Ultrashort X-ray Pulses Research Articles

The dynamics of lithium atom photoionization by ultrashort-pulse x-rays

The beam intensity has to approach relativistic values in order to achieve atomic resolution in diffraction studies of molecule’s structure using x-ray free electron lasers. The existing methods for evaluating the sample damage in such conditions have a number of limitations. The damaging dynamics can be studied by the trajectory method developed in our previous studies. It enables one to calculate the probability of photoionization of atoms in a wide range of x-ray field parameters, including those for strong ultrashort x-ray pulses approaching relativistic intensity. The method also enables one to bypass many limitations of other methods in the analysis of the dynamics of sample damaging process. In this paper we use this method to evaluate the probability of lithium atom photoionization by ultrashort-pulse x-rays.

Ultrashort Free-Electron Laser X-ray Pulses

For the investigation of processes happening on the time scale of the motion of bound electrons, well-controlled X-ray pulses with durations in the few-femtosecond and even sub-femtosecond range are a necessary prerequisite. Novel free-electron lasers sources provide these ultrashort, high-brightness X-ray pulses, but their unique aspects open up concomitant challenges for their characterization on a suitable time scale. In this review paper we describe progress and results of recent work on ultrafast pulse characterization at soft and hard X-ray free-electron lasers. We report on different approaches to laser-assisted time-domain measurements, with specific focus on single-shot characterization of ultrashort X-ray pulses from self-amplified spontaneous emission-based and seeded free-electron lasers. The method relying on the sideband measurement of X-ray electron ionization in the presence of a dressing optical laser field is described first. When the X-ray pulse duration is shorter than half the oscillation period of the streaking field, few-femtosecond characterization becomes feasible via linear streaking spectroscopy. Finally, using terahertz fields alleviates the issue of arrival time jitter between streaking laser and X-ray pulse, but compromises the achievable temporal resolution. Possible solutions to these remaining challenges for single-shot, full time–energy characterization of X-ray free-electron laser pulses are proposed in the outlook at the end of the review.

Soft x-ray induced femtosecond solid-to-solid phase transition

Soft x-rays were applied to induce graphitization of diamond through a non-thermal solid-to-solid phase transition. This process was observed within poly-crystalline diamond with a time-resolved experiment using ultrashort soft x-ray pulses of duration 52.5 fs and cross correlated by an optical pulse of duration 32.8 fs. This scheme enabled for the first time the measurement of a phase transition on a timescale of ∼150 fs. Excellent agreement between experiment and theoretical predictions was found, using a dedicated code that followed the non-equilibrium evolution of the irradiated diamond including all transient electronic and structural changes. These observations confirm that soft x-rays can induce a non-thermal ultrafast solid-to-solid phase transition on a hundred femtosecond timescale.

Status of the SACLA Facility

This article reports the current status of SACLA, SPring-8 Angstrom Compact free electron LAser, which has been producing stable X-ray Free Electron Laser (XFEL) light since 2012. A unique injector system and a short-period in-vacuum undulator enable the generation of ultra-short coherent X-ray pulses with a wavelength shorter than 0.1 nm. Continuous development of accelerator technologies has steadily improved XFEL performance, not only for normal operations but also for fast switching operation of the two beamlines. After upgrading the broadband spontaneous-radiation beamline to produce soft X-ray FEL with a dedicated electron beam driver, it is now possible to operate three FEL beamlines simultaneously. Beamline/end-station instruments and data acquisition/analyzation systems have also been upgraded to allow advanced experiments. These efforts have led to the production of novel results and will offer exciting new opportunities for users from many fields of science.

Mapping few-femtosecond slices of ultra-relativistic electron bunches

Free-electron lasers are unique sources of intense and ultra-short x-ray pulses that led to major scientific breakthroughs across disciplines from matter to materials and life sciences. The essential element of these devices are micrometer-sized electron bunches with high peak currents, low energy spread, and low emittance. Advanced FEL concepts such as seeded amplifiers rely on the capability of analyzing and controlling the electron beam properties with few-femtosecond time resolution. One major challenge is to extract tomographic slice parameters instead of projected electron beam properties. Here, we demonstrate that a radio-frequency deflector in combination with a dipole spectrometer not only allows for single-shot extraction of a seeded FEL pulse profile, but also provides information on the electron slice emittance and energy spread. The seeded FEL power profile can be directly related to the derived slice emittance as a function of intra-bunch coordinate with a resolution down to a few femtoseconds.

Molecular Dynamics of XFEL-Induced Photo-Dissociation, Revealed by Ion-Ion Coincidence Measurements

X-ray free electron lasers (XFELs) providing ultrashort intense pulses of X-rays have proven to be excellent tools to investigate the dynamics of radiation-induced dissociation and charge redistribution in molecules and nanoparticles. Coincidence techniques, in particular multi-ion time-of-flight (TOF) coincident experiments, can provide detailed information on the photoabsorption, charge generation, and Coulomb explosion events. Here we review several such recent experiments performed at the SPring-8 Angstrom Compact free electron LAser (SACLA) facility in Japan, with iodomethane, diiodomethane, and 5-iodouracil as targets. We demonstrate how to utilize the momentum-resolving capabilities of the ion TOF spectrometers to resolve and filter the coincidence data and extract various information essential in understanding the time evolution of the processes induced by the XFEL pulses.

Diffraction based method to reconstruct the spectrum of the Thomson scattering x-ray source.

As Thomson scattering x-ray sources based on the collision of intense laser and relativistic electrons have drawn much attention in various scientific fields, there is an increasing demand for the effective methods to reconstruct the spectrum information of the ultra-short and high-intensity x-ray pulses. In this paper, a precise spectrum measurement method for the Thomson scattering x-ray sources was proposed with the diffraction of a Highly Oriented Pyrolytic Graphite (HOPG) crystal and was demonstrated at the Tsinghua Thomson scattering X-ray source. The x-ray pulse is diffracted by a 15 mm (L) ×15 mm (H)× 1 mm (D) HOPG crystal with 1° mosaic spread. By analyzing the diffraction pattern, both x-ray peak energies and energy spectral bandwidths at different polar angles can be reconstructed, which agree well with the theoretical value and simulation. The higher integral reflectivity of the HOPG crystal makes this method possible for single-shot measurement.

First functionality tests of a 64 × 64 pixel DSSC sensor module connected to the complete ladder readout

The European X-ray Free Electron Laser (XFEL.EU) will provide every 0.1 s a train of 2700 spatially coherent ultrashort X-ray pulses at 4.5 MHz repetition rate. The Small Quantum Systems (SQS) instrument and the Spectroscopy and Coherent Scattering instrument (SCS) operate with soft X-rays between 0.5 keV–6 keV. The DEPFET Sensor with Signal Compression (DSSC) detector is being developed to meet the requirements set by these two XFEL.EU instruments. The DSSC imager is a 1 mega-pixel camera able to store up to 800 single-pulse images per train. The so-called ladder is the basic unit of the DSSC detector. It is the single unit out of sixteen identical-units composing the DSSC-megapixel camera, containing all representative electronic components of the full-size system and allows testing the full electronic chain. Each DSSC ladder has a focal plane sensor with 128× 512 pixels. The read-out ASIC provides full-parallel readout of the sensor pixels. Every read-out channel contains an amplifier and an analog filter, an up-to 9 bit ADC and the digital memory. The ASIC amplifier have a double front-end to allow one to use either DEPFET sensors or Mini-SDD sensors. In the first case, the signal compression is a characteristic intrinsic of the sensor; in the second case, the compression is implemented at the first amplification stage. The goal of signal compression is to meet the requirement of single-photon detection capability and wide dynamic range. We present the first results of measurements obtained using a 64× 64 pixel DEPFET sensor attached to the full final electronic and data-acquisition chain.

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

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.

Chirped pulse amplification in an extreme-ultraviolet free-electron laser.

Chirped pulse amplification in optical lasers is a revolutionary technique, which allows the generation of extremely powerful femtosecond pulses in the infrared and visible spectral ranges. Such pulses are nowadays an indispensable tool for a myriad of applications, both in fundamental and applied research. In recent years, a strong need emerged for light sources producing ultra-short and intense laser-like X-ray pulses, to be used for experiments in a variety of disciplines, ranging from physics and chemistry to biology and material sciences. This demand was satisfied by the advent of short-wavelength free-electron lasers. However, for any given free-electron laser setup, a limit presently exists in the generation of ultra-short pulses carrying substantial energy. Here we present the experimental implementation of chirped pulse amplification on a seeded free-electron laser in the extreme-ultraviolet, paving the way to the generation of fully coherent sub-femtosecond gigawatt pulses in the water window (2.3–4.4 nm).

Normal Auger processes with ultrashort x-ray pulses in neon

Modern x-ray sources enable the production of coherent x-ray pulses with a pulse duration in the same order as the characteristic lifetimes of core-hole states of atoms and molecules. These pulses enable the manipulation of the core-hole population during Auger decay processes, modifying the lineshape of the electron spectra. In this work, we present a theoretical model to study those effects in Neon. We identify effects in the Auger-photoelectron coincidence spectrum due to the duration and intensity of the pulses. The normal Auger line-shape is recovered in Auger electron spectrum integrated over all photoelectron energies.

Particle-in-cell simulation of x-ray wakefield acceleration and betatron radiation in nanotubes

Though wakefield acceleration in crystal channels has been previously proposed, x-ray wakefield acceleration has only recently become a realistic possibility since the invention of the single-cycled optical laser compression technique. We investigate the acceleration due to a wakefield induced by a coherent, ultrashort x-ray pulse guided by a nanoscale channel inside a solid material. By two-dimensional particle in- cell computer simulations, we show that an acceleration gradient of TeV/cm is attainable. This is about 3 orders of magnitude stronger than that of the conventional plasma-based wakefield accelerations, which implies the possibility of an extremely compact scheme to attain ultrahigh energies. In addition to particle acceleration, this scheme can also induce the emission of high energy photons at ~O(10-100) MeV. Our simulations confirm such high energy photon emissions, which is in contrast with that induced by the optical laser driven wakefield scheme. In addition to this, the significantly improved emittance of the energetic electrons has been discussed.

Establishing nonlinearity thresholds with ultraintense X-ray pulses.

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.

Current status of the CXI beamline at the PAL-XFEL

The Pohang Accelerator Laboratory’s X-ray free electron laser (PAL-XFEL) is a research facility currently under construction. It will provide ultra-bright (1 × 1012 photons/pulse at 12.4 keV) and ultra-short (10 − 60 femtosecond) X-ray pulses. The CXI (coherent X-ray imaging) hard X-ray experimental station is designed to deliver brilliant hard X-rays (2 − 20.4 keV) and to measure diffraction signals with a forward scattering geometry. It will not only offer imaging studies of biological, chemical and physical samples with the “diffraction-before-destruction” scheme, but also be helpful in high-field hard X-ray physics and material science. The scientific programs are currently aimed at serial femtosecond crystallography (SFX) and coherent diffraction imaging (CDI) for bio specimens, nano materials, etc. In this paper, we describe the beamline layout, beam diagnostics, X-ray focusing optics, sample environments and detector system at the CXI experimental hutch.

XFEL data analysis for structural biology

X-ray Free Electron Lasers (XFELs) have advanced research in structure biology, by exploiting their ultra-short and bright X-ray pulses. The resulting “diffraction before destruction” experimental approach allows data collection to outrun radiation damage, a crucial factor that has often limited resolution in the structure determination of biological molecules. Since the first hard X-ray laser (the Linac Coherent Light Source (LCLS) at SLAC) commenced operation in 2009, serial femtosecond crystallography (SFX) has rapidly matured into a method for the structural analysis of nano- and micro-crystals. At the same time, single particle structure determination by coherent diffractive imaging, with one particle (such as a virus) per shot, has been under intense development. In this review we describe these applications of X-ray lasers in structural biology, with a focus particularly on aspects of data analysis for the computational research community.We summarize the key problems in data analysis and model reconstruction, and provide perspectives on future research using computational methods.

High-repetition-rate and high-photon-flux 70 eV high-harmonic source for coincidence ion imaging of gas-phase molecules.

Unraveling and controlling chemical dynamics requires techniques to image structural changes of molecules with femtosecond temporal and picometer spatial resolution. Ultrashort-pulse x-ray free-electron lasers have significantly advanced the field by enabling advanced pump-probe schemes. There is an increasing interest in using table-top photon sources enabled by high-harmonic generation of ultrashort-pulse lasers for such studies. We present a novel high-harmonic source driven by a 100 kHz fiber laser system, which delivers 1011 photons/s in a single 1.3 eV bandwidth harmonic at 68.6 eV. The combination of record-high photon flux and high repetition rate paves the way for time-resolved studies of the dissociation dynamics of inner-shell ionized molecules in a coincidence detection scheme. First coincidence measurements on CH3I are shown and it is outlined how the anticipated advancement of fiber laser technology and improved sample delivery will, in the next step, allow pump-probe studies of ultrafast molecular dynamics with table-top XUV-photon sources. These table-top sources can provide significantly higher repetition rates than the currently operating free-electron lasers and they offer very high temporal resolution due to the intrinsically small timing jitter between pump and probe pulses.

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

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.

TH-AB-209-07: High Resolution X-Ray-Induced Acoustic Computed Tomography

Purpose: X-ray radiographic absorption imaging is an invaluable tool in medical diagnostics, biology and materials science. However, the use of conventional CT is limited by two factors: the detection sensitivity to weak absorption material and the radiation dose from CT scanning. The purpose of this study is to explore X-ray induced acoustic computed tomography (XACT), a new imaging modality, which combines X-ray absorption contrast and high ultrasonic resolution to address these challenges. Methods: First, theoretical models was built to analyze the XACT sensitivity to X-ray absorption and calculate the minimal radiation dose in XACT imaging. Then, an XACT system comprised of an ultrashort X-ray pulse, a low noise ultrasound detector and a signal acquisition system was built to evaluate the X-ray induced acoustic signal generation. A piece of chicken bone and a phantom with two golden fiducial markers were exposed to 270 kVp X-ray source with 60 ns exposure time, and the X-ray induced acoustic signal was received by a 2.25MHz ultrasound transducer in 200 positions. XACT images were reconstructed by a filtered back-projection algorithm. Results: The theoretical analysis shows that X-ray induced acoustic signals have 100% relative sensitivity to X-ray absorption, but not to X-ray scattering. Applying this innovative technology to breast imaging, we can reduce radiation dose by a factor of 50 compared with newly FDA approved breast CT. The reconstructed images of chicken bone and golden fiducial marker phantom reveal that the spatial resolution of the built XACT system is 350µm. Conclusion: In XACT, the imaging sensitivity to X-ray absorption is improved and the imaging dose is dramatically reduced by using ultrashort pulsed X-ray. Taking advantage of the high ultrasonic resolution, we can also perform 3D imaging with a single X-ray pulse. This new modality has the potential to revolutionize x-ray imaging applications in medicine and biology.

Ultrafast spectroscopy: A glimpse of spin motion.

Ultrashort pulses of X-rays from a free-electron laser capture the spatiotemporal evolution of spins in the different crystallographic directions of a complex magnetic material.

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

We study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength of ( 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 . 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.