No abstract

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 ~1020 W/cm2 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.

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.

We report the generation of ultrahigh brightness X-ray pulses using the Fresh Bunch Self-Seeding (FBSS) method in an X-ray Free Electron Laser (XFEL). The FBSS method uses two different electron slices or bunches, one to generate the seed and the other to amplify it after the monochromator. This method circumvents the trade-off between the seed power and electron slice energy spread, which limits the efficiency of regular self-seeded FELs. The experiment, the performance of which is limited by existing hardware, shows FBSS feasibility, generating 5.5 keV photon pulses which are 9 fs long and of 7.3 ×10−5 bandwidth and 50 GW power. FBSS performance is compared with Self Amplified Spontaneous Emission/self-seeding performance, measuring a brightness increase of twelve/two times, respectively. In an optimized XFEL, FBSS can increase the peak power a hundred times more than state-of-the-art to multi-TW, opening new research areas for nonlinear science and single molecule imaging.

Free electron lasers in the X-ray regime require a good slice alignment along the electron bunch to achieve their best performance. A transverse beam slice shift reduces this alignment and spoils projected emittance and optics. Coherent synchrotron radiation specifically for over-compression and transverse wakefields are major contributors to this. In the case of the large-bandwidth operation, based on a strictly monotonic energy chirp of the bunch, the here introduced correction additionally enhances the spectral bandwidth of the FEL pulse. Well-defined leaking of dispersion at places with a strictly monotonic longitudinal phase space can compensate a beam tilt. This work presents a way to characterize the beam tilt as well as a method to correct for it within a linear accelerator with at least one high dispersive section with corrector magnets.