) ω-2θ scans were used to determine In incorporation. The maximum In incorporation was observed to be 20, 33 and 38% for the sharp transition from NFs to NCs and NWNs, respectively. The charge carrier dynamics of these grown NSs were probed using Ultrafast Femtosecond Transient Absorption Spectroscopy (UFTAS) with excitation at 350 nm pump wavelength. The UFTAS studies show the comparative charge carriers dynamics of the NWS, NCs and NFs. The charge carrier studies show a higher lifetime in NWNs as compare to NCs and NFs. Further, to examine electronic structure and level of degeneracy of these NSs, core-level and valence band spectra were analyzed by X-ray photoelectron spectroscopy (XPS), which manifest the upward band bending ranging from 0.2 eV to 0.4 eV.

Microjet formation and hard x-ray production from a liquid metal target irradiated by intense femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Lar'kin, A.; Uryupina, D.; Ivanov, K.; Savel'ev, A.; Bonnet, T.; Gobet, F.; Hannachi, F.; Tarisien, M.; Versteegen, M.; Spohr, K.; Breil, J.; Chimier, B.; Dorchies, F.; Fourment, C.; Leguay, P.-M.; Tikhonchuk, V. T.

2014-09-01

By using a liquid metal as a target one may significantly enhance the yield of hard x-rays with a sequence of two intense femtosecond laser pulses. The influence of the time delay between the two pulses is studied experimentally and interpreted with numerical simulations. It was suggested that the first arbitrary weak pulse produces microjets from the target surface, while the second intense pulse provides an efficient electron heating and acceleration along the jet surface. These energetic electrons are the source of x-ray emission while striking the target surface. The microjet formation is explained based on the results given by both optical diagnostics and hydrodynamic modeling by a collision of shocks originated from two distinct zones of laser energy deposition.

Ultrafast and nonlinear surface-enhanced Raman spectroscopy.

PubMed

Gruenke, Natalie L; Cardinal, M Fernanda; McAnally, Michael O; Frontiera, Renee R; Schatz, George C; Van Duyne, Richard P

2016-04-21

Ultrafast surface-enhanced Raman spectroscopy (SERS) has the potential to study molecular dynamics near plasmonic surfaces to better understand plasmon-mediated chemical reactions such as plasmonically-enhanced photocatalytic or photovoltaic processes. This review discusses the combination of ultrafast Raman spectroscopic techniques with plasmonic substrates for high temporal resolution, high sensitivity, and high spatial resolution vibrational spectroscopy. First, we introduce background information relevant to ultrafast SERS: the mechanisms of surface enhancement in Raman scattering, the characterization of plasmonic materials with ultrafast techniques, and early complementary techniques to study molecule-plasmon interactions. We then discuss recent advances in surface-enhanced Raman spectroscopies with ultrafast pulses with a focus on the study of molecule-plasmon coupling and molecular dynamics with high sensitivity. We also highlight the challenges faced by this field by the potential damage caused by concentrated, highly energetic pulsed fields in plasmonic hotspots, and finally the potential for future ultrafast SERS studies.

Liquid sample delivery techniques for serial femtosecond crystallography

PubMed Central

Weierstall, Uwe

2014-01-01

X-ray free-electron lasers overcome the problem of radiation damage in protein crystallography and allow structure determination from micro- and nanocrystals at room temperature. To ensure that consecutive X-ray pulses do not probe previously exposed crystals, the sample needs to be replaced with the X-ray repetition rate, which ranges from 120 Hz at warm linac-based free-electron lasers to 1 MHz at superconducting linacs. Liquid injectors are therefore an essential part of a serial femtosecond crystallography experiment at an X-ray free-electron laser. Here, we compare different techniques of injecting microcrystals in solution into the pulsed X-ray beam in vacuum. Sample waste due to mismatch of the liquid flow rate to the X-ray repetition rate can be addressed through various techniques. PMID:24914163

X-Ray Detector for 1 to 30 keV

NASA Technical Reports Server (NTRS)

Alcorn, G.; Jackson, J., Jr; Grant, P.; Marshall, F.

1983-01-01

Array of silicon X-ray detecting diodes measures photon energy and provides image of X-ray pattern. Regardless of thickness of new X-ray detector, depletion region extends through it. Impinging X-rays generate electrons in quantities proportional to X-ray energy. X-ray detector is mated to chargecoupled-device array for image generation and processing. Useful in industrial part inspection, pulsed-plasma research and medical application.

Diagnostics of underwater electrical wire explosion through a time- and space-resolved hard x-ray source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sheftman, D.; Shafer, D.; Efimov, S.

2012-10-15

A time- and space-resolved hard x-ray source was developed as a diagnostic tool for imaging underwater exploding wires. A {approx}4 ns width pulse of hard x-rays with energies of up to 100 keV was obtained from the discharge in a vacuum diode consisting of point-shaped tungsten electrodes. To improve contrast and image quality, an external pulsed magnetic field produced by Helmholtz coils was used. High resolution x-ray images of an underwater exploding wire were obtained using a sensitive x-ray CCD detector, and were compared to optical fast framing images. Future developments and application of this diagnostic technique are discussed.

Diagnostics of underwater electrical wire explosion through a time- and space-resolved hard x-ray source.

PubMed

Sheftman, D; Shafer, D; Efimov, S; Gruzinsky, K; Gleizer, S; Krasik, Ya E

2012-10-01

A time- and space-resolved hard x-ray source was developed as a diagnostic tool for imaging underwater exploding wires. A ~4 ns width pulse of hard x-rays with energies of up to 100 keV was obtained from the discharge in a vacuum diode consisting of point-shaped tungsten electrodes. To improve contrast and image quality, an external pulsed magnetic field produced by Helmholtz coils was used. High resolution x-ray images of an underwater exploding wire were obtained using a sensitive x-ray CCD detector, and were compared to optical fast framing images. Future developments and application of this diagnostic technique are discussed.

Single-electron pulses for ultrafast diffraction

PubMed Central

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

2010-01-01

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