The ability to fully characterize ultrashort, ultra-intense X-ray pulses at free-electron lasers (FELs) will be crucial in experiments ranging from single-molecule imaging to extreme-timescale X-ray science. This issue is especially important at current-generation FELs, which are primarily based on self-amplified spontaneous emission and radiate with parameters that fluctuate strongly from pulse to pulse. Using single-cycle terahertz pulses from an optical laser, we have extended the streaking techniques of attosecond metrology to measure the temporal profile of individual FEL pulses with 5 fs full-width at half-maximum accuracy, as well as their arrival on a time base synchronized to the external laser to within 6 fs r.m.s. Optical laser-driven terahertz streaking can be utilized at any X-ray photon energy and is non-invasive, allowing it to be incorporated into any pump–probe experiment, eventually characterizing pulses before and after interaction with most sample environments

X-ray free-electron lasers, with pulse durations ranging from a few to several hundred femtoseconds, are uniquely suited for studying atomic, molecular, chemical and biological systems. Characterizing the temporal profiles of these femtosecond X-ray pulses that vary from shot to shot is not only challenging but also important for data interpretation. Here we report the time-resolved measurements of X-ray free-electron lasers by using an X-band radiofrequency transverse deflector at the Linac Coherent Light Source. We demonstrate this method to be a simple, non-invasive technique with a large dynamic range for single-shot electron and X-ray temporal characterization. A resolution of less than 1 fs root mean square has been achieved for soft X-ray pulses. The lasing evolution along the undulator has been studied with the electron trapping being observed as the X-ray peak power approaches 100 GW.

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The X-ray free-electron laser has opened a new era for photon science, improving the X-ray brightness by ten orders of magnitude over previously available sources. Similar to an optical laser, the spectral and temporal structure of the radiation pulses can be tailored to the specific needs of many experiments by accurately manipulating the lasing medium, that is, the electron beam. Here we report the generation of mJ-level two-colour hard X-ray pulses of few femtoseconds duration with an XFEL driven by twin electron bunches at the Linac Coherent Light Source. This performance represents an improvement of over an order of magnitude in peak power over state-of-the-art two-colour XFELs. The unprecedented intensity and temporal coherence of this new two-colour X-ray free-electron laser enable an entirely new set of scientific applications, ranging from X-ray pump/X-ray probe experiments to the imaging of complex biological samples with multiple wavelength anomalous dispersion.

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarily by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses.

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We propose a novel method to characterize the temporal duration and shape of femtosecond x-ray pulses in a free-electron laser (FEL) by measuring the time-resolved electron-beam energy loss and energy spread induced by the FEL process, with a transverse radio-frequency deflector located after the undulator. Its merits are simplicity, high resolution, wide diagnostic range, and noninvasive to user operation. When the system is applied to the Linac Coherent Light Source, the world's most powerful x-ray FEL, it can provide single-shot measurements of the electron-beam and x-ray pulses with a resolution on the order of 1-2 femtoseconds rms.

The microbunching instability (MBI) is a well-known problem for high brightness electron beams and has been observed at accelerator facilities around the world. Free-electron lasers (FELs) are particularly susceptible to MBI, which can distort the longitudinal phase space and increase the beam's slice energy spread (SES). Past studies of MBI at the Linac Coherent Light Source (LCLS) relied on optical transition radiation to infer the existence of microbunching. With the development of the x-band transverse deflecting cavity (XTCAV), we can for the first time directly image the longitudinal phase space at the end of the accelerator and complete a comprehensive study of MBI, revealing both detailed MBI behavior as well as insights into mitigation schemes. The fine time resolution of the XTCAV also provides the first LCLS measurements of the final SES, a critical parameter for many advanced FEL schemes. Detailed MBI and SES measurements can aid in understanding MBI mechanisms, benchmarking simulation codes, and designing future high-brightness accelerators.