We report the first generation of coherent, tunable, variable-polarization, soft X-ray femtosecond pulses, generated by a\ud seeded free-electron laser (FEL) operating in the fresh bunch, two-stage harmonic upshift configuration. Characterization\ud of the radiation proves this FEL configuration can produce single-transverse-mode, narrow-spectral-bandwidth output\ud pulses of several tens of microjoules energy and low pulse-to-pulse wavelength jitter at final wavelengths of 10.8 nm and\ud below. The fresh bunch configuration enhances the FEL emission at high harmonic orders by avoiding a gain depression\ud due to the energy spread induced by the first-stage FEL interaction. Coherent signals measured down to 4.3 nm suggest\ud this configuration is directly scalable to photon energies that will enable scientific investigations below the carbon K-edge,\ud including access to the L-edges of many magnetic materials, with an energy per pulse unlocking the gate for experiments\ud in the soft X-ray region with close to Fourier-transform-limited pulses

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Extreme ultraviolet and X-ray free-electron lasers (FELs) produce short-wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilized for many experiments previously possible only at long wavelengths: multiphoton ionization, pumping an atomic laser and four-wave mixing spectroscopy. However one important optical technique, coherent control, has not yet been demonstrated, because self-amplified spontaneous emission FELs have limited longitudinal coherence. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent, and two-colour emission is predicted to be coherent. Here, we demonstrate the phase correlation of two colours, and manipulate it to control an experiment. Light of wavelengths 63.0 and 31.5nm ionized neon, and we controlled the asymmetry of the photoelectron angular distribution by adjusting the phase, with a temporal resolution of 3as. This opens the door to new short-wavelength coherent control experiments with ultrahigh time resolution and chemical sensitivity

Exploring the dynamics of matter driven to extreme non-equilibrium states by an intense ultrashort X-ray pulse is becoming reality, thanks to the advent of free-electron laser technology that allows development of different schemes for probing the response at variable time delay with a second pulse. Here we report the generation of two-colour extreme ultraviolet pulses of controlled wavelengths, intensity and timing by seeding of high-gain harmonic generation free-electron laser with multiple independent laser pulses. The potential of this new scheme is demonstrated by the time evolution of a titanium-grating diffraction pattern, tuning the two coherent pulses to the titanium M-resonance and varying their intensities. This reveals that an intense pulse induces abrupt pattern changes on a time scale shorter than hydrodynamic expansion and ablation. This result exemplifies the essential capabilities of the jitter-free multiple-colour free-electron laser pulse sequences to study evolving states of matter with element sensitivity.