Spontaneous periodic ordering on the surface and in the bulk of dielectrics irradiated by ultrafast laser: a shared electromagnetic origin.

Periodic self-organization of matter beyond the diffraction limit is a puzzling phenomenon, typical both for surface and bulk ultrashort laser processing. Here we compare the mechanisms of periodic nanostructure formation on the surface and in the bulk of fused silica. We show that volume nanogratings and surface nanoripples having subwavelength periodicity and oriented perpendicular to the laser polarization share the same electromagnetic origin. The nanostructure orientation is defined by the near-field local enhancement in the vicinity of the inhomogeneous scattering centers. The periodicity is attributed to the coherent superposition of the waves scattered at inhomogeneities. Numerical calculations also support the multipulse accumulation nature of nanogratings formation on the surface and inside fused silica. Laser surface processing by multiple laser pulses promotes the transition from the high spatial frequency perpendicularly oriented nanoripples to the low spatial frequency ripples, parallel or perpendicular to the laser polarization. The latter structures also share the electromagnetic origin, but are related to the incident field interference with the scattered far-field of rough non-metallic or transiently metallic surfaces. The characteristic ripple appearances are predicted by combined electromagnetic and thermo-mechanical approaches and supported by SEM images of the final surface morphology and by time-resolved pump-probe diffraction measurements.

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.

Femtosecond laser-induced periodic surface structures on silicon upon polarization controlled two-color double-pulse irradiation.

Two-color double-fs-pulse experiments were performed on silicon wafers to study the temporally distributed energy deposition in the formation of laser-induced periodic surface structures (LIPSS). A Mach-Zehnder interferometer generated parallel or cross-polarized double-pulse sequences at 400 and 800 nm wavelength, with inter-pulse delays up to a few picoseconds between the sub-ablation 50-fs-pulses. Multiple two-color double-pulse sequences were collinearly focused by a spherical mirror to the sample. The resulting LIPSS characteristics (periods, areas) were analyzed by scanning electron microscopy. A wavelength-dependent plasmonic mechanism is proposed to explain the delay-dependence of the LIPSS. These two-color experiments extend previous single-color studies and prove the importance of the ultrafast energy deposition for LIPSS formation.

Time-resolved microscopy with random lasers.

We demonstrate that random lasers provide an outstanding strobe light source for time-resolved microscopy. Utilizing a random laser to illuminate a commercially available microscope enables single exposure, speckle-free time-resolved imaging. Aside from conventional optical transmission microscopy, we also perform time-resolved investigations in phase contrast mode. We apply this method to the monitoring of fs-laser-induced microdot formation in bulk a-SIO(2). Time-resolved investigations show that microdot formation lasts over several microseconds after laser excitation.

Rippled area formed by surface plasmon polaritons upon femtosecond laser double-pulse irradiation of silicon.

The formation of near-wavelength laser-induced periodic surface structures (LIPSS) on silicon upon irradiation with sequences of Ti:sapphire femtosecond laser pulse pairs (pulse duration 150 fs, central wavelength 800 nm) is studied theoretically. For this purpose, the nonlinear generation of conduction band electrons in silicon and their relaxation is numerically calculated using a two-temperature model approach including intrapulse changes of optical properties, transport, diffusion and recombination effects. Following the idea that surface plasmon polaritons (SPP) can be excited when the material turns from semiconducting to metallic state, the "SPP active area" is calculated as function of fluence and double-pulse delay up to several picoseconds and compared to the experimentally observed rippled surface areas. Evidence is presented that multi-photon absorption explains the large increase of the rippled area for temporally overlapping pulses. For longer double-pulse delays, relevant relaxation processes are identified. The results demonstrate that femtosecond LIPSS on silicon are caused by the excitation of SPP and can be controlled by temporal pulse shaping.

Time-resolved imaging of laser-induced refractive index changes in transparent media.

We describe a method to visualize ultrafast laser-induced refractive index changes in transparent materials with a 310 fs impulse response and a submicrometer spatial resolution. The temporal profile of the laser excitation sequence can be arbitrarily set on the subpicosecond and picosecond time scales with a pulse shaping unit, allowing for complex laser excitation. Time-resolved phase contrast microscopy reveals the real part of the refractive index change and complementary time-resolved optical transmission microscopy measurements give access to the imaginary part of the refractive index in the irradiated region. A femtosecond laser source probes the complex refractive index changes from the excitation time up to 1 ns, and a frequency-doubled Nd:YAG laser emitting 1 ns duration pulses is employed for collecting data at longer time delays, when the evolution is slow. We demonstrate the performance of our setup by studying the energy relaxation in a fused silica sample after irradiation with a double pulse sequence. The excitation pulses are separated by 3 ps. Our results show two dimensional refractive index maps at different times from 200 fs to 100 µs after the laser excitation. On the subpicosecond time scale we have access to the spatial characteristics of the energy deposition into the sample. At longer times (800 ps), time-resolved phase contrast microscopy shows the appearance of a strong compression wave emitted from the excited region. On the microsecond time scale, we observe energy transfer outside the irradiated region.

Extended-area nanostructuring of TiO2 with femtosecond laser pulses at 400 nm using a line focus.

An efficient way to generate nanoscale laser-induced periodic surface structures (LIPSS) in rutile-type TiO(2) with frequency-converted femtosecond laser pulses at wavelengths around 400 nm is reported. Extended-area structuring on fixed and moving substrates was obtained by exploiting the line focus of a cylindrical lens. Under defined conditions with respect to pulse number, pulse energy and scanning velocity, two types of ripple-like LIPSS with high and low spatial frequencies (HSFL, LSFL) with periods in the range of 90 nm and 340 nm, respectively, were formed. In particular, lower numbers of high energetic pulses favour the generation of LSFL whereas higher numbers of lower energetic pulses enable the preferential creation of HSFL. Theoretical calculations on the basis of the Drude model support the assumption that refractive index changes by photo-excited carriers are a major mechanism responsible for LSFL. Furthermore, the appearance of random substructures as small as 30 nm superimposing low spatial frequency ripples is demonstrated and their possible origin is discussed.

Low-loss waveguides fabricated in BK7 glass by high repetition rate femtosecond fiber laser.

For the first time femtosecond-laser writing has inscribed low-loss optical waveguides in Schott BK7 glass, a commercially important type of borosilicate widely used in optical applications. The use of a variable repetition rate laser enabled the identification of a narrow processing window at 1 MHz repetition rate with optimal waveguides exhibiting propagation losses of 0.3 dB/cm and efficient mode matching to standard optical fibers at a 1550 nm wavelength. The waveguides were characterized by complementary phase contrast and optical transmission microscopy, identifying a micrometer-sized guiding region within a larger complex structure of both positive and negative refractive index variations.

Scalable multichannel micromachining with pseudo-nondiffracting vacuum ultraviolet beam arrays generated by thin-film axicons.

Scalable multichannel microstructuring was demonstrated by multiplexing a focused molecular fluorine laser beam with cylindrical nanolayer microaxicons into an array of converging pseudo-nondiffracting subbeams. The axicons were fabricated by shadow-mask vapor deposition of magnesium fluoride onto substrates of identical material. Long-period surface gratings of variable pitch were generated on poly(methyl methacrylate) by varying the target position within the converging periodic focal lines.