Streaking of photoelectrons with optical lasers has been widely used for temporal characterization of attosecond extreme ultraviolet pulses. Recently, this technique has been adapted to characterize femtosecond x-ray pulses in free-electron lasers with the streaking imprinted by farinfrared and Terahertz (THz) pulses. Here, we report successful implementation of THz streaking for time-stamping of an ultrashort relativistic electron beam of which the energy is several orders of magnitude higher than photoelectrons. Such ability is especially important for MeV ultrafast electron diffraction (UED) applications where electron beams with a few femtosecond pulse width may be obtained with longitudinal compression while the arrival time may fluctuate at a much larger time scale. Using this laser-driven THz streaking technique, the arrival time of an ultrashort electron beam with 6 fs (rms) pulse width has been determined with 1.5 fs (rms) accuracy. Furthermore, we have proposed and demonstrated a non-invasive method for correction of the timing jitter with femtosecond accuracy through measurement of the compressed beam energy, which may allow one to advance UED towards sub-10 fs frontier far beyond the ∼100 fs (rms) jitter.

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In low-dimensional systems with strong electronic correlations, the application of an ultrashort laser pulse often yields novel phases that are otherwise inaccessible. The central challenge in understanding such phenomena is to determine how dimensionality and many-body correlations together govern the pathway of a non-adiabatic transition. To this end, we examine a layered compound, 1T-TiSe2, whose three-dimensional charge-density-wave (3D CDW) state also features exciton condensation due to strong electron-hole interactions. We find that photoexcitation suppresses the equilibrium 3D CDW while creating a nonequilibrium 2D CDW. Remarkably, the dimension reduction does not occur unless bound electron-hole pairs are broken. This relation suggests that excitonic correlations maintain the out-of-plane CDW coherence, settling a long-standing debate over their role in the CDW transition. Our findings demonstrate how optical manipulation of electronic interaction enables one to control the dimensionality of a broken-symmetry order, paving the way for realizing other emergent states in strongly correlated systems.

Vanadium dioxide (VO2) exhibits an insulator-to-metal transition accompanied by a structural transition near room temperature. This transition can be triggered by an ultrafast laser pulse. Exotic transient states, such as a metallic state without structural transition, were also proposed. These unique characteristics let VO2 have great potential in thermal switchable devices and photonic applications. Although great efforts have been made, the atomic pathway during the photoinduced phase transition is still not clear. Here, we synthesize freestanding quasi-single-crystal VO2 films and examine their photoinduced structural phase transition with mega-electron-volt ultrafast electron diffraction. Leveraging the high signal-to-noise ratio and high temporal resolution, we observe that the disappearance of vanadium dimers and zigzag chains does not coincide with the transformation of crystal symmetry. After photoexcitation, the initial structure is strongly modified within 200 femtoseconds, resulting in a transient monoclinic structure without vanadium dimers and zigzag chains. Then, it continues to evolve to the final tetragonal structure in approximately 5 picoseconds. In addition, only one laser fluence threshold instead of two thresholds suggested in polycrystalline samples is observed in our quasi-single-crystal samples. Our findings provide essential information for a comprehensive understanding of the photoinduced ultrafast phase transition in VO2.