Surface topography of ultrashort laser-irradiated CaF2

A single-crystal CaF₂ (111) was irradiated with single and multiple laser (Ti:sapphire, 800 nm, 25 fs) shots at fluences ranging from 0.25 to 1.5 J cm^?2. In this fluence regime, a single laser pulse usually leads to typical bump-like features ranging from 200 nm to 1.5 μm in diameter and 10–50 nm in height. These bumps are related to compressive stresses due to a pressure build-up induced by fast laser heating and their subsequent relaxation. When CaF₂ is irradiated with successive (in our case 20) shots at a laser fluence of 1.5 J cm^?2, nanocavities at the top of the microbumps are observed. The formation of these nanocavities is regarded as an explosion and is attributed to the explosive expansion generated by shock waves due to laser-induced plasma after the nonlinear absorption of the laser energy by the material. Such kinds of surface structures at the nanometre scale could be attractive for nanolithography.     

Computational study of plasma-assisted photoacoustic response from gold nanoparticles irradiated by off-resonance ultrafast laser

The gold nanoparticles (AuNPs) are capable of enhancing the incident laser field in the form of scattered near field for even an off-resonance irradiation where the incident laser wavelength is far away from the localized surface plasmon resonance (LSPR). If the intensity of the pulse laser is large enough, this capability can be employed to generate a highly localized free electron (plasma) in the vicinity of the particles. The generated plasma can absorb more energy during the pulse, and this energy deposition can be considered as an energy source for structural mechanics calculations in the surrounding media to generate a photoacoustic (PA) signal. To show this, in this paper, we model plasma-mediated PA pressure wave propagation from a 100-nm AuNPs and the surrounding media irradiated by an ultrashort pulse laser. In this model, the AuNP is immersed in water and the laser pulse width is ranging from 70 fs to 2 ps at the wavelength of 800 nm (off-resonance). Our results qualitatively show the substantial impact of the energy deposition in plasma on the PA signal through boosting the pressure amplitudes up to ～1000 times compared to the conventional approach.     

fs Laser surface nano-structuring of high refractory ceramics to enhance solar radiation absorbance

The surface and structural modification of titanium (Ti) has been explored after the interaction of ultrashort laser pulses with the surface target. The targets were exposed by femtosecond Ti: Sapphire laser pulses in liquid (ethanol) and dry (air) environment. In order to explore the effect of pulse energy, the targets were exposed to 1,000 succeeding pulses for various pulse energies ranging from 200 to 500 μJ for pulse duration of 25 fs. SEM analyses were performed for central as well as the peripheral ablated areas of the target. It was found that in the case of ethanol (both for central and peripheral ablated areas) there is a grain growth along with nanoscale pores and dots when the target was irradiated for 200 μJ. For intermediate energies (300–400 μJ), grains of 1–2 μm with distinct boundaries are formed in the central ablated area. Whereas in the peripheral ablated area, laser-induced periodic surface structures (LIPSS) and globules are grown. For the highest pulse energy (500 μJ), distinct grains are observed for both regions. However, in the peripheral area the grains are of bigger size with cracks along the boundaries. In case of ablation in air, in the center of ablated areas, island-like structures with multiple ablative layer or LIPSS and nanoscale spheres are observed both for lower and intermediate pulse energies. For the highest pulse energy only nanoscale LIPSS could be observed. For ablation in air at the peripheral areas, well-defined, laser-induced periodic surface structures are observed for all pulse energies. Raman spectroscopy reveals that the liquid (ethanol) environment forms the carbonyl compounds with the metal and induces C–C stretching vibration, whereas in case of air, hydroxo complexes are formed. It has been found that surface treatment of Ti with ultrashort (25 fs) laser radiation in ethanol environment allows the growth of particular surface structures in the form of grains and simultaneously induces changes in its chemical composition.     

Implications of transient changes of optical and surface properties of solids during femtosecond laser pulse irradiation to the formation of laser-induced periodic surface structures

The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of silicon wafer surfaces by linearly polarized Ti:sapphire femtosecond laser pulses (pulse duration 130 fs, central wavelength 800 nm) is studied experimentally and theoretically. In the experiments, so-called low-spatial frequency LIPSS (LSFL) were found with periods smaller than the laser wavelength and an orientation perpendicular to the polarization. The experimental results are analyzed by means of a new theoretical approach, which combines the widely accepted LIPSS theory of Sipe et al. with a Drude model, in order to account for transient (intra-pulse) changes of the optical properties of the irradiated materials. It is found that the LSFL formation is caused by the excitation of surface plasmon polaritons, SPPs, once the initially semiconducting material turns to a metallic state upon formation of a dense free-electron-plasma in the material and the subsequent interference between its electrical field with that of the incident laser beam resulting in a spatially modulated energy deposition at the surface. Moreover, the influence of the laser-excited carrier density and the role of the feedback upon the multi-pulse irradiation and its relation to the excitation of SPP in a grating-like surface structure is discussed.     

Micromechanism of sulfurizing activated carbon and its ability to adsorb mercury

The effect of ambient environment (dry or wet) and overlapping laser pulses on the laser ablation performance of brass has been investigated. For this purpose, a Q-switched, frequency doubled Nd:YAG laser with a wavelength of 532 nm, pulse energy of 150 mJ, pulse width of 6 ns and repetition rate of 10 Hz is employed. In order to explore the effect of ambient environments, brass targets have been exposed in deionized water, methanol and air. The targets are exposed for 1000, 2000, 3000 and 4000 succeeding pulses in each atmosphere. The surface morphology and chemical composition of ablated targets have been characterized by using Scanning Electron Microscope (SEM), Atomic Force Microscope (AFM) and Attenuated Total Reflection (ATR) techniques. In case of liquid environment, various features like nano- and micro-scale laser-induced periodic surface structures with periodicity 500 nm–1 μm, cavities of size few micrometers with multiple ablative layers and phenomenon of thermal stress cracking are observed. These features are originated by various chemical and thermal phenomena induced by laser heating at the liquid–solid interfaces. The convective bubble motion, explosive boiling, pressure gradients, cluster and colloid formation due to confinement effects of liquids are possible cause for such kind of features. The metal oxides and alcohol formed on irradiated surface are also playing the significant role for the formation of these kinds of structure. In case of air one huge crater is formed along with the redeposition of sputtered material and is ascribed to laser-induced evaporation and oxide formation.     

Experimental investigation of ablation efficiency and plasma expansion during femtosecond and nanosecond laser ablation of silicon

Femtosecond laser (Ti:sapphire, 100 fs pulse duration) ablation of silicon in air was compared with nanosecond laser (Nd:YAG, 3 ns pulse duration) ablation at ultraviolet wavelength (266 nm). Laser ablation efficiency was studied by measuring crater depth as a function of pulse number. For the same number of laser pulses, the fs-ablated crater was about two times deeper than the ns-crater. The temperature and electron number density of the laser-induced plasma were determined from spectroscopic measurements. The electron number density and temperature of fs-induced plasmas decreased faster than ns-induced plasmas due to different energy deposition mechanisms. Images of the laser-induced plasma were obtained with femtosecond time-resolved laser shadowgraph imaging. Plasma expansion in both the perpendicular and the lateral directions were compared. PACS 52.38.Mf; 52.30.-q     

Dynamics of the formation of laser-induced periodic surface structures on dielectrics and semiconductors upon femtosecond laser pulse irradiation sequences

The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of fused silica and silicon with multiple (N _DPS) 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.     

Frequency shifting of sub-100 fs laser pulses by stimulated Raman scattering in a capillary filled with pressurized gas

The technique of Raman conversion of sub-100 fs laser pulses based on excitation of active medium by two orthogonally polarized pulses has been developed for Raman lasers with a glass capillary. 52 fs Stokes pulse at the wavelength of 1200 nm has been generated by stimulated Raman scattering of 48 fs Ti:sapphire laser pulse at the wavelength of 800 nm in hydrogen. 13% energy conversion efficiency has been achieved at pulse repetition rate up to 2 kHz.     

Diffraction of white-light supercontinuum by femtosecond laser-induced transient grating in carbon bisulfide

Experiments on fs laser-induced transient grating (LITG) in carbon bisulfide (CS2 ) are carried out to explore the chirp characteristics of a white-light supercontinuum (SC) generated by a 800-nm, 160-fs laser pulse in a 4-mm thick Al2O3 crystal. Two orders of diffraction signals of SC by fs LITG in CS2 are observed, demonstrating that both the third-order process and the fifth-order process are present simultaneously. The experimental results also imply that the formation of an fs transient refractive-index grating in CS2 is mainly due to the electronic polarization process.     

The influence of ultra-fast temporal energy regulation on the morphology of Si surfaces through femtosecond double pulse laser irradiation

The effect of ultra-short laser-induced morphological changes upon irradiation of silicon with double pulse sequences is investigated under conditions that lead to mass removal. The temporal delay between 12 double and equal-energy pulses (E _p=0.24 J/cm² each, with pulse duration t _p=430 fs, 800 nm laser wavelength) was varied between 0 and 14 ps and a decrease of the damaged area, crater depth size and periodicity of the induced subwavelength ripples (by 3–4 %) was observed with increasing pulse delay. The proposed underlying mechanism is based on the combination of carrier excitation and energy thermalization and capillary wave solidification and aims to provide an alternative explanation of the control of ripple periodicity by temporal pulse tailoring. This work demonstrates the potential of pulse shaping technology to improve ultra-fast laser-assisted micro/nanoprocessing.     

197 nm femtosecond laser-pulse duration: comparison of autocorrelation measurements

An easy and reliable way is presented to measure the duration of UV femtosecond laser pulses of λ < 200 nm. The used autocorrelation techniques are based on two-photon absorption (TPA) in different TPA media, especially calcium fluoride (CaF₂). For 197 nm, the laser-pulse energy transmission and the laser-induced fluorescence of self-trapped excitons at 278 nm are applied. Both methods yield nearly the same second-order autocorrelation functions allowing to analyze the investigated laser pulse and obtain its duration of $(350\pm10)$  fs.     

Compression of long-cavity Ti:sapphire oscillator pulses with large-mode-area photonic crystal fibers

Motivated by the pulse compression challenge of novel long-cavity, high-pulse-energy Ti:sapphire laser oscillators, we report on ~280 nm supercontinuum generation and 4.5-times compression of close to transform limited, high-energy oscillator pulses using different large-mode-area photonic crystal fibers and standard chirped mirrors. As input, we used pulses of a long-cavity Ti:sapphire oscillator with 190 nJ pulse energy, 70 fs pulse length and 3.6 MHz repetition rate. Compressed pulses at the fiber/compressor output had a duration of 15–18 fs with up to 100 nJ pulse energy representing as much as 53 % throughput for the fiber/chirped mirror system. Using transform-limited input pulses, we could use short fiber pieces and thus a simple, low-dispersion chirped mirror compressor comprised of one pair of mirrors.     

Simulation of rippled structure adjustments based on localized transient electron dynamics control by femtosecond laser pulse trains

This study investigates the effects of pulse energy distributions on subwavelength ripple structures (the ablation shapes and subwavelength ripples) using the plasma model with the consideration of laser particle–wave duality. In the case studies, the laser pulse (800 nm, 50 fs) trains consist of double pulses within a train with the energy ratios of 1:2, 1:1, and 2:1. Localized transient electron densities, material optical properties, and surface plasmon generation are strongly affected by the energy distributions. Hence, the adjustment of the ablation shape and subwavelength ripples can be achieved based on localized transient electron dynamics control during femtosecond laser pulse train processing of dielectrics. The simulation results show that better, more uniform structures, in terms of ablation shapes and subwavelength ripples, can be easily formed at a lower fluence or subpulse energy ratio of 1:1 with a fixed fluence. It is also found that pulse trains at a 1:1 energy ratio are preferred for drilling high-aspect-ratio microholes or microchannels.     

Non-adiabatic transition in C2H5OH+ on a light-dressed potential energy surface by ultrashort pump-and-probe laser pulses

We experimentally investigate how parameters of ultrashort laser pulses such as the pulse width and wavelength could induce changes in the dynamics of vibrational wave packets on the light-dressed-potential energy surface (LD-PES) of C₂H₅OH⁺ using a pump-and-probe pulse excitation scheme. The probability of non-adiabatic transition at 800 nm from the singly ionized ground state to the repulsive excited state leading to C–O bond breaking is enhanced when a probe laser pulse is delayed by ～180 fs. At this pulse delay, on the other hand, C–C bond breaking is significantly suppressed. Therefore, the deformation of LD-PES is considered to change the direction of the wave packet traveling originally along the C–C stretching into the direction along the C–O stretching. This non-adiabatic transition leading to the redirection of the dissociating wave packet is found to occur more efficiently at the probe laser wavelengths at 400 nm than at 800 nm. The critical pulse delay is still ～180 fs even at 400 nm.     

Sub-100-nm laser-induced periodic surface structures upon irradiation of titanium by Ti:sapphire femtosecond laser pulses in air

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.     

SEM and Raman spectroscopy analyses of laser-induced periodic surface structures grown by ethanol-assisted femtosecond laser ablation of chromium

The effect of fluence and pulse duration on the growth of nanostructures on chromium (Cr) surfaces has been investigated upon irradiation of femtosecond (fs) laser pulses in a liquid confined environment of ethanol. In order to explore the effect of fluence, targets were exposed to 1000 pulses at various peak fluences ranging from 4.7 to 11.8?J?cm^–2 for pulse duration of ～25?fs. In order to explore the effect of pulse duration, targets were exposed to fs laser pulses of various pulse durations ranging from 25 to 100?fs, for a constant fluence of 11.8?J?cm^–2. Surface morphology and structural transformations have been analyzed by scanning electron microscopy and Raman spectroscopy, respectively. After laser irradiation, disordered sputtered surface with intense melting and cracking is obtained at the central ablated areas, which are augmented with increasing laser fluence due to enhanced thermal effects. At the peripheral ablated areas, where local fluence is approximately in the range of 1.4–4?mJ?cm^–2, very well-defined laser-induced periodic surface structures (LIPSS) with periodicity ranging from 270 to 370?nm along with dot-like structures are formed. As far as the pulse duration is concerned, a significant effect on the surface modification of Cr has been revealed. In the central ablated areas, for the shortest pulse duration (25?fs), only melting has been observed. However, LIPSS with dot-like structures and droplets have been grown for longer pulse durations. The periodicity of LIPSS increases and density of dot-like structures decreases with increasing pulse duration. The chemical and structural modifications of irradiated Cr have been revealed by Raman spectroscopy. It confirms the formation of new bands of chromium oxides and enol complexes or Cr-carbonyl compounds. The peak intensities of identified bands are dependent upon laser fluence and pulse duration.     

Preparation of C/Ni–NiO composite nanofibers for anode materials in lithium-ion batteries

We report here on a systematic study about the formation of laser-induced periodic surface structures (LIPSS) on biopolymers. Self-standing films of the biopolymers chitosan, starch and the blend of chitosan with the synthetic polymer poly (vinyl pyrrolidone), PVP, were irradiated in air with linearly polarized laser beams at 193, 213 and 266 nm, with pulse durations in the range of 6–17 ns. The laser-induced periodic surface structures were topographically characterized by atomic force microscopy and the chemical modifications induced by laser irradiation were inspected via Raman spectroscopy. Formation of LIPSS parallel to the laser polarization direction, with periods similar to the laser wavelength, was observed at efficiently absorbed wavelengths in the case of the amorphous biopolymer chitosan and its blend with PVP, while formation of LIPSS is prevented in the crystalline starch biopolymer.     

Rippled area formed by surface plasmon polaritons upon femtosecond laser double-pulse irradiation of silicon: the role of carrier generation and relaxation processes

The formation of laser-induced periodic surface structures (LIPSS, ripples) upon irradiation of silicon with multiple irradiation sequences consisting of femtosecond laser pulse pairs (pulse duration 150 fs, central wavelength 800 nm) is studied numerically using a rate equation system along with a two-temperature model accounting for one- and two-photon absorption and subsequent carrier diffusion and Auger recombination processes. The temporal delay between the individual equal-energy fs-laser pulses was varied between 0 and ～4 ps for quantification of the transient carrier densities in the conduction band of the laser-excited silicon. The results of the numerical analysis reveal the importance of carrier generation and relaxation processes in fs-LIPSS formation on silicon and quantitatively explain the two time constants of the delay-dependent decrease of the low spatial frequency LIPSS (LSFL) area observed experimentally. The role of carrier generation, diffusion and recombination is quantified individually.     

Effects of initial humidity and temperature on laser-filamentation-induced condensation and snow formation

We investigated the effects of initial humidity and temperature on the formation of water condensation and various snowflake patterns by firing high-repetition filaments of femtosecond Ti-sapphire laser pulses at 9 mJ/50 fs per pulse into a cloud chamber. While adjusting initial temperature and humidity distributions near the filaments, snowflakes and ice particles with various shapes and sizes were observed on the bottom cold plate. In addition, significant differences were found in the weights of the laser-induced snow below the filament center. From those data, initial conditions of low temperature (<?15 °C) and high humidity (relative to water RH_w > (90 ± 11) % and to ice RH_i > (120 ± 15) %) were found being important to assist an efficient laser-filamentation-induced condensation and snow formation.     

Progressive formation of fine and coarse ripples on SiC surface by repeated irradiation of femtosecond laser pulses

In this work, we report the progressive formation of first nanoparticles, next fine ripples, and eventually coarse ripples during the irradiation of single-crystal 6H-SiC surfaces with increasing number of femtosecond laser pulses (λ = 515 nm, τ = 250 fs, repetition rate = 100 kHz). At laser fluences greater than the single-pulse ablation threshold, nanoparticles were produced on the surface by the first few pulses over which fine ripple patterns overlapped at increased pulse numbers. As the pulse number was further increased over ten, the surface was gradually transformed into a coarse ripple–covered one. At laser fluence below the threshold, however, only fine ripples were formed nonuniformly.