X-ray Laser Pulses Research Articles

MolDStruct: Modeling the dynamics and structure of matter exposed to ultrafast x-ray lasers with hybrid collisional-radiative/molecular dynamics.

We describe a method to compute photon-matter interaction and atomic dynamics with x-ray lasers using a hybrid code based on classical molecular dynamics and collisional-radiative calculations. The forces between the atoms are dynamically determined based on changes to their electronic occupations and the formation of a free electron cloud created from the irradiation of photons in the x-ray spectrum. The rapid transition from neutral solid matter to dense plasma phase allows the use of screened potentials, reducing the number of non-bonded interactions. In combination with parallelization through domain decomposition, the hybrid code handles large-scale molecular dynamics and ionization. This method is applicable for large enough samples (solids, liquids, proteins, viruses, atomic clusters, and crystals) that, when exposed to an x-ray laser pulse, turn into a plasma in the first few femtoseconds of the interaction. We present four examples demonstrating the applicability of the method. We investigate the non-thermal heating and scattering of bulk water and damage-induced dynamics of a protein crystal using an x-ray pump-probe scheme. In both cases, we compare to the experimental data. For single particle imaging, we simulate the ultrafast dynamics of a methane cluster exposed to a femtosecond x-ray laser. In the context of coherent diffractive imaging, we study the fragmentation as given by an x-ray pump-probe setup to understand the evolution of radiation damage in the time range of hundreds of femtoseconds.

Harmonic generation and modulation based on intense x-ray interaction with crystal-like structures

The rapid advancement of x-ray free-electron laser technology facilitates the attainment of relativistic attosecond x-ray laser pulses in the future. It could serve as an ideal source to explore x-ray-driven high-energy density physics, such as particle acceleration and secondary radiation at solid densities. Here, utilizing particle-in-cell simulations, we systematically investigate high-order harmonic generation (HHG) based on intense x-ray lasers interacting with crystal-like structures. We find that the nonlinear interaction induces significant HHGs that are highly modulated due to the periodic target structure. By varying the spacing of the density spikes, the resonant conditions are tuned such that the efficiency of HHGs is drastically different. While each order of harmonic has multiple propagating directions, we find that the intensity can be enhanced significantly in the non-Bragg condition case than that in the Bragg case. The results indicate an approach to manipulate HHG emission driven by strong-field x-rays.

Relativistic and nondipole effects in multiphoton ionization of hydrogen by a high-intensity x-ray laser pulse

Relativistic and nondipole effects in multiphoton ionization of hydrogen by a high-intensity x-ray laser pulse

Sub-nanometer scale depth patterning on sapphire crystal by femtosecond soft x-ray laser pulse irradiation.

Damage thresholds and structures on a metal aluminum and an aluminum oxide crystal induced by the soft x-ray free electron laser irradiations were evaluated. Distinctive differences in damage thresholds and structures were observed for these materials. On the aluminum oxide crystal surface, in particular, a novel, to the best of our knowledge, surface processing, which we suggest defining as "peeling," was recognized. Surface structures formed by peeling had extremely shallow patterning of sub-nanometer depth. For the newly observed peeling process, we proposed a scission of chemical bond, i.e., binding energy model, in the crystal.

Dynamic optical spectroscopy and pyrometry of static targets under optical and x-ray laser heating at the European XFEL

Experiments accessing extreme conditions at x-ray free electron lasers (XFELs) involve rapidly evolving conditions of temperature. Here, we report time-resolved, direct measurements of temperature using spectral streaked optical pyrometry of x-ray and optical laser-heated states at the High Energy Density instrument of the European XFEL. This collection of typical experiments, coupled with numerical models, outlines the reliability, precision, and meaning of time dependent temperature measurements using optical emission at XFEL sources. Dynamic temperatures above 1500 K are measured continuously from spectrally- and temporally-resolved thermal emission at 450–850 nm, with time resolution down to 10–100 ns for 1–200 μs streak camera windows, using single shot and integrated modes. Targets include zero-pressure foils free-standing in air and in vacuo, and high-pressure samples compressed in diamond anvil cell multi-layer targets. Radiation sources used are 20-fs hard x-ray laser pulses at 17.8 keV, in single pulses or 2.26 MHz pulse trains of up to 30 pulses, and 250-ns infrared laser single pulses. A range of further possibilities for optical measurements of visible light in x-ray laser experiments using streak optical spectroscopy are also explored, including for the study of x-ray induced optical fluorescence, which often appears as background in thermal radiation measurements. We establish several scenarios where combined emissions from multiple sources are observed and discuss their interpretation. Challenges posed by using x-ray lasers as non-invasive probes of the sample state are addressed.

Coherent population transfer in the interaction of five-state nuclei with x-ray lasers using chain-STIRAP technique

The complete population transfer from the first state to the fifth one in a five-state nuclear system that interacts with four x-ray laser pulses has been theoretically studied using the chain-STIRAP technique. In this scheme, it is assumed that the accelerated nucleus interacts with four x-ray laser pulses, and the relativistic factor is adjusted so that the resonance condition is established between the x-ray laser frequencies and the transition frequency of the nucleus. In this study, by establishing the adiabatic condition, the Hamiltonian of the system remains in the dark state. Therefore, the second and fourth states are not populated during the time evolution. Also, to eliminate the population of the third state during the interaction, the middle pulses are considered more significant compared to the first and last pulses. For the numerical study, 168Er is considered and, it is shown that the population is completely transferred from the first state to the fifth state.

Composite pulses for population transfer in the interaction of two-level nuclear systems with X-ray laser pulses

Composite pulses for population transfer in the interaction of two-level nuclear systems with X-ray laser pulses

Extreme focusing of high power x-ray lasers to relativistic intensity with a concave plasma lens

The intensity of present x-ray lasers is still far from relativistic due to equipment damage by the powerful radiation involved in the generation process. We propose to use a microscopic concave plasma lens to tightly focus terawatt x-ray pulses to relativistic intensity by avoiding the destructive instabilities arising from the laser-plasma interaction in the focusing process. Three-dimensional particle-in-cell simulations show that an intense x-ray laser pulse can be focused to a tiny spot of the wavelength scale at ultrahigh intensity while well preserving its original spatiotemporal profile. The resulting pulse can exceed the relativistic intensity threshold [$(1.37\ifmmode\times\else\texttimes\fi{}{10}^{24}/{\ensuremath{\lambda}}_{\mathrm{nm}}^{2})\phantom{\rule{3.33333pt}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$, with ${\ensuremath{\lambda}}_{\mathrm{nm}}$ being the wavelength normalized by nanometers] by two orders of magnitude. Such intense nano-sized x-ray pulses can be useful for exploring nonlinear phenomena in the strong-field quantum electrodynamics regime, as well as in high-energy-density science and astrophysics.

Ionization of Xenon Clusters by a Hard X-ray Laser Pulse

Ultrashort pulse X-ray free electron lasers (XFFLs) provided us with an unprecedented regime of X-ray intensities, revolutionizing ultrafast structure determination and paving the way to the novel field of non-linear X-ray optics. While pioneering studies revealed the formation of a nanoplasma following the interaction of an XFEL pulse with nanometer-scale matter, nanoplasma formation and disintegration processes are not completely understood, and the behavior of trapped electrons in the electrostatic potential of highly charged species is yet to be decrypted. Here we report the behavior of the nanoplasma created by a hard X-ray pulse interacting with xenon clusters by using electron and ion spectroscopy. To obtain a deep insight into the formation and disintegration of XFEL-ignited nanoplasma, we studied the XFEL-intensity and cluster-size dependencies of the ionization dynamics. We also present the time-resolved data obtained by a near-infrared (NIR) probe pulse in order to experimentally track the time evolution of plasma electrons distributed in the XFEL-ignited nanoplasma. We observed an unexpected time delay dependence of the ion yield enhancement due to the NIR pulse heating, which demonstrates that the plasma electrons within the XFEL-ignited nanoplasma are inhomogeneously distributed in space.

Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice

Recent experiments continue to find evidence for a liquid-liquid phase transition (LLPT) in supercooled water, which would unify our understanding of the anomalous properties of liquid water and amorphous ice. These experiments are challenging because the proposed LLPT occurs under extreme metastable conditions where the liquid freezes to a crystal on a very short time scale. Here, we analyze models for the LLPT to show that coexistence of distinct high-density and low-density liquid phases may be observed by subjecting low-density amorphous (LDA) ice to ultrafast heating. We then describe experiments in which we heat LDA ice to near the predicted critical point of the LLPT by an ultrafast infrared laser pulse, following which we measure the structure factor using femtosecond x-ray laser pulses. Consistent with our predictions, we observe a LLPT occurring on a time scale < 100 ns and widely separated from ice formation, which begins at times >1 μs.

Decreasing ultrafast x-ray pulse durations with saturable absorption and resonant transitions.

Saturable absorption is a nonlinear effect where a material's ability to absorb light is frustrated due to a high influx of photons and the creation of electron vacancies. Experimentally induced saturable absorption in copper revealed a reduction in the temporal duration of transmitted x-ray laser pulses, but a detailed account of changes in opacity and emergence of resonances is still missing. In this computational work, we employ nonlocal thermodynamic equilibrium plasma simulations to study the interaction of femtosecond x rays and copper. Following the onset of frustrated absorption, we find that a K-M resonant transition occurring at highly charged states turns copper opaque again. The changes in absorption generate a transient transparent window responsible for the shortened transmission signal. We also propose using fluorescence induced by the incident beam as an alternative source to achieve shorter x-ray pulses. Intense femtosecond x rays are valuable to probe the structure and dynamics of biological samples or to reach extreme states of matter. Shortened pulses could be relevant for emerging imaging techniques.

Molecular photodissociation dynamics revealed by Coulomb explosion imaging.

Coulomb explosion imaging (CEI) methods are finding ever-growing use as a means of exploring and distinguishing the static stereo-configurations of small quantum systems (molecules, clusters, etc). CEI experiments initiated by ultrafast (femtosecond-duration) laser pulses also allow opportunities to track the time-evolution of molecular structures, and thereby advance understanding of molecular fragmentation processes. This Perspective illustrates two emerging families of dynamical studies. 'One-colour' studies (employing strong field ionisation driven by intense near infrared or single X-ray or extreme ultraviolet laser pulses) afford routes to preparing multiply charged molecular cations and exploring how their fragmentation progresses from valence-dominated to Coulomb-dominated dynamics with increasing charge and how this evolution varies with molecular size and composition. 'Two-colour' studies use one ultrashort laser pulse to create electronically excited neutral molecules (or monocations), whose structural evolution is then probed as a function of pump-probe delay using an ultrafast ionisation pulse along with time and position-sensitive detection methods. This latter type of experiment has the potential to return new insights into not just molecular fragmentation processes but also charge transfer processes between moieties separating with much better defined stereochemical control than in contemporary ion-atom and ion-molecule charge transfer studies.

Exploring fingerprints of ultrafast structural dynamics in molecular solutions with an X-ray laser.

We apply ultrashort X-ray laser pulses to track optically excited structural dynamics of [Ir2(dimen)4]2+ molecules in solution. In our exploratory study we determine angular correlations in the scattered X-rays, which comprise a complex fingerprint of the ultrafast dynamics. Model-assisted analysis of the experimental correlation data allows us to elucidate various aspects of the photoinduced changes in the excited molecular ensembles. We unambiguously identify that in our experiment the photoinduced transition dipole moments in [Ir2(dimen)4]2+ molecules are oriented perpendicular to the Ir-Ir bond. The analysis also shows that the ground state conformer of [Ir2(dimen)4]2+ with a larger Ir-Ir distance is mostly responsible for the formation of the excited state. We also reveal that the ensemble of solute molecules can be characterized with a substantial structural heterogeneity due to solvent influence. The proposed X-ray correlation approach offers an alternative path for studies of ultrafast structural dynamics of molecular ensembles in the liquid and gas phases.

Femtosecond-Terawatt Hard X-Ray Pulse Generation with Chirped Pulse Amplification on a Free Electron Laser.

Advances of high intensity lasers have opened up the field of strong field physics and led to a broad range of technological applications. Recent x-ray laser sources and optics development makes it possible to obtain extremely high intensity and brightness at x-ray wavelengths. In this Letter, we present a system design that implements chirped pulse amplification for hard x-ray free electron lasers. Numerical modeling with realistic experimental parameters shows that near-transform-limit single-femtosecond hard x-ray laser pulses with peak power exceeding 1TW and brightness exceeding 4×10^{35} s^{-1} mm^{-2} mrad^{-2}0.1% bandwdith^{-1} can be consistently generated. Realization of such beam qualities is essential for establishing systematic and quantitative understanding of strong field x-ray physics and nonlinear x-ray optics phenomena.

Delayed Onset and Directionality of X-Ray-Induced Atomic Displacements Observed on Subatomic Length Scales.

Transient structural changes of Al_{2}O_{3} on subatomic length scales following irradiation with an intense x-ray laser pulse (photon energy: 8.70keV; pulse duration: 6fs; fluence: 8×10^{2} J/cm^{2}) have been investigated by using an x-ray pump x-ray probe technique. The measurement reveals that aluminum and oxygen atoms remain in their original positions by ∼20 fs after the intensity maximum of the pump pulse, followed by directional atomic displacements at the fixed unit cell parameters. By comparing the experimental results and theoretical simulations, we interpret that electron excitation and relaxation triggered by the pump pulse modify the potential energy surface and drives the directional atomic displacements. Our results indicate that high-resolution x-ray structural analysis with the accuracy of 0.01Å is feasible even with intense x-ray pulses by making the pulse duration shorter than the timescale needed to complete electron excitation and relaxation processes, which usually take up to a few tens of femtoseconds.

Hard x-ray intensity autocorrelation using direct two-photon absorption

The authors show a direct characterization of 9-keV x-ray laser pulse duration and find that temporal shapes of fluctuating ultrashort x-ray pulses can be tailored through Bragg diffraction in perfect crystals.

Online single-shot characterization of ultrafast pulses from high-gain free-electron lasers

X-ray free-electron lasers (FELs) provide cutting-edge tools for fundamental researches to study nature down to the atomic level at a time-scale that fits this resolution. A precise knowledge of temporal information of FEL pulses is the central issue for its applications. Here we proposed and demonstrated a novel method to determine the FEL temporal profiles online. This robust method, designed for ultrafast FELs, allows researchers to acquire real-time longitudinal profiles of FEL pulses as well as their arrive times with respect to the external optical laser with a resolution better than 6 fs. Based on this method, we can also directly measure various properties of FEL pulses and correlations between them online. This helps us to further understand the FEL lasing processes and realize the generation of stable, nearly fully coherent soft X-ray laser pulses at the Shanghai Soft X-ray FEL facility. This method will enhance the experimental opportunities for ultrafast science in various areas.

X-ray free-electron laser heating of water at picosecond time scale

Split-pulse x-ray photon correlation spectroscopy using x-ray free-electron laser is a promising tool to probe atomic dynamics in liquid and soft-matter in picosecond time scale, which has been accessible only by spectroscopy. However, sample heating by x-ray beam is a major obstacle for this technique. Using molecular dynamics and the two-temperature model we examine the atomic level response of water to x-ray laser pulse at picosecond time scale and compare with observations from recent x-ray free-electron laser experiments. We investigate the effects of the heating due to x-ray laser pulses of different energies and the effects of the heat dissipation on the structure and dynamics of water through the atomic density correlation and the dynamic structure factor. Our results indicate, in agreement with experiment that in addition to the beam energy the time delay between the two pulses is a critical factor for obtaining reliable information on the atomic level dynamics of water.

Superposition of nuclear states in multi-lambda systems using x-ray laser pulses

Nuclear-state population transfer in the multi-lambda systems with N = 5 that interact with four x-ray laser pulses are investigated theoretically. By using the coincident pulses and stimulated Raman adiabatic passage (STIRAP) techniques, the population transfer from one initially populated ground state to an arbitrary coherent superposition of other ground states. Since the frequency of currently available x-ray lasers is lower than the gamma rays, in this method, x-ray laser pulses with different frequencies are interacting with the accelerated nuclei. We employ the Morris-Shore transformation to reduce the five-states system to two separate three-state and two-state linkage. The required laser intensities were calculated, which satisfy the conditions of coincident pulses and multi-lambda STIRAP techniques. Considering the spontaneous emission from excited states, the master equation has to be used for numerical study, and it is shown that an arbitrary superposition of final ground states can be obtained. Also, it is observed that by increasing the number of coincident pulses, the population of ground states gets closer to the ideal situation.

Ultrafast dynamics and scattering of protic ionic liquids induced by XFEL pulses.

X-rays are routinely used for structural studies through scattering, and femtosecond X-ray lasers can probe ultrafast dynamics. We aim to capture the femtosecond dynamics of liquid samples using simulations and deconstruct the interplay of ionization and atomic motion within the X-ray laser pulse. This deconstruction is resolution dependent, as ionization influences the low momentum transfers through changes in scattering form factors, while atomic motion has a greater effect at high momentum transfers through loss of coherence. Our methodology uses a combination of classical molecular dynamics and plasma simulation on a protic ionic liquid to quantify the contributions to the scattering signal and how these evolve with time during the X-ray laser pulse. Our method is relevant for studies of organic liquids, biomolecules in solution or any low-Z materials at liquid densities that quickly turn into a plasma while probed with X-rays.