Studying ultrafast processes on the nanoscale with element specificity requires a powerful femtosecond source of tunable extreme-ultraviolet (XUV) or x-ray radiation, such as a free-electron laser (FEL). Current efforts in FEL development are aimed at improving the wavelength tunability and multicolor operation, which will potentially lead to the development of new characterization techniques offering a higher chemical sensitivity and improved spatial resolution. One of the most promising approaches is the echo-enabled harmonic generation (EEHG), where two external seed lasers are used to precisely control the spectro-temporal properties of the FEL pulse. Here, we study the expected performance of EEHG at the FERMI FEL, using numerical simulations. We show that, by employing the existing FERMI layout with minor modifications, the EEHG scheme will be able to produce gigawatt peak-power pulses at wavelengths as short as 5 nm. We discuss some possible detrimental effects that may affect the performance of EEHG and compare the results to the existing double-stage FEL cascade, currently in operation at FERMI. Finally, our simulations show that, after substantial machine upgrades, EEHG has the potential to deliver coherent multicolor pulses reaching wavelengths as short as 3 nm, enabling x-ray pump-x-ray probe experiments in the water window.

We have examined the transmission of soft X-ray pulses from the FERMI free electron laser through carbon films of varying thickness, quantifying nonlinear effects of pulses above and below the carbon K-edge. At typical of soft X-ray free electron laser intensities, pulses exhibit linear absorption at photon energies above and below the K-edge, ∼308 and ∼260 eV, respectively; whereas two-photon absorption becomes significant slightly below the K-edge, ∼284.2 eV. The measured two-photon absorption cross section at 284.18 eV (∼6 × 10−48 cm4 s) is 7 orders of magnitude above what is expected from a simple theory based on hydrogen-like atoms - a result of resonance effects.

X-ray free-electron lasers (FELs), which amplify light emitted by a relativistic electron beam, are extending nonlinear optical techniques to shorter wavelengths, adding element specificity by exciting and probing electronic transitions from core levels. These techniques would benefit tremendously from having a stable FEL source, generating spectrally pure and wavelength-tunable pulses. We show that such requirements can be met by operating the FEL in the so-called echo-enabled harmonic generation (EEHG) configuration. Here, two external conventional lasers are used to precisely tailor the longitudinal phase space of the electron beam before emission of X-rays. We demonstrate high-gain EEHG lasing producing stable, intense, nearly fully coherent pulses at wavelengths as short as 5.9 nm (~211 eV) at the FERMI FEL user facility. Low sensitivity to electron-beam imperfections and observation of stable, narrow-band, coherent emission down to 2.6 nm (~474 eV) make the technique a prime candidate for generating laser-like pulses in the X-ray spectral region, opening the door to multidimensional coherent spectroscopies at short wavelengths.