Attosecond X-ray Research Articles

“Beam à la carte”: Laser heater shaping for attosecond pulses in a multiplexed x-ray free-electron laser

Electron beam shaping allows the control of the temporal properties of x-ray free-electron laser pulses from femtosecond to attosecond timescales. Here, we demonstrate the use of a laser heater to shape electron bunches and enable the generation of attosecond x-ray pulses. We demonstrate that this method can be applied in a selective way, shaping a targeted subset of bunches while leaving the remaining bunches unchanged. This experiment enables the delivery of shaped x-ray pulses to multiple undulator beamlines, with pulse properties tailored to specialized scientific applications.

Topological phase transitions via attosecond x-ray absorption spectroscopy

We present a numerical experiment that demonstrates the possibility to capture topological phase transitions via an x-ray absorption spectroscopy scheme. We consider a Chern insulator whose topological phase is tuned via a second-order hopping. We perform time-dynamics simulations of the out-of-equilibrium laser-driven electron motion that enables us to model a realistic attosecond spectroscopy scheme. In particular, we use an ultrafast scheme with a circularly polarized IR pump pulse and an attosecond x-ray probe pulse. A laser-induced dichroism-type spectrum shows a clear signature of the topological phase transition. We are able to connect these signatures with the Berry structure of the system. This work extend the applications of attosecond absorption spectroscopy to systems presenting a non-trivial topological phase.

Attosecond impulsive stimulated X-ray Raman scattering in liquid water.

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a nonlinear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity-dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarization response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density.

Few-femtosecond soft X-ray transient absorption spectroscopy with tuneable DUV-Vis pump pulses

Achieving few-femtosecond resolution for a pump-probe experiment is crucial to measuring the fastest electron dynamics and for creating superpositions of valence states in quantum systems. However, traditional UV-Vis pump pulses cannot achieve few-fs durations and usually operate at fixed wavelengths. Here, we present, to our knowledge, an unprecedented temporal resolution and pump tuneability for UV-Vis-pumped soft X-ray transient absorption spectroscopy. We have combined few-fs deep-UV to visible tuneable pump pulses from resonant dispersive wave emission in hollow capillary fiber with attosecond soft X-ray probe pulses from high harmonic generation. We achieve sub-5-fs time resolution, sub-fs interferometric stability, and continuous tuneability of the pump pulses from 230 to 700 nm. We demonstrate that the pump can initiate an ultrafast photochemical reaction and that the dynamics at different atomic sites can be resolved simultaneously. These capabilities will allow studies of the fastest electronic dynamics in a large range of photochemical, photobiological and photovoltaic reactions.

Attosecond delays in X-ray molecular ionization.

The photoelectric effect is not truly instantaneous but exhibits attosecond delays that can reveal complex molecular dynamics1-7. Sub-femtosecond-duration light pulses provide the requisite tools to resolve the dynamics of photoionization8-12. Accordingly, the past decade has produced a large volume of work on photoionization delays following single-photon absorption of an extreme ultraviolet photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required X-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. Here we report measurements of the X-ray photoemission delay of core-level electrons, with unexpectedly large delays, ranging up to 700 as in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft X-ray pulses from a free-electron laser to scan across the entire region near the K-shell threshold. Furthermore, we find that the delay spectrum is richly modulated, suggesting several contributions, including transient trapping of the photoelectron owing to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule and multi-electron scattering effects. The results demonstrate how X-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

Wavelength scaling and multicolor operation of a plasma-driven attosecond x-ray source via harmonic generation

Wavelength scaling and multicolor operation of a plasma-driven attosecond x-ray source via harmonic generation

Attosecond two-color x-ray free-electron lasers with dual chirp-taper configuration and bunching inheritance

Attosecond x-ray pulses play a crucial role in the study of ultrafast phenomena occurring within inner and valence electrons. To achieve attosecond time-resolution studies and gain control over electronic wave functions, it is crucial to develop techniques capable of generating and synchronizing two-color x-ray pulses at the attosecond scale. In this paper, we present a novel approach for generating attosecond pulse pairs using a dual chirp-taper free-electron laser with bunching inheritance. An electron beam with a sinusoidal energy chirp, introduced by the external laser, passes through the main undulator and afterburner, both with tapers. Two-color x-ray pulses are generated from the main undulator and the afterburner, respectively, with temporal separations of several femtoseconds and energy separations of tens of electron volts. Notably, the afterburner is much shorter than the main undulator due to the bunching inheritance, which reduces the distance between two source points and alleviates the beamline focusing requirements of the two-color pulses. A comprehensive stability analysis is conducted in this paper, considering the individual effects of shot noise from self-amplified spontaneous emission and carrier-envelope phase jitter of the few-cycle laser. The results show that the radiation from the afterburner exhibits excellent stability in the proposed scheme, which is beneficial for x-ray pump-probe experiments. The proposed scheme opens up new possibilities for attosecond science enabled by x-ray attosecond pump-probe techniques and coherent control of ultrafast electronic wave packets in quantum systems. Published by the American Physical Society 2024

Generation of attosecond gigawatt soft x-ray pulses through coherent Thomson backscattering.

Collision between relativistic electron sheets and counterpropagating laser pulses is recognized as a promising way to produce intense attosecond x rays through coherent Thomson backscattering (TBS). In a double-layer scheme, the electrons in an ultrathin solid foil are first pushed out by an intense laser driver and then interact with the laser reflected off a second foil to form a high-density relativistic electron sheet with vanishing transverse momentum. However, the repulsion between these concentrated electrons can increase the thickness of the layer, reducing both its density and subsequently the coherent TBS. Here, we present a systematic study on the evolution of the flying electron layer and find that its resulting thickness is determined by the interplay between the intrinsic space-charge expansion and the velocity compression induced by the drive laser. How the laser driver, the target areal density, the reflector, and the collision laser intensity affect the properties of the produced x rays is explored. Multidimensional particle-in-cell simulations indicate that employing this scheme in the nonlinear regime has the potential to stably produce soft x rays with several gigawatt peak power in hundreds of terawatt ultrafast laser facilities. The pulse duration can be tuned to tens of attoseconds. This compact and intense attosecond x-ray source may have broad applications in attosecond science.

Construction and Operation Plan for the Second Hard X-ray Beamline at PAL-XFEL

The second hard X-ray beamline (HX2) at PAL-XFEL (Pohang Accelerator Laboratory X-ray Free Electron Laser) is currently in progress for construction to meet the increasing demands of researchers in various fields. With higher electron beam energy and a larger undulator parameter K, HX2 can deliver over twice the FEL intensity of the existing hard X-ray beamline (HX1) in the photon energy range of 2 to 7 keV. Consequently, HX1 will operate within the electron beam energy range of 7 to 10.5 GeV, providing FELs from 6.5 to 20 keV when both HX1 and HX2 are operated simultaneously. Most of the components have already been designed and prepared, enabling us to start construction as scheduled. Following this construction, we have also the upgrade plan for advanced operation of new extreme X-ray sources such as attosecond X-ray pulses and TW (1012 W, terawatt) scale X-ray pulses. In this report, we will introduce about construction and future upgrade plan of HX2 at PAL-XFEL.

Terawatt-scale attosecond X-ray pulses from a cascaded superradiant free-electron laser

Terawatt-scale attosecond X-ray pulses from a cascaded superradiant free-electron laser

Isolated attosecond electron and hard x-ray pulse generation by ultra-intense spatiotemporal vortex laser

The spatiotemporal optical vortex (STOV) laser pulse, characterized by containing a space-time dependent spiral phase structure and intrinsic transverse orbital angular momentum (OAM), has been of much recent research interest for basic physics as well as potential applications in optical communication and manipulation, as well as the attosecond sciences. Here we consider electron acceleration and generation of attosecond hard x-rays by irradiating a thin foil with intense STOV laser pulse. It is found that the affected foil electrons can be trapped and acquire transverse OAM, or synchrotron-like motion, from the STOV, as well as accelerated forward by the transverse and enhanced axial laser electric fields to form a tiny energetic bunch at the front of the laser pulse and emit short ( ∼400 attosecond) high-flux ( >109 photons per pulse) hard (100–1000 keV) x rays.

Probing Liquid Water’s Structure with Attosecond X-Ray Pulses

Probing Liquid Water’s Structure with Attosecond X-Ray Pulses

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.

Attosecond-pump attosecond-probe x-ray spectroscopy of liquid water.

Attosecond-pump/attosecond-probe experiments have long been sought as the most straightforward method for observing electron dynamics in real time. Although there has been much success with overlapped near-infrared femtosecond and extreme ultraviolet attosecond pulses combined with theory, true attosecond-pump/attosecond-probe experiments have been limited. We used a synchronized attosecond x-ray pulse pair from an x-ray free-electron laser to study the electronic response to valence ionization in liquid water through all x-ray attosecond transient absorption spectroscopy (AX-ATAS). Our analysis showed that the AX-ATAS response is confined to the subfemtosecond timescale, eliminating any hydrogen atom motion and demonstrating experimentally that the 1b1 splitting in the x-ray emission spectrum is related to dynamics and is not evidence of two structural motifs in ambient liquid water.

Tracing Photoinduced Hydrogen Migration in Alcohol Dications from Time-Resolved Molecular-Frame Photoelectron Angular Distributions.

The recent implementation of attosecond and few-femtosecond X-ray pump/X-ray probe schemes in large-scale free-electron laser facilities has opened the way to visualize fast nuclear dynamics in molecules with unprecedented temporal and spatial resolution. Here, we present the results of theoretical calculations showing how polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) can be used to visualize the dynamics of hydrogen migration in methanol, ethanol, propanol, and isopropyl alcohol dications generated by X-ray irradiation of the corresponding neutral species. We show that changes in the PA-MFPADs with the pump-probe delay as a result of intramolecular photoelectron diffraction carry information on the dynamics of hydrogen migration in real space. Although visualization of this dynamics is more straightforward in the smaller systems, methanol and ethanol, one can still recognize the signature of that motion in propanol and isopropyl alcohol and assign a tentative path to it. A possible pathway for a corresponding experiment requires an angularly resolved detection of photoelectrons in coincidence with molecular fragment ions used to define a molecular frame of reference. Such studies have become, in principle, possible since the first XFELs with sufficiently high repetition rates have emerged. To further support our findings, we provide experimental evidence of H migration in ethanol-OD from ion-ion coincidence measurements performed with synchrotron radiation.

Attosecond x-ray free-electron lasers utilizing an optical undulator in a self-selection regime

Attosecond x-ray free-electron lasers utilizing an optical undulator in a self-selection regime

Rebuilding the vibrational wavepacket in TRAS using attosecond X-ray pulses

Time-resolved X-ray photoelectron spectroscopy (TXPS) is a well-established technique to probe coherent nuclear wavepacket dynamics using both table-top and free-electron-based ultrafast X-ray lasers. Energy resolution, however, becomes compromised for a very short pulse duration in the sub-femtosecond range. By resonantly tuning the X-ray pulse to core-excited states undergoing Auger decay, this drawback of TXPS can be mitigated. While resonant Auger-electron spectroscopy (RAS) can recover the vibrational structures not hidden by broadband excitation, the full reconstruction of the wavepacket is a standing challenge. Here, we theoretically demonstrate how the complete information of a nuclear wavepacket, i.e., the populations and relative phases of the vibrational states constituting the wavepacket, can be retrieved from time-resolved RAS (TRAS) measurements. Thus, TRAS offers key insights into coupled nuclear and electronic dynamics in complex systems on ultrashort timescales, providing an alternative to leverage femtosecond and attosecond X-ray probe pulses.

Enhanced optical conductivity and many-body effects in strongly-driven photo-excited semi-metallic graphite

The excitation of quasi-particles near the extrema of the electronic band structure is a gateway to electronic phase transitions in condensed matter. In a many-body system, quasi-particle dynamics are strongly influenced by the electronic single-particle structure and have been extensively studied in the weak optical excitation regime. Yet, under strong optical excitation, where light fields coherently drive carriers, the dynamics of many-body interactions that can lead to new quantum phases remain largely unresolved. Here, we induce such a highly non-equilibrium many-body state through strong optical excitation of charge carriers near the van Hove singularity in graphite. We investigate the system’s evolution into a strongly-driven photo-excited state with attosecond soft X-ray core-level spectroscopy. We find an enhancement of the optical conductivity of nearly ten times the quantum conductivity and pinpoint it to carrier excitations in flat bands. This interaction regime is robust against carrier-carrier interaction with coherent optical phonons acting as an attractive force reminiscent of superconductivity. The strongly-driven non-equilibrium state is markedly different from the single-particle structure and macroscopic conductivity and is a consequence of the non-adiabatic many-body state.

Self-Referenced Spectral Interferometry for Single-Shot Characterization of Ultrashort Free-Electron Laser Pulses.

An attosecond x-ray pulse with known spectrotemporal information is an essential tool for the investigation of ultrafast electron dynamics in quantum systems. Ultrafast free-electron lasers (FELs) have the unique advantage on unprecedented high intensity at x-ray wavelengths. However, no suitable method has been established so far for the spectrotemporal characterization of these ultrashort x-ray pulses. In this Letter, a simple method has been proposed based on self-referenced spectral interferometry for reconstructing the temporal profile and phase of ultrashort FEL pulses. We have demonstrated that the proposed method is reliable to completely characterize the attosecond x-ray FEL pulses with an error at the level of a few percent. Moreover, the first proof-of-principle experiment has been performed to achieve the single-shot spectrotemporal characterization of ultrashort pulses from a high-gain FEL. The precision of the proposed method will be enhanced with the decrease of the pulse duration, paving a new way for complete attosecond pulse characterization at x-ray FELs.

Generating high repetition rate X-ray attosecond pulses in a diffraction limited storage ring

To steer and track electron motion in atoms, molecules, and nanostructures, light pulses with attosecond duration and high repetition rate are required. In this paper, we use the angular dispersion-induced microbunching scheme and a few-cycle laser within a straight section (a few meters) of a diffraction-limited storage ring to generate a coherent high-flux attosecond pulse in the water window region. Simulation results based on the Southern Advanced Photon Source indicate that the proposed method can generate a chirp-free Fourier transform limited pulse with a minimum duration of 50 as, a maximum repetition rate of a few MHz, and a maximum average flux of about 4.4times 10^{11} photons/s/1%Bw.