We have investigated nonlinear laser ̶ matter interaction inside silicon under tight focusing conditions by continuously tuning driving pulse duration from femtosecond to picosecond timescales. Such tailoring of laser pulse width provides a new route for energy delivery into a microvolume avoiding two-photon absorption and plasma defocusing in the pre-focal region. As a result, we have achieved values of saturated deposited energy density and plasma electron concentration of as high as 1 kJ cm −3 and 10 19 cm −3 respectively, which is lower than the threshold of irreversible structural transformation. For further increase of energy delivery inside silicon, a two-color technique supported by extremely tight focusing can be realized, forming a roadmap to the 3D industrial micromachining of planar bulk silicon.

We report on the numerical investigation of spectral enrichment under mid-infrared (4.4 μm) laser filamentation in CaF2 and the influence of the external focusing on this nonlinear phenomenon. It is shown that the supercontinuum generation is related to the rapid free-electron increase and appears when nonlinear and diffraction lengths are practically the same. With further pulse propagation, the anti-Stokes wing (ASW) is formed which is caused by the pulse splitting. Looser focusing leads to pulse splitting be closer to the point of supercontinuum formation along the propagation axis. The ASW experiences a red-shift when external focusing is applied due to increased free-electron density.

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Being the second most abundant element on earth after oxygen, silicon remains the working horse for key technologies for the years. Novel photonics platform for high-speed data transfer and optical memory demands higher flexibility of the silicon modification, including on-chip and in-bulk inscription regimes. These are deepness, three-dimensionality, controllability of sizes and morphology of created modifications. Mid-IR (beyond 4 µm) ultrafast lasers provide the required control for all these parameters not only on the surface (as in the case of the lithographic techniques), but also inside the bulk of the semiconductor, paving the way to an unprecedented variety of properties that can be encoded via such an excitation. We estimated the deposited energy density as 6 kJ cm−3 inside silicon under tight focusing of mid-IR femtosecond laser radiation, which exceeds the threshold value determined by the specific heat of fusion (~ 4 kJ cm−3). In such a regime, we successfully performed single-pulse silicon microstructuring. Using third-harmonic and near-IR microscopy, and molecular dynamics, we demonstrated that there is a low-density region in the center of a micromodification, surrounded by a “ring” with higher density, that could be an evidence of its micro-void structure. The formation of created micromodification could be controlled in situ using third-harmonic generation microscopy. The numerical simulation indicates that single-shot damage becomes possible due to electrons heating in the conduction band up to 8 eV (mean thermal energy) and the subsequent generation of microplasma with an overcritical density of 8.5 × 1021 cm−3. These results promise to be the foundation of a new approach of deep three-dimensional single-shot bulk micromachining of silicon.