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.

Exploring coherent electron excitation and migration dynamics by electron diffraction with ultrashort X-ray pulses.

PubMed

Yuan, Kai-Jun; Bandrauk, André D

2017-10-04

Exploring ultrafast charge migration is of great importance in biological and chemical reactions. We present a scheme to monitor attosecond charge migration in molecules by electron diffraction with spatial and temporal resolutions from ab initio numerical simulations. An ultraviolet pulse creates a coherent superposition of electronic states, after which a time-delayed attosecond X-ray pulse is used to ionize the molecule. It is found that diffraction patterns in the X-ray photoelectron spectra show an asymmetric structure, which is dependent on the time delay between the pump-probe pulses, encoding the information of molecular orbital symmetry and chemical bonding. We describe these phenomena by developing an electronic time-dependent ultrafast molecular photoionization model of a coherent superposition state. The periodical distortion of electron diffraction patterns illustrates the evolution of the electronic coherence, providing a tool for attosecond imaging of ultrafast molecular reaction processes.

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.

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).

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.

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.

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

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

Ultra-short wavelength x-ray system

DOEpatents

Umstadter, Donald [Ann Arbor, MI; He, Fei [Ann Arbor, MI; Lau, Yue-Ying [Potomac, MD

2008-01-22

A method and apparatus to generate a beam of coherent light including x-rays or XUV by colliding a high-intensity laser pulse with an electron beam that is accelerated by a synchronized laser pulse. Applications include x-ray and EUV lithography, protein structural analysis, plasma diagnostics, x-ray diffraction, crack analysis, non-destructive testing, surface science and ultrafast science.

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

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.

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

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.

Ultrafast Science Opportunities with Electron Microscopy

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

Durr, Hermann

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

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

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).

Two-colour hard X-ray free-electron laser with wide tunability.

PubMed

Hara, Toru; Inubushi, Yuichi; Katayama, Tetsuo; Sato, Takahiro; Tanaka, Hitoshi; Tanaka, Takashi; Togashi, Tadashi; Togawa, Kazuaki; Tono, Kensuke; Yabashi, Makina; Ishikawa, Tetsuya

2013-01-01

Ultrabrilliant, femtosecond X-ray pulses from X-ray free-electron lasers (XFELs) have promoted the investigation of exotic interactions between intense X-rays and matters, and the observation of minute targets with high spatio-temporal resolution. Although a single X-ray beam has been utilized for these experiments, the use of multiple beams with flexible and optimum beam parameters should drastically enhance the capability and potentiality of XFELs. Here we show a new light source of a two-colour double-pulse (TCDP) XFEL in hard X-rays using variable-gap undulators, which realizes a large and flexible wavelength separation of more than 30% with an ultraprecisely controlled time interval in the attosecond regime. Together with sub-10-fs pulse duration and multi-gigawatt peak powers, the TCDP scheme enables us to elucidate X-ray-induced ultrafast transitions of electronic states and structures, which will significantly contribute to the advancement of ultrafast chemistry, plasma and astronomical physics, and quantum X-ray optics.

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.

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.

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.”

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.

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.

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

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

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

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.

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

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.

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.

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

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

Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

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

Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan

Here, ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbitalmore » and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.« less

Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

DOE PAGES

Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan; ...

2016-10-07

Here, ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbitalmore » and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.« less

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

SLAC pulsed X-ray facility

NASA Astrophysics Data System (ADS)

Ipe, N. E.; McCall, R. C.; Baker, E. D.

1986-05-01

The Stanford Linear Accelerator Center (SLAC) operates a high energy (up to 33 GeV) linear accelerator delivering pulses up to a few microseconds wide. The pulsed nature of the electron beam creates problems in the detection and measurement of radiation both from the accelerator beam and the klystrons that provide the RF power for the accelerator. Hence, a pulsed X-ray facility has been built at SLAC mainly for the purpose of testing the response of different radiation detection instruments to pulsed radiation fields. The X-ray tube consists of an electron gun with a control grid. This provides a stream of pulsed electrons that can be accelerated towards a confined target-window. The window is made up of aluminum 0.051 cm (20 mils) thick, plated on the vacuum side with a layer of gold 0.0006 cm (1/4 mil) thick. The frequency of electron pulses can be varied by an internal pulser from 60 to 360 pulses per second with pulse widths of 360 ns to 5 ms. The pulse amplitude can be varied over a wide range of currents. An external pulser can be used to obtain other frequencies or special pulse shapes. The voltage across the gun can be varied from 0 to 100 kV. The major part of the X-ray tube is enclosed in a large walk-in-cabinet made of 1.9 cm (3/4 in) plywood and lined with 0.32 cm (1/8 in) lead to make a very versatile facility.

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

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

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 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

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.

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.

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.

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.

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.

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 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.

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.

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.

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

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.

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.

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.

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 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.

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.

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.

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.

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

Angular-split/temporal-delay approach to ultrafast protein dynamics at XFELs.

PubMed

Ren, Zhong; Yang, Xiaojing

2016-07-01

X-ray crystallography promises direct insights into electron-density changes that lead to and arise from structural changes such as electron and proton transfer and the formation, rupture and isomerization of chemical bonds. The ultrashort pulses of hard X-rays produced by free-electron lasers present an exciting opportunity for capturing ultrafast structural events in biological macromolecules within femtoseconds after photoexcitation. However, shot-to-shot fluctuations, which are inherent to the very process of self-amplified spontaneous emission (SASE) that generates the ultrashort X-ray pulses, are a major source of noise that may conceal signals from structural changes. Here, a new approach is proposed to angularly split a single SASE pulse and to produce a temporal delay of picoseconds between the split pulses. These split pulses will allow the probing of two distinct states before and after photoexcitation triggered by a laser pulse between the split X-ray pulses. The split pulses originate from a single SASE pulse and share many common properties; thus, noise arising from shot-to-shot fluctuations is self-canceling. The unambiguous interpretation of ultrafast structural changes would require diffraction data at atomic resolution, as these changes may or may not involve any atomic displacement. This approach, in combination with the strategy of serial crystallography, offers a solution to study ultrafast dynamics of light-initiated biochemical reactions or biological processes at atomic resolution.

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.

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.

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.

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.

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

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

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.

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.

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.

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.

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.

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

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

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 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.

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

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

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.

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.

Observation of pulsed hard X-rays/gamma-rays from PSR 1509-58

NASA Astrophysics Data System (ADS)

Gunji, S.; Hirayama, M.; Kamae, T.; Miyazaki, S.; Sekimoto, Y.; Takahashi, T.; Tamura, T.; Tanaka, M.; Yamasaki, N.; Yamagami, T.; Nomachi, M.; Murakami, H.; Braga, J.; Neri, J. A.

1994-06-01

We observed a young rotation-powered pulsar, PSR 1509-58, in the hard X-ray/gamma-ray or the soft gamma-ray band with a balloon-borne detector in Brazil on 1991 November 19 (UT). With a timing analysis we detected pulsations in the energy band 94-240 keV at the 150.687 ms period determined from radio observations. The pulsating flux is (7.1 +/- 1.7) x 10-4 per sq cm per sec in this band, and the energy spectrum follows a power law with photon index alpha = 1.64 +/- 0.4. The averaged pulse profile shows a broad single peak with a sharp rise and has a duty cycle around 50% or higher: these features are similar to what have been observed in the X-ray band by the Ginga satellite. Based on the data available now, the fraction of energy transformed from rotational energy loss to pulsed/nonpulsed soft gamma-ray radiation is estimated. If the solid angle swept by the pulsed beam is about the same as for the Crab pulsar (PSR 0531+21) and the Vela pulsar (PSR 0833-45), PSR 1509-58 turn out to be an extremely efficient pulsar, converting a large fraction of its rotational energy loss to radiation, as the outer gap model predicts. The observed pulsed spectrum, however, is strong in the soft gamma-ray band, in a sharp contrast to what has been observed in the Vela pulsar, a pulsar expected to be similar PSR 1509-58 in the outer gap model. The fact that the pulse profile remains broad and single-peaked in the soft gamma-ray band is also new for Crab-like pulsars. In these regards, PSR 1509-58 may require some alteration to the standard outer gap model or even a new model for gamma-ray emission in pulsars.

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.

Establishing nonlinearity thresholds with ultraintense X-ray pulses

DOE PAGES

Szlachetko, Jakub; Hoszowska, Joanna; Dousse, Jean-Claude; ...

2016-09-13

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.more » Consequently, accurate knowledge about the threshold for nonlinear X-ray signals is essential. Here in this paper 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.« less

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

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.

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

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

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

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.

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.

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.

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).

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

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.

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.

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.

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

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

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

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.

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.

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.

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.

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.

Ultrafast Manipulation of Magnetic Order with Electrical Pulses

NASA Astrophysics Data System (ADS)

Yang, Yang

During the last 30 years spintronics has been a very rapidly expanding field leading to lots of new interesting physics and applications. As with most technology-oriented fields, spintronics strives to control devices with very low energy consumption and high speed. The combination of spin and electronics inherent to spintronics directly tackles energy efficiency, due to the non-volatility of magnetism. However, speed of operation of spintronic devices is still rather limited ( nanoseconds), due to slow magnetization precessional frequencies. Ultrafast magnetism (or opto-magnetism) is a relatively new field that has been very active in the last 20 years. The main idea is that intense femtosecond laser pulses can be used in order to manipulate the magnetization at very fast time-scales ( 100 femtoseconds). However, the use of femtosecond lasers poses great application challenges such as diffraction limited optical spot sizes which hinders device density, and bulky and expensive integration of femtosecond lasers into devices. In this thesis, our efforts to combine ultrafast magnetism and spintronics are presented. First, we show that the magnetization of ferrimagnetic GdFeCo films can be switched by picosecond electronic heat current pulses. This result shows that a non-thermal distribution of electrons directly excited by laser is not necessary for inducing ultrafast magnetic dynamics. Then, we fabricate photoconductive switch devices on a LT-GaAs substrate, to generate picosecond electrical pulses. Intense electrical pulses with 10ps (FWHM) duration and peak current up to 3A can be generated and delivered into magnetic films. Distinct magnetic dynamics in CoPt films are found between direct optical heating and electrical heating. More importantly, by delivering picosecond electrical pulses into GdFeCo films, we are able to deterministically reverse the magnetization of GdFeCo within 10ps. This is more than one order of magnitude faster than any other electrically

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

Ultrafast magnetization reversal by picosecond electrical pulses

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

Yang, Yang; Wilson, Richard B.; Gorchon, Jon

The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. Here, we unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electricalmore » switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.« less

Ultrafast magnetization reversal by picosecond electrical pulses

DOE PAGES

Yang, Yang; Wilson, Richard B.; Gorchon, Jon; ...

2017-11-03

The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. Here, we unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electricalmore » switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.« less

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.

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.

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.

A Non-thermal Pulsed X-Ray Emission of AR Scorpii

NASA Astrophysics Data System (ADS)

Takata, J.; Hu, C.-P.; Lin, L. C. C.; Tam, P. H. T.; Pal, P. S.; Hui, C. Y.; Kong, A. K. H.; Cheng, K. S.

2018-02-01

We report the analysis result of UV/X-ray emission from AR Scorpii, which is an intermediate polar (IP) composed of a magnetic white dwarf and an M-type star, with the XMM-Newton data. The X-ray/UV emission clearly shows a large variation over the orbit, and their intensity maximum (or minimum) is located at the superior conjunction (or inferior conjunction) of the M star orbit. The hardness ratio of the X-ray emission shows a small variation over the orbital phase and shows no indication of the absorption by an accretion column. These properties are naturally explained by the emission from the M star surface rather than that from the accretion column on the white dwarf’s (WD) star, which is similar to usual IPs. Additionally, the observed X-ray emission also modulates with the WD’s spin with a pulse fraction of ∼14%. The peak position is aligned in the optical/UV/X-ray band. This supports the hypothesis that the electrons in AR Scorpii are accelerated to a relativistic speed and emit non-thermal photons via the synchrotron radiation. In the X-ray bands, evidence of the power-law spectrum is found in the pulsed component, although the observed emission is dominated by the optically thin thermal plasma emissions with several different temperatures. It is considered that the magnetic dissipation/reconnection process on the M star surface heats up the plasma to a temperature of several keV and also accelerates the electrons to the relativistic speed. The relativistic electrons are trapped in the WD’s closed magnetic field lines by the magnetic mirror effect. In this model, the observed pulsed component is explained by the emissions from the first magnetic mirror point.

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.

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

Liquid explosions induced by X-ray laser pulses

DOE PAGES

Stan, Claudiu A.; Milathianaki, Despina; Laksmono, Hartawan; ...

2016-05-23

Explosions are spectacular and intriguing phenomena that expose the dynamics of matter under extreme conditions. We investigated, using time-resolved imaging, explosions induced by ultraintense X-ray laser pulses in water drops and jets. Our observations revealed an explosive vaporization followed by high-velocity interacting flows of liquid and vapour, and by the generation of shock trains in the liquid jets. These flows are different from those previously observed in laser ablation, owing to a simpler spatial pattern of X-ray absorption. We show that the explosion dynamics in our experiments is consistent with a redistribution of absorbed energy, mediated by a pressure ormore » shock wave in the liquid, and we model the effects of explosions, including their adverse impact on X-ray laser experiments. As a result, X-ray laser explosions have predictable dynamics that may prove useful for controlling the state of pure liquids over broad energy scales and timescales, and for triggering pressure-sensitive molecular dynamics in solutions.« 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

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.

Realizing Ultrafast Electron Pulse Self-Compression by Femtosecond Pulse Shaping Technique.

PubMed

Qi, Yingpeng; Pei, Minjie; Qi, Dalong; Yang, Yan; Jia, Tianqing; Zhang, Shian; Sun, Zhenrong

2015-10-01

Uncorrelated position and velocity distribution of the electron bunch at the photocathode from the residual energy greatly limit the transverse coherent length and the recompression ability. Here we first propose a femtosecond pulse-shaping method to realize the electron pulse self-compression in ultrafast electron diffraction system based on a point-to-point space-charge model. The positively chirped femtosecond laser pulse can correspondingly create the positively chirped electron bunch at the photocathode (such as metal-insulator heterojunction), and such a shaped electron pulse can realize the self-compression in the subsequent propagation process. The greatest advantage for our proposed scheme is that no additional components are introduced into the ultrafast electron diffraction system, which therefore does not affect the electron bunch shape. More importantly, this scheme can break the limitation that the electron pulse via postphotocathode static compression schemes is not shorter than the excitation laser pulse due to the uncorrelated position and velocity distribution of the initial electron bunch.

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

Pulsed x-ray generator for commercial gas lasers

NASA Astrophysics Data System (ADS)

Bollanti, S.; Bonfigli, F.; Di Lazzaro, P.; Flora, F.; Giordano, G.; Letardi, T.; Murra, D.; Schina, G.; Zheng, C. E.

2001-10-01

We have designed and tested a 1-m-long x-ray diode based on innovative plasma cathodes, which exploit commercial spark plugs as electron emitters. Based on the results of a numerical study, we optimized both diode geometry (e.g., the angle between anode and cathode surfaces, the thickness of the Al window) and electrical circuitry (e.g., the capacitance in series to each spark plug, the peak voltage of the anode) of our x-ray generator. The overall result is a simple and efficient circuitry, giving a total diode current in excess of 2.1 kA with a breakdown voltage of 70 kV, which generates a 50 ns rise-time x-ray pulse with a spatially averaged dosage of up to 6×10-4 Gy when using a Pb-wrapped anode. The double-diode x-ray generator was operated for 1.5×106 shots at a repetition rate of up to 30 Hz, and the lifetime test was interrupted without any fault. During the lifetime test, it was not necessary to adjust any working parameter. At the end of the lifetime test, the x-ray emission uniformity was better than 80% along the longitudinal axis. This x-ray generator has a lifetime, reliability, and cost fitting the requirements of industrial users. Among the broad range of potential applications, this x-ray generator is particularly suitable to ionize discharge pumped gas lasers, like TEA CO2 and excimer lasers, including those operated by x-ray triggered discharges.

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.

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.

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

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.

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.

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.

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

Pile-up corrections in laser-driven pulsed X-ray sources

NASA Astrophysics Data System (ADS)

Hernández, G.; Fernández, F.

2018-06-01

A formalism for treating the pile-up produced in solid-state detectors by laser-driven pulsed X-ray sources has been developed. It allows the direct use of X-ray spectroscopy without artificially decreasing the number of counts in the detector, assuming the duration of a pulse is much shorter than the detector response time and the loss of counts from the energy window of the detector can be modeled or neglected. Experimental application shows that having a small amount of pile-up subsequently corrected improves the signal-to-noise ratio, which would be more beneficial than the strict single-hit condition usually imposed on this detectors.

Pulse pile-up in hard X-ray detector systems. [for solar X-rays

NASA Technical Reports Server (NTRS)

Datlowe, D. W.

1975-01-01

When pulse-height spectra are measured by a nuclear detection system at high counting rates, the probability that two or more pulses will arrive within the resolving time of the system is significant. This phenomenon, pulse pile-up, distorts the pulse-height spectrum and must be considered in the interpretation of spectra taken at high counting rates. A computational technique for the simulation of pile-up is developed. The model is examined in the three regimes where (1) the time between pulses is long compared to the detector-system resolving time, (2) the time between pulses is comparable to the resolving time, and (3) many pulses occur within the resolving time. The technique is used to model the solar hard X-ray experiment on the OSO-7 satellite; comparison of the model with data taken during three large flares shows excellent agreement. The paper also describes rule-of-thumb tests for pile-up and identifies the important detector design factors for minimizing pile-up, i.e., thick entrance windows and short resolving times in the system electronics.

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

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.

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.

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.

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.

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.

Ultrafast Kα x-ray Thomson scattering from shock compressed lithium hydride

DOE PAGES

Kritcher, A. L.; Neumayer, P.; Castor, J.; ...

2009-04-13

Spectrally and temporally resolved x-ray Thomson scattering using ultrafast Ti Kα x rays has provided experimental validation for modeling of the compression and heating of shocked matter. The coalescence of two shocks launched into a solid density LiH target by a shaped 6 ns heater beam was observed from rapid heating to temperatures of 2.2 eV, enabling tests of shock timing models. Here, the temperature evolution of the target at various times during shock progression was characterized from the intensity of the elastic scattering component. The observation of scattering from plasmons, electron plasma oscillations, at shock coalescence indicates a transitionmore » to a dense metallic plasma state in LiH. From the frequency shift of the measured plasmon feature the electron density was directly determined with high accuracy, providing a material compression of a factor of 3 times solid density. The quality of data achieved in these experiments demonstrates the capability for single shot dynamic characterization of dense shock compressed matter. Here, the conditions probed in this experiment are relevant for the study of the physics of planetary formation and to characterize inertial confinement fusion targets for experiments such as on the National Ignition Facility, Lawrence Livermore National Laboratory.« less

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.

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.

ROSAT observations of pulsed soft X-ray emission from PSR 1055-52

NASA Technical Reports Server (NTRS)

Oegelman, Hakki; Finley, John P.

1993-01-01

Utilizing the position-sensitive proportional counter and the high-resolution imager aboard the orbiting X-ray observatory ROSAT, we have detected pulsations at the radio period from the pulsar PSR 1055-52. The pulse shapes are energy-dependent and show a transition at about 0.5 keV where the phase angle of the pulse peak changes by about -120 deg and the pulsed fraction increases from 11 percent to 63 percent toward larger energies. Simple spectral models are found to be unsatisfactory, while multicomponent models, such as a soft blackbody and hard power-law tail, yield better fits to the pulse-height data. The hard power-law tail is consistent with the extension of the recently reported EGRET results and may indicate a common emission mechanism for the X-ray through GeV gamma-ray regime. The soft blackbody component with T(infinity) = (7.5 +/- 0.6) x 10 exp 5 K, if interpreted as the initial cooling of a neutron star, is consistent with standard cooling models and does not require the presence of exotic components.

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

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

Pulsed x-ray sources for characterization of gated framing cameras

NASA Astrophysics Data System (ADS)

Filip, Catalin V.; Koch, Jeffrey A.; Freeman, Richard R.; King, James A.

2017-08-01

Gated X-ray framing cameras are used to measure important characteristics of inertial confinement fusion (ICF) implosions such as size and symmetry, with 50 ps time resolution in two dimensions. A pulsed source of hard (>8 keV) X-rays, would be a valuable calibration device, for example for gain-droop measurements of the variation in sensitivity of the gated strips. We have explored the requirements for such a source and a variety of options that could meet these requirements. We find that a small-size dense plasma focus machine could be a practical single-shot X-ray source for this application if timing uncertainties can be overcome.

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.

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.

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

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.

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.

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.

Discovery of X-Ray Emission from the Crab Pulsar at Pulse Minimum

NASA Technical Reports Server (NTRS)

Tennant, Allyn F.; Becker, Werner; Juda, Michael X.; Elsner, Ronald F.; Kolodziejczak, Jeffery J.; Murray, Stephen S.; ODell, Stephen L.; Paerels, Frits; Swartz, Douglas A.; Shibazaki, Noriaki;

Discovery of X-Ray Emission from the Crab Pulsar at Pulse Minimum

NASA Technical Reports Server (NTRS)

Tennant, Allyn F.; Becker, Werner; Juda, Michael; Elsner, Ronald F.; Kolodziejczak, Jeffery J.; Murray, Stephen S.; ODell, Stephen L.; Paerels, Frits; Swartz, Douglas A.

2001-01-01

The Chandra X-Ray Observatory observed the Crab pulsar using the Low-Energy Transmission Grating with the High-Resolution Camera. Time-resolved zeroth-order images reveal that the pulsar emits X-rays at all pulse phases. Analysis of the flux at minimum - most likely non-thermal in origin - places an upper limit (T(sub infinity) < 2.1 MK) on the surface temperature of the underlying neutron star. In addition, analysis of the pulse profile establishes that the error in the Chandra-determined absolute time is quite small, -0.2 +/- 0.1 ms.

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

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

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.

Hercules X-1: Pulsed gamma-rays detected above 150 GeV

NASA Technical Reports Server (NTRS)

Cawley, M. F.; Fegan, D. J.; Gibbs, K. G.; Gorham, P. W.; Kenny, S.; Lamb, R. C.; Liebing, D. F.; Porter, N. A.; Stenger, V. J.; Weekes, T. C.

1985-01-01

The 1.24 second binary pulsar Her X-1, first observed in X-rays in 1971 by UHURU has now been seen as a sporadic gamma ray source from 1 TeV up to at least 500 TeV. In addition, reprocessed optical and infrared pulses are seen from the companion star HZ Herculis. Thus measurements of the Her X-1/HZ Herculis system span 15 decades in energy, rivaling both the Crab pulsar and Cygnus X-3 in this respect for a discrete galactic source.

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.

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

Long pulse Soft X-ray Emission from Laser Generated Irradiated Gold Foils

NASA Astrophysics Data System (ADS)

Davis, Joshua; Frank, Yechiel; Raicher, Erez; Fraenkel, Moshe; Keiter, Paul; Klein, Sallee; Drake, R. P.; Shvarts, Dov

2016-10-01

Long pulse soft x-ray sources (SXS) allow for flexibility in high-energy-density experimental designs by providing a means of driving matter to the high temperatures needed, for example to study radiation waves in different materials. SXSs can be made by using lasers to heat a high-Z thin foil, which then acts as a quasi-blackbody emitter. Previous studies of the x-ray emission characteristics of gold foils have focused on laser pulses of 1ns or less. We performed experiments using a 6.0ns laser pulse with energy of 2kJ on the Omega-60 system to generate and characterize multi-ns laser heated Au foils of thicknesses between 0.5-2.0 μm. We measured the 2D spatial profile of the emission with a soft x-ray camera and the time history of the emission with the Dante photodiode array . Effective temperatures for the emission were then calculated using the Dante measurements. Discussion of experimental results and a comparison with 1-D Rad-Hydro NLTE simulations will be presented.

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.

Pulse-periodic generation of supershort avalanche electron beams and X-ray emission

NASA Astrophysics Data System (ADS)

Baksht, E. Kh.; Burachenko, A. G.; Erofeev, M. V.; Tarasenko, V. F.

2014-05-01

Pulse-periodic generation of supershort avalanche electron beams (SAEBs) and X-ray emission in nitrogen, as well as the transition from a single-pulse mode to a pulse-periodic mode with a high repetition frequency, was studied experimentally. It is shown that, in the pulse-periodic mode, the full width at halfmaximum of the SAEB is larger and the decrease rate of the gap voltage is lower than those in the single-pulse mode. It is found that, when the front duration of the voltage pulse at a nitrogen pressure of 90 Torr decreases from 2.5 to 0.3 ns, the X-ray exposure dose in the pulse-periodic mode increases by more than one order of magnitude and the number of SAEB electrons also increases. It is shown that, in the pulse-periodic mode of a diffuse discharge, gas heating in the discharge gap results in a severalfold increase in the SAEB amplitude (the number of electrons in the beam). At a generator voltage of 25 kV, nitrogen pressure of 90 Torr, and pulse repetition frequency of 3.5 kHz, a runaway electron beam was detected behind the anode foil.

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

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

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

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.

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

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%.

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

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

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.

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

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

X-Ray Pulse Selector With 2 ns Lock-in Phase Setting And Stability

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

Lindenau, B.; Raebiger, J.; Polachowski, S.

2004-05-12

Selector devices, which are based on magnetically suspended, high speed triangular shutter rotors, have been designed and built in cooperation with ESRF, APS, and recently Spring-8 for time resolved studies with isolated x-ray pulses at white beam lines. The x-ray pulse selection is accomplished by means of a beam channel along one of the edges of the triangular rotor, which opens once per revolution. Entrance and exit apertures of the channel can be designed wedge shaped for variable tuning of the channel height between 0.1 mm to 0.9 mm. At the 1 kHz maximum operation frequency of a 220 mmmore » diameter disk with 190 mm channel length, the practicable open times of the channel are demonstrated to range down to 200 ns. The selector drive electronics is directly coupled to the storage ring RF clock for rotational phase control. It allows for continuous selector operation in phase locked mode to the temporal pulse structure of the synchrotron at 2 ns RMS stability. The phase angle between the pulse transmission period and the synchrotron bunch sequence can be adjusted with similar precision for X-ray pulse selection according to the experimental needs. ID09, Michael Wulff ; BioCARS 14-BM, Reinhard Pahl; BL40-XU, Shin-ichi Adachi.« 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.

Few-cycle pulse generation in an x-ray free-electron laser.

PubMed

Dunning, D J; McNeil, B W J; Thompson, N R

2013-03-08

A method is proposed to generate trains of few-cycle x-ray pulses from a free-electron laser (FEL) amplifier via a compact "afterburner" extension consisting of several few-period undulator sections separated by electron chicane delays. Simulations show that in the hard x ray (wavelength ~0.1 nm; photon energy ~10 keV) and with peak powers approaching normal FEL saturation (GW) levels, root mean square pulse durations of 700 zs may be obtained. This is approximately two orders of magnitude shorter than that possible for normal FEL amplifier operation. The spectrum is discretely multichromatic with a bandwidth envelope increased by approximately 2 orders of magnitude over unseeded FEL amplifier operation. Such a source would significantly enhance research opportunity in atomic dynamics and push capability toward nuclear dynamics.

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.

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

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

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

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

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.

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.

Pulse periods and the long-term variations of the X-ray pulsars VELA X-1 and Centaurus X-3

NASA Astrophysics Data System (ADS)

Tsunemi, Hiroshi

The paper reports recent determinations of the pulse period for two X-ray pulsars, Vela X-1 and Cen X-3, made in 1987 with the All Sky Monitor (ASM) on board the Ginga satellite. The heliocentric pulse periods are 283.09 + or - 0.01 s and 4.8229 + or - 0.0001 s, respectively. These are the longest and shortest values in their respective observational histories. The random walk model for the Vela X-1 pulsar can explain this result as well as those obtained previously. It is also noted that the pulse-period change for the Cen X-3 system shows a 9-yr periodicity. This is probably due to the activity of the companion star rather than to Doppler-shift variations due to a third body or the precession of the neutron star.

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

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

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.

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

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.

Radiation-Induced Chemical Dynamics in Ar Clusters Exposed to Strong X-Ray Pulses.

PubMed

Kumagai, Yoshiaki; Jurek, Zoltan; Xu, Weiqing; Fukuzawa, Hironobu; Motomura, Koji; Iablonskyi, Denys; Nagaya, Kiyonobu; Wada, Shin-Ichi; Mondal, Subhendu; Tachibana, Tetsuya; Ito, Yuta; Sakai, Tsukasa; Matsunami, Kenji; Nishiyama, Toshiyuki; Umemoto, Takayuki; Nicolas, Christophe; Miron, Catalin; Togashi, Tadashi; Ogawa, Kanade; Owada, Shigeki; Tono, Kensuke; Yabashi, Makina; Son, Sang-Kil; Ziaja, Beata; Santra, Robin; Ueda, Kiyoshi

2018-06-01

We show that electron and ion spectroscopy reveals the details of the oligomer formation in Ar clusters exposed to an x-ray free electron laser (XFEL) pulse, i.e., chemical dynamics triggered by x rays. With guidance from a dedicated molecular dynamics simulation tool, we find that van der Waals bonding, the oligomer formation mechanism, and charge transfer among the cluster constituents significantly affect ionization dynamics induced by an XFEL pulse of moderate fluence. Our results clearly demonstrate that XFEL pulses can be used not only to "damage and destroy" molecular assemblies but also to modify and transform their molecular structure. The accuracy of the predictions obtained makes it possible to apply the cluster spectroscopy, in connection with the respective simulations, for estimation of the XFEL pulse fluence in the fluence regime below single-atom multiple-photon absorption, which is hardly accessible with other diagnostic tools.

Radiation-Induced Chemical Dynamics in Ar Clusters Exposed to Strong X-Ray Pulses

NASA Astrophysics Data System (ADS)

Kumagai, Yoshiaki; Jurek, Zoltan; Xu, Weiqing; Fukuzawa, Hironobu; Motomura, Koji; Iablonskyi, Denys; Nagaya, Kiyonobu; Wada, Shin-ichi; Mondal, Subhendu; Tachibana, Tetsuya; Ito, Yuta; Sakai, Tsukasa; Matsunami, Kenji; Nishiyama, Toshiyuki; Umemoto, Takayuki; Nicolas, Christophe; Miron, Catalin; Togashi, Tadashi; Ogawa, Kanade; Owada, Shigeki; Tono, Kensuke; Yabashi, Makina; Son, Sang-Kil; Ziaja, Beata; Santra, Robin; Ueda, Kiyoshi

2018-06-01

We show that electron and ion spectroscopy reveals the details of the oligomer formation in Ar clusters exposed to an x-ray free electron laser (XFEL) pulse, i.e., chemical dynamics triggered by x rays. With guidance from a dedicated molecular dynamics simulation tool, we find that van der Waals bonding, the oligomer formation mechanism, and charge transfer among the cluster constituents significantly affect ionization dynamics induced by an XFEL pulse of moderate fluence. Our results clearly demonstrate that XFEL pulses can be used not only to "damage and destroy" molecular assemblies but also to modify and transform their molecular structure. The accuracy of the predictions obtained makes it possible to apply the cluster spectroscopy, in connection with the respective simulations, for estimation of the XFEL pulse fluence in the fluence regime below single-atom multiple-photon absorption, which is hardly accessible with other diagnostic tools.

Demonstration of Two-Atom Entanglement with Ultrafast Optical Pulses

NASA Astrophysics Data System (ADS)

Wong-Campos, J. D.; Moses, S. A.; Johnson, K. G.; Monroe, C.

2017-12-01

We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just ten pulses, each of ˜20 ps duration, and demonstrate an entangled Bell state with (76 ±1 )% fidelity. These results pave the way for entanglement operations within a large collection of qubits by exciting only local modes of motion.

Demonstration of Two-Atom Entanglement with Ultrafast Optical Pulses.

PubMed

Wong-Campos, J D; Moses, S A; Johnson, K G; Monroe, C

2017-12-08

We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just ten pulses, each of ∼20  ps duration, and demonstrate an entangled Bell state with (76±1)% fidelity. These results pave the way for entanglement operations within a large collection of qubits by exciting only local modes of motion.

A pulse shape discriminator and an online system for the balloon-borne hard X-ray/gamma-ray detector

NASA Astrophysics Data System (ADS)

Takahashi, T.; Kamae, T.; Tanaka, M.; Gunji, S.; Miyazuki, S.; Tamura, T.; Sekimoto, Y.; Yamaoka, N.; Nishimura, J.; Yajima, N.

Attention is given to a new kind of phoswich counters (the well-type phoswich counter) that will be capable of detecting very low flux hard X-rays/gamma-rays (40-1000 keV) from astronomical objects. A specially designed pulse-shape discriminator (PSD) selects hard X-rays/gamma-rays that has deposited energy only in the detection part. Sixty-four such counters are assembled into an array where each phoswich element acts as an active shield to the neighboring elements too. The ADCs, the TDCs, the hit-pattern latches, and the precision clock are read out by a VME-based online system, stored on an 8-mm video tape, and transmitted to the ground station. The design and performance of the pulse shape discriminator and the online system are described.

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 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.

Generation of subterawatt-attosecond pulses in a soft x-ray free-electron laser

DOE PAGES

Huang, Senlin; Ding, Yuantao; Huang, Zhirong; ...

2016-08-15

Here, we propose a novel scheme to generate attosecond soft x rays in a self-seeded free-electron laser (FEL) suitable for enabling attosecond spectroscopic investigations. A time-energy chirped electron bunch with additional sinusoidal energy modulation is adopted to produce a short seed pulse through a self-seeding monochromator. This short seed pulse, together with high electron current spikes and a cascaded delay setup, enables a high-efficiency FEL with a fresh bunch scheme. Simulations show that using the Linac Coherent Light Source (LCLS) parameters, soft x-ray pulses with a FWHM of 260 attoseconds and a peak power of 0.5 TW can be obtained.more » This scheme also has the feature of providing a stable central wavelength determined by the self-seeding monochromator.« 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.

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.

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

X-ray Evidence for Ultra-Fast Outflows in Local AGNs

NASA Astrophysics Data System (ADS)

Tombesi, F.; Cappi, M.; Sambruna, R. M.; Reeves, J. N.; Reynolds, C. S.; Braito, V.; Dadina, M.

2012-08-01

X-ray evidence for ultra-fast outflows (UFOs) has been recently reported in a number of local AGNs through the detection of blue-shifted Fe XXV/XXVI absorption lines. We present the results of a comprehensive spectral analysis of a large sample of 42 local Seyferts and 5 Broad-Line Radio Galaxies (BLRGs) observed with XMM-Newton and Suzaku. We detect UFOs in ga 40% of the sources. Their outflow velocities are in the range ˜ 0.03-0.3c, with a mean value of ˜ 0.14c. The ionization is high, in the range logℰ ˜3-6rm erg s-1 cm, and also the associated column densities are large, in the interval ˜ 1022-1024rm cm-2. Overall, these results point to the presence of highly ionized and massive outflowing material in the innermost regions of AGNs. Their variability and location on sub-pc scales favor a direct association with accretion disk winds/outflows. This also suggests that UFOs may potentially play a significant role in the AGN cosmological feedback besides jets, and their study can provide important clues on the connection between accretion disks, winds, and jets.

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

A Study of Pulse Shape Evolution and X-Ray Reprocessing in Her X-1

NASA Technical Reports Server (NTRS)

Cushman, Paula P.

1998-01-01

This study focused on the pulse shape evolution and spectral properties of the X-ray binary Her X-1 with regard to the well known 35-day cycle of Her X-1. A follow-up set of RXTE observations has been conducted in RXTE AO-2 phase and the two observation sets are being analyzed together. We presented results of early analysis of pulse shape evolution in "Proceedings of the Fourth Compton Symposium". More advanced analysis was presented at the HEAD meeting in November, 1997 in Estes Park, Colorado. A related study of the 35-day cycle using RXTE/ASM data, which laid out the overall picture within which the more detailed PCA observations could be placed has also been conducted. The results of this study have been published. A pair of papers on the detailed pulse evolution and the spectral/color evolution are currently being prepared for publication. Some of the significant results of this study have been a confirmation of the detailed pulse profile changes at the end of the Main High state in HerX-1 first observed by GINGA, observations of the pulse evolution in several Short High states which agree with the pulse evolution pattern predicted using a disk occultation model, observation of a systematic lengthening of the eclipse egress during the Main High state of the 35-day phase and observation of a new type of extended eclipse ingress during which pulsations cease to observed during the Short High state.

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.

Characterization of short-pulse laser-produced x-rays for diagnosing magnetically driven cylindrical isentropic compression

NASA Astrophysics Data System (ADS)

Sawada, Hiroshi; Daykin, Tyler; Bauer, Bruno; Beg, Farhat

2017-10-01

We have developed an experimental platform to study material properties of magnetically compressed cylinder using a 1 MA pulsed power generator Zebra and a 50 TW subpicosecond short-pulse laser Leopard at the UNR's Nevada Terawatt Facility. According to a MHD simulation, strong magnetic fields generated by 100 ns rise time Zebra current can quasi-isentropically compress a material to the strongly coupled plasma regime. Taking advantage of the cylindrical geometry, a metal rod can be brought to higher pressures than that in the planar geometry. To diagnose the compressed rod with high precision x-ray measurements, an initial laser-only experiment was carried out to characterize laser-produced x-rays. Interaction of a high-intensity, short-pulse laser with solids produces broadband and monochromatic x-rays with photon energies high enough to probe dense metal rods. Bremsstrahlung was measured with Imaging plate-based filter stack spectrometers and monochromatic 8.0 keV Cu K-alpha was recorded with an absolutely calibrated Bragg crystal spectrometer. The broadband x-ray source was applied to radiography of thick metal objects and different filter materials were tested. The experimental results and a design of a coupled experiment will be presented.

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.

A bright attosecond x-ray pulse train generation in a double-laser-driven cone target

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

Hu, Li-Xiang; Yu, Tong-Pu, E-mail: tongpu@nudt.edu.cn; Shao, Fu-Qiu

By using full three-dimensional particle-in-cell and Monte Carlo simulations, we investigate the generation of a high-brightness attosecond x-ray pulse train in a double-laser-driven cone target. The scheme makes use of two lasers: the first high-intensity laser with a laser peak intensity 1.37 × 10{sup 20 }W/cm{sup 2} irradiates the cone and produces overdense attosecond electron bunches; the second counterpropagating weakly relativistic laser with a laser peak intensity 4.932 × 10{sup 17 }W/cm{sup 2} interacts with the produced electron bunches and a bright x-ray pulse train is generated by Thomson backscattering of the second laser off the attosecond electron bunches. It is shown that the photon fluxmore » rises by 5 times using the cone target as compared with a normal channel. Meanwhile, the x-ray peak brightness increases significantly from 1.4 × 10{sup 21}/(s mm{sup 2} mrad{sup 2} 0.1 keV) to 6.0 × 10{sup 21}/(s mm{sup 2} mrad{sup 2} 0.1 keV), which is much higher than that of the Thomson x-ray source generated from traditional accelerators. We also discuss the influence of the laser and target parameters on the x-ray pulse properties. This compact bright x-ray source may have diverse applications, e.g., the study of electric dynamics and harmonics emission in the atomic scale.« 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

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

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

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

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

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.

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.

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

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

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.

Characterisation of flash X-ray source generated by Kali-1000 Pulse Power System

NASA Astrophysics Data System (ADS)

Satyanarayana, N.; Durga Prasada Rao, A.; Mittal, K. C.

2016-02-01

The electron beam-driven Rod Pinch Diode (RPD) is presently fielded on KALI-1000 Pulse Power System at Bhabha Atomic Research Centre, Visakhapatnam and is a leading candidate for future flash X-ray radiographic sources. The diode is capable of producing less than 2-mm radiation spot sizes and greater than 350 milli rads of dose measured at 1 m from the X-ray source. KALI-1000 Pulse Power Source is capable of delivering up to 600 kV using a Tesla Transformer with Demineralized Insulated Transmission Line (DITL), the diode typically operates between 250-330 kV . Since the radiation dose has a power-law dependence on diode voltage, this limits the dose production on KALI-1000 system. Radiation dose with angular variation is measured using thermoluminescent detectors (TLD's) and the X-ray spot size is measured using pin hole arrangement with image plate (IP) to obtain the time-integrated source profile as well as a time-resolved spot diagnostic. An X-ray pinhole camera was used to pick out where the energetic e-beam connects to the anode. Ideally the diode should function such that the radiation is emitted from the tip. The camera was mounted perpendicular to the machine's axis to view the radiation from the tip. Comparison of the spot sizes of the X-ray sources obtained by the pin hole and rolled edge arrangements was carried and results obtained by both the techniques are with in ± 10% of the average values.

Generation of plasma X-ray sources via high repetition rate femtosecond laser pulses

NASA Astrophysics Data System (ADS)

Baguckis, Artūras; Plukis, Artūras; Reklaitis, Jonas; Remeikis, Vidmantas; Giniūnas, Linas; Vengris, Mikas

2017-12-01

In this study, we present the development and characterization of Cu plasma X-ray source driven by 20 W average power high repetition rate femtosecond laser in ambient atmosphere environment. The peak Cu- Kα photon flux of 2.3 × 109 photons/s into full solid angle is demonstrated (with a process conversion efficiency of 10-7), using pulses with peak intensity of 4.65 × 1014 W/cm2. Such Cu- Kα flux is significantly larger than others found in comparable experiments, performed in air environment. The effects of resonance plasma absorption process, when optimized, are shown to increase measured flux by the factor of 2-3. The relationship between X-ray photon flux and plasma-driving pulse repetition rate is quasi-linear, suggesting that fluxes could further be increased to 1010 photons/s using even higher average powers of driving radiation. These results suggest that to fully utilize the potential of high repetition rate laser sources, novel target material delivery systems (for example, jet-based ones) are required. On the other hand, this study demonstrates that high energy lasers currently used for plasma X-ray sources can be conveniently and efficiently replaced by high average power and repetition rate laser radiation, as a way to increase the brightness of the generated X-rays.

Pulse-resolved intensity measurements at a hard X-ray FEL using semi-transparent diamond detectors

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

Roth, Thomas; Freund, Wolfgang; Boesenberg, Ulrike

Solid-state ionization chambers are presented based on thin diamond crystals that allow pulse-resolved intensity measurements at a hard X-ray free-electron laser (FEL), up to the 4.5 MHz repetition rate that will become available at the European XFEL. Due to the small X-ray absorption of diamond the thin detectors are semi-transparent which eases their use as non-invasive monitoring devices in the beam. FELs are characterized by strong pulse-to-pulse intensity fluctuations due to the self-amplified spontaneous emission (SASE) process and in many experiments it is mandatory to monitor the intensity of each individual pulse. Two diamond detectors with different electrode materials, berylliummore » and graphite, were tested as intensity monitors at the XCS endstation of the Linac Coherent Light Source (LCLS) using the pink SASE beam at 9 keV. The performance is compared with LCLS standard monitors that detect X-rays backscattered from thin SiN foils placed in the beam. In conclusion, the graphite detector can also be used as a beam position monitor although with rather coarse resolution.« less

Pulse-resolved intensity measurements at a hard X-ray FEL using semi-transparent diamond detectors

DOE PAGES

Roth, Thomas; Freund, Wolfgang; Boesenberg, Ulrike; ...

2018-01-01

Solid-state ionization chambers are presented based on thin diamond crystals that allow pulse-resolved intensity measurements at a hard X-ray free-electron laser (FEL), up to the 4.5 MHz repetition rate that will become available at the European XFEL. Due to the small X-ray absorption of diamond the thin detectors are semi-transparent which eases their use as non-invasive monitoring devices in the beam. FELs are characterized by strong pulse-to-pulse intensity fluctuations due to the self-amplified spontaneous emission (SASE) process and in many experiments it is mandatory to monitor the intensity of each individual pulse. Two diamond detectors with different electrode materials, berylliummore » and graphite, were tested as intensity monitors at the XCS endstation of the Linac Coherent Light Source (LCLS) using the pink SASE beam at 9 keV. The performance is compared with LCLS standard monitors that detect X-rays backscattered from thin SiN foils placed in the beam. In conclusion, the graphite detector can also be used as a beam position monitor although with rather coarse resolution.« less

Double-Wall Carbon Nanotubes for Wide-Band, Ultrafast Pulse Generation

PubMed Central

2014-01-01

We demonstrate wide-band ultrafast optical pulse generation at 1, 1.5, and 2 μm using a single-polymer composite saturable absorber based on double-wall carbon nanotubes (DWNTs). The freestanding optical quality polymer composite is prepared from nanotubes dispersed in water with poly(vinyl alcohol) as the host matrix. The composite is then integrated into ytterbium-, erbium-, and thulium-doped fiber laser cavities. Using this single DWNT–polymer composite, we achieve 4.85 ps, 532 fs, and 1.6 ps mode-locked pulses at 1066, 1559, and 1883 nm, respectively, highlighting the potential of DWNTs for wide-band ultrafast photonics. PMID:24735347

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

XUV and x-ray elastic scattering of attosecond electromagnetic pulses on atoms

NASA Astrophysics Data System (ADS)

Rosmej, F. B.; Astapenko, V. A.; Lisitsa, V. S.

2017-12-01

Elastic scattering of electromagnetic pulses on atoms in XUV and soft x-ray ranges is considered for ultra-short pulses. The inclusion of the retardation term, non-dipole interaction and an efficient scattering tensor approximation allowed studying the scattering probability in dependence of the pulse duration for different carrier frequencies. Numerical calculations carried out for Mg, Al and Fe atoms demonstrate that the scattering probability is a highly nonlinear function of the pulse duration and has extrema for pulse carrier frequencies in the vicinity of the resonance-like features of the polarization charge spectrum. Closed expressions for the non-dipole correction and the angular dependence of the scattered radiation are obtained.

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.

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

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

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

Compact X-ray sources: X-rays from self-reflection

NASA Astrophysics Data System (ADS)

Mangles, Stuart P. D.

2012-05-01

Laser-based particle acceleration offers a way to reduce the size of hard-X-ray sources. Scientists have now developed a simple scheme that produces a bright flash of hard X-rays by using a single laser pulse both to generate and to scatter an electron beam.

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.

Material processing with fiber based ultrafast pulse delivery

NASA Astrophysics Data System (ADS)

Baumbach, S.; Stockburger, R.; Führa, B.; Zoller, S.; Thum, S.; Moosmann, J.; Maier, D.; Kanal, F.; Russ, S.; Kaiser, E.; Budnicki, A.; Sutter, D. H.; Pricking, S.; Killi, A.

2018-02-01

We report on TRUMPF's ultrafast laser systems equipped with industrialized hollow core fiber laser light cables. Beam guidance in general by means of optical fibers, e.g. for multi kilowatt cw laser systems, has become an integral part of laser-based material processing. One advantage of fiber delivery, among others, is the mechanical separation between laser and processing head. An equally important benefit is given by the fact that the fiber end acts as an opto-mechanical fix-point close to successive optical elements in the processing head. Components like lenses, diffractive optical elements etc. can thus be designed towards higher efficiency which results in better material processing. These aspects gain increasing significance when the laser system operates in fundamental mode which is usually the case for ultrafast lasers. Through the last years beam guidance of ultrafast laser pulses by means of hollow core fiber technology established very rapidly. The combination of TRUMPF's long-term stable ultrafast laser sources, passive fiber coupling, connector and packaging forms a flexible and powerful system for laser based material processing well suited for an industrial environment. In this article we demonstrate common material processing applications with ultrafast lasers realized with TRUMPF's hollow core fiber delivery. The experimental results are contrasted and evaluated against conventional free space propagation in order to illustrate the performance of flexible ultrafast beam delivery.

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.

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.

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.

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

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.

X-ray evidence for ultra-fast outflows in AGNs

NASA Astrophysics Data System (ADS)

Tombesi, Francesco; Sambruna, Rita; Braito, Valentina; Reeves, James; Reynolds, Christopher; Cappi, Massimo

2012-07-01

X-ray evidence for massive, highly ionized, ultra-fast outflows (UFOs) has been recently reported in a number of AGNs through the detection of blue-shifted Fe XXV/XXVI absorption lines. We present the results of a comprehensive spectral analysis of a large sample of 42 local Seyferts and 5 radio galaxies observed with XMM-Newton and Suzaku. We assessed the global detection significance of the absorption lines and performed a detailed photo-ionization modeling. We find that UFOs are common phenomena, being present in >40% of the sources. Their outflow velocity distribution is in the range ˜0.03--0.3c, with mean value of ˜0.14c. The ionization parameter is very high, in the range logξ˜3--6 erg~s^{-1}~cm, and the associated column densities are also large, in the range ˜10^{22}--10^{24} cm^{-2}. Their location is constrained at ˜0.0003--0.03pc (˜10^2--10^4 r_s) from the central black hole, consistent with what is expected for accretion disk winds/outflows. The mass outflow rates are in the interval ˜0.01--1M_{⊙}~yr^{-1} and the associated mechanical power is high, in the range ˜10^{43}--10^{45} erg/s. Therefore, UFOs are capable to provide a significant contribution to the AGN cosmological feedback and their study can provide important clues on the connection between accretion disks, winds and jets.

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.

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

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

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].

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.

Development of a Real-Time Pulse Processing Algorithm for TES-Based X-Ray Microcalorimeters

NASA Technical Reports Server (NTRS)

Tan, Hui; Hennig, Wolfgang; Warburton, William K.; Doriese, W. Bertrand; Kilbourne, Caroline A.

2011-01-01

We report here a real-time pulse processing algorithm for superconducting transition-edge sensor (TES) based x-ray microcalorimeters. TES-based. microca1orimeters offer ultra-high energy resolutions, but the small volume of each pixel requires that large arrays of identical microcalorimeter pixe1s be built to achieve sufficient detection efficiency. That in turn requires as much pulse processing as possible must be performed at the front end of readout electronics to avoid transferring large amounts of data to a host computer for post-processing. Therefore, a real-time pulse processing algorithm that not only can be implemented in the readout electronics but also achieve satisfactory energy resolutions is desired. We have developed an algorithm that can be easily implemented. in hardware. We then tested the algorithm offline using several data sets acquired with an 8 x 8 Goddard TES x-ray calorimeter array and 2x16 NIST time-division SQUID multiplexer. We obtained an average energy resolution of close to 3.0 eV at 6 keV for the multiplexed pixels while preserving over 99% of the events in the data sets.

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.

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.

Tunable X-ray source

DOEpatents

Boyce, James R [Williamsburg, VA

2011-02-08

A method for the production of X-ray bunches tunable in both time and energy level by generating multiple photon, X-ray, beams through the use of Thomson scattering. The method of the present invention simultaneously produces two X-ray pulses that are tunable in energy and/or time.

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.

X-ray evidence for ultra-fast outflows in Seyfert galaxies

NASA Astrophysics Data System (ADS)

Tombesi, Francesco; Braito, Valentina; Reeves, James; Cappi, Massimo; Dadina, Mauro

2012-07-01

X-ray evidence for massive, highly ionized, ultra-fast outflows (UFOs) has been recently reported in a number of AGNs through the detection of blue-shifted Fe XXV/XXVI absorption lines. We present the results of a comprehensive spectral analysis of a large sample of 42 local Seyferts observed with XMM-Newton. Similar results are also obtained from a Suzaku analysis of 5 radio galaxies. We find that UFOs are common phenomena, being present in >40% of the sources. Their outflow velocity distribution is in the range ˜0.03--0.3c, with mean value of ˜0.14c. The ionization parameter is very high, in the range logξ˜3--6 erg~s^{-1}~cm, and the associated column densities are also large, in the range ˜10^{22}--10^{24} cm^{-2}. Their location is constrained at ˜0.0003--0.03pc (˜10^2--10^4 r_s) from the central black hole, consistent with what is expected for accretion disk winds/outflows. The mass outflow rates are in the interval ˜0.01--1M_{⊙}~yr^{-1}. The associated mechanical power is also high, in the range ˜10^{43}--10^{45} erg/s, which indicates that UFOs are capable to provide a significant contribution to the AGN cosmological feedback.

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.

Long-Term Time Variability in the X-Ray Pulse Shape of the Crab Nebula Pulsar

NASA Astrophysics Data System (ADS)

Fazio, Giovanni G.

2000-01-01

This is the final performance report for our grant 'Long-Term Time Variability in the X-Ray Pulse Shape of the Crab Nebula Pulsar.' In the first year of this grant, we received the 50,000-second ROSAT (German acronym for X-ray satellite) High Resolution Images (HRI) observation of the Crab Nebula pulsar. We used the data to create a 65-ms-resolution pulse profile and compared it to a similar pulse profile obtained in 1991. No statistically significant differences were found. These results were presented at the January 1998 meeting of the American Astronomical Society. Since then, we have performed more sensitive analyses to search for potential changes in the pulse profile shape between the two data sets. Again, no significant variability was found. In order to augment this long (six-year) baseline data set, we have analyzed archival observations of the Crab Nebula pulsar with the Rossi X-Ray Timing Explorer (RXTE). While these observations have shorter time baselines than the ROSAT data set, their higher signal-to-noise offers similar sensitivity to long-term variability. Again, no significant variations have been found, confirming our ROSAT results. This work was done in collaboration with Prof. Stephen Eikenberry, Cornell University. These analyses will be included in Cornell University graduate student Dae-Sik Moon's doctoral thesis.

The determination of the pulse pile-up reject (PUR) counting for X and gamma ray spectrometry

NASA Astrophysics Data System (ADS)

Karabıdak, S. M.; Kaya, S.

2017-02-01

The collection the charged particles produced by the incident radiation on a detector requires a time interval. If this time interval is not sufficiently short compared with the peaking time of the amplifier, a loss in the recovered signal amplitude occurs. Another major constraint on the throughput of modern x or gamma-ray spectrometers is the time required for the subsequent the pulse processing by the electronics. Two above-mentioned limitations are cause of counting losses resulting from the dead time and the pile-up. The pulse pile-up is a common problem in x and gamma ray radiation detection systems. The pulses pile-up in spectroscopic analysis can cause significant errors. Therefore, inhibition of these pulses is a vital step. A way to reduce errors due to the pulse pile-up is a pile-up inspection circuitry (PUR). Such a circuit rejects some of the pulse pile-up. Therefore, this circuit leads to counting losses. Determination of these counting losses is an important problem. In this work, a new method is suggested for the determination of the pulse pile-up reject.

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.

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

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

Correlations in Scattered X-Ray Laser Pulses Reveal Nanoscale Structural Features of Viruses

NASA Astrophysics Data System (ADS)

Kurta, Ruslan P.; Donatelli, Jeffrey J.; Yoon, Chun Hong; Berntsen, Peter; Bielecki, Johan; Daurer, Benedikt J.; DeMirci, Hasan; Fromme, Petra; Hantke, Max Felix; Maia, Filipe R. N. C.; Munke, Anna; Nettelblad, Carl; Pande, Kanupriya; Reddy, Hemanth K. N.; Sellberg, Jonas A.; Sierra, Raymond G.; Svenda, Martin; van der Schot, Gijs; Vartanyants, Ivan A.; Williams, Garth J.; Xavier, P. Lourdu; Aquila, Andrew; Zwart, Peter H.; Mancuso, Adrian P.

2017-10-01

We use extremely bright and ultrashort pulses from an x-ray free-electron laser (XFEL) to measure correlations in x rays scattered from individual bioparticles. This allows us to go beyond the traditional crystallography and single-particle imaging approaches for structure investigations. We employ angular correlations to recover the three-dimensional (3D) structure of nanoscale viruses from x-ray diffraction data measured at the Linac Coherent Light Source. Correlations provide us with a comprehensive structural fingerprint of a 3D virus, which we use both for model-based and ab initio structure recovery. The analyses reveal a clear indication that the structure of the viruses deviates from the expected perfect icosahedral symmetry. Our results anticipate exciting opportunities for XFEL studies of the structure and dynamics of nanoscale objects by means of angular correlations.

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.

The Experimental Study of Characterized Noble Gas Puffs Irradiated by Ultra-Short Laser Pulses Compared with X-Pinches as an X-Ray Source

NASA Astrophysics Data System (ADS)

Schultz, Kimberly Ann

The goal of this dissertation is to study the basic physics and X-ray emission (1-10 keV) of two X-ray sources: X-pinch plasmas and a clustered gas-puff irradiated by an ultrashort laser pulse. X-pinches and other typical X-ray sources using solid targets create hot debris that can damage sensitive equipment. Therefore, to perform sensitive backlighting or X-ray effects testing, debris-free sources of radiation must be investigated. In this work, the author presents a broad study of clustered noble gas puffs including characterization measurements and laser heating experiments using several gas nozzles and multiple gases. Ultimately, the goal is to compare the laser-irradiated gas-puff and X-pinch plasmas as X-ray sources. Characterization of the gas puffs is performed at the Radiation Physics Laboratory at the University of Nevada, Reno (UNR) Physics Department using optical interferometry and Rayleigh scattering to determine density and cluster radius. By changing the gas-puff variables control of both the density and cluster size of the gas jets is obtained. Two laser systems provide the high intensities desired for the laser-irradiated gas puff experiments: the UNR Leopard Laser (1-2x1019 W/cm2) and the Lawrence Livermore National Laboratory's Titan Laser (7x1019 W/cm2). X-ray emission is studied as a function of laser pulse parameters, gas target type, gas puff density, and the gas-delay timing between puff initiation and laser interaction with the puff. The tested gases are Ar, Kr, Xe, and four mixtures of the noble gases. Time-resolved X-ray measurements are captured with Silicon diodes and photoconducting diamond detectors. Electron beam detectors include Faraday cups and a high-energy (> 1 MeV) electron spectrometer. Modeling of spectra from X-ray crystal spectrometers provides plasma density and temperature measurement and a molecular dynamics (MD) code describes cluster interactions with the laser pulse. The conversion of laser energy into X rays is also

The 5 Hour Pulse Period and Broadband Spectrum of the Symbiotic X-Ray Binary 3A 1954+319

NASA Technical Reports Server (NTRS)

Marcu, Diana M.; Fuerst, Felix; Pottschmidt, Katja; Grinberg, Victoria; Miller, Sebstian; Wilms, Joern; Postnov, Konstantin A.; Corbet, Robin H. D.; Markwardt, Craig B.; Cadolle Bel, Marion

2011-01-01

We present an analysis of the highly variable accreting X-ray pulsar 3A 1954+319 using 2005-2009 monitoring data obtained with INTEGRAL and Swift. This considerably extends the pulse period history and covers flaring episodes in 2005 and 2008. In 2006 the source was identified as one of only a few known symbiotic X-ray binaries, Le" systems composed of a neutron star accreting from the inhomogeneous medium around an M-giant star. The extremely long pulse period of approximately 5.3 h is directly visible in the 2008 INTEGRAL-ISGRI outburst light curve. The pulse profile is double peaked and not significantly energy dependent. During the outburst a strong spin-up of -1.8 x 10(exp -4) h h(exp -1) occurred. Between 2005 and 2008 a long term spin-down trend of 2.1 x 10(exp -5) h h(exp -1) was observed for the first time for this source. The 3-80 keV pulse peak spectrum of 3A 1954+319 during the 2008 flare could be well described by a thermal Comptonization model. We interpret the results within the framework of a recently developed quasi-spherical accretion model for symbiotic X-ray binaries.

Optimal generation of spatially coherent soft X-ray isolated attosecond pulses in a gas-filled waveguide using two-color synthesized laser pulses

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

Jin, Cheng; Hong, Kyung -Han; Lin, C. D.

2016-12-08

Here, we numerically demonstrate the generation of intense, low-divergence soft X-ray isolated attosecond pulses in a gas-filled hollow waveguide using synthesized few-cycle two-color laser waveforms. The waveform is a superposition of a fundamental and its second harmonic optimized such that highest harmonic yields are emitted from each atom. We then optimize the gas pressure and the length and radius of the waveguide such that bright coherent high-order harmonics with angular divergence smaller than 1 mrad are generated, for photon energy from the extreme ultraviolet to soft X-rays. By selecting a proper spectral range enhanced isolated attosecond pulses are generated. Wemore » study how dynamic phase matching caused by the interplay among waveguide mode, neutral atomic dispersion, and plasma effect is achieved at the optimal macroscopic conditions, by performing time-frequency analysis and by analyzing the evolution of the driving laser’s electric field during the propagation. Our results, when combined with the on-going push of high-repetition-rate lasers (sub- to few MHz’s) may eventually lead to the generation of high-flux, low-divergence soft X-ray tabletop isolated attosecond pulses for applications.« less

Thin film beam splitter multiple short pulse generation for enhanced Ni-like Ag x-ray laser emission.

PubMed

Cojocaru, Gabriel V; Ungureanu, Razvan G; Banici, Romeo A; Ursescu, Daniel; Delmas, Olivier; Pittman, Moana; Guilbaud, Olivier; Kazamias, Sophie; Cassou, Kevin; Demailly, Julien; Neveu, Olivier; Baynard, Elsa; Ros, David

2014-04-15

An alternative, novel multiple pulse generation scheme was implemented directly after the optical compressor output of an x-ray pump laser. The new method uses a polarization sensitive thin film beam splitter and a half-wavelength wave plate for tuning the energy ratio in the multiple short pulses. Based on this method, an extensive study was made of the running parameters for a grazing incidence pumped silver x-ray laser (XRL) pumped with a long pulse of 145 mJ in 6 ns at 532 nm and up to 1.45 J in few picoseconds at 810 nm. Fivefold enhancement in the emission of the silver XRL was demonstrated using the new pump method.

Precision machining of pig intestine using ultrafast laser pulses

NASA Astrophysics Data System (ADS)

Beck, Rainer J.; Góra, Wojciech S.; Carter, Richard M.; Gunadi, Sonny; Jayne, David; Hand, Duncan P.; Shephard, Jonathan D.

2015-07-01

Endoluminal surgery for the treatment of early stage colorectal cancer is typically based on electrocautery tools which imply restrictions on precision and the risk of harm through collateral thermal damage to the healthy tissue. As a potential alternative to mitigate these drawbacks we present laser machining of pig intestine by means of picosecond laser pulses. The high intensities of an ultrafast laser enable nonlinear absorption processes and a predominantly nonthermal ablation regime. Laser ablation results of square cavities with comparable thickness to early stage colorectal cancers are presented for a wavelength of 1030 nm using an industrial picosecond laser. The corresponding histology sections exhibit only minimal collateral damage to the surrounding tissue. The depth of the ablation can be controlled precisely by means of the pulse energy. Overall, the application of ultrafast lasers to ablate pig intestine enables significantly improved precision and reduced thermal damage to the surrounding tissue compared to conventional techniques.

Specific features of thermocouple calorimeter application for measurements of pulsed X-ray emission from plasma

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

Gavrilov, V. V.; Fasakhov, I. K.

2012-01-15

It is shown that the accuracy of time-integrated measurements of pulsed X-ray emission from hot plasma with calibrated thermocouple calorimeters is mainly determined by two factors. The first and the most important factor is heating of the filter by the absorbed X-rays; as a result, the calorimeter measures the thermal radiation of the filter, which causes appreciable distortion of the temporal profile and amplitude of the recorded signal. The second factor is the dependence of the effective depth of X-ray absorption in the dielectric that covers the entrance window of the calorimeter on the energy of X-ray photons, i.e., onmore » the recorded radiation spectrum. The results of model calculations of the calorimeter signal are compared with the experimental data.« less

Correlations in Scattered X-Ray Laser Pulses Reveal Nanoscale Structural Features of Viruses

DOE PAGES

Kurta, Ruslan P.; Donatelli, Jeffrey J.; Yoon, Chun Hong; ...

2017-10-12

We use extremely bright and ultrashort pulses from an x-ray free-electron laser (XFEL) to measure correlations in x rays scattered from individual bioparticles. This allows us to go beyond the traditional crystallography and single-particle imaging approaches for structure investigations. We employ angular correlations to recover the three-dimensional (3D) structure of nanoscale viruses from x-ray diffraction data measured at the Linac Coherent Light Source. Correlations provide us with a comprehensive structural fingerprint of a 3D virus, which we use both for model-based and ab initio structure recovery. The analyses reveal a clear indication that the structure of the viruses deviates frommore » the expected perfect icosahedral symmetry. Lastly, our results anticipate exciting opportunities for XFEL studies of the structure and dynamics of nanoscale objects by means of angular correlations.« less

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

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

Simultaneous, single-pulse, synchrotron x-ray imaging and diffraction under gas gun loading

DOE PAGES

Fan, D.; Huang, J. W.; Zeng, X. L.; ...

2016-05-23

We develop a mini gas gun system for simultaneous, single-pulse, x-ray diffraction and imaging under high strain-rate loading at the beamline 32-ID of the Advanced Photon Source. In order to increase the reciprocal space covered by a small-area detector, a conventional target chamber is split into two chambers: a narrowed measurement chamber and a relief chamber. The gas gun impact is synchronized with synchrotron x-ray pulses and high-speed cameras. Depending on a camera’s capability, multiframe imaging and diffraction can be achieved. The proof-of-principle experiments are performed on single-crystal sapphire. The diffraction spots and images during impact are analyzed to quantifymore » lattice deformation and fracture; diffraction peak broadening is largely caused by fracture-induced strain inhomogeneity. Finally, our results demonstrate the potential of such multiscale measurements for revealing and understanding high strain-rate phenomena at dynamic extremes.« less

Simultaneous, single-pulse, synchrotron x-ray imaging and diffraction under gas gun loading

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

Fan, D.; Luo, S. N., E-mail: sluo@pims.ac.cn; Key Laboratory of Advanced Technologies of Materials, Ministry of Education, Southwest Jiaotong University, Chengdu, Sichuan 610031

We develop a mini gas gun system for simultaneous, single-pulse, x-ray diffraction and imaging under high strain-rate loading at the beamline 32-ID of the Advanced Photon Source. In order to increase the reciprocal space covered by a small-area detector, a conventional target chamber is split into two chambers: a narrowed measurement chamber and a relief chamber. The gas gun impact is synchronized with synchrotron x-ray pulses and high-speed cameras. Depending on a camera’s capability, multiframe imaging and diffraction can be achieved. The proof-of-principle experiments are performed on single-crystal sapphire. The diffraction spots and images during impact are analyzed to quantifymore » lattice deformation and fracture; fracture is dominated by splitting cracks followed by wing cracks, and diffraction peaks are broadened likely due to mosaic spread. Our results demonstrate the potential of such multiscale measurements for studying high strain-rate phenomena at dynamic extremes.« less

Simultaneous, single-pulse, synchrotron x-ray imaging and diffraction under gas gun loading

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

Fan, D.; Huang, J. W.; Zeng, X. L.

We develop a mini gas gun system for simultaneous, single-pulse, x-ray diffraction and imaging under high strain-rate loading at the beamline 32-ID of the Advanced Photon Source. In order to increase the reciprocal space covered by a small-area detector, a conventional target chamber is split into two chambers: a narrowed measurement chamber and a relief chamber. The gas gun impact is synchronized with synchrotron x-ray pulses and high-speed cameras. Depending on a camera’s capability, multiframe imaging and diffraction can be achieved. The proof-of-principle experiments are performed on single-crystal sapphire. The diffraction spots and images during impact are analyzed to quantifymore » lattice deformation and fracture; diffraction peak broadening is largely caused by fracture-induced strain inhomogeneity. Finally, our results demonstrate the potential of such multiscale measurements for revealing and understanding high strain-rate phenomena at dynamic extremes.« less

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 electron dynamics in phenylalanine initiated by attosecond pulses.

PubMed

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

2014-10-17

In the past decade, attosecond technology has opened up the investigation of ultrafast electronic processes in atoms, simple molecules, and solids. Here, we report the application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine and the subsequent detection of ultrafast dynamics on a sub-4.5-femtosecond temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules represents a crucial step forward in attosecond science, which is progressively moving toward the investigation of more and more complex systems. Copyright © 2014, American Association for the Advancement of Science.

The UHURU X-ray instrument.

NASA Technical Reports Server (NTRS)

Jagoda, N.; Austin, G.; Mickiewicz, S.; Goddard, R.

1972-01-01

On Dec. 12, 1970, the UHURU X-ray observatory was launched into equatorial orbit with the prime mission of conducting an all-sky survey of astronomical X-ray sources with intensities of 0.00005 Sco-X1 or greater. The X-ray detection system contains 12 gas-filled proportional counters, 6 behind each collimator. The aspect system is discussed together with the structure, the pulse height analyzer, the command system, the calibration system, and the power distribution system. Pulse shape discrimination circuits used on UHURU use the same technique that was used on the system originally developed for large area proportional counters described by Gorenstein and Mickiewicz (1968).

Ultrafast absorption of intense x rays by nitrogen molecules

NASA Astrophysics Data System (ADS)

Buth, Christian; Liu, Ji-Cai; Chen, Mau Hsiung; Cryan, James P.; Fang, Li; Glownia, James M.; Hoener, Matthias; Coffee, Ryan N.; Berrah, Nora

2012-06-01

We devise a theoretical description for the response of nitrogen molecules (N2) to ultrashort and intense x rays from the free electron laser Linac Coherent Light Source (LCLS). We set out from a rate-equation description for the x-ray absorption by a nitrogen atom. The equations are formulated using all one-x-ray-photon absorption cross sections and the Auger and radiative decay widths of multiply-ionized nitrogen atoms. Cross sections are obtained with a one-electron theory and decay widths are determined from ab initio computations using the Dirac-Hartree-Slater (DHS) method. We also calculate all binding and transition energies of nitrogen atoms in all charge states with the DHS method as the difference of two self-consistent field (SCF) calculations (ΔSCF method). To describe the interaction with N2, a detailed investigation of intense x-ray-induced ionization and molecular fragmentation are carried out. As a figure of merit, we calculate ion yields and the average charge state measured in recent experiments at the LCLS. We use a series of phenomenological models of increasing sophistication to unravel the mechanisms of the interaction of x rays with N2: a single atom, a symmetric-sharing model, and a fragmentation-matrix model are developed. The role of the formation and decay of single and double core holes, the metastable states of N_2^{2+}, and molecular fragmentation are explained.

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.

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, Arthur; Trebino, Rick P.

1999-08-10

Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques.

Short Pulse High Brightness X-ray Production with the PLEIADES Thomson Scattering Source

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

Anderson, S G; Barty, C P J; Betts, S M

2003-07-01

We describe PLEIADES, a compact, tunable, high-brightness, ultra-short pulse, Thomson x-ray source. The peak brightness of the source is expected to exceed 10{sup 20} photons/s/0.1% bandwidth/mm{sup 2}/mrad{sup 2}. Initial results are reported and compared to theoretical calculations.

High-rate x-ray spectroscopy in mammography with a CdTe detector: a digital pulse processing approach.

PubMed

Abbene, L; Gerardi, G; Principato, F; Del Sordo, S; Ienzi, R; Raso, G

2010-12-01

Direct measurement of mammographic x-ray spectra under clinical conditions is a difficult task due to the high fluence rate of the x-ray beams as well as the limits in the development of high resolution detection systems in a high counting rate environment. In this work we present a detection system, based on a CdTe detector and an innovative digital pulse processing (DPP) system, for high-rate x-ray spectroscopy in mammography. The DPP system performs a digital pile-up inspection and a digital pulse height analysis of the detector signals, digitized through a 14-bit, 100 MHz digitizer, for x-ray spectroscopy even at high photon counting rates. We investigated on the response of the digital detection system both at low (150 cps) and at high photon counting rates (up to 500 kcps) by using monoenergetic x-ray sources and a nonclinical molybdenum anode x-ray tube. Clinical molybdenum x-ray spectrum measurements were also performed by using a pinhole collimator and a custom alignment device. The detection system shows excellent performance up to 512 kcps with an energy resolution of 4.08% FWHM at 22.1 keV. Despite the high photon counting rate (up to 453 kcps), the molybdenum x-ray spectra, measured under clinical conditions, are characterized by a low number of pile-up events. The agreement between the attenuation curves and the half value layer values, obtained from the measured spectra, simulated spectra, and from the exposure values directly measured with an ionization chamber, also shows the accuracy of the measurements. These results make the proposed detection system a very attractive tool for both laboratory research and advanced quality controls in mammography.

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

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

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

2016-01-01

This report will describe our recent studies of transition metal complex structural dynamics on the fs and ps time scales using an X-ray free electron laser source, Linac Coherent Light Source (LCLS). Ultrafast XANES spectra at the Ni K-edge of nickel(II) tetramesitylporphyrin (NiTMP) were successfully measured for optically excited state at a timescale from 100 fs to 50 ps, providing insight into its sub-ps electronic and structural relaxation processes. Importantly, a transient reduced state Ni(I) (π, 3dx2-y2) electronic state is captured through the interpretation of a short-lived excited state absorption on the low-energy shoulder of the edge, which is aidedmore » by the computation of X-ray transitions for postulated excited electronic states. The observed and computed inner shell to valence orbital transition energies demonstrate and quantify the influence of electronic configuration on specific metal orbital energies. A strong influence of the valence orbital occupation on the inner shell orbital energies indicates that one should not use the transition energy from 1s to other orbitals to draw conclusions about the d-orbital energies. For photocatalysis, a transient electronic configuration could influence d-orbital energies up to a few eV and any attempt to steer the reaction pathway should account for this to ensure that external energies can be used optimally in driving desirable processes. NiTMP structural evolution and the influence of the porphyrin macrocycle conformation on relaxation kinetics can be likewise inferred from this study.« less

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.

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

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, A.; Trebino, R.P.

1999-08-10

Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques. 2 figs.

The high-energy pulsed X-ray spectrum of Hercules X-1 as observed with OSO 8

NASA Technical Reports Server (NTRS)

Maurer, G. S.; Dennis, B. R.; Coe, M. J.; Crannell, C. J.; Dolan, J. F.; Frost, K. J.; Orwig, L. E.; Cutler, E. P.

1979-01-01

Hercules X-1 was observed from August 30 to September 10, 1977, by using the high-energy X-ray scintillation spectrometer on board the OSO 8 satellite. The observation, during which the source was monitored continually for nearly an entire ON-state, covered the energy range from 16 to 280 keV. Pulsed-flux measurements as a function of binary orbit and binary phase are presented for energies between 16 and 98 keV. The pulsed flux between 16 and 33 keV exhibited a sharp decrease following the fourth binary orbit and was consistent with zero pulsed flux thereafter. Only weak evidence was found for temporal variation in the pulsed flux between 33 and 98 keV. The pulsed spectrum has been fitted with a power law, a thermal spectrum without features, and a thermal spectrum with a superposed Gaussian centered at 55 keV. The latter fit has the smallest value of chi-square per degree of freedom, and the resulting integrated line intensity is approximately 0.0015 photon/sec per sq cm for a width of 3.1 (+9.1, -2.6) keV. This result, while of low statistical significance, agrees with the value observed by Truemper (1978) during the same ON-state.

Simple Method to Generate Terawatt-Attosecond X-Ray Free-Electron-Laser Pulses.

PubMed

Prat, Eduard; Reiche, Sven

2015-06-19

X-ray free-electron lasers (XFELs) are cutting-edge research tools that produce almost fully coherent radiation with high power and short-pulse length with applications in multiple science fields. There is a strong demand to achieve even shorter pulses and higher radiation powers than the ones obtained at state-of-the-art XFEL facilities. In this context we propose a novel method to generate terawatt-attosecond XFEL pulses, where an XFEL pulse is pushed through several short good-beam regions of the electron bunch. In addition to the elements of conventional XFEL facilities, the method uses only a multiple-slotted foil and small electron delays between undulator sections. Our scheme is thus simple, compact, and easy to implement both in already operating as well as future XFEL projects. We present numerical simulations that confirm the feasibility and validity of our proposal.

Direct micromachining of quartz glass plates using pulsed laser plasma soft x-rays

NASA Astrophysics Data System (ADS)

Makimura, Tetsuya; Miyamoto, Hisao; Kenmotsu, Youichi; Murakami, Kouichi; Niino, Hiroyuki

2005-03-01

We have investigated direct micromachining of quartz glass, using pulsed laser plasma soft x-rays (LPSXs) having a potential capability of nanomachining because the diffraction limit is ˜10nm. The LPSX's were generated by irradiation of a Ta target with 532nm laser light from a conventional Q switched Nd :YAG laser at 700mJ/pulse. In order to achieve a sufficient power density of LPSX's beyond the ablation threshold, we developed an ellipsoidal mirror to obtain efficient focusing of LPSXs at around 10nm. It was found that quartz glass plates are smoothly ablated at 45nm/shot using the focused and pulsed LPSX's.

Nonlinear X-Ray and Auger Spectroscopy at X-Ray Free-Electron Laser Sources

NASA Astrophysics Data System (ADS)

Rohringer, Nina

2015-05-01

X-ray free-electron lasers (XFELs) open the pathway to transfer non-linear spectroscopic techniques to the x-ray domain. A promising all x-ray pump probe technique is based on coherent stimulated electronic x-ray Raman scattering, which was recently demonstrated in atomic neon. By tuning the XFEL pulse to core-excited resonances, a few seed photons in the spectral tail of the XFEL pulse drive an avalanche of resonant inelastic x-ray scattering events, resulting in exponential amplification of the scattering signal by of 6-7 orders of magnitude. Analysis of the line profile of the emitted radiation permits to demonstrate the cross over from amplified spontaneous emission to coherent stimulated resonance scattering. In combination with statistical covariance mapping, a high-resolution spectrum of the resonant inelastic scattering process can be obtained, opening the path to coherent stimulated x-ray Raman spectroscopy. An extension of these ideas to molecules and a realistic feasibility study of stimulated electronic x-ray Raman scattering in CO will be presented. Challenges to realizing stimulated electronic x-ray Raman scattering at present-day XFEL sources will be discussed, corroborated by results of a recent experiment at the LCLS XFEL. Due to the small gain cross section in molecular targets, other nonlinear spectroscopic techniques such as nonlinear Auger spectroscopy could become a powerful alternative. Theory predictions of a novel pump probe technique based on resonant nonlinear Auger spectroscopic will be discussed and the method will be compared to stimulated x-ray Raman spectroscopy.

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.

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

Table-top soft x-ray microscope using laser-induced plasma from a pulsed gas jet.

PubMed

Müller, Matthias; Mey, Tobias; Niemeyer, Jürgen; Mann, Klaus

2014-09-22

An extremely compact soft x-ray microscope operating in the "water window" region at the wavelength λ = 2.88 nm is presented, making use of a long-term stable and nearly debris-free laser-induced plasma from a pulsed nitrogen gas jet target. The well characterized soft x-ray radiation is focused by an ellipsoidal grazing incidence condenser mirror. Imaging of a sample onto a CCD camera is achieved with a Fresnel zone plate using magnifications up to 500x. The spatial resolution of the recorded microscopic images is about 100 nm as demonstrated for a Siemens star test pattern.

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.

Anti-correlation between X-ray luminosity and pulsed fraction in the Small Magellanic Cloud pulsar SXP 1323

NASA Astrophysics Data System (ADS)

Yang, Jun; Zezas, Andreas; Coe, Malcolm J.; Drake, Jeremy J.; Hong, JaeSub; Laycock, Silas G. T.; Wik, Daniel R.

2018-05-01

We report the evidence for the anti-correlation between pulsed fraction (PF) and luminosity of the X-ray pulsar SXP 1323, found for the first time in a luminosity range 1035-1037 erg s-1 from observations spanning 15 years. The phenomenon of a decrease in X-ray PF when the source flux increases has been observed in our pipeline analysis of other X-ray pulsars in the Small Magellanic Cloud (SMC). It is expected that the luminosity under a certain value decreases as the PF decreases due to the propeller effect. Above the propeller region, an anti-correlation between the PF and flux might occur either as a result of an increase in the un-pulsed component of the total emission or a decrease of the pulsed component. Additional modes of accretion may also be possible, such as spherical accretion and a change in emission geometry. At higher mass accretion rates, the accretion disk could also extend closer to the neutron star (NS) surface, where a reduced inner radius leads to hotter inner disk emission. These modes of plasma accretion may affect the change in the beam configuration to fan-beam dominant emission.

Terahertz pulsed imaging for the monitoring of dental caries: a comparison with x-ray imaging

NASA Astrophysics Data System (ADS)

Karagoz, Burcu; Kamburoglu, Kıvanc; Altan, Hakan

2017-07-01

Dental caries in sliced samples are investigated using terahertz pulsed imaging. Frequency domain terahertz response of these structures consistent with X-ray imaging results show the potential of this technique in the detection of early caries.

High repetition rate compact source of nanosecond pulses of 5-100 keV x-ray photons

NASA Astrophysics Data System (ADS)

Khacef, A.; Viladrosa, R.; Cachoncinlle, C.; Robert, E.; Pouvesle, J. M.

1997-06-01

A powerful, compact, and repetitive flash x-ray system based on a cable transformer technology powered by ceramic capacitors in a Blumlein-like configuration has been developed. Open circuit voltages in excess of 100 kV can be achieved while commutation occurs at low voltage (<20 kV). The x-ray emission from a low impedance x-ray diode with a hollow cathode configuration was observed under a wide range of experimental conditions. The critical parameters limiting the flash x-ray performances are mainly the pressure in the x-ray diode and the anode-cathode space. This true table top device is able to produce doses up to 1 R per shot, measured at the output window, of x-rays between 5 and 100 keV. The pulse widths were about 20 ns and the maximum repetition rate was about 60 Hz. Operation is possible in air or in other gases (He, Ne, Ar, Kr, Xe, H2, N2) at pressures varying from 10-3 mbar for xenon to about 1 mbar for helium.

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.

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

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.

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.

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.

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 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.

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.

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.

Hidden explosives detector employing pulsed neutron and x-ray interrogation

DOEpatents

Schultz, F.J.; Caldwell, J.T.

1993-04-06

Methods and systems for the detection of small amounts of modern, highly-explosive nitrogen-based explosives, such as plastic explosives, hidden in airline baggage. Several techniques are employed either individually or combined in a hybrid system. One technique employed in combination is X-ray imaging. Another technique is interrogation with a pulsed neutron source in a two-phase mode of operation to image both nitrogen and oxygen densities. Another technique employed in combination is neutron interrogation to form a hydrogen density image or three-dimensional map. In addition, deliberately-placed neutron-absorbing materials can be detected.

Hidden explosives detector employing pulsed neutron and x-ray interrogation

DOEpatents

Schultz, Frederick J.; Caldwell, John T.

1993-01-01

Methods and systems for the detection of small amounts of modern, highly-explosive nitrogen-based explosives, such as plastic explosives, hidden in airline baggage. Several techniques are employed either individually or combined in a hybrid system. One technique employed in combination is X-ray imaging. Another technique is interrogation with a pulsed neutron source in a two-phase mode of operation to image both nitrogen and oxygen densities. Another technique employed in combination is neutron interrogation to form a hydrogen density image or three-dimensional map. In addition, deliberately-placed neutron-absorbing materials can be detected.

Time of flight emission spectroscopy of laser produced nickel plasma: Short-pulse and ultrafast excitations

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

Smijesh, N.; Chandrasekharan, K.; Joshi, Jagdish C.

2014-07-07

We report the experimental investigation and comparison of the temporal features of short-pulse (7 ns) and ultrafast (100 fs) laser produced plasmas generated from a solid nickel target, expanding into a nitrogen background. When the ambient pressure is varied in a large range of 10⁻⁶Torr to 10²Torr, the plume intensity is found to increase rapidly as the pressure crosses 1 Torr. Time of flight (TOF) spectroscopy of emission from neutral nickel (Ni I) at 361.9 nm (3d⁹(²D) 4p → 3d⁹(²D) 4s transition) reveals two peaks (fast and slow species) in short-pulse excitation and a single peak in ultrafast excitation. Themore » fast and slow peaks represent recombined neutrals and un-ionized neutrals, respectively. TOF emission from singly ionized nickel (Ni II) studied using the 428.5 nm (3p⁶3d⁸(³P) 4s→ 3p⁶3d⁹ 4s) transition shows only a single peak for either excitation. Velocities of the neutral and ionic species are determined from TOF measurements carried out at different positions (i.e., at distances of 2 mm and 4 mm, respectively, from the target surface) on the plume axis. Measured velocities indicate acceleration of neutrals and ions, which is caused by the Coulomb pull of the electrons enveloping the plume front in the case of ultrafast excitation. Both Coulomb pull and laser-plasma interaction contribute to the acceleration in the case of short-pulse excitation. These investigations provide new information on the pressure dependent temporal behavior of nickel plasmas produced by short-pulse and ultrafast laser pulses, which have potential uses in applications such as pulsed laser deposition and laser-induced nanoparticle generation.« less

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

NASA Astrophysics Data System (ADS)

Qi, Y.; Liu, S.; Lindenberg, A. M.; Rappe, A. M.

2018-01-01

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈1011 K /s ) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO3 occurring on few picosecond time scales. We explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on a ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO3 and BaTiO3 . Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.

In situ x-ray surface diffraction chamber for pulsed laser ablation film growth studies

NASA Astrophysics Data System (ADS)

Tischler, J. Z.; Eres, G.; Lowndes, D. H.; Larson, B. C.; Yoon, M.; Chiang, T.-C.; Zschack, Paul

2000-06-01

Pulsed laser deposition is highly successful for growing complex films such as oxides for substrate buffer layers and HiTc oxide superconductors. A surface diffraction chamber has been constructed to study fundamental aspects of non-equilibrium film growth using pulsed laser deposition. Due to the pulsed nature of the ablating laser, the deposited atoms arrive on the substrate in short sub-millisecond pulses. Thus monitoring the surface x-ray diffraction following individual laser pulses (with resolution down to ˜1 ms) provides direct information on surface kinetics and the aggregation process during film growth. The chamber design, based upon a 2+2 surface diffraction geometry with the modifications necessary for laser ablation, is discussed, and initial measurements on homo-epitaxial growth of SrTiO3 are presented.

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.

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

Modelling multi-pulse population dynamics from ultrafast spectroscopy.

PubMed

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

2011-03-21

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

Modelling Multi-Pulse Population Dynamics from Ultrafast Spectroscopy

PubMed Central

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

2011-01-01

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

Vela X-1 pulse timing. II - Variations in pulse frequency

NASA Technical Reports Server (NTRS)

Deeter, J. E.; Boynton, P. E.; Lamb, F. K.; Zylstra, G.

1989-01-01

The pulsed X-ray emission of Vela X-1 during May 1978 and December-January 1978-1979 is investigated analytically on the basis of published satellite observations. The data are compiled in tables and graphs and discussed in detail, with reference to data for the entire 1975-1982 period. Variations in pulse frequency are identified on time scales from 2 to 2600 days; the lower nine octaves are characterized as white noise (or random walk in pulse frequency), while the longer-period variations are attributed to changes in neutron-star rotation rates.

Experimental strategies for imaging bioparticles with femtosecond hard X-ray pulses

PubMed Central

Okamoto, Kenta; Bielecki, Johan; Maia, Filipe R. N. C.; Mühlig, Kerstin; Seibert, M. Marvin; Hantke, Max F.; Benner, W. Henry; Svenda, Martin; Ekeberg, Tomas; Loh, N. Duane; Pietrini, Alberto; Zani, Alessandro; Rath, Asawari D.; Westphal, Daniel; Kirian, Richard A.; Awel, Salah; Wiedorn, Max O.; van der Schot, Gijs; Carlsson, Gunilla H.; Hasse, Dirk; Sellberg, Jonas A.; Barty, Anton; Andreasson, Jakob; Boutet, Sébastien; Williams, Garth; Koglin, Jason; Hajdu, Janos; Larsson, Daniel S. D.

2017-01-01

This study explores the capabilities of the Coherent X-ray Imaging Instrument at the Linac Coherent Light Source to image small biological samples. The weak signal from small samples puts a significant demand on the experiment. Aerosolized Omono River virus particles of ∼40 nm in diameter were injected into the submicrometre X-ray focus at a reduced pressure. Diffraction patterns were recorded on two area detectors. The statistical nature of the measurements from many individual particles provided information about the intensity profile of the X-ray beam, phase variations in the wavefront and the size distribution of the injected particles. The results point to a wider than expected size distribution (from ∼35 to ∼300 nm in diameter). This is likely to be owing to nonvolatile contaminants from larger droplets during aerosolization and droplet evaporation. The results suggest that the concentration of nonvolatile contaminants and the ratio between the volumes of the initial droplet and the sample particles is critical in such studies. The maximum beam intensity in the focus was found to be 1.9 × 1012 photons per µm2 per pulse. The full-width of the focus at half-maximum was estimated to be 500 nm (assuming 20% beamline transmission), and this width is larger than expected. Under these conditions, the diffraction signal from a sample-sized particle remained above the average background to a resolution of 4.25 nm. The results suggest that reducing the size of the initial droplets during aerosolization is necessary to bring small particles into the scope of detailed structural studies with X-ray lasers. PMID:28512572

Experimental strategies for imaging bioparticles with femtosecond hard X-ray pulses

DOE PAGES

Daurer, Benedikt J.; Okamoto, Kenta; Bielecki, Johan; ...

2017-04-07

This study explores the capabilities of the Coherent X-ray Imaging Instrument at the Linac Coherent Light Source to image small biological samples. The weak signal from small samples puts a significant demand on the experiment. AerosolizedOmono River virusparticles of ~40 nm in diameter were injected into the submicrometre X-ray focus at a reduced pressure. Diffraction patterns were recorded on two area detectors. The statistical nature of the measurements from many individual particles provided information about the intensity profile of the X-ray beam, phase variations in the wavefront and the size distribution of the injected particles. The results point to amore » wider than expected size distribution (from ~35 to ~300 nm in diameter). This is likely to be owing to nonvolatile contaminants from larger droplets during aerosolization and droplet evaporation. The results suggest that the concentration of nonvolatile contaminants and the ratio between the volumes of the initial droplet and the sample particles is critical in such studies. The maximum beam intensity in the focus was found to be 1.9 × 10 12photons per µm 2per pulse. The full-width of the focus at half-maximum was estimated to be 500 nm (assuming 20% beamline transmission), and this width is larger than expected. Under these conditions, the diffraction signal from a sample-sized particle remained above the average background to a resolution of 4.25 nm. Finally, the results suggest that reducing the size of the initial droplets during aerosolization is necessary to bring small particles into the scope of detailed structural studies with X-ray lasers.« less

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

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

Single- and double-core-hole ion emission spectroscopy of transient neon plasmas produced by ultraintense x-ray laser pulses

NASA Astrophysics Data System (ADS)

Gao, Cheng; Zeng, Jiaolong; Yuan, Jianmin

2016-02-01

Single-core-hole (SCH) and double-core-hole (DCH) spectroscopy is investigated systematically for neon gas in the interaction with ultraintense x-ray pulses with photon energy from 937 eV to 2000 eV. A time-dependent rate equation, implemented in detailed level accounting approximation, is utilized to study the dynamical evolution of the level population and emission properties of the laser-produced highly transient plasmas. The plasma-density effects on level populations and charge-state distribution are demonstrated with an x-ray photon energy of 2000 eV. It is shown that atomic number density of relevant experiment is about 1 × 1018 cm-3, which is comparable to a recent experiment. At this density, we systematically investigate the emissivity of the transient neon plasmas. For laser photon energy in the range 937-1360 eV, resonant absorptions (RA) of 1s\\to {np} (n≥slant 2) transitions play important roles in time evolution of the population and DCH emission spectroscopy. The RA effects are illustrated in detail for an x-ray pulse of 944 eV photon energy, which creates the 1s\\to 2p RA from the SCH states (1s2{s}22{p}4, 1s2s2p5, and 1s2p6) of Ne3+. After averaging over the space and time distribution of x-ray pulse, DCH emission spectroscopy is studied at x-ray photon energies of 937, 944, 955, 968, 980, and 990 eV, where there exist 1s\\to 2p resonances from SCH states of Ne2+-Ne7+. The processes with producing DCH states are discussed. For x-ray photon energy larger than 1360 eV, no RA exist and transient plasmas show different features in the DCH spectroscopy.

Ultrafast pulsed laser utilizing broad bandwidth laser glass

DOEpatents

Payne, Stephen A.; Hayden, Joseph S.

1997-01-01

An ultrafast laser uses a Nd-doped phosphate laser glass characterized by a particularly broad emission bandwidth to generate the shortest possible output pulses. The laser glass is composed primarily of P.sub.2 O.sub.5, Al.sub.2 O.sub.3 and MgO, and possesses physical and thermal properties that are compatible with standard melting and manufacturing methods. The broad bandwidth laser glass can be used in modelocked oscillators as well as in amplifier modules.

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

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.

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

Generation of double pulses at the Shanghai soft X-ray free electron laser facility

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

Wang, Zhen; Feng, Chao; Gu, Qiang

2017-01-28

In this paper, we present the promise of a new method generating double electron pulses with the picosecond-scale pulse length and the tunable interpulse spacing at several picoseconds, which has been witnessed an impressive potential of application in pump-probe techniques, two-color X-ray free electron laser (FEL), high-gradient witness bunch acceleration in a plasma, etc. Three-dimensional simulations are carried out to analyze the dynamic of the electron beam in the linear accelerator. Some comparisons have been made between the new method and the existing ways as well.

Pulse Repetition Frequency Effects In A High Average Power X-Ray Preionised Excimer Laser

NASA Astrophysics Data System (ADS)

Fontaine, Bernard L.; Forestier, Bernard M.; Delaporte, Philippe C.; Canarelli, Patrick

1989-10-01

Experimental study of waves damping in a high repetition rate excimer laser is undertaken. Excitation of laser active medium in a subsonic loop is achieved by means of a classical discharge, through transfer capacitors. The discharge stability is controlled by a wire ion plasma (w.i.p.) X-rays gun. The strong acoustic waves induced by the active medium excitation may lead to a decrease, at high PRF, of the energy per pulse. First results of the influence of a damping of induced density perturbations between two successive pulses are presented.

Ultrafast synchrotron X-ray imaging studies of microstructure fragmentation in solidification under ultrasound

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

Wang, Bing; Tan, Dongyue; Lee, Tung Lik

Ultrasound processing of metal alloys is an environmental friendly and promising green technology for liquid metal degassing and microstructural refinement. However many fundamental issues in this field are still not fully understood, because of the difficulties in direct observation of the dynamic behaviours caused by ultrasound inside liquid metal and semisolid metals during the solidification processes. In this paper, we report a systematic study using the ultrafast synchrotron X-ray imaging (up to 271,554 frame per second) technique available at the Advanced Photon Source, USA and Diamond Light Source, UK to investigate the dynamic interactions between the ultrasonic bubbles/acoustic flow andmore » the solidifying phases in a Bi-8%Zn alloy. The experimental results were complimented by numerical modelling. The chaotic bubble implosion and dynamic bubble oscillations were revealed in-situ for the first time in liquid metal and semisolid metal. The fragmentation of the solidifying Zn phases and breaking up of the liquid-solid interface by ultrasonic bubbles and enhanced acoustic flow were clearly demonstrated and agreed very well with the theoretical calculations. The research provides unambiguous experimental evidence and robust theoretical interpretation in elucidating the dominant mechanisms of microstructure fragmentation and refinement in solidification under ultrasound.« less

Ultrafast synchrotron X-ray imaging studies of microstructure fragmentation in solidification under ultrasound

DOE PAGES

Wang, Bing; Tan, Dongyue; Lee, Tung Lik; ...

2017-11-03

Ultrasound processing of metal alloys is an environmental friendly and promising green technology for liquid metal degassing and microstructural refinement. However many fundamental issues in this field are still not fully understood, because of the difficulties in direct observation of the dynamic behaviours caused by ultrasound inside liquid metal and semisolid metals during the solidification processes. In this paper, we report a systematic study using the ultrafast synchrotron X-ray imaging (up to 271,554 frame per second) technique available at the Advanced Photon Source, USA and Diamond Light Source, UK to investigate the dynamic interactions between the ultrasonic bubbles/acoustic flow andmore » the solidifying phases in a Bi-8%Zn alloy. The experimental results were complimented by numerical modelling. The chaotic bubble implosion and dynamic bubble oscillations were revealed in-situ for the first time in liquid metal and semisolid metal. The fragmentation of the solidifying Zn phases and breaking up of the liquid-solid interface by ultrasonic bubbles and enhanced acoustic flow were clearly demonstrated and agreed very well with the theoretical calculations. The research provides unambiguous experimental evidence and robust theoretical interpretation in elucidating the dominant mechanisms of microstructure fragmentation and refinement in solidification under ultrasound.« less

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

Polarization and Thickness Dependent Absorption Properties of Black Phosphorus: New Saturable Absorber for Ultrafast Pulse Generation

PubMed Central

Li, Diao; Jussila, Henri; Karvonen, Lasse; Ye, Guojun; Lipsanen, Harri; Chen, Xianhui; Sun, Zhipei

2015-01-01

Black phosphorus (BP) has recently been rediscovered as a new and interesting two-dimensional material due to its unique electronic and optical properties. Here, we study the linear and nonlinear optical properties of BP flakes. We observe that both the linear and nonlinear optical properties are anisotropic and can be tuned by the film thickness in BP, completely different from other typical two-dimensional layered materials (e.g., graphene and the most studied transition metal dichalcogenides). We then use the nonlinear optical properties of BP for ultrafast (pulse duration down to ~786 fs in mode-locking) and large-energy (pulse energy up to >18 nJ in Q-switching) pulse generation in fiber lasers at the near-infrared telecommunication band ~1.5 μm. We observe that the output of our BP based pulsed lasers is linearly polarized (with a degree-of-polarization ~98% in mode-locking, >99% in Q-switching, respectively) due to the anisotropic optical property of BP. Our results underscore the relatively large optical nonlinearity of BP with unique polarization and thickness dependence, and its potential for polarized optical pulse generation, paving the way to BP based nonlinear and ultrafast photonic applications (e.g., ultrafast all-optical polarization switches/modulators, frequency converters etc.). PMID:26514090

Apparatus for monitoring X-ray beam alignment

DOEpatents

Steinmeyer, Peter A.

1991-10-08

A self-contained, hand-held apparatus is provided for minitoring alignment of an X-ray beam in an instrument employing an X-ray source. The apparatus includes a transducer assembly containing a photoresistor for providing a range of electrical signals responsive to a range of X-ray beam intensities from the X-ray beam being aligned. A circuit, powered by a 7.5 VDC power supply and containing an audio frequency pulse generator whose frequency varies with the resistance of the photoresistor, is provided for generating a range of audible sounds. A portion of the audible range corresponds to low X-ray beam intensity. Another portion of the audible range corresponds to high X-ray beam intensity. The transducer assembly may include an a photoresistor, a thin layer of X-ray fluorescent material, and a filter layer transparent to X-rays but opaque to visible light. X-rays from the beam undergoing alignment penetrate the filter layer and excite the layer of fluorescent material. The light emitted from the fluorescent material alters the resistance of the photoresistor which is in the electrical circuit including the audio pulse generator and a speaker. In employing the apparatus, the X-ray beam is aligned to a complete alignment by adjusting the X-ray beam to produce an audible sound of the maximum frequency.

Apparatus for monitoring X-ray beam alignment

DOEpatents

Steinmeyer, P.A.

1991-10-08

A self-contained, hand-held apparatus is provided for monitoring alignment of an X-ray beam in an instrument employing an X-ray source. The apparatus includes a transducer assembly containing a photoresistor for providing a range of electrical signals responsive to a range of X-ray beam intensities from the X-ray beam being aligned. A circuit, powered by a 7.5 VDC power supply and containing an audio frequency pulse generator whose frequency varies with the resistance of the photoresistor, is provided for generating a range of audible sounds. A portion of the audible range corresponds to low X-ray beam intensity. Another portion of the audible range corresponds to high X-ray beam intensity. The transducer assembly may include an a photoresistor, a thin layer of X-ray fluorescent material, and a filter layer transparent to X-rays but opaque to visible light. X-rays from the beam undergoing alignment penetrate the filter layer and excite the layer of fluorescent material. The light emitted from the fluorescent material alters the resistance of the photoresistor which is in the electrical circuit including the audio pulse generator and a speaker. In employing the apparatus, the X-ray beam is aligned to a complete alignment by adjusting the X-ray beam to produce an audible sound of the maximum frequency. 2 figures.

Ultrafast pulsed laser utilizing broad bandwidth laser glass

DOEpatents

Payne, S.A.; Hayden, J.S.

1997-09-02

An ultrafast laser uses a Nd-doped phosphate laser glass characterized by a particularly broad emission bandwidth to generate the shortest possible output pulses. The laser glass is composed primarily of P{sub 2}O{sub 5}, Al{sub 2}O{sub 3} and MgO, and possesses physical and thermal properties that are compatible with standard melting and manufacturing methods. The broad bandwidth laser glass can be used in modelocked oscillators as well as in amplifier modules. 7 figs.

Performance verification and system integration tests of the pulse shape processor for the soft x-ray spectrometer onboard ASTRO-H

NASA Astrophysics Data System (ADS)

Takeda, Sawako; Tashiro, Makoto S.; Ishisaki, Yoshitaka; Tsujimoto, Masahiro; Seta, Hiromi; Shimoda, Yuya; Yamaguchi, Sunao; Uehara, Sho; Terada, Yukikatsu; Fujimoto, Ryuichi; Mitsuda, Kazuhisa

2014-07-01

The soft X-ray spectrometer (SXS) aboard ASTRO-H is equipped with dedicated digital signal processing units called pulse shape processors (PSPs). The X-ray microcalorimeter system SXS has 36 sensor pixels, which are operated at 50 mK to measure heat input of X-ray photons and realize an energy resolution of 7 eV FWHM in the range 0.3-12.0 keV. Front-end signal processing electronics are used to filter and amplify the electrical pulse output from the sensor and for analog-to-digital conversion. The digitized pulses from the 36 pixels are multiplexed and are sent to the PSP over low-voltage differential signaling lines. Each of two identical PSP units consists of an FPGA board, which assists the hardware logic, and two CPU boards, which assist the onboard software. The FPGA board triggers at every pixel event and stores the triggering information as a pulse waveform in the installed memory. The CPU boards read the event data to evaluate pulse heights by an optimal filtering algorithm. The evaluated X-ray photon data (including the pixel ID, energy, and arrival time information) are transferred to the satellite data recorder along with event quality information. The PSP units have been developed and tested with the engineering model (EM) and the flight model. Utilizing the EM PSP, we successfully verified the entire hardware system and the basic software design of the PSPs, including their communication capability and signal processing performance. In this paper, we show the key metrics of the EM test, such as accuracy and synchronicity of sampling clocks, event grading capability, and resultant energy resolution.

A laser driven pulsed X-ray backscatter technique for enhanced penetrative imaging.

PubMed

Deas, R M; Wilson, L A; Rusby, D; Alejo, A; Allott, R; Black, P P; Black, S E; Borghesi, M; Brenner, C M; Bryant, J; Clarke, R J; Collier, J C; Edwards, B; Foster, P; Greenhalgh, J; Hernandez-Gomez, C; Kar, S; Lockley, D; Moss, R M; Najmudin, Z; Pattathil, R; Symes, D; Whittle, M D; Wood, J C; McKenna, P; Neely, D

2015-01-01

X-ray backscatter imaging can be used for a wide range of imaging applications, in particular for industrial inspection and portal security. Currently, the application of this imaging technique to the detection of landmines is limited due to the surrounding sand or soil strongly attenuating the 10s to 100s of keV X-rays required for backscatter imaging. Here, we introduce a new approach involving a 140 MeV short-pulse (< 100 fs) electron beam generated by laser wakefield acceleration to probe the sample, which produces Bremsstrahlung X-rays within the sample enabling greater depths to be imaged. A variety of detector and scintillator configurations are examined, with the best time response seen from an absorptive coated BaF2 scintillator with a bandpass filter to remove the slow scintillation emission components. An X-ray backscatter image of an array of different density and atomic number items is demonstrated. The use of a compact laser wakefield accelerator to generate the electron source, combined with the rapid development of more compact, efficient and higher repetition rate high power laser systems will make this system feasible for applications in the field. Content includes material subject to Dstl (c) Crown copyright (2014). Licensed under the terms of the Open Government Licence except where otherwise stated. To view this licence, visit http://www.nationalarchives.gov.uk/doc/open-government-licence/version/3 or write to the Information Policy Team, The National Archives, Kew, London TW9 4DU, or email: psi@ nationalarchives.gsi.gov.uk.

Soft X-Ray Optics by Pulsed Laser Deposition

NASA Technical Reports Server (NTRS)

Fernandez, Felix E.

1996-01-01

Mo/Si and C/Co multilayers for soft x-ray optics were designed for spectral regions of interest in possible applications. Fabrication was effected by Pulsed Laser Deposition using Nd:YAG (355 nm) or excimer (248 nm) lasers in order to evaluate the suitability of this technique. Results for Mo/Si structures were not considered satisfactory due mainly to problems with particulate production and target surface modification during Si ablation. These problems may be alleviated by a two-wavelength approach, using separate lasers for each target. Results for C/Co multilayers are much more encouraging, since indication of good layering was observed for extremely thin layers. We expect to continue investigating this possibility. In order to compete with traditional PVD techniques, it is necessary to achieve film coverage uniformity over large enough areas. It was shown that this is feasible, and novel means of achieving it were devised.

Unification of X-ray Winds in Seyfert Galaxies: From Ultra-fast Outflows to Warm Absorbers

NASA Astrophysics Data System (ADS)

Tombesi, Francesco; Cappi, M.; Reeves, J.; Nemmen, R.; Braito, V.; Gaspari, M.; Reynolds, C. S.

2013-04-01

The existence of ionized X-ray absorbing layers of gas along the line of sight to the nuclei of Seyfert galaxies is a well established observational fact. This material is systematically outflowing and shows a large range in parameters. However, its actual nature and dynamics are still not clear. In order to gain insights into these important issues we performed a literature search for papers reporting the parameters of the soft X-ray warm absorbers (WAs) in 35 type 1 Seyferts and compared their properties to those of the ultra-fast outflows (UFOs) detected in the same sample. The fraction of sources with WAs is >60%, consistent with previous studies. The fraction of sources with UFOs is >34%, >67% of which also show WAs. The large dynamic range obtained when considering all the absorbers together allows us, for the first time, to investigate general relations among them. In particular, we find significant correlations indicating that the closer the absorber is to the central black hole, the higher the ionization, column, outflow velocity and consequently the mechanical power. The absorbers continuously populate the whole parameter space, with the WAs and the UFOs lying always at the two ends of the distribution. This strongly suggest that these absorbers, often considered of different types, could actually represent parts of a single large-scale stratified outflow observed at different locations from the black hole. The observed parameters and correlations are consistent with both radiation pressure through Compton scattering and MHD processes contributing to the outflow acceleration, the latter playing a major role. Most of the absorbers, especially the UFOs, have a sufficiently high mechanical power to significantly contribute to the AGN feedback.

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

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

Qi, Y.; Liu, S.; Lindenberg, A. M.

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈ 10 11 K/s) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO 3 occurring on few picosecond time scales. Here, we explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on amore » ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO 3 and BaTiO 3. Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.« less

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

DOE PAGES

Qi, Y.; Liu, S.; Lindenberg, A. M.; ...

2018-01-30

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈ 10 11 K/s) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO 3 occurring on few picosecond time scales. Here, we explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on amore » ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO 3 and BaTiO 3. Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.« less

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.

Oxidized nanocrystalline Fe-Cu pseudoalloy subjected to high pressure and electrodischarge pulses: Mössbauer and x-ray investigations

NASA Astrophysics Data System (ADS)

Gavriliuk, A. G.; Voitkovsky, V. S.; Sidorov, V. A.; Filonenko, V. P.; Tsiok, O. B.; Khvostantsev, L. G.

1998-05-01

Nanocrystalline Fe15Cu85 pseudoalloy has been subjected to pulsed heating up to 1500 K at high pressure (8 GPa). Two regimes were studied: the direct heating using electrodischarge through the sample and indirect heating with the use of cylindrical heater around the sample. The temperature and time conditions in both types of experiments were adjusted to be equivalent. The discharge parameters (stored energy, discharge time, and magnitude of current pulse) were sufficient to move defects by conduction electrons, but insufficient to melt the sample. The properties of treated samples were studied using Mössbauer absorption spectra and x-ray diffraction for three types of samples: (a) primary powder treated by high pressure up to 8 GPa, (b) powder subjected to indirect pulsed heating at 8 GPa, (c) powder treated by electrical pulses at 8 GPa. The x-ray diffraction pattern of primary powder exhibits peaks of copper, iron, and copper oxide (CuO). The Mössbauer spectrum of primary powder exhibits six peaks of alpha iron and some peaks near zero velocity due to the small iron clusters in the copper matrix and ultrafine clusters of paramagnetic phase x-Fe2O3. The transformation of CuO to Cu2O takes place in the course of indirect heating, the Mössbauer spectrum being almost unchanged. The direct electrodischarge heating causes the appearance of new magnetic phase with the magnetic field on iron nucleus 505 kOe, which corresponds to α-Fe2O3. The formation of α-Fe2O3 was confirmed by x-ray diffraction. At the same time the transformation of CuO to Cu2O is incomplete. These experiments demonstrate that high density current pulses, causing the electron wind, can be a useful tool to influence the structure of nanocrystalline powder.

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

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

Osaka, Taito; Hirano, Takashi; Morioka, Yuki

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

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

DOE PAGES

Osaka, Taito; Hirano, Takashi; Morioka, Yuki; ...

2017-10-13

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

Double core-hole emissivity of transient aluminum plasmas produced in the interaction with ultra-intense x-ray laser pulse

NASA Astrophysics Data System (ADS)

Gao, Cheng; Zeng, Jiaolong; Yuan, Jianmin

2015-11-01

Emissivity of single core-hole (SCH) and double core-hole (DCH) states of aluminum plasmas produced in the interaction with ultra-intense x-ray laser pulse interaction are investigated systematically by solving the time-dependent rate equation implemented in the detailed level accounting approximation. We first demonstrated the plasma density effects on level populations and charge state distribution. Compared with recent experiments, it is shown that the plasma density effects play important roles in the evolution dynamics. Then we systematically investigated the emissivity of the transient aluminum plasmas produced by the x-ray laser pulses with a few photon energies above the threshold photon energy to create DCH states. For the laser photon energy where there are resonant absorptions (RA), 1s-np transitions with both full 1s and SCH 1s states play important roles in time evolution of the population and DCH emission spectroscopy. The significant RA effects are illustrated in detail for x-ray pulses, which creates the 1s-2p resonant absorption from the SCH states of Al VII. With the increase of the photon energy, the emissions from lower charge states become larger.

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.

Time-resolved study of SrTiO3 homoepitaxial pulsed-laser deposition using surface x-ray diffraction

NASA Astrophysics Data System (ADS)

Eres, G.; Tischler, J. Z.; Yoon, M.; Larson, B. C.; Rouleau, C. M.; Lowndes, D. H.; Zschack, P.

2002-05-01

Homoepitaxy of SrTiO3 by pulsed-laser deposition has been studied using in situ time-resolved surface x-ray diffraction in the temperature range of 310 °C to 780 °C. Using a two-detector configuration, surface x-ray diffraction intensities were monitored simultaneously at the (0 0 1/2) specular and the (0 1 1/2) off-specular truncation rod positions. Abrupt intensity changes in both the specular and off-specular rods after laser pulses indicated prompt crystallization into SrTiO3 layers followed by slower intra- and interlayer surface rearrangements on time scales of seconds. Specular rod intensity oscillations indicated layer-by-layer growth, while off-specular rod intensity measurements suggested the presence of transient in-plane lattice distortions for depositions above 600 °C.

Accretion torques in X-ray pulsars

NASA Technical Reports Server (NTRS)

Rappaport, S.; Joss, P. C.

1977-01-01

An analysis of the accretion process in an X-ray pulsar, whereby angular momentum is transferred to the star and its rotation period is changed, is presented, and an expression for the fractional rate of change of the pulse period in terms of X-ray luminosity and other star parameters is derived. It is shown that observed characteristic spin-up time scales for seven X-ray pulsars strongly support the view that in every source (1) the pulse period reflects the rotation period of a compact object, (2) the accretion is mediated by a disk surrounding the compact object and rotating in the same sense, and (3) the compact object is a neutron star rather than a white dwarf.

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

Modeling the performance of a photon counting x-ray detector for CT: energy response and pulse pileup effects.

PubMed

Taguchi, Katsuyuki; Zhang, Mengxi; Frey, Eric C; Wang, Xiaolan; Iwanczyk, Jan S; Nygard, Einar; Hartsough, Neal E; Tsui, Benjamin M W; Barber, William C

2011-02-01

Recently, photon counting x-ray detectors (PCXDs) with energy discrimination capabilities have been developed for potential use in clinical computed tomography (CT) scanners. These PCXDs have great potential to improve the quality of CT images due to the absence of electronic noise and weights applied to the counts and the additional spectral information. With high count rates encountered in clinical CT, however, coincident photons are recorded as one event with a higher or lower energy due to the finite speed of the PCXD. This phenomenon is called a "pulse pileup event" and results in both a loss of counts (called "deadtime losses") and distortion of the recorded energy spectrum. Even though the performance of PCXDs is being improved, it is essential to develop algorithmic methods based on accurate models of the properties of detectors to compensate for these effects. To date, only one PCXD (model DXMCT-1, DxRay, Inc., Northridge, CA) has been used for clinical CT studies. The aim of that study was to evaluate the agreement between data measured by DXMCT-1 and those predicted by analytical models for the energy response, the deadtime losses, and the distorted recorded spectrum caused by pulse pileup effects. An energy calibration was performed using 99mTc (140 keV), 57Co (122 keV), and an x-ray beam obtained with four x-ray tube voltages (35, 50, 65, and 80 kVp). The DXMCT-1 was placed 150 mm from the x-ray focal spot; the count rates and the spectra were recorded at various tube current values from 10 to 500 microA for a tube voltage of 80 kVp. Using these measurements, for each pulse height comparator we estimated three parameters describing the photon energy-pulse height curve, the detector deadtime tau, a coefficient k that relates the x-ray tube current I to an incident count rate a by a = k x I, and the incident spectrum. The mean pulse shape of all comparators was acquired in a separate study and was used in the model to estimate the distorted recorded

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

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.

X-ray laser microscope apparatus

DOEpatents

Suckewer, Szymon; DiCicco, Darrell S.; Hirschberg, Joseph G.; Meixler, Lewis D.; Sathre, Robert; Skinner, Charles H.

1990-01-01

A microscope consisting of an x-ray contact microscope and an optical microscope. The optical, phase contrast, microscope is used to align a target with respect to a source of soft x-rays. The source of soft x-rays preferably comprises an x-ray laser but could comprise a synchrotron or other pulse source of x-rays. Transparent resist material is used to support the target. The optical microscope is located on the opposite side of the transparent resist material from the target and is employed to align the target with respect to the anticipated soft x-ray laser beam. After alignment with the use of the optical microscope, the target is exposed to the soft x-ray laser beam. The x-ray sensitive transparent resist material whose chemical bonds are altered by the x-ray beam passing through the target mater GOVERNMENT LICENSE RIGHTS This invention was made with government support under Contract No. De-FG02-86ER13609 awarded by the Department of Energy. The Government has certain rights in this invention.

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