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Paper des Monats
- ja (3)
The influence of different laser pulse lengths on the removal of a polymer layer from metal substrates was investigated. As model systems, doped poly(methylmetacrylate) (PMMA) on titanium and tungsten substrates were selected.
The ablation threshold and irradiation spot morphology of titanium and tungsten were compared for femtosecond (fs) and nanosecond (ns) laser irradiation and different pulse numbers. Nanosecond laser treatment resulted in a non-homogeneous surface morphology for both titanium and tungsten substrates. Femtosecond irradiation of tungsten revealed a homogeneous ablation spot with little changes in the surface morphology. For titanium, the formation of columnar structures within the irradiation spot was observed.
Two different dopant concentrations were used for PMMA to achieve an equal linear absorption coefficient for the femto- and nanosecond laser wavelengths of 790 and 1064 nm. The best results were achieved for the removal of doped PMMA by femtosecond laser irradiation, where only a minimal modification of the metal surface was detected. In the case of nanosecond laser exposure, a pronounced change of the structure was observed, suggesting that damage-free cleaning of the selected metal may only be possible using femtosecond laser pulses. Different experimental parameters, such as laser fluence, pulse repetition rate and sample speed were also investigated to optimize the cleaning quality of doped PMMA from tungsten substrates with femtosecond laser pulses.
A bottom-up approach is presented for the production of arrays of indium islands on a molybdenum layer on glass, which can serve as micro-sized precursors for indium compounds such as copper-indium-gallium-diselenide used in photovoltaics. Femtosecond laser ablation of glass and a subsequent deposition of a molybdenum film or direct laser processing of the molybdenum film both allow the preferential nucleation and growth of indium islands at the predefined locations in a following indium-based physical vapor deposition (PVD) process. A proper choice of laser and deposition parameters ensures the controlled growth of indium islands exclusively at the laser ablated spots. Based on a statistical analysis, these results are compared to the non-structured molybdenum surface, leading to randomly grown indium islands after PVD.
Laser-induced periodic surface structures (LIPSS, ripples) are a universal phenomenon that can be observed on almost any material after the irradiation by linearly polarized laser beams, particularly when using ultrashort laser pulses with durations in the femtosecond to picosecond range. During the past years significantly increasing industrial and research activities have been reported in the field of LIPSS, since their generation in a single-step process provides a simple way of nanostructuring and surface functionalization towards the control of optical, mechanical or chemical surface properties. In this contribution the mechanisms of formation and current trends and applications of LIPSS are reviewed, including the colorization of technical surfaces, the control of surface wetting properties, the mimicry of the natural texture of animals, the tailoring of surface colonization by bacterial biofilms, the advancement of leadless medical pacemakers, and the improvement of the tribological performance of nanostructured metal surfaces.
The formation of nearly wavelength-sized laser-induced periodic surface structures (LIPSS) on
single-crystalline silicon upon irradiation with single (N = 1) and multiple (N ≤ 1000) linearly
polarized femtosecond (fs) laser pulses (pulse duration τ = 130 fs, central wavelength λ = 800 nm)
in air is studied experimentally. Scanning electron microscopy (SEM) and optical microscopy are
used for imaging of the ablated surface morphologies, both revealing LIPSS with periodicities close
to the laser wavelength and an orientation always perpendicular to the polarization of the fs-laser
beam. It is experimentally demonstrated that these LIPSS can be formed in silicon upon irradiation
by single fs-laser pulses—a result that is additionally supported by a recent theoretical model.
Two-dimensional Fourier transforms of the SEM images allow the detailed analysis of the
distribution of the spatial frequencies of the LIPSS and indicate, at a fixed peak fluence, a
monotonous decrease in their mean spatial period between ~770 nm (N = 1) and 560 nm (N
= 1000). The characteristic decrease in the LIPSS period is caused by a feedback-mechanism acting
upon excitation of surface plasmon polaritons at the rough silicon surface which is developing under
the action of multiple pulses into a periodically corrugated surface.
The possibility to excite surface plasmon polaritons (SPPs) at the interface between two media depends on the optical properties of both media and geometrical aspects. Specific conditions allowing the coupling of light with a plasmon-active interface must be satisfied. Plasmonic effects are well described in noble metals where the imaginary part of the dielectric permittivity is often neglected ('perfect medium approximation (PMA)'). However, some systems exist for which such approximation cannot be applied, hence requiring a refinement of the common SPP theory. In this context, several properties of SPPs such as excitation conditions, period of the electromagnetic field modulation and SPP lifetime then may strongly deviate from that of the PMA. In this paper, calculations taking into account the imaginary part of the dielectric permittivities are presented. The model identifies analytical terms which should not be neglected in the mathematical description of SPPs on lossy materials. These calculations are applied to numerous material combinations resulting in a prediction of the corresponding SPP features. A list of plasmon-active interfaces is provided along with a quantification of the above mentioned SPP properties in the regime where the PMA is not applicable.
Single-pulse femtosecond laser-induced forward transfer (LIFT, 30 fs, 790 nm) is used to deposit micron-sized dots of copper and/or indium onto a molybdenum layer on glass. Such systems can serve as precursors for the bottom-up manufacturing of micro-concentrator solar cells based on copper-indium-gallium-diselenide. The influence of the thickness of the copper, indium and combined copper-indium donor layers on the quality of the transferred dots was qualified by scanning electron microscopy, energy-dispersive X-ray analysis, and optical microscopy. The potential for manufacturing of a spatial arrangement adapted to the geometry of micro-lens arrays needed for micro-concentrator solar cells is demonstrated.
A promising technology in photovoltaics is based on micro-concentrator solar cells, where the photovoltaic active area is realized as an array of sub-millimeter sized thin-film solar cells. For copper-indium-gallium-diselenide (CIGSe), the solar cells can be arranged in the foci of a regular arrangement of micro-lenses to enhance their efficiency by light concentration, to allow a better heat dissipation and to save expensive raw material (indium). Different approaches to produce micro-sized precursors of CIGSe absorbers on molybdenum are presented using 30-fs laser pulses at 790 nm wavelength. On the one hand, a multi pulse surface structuring of the molybdenum or the underlying glass substrate and a subsequent physical vapor deposition (PVD) process were used for a site-selective aggregation of indium droplets. On the other hand, a single pulse laser-induced forward transfer (LIFT) was utilized to selectively deposit combined copper/indium/gallium precursor pixels on the molybdenum back contact of the solar cell. It was demonstrated that a postprocessing (selenization, isolation, contacting) of the laser-generated micro-sized precursors results in an array of working CIGSe solar cells with an efficiency of 2.8% for 1 sun illumination.
A new approach is presented to quantify the so-called "heat affected zone" (HAZ) during
femtosecond laser pulse processing. Ablation of titanium nitride (TiN) thin films (~3 μm
thickness) by multiple femtosecond laser pulses (τ=130 fs, λ=800 nm) in air environment was
studied by means of two different surface analytical methods both being sensitive to chemical
alterations at the surface. Scanning Auger electron microscopy was applied for a visualization of the
spatial distribution of specific elements (Ti, O) within the laser-modified areas. The chemical state
of the irradiated surface was revealed by complementary x-ray photoelectron spectroscopy. Both
methods were used for a depth-profiling chemical analysis (tracking the elements Ti, N, O, and C)
using an Ar-ion beam for surface sputtering. In a narrow laser fluence range slightly below the
ablation threshold of TiN significant superficial oxidation can be observed leading to the formation
of substoichiometric TiO2-x. At fluences above the ablation threshold, an increased titanium
concentration is observed within the entire ablation craters. Following upon sputter removal the
elemental distribution into the depth of the nonablated material, the results allow an estimation of
the heat-affected zone for femtosecond laser ablation in air environment. According to our analyses,
the HAZ extends up to a few hundreds of nanometers into the nonablated material.
Femtosecond laser pulses are close to industrial use. The advantages of ultrashort laser pulses for micromachining applications especially in the case of dielectric and biological samples down to pulse durations of 5 fs have been established. The current international standards of laser safety are primarily concerned with CW and pulsed lasers down to the nanosecond range. Therefore, human tissue and laser-protection equipment was investigated with respect to its resistance and protection performance for femtosecond laser illumination down to 30 fs. This included filter glasses for laser protection eyewear, polymer and textile materials used in curtains and guards. Bulk absorber filters can provide enough protection against laser radiation, give a sufficiently broad absorption spectrum. Materials are damaged more easily by femtosecond laser radiation. The need for sufficient spectral broadness as well as the different damage thresholds have to be included in international laser safety standards. This work should trigger the development of novel eye-protection devices that are lighter and ergonomically more acceptable than present commercial models.
Zusammenfassung
Laser pulses in the 10-fs domain provide a quality of micromachining of fused silica and borosilicate glass that is unobtainable with longer pulses in the range of several 100 femtoseconds up to picoseconds. The shortening of the pulses reduces the statistical behavior of the material removal and the ablation process thus attains a more deterministic and reproducible character. The improved reproducibility of ablation is accompanied by significantly smoother morphology. This offers the potential for lateral and vertical machining precision of the order of 100 nm and 10 nm, respectively.
The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of silicon by multiple (N = 100) linearly polarized Ti:sapphire femtosecond laser pulses (duration τ = 30 fs, center wavelength λ0 ~ 790 nm) is studied experimentally in air and water environment. The LIPSS surface morphologies are characterized by scanning electron microscopy and their spatial periods are quantified by two-dimensional Fourier analyses. It is demonstrated that the irradiation environment significantly influences the periodicity of the LIPSS. In air, so-called low-spatial frequency LIPSS (LSFL) were found with periods somewhat smaller than the laser wavelength (ΛLSFL ~ 0.7 × λ0) and an orientation perpendicular to the laser polarization. In contrast, for laser processing in water a reduced ablation threshold and LIPSS with approximately five times smaller periods ΛLIPSS ~ 0.15 × λ0 were observed in the same direction as in air. The results are discussed within the frame of recent LIPSS theories and complemented by a thin film based surface plasmon polariton model, which successfully describes the tremendously reduced LIPSS periods in water.
Recent publications indicate that the order of electrochemical anodization (before or after the laser processing step) plays an important role for the response of bone-forming osteoblasts—an effect that can be utilized for improving permanent dental or removable bone implants. For exploring these different surface functionalities, multimethod morphological, structural, and chemical characterizations are performed in combination with electrochemical pre- and postanodization for two different characteristic microspikes covered by nanometric laser-induced periodic surface structures on Ti–6Al–4V upon irradiation with near-infrared ps-laser pulses (1030 nm wavelength, ≈1 ps pulse duration, 67 and 80 kHz pulse repetition frequency) at two distinct sets of laser fluence and beam scanning parameters. This work involves morphological and topographical investigations by scanning electron microscopy and white light interference microscopy, structural material examinations via X-ray diffraction, and micro-Raman spectroscopy, as well as near-surface chemical analyses by X-ray photoelectron spectroscopy and hard X-ray photoelectron spectroscopy. The results allow to qualify the mean laser ablation depth, assess the spike geometry and surface roughness parameters, and provide new detailed insights into the near-surface oxidation that may affect the different cell growth behavior for pre- or postanodized medical implants.
Near-ablation threshold investigations focusing on the generation of periodic nanostructures and their correlation with physico-chemical
properties of the solid phase such as e.g., the material-dependent surface energy, were conducted. Molecular dynamic modelling in the
sub-picosecond time domain was used to consider ultrafast opto-electronic processes triggering surface reorganization reactions.
Fluid containment of solid interfaces showed strong influence on the resulting micro- and nanostructures due to its drastic reduction of the
surface energy. The phenomena are discussed in respect to the minimization of the surface free energy in dependence of material composition
and interfacial structure.
Ablation experiments in several glasses with single and multishot irradiation by laser pulses in the 10-fs pulse duration domain are presented; physical and technological implications are discussed. We demonstrate that these short pulses offer the potential for lateral and vertical machining precision of the order of 100 nm.
In situ optical second-harmonic generation (SHG) on centrosymmetric crystalline semiconductor electrodes opens up a new field of in situ investigations of hurried solid state interfaces and metal front contacts relevant to electronic and photovoltaic devices, which are rarely accessible by other methods. Photoelectrochemical nanosecond- and femtosecond-pulse laser investigations of silicon (111) electrodes show that in situ SHG is feasible in such complex interfacial systems. In a p-p polarization configuration, the azimuthal dependence of the SHG from oxide-covered and bare n-Si (111) electrodes, with and without Ni contact deposits, have been studied. Etching and regrowth of silicon oxides as well as burried interfacial electric field distributions were monitored. In situ SHG is shown to be extremely sensitive to trapped interfacial charge, crystal misorientations and surface step arrays. An advantage of femtosecond-pulses is the fact that illumination fluences that are well below the damage threshold, but still with sufficient power density, can be applied. (Author)
The formation of nearly wavelength-sized laser-induced periodic surface structures (LIPSSs) on single-crystalline silicon upon irradiation with single or multiple femtosecond-laser pulses (pulse duration τ=130 fs and central wavelength λ=800 nm) in air is studied experimentally and theoretically. In our theoretical approach, we model the LIPSS formation by combining the generally accepted first-principles theory of Sipe and co-workers with a Drude model in order to account for transient intrapulse changes in the optical properties of the material due to the excitation of a dense electron-hole plasma. Our results are capable to explain quantitatively the spatial periods of the LIPSSs being somewhat smaller than the laser wavelength, their orientation perpendicular to the laser beam polarization, and their characteristic fluence dependence. Moreover, evidence is presented that surface plasmon polaritons play a dominant role during the initial stage of near-wavelength-sized periodic surface structures in femtosecond-laser irradiated silicon, and it is demonstrated that these LIPSSs can be formed in silicon upon irradiation by single femtosecond-laser pulses.
On the damage behavior of dielectric films when illuminated with multiple femtosecond laser pulses
(2005)
The physical effects reducing the damage threshold of dielectric films when exposed to multiple femtosecond pulses are investigated.
The measured temperature increase of a Ta2O5 film scales exponentially with the pulse fluence. A polarized luminescence signal is observed that
depends quadratically on the pulse fluence and is attributed to twophoton excitation of self-trapped excitons that form after band-to-band
excitation. The damage fluence decreases with increasing pulse number, but is independent of the repetition rate from 1 Hz to 1 kHz at a constant
pulse number. The repetition rate dependence of the breakdown threshold is also measured for TiO2 , HfO2,
Al2O3, and SiO2 films. A theoretical model is presented that explains these findings.