Dynamic control of material properties using strong-field, narrowband THz sources has drawn attention because it allows selective manipulation of quantum states on demand by coherent excitation of specific low-energy modes in solids. Yet, the lack of powerful narrowband lasers with frequencies in the range of a few to a few tens of THz has restricted the exploration of hidden states in condensed matter. Here, we report the optimization of an optical parametric amplifier (OPA) and the efficient generation of a strong, narrowband THz field. The OPA has a total conversion efficiency of > 55%, which is the highest value reported to date, with an excellent energy-stability of 0.7% RMS over 3 h. We found that the injection of a high-energy signal beam to a power amplification stage in an OPA leads to high-efficiency and a super-Gaussian profile. By difference-frequency generation of two chirped OPA signal pulses in an organic nonlinear crystal, we obtained a THz pulse with an energy of 3.2 μJ, a bandwidth of 0.5 THz, and a pulse duration of 860 fs tunable between the 4 and 19 THz regions. This corresponds to an internal THz conversion efficiency of 0.4% and a THz field strength of 6.7 MV/cm. This approach demonstrates an effective way to generate narrow-bandwidth, intense THz fields.

High-intensity X-ray free-electron laser (XFEL) beams create transient and non-equilibrium dense states of matter in solid-density targets. These states can be used to develop atomic X-ray lasers with narrow bandwidth and excellent longitudinal coherence, which is not possible with current XFEL pulses. An atomic kinetics model is used to simulate the population dynamics of atomic inner-shell vacancy states in Mg, Al, and Si, revealing the feasibility of population inversion between K-shell and L-shell vacancy states. We also discuss the gain characteristics of these states implying the possibility of atomic X-ray lasers based on inner-shell vacancy states in the 1.5 keV region. The development of atomic X-ray lasers could have applications in high-resolution spectroscopy and nonlinear optics in the X-ray region.

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.

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.