Hard X-ray Pulses Research Articles

A Highly Stable-Output Kilohertz Femtosecond Hard X-ray Pulse Source for Ultrafast X-ray Diffraction

Femtosecond hard X-ray pulses generated by laser-driven plasma sources are eminently suitable to probe structural dynamics due to the angstrom spatial resolution and sub-picosecond time resolution. However, the insufficient flux of X-ray photons and high pulse-to-pulse instability compared with the large-scale ultrashort X-ray source, such as X-ray free-electron laser and synchrotrons, largely restricts its applications. In this work, we have optimized automation control and mechanical designs to significantly enhance the reliability and photon flux in our femtosecond laser plasma-induced X-ray source. Specifically, the optimized source provides a reliable pulse-to-pulse stability with a fluctuation of less than 1% (root-mean-square) and a total flux of Cu-Kα X-ray photons above 1011 photons/s. To confirm its functionality, ultrafast X-ray diffraction experiments are conducted on two different samples and the high consistency with previous results verifies the system’s superior performance.

Underdamped longitudinal soft modes in ionic crystallites-lattice and charge motions observed by ultrafast x-ray diffraction.

Soft modes in crystals are lattice vibrations with frequencies that decrease and eventually vanish as the temperature approaches a critical point, e.g., a structural change due to a phase transition. In ionic para- or ferroelectric materials, the frequency decrease is connected with a diverging electric susceptibility and, for infrared active modes, a strong increase in oscillator strength. The traditional picture describes soft modes as overdamped transverse optical phonons of a hybrid vibrational-electronic character. In this context, potassium dihydrogen phosphate (KH2PO4, KDP) has been studied for decades as a prototypical material with, however, inconclusive results regarding the soft modes in its para- and ferroelectric phase. There are conflicting assignments of soft-mode frequencies and damping parameters. We report the first observation of a longitudinal underdamped soft mode in paraelectric KDP. Upon impulsive femtosecond Raman excitation of coherent low-frequency phonons in the electronic ground state of KDP crystallites, transient powder diffraction patterns are recorded with femtosecond hard x-ray pulses. Electron density maps derived from the x-ray data reveal oscillatory charge relocations over interatomic distances, much larger than the sub-picometer nuclear displacements, a direct hallmark of soft-mode behavior. The strongly underdamped character of the soft mode manifests in charge oscillations persisting for more than 10 ps. The soft-mode frequency decreases from 0.55 THz at T = 295 K to 0.39 THz at T = 175 K. An analysis of the Raman excitation conditions in crystallites and the weak damping demonstrate a longitudinal character. Our results extend soft-mode physics well beyond the traditional picture and pave the way for an atomic-level characterization of soft modes.

Resonantly Enhanced Difference-Frequency Generation in the Core X-ray Absorption of Molecules.

We use real-time time-dependent density functional theory simulations to numerically demonstrate that resonantly enhanced difference-frequency generation (re-DFG) involving intense ultrashort coherent X-ray pulses can selectively excite core states of atoms in molecules. As a model case, we evaluate the spectral selectivity of re-DFG excitation of the oxygen K-edge by illumination of a single gas-phase water molecule with two-color X-ray pulses of different photon energies and durations. The re-DFG excitation is further probed by a small delayed pulse with central photon energy resonant with the oxygen K-edge peak absorption line. Based on these results, we anticipate that highly selective excitation by re-DFG X-ray nonlinear processes might be achieved in more complex molecular systems and bulk materials by using highly penetrating two-color hard X-ray pulses, with extensive applications.

Precise Timing and Phase-resolved Spectroscopy of the Young Pulsar J1617–5055 with NuSTAR

Abstract We report on a Nuclear Spectroscopic Telescope Array (NuSTAR) observation of the young, energetic pulsar PSR J1617–5055. Parkes Observatory 3 GHz radio observations of the pulsar (taken about 7 yr before the NuSTAR observations) are also reported here. NuSTAR detected pulsations at a frequency of f ≈ 14.4 Hz (P ≈ 69.44 ms) and, in addition, the observation was long enough to measure the source’s frequency derivative, f ̇ ≈ − 2.8 × 10 − 11 Hz s−1. We find that the pulsar shows one peak per period at both hard X-ray and radio wavelengths, but that the hard X-ray pulse is broader (having a duty cycle of ∼0.7), than the radio pulse (having a duty cycle of ∼0.08). Additionally, the radio pulse is strongly linearly polarized. J1617's phase-integrated hard X-ray spectrum is well fit by an absorbed power-law model, with a photon index Γ = 1.59 ± 0.02. The hard X-ray pulsations are well described by three Fourier harmonics, and have a pulsed fraction that increases with energy. We also fit the phase-resolved NuSTAR spectra with an absorbed power-law model in five phase bins and find that the photon index varies with phase from Γ = 1.52 ± 0.03 at phases around the flux maximum to Γ = 1.79 ± 0.06 around the flux minimum. Last, we compare our results with other pulsars whose magnetospheric emission is detected at hard X-ray energies and find that, similar to previous studies, J1617's hard X-ray properties are more similar to the MeV pulsars than the GeV pulsars.

Nonuniform Flow Dynamics Probed by Nanosecond X-Ray Speckle Visibility Spectroscopy.

We report observations of nanosecond nonuniform colloidal dynamics in a free flowing liquid jet using ultrafast x-ray speckle visibility spectroscopy. Utilizing a nanosecond double-bunch mode, the Linac Coherent Light Source free electron laser produced pairs of femtosecond coherent hard x-ray pulses. By exploring anisotropy in the visibility of summed speckle patterns which relates to the correlation functions, we evaluate not only the average particle flow rate in a colloidal nanoparticle jet, but also the nonuniform flow field within. The methodology presented here establishes the foundation for the study of nano- and atomic-scale inhomogeneous fluctuations in complex matter using x-ray free electron laser sources.

AstroSat-CZTI as a hard X-ray pulsar monitor

The Cadmium Zinc Telluride Imager (CZTI) is an imaging instrument onboard AstroSat. This instrument operates as a nearly open all-sky detector above ~60 keV, making possible long integrations irrespective of the spacecraft pointing. We present a technique based on the AstroSat-CZTI data to explore the hard X-ray characteristics of the $\gamma$-ray pulsar population. We report highly significant ($\sim 30\sigma$) detection of hard X-ray (60--380 keV) pulse profile of the Crab pulsar using $\sim$5000 ks of CZTI observations within 5 to 70 degrees of Crab position in the sky, using a custom algorithm developed by us. Using Crab as our test source, we estimate the off-axis sensitivity of the instrument and establish AstroSat-CZTI as a prospective tool in investigating hard X-ray characteristics of $\gamma$-ray pulsars as faint as 10 mCrab.

Optics-on-a-chip for ultrafast manipulation of 350-MHz hard x-ray pulses.

Microelectromechanical systems (MEMS) are miniature devices integrated into a vast range of industrial and consumer applications. Optical MEMS are developed for dynamic spatiotemporal control in lightwave manipulation and communication as modulators, switches, multiplexers, spectrometer, etc. However, they have not been shown to function similarly in sub-nm wavelength regimes, namely, with hard x-rays, as high-brilliance pulsed x-rays have proven powerful for addressing challenges in time-domain science, from energy conversion to neurobiological control. While desirable temporal properties of x-ray pulses can be enhanced by optics, conventional x-ray optics are inherently massive in size, hence, never dynamic. We demonstrate highly ultrafast x-ray optics-on-a-chip based on MEMS capable of modulating hard x-ray pulses exceeding 350 MHz, 103× higher than any other mechanical modulator, with a pulse purity >106 without compromising the spectral brilliance. Moreover, the timing characteristics of the devices can be tuned on-the-fly to deliver optimal pulse properties to create a host of dynamic x-ray instruments and applications, impossible with traditional optics of 109× bulkier and more massive. The advent of the ultrafast optics-on-a-chip heralds a new paradigm of x-ray photonics, time-domain science, and accelerator diagnostics, especially at not only the future-generation light sources that offer coherent and high-frequency pulses but also lab-based facilities that normally do not offer timing structures.

Suppression of thermal nanoplasma emission in clusters strongly ionized by hard x-rays

Using electron and ion spectroscopy, we studied the electron and nuclear dynamics in ∼50 000-atom large krypton clusters, following excitation with an intense hard x-ray pulse. Beyond the single pulse experiment, we also present the results of a time-resolved, x-ray pump–near-infrared probe measurement that allows one to learn about the time evolution of the system. After core ionization of the atoms by x-ray photons, trapped Auger and secondary electrons form a nanoplasma in which the krypton ions are embedded, according to the already published scenario. While the ion data show expected features, the electron emission spectra miss the expected pump–probe delay-dependent enhancement except for a slight enhancement in the energy range below 2 eV. Theoretical simulations help to reveal that, due to the deep trapping potential of the ions during the long time expansion accompanied by electron–ion recombination, thermal emission from the transient nanoplasma becomes quenched.

A self-referenced in-situ arrival time monitor for X-ray free-electron lasers.

We present a novel, highly versatile, and self-referenced arrival time monitor for measuring the femtosecond time delay between a hard X-ray pulse from a free-electron laser and an optical laser pulse, measured directly on the same sample used for pump-probe experiments. Two chirped and picosecond long optical supercontinuum pulses traverse the sample with a mutually fixed time delay of 970 fs, while a femtosecond X-ray pulse arrives at an instant in between both pulses. Behind the sample the supercontinuum pulses are temporally overlapped to yield near-perfect destructive interference in the absence of the X-ray pulse. Stimulation of the sample with an X-ray pulse delivers non-zero contributions at certain optical wavelengths, which serve as a measure of the relative arrival time of the X-ray pulse with an accuracy of better than 25 fs. We find an excellent agreement of our monitor with the existing timing diagnostics at the SACLA XFEL with a Pearson correlation value of 0.98. We demonstrate a high sensitivity to measure X-ray pulses with pulse energies as low as 30 upmu J. Using a free-flowing liquid jet as interaction sample ensures the full replacement of the sample volume for each X-ray/optical event, thus enabling its utility even at MHz repetition rate XFEL sources.

Refractive Guide Switching a Regenerative Amplifier Free-Electron Laser for High Peak and Average Power Hard X Rays.

We present an x-ray regenerative amplifier free-electron laser design capable of producing fully coherent hard x-ray pulses across a broad tuning range at a high steady state repetition rate. The scheme leverages a strong undulator taper and an apertured diamond output-coupling cavity crystal to produce both high peak and average spectral brightness radiation that is 2 to 3 orders of magnitude greater than conventional single-pass self-amplified spontaneous emission free-electron laser amplifiers. Refractive guiding in the postsaturation regime is found to play a key role in passively controlling the stored cavity power. The scheme is explored both analytically and numerically in the context of the Linac Coherent Light Source II High Energy upgrade.

Thermal loading on crystals in an x-ray free-electron laser oscillator

X-ray free electron laser oscillators (XFELO) is future light source to produce fully coherent hard X-ray pulses. The X-rays circulate in an optical cavity built from multiple Bragg reflecting mirrors, which has a high reflectance in a bandwidth of ten meV level. The X-ray crystal mirrors exposed to intense X-ray beams in the cavity are subjects to thermal deformations that shift and distort the Bragg reflection. Therefore, the stability of the XFELO operation relies on the abilities of mirrors to preserve the Bragg reflection under such heat load. A new approach was used to analyze the heat load of mirrors and the XFELO operation. The essential light-matter interaction is simulated by the GEANT4 with a dedicated Bragg-reflection physical process to obtain the precise absorption information of the XFELO pulse in the crystals. The transient thermal conduction is analyzed by the finite-element analysis software upon the energy absorption information extract from GEANT4 simulation. A simplified heat-load model is then developed to integrate the heat load in the XFELO. With the help of the heat-load model, the analysis of XFELO operating with several cryogenically cooled diamond mirrors is conducted. The results indicate that the heat load would induce an oscillation when XFELO operates without enough cooling.

Novel Clues to the Physics of Magnetars as Probed with Detailed Pulse-Timing Studies

AbstractBroadband X-ray data of five magnetars show that their hard X-ray pulses suffer periodic phase modulations, at a period ∼ 104 times their pulse period. The phenomenon is interpreted as a result of free precession of neutron stars that are prolately deformed to an asphericity of ∼ 10−4, by the magnetic stress of toroidal fields reaching ∼ 1016 G. The behavior is absent in their soft X-ray pulses, probably due to a higher emission symmetry. The ultra-high toroidal fields, considered common to magnetars, may persist longer than their dipole fields.

A MHz-repetition-rate hard X-ray free-electron laser driven by a superconducting linear accelerator

The European XFEL is a hard X-ray free-electron laser (FEL) based on a high-electron-energy superconducting linear accelerator. The superconducting technology allows for the acceleration of many electron bunches within one radio-frequency pulse of the accelerating voltage and, in turn, for the generation of a large number of hard X-ray pulses. We report on the performance of the European XFEL accelerator with up to 5,000 electron bunches per second and demonstrating a full energy of 17.5 GeV. Feedback mechanisms enable stabilization of the electron beam delivery at the FEL undulator in space and time. The measured FEL gain curve at 9.3 keV is in good agreement with predictions for saturated FEL radiation. Hard X-ray lasing was achieved between 7 keV and 14 keV with pulse energies of up to 2.0 mJ. Using the high repetition rate, an FEL beam with 6 W average power was created.

Thermomechanical response of thickly tamped targets and diamond anvil cells under pulsed hard x-ray irradiation

In the laboratory study of extreme conditions of temperature and density, the exposure of matter to high intensity radiation sources has been of central importance. Here, we interrogate the performance of multi-layered targets in experiments involving high intensity, hard x-ray irradiation, motivated by the advent of extremely high brightness hard x-ray sources, such as free electron lasers and 4th-generation synchrotron facilities. Intense hard x-ray beams can deliver significant energy in targets having thick x-ray transparent layers (tampers) around samples of interest for the study of novel states of matter and materials’ dynamics. Heated-state lifetimes in such targets can approach the microsecond level, regardless of radiation pulse duration, enabling the exploration of conditions of local thermal and thermodynamic equilibrium at extreme temperature in solid density matter. The thermal and mechanical responses of such thick layered targets following x-ray heating, including hydrodynamic relaxation and heat flow on picosecond to millisecond timescales, are modeled using radiation hydrocode simulation, finite element analysis, and thermodynamic calculations. Assessing the potential for target survival over one or more exposures and resistance to damage arising from heating and resulting mechanical stresses, this study doubles as an investigation into the performance of diamond anvil high pressure cells under high x-ray fluences. Long used in conjunction with synchrotron x-ray radiation and high power optical lasers, the strong confinement afforded by such cells suggests novel applications at emerging high intensity x-ray facilities and new routes to studying thermodynamic equilibrium states of warm, very dense matter.

Observation of the molecular response to light upon photoexcitation

When a molecule interacts with light, its electrons can absorb energy from the electromagnetic field by rapidly rearranging their positions. This constitutes the first step of photochemical and photophysical processes that include primary events in human vision and photosynthesis. Here, we report the direct measurement of the initial redistribution of electron density when the molecule 1,3-cyclohexadiene (CHD) is optically excited. Our experiments exploit the intense, ultrashort hard x-ray pulses of the Linac Coherent Light Source (LCLS) to map the change in electron density using ultrafast x-ray scattering. The nature of the excited electronic state is identified with excellent spatial resolution and in good agreement with theoretical predictions. The excited state electron density distributions are thus amenable to direct experimental observation.

Applications and Limits of Time-to-Energy Mapping of Protein Crystal Diffraction Using Energy-Chirped Polychromatic XFEL Pulses

A broadband energy-chirped hard X-ray pulse has been demonstrated at the SwissFEL (free electron laser) with up to 4% bandwidth. We consider the characteristic parameters for analyzing the time dependence of stationary protein diffraction with energy-chirped pulses. Depending on crystal mosaic spread, convergence, and recordable resolution, individual reflections are expected to spend at least ≈ 50 attoseconds and up to ≈ 8 femtoseconds in reflecting condition. Using parameters for a chirped XFEL pulse obtained from simulations of 4% bandwidth conditions, ray-tracing simulations have been carried out to demonstrate the temporal streaking across individual reflections and resolution ranges for protein crystal diffraction. Simulations performed at a higher chirp (10%) emphasize the importance of chirp magnitude that would allow increased observation statistics for the temporal separation of individual reflections for merging and structure determination. Finally, we consider the fundamental limitation for obtaining time-dependent observations using chirped pulse diffraction. We consider the maximum theoretical time resolution achievable to be on the order of 50–200 as from the instantaneous bandwidth of the chirped SASE pulse. We then assess the ability to propagate ultrafast optical pulses for pump-probe cross-correlation under characteristic conditions of material dispersion; in this regard, the limiting factors for time resolution scale with crystal thickness. Crystals that are below a few microns in size will be necessary for subfemtosecond time resolution.

Attosecond Coherence Time Characterization in Hard X-Ray Free-Electron Laser

One of the key challenges in scientific researches based on free-electron lasers (FELs) is the characterization of the coherence time of the ultra-fast hard x-ray pulse, which fundamentally influences the interaction process between x-rays and materials. Conventional optical methods, based on autocorrelation, are very difficult to realize due to the lack of mirrors. Here, we experimentally demonstrate a novel method which yields a coherence time of 174.7 attoseconds for the 6.92 keV FEL pulses at the Linac Coherent Light Source. In our experiment, a phase shifter is adopted to control the cross-correlation between x-ray and microbunched electrons. This approach provides critical diagnostics for the temporal coherence of x-ray FELs and is universal for general machine parameters; applicable for wide range of photon energy, radiation brightness, repetition rate and FEL pulse duration.

Polarization control of an x-ray free electron laser oscillator

High-intensity, fully coherent x-ray pulse with a tunable polarization over a wide spectral range is of great importance to many experiments. In this paper, we propose a tapered crossed-polarized undulator configuration for an x-ray free electron laser oscillator (XFELO) to produce arbitrarily polarized x-ray pulses in the hard x-ray region. A numerical example utilizing the parameters of the Shanghai High-Repetition-Rate XFEL and Extreme Light Facility (SHINE) is presented to demonstrate the generation of polarization controllable, fully coherent hard x-ray pulses with 99.9% polarization degree and 20 kHz polarization switching rate. The analysis presents that this scheme holds the possibility to be used in an energy tunable XFELO built from multiple Bragg mirrors.

Effect of high slice energy spread of an electron beam on the generation of isolated, terawatt, attosecond X-ray free-electron laser pulse

Attosecond (asec) X-ray free-electron laser (XFEL) has attracted considerable interest over the past years. Nowadays typical XFEL application experiments demand 1010–1011 photons per pulse, which corresponds to a peak power of terawatts (TW) in case of asec hard X-ray pulse. To the realization of such TW asec-XFEL pulse, however, the unavoidable increase of slice energy spread (SES) due to laser heater, which is commonly used to mitigate the micro-bunching instability (MBI), would be a major obstacle. To deal with this problem, the effect of such a SES is investigated in this work. The results reveal that (1) SES of a current spike is linearly proportional to the peak current of a current spike in an electron beam, (2) surprisingly, this linearity is independent of the wavelength of an energy modulation driving laser which is used to make a current spike and (3) the gain length of current spike in the undulator is sensitive to the initial SES, so there is an optimal peak current of the current spike for successful FEL lasing process. Utilizing these characteristics, a series of simulations with parameters for Pohang Accelerator Laboratory X-ray Free Electron Laser was carried out to demonstrate that an isolated, TW asec-XFEL pulse can be generated even when the SES is increased due to the usage of laser heater to prevent the MBI in the XFEL. We show that an isolated X-ray pulse with >1 TW and a pulse duration of 73 as (~3 × 1010 photons/pulse at 12.4 keV or 0.1 nm) can be generated by using ten current spikes with optimal peak current. It becomes clear for the first time that the disadvantage from the increased SES can be indeed overcome.

Energy fluence measurement for pulse hard X-ray

<sec>Pulsed high-energy fluence X-ray source is based on the “Flash II” accelerator. It can be used to carry out effect vulnerability and sensitivity test of unit level system generated electromagnetic pulse (SGEMP). The energy fluence of pulsed hard X-ray is a main parameter of the equipment beam. At present, theoretical calculation method is widely used. Energy fluence can be calculated according to the dose, energy spectrum and energy absorption coefficient of each energy segment.</sec><sec>The principle measuring energy fluence of pulsed hard X-ray by total absorption method is introduced. The photoelectric cell with lutetium silicate (LSO) scintillator is selected as a core component of the detection system, and the measurement system is developed. It is composed of scintillation detector, LSO scintillator, dimmer film, photon collimator, visible light shielding material, power supply and signal collecting system. The conversion coefficient between the incident photon energy and the waveform parameter is calibrated by a standard X-ray source. </sec><sec>The energy fluence measurement experiment is carried out with the high-energy beam source of the “Flash II” accelerator as an experimental platform. In order to meet the requirements of the effect test experiments, the series diode structure is used in the accelerator for forming a high strength and large area uniform X-ray source. In the experiment, the LiF TLD is located in the front of the phototube and used to monitor the dose. According to the measured waveform, the actual energy of the incident photons is calculated. Combined with the receiving area of incident photons, the energy fluence of pulsed hard X-ray is calculated. The average measured value is 35.9 mJ/cm<sup>2</sup> in 5 consecutive experiments. Energy fluence calculated from the measured dose and energy spectrum is 39.8 mJ/cm<sup>2</sup>. The results of the two methods are compared.</sec><sec>It can be found that the experimental result is about 9.8% smaller than the theoretical value. The reasons are as follows. According to the law of exponential decay of rays in matter, in fact, the scintillator cannot absorb all the rays, and some of the rays can penetrate through, the energy of these rays cannot be detected, and thus giving rise to small experimental value. Due to the limited energy point of quasi-monoenergetic source, the sensitivity under the mean photon energy is taken as the sensitivity of the detector, and therefore there is a certain degree of uncertainty. </sec><sec>The successful application of the measurement technology provides a good experimental method for the following similar research, and can also provide a reference for X-ray intensity analysis.</sec>