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Multiple pulse investigations of 130-fs Ti:sapphire laser-induced damage of a high reflecting mirror consisting of alternating ?/4-layers of Ta2O5 and SiO2 and a single 500-nm Ta2O5 film were performed. In both cases, fused silica served as the substrate. For a fixed number of 1000 laser pulses per spot, a decrease in the damage threshold fluence of the mirror by a factor of two was observed by changing the repetition rate from 10 Hz to 1 kHz. A single 500-nm Ta2O5 film shows higher damage resistance compared to the mirror. The mirror and the Ta2O5 film samples were partially coated with a 300-nm-thick aluminium layer. The aluminium coating does not influence the damage threshold of the dielectrics underneath.
Structure formation on the surface of indium phosphide irradiated by femtosecond laser pulses
(2005)
Laser-induced periodic surface structures (LIPSS; ripples) with different spatial characteristics have been observed after irradiation of single-crystalline indium phosphide (c-InP) with multiple linearly polarized femtosecond pulses (130 fs, 800 nm) in air. With an increasing number of pulses per spot, N, up to 100, a characteristic evolution of two different types of ripples has been observed, i.e., (i) the growth of a grating perpendicular to the polarization vector consisting of nearly wavelength-sized periodic lines and (ii), in a specific pulse number regime (N = 530), the additional formation of equally oriented ripples with a spatial period close to half of the laser wavelength. For pulse numbers higher than 50, the formation of micrometer-spaced grooves has been found, which are oriented perpendicular to the ripples. These topographical surface alterations are discussed in the frame of existing LIPSS theories.
The effects of single femtosecond laser pulse irradiation (130 fs pulse duration, 800 nm center wavelength) on the structure of binary lithium silicate glasses of varying chemical compositions were investigated by micro-Raman spectroscopy. Permanent modifications were generated at the surface of the glass samples with varying laser fluences in the ablative regime and evaluated for changes in the corresponding Raman band positions and bandwidths. For increasing laser fluences, the position of certain Raman bands changed, indicating an increase in the mass density of the glass inside the irradiated area. Simultaneously, the widths of all investigated bands increased, indicating a higher degree of disorder in the glass structure with respect to bond-angle and bond-length variations.
The formation of laser-induced periodic surface structures (LIPSS) in different materials (metals, semiconductors, and dielectrics) upon irradiation with linearly polarized fs-laser pulses (τ~30–150 fs, λ~800 nm) in air environment is studied experimentally and theoretically. In metals, predominantly low-spatial-frequency-LIPSS with periods close to the laser wavelength λ are observed perpendicular to the polarization. Under specific irradiation conditions, high-spatial-frequency-LIPSS with sub-100-nm spatial periods (~λ/10) can be generated. For semiconductors, the impact of transient changes of the optical properties to the LIPSS periods is analyzed theoretically and experimentally. In dielectrics, the importance of transient excitation stages in the LIPSS formation is demonstrated experimentally using (multiple) double-fs-laser-pulse irradiation sequences. A characteristic decrease of the LIPSS periods is observed for double-pulse delays of less than 2 ps.
The formation of laser-induced periodic surface structures (LIPSS) on two different silica polymorphs (single-crystalline synthetic quartz and commercial fused silica glass) upon irradiation in air with multiple linearly polarized single- and double-fs-laser pulse sequences (τ = 150 fs pulse duration, λ = 800nm center wavelength, temporal pulse separation Δt < 40 ps) is studied experimentally and theoretically. Two distinct types of fs-LIPSS [so-called low-spatial-frequency LIPSS (LSFL) and high-spatial-frequency LIPSS (HSFL)] with different spatial periods and orientations were identified. Their appearance was characterized with respect to the experimental parameters peak laser fluence and number of laser pulses per spot. Additionally, the 'dynamics' of the LIPSS formation was addressed in complementary double-fs-pulse experiments with varying delays, revealing a characteristic change of the LSFL periods. The experimental results are interpreted on the basis of a Sipe-Drude model considering the carrier dependence of the optical properties of fs-laser excited silica. This new approach provides an explanation of the LSFL orientation parallel to the laser beam polarisation in silica—as opposed to the behaviour of most other materials.
The formation of laser-induced periodic surface structures upon irradiation of titanium, silicon, and fused silica with multiple irradiation sequences consisting of parallel polarized Ti:sapphire femtosecond laser pulse pairs (pulse duration 50–150 fs, central wavelength ~800 nm) is studied experimentally. The temporal delay between the individual near-equal energy fs-laser pulses was varied between 0 and 5 ps with a temporal resolution of better than 0.2 ps. The surface morphology of the irradiated surface areas is characterized by means of scanning electron microscopy (SEM). In all materials a decrease of the rippled surface area is observed for increasing delays. The characteristic delay decay scale is quantified and related to material dependent excitation and energy relaxation processes.
The irradiation of ~0.9-µm-thick hydrogenated amorphous carbon (a-C:H) layers deposited on silicon substrates with single femtosecond (fs) laser pulses (35 fs pulse duration, 790 nm centre wavelength) in air is studied experimentally. Irradiation spots have been generated with different peak fluences and subsequently investigated by optical topometry, micro Raman spectroscopy and microscale mechanical indentation in order to evaluate their microscopic, topographical, structural and mechanical properties (e.g. elastic modulus). By this multi-method approach, a clear separation of different effects (delamination and graphitisation) becomes possible. The joint application of mechanical and spectroscopic techniques provides unique insights into the effects of the fs-laser radiation on the carbon layer.
Femtosecond diffraction dynamics of laser-induced periodic surface structures on fused silica
(2013)
The formation of laser-induced periodic surface structures (LIPSS) on fused silica upon irradiation with linearly polarized fs-laser pulses (50 fs pulse duration, 800?nm center wavelength) is studied experimentally using a transillumination femtosecond time-resolved (0.1 ps-1 ns) pump-probe diffraction approach. This allows to reveal the generation dynamics of near-wavelength-sized LIPSS showing a transient diffraction at specific spatial frequencies even before a corresponding permanent surface relief was observed. The results confirm that the ultrafast energy deposition to the materials surface plays a key role and triggers subsequent physical mechanisms such as carrier scattering into self-trapped excitons.
The effects of femtosecond laser pulse irradiation on the glass structure of alkaline silicate glasses were investigated by x-ray absorption near edge structure spectroscopy using the beamline of the Physikalisch-Technische Bundesanstalt at the electron synchrotron BESSY II in Berlin (Germany) by analyzing the magnesium Κ-edge absorption peak for different laser fluences. The application of fluences above the material modification threshold (2.1 J/cm²) leads to a characteristic shift of ~1.0 eV in the Κ-edge revealing a reduced (~3%) mean magnesium bond length to the ligated oxygen ions (Mg-O) along with a reduced average coordination number of the Mg ions.
The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of fused silica with multiple irradiation sequences of parallel polarized Ti:sapphire femtosecond laser pulse pairs (160 fs pulse duration, 800 nm central wavelength) was studied experimentally. For that purpose, a Michelson interferometer was used to generate near-equal-energy double-pulse sequences allowing the temporal pulse delay between the parallel-polarized individual fs-laser pulses to be varied between 0 and 40 ps with ~0.2 ps temporal resolution. The surface morphologies of the irradiated surface areas were characterized by means of scanning electron and scanning force microscopy. In the sub-ps delay range a strong decrease of the LIPSS periods and the ablation crater depths with the double-pulse delay was observed indicating the importance of the laser-induced free-electron plasma in the conduction band of the solids for the formation of LIPSS.
The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of fused silica and silicon with multiple (NDPS) irradiation sequences consisting of linearly polarized femtosecond laser pulse pairs (pulse duration ~150 fs, central wavelength ~800 nm) is studied experimentally. Nearly equal-energy double-pulse sequences are generated allowing the temporal pulse delay Δt between the cross-polarized individual fs-laser pulses to be varied from -40 ps to +40 ps with a resolution of ~0.2 ps. The surface morphologies of the irradiated surface areas are characterized by means of scanning electron and scanning force microscopy. Particularly for dielectrics in the sub-ps delay range striking differences in the orientation and spatial characteristics of the LIPSS can be observed. For fused silica, a significant decrease of the LIPSS spatial periods from ~790 nm towards ~550 nm is demonstrated for delay changes of less than ~2 ps. In contrast, for silicon under similar irradiation conditions, the LIPSS periods remain constant (~760 nm) for delays up to 40 ps. The results prove the impact of laser-induced electrons in the conduction band of the solid and associated transient changes of the optical properties on fs-LIPSS formation.
The formation of laser-induced periodic surface structures (LIPSS) on titanium upon irradiation with linearly polarized femtosecond (fs) laser pulses (τ = 30 fs, λ = 790 nm) in an air environment is studied experimentally and theoretically. In the experiments, the dependence on the laser fluence and the number of laser pulses per irradiation spot has been analyzed. For a moderate number of laser pulses (N < 1000) and at fluences between ~0.09 and ~0.35 J/cm², predominantly low-spatial-frequency-LIPSS with periods between 400 nm and 800 nm are observed perpendicular to the polarization. In a narrow fluence range between 0.05 and 0.09 J/cm², high-spatial-frequency-LIPSS with sub-100-nm spatial periods (~λ/10) can be generated with an orientation parallel to the polarization (N = 50). These experimental results are complemented by calculations based on a theoretical LIPSS model and compared to the present literature.
We investigated the initial modification and ablation of crystalline silicon with single and multiple Ti:sapphire laser pulses of 5 to 400 fs duration. In accordance with earlier established models, we found the phenomena amorphization, melting, re-crystallization, nucleated vaporization, and ablation to occur with increasing laser fluence down to the shortest pulse durations. We noticed new morphological features (bubbles) as well as familiar ones (ripples, columns). A nearly constant ablation threshold fluence on the order of 0.2 J/cm2 for all pulse durations and multiple-pulse irradiation was observed. For a duration of ,100 fs, significant incubation can be observed, whereas for 5 fs pulses, the ablation threshold does not depend on the pulse number within the experimental error. For micromachining of silicon, a pulse duration of less than 500 fs is not advantageous.
The ultrafast laser ablation of silicon has been investigated experimentally and theoretically. The theoretical description is based on molecular dynamics (MD) simulations combined with a microscopic electronic model. We determine the thresholds of melting and ablation for two different pulse durations =20 and 500 fs. Experiments have been performed using 100 Ti:Sap-phire laser pulses per spot in air environment. The ablation thresholds were determined for pulses with a duration of 25 and 400 fs, respectively. Good agreement is obtained between theory and experiment.
Laser ablation of single-crystalline indium phosphide (InP) was performed in air by means of linearly polarized Ti : sapphire femtosecond pulses (800 nm, 130 fs, 10 Hz). As a result of the irradiation with a variable number of laser pulses per spot (N /spl les/ 5), several morphological changes (crater formation, rim formation, ripple structures, and cones) were observed. These effects were explored using force modulation microscopy (FMM), a technique based on scanning force microscopy, allowing the simultaneous imaging of both topography and local stiffness at a high lateral resolution. The first laser pulse induces the formation of a protruding rim (height < 20 nm, width /spl ap/ 300 nm) bordering the ablated crater. A Fourier analysis of the multipulse generated topographies reveals the formation of wavelength-sized periodic ripples (modulation depth < 100 nm) with an orientation perpendicular to that of the electric field vector of the laser radiation. Besides these morphological alterations, material modifications were also observed in the irradiated regions by means of the FMM technique. Within the ablated craters, local stiffness variations were found revealing an inhomogeneous material composition/structure as a consequence of the femtosecond pulse laser treatment.
Femtosecond time-resolved microscopy has been used to analyze the structural transformation dynamics (melting, ablation, and solidification phenomena) induced by single intense 130 fs laser pulses in single-crystalline (100)-indium phosphide wafers in air on a time scale from ~100 fs up to 8 ns. In the ablative regime close to the ablation threshold, transient surface reflectivity patterns are observed by fs microscopy on a ps to ns time scale as a consequence of the complex spatial density structure of the ablating material (dynamic Newton fringes). At higher fluences, exceeding six times the ablation threshold, optical breakdown causes another, more violent ablation regime, which reduces the energy deposition depth along with the time of significant material removal. As a consequence, ablation lasts longer in a ring-shaped region around the region of optical breakdown. This leads to the formation of a crater profile with a central protrusion. In the melting regime below the ablation threshold, the melting dynamics of indium phosphide has been quantified and subsequent superficial amorphization has been observed upon solidification on the ns time scale leading to amorphous layer thicknesses of the order of a few tens of nanometers.
We report self-assembly of periodic surface structures in a commercial block copolymer (BCP) (Filofocon A) upon irradiation with a few tens of excimer laser pulses (20 ns, 193 nm) at fluences above the ablation threshold. This new type of structures is characterized by much larger periods than those characteristic for Laser-Induced Periodic Surface Structures (LIPSS) and features nanochains instead of ripples. We find a period of 790?nm at 400 mJ/cm², scaling linearly with laser fluence up to a maximum of 1.0 µm. While an entangled random network of nanochains is produced for normal-incidence and non-polarized light, nanochain alignment can be achieved either by irradiation at an angle or by using linearly polarized light, forming a lamella-like structure. In both cases, the nanochains are aligned parallel to the penetrating polarization orientation and their period does not show a dependence on the angle of incidence, as opposed to the general behavior of standard LIPSS. Also, our results show that the chains are not formed by frozen capillary waves. In contrast, we show analogies of the nanochains produced to lamellar structures fabricated on a smaller scale in other BCP. We discuss the origin of the self-assembly process in terms of a combination of chemical (BCP), optical (surface scattering), and thermal (melting, coarsening, and ablation) effects.
Nonlinear optical properties such as the nonlinear refractive index and nonlinear absorption are characterized by z-scan measurements for a series of silicate glasses upon irradiation with laser pulses of 130 fs duration and 800 nm center wavelength. The stoichiometry of the silicate glasses is varied systematically to reveal the influence of the glass composition on the nonlinear optical properties. Additionally, the thermal properties such as glass–transformation temperature and thermal expansion coefficient are obtained from dilatometric measurements. It is found that the nonlinear refractive index is mainly related to the silica matrix. The nonlinear absorption is increased with the addition of network–forming ions.
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.