Femtosecond Double-pulse Irradiation Research Articles

Formation of nanograting in fused silica by temporally delayed femtosecond double-pulse irradiation

A 1 kHz femtosecond double-pulse sequence irradiation is used to study the temporal evolution of nanograting in fused silica by controlling the delay times and polarization combinations of two independent beams from a Mach–Zehnder interferometer. A lateral laser-scan experiment with speed at 5 µm s−1 and each pulse energy of 1 µJ is firstly performed with the delay time from sub-picosecond to 10 ps, and then the written nanostructures are systematically studied under a cross-polarized microscope because the intensity of birefringence signal nearly corresponds to optical retardance and development level of the induced nanograting. The trend shows that the induced nanogratings can continue developing with a decrease of delay time in the case of the linear polarization pulse arriving before. In another vertical laser-scan experiment at the same speed and pulse energy, the morphologies of nanogratings embedded in the lines are characterized by scanning electron microscope after mechanical polishing and chemical etching. The self-organized patterns have a commonly spatial period of 200–300 nm and the orientation is always perpendicular to the polarization of the first laser pulse, and the second pulse in each sequence seems to promote the as-formed nanograting developing further even if the polarized direction is different from the previous pulse. These new findings verify again that a localized memory effect can make positive feedback to reinforce the patterned nanostripes. In that process, the impact ionization from the seed electrons left by the first pulse excitation and the photoionization of self-trapped excitons with lower ionization threshold results in an increase of the re-excited carriers during the second pulse irradiation and the subsequent development of the as-formed nanograting. Our result provides further proofs for understanding the physical mechanism of nanograting strongly connection with the interplay on multiple ionization channels.

Laser-induced periodic surface structures on zinc oxide crystals upon two-colour femtosecond double-pulse irradiation

In order to study the temporally distributed energy deposition in the formation of laser-induced periodic surface structures (LIPSS) on single-crystalline zinc oxide (ZnO), two-colour double-fs-pulse experiments were performed. Parallel or cross-polarised double-pulse sequences at 400 and 800 nm wavelength were generated by a Mach–Zehnder interferometer, exhibiting inter-pulse delays up to a few picoseconds between the sub-ablation 50-fs-pulses. Twenty two-colour double-pulse sequences were collinearly focused by a spherical mirror to the sample surface. The resulting LIPSS periods and areas were analysed by scanning electron microscopy. The delay-dependence of these LIPSS characteristics shows a dissimilar behaviour when compared to the semiconductor silicon, the dielectric fused silica, or the metal titanium. A wavelength-dependent plasmonic mechanism is proposed to explain the delay-dependence of the LIPSS on ZnO when considering multi-photon excitation processes. Our results support the involvement of nonlinear processes for temporally overlapping pulses. These experiments extend previous two-colour studies on the indirect semiconductor silicon towards the direct wide band-gap semiconductor ZnO and further manifest the relevance of the ultrafast energy deposition for LIPSS formation.

Laser-induced periodic surface structures on titanium upon single- and two-color femtosecond double-pulse irradiation.

Single- and two-color double-fs-pulse experiments were performed on titanium to study the dynamics of the formation of laser-induced periodic surface structures (LIPSS). A Mach-Zehnder inter-ferometer generated polarization controlled (parallel or cross-polarized) double-pulse sequences in two configurations - either at 800 nm only, or at 400 and 800 nm wavelengths. The inter-pulse delays of the individual 50-fs pulses ranged up to some tens of picoseconds. Multiple of these single- or two-color double-fs-pulse sequences were collinearly focused by a spherical mirror to the sample surface. In both experimental configurations, the peak fluence of each individual pulse was kept below its respective ablation threshold and only the joint action of both pulses lead to the formation of LIPSS. Their resulting characteristics were analyzed by scanning electron microscopy and the periods were quantified by Fourier analyses. The LIPSS periods along with the orientation allow a clear identification of the pulse which dominates the energy coupling to the material. A plasmonic model successfully explains the delay-dependence of the LIPSS on titanium and confirms the importance of the ultrafast energy deposition stage for LIPSS formation.