Understanding the interplay between optical pulse parameters and ultrafast material response is critical in achieving efficient and controlled laser nanomachining. In general, the key to initiate material processing is the deposition of a sufficient energy density within the electronic system. In dielectrics this critical energy density corresponds typically to a plasma frequency in the near-IR spectral region. Creating this density instantaneously with ultrashort laser pulses of a few tens of femtoseconds pulse duration in the same spectral region, the penetration depth into the material will strongly decrease with increasing electron density. Consequently, staying below this critical density will allow deep penetration depths. This calls for delayed ionization processes to deposit the energy for processing, thus introducing the temporal structure of the laser pulses as a control parameter. In this contribution we demonstrate this concept experimentally and substantiate the physical picture with numerical calculations. Bandwidth-limited pulses of 30 fs pulse duration are stretched up to 1.5 ps either temporally symmetrically or temporally asymmetrically. The interplay between pulse structure and material response is optimally exploited by the asymmetrically structured temporal Airy pulses leading to the inherently efficient creation of high aspect ratio nanochannels. Depths in the range of several micrometers and diameters around 250 nm are created within a single laser shot and without making use of selffocusing and filamentation processes. In addition to the machining of nanophotonic devices in dielectrics, the technique has the potential to enhance laser-based nanocell surgery and cell poration techniques.

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We have investigated the use of tightly focused, temporally shaped femtosecond (fs)-laser pulses for producing nanostructures in two dielectric materials (sapphire and phosphate glass) with different characteristics in their response to pulsed laser radiation. For this purpose, laser pulses shaped by third-order dispersion (TOD) were used to generate temporally asymmetric excitation pulses, leading to the single-step production of subwavelength ablative and subablative surface structures. When compared to previous works on the interaction of tightly focused TOD-shaped pulses with fused silica, we show here that this approach leads to very different nanostructure morphologies, namely, clean nanopits without debris surrounding the crater in sapphire and well-outlined nanobumps and nanovolcanoes in phosphate glass. Although in sapphire the debris-free processing is associated with the much lower viscosity of the melt compared to fused silica, nanobump formation in phosphate glass is caused by material network expansion (swelling) upon resolidification below the ablation threshold. The formation of nanovolcanoes is a consequence of the combined effect of material network expansion and ablation occurring in the periphery and central part of the irradiated region, respectively. It is shown that the induced morphologies can be efficiently controlled by modulating the TOD coefficient of the temporally shaped pulses.

ContentsContents geformte Laserpulse zu einer räumlichen Anregungsverteilung führen, die im Vergleich zu bandbreitebegrenzten Laserpulsen eine um die Hälfte reduzierten Fläche hat, dafür aber umso größere Tiefe erreicht. Diese Ergebnisse werden im Kontext aktueller post-mortem Experimente diskutiert.

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