Extreme nonlinear interactions of THz electromagnetic fields with matter are the next frontier in nonlinear optics. However, reaching this frontier in free space is limited by the existing lack of appropriate powerful THz sources. Here, we experimentally demonstrate that two-color filamentation of femtosecond mid-infrared laser pulses at 3.9 μm allows one to generate ultrashort sub-cycle THz pulses with sub-milijoule energy and THz conversion efficiency of 2.36%, resulting in THz field amplitudes above 100 MV cm −1. Our numerical simulations predict that the observed THz yield can be significantly upscaled by further optimizing the experimental setup. Finally, in order to demonstrate the strength of our THz source, we show that the generated THz pulses are powerful enough to induce nonlinear cross-phase modulation in electro-optic crystals. Our work paves the way toward free space extreme nonlinear THz optics using affordable table-top laser systems.

An important challenge in the field of three-dimensional ultrafast laser processing is to achieve permanent modifications in the bulk of silicon and narrow-gap materials. Recent attempts by increasing the energy of infrared ultrashort pulses have simply failed. Here, we establish that it is because focusing with a maximum numerical aperture of about 1.5 with conventional schemes does not allow overcoming strong nonlinear and plasma effects in the pre-focal region. We circumvent this limitation by exploiting solid-immersion focusing, in analogy to techniques applied in advanced microscopy and lithography. By creating the conditions for an interaction with an extreme numerical aperture near 3 in a perfect spherical sample, repeatable femtosecond optical breakdown and controllable refractive index modifications are achieved inside silicon. This opens the door to the direct writing of three-dimensional monolithic devices for silicon photonics. It also provides perspectives for new strong-field physics and warm-dense-matter plasma experiments.

Generation and application of energetic, broadband terahertz pulses (bandwidth ~0.1–50 THz) is an active and contemporary area of research. The main thrust is toward the development of efficient sources with minimum complexities—a true table-top setup. In this work, we demonstrate the generation of terahertz radiation via ultrashort pulse induced filamentation in liquids—a counterintuitive observation due to their large absorption coefficient in the terahertz regime. The generated terahertz energy is more than an order of magnitude higher than that obtained from the two-color filamentation of air (the most standard table-top technique). Such high terahertz energies would generate electric fields of the order of MV cm-1, which opens the doors for various nonlinear terahertz spectroscopic applications. The counterintuitive phenomenon has been explained via the solution of nonlinear pulse propagation equation in the liquid medium.