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X-ray free-electron lasers (XFELs) can probe chemical and biological reactions as they unfold with unprecedented spatial and temporal resolution. A principal challenge in this pursuit involves the delivery of samples to the X-ray interaction point in such a way that produces data of the highest possible quality and with maximal efficiency. This is hampered by intrinsic constraints posed by the light source and operation within a beamline environment. For liquid samples, the solution typically involves some form of high-speed liquid jet, capable of keeping up with the rate of X-ray pulses. However, conventional jets are not ideal because of radiation-induced explosions of the jet, as well as their cylindrical geometry combined with the X-ray pointing instability of many beamlines which causes the interaction volume to differ for every pulse. This complicates data analysis and contributes to measurement errors. An alternative geometry is a liquid sheet jet which, with its constant thickness over large areas, eliminates the problems related to X-ray pointing. Since liquid sheets can be made very thin, the radiation-induced explosion is reduced, boosting their stability. These are especially attractive for experiments which benefit from small interaction volumes such as fluctuation X-ray scattering and several types of spectroscopy. Although their use has increased for soft X-ray applications in recent years, there has not yet been wide-scale adoption at XFELs. Here, gas-accelerated liquid sheet jet sample injection is demonstrated at the European XFEL SPB/SFX nano focus beamline. Its performance relative to a conventional liquid jet is evaluated and superior performance across several key factors has been found. This includes a thickness profile ranging from hundreds of nanometres to 60 nm, a fourfold increase in background stability and favorable radiation-induced explosion dynamics at high repetition rates up to 1.13 MHz. Its minute thickness also suggests that ultra

The past, current and planned future developments of X-ray imagers in the Photon-Science Detector Group at DESY-Hamburg is presented. the X-ray imagers are custom developed and tailored to the different X-ray sources in Hamburg, including the storage ring PETRA III/IV; the VUV-soft X-ray free electron laser FLASH, and the European Free-Electron Laser. Each source puts different requirements on the X-ray detectors, which is described in detail, together with the technical solutions implemented.

X-ray free-electron lasers (XFELs) can probe chemical and biological reactions as they unfold with unprecedented spatial and temporal resolution. A principal challenge in this pursuit involves the delivery of samples to the X-ray interaction point in such a way that produces data of the highest possible quality and with maximal efficiency. This is hampered by intrinsic constraints posed by the light source and operation within a beamline environment. For liquid samples, the solution typically involves some form of high-speed liquid jet, capable of keeping up with the rate of X-ray pulses. However, conventional jets are not ideal because of radiation-induced explosions of the jet, as well as their cylindrical geometry combined with the X-ray pointing instability of many beamlines which causes the interaction volume to differ for every pulse. This complicates data analysis and contributes to measurement errors. An alternative geometry is a liquid sheet jet which, with its constant thickness over large areas, eliminates the problems related to X-ray pointing. Since liquid sheets can be made very thin, the radiation-induced explosion is reduced, boosting their stability. These are especially attractive for experiments which benefit from small interaction volumes such as fluctuation X-ray scattering and several types of spectroscopy. Although their use has increased for soft X-ray applications in recent years, there has not yet been wide-scale adoption at XFELs. Here, gas-accelerated liquid sheet jet sample injection is demonstrated at the European XFEL SPB/SFX nano focus beamline. Its performance relative to a conventional liquid jet is evaluated and superior performance across several key factors has been found. This includes a thickness profile ranging from hundreds of nanometres to 60 nm, a fourfold increase in background stability and favorable radiation-induced explosion dynamics at high repetition rates up to 1.13 MHz. Its minute thickness also suggests that ultra

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Free-electron lasers could enable X-ray imaging of single biological macro-molecules and the study of protein dynamics, paving the way for a powerful new imaging tool in structural biology, but a low signal-to-noise ratio and missing regions in the detectors, colloquially termed 'masks', affect data collection and hamper real-time evaluation of experimental data. In this article, the challenges posed by noise and masks are tackled by introducing a neural network pipeline that aims to restore diffraction intensities. For training and testing of the model, a data set of diffraction patterns was simulated from 10 900 different proteins with molecular weights within the range of 10-100 kDa and collected at a photon energy of 8 keV. The method is compared with a simple low-pass filtering algorithm based on autocorrelation constraints. The results show an improvement in the mean-squared error of roughly two orders of magnitude in the presence of masks compared with the noisy data. The algorithm was also tested at increasing mask width, leading to the conclusion that demasking can achieve good results when the mask is smaller than half of the central speckle of the pattern. The results highlight the competitiveness of this model for data processing and the feasibility of restoring diffraction intensities from unknown structures in real time using deep learning methods. Finally, an example is shown of this preprocessing making orientation recovery more reliable, especially for data sets containing very few patterns, using the expansion-maximization-compression algorithm.

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Free-electron lasers could enable X-ray imaging of single biological macro-molecules and the study of protein dynamics, paving the way for a powerful new imaging tool in structural biology, but a low signal-to-noise ratio and missing regions in the detectors, colloquially termed 'masks', affect data collection and hamper real-time evaluation of experimental data. In this article, the challenges posed by noise and masks are tackled by introducing a neural network pipeline that aims to restore diffraction intensities. For training and testing of the model, a data set of diffraction patterns was simulated from 10 900 different proteins with molecular weights within the range of 10-100 kDa and collected at a photon energy of 8 keV. The method is compared with a simple low-pass filtering algorithm based on autocorrelation constraints. The results show an improvement in the mean-squared error of roughly two orders of magnitude in the presence of masks compared with the noisy data. The algorithm was also tested at increasing mask width, leading to the conclusion that demasking can achieve good results when the mask is smaller than half of the central speckle of the pattern. The results highlight the competitiveness of this model for data processing and the feasibility of restoring diffraction intensities from unknown structures in real time using deep learning methods. Finally, an example is shown of this preprocessing making orientation recovery more reliable, especially for data sets containing very few patterns, using the expansion-maximization-compression algorithm.

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Free-electron lasers could enable X-ray imaging of single biological macro-molecules and the study of protein dynamics, paving the way for a powerful new imaging tool in structural biology, but a low signal-to-noise ratio and missing regions in the detectors, colloquially termed 'masks', affect data collection and hamper real-time evaluation of experimental data. In this article, the challenges posed by noise and masks are tackled by introducing a neural network pipeline that aims to restore diffraction intensities. For training and testing of the model, a data set of diffraction patterns was simulated from 10 900 different proteins with molecular weights within the range of 10-100 kDa and collected at a photon energy of 8 keV. The method is compared with a simple low-pass filtering algorithm based on autocorrelation constraints. The results show an improvement in the mean-squared error of roughly two orders of magnitude in the presence of masks compared with the noisy data. The algorithm was also tested at increasing mask width, leading to the conclusion that demasking can achieve good results when the mask is smaller than half of the central speckle of the pattern. The results highlight the competitiveness of this model for data processing and the feasibility of restoring diffraction intensities from unknown structures in real time using deep learning methods. Finally, an example is shown of this preprocessing making orientation recovery more reliable, especially for data sets containing very few patterns, using the expansion-maximization-compression algorithm.

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Free-electron lasers could enable X-ray imaging of single biological macro-molecules and the study of protein dynamics, paving the way for a powerful new imaging tool in structural biology, but a low signal-to-noise ratio and missing regions in the detectors, colloquially termed 'masks', affect data collection and hamper real-time evaluation of experimental data. In this article, the challenges posed by noise and masks are tackled by introducing a neural network pipeline that aims to restore diffraction intensities. For training and testing of the model, a data set of diffraction patterns was simulated from 10 900 different proteins with molecular weights within the range of 10-100 kDa and collected at a photon energy of 8 keV. The method is compared with a simple low-pass filtering algorithm based on autocorrelation constraints. The results show an improvement in the mean-squared error of roughly two orders of magnitude in the presence of masks compared with the noisy data. The algorithm was also tested at increasing mask width, leading to the conclusion that demasking can achieve good results when the mask is smaller than half of the central speckle of the pattern. The results highlight the competitiveness of this model for data processing and the feasibility of restoring diffraction intensities from unknown structures in real time using deep learning methods. Finally, an example is shown of this preprocessing making orientation recovery more reliable, especially for data sets containing very few patterns, using the expansion-maximization-compression algorithm.

The ultraviolet (UV)-induced dissociation and photofragmentation of gas-phase CH2BrI molecules induced by intense femtosecond extreme ultraviolet (XUV) pulses at three different photon energies are studied by multi-mass ion imaging. Using a UV-pump-XUV-probe scheme, charge transfer between highly charged iodine ions and neutral CH2Br radicals produced by C-I bond cleavage is investigated. In earlier charge-transfer studies, the center of mass of the molecules was located along the axis of the bond cleaved by the pump pulse. In the present case of CH2BrI, this is not the case, thus inducing a rotation of the fragment. We discuss the influence of the rotation on the charge transfer process using a classical over-the-barrier model. Our modeling suggests that, despite the fact that the dissociation is slower due to the rotational excitation, the critical interatomic distance for charge transfer is reached faster. Furthermore, we suggest that charge transfer during molecular fragmentation may be modulated in a complex way.

Free-electron lasers could enable X-ray imaging of single biological macro-molecules and the study of protein dynamics, paving the way for a powerful new imaging tool in structural biology, but a low signal-to-noise ratio and missing regions in the detectors, colloquially termed 'masks', affect data collection and hamper real-time evaluation of experimental data. In this article, the challenges posed by noise and masks are tackled by introducing a neural network pipeline that aims to restore diffraction intensities. For training and testing of the model, a data set of diffraction patterns was simulated from 10 900 different proteins with molecular weights within the range of 10-100 kDa and collected at a photon energy of 8 keV. The method is compared with a simple low-pass filtering algorithm based on autocorrelation constraints. The results show an improvement in the mean-squared error of roughly two orders of magnitude in the presence of masks compared with the noisy data. The algorithm was also tested at increasing mask width, leading to the conclusion that demasking can achieve good results when the mask is smaller than half of the central speckle of the pattern. The results highlight the competitiveness of this model for data processing and the feasibility of restoring diffraction intensities from unknown structures in real time using deep learning methods. Finally, an example is shown of this preprocessing making orientation recovery more reliable, especially for data sets containing very few patterns, using the expansion-maximization-compression algorithm.

The outcomes and timescales of molecular nonadiabatic dynamics are decisively impacted by the quantum coherences generated at localized molecular regions. In time-resolved X-ray diffraction imaging, these coherences create distinct signatures via inelastic photon scattering, but they are buried under much stronger background elastic features. Here, we exploit the rich dynamical information encoded in the inelastic patterns, which we reveal by frequency-dispersed covariance ultrafast powder X-ray diffraction of stochastic X-ray free-electron laser pulses. This is demonstrated for the photoisomerization of azobenzene involving the passage through a conical intersection, where the nuclear wave packet branches and explores different quantum pathways. Snapshots of the coherence dynamics are obtained at high frequency shifts, not accessible with conventional diffraction measurements. These provide access to the timing and to the confined spatial distribution of the valence electrons directly involved in the conical intersection passage. This study can be extended to full three-dimensional imaging of conical intersections with ultrafast X-ray and electron diffraction.

Most crystallographic data processing methods use pixel integration. In serial femtosecond crystallography (SFX), the intricate interaction between the reciprocal lattice point and the Ewald sphere is integrated out by averaging symmetrically equivalent observations recorded across a large number (104-106) of exposures. Although sufficient for generating biological insights, this approach converges slowly, and using it to accurately measure anomalous differences has proved difficult. This report presents a novel approach for increasing the accuracy of structure factors obtained from SFX data. A physical model describing all observed pixels is defined to a degree of complexity such that it can decouple the various contributions to the pixel intensities. Model dependencies include lattice orientation, unit-cell dimensions, mosaic structure, incident photon spectra and structure factor amplitudes. Maximum likelihood estimation is used to optimize all model parameters. The application of prior knowledge that structure factor amplitudes are positive quantities is included in the form of a reparameterization. The method is tested using a synthesized SFX dataset of ytterbium(III) lysozyme, where each X-ray laser pulse energy is centered at 9034 eV. This energy is 100 eV above the Yb3+ L-III absorption edge, so the anomalous difference signal is stable at 10 electrons despite the inherent energy jitter of each femtosecond X-ray laser pulse. This work demonstrates that this approach allows the determination of anomalous structure factors with very high accuracy while requiring an order-of-magnitude fewer shots than conventional integration-based methods would require to achieve similar results.

Most crystallographic data processing methods use pixel integration. In serial femtosecond crystallography (SFX), the intricate interaction between the reciprocal lattice point and the Ewald sphere is integrated out by averaging symmetrically equivalent observations recorded across a large number (104-106) of exposures. Although sufficient for generating biological insights, this approach converges slowly, and using it to accurately measure anomalous differences has proved difficult. This report presents a novel approach for increasing the accuracy of structure factors obtained from SFX data. A physical model describing all observed pixels is defined to a degree of complexity such that it can decouple the various contributions to the pixel intensities. Model dependencies include lattice orientation, unit-cell dimensions, mosaic structure, incident photon spectra and structure factor amplitudes. Maximum likelihood estimation is used to optimize all model parameters. The application of prior knowledge that structure factor amplitudes are positive quantities is included in the form of a reparameterization. The method is tested using a synthesized SFX dataset of ytterbium(III) lysozyme, where each X-ray laser pulse energy is centered at 9034 eV. This energy is 100 eV above the Yb3+ L-III absorption edge, so the anomalous difference signal is stable at 10 electrons despite the inherent energy jitter of each femtosecond X-ray laser pulse. This work demonstrates that this approach allows the determination of anomalous structure factors with very high accuracy while requiring an order-of-magnitude fewer shots than conventional integration-based methods would require to achieve similar results.

Research at modern light sources continues to improve our knowledge of the natural world, from the subtle workings of life to matter under extreme conditions. Free-electron lasers, for instance, have enabled the characterization of biomolecular structures with sub-angstrom spatial resolution, and paved the way to controlling the molecular functions. On the other hand, attosecond temporal resolution is necessary to broaden our scope of the ultrafast world. Here we discuss attosecond pulse generation beyond present capabilities. Furthermore, we review three recently proposed methods of generating attosecond x-ray pulses. These novel methods exploit the coherent radiation of microbunched electrons in undulators and the tailoring of the emitted wavefronts. The computed pulse energy outperforms pre-existing technologies by three orders of magnitude. Specifically, our simulations of the proposed Soft X-ray Laser at MAX IV (Lund, Sweden) show that a pulse duration of 50-100 as and a pulse energy up to 5 mu J is feasible with the novel methods. In addition, the methods feature pulse shape control, enable the incorporation of orbital angular momentum, and can be used in combination with modern compact free-electron laser setups.

Research at modern light sources continues to improve our knowledge of the natural world, from the subtle workings of life to matter under extreme conditions. Free-electron lasers, for instance, have enabled the characterization of biomolecular structures with sub-angstrom spatial resolution, and paved the way to controlling the molecular functions. On the other hand, attosecond temporal resolution is necessary to broaden our scope of the ultrafast world. Here we discuss attosecond pulse generation beyond present capabilities. Furthermore, we review three recently proposed methods of generating attosecond x-ray pulses. These novel methods exploit the coherent radiation of microbunched electrons in undulators and the tailoring of the emitted wavefronts. The computed pulse energy outperforms pre-existing technologies by three orders of magnitude. Specifically, our simulations of the proposed Soft X-ray Laser at MAX IV (Lund, Sweden) show that a pulse duration of 50-100 as and a pulse energy up to 5 mu J is feasible with the novel methods. In addition, the methods feature pulse shape control, enable the incorporation of orbital angular momentum, and can be used in combination with modern compact free-electron laser setups.

Free superfluid helium droplets constitute a versatile medium for a diverse range of experiments in physics and chemistry that extend from studies of the fundamental laws of superfluid motion to the synthesis of novel nanomaterials. In particular, the emergence of quantum vortices in rotating helium droplets is one of the most dramatic hallmarks of superfluidity and gives detailed access to the wave function describing the quantum liquid. This review provides an introduction to quantum vorticity in helium droplets, followed by a historical account of experiments on vortex visualization in bulk superfluid helium and a more detailed discussion of recent advances in the study of the rotational motion of isolated, nano- to micrometer-scale superfluid helium droplets. Ultrafast X-ray and extreme ultraviolet scattering techniques enabled by X-ray free-electron lasers and high-order harmonic generation in particular have facilitated the in situ detection of droplet shapes and the imaging of vortex structures inside individual, isolated droplets. New applications of helium droplets ranging from studies of quantum phase separations to mechanisms of low-temperature aggregation are discussed.

Free superfluid helium droplets constitute a versatile medium for a diverse range of experiments in physics and chemistry that extend from studies of the fundamental laws of superfluid motion to the synthesis of novel nanomaterials. In particular, the emergence of quantum vortices in rotating helium droplets is one of the most dramatic hallmarks of superfluidity and gives detailed access to the wave function describing the quantum liquid. This review provides an introduction to quantum vorticity in helium droplets, followed by a historical account of experiments on vortex visualization in bulk superfluid helium and a more detailed discussion of recent advances in the study of the rotational motion of isolated, nano- to micrometer-scale superfluid helium droplets. Ultrafast X-ray and extreme ultraviolet scattering techniques enabled by X-ray free-electron lasers and high-order harmonic generation in particular have facilitated the in situ detection of droplet shapes and the imaging of vortex structures inside individual, isolated droplets. New applications of helium droplets ranging from studies of quantum phase separations to mechanisms of low-temperature aggregation are discussed.

Serial femtosecond crystallography of two-dimensional membrane-protein crystals at X-ray free-electron lasers has the potential to address the dynamics of functionally relevant large-scale motions, which can be sterically hindered in three-dimensional crystals and suppressed in cryocooled samples. In previous work, diffraction data limited to a two-dimensional reciprocal-space slice were evaluated and it was demonstrated that the low intensity of the diffraction signal can be overcome by collecting highly redundant data, thus enhancing the achievable resolution. Here, the application of a newly developed method to analyze diffraction data covering three reciprocal-space dimensions, extracting the reciprocal-space map of the structure-factor amplitudes, is presented. Despite the low resolution and completeness of the data set, it is shown by molecular replacement that the reconstructed amplitudes carry meaningful structural information. Therefore, it appears that these intrinsic limitations in resolution and completeness from two-dimensional crystal diffraction may be overcome by collecting highly redundant data along the three reciprocal-space axes, thus allowing the measurement of large-scale dynamics in pump-probe experiments.

This introductory article is a synopsis of the status and prospects of particle-beam-driven plasma wakefield acceleration (PWFA). Conceptual and experimental breakthroughs obtained over the last years have initiated a rapid growth of the research field, and increased maturity of underlying technology allows an increasing number of research groups to engage in experimental R&D. We briefly describe the fundamental mechanisms of PWFA, from which its chief attractions arise. Most importantly, this is the capability of extremely rapid acceleration of electrons and positrons at gradients many orders of magnitude larger than in conventional accelerators. This allows the size of accelerator units to be shrunk from the kilometre to metre scale, and possibly the quality of accelerated electron beam output to be improved by orders of magnitude. In turn, such compact and high-quality accelerators are potentially transformative for applications across natural, material and life sciences. This overview provides contextual background for the manuscripts of this issue, resulting from a Theo Murphy meeting held in the summer of 2018. This article is part of the Theo Murphy meeting issue 'Directions in particle beam-driven plasma wakefield acceleration'.

Previous proof-of-concept measurements on single-layer two-dimensional membrane-protein crystals performed at X-ray free-electron lasers (FELs) have demonstrated that the collection of meaningful diffraction patterns, which is not possible at synchrotrons because of radiation-damage issues, is feasible. Here, the results obtained from the analysis of a thousand single-shot, room-temperature X-ray FEL diffraction images from two-dimensional crystals of a bacteriorhodopsin mutant are reported in detail. The high redundancy in the measurements boosts the intensity signal-to-noise ratio, so that the values of the diffracted intensities can be reliably determined down to the detector-edge resolution of 4 Å. The results show that two-dimensional serial crystallography at X-ray FELs is a suitable method to study membrane proteins to near-atomic length scales at ambient temperature. The method presented here can be extended to pump-probe studies of optically triggered structural changes on submillisecond timescales in two-dimensional crystals, which allow functionally relevant large-scale motions that may be quenched in three-dimensional crystals.

There is a great interest in generating high-power hard X-ray Free Electron Laser (FEL) in the terawatt (TW) level that can enable coherent diffraction imaging of complex molecules like proteins and probe fundamental high-field physics. A feasibility study of producing such X-ray pulses was carried out employing a configuration beginning with a Self-Amplified Spontaneous Emission FEL, followed by a “self-seeding” crystal monochromator generating a fully coherent seed, and finishing with a long tapered undulator where the coherent seed recombines with the electron bunch and is amplified to high power. The undulator tapering profile, the phase advance in the undulator break sections, the quadrupole focusing strength, etc. are parameters to be optimized. A Genetic Algorithm (GA) is adopted for this multi-dimensional optimization. Concrete examples are given for LINAC Coherent Light Source (LCLS) and LCLS-II-type systems. Analytical estimate is also developed to cross check the simulation and optimization results as a quick and complimentary tool.

There is a great interest in generating high-power hard X-ray Free Electron Laser (FEL) in the terawatt (TW) level that can enable coherent diffraction imaging of complex molecules like proteins and probe fundamental high-field physics. A feasibility study of producing such X-ray pulses was carried out employing a configuration beginning with a Self-Amplified Spontaneous Emission FEL, followed by a “self-seeding” crystal monochromator generating a fully coherent seed, and finishing with a long tapered undulator where the coherent seed recombines with the electron bunch and is amplified to high power. The undulator tapering profile, the phase advance in the undulator break sections, the quadrupole focusing strength, etc. are parameters to be optimized. A Genetic Algorithm (GA) is adopted for this multi-dimensional optimization. Concrete examples are given for LINAC Coherent Light Source (LCLS) and LCLS-II-type systems. Analytical estimate is also developed to cross check the simulation and optimization results as a quick and complimentary tool.

The paper presents a quantum mechanical treatment for analyzing the Smith-Purcell radiation generated by charged particles passing over a periodic conducting structure. In our theoretical model, the electrons interact with a surface harmonic wave excited near the diffraction grating when the electron velocity is almost equal to the phase velocity of the surface wave. Then, the surface harmonic wave is electromagnetically coupled to a radiation mode. The dynamics of electrons are analyzed quantum mechanically where the electron is represented as a traveling electron wave with a finite spreading length. The conversion of the surface wave into a propagating mode is analyzed using the classical Maxwell equations. In the small-signal gain regime, closed-form expressions for the contributions of the stimulated and spontaneous emissions to the evolution of the surface wave are derived. The inclusion of the spreading length of the electron wave to the emission spectral line is investigated. Finally, we compare our results based on the quantum mechanical description of electron and those based on the classical approach where a good agreement is confirmed. © 2015 Elsevier B.V., Embargo Period 24 months

Traveling-Wave Thomson-Scattering (TWTS) provides optical undulators with hundreds to thousands of undulator periods from high-power, pulse-front tilted lasers pulses. These allow to realize optical free-electron lasers (OFELs) with state-of-the-art technology in electron accelerators and laser systems. TWTS employs a side-scattering geometry where laser and electron propagation direction of motion enclose the interaction angle. Tilting the laser pulse front with respect to the wave front by half the interaction angle ensures continuous overlap over the whole laser pulse width while the electrons cross the laser beam path. Scaling laws and analytical models allow identifying experimentally promising FEL regimes for feasible setup geometries. However, selfconsistently including all non-ideal effects in a 3D FEL simulations is desirable for predicting TWTS-OFEL designs with quantitive performance and tolerance characteristics suitable for engineering an optimal proof-of-principle experiment. In this talk we outline the challenges that existing FEL codes cannot cope with the non-collinear geometry of TWTS-OFELs, show how we solve these using the particle-in-cell code PIConGPU as 3D-FEL code and present first results.

Traveling-Wave Thomson-Scattering (TWTS) provides optical undulators with hundreds to thousands of undulator periods from high-power, pulse-front tilted lasers pulses. These allow to realize optical free-electron lasers (OFELs) with state-of-the-art technology in electron accelerators and laser systems. TWTS employs a side-scattering geometry where laser and electron propagation direction of motion enclose the interaction angle. Tilting the laser pulse front with respect to the wave front by half the interaction angle ensures continuous overlap over the whole laser pulse width while the electrons cross the laser beam path. Scaling laws and analytical models allow identifying experimentally promising FEL regimes for feasible setup geometries. However, selfconsistently including all non-ideal effects in a 3D FEL simulations is desirable for predicting TWTS-OFEL designs with quantitive performance and tolerance characteristics suitable for engineering an optimal proof-of-principle experiment. In this talk we outline the challenges that existing FEL codes cannot cope with the non-collinear geometry of TWTS-OFELs, show how we solve these using the particle-in-cell code PIConGPU as 3D-FEL code and present first results.

The latest virtual special issue of Journal of Applied Crystallography (http://journals.iucr.org/special_issues/2016/ccpfel) collects software for free-electron laser research and presents tools for a range of topics such as simulation of experiments, online monitoring of data collection, selection of hits, diagnostics of data quality, data management, data analysis and structure determination for both nanocrystallography and single-particle diffractive imaging. This article provides an introduction to the special issue.

For over 10 years, laser plasma acceleration (LPA) has been a rapidly growing technologyused to create electron beams on length-scales much smaller than that of a conventionalRF-accelerator [1]. As electron beam properties improve, research for LPAs is expanding totake advantage of the creation and accessibility of high-quality electron beams from plasmatargets. Two applications which are currently being explored are a multi-stage plasmaaccelerator to reach energies greater than those a single-stage accelerator can achieve andexploring the possibility of an LPA based free-electron laser (FEL) light source. Researchsupporting both of these efforts has been performed on the 50 TW TREX laser system atthe BELLA Center at the Lawrence Berkeley National Lab, and the results of these effortsare described in this dissertation.Using chirped-pulsed amplification to produce high-quality laser pulses up to petawattlevels, experimental results have yielded laser driven electron beam energies up to 4.25GeV [2]. By tuning the density of the target, the accelerating gradients sustained by theplasma can grow beyond 100 GeV/m [3] (10^3 times larger than that of a conventional RFaccelerator). However, limiting factors such as dephasing of the electron beam from theplasma wake, defocusing of a laser pulse, and energy depletion of the laser into the plasmalimit the maximum sensible length of a plasma accelerator. Staging the LPA with two ormore accelerating modules could be the next step towards producing beams with energiesgreater than those possible with a single stage.One requirement for staged acceleration is that the laser pulse used to drive the firstaccelerating stage must be coupled out of the beamline, and a fresh laser pulse must becoupled in for the second stage to post accelerate the electrons. To do this while maintaininga short scale length between the two stages requires an optic to be placed near the final focus of the second laser pulse. Because damage will occur when t

For over 10 years, laser plasma acceleration (LPA) has been a rapidly growing technologyused to create electron beams on length-scales much smaller than that of a conventionalRF-accelerator [1]. As electron beam properties improve, research for LPAs is expanding totake advantage of the creation and accessibility of high-quality electron beams from plasmatargets. Two applications which are currently being explored are a multi-stage plasmaaccelerator to reach energies greater than those a single-stage accelerator can achieve andexploring the possibility of an LPA based free-electron laser (FEL) light source. Researchsupporting both of these efforts has been performed on the 50 TW TREX laser system atthe BELLA Center at the Lawrence Berkeley National Lab, and the results of these effortsare described in this dissertation.Using chirped-pulsed amplification to produce high-quality laser pulses up to petawattlevels, experimental results have yielded laser driven electron beam energies up to 4.25GeV [2]. By tuning the density of the target, the accelerating gradients sustained by theplasma can grow beyond 100 GeV/m [3] (10^3 times larger than that of a conventional RFaccelerator). However, limiting factors such as dephasing of the electron beam from theplasma wake, defocusing of a laser pulse, and energy depletion of the laser into the plasmalimit the maximum sensible length of a plasma accelerator. Staging the LPA with two ormore accelerating modules could be the next step towards producing beams with energiesgreater than those possible with a single stage.One requirement for staged acceleration is that the laser pulse used to drive the firstaccelerating stage must be coupled out of the beamline, and a fresh laser pulse must becoupled in for the second stage to post accelerate the electrons. To do this while maintaininga short scale length between the two stages requires an optic to be placed near the final focus of the second laser pulse. Because damage will occur when t

A hard x-ray free-electron laser (XFEL) provides an x-ray source with an extraordinary high peak-brilliance, a time structure with extremely short pulses and with a large degree of coherence, opening the door to new scientific fields. Many XFEL experiments require the x-ray beam to be focused to nanometer dimensions or, at least, benefit from such a focused beam. A detailed knowledge about the illuminating beam helps to interpret the measurements or is even inevitable to make full use of the focused beam. In this paper we report on focusing an XFEL beam to a transverse size of 125nm and how we applied ptychographic imaging to measure the complex wavefield in the focal plane in terms of phase and amplitude. Propagating the wavefield back and forth we are able to reconstruct the full caustic of the beam, revealing aberrations of the nano-focusing optic. By this method we not only obtain the averaged illumination but also the wavefield of individual XFEL pulses., QC 20131118

The magnetic phase transitions for Gd(0 0 0 1) grown on W(1 1 0) - a bulk transition at 293 K and a surface transition about 85 K above this - are found to influence the energy separation of the Gd 5s and 4s core-photoelectron doublets. The 5s doublet separation ¿E5s changes over a range of temperatures spanning these transitions, and decreases by a maximum of 60 meV in this region, but then recovers its original value; the 4s doublet shows a smaller change in the reverse direction, which does not recover at high temperature. Some of these effects are semi-quantitatively understood from free-atom multiplet theory and from theoretical calculations based on all-electron LDA+U calculations including 4f electron correlation effects. However, the high-temperature behavior of the data also suggest a dynamical nature to these effects via spin-dependent electron screening that is influenced by magnetic fluctuations. Several avenues for studying such effects in a time-resolved manner in future experiments are discussed.

A complete set of structure factors has been extracted from hundreds of thousands of femtosecond single-shot X-ray microdiffraction patterns taken from randomly oriented nanocrystals. The method of Monte Carlo integration over crystallite size and orientation was applied to experimental data from Photosystem I nanocrystals. This arrives at structure factors from many partial reflections without prior knowledge of the particle-size distribution. The data were collected at the Linac Coherent Light Source (the first hard-X-ray laser user facility), to which was fitted a hydrated protein nanocrystal injector jet, according to the method of serial crystallography. The data are single 'still' diffraction snapshots, each from a different nanocrystal with sizes ranging between 100 nm and 2 mu m, so the angular width of Bragg peaks was dominated by crystal-size effects. These results were compared with single-crystal data recorded from large crystals of Photosystem I at the Advanced Light Source and the quality of the data was found to be similar. The implications for improving the efficiency of data collection by allowing the use of very small crystals, for radiation-damage reduction and for time-resolved diffraction studies at room temperature are discussed.

The past few years have seen a tremendous growth in the field of coherent X-ray diffractive imaging, in large part due to X-ray free-electron lasers which provide a peak brilliance billions of times higher than that of synchrotrons. However, this rapid development in terms of hardware has not been matched on the software side. The release of Hawk is intended to close this gap. To the authors knowledge Hawk is the first publicly available and fully open source software program for reconstructing images from continuous diffraction patterns. The software handles all steps leading from a raw diffraction pattern to a reconstructed two-dimensional image including geometry determination, background correction, masking and phasing. It also includes preliminary three-dimensional support and support for graphics processing units using the Compute Unified Device Architecture, which speeds up processing by orders of magnitude compared to a single central processing unit. Hawk implements numerous algorithms and is easily extended. This, in combination with its open-source licence, provides a platform for other groups to test, develop and distribute their own algorithms.

The major advances in the actual and predicted performances of new light sources (low-emittance storage rings and soft and hard X-ray free-electron lasers) in the last few years have provided a new impulse to the development of atomic and molecular physics, in particular in what concerns electronic structure and dynamics of atoms, molecules, liquids and clusters investigated with photoelectron spectroscopy, resonant inelastic X-ray scattering and ion spectroscopy. We present here a review on the present trends and future perspectives of the field, with special emphasis on the new possibilities offered by the characteristics of the new sources (high brilliance, low emittance, short pulses). Several examples will be provided concerning state-of-the-art present results and future developments. (C) 2010 Elsevier B.V. All rights reserved.

type:text, A time-resolved photoelectron imaging using a femtosecond ultraviolet (UV) laser and a vacuum UV freeelectron laser is presented. Ultrafast internal conversion and intersystem crossing in pyrazine in a supersonic molecular beam were clearly observed in the time profiles of photoioinzation intensity and time-dependent photoelectron images.

The topic of this chapter is a survey on the main applications of free-electron lasers (FELs) in physical sciences. The merits of FELs are discussed with respect to other available laser sources. For the wavelength ranges, where FELs contributed significantly to advances in physical sciences, specific examples of the research with FELs are given.

This thesis investigates active mirror alignment systems of a free electron laser (FEL) for future integration as a ship self-defense weapon. An issue with this integration is the effect of low-frequency shipboard vibrations on the optical cavity mirrors. Alignment of the cavity mirrors is required for the proper operation of any type of laser. Mirror alignment is especially critical for an FEL because the electron beam and optical mode must substantially overlap. Laboratory FEL facilities, along with other laboratory high energy facilities that employ active mirror alignment systems, are investigated. In addition, a model theory for controlling the vibrations of a single-degree-of-freedom system is developed, and experiments with a simple mirror alignment system are described. Reduction of an impressed vibration amplitude by a factor of five is achieved, compared to a factor of fifteen that is achieved in major laboratory systems with sophisticated control systems. The purpose of these efforts is to understand the underlying physics of vibration control. The knowledge forms a basis for follow-on research towards the development of a prototype shipboard active mirror alignment system., http://archive.org/details/activemirrorlign109453981, Lieutenant Commander, United States Navy, Approved for public release; distribution is unlimited.

A time-resolved photoelectron imaging using a femtosecond ultraviolet (UV) laser and a vacuum UV freeelectron laser is presented. Ultrafast internal conversion and intersystem crossing in pyrazine in a supersonic molecular beam were clearly observed in the time profiles of photoioinzation intensity and time-dependent photoelectron images.