Resonant X-ray excitation of the nuclear clock isomer 45Sc.

Resonant oscillators with stable frequencies and large quality factors help us to keep track of time with high precision. Examples range from quartz crystal oscillators in wristwatches to atomic oscillators in atomic clocks, which are, at present, our most precise time measurement devices1. The search for more stable and convenient reference oscillators is continuing2-6. Nuclear oscillators are better than atomic oscillators because of their naturally higher quality factors and higher resilience against external perturbations7-9. One of the most promising cases is an ultra-narrow nuclear resonance transition in 45Sc between the ground state and the 12.4-keV isomeric state with a long lifetime of 0.47 s (ref. 10). The scientific potential of 45Sc was realized long ago, but applications require 45Sc resonant excitation, which in turn requires accelerator-driven, high-brightness X-ray sources11 that have become available only recently. Here we report on resonant X-ray excitation of the 45Sc isomeric state by irradiation of Sc-metal foil with 12.4-keV photon pulses from a state-of-the-art X-ray free-electron laser and subsequent detection of nuclear decay products. Simultaneously, the transition energy was determined as [Formula: see text] with an uncertainty that is two orders of magnitude smaller than the previously known values. These advancements enable the application of this isomer in extreme metrology, nuclear clock technology, ultra-high-precision spectroscopy and similar applications.

Imaging via Correlation of X-Ray Fluorescence Photons.

We demonstrate that x-ray fluorescence emission, which cannot maintain a stationary interference pattern, can be used to obtain images of structures by recording photon-photon correlations in the manner of the stellar intensity interferometry of Hanbury Brown and Twiss. This is achieved utilizing femtosecond-duration pulses of a hard x-ray free-electron laser to generate the emission in exposures comparable to the coherence time of the fluorescence. Iterative phasing of the photon correlation map generated a model-free real-space image of the structure of the emitters. Since fluorescence can dominate coherent scattering, this may enable imaging uncrystallised macromolecules.

Shot-to-shot two-dimensional photon intensity diagnostics within megahertz pulse-trains at the European XFEL.

Characterizing the properties of X-ray free-electron laser (XFEL) sources is a critical step for optimization of performance and experiment planning. The recent availability of MHz XFELs has opened up a range of new opportunities for novel experiments but also highlighted the need for systematic measurements of the source properties. Here, MHz-enabled beam imaging diagnostics developed for the SPB/SFX instrument at the European XFEL are exploited to measure the shot-to-shot intensity statistics of X-ray pulses. The ability to record pulse-integrated two-dimensional transverse intensity measurements at multiple planes along an XFEL beamline at MHz rates yields an improved understanding of the shot-to-shot photon beam intensity variations. These variations can play a critical role, for example, in determining the outcome of single-particle imaging experiments and other experiments that are sensitive to the transverse profile of the incident beam. It is observed that shot-to-shot variations in the statistical properties of a recorded ensemble of radiant intensity distributions are sensitive to changes in electron beam current density. These changes typically occur during pulse-distribution to the instrument and are currently not accounted for by the existing suite of imaging diagnostics. Modulations of the electron beam orbit in the accelerator are observed to induce a time-dependence in the statistics of individual pulses - this is demonstrated by applying radio-frequency trajectory tilts to electron bunch-trains delivered to the instrument. We discuss how these modifications of the beam trajectory might be used to modify the statistical properties of the source and potential future applications.

Observation of Seeded Mn Kß Stimulated X-Ray Emission Using Two-Color X-Ray Free-Electron Laser Pulses.

Kß x-ray emission spectroscopy is a powerful probe for electronic structure analysis of 3d transition metal systems and their ultrafast dynamics. Selectively enhancing specific spectral regions would increase this sensitivity and provide fundamentally new insights. Recently we reported the observation and analysis of Kα amplified spontaneous x-ray emission from Mn solutions using an x-ray free-electron laser to create the 1s core-hole population inversion [Kroll et al., Phys. Rev. Lett. 120, 133203 (2018)PRLTAO0031-900710.1103/PhysRevLett.120.133203]. To apply this new approach to the chemically more sensitive but much weaker Kß x-ray emission lines requires a mechanism to outcompete the dominant amplification of the Kα emission. Here we report the observation of seeded amplified Kß x-ray emission from a NaMnO_{4} solution using two colors of x-ray free-electron laser pulses, one to create the 1s core-hole population inversion and the other to seed the amplified Kß emission. Comparing the observed seeded amplified Kß emission signal with that from conventional Kß emission into the same solid angle, we obtain a signal enhancement of more than 10^{5}. Our findings are the first important step of enhancing and controlling the emission of selected final states of the Kß spectrum with applications in chemical and materials science.

Dispersion-Based Fresh-Slice Scheme for Free-Electron Lasers.

The fresh-slice technique improved the performance of several self-amplified spontaneous emission free-electron laser schemes by granting selective control on the temporal lasing slice without spoiling the other electron bunch slices. So far, the implementation has required a special insertion device to create the beam yaw, called a dechirper. We demonstrate a novel scheme to enable fresh-slice operation based on electron energy chirp and orbit dispersion that can be implemented at any free-electron laser facility without additional hardware.

Generation of High-Power High-Intensity Short X-Ray Free-Electron-Laser Pulses.

X-ray free-electron lasers combine a high pulse power, short pulse length, narrow bandwidth, and high degree of transverse coherence. Any increase in the photon pulse power, while shortening the pulse length, will further push the frontier on several key x-ray free-electron laser applications including single-molecule imaging and novel nonlinear x-ray methods. This Letter shows experimental results at the Linac Coherent Light Source raising its maximum power to more than 300% of the current limit while reducing the photon pulse length to 10 fs. This was achieved by minimizing residual transverse-longitudinal centroid beam offsets and beam yaw and by correcting the dispersion when operating over 6 kA peak current with a longitudinally shaped beam.

High-Power Femtosecond Soft X Rays from Fresh-Slice Multistage Free-Electron Lasers.

We demonstrate a novel multistage amplification scheme for self-amplified spontaneous-emission free electron lasers for the production of few femtosecond pulses with very high power in the soft x-ray regime. The scheme uses the fresh-slice technique to produce an x-ray pulse on the bunch tail, subsequently amplified in downstream undulator sections by fresh electrons. With three-stages amplification, x-ray pulses with an energy of hundreds of microjoules are produced in few femtoseconds. For single-spike spectra x-ray pulses the pulse power is increased more than an order of magnitude compared to other techniques in the same wavelength range.

Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes.

We report the observation and analysis of the gain curve of amplified Kα x-ray emission from solutions of Mn(II) and Mn(VII) complexes using an x-ray free electron laser to create the 1s core-hole population inversion. We find spectra at amplification levels extending over 4 orders of magnitude until saturation. We observe bandwidths below the Mn 1s core-hole lifetime broadening in the onset of the stimulated emission. In the exponential amplification regime the resolution corrected spectral width of ∼1.7 eV FWHM is constant over 3 orders of magnitude, pointing to the buildup of transform limited pulses of ∼1 fs duration. Driving the amplification into saturation leads to broadening and a shift of the line. Importantly, the chemical sensitivity of the stimulated x-ray emission to the Mn oxidation state is preserved at power densities of ∼10^{20} W/cm^{2} for the incoming x-ray pulses. Differences in signal sensitivity and spectral information compared to conventional (spontaneous) x-ray emission spectroscopy are discussed. Our findings build a baseline for nonlinear x-ray spectroscopy for a wide range of transition metal complexes in inorganic chemistry, catalysis, and materials science.