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.

Direct three-dimensional (3D) laser writing of waveguides is highly advanced in a wide range of bandgap materials, but has no equivalent in silicon so far. We show that nanosecond laser single-pass irradiation is capable of producing channel micro-modifications deep into crystalline silicon. With an appropriate shot overlap, a relative change of the refractive index exceeding 10^-3 is obtained without apparent nonuniformity at the micrometer scale. Despite the remaining challenge of propagation losses, we show that the created structures form, to the best of our knowledge, the first laser-written waveguides in the bulk of monolithic silicon samples. This paves the way toward the capability of producing 3D architectures for the rapidly growing field of silicon photonics.

The metrology of laser-induced damage usually finds a single transition from 0% to 100% damage probability when progressively increasing the laser energy in experiments. We observe that picosecond pulses at 2-µm wavelength focused inside silicon provide a response that strongly deviates from this. Supported by nonlinear propagation simulations and energy flow analyses, we reveal an increased light delocalization for near critical power conditions. This leads to a nonmonotonic evolution of the peak delivered fluence as a function of the incoming pulse of the energy, a situation more complex than the clamping of the intensity until now observed in ultrafast regimes. Compared to femtosecond lasers, our measurements show that picosecond sources lead to reduced thresholds for three-dimensional (3D) writing inside silicon that is highly desirable. However, strong interplays between nonlinear effects persist and should not be ignored for the performance of future technological developments. We illustrate this aspect by carefully retrieving from the study the conditions for a demonstration of 3D data inscription inside a silicon wafer.