High-contrast, intense single-cycle pulses are highly desirable tools in ultrafast science, enabling highest temporal resolution, pushing matter to extreme conditions, and serving as drivers in petahertz electronics. In this Letter, we use thin solid plates in a double multi-plate supercontinuum configuration, delivering a broadband spectrum spanning from ∼ 400 to ∼ 1000 n m at the − 20 d B intensity level to produce a single-cycle pulse. We show that the spectral broadening by self-phase modulation with few-cycle pulses is more suitable for compression than the single-cycle limit than with multi-cycle pulses. The pulses are compressed to 2.6 fs pulses, close to the transform limit of 2.55 fs, with an energy of 0.235 mJ. They exhibit an excellent power stability of 0.5% rms over 3 h and a beam profile. The obtained single-cycle pulses can be utilized in many applications, such as generation of isolated attosecond pulses via high-order harmonic generation, investigation of ultrafast phenomena with extreme temporal resolution, or high-intensity laser-solid experiments.

Chemical and physical processes in molecules can be controlled through the manipulation of quantum interferences between rotational, vibrational, and electronic degrees of freedom. Most of the past efforts have been focused on the control of nuclear dynamics. Even though electronic coherence and its coupling to nuclear degrees of freedom may profoundly affect the outcome of these processes, electron dynamics have received less attention. Proper investigation of electron dynamics in materials demands ultrafast sources in the visible, ultraviolet (UV), and extreme ultraviolet (XUV) spectral region. For this purpose, a few-cycle deep-UV and XUV beamlines have been constructed for studying ultrafast electron dynamics in molecules. To ensure the required high temporal resolution on the attosecond time scale, vibration isolation from environmental mechanical noise and active stabilization have been implemented to achieve attosecond timing control between pump and probe pulses with excellent stability. This is achieved with an actively phase-stabilized double-layer Mach-Zehnder interferometer system capable of continuous time-delay scans over a range of 200 fs with a root-mean-square timing jitter of only 13 as over a few seconds and ~80 as of peak-to-peak drift over several hours.

We demonstrate high-contrast, intense single-cycle pulses by enhancing the self-phase modulation for spectral broadening in two-stage of all-solid-state multiple-plate setups. The output pulses are compressed to 2.6 fs, close to the transform-limited of 2.55 fs.

Energetic, few-fs pulses in the deep-UV region are highly desirable for exploring ultrafast processes on their natural time scales, especially in molecules. The deep-UV source can be generated from gas media irradiated with few-cycle near-infrared laser pulses via a third-order frequency conversion process, which is a perturbative mechanism in a relatively weak field regime. In this work, we demonstrate that the deep-UV generation process is significantly affected by also even higher nonlinear processes, such as the ionization depletion of gas and plasma-induced spatiotemporal distortion of propagating light. In the experiment, by optimizing the deep-UV (3.6–5.7 eV) generation efficiency, the highest deep-UV energy of 1 μJ was observed from a moderately ionized 0.8-bar Ar gas target. The observed UV spectra exhibited frequency shifts depending on the experimental conditions—gas type, gas pressure, and the gas cell location—supporting the importance of the highly nonlinear mechanisms. The experimental observations were well corroborated by numerical simulations.