Reconstruction of Laser-Induced Surface Topography from Electron Backscatter Diffraction Patterns.

International audience

Controlling the surface morphology at the subwavelength scale is one of the cornerstones of modern nanophotonics. Femtosecond laser-induced surface structuring is a viable technique for the large-scale formation of nano- and microscale structures. A typical example is the formation of one-dimensional laser-induced periodic surface structures (LIPSSs), which can lead to strong modifications of optical and wetting properties of the material surface. Creating two-dimensional (2D) patterned structures, however, is a more challenging and rewarding task. Here, we demonstrate a single step method for fabricating various subwavelength structures on the cobalt (Co) surface using different laser fluences (0.12–0.24 J/cm2) and time delay (0–30 ps) between double pulses. More importantly, we can control the geometry and organization of the formed structures demonstrating spherical, triangular, rhombic, and high spatial frequency LIPSSs using two temporally delayed orthogonally polarized femtosecond laser beams. We show that the laser fluence and delay time between the two beams are the controlling parameters for realizing the different surface morphologies. We provide a numerically supported, phenomenological model to explain the formed 2D structures. Our model employs elements from both the scattered surface-wave interference and the self-organization theories that are commonly used to explain uniform surface structures.

In this research, the formation of laser-induced periodic surface structures (LIPSS) on the nickel surface by femtosecond laser pulses was investigated. In the experiment, we used a commercially available amplified Ti:sapphire laser system that generated 164 fs laser pulses with a maximum pulse energy (Ep) of 1 mJ at a 1 kHz repetition rate and with a central wavelength λ= 780 nm. To obtain a fine periodic ordering of surface nanostructures, the laser beam, through a 0.2 mm pinhole aperture positioned near the 10× objective lens, was focused onto the sample. The samples were mounted on an XYZ-translation stage and irradiated in static and line-scanning experiment. The morphology of the induced periodic structure was examined by scanning electron microscopy. The surface profile was measured by atomic force microscopy. LIPSS with a period of around 700 nm entirely covered the irradiated area. Large area of LIPSS in the nickel surface was produced in line-scanning experiment. The mechanism of the formation of LIPSS in the entire irradiated area in static irradiation was discussed. The function of a 0.2 mm pinhole aperture was studied. The regular LIPSS on the nickel surface changed the optical property of the surface. The regular LIPSS on nickel surface could be also applied on the micro-mould fabrication.

In order to demonstrate the formation of laser-induced periodic surface structures (LIPSS), simulations were performed to investigate the effect of multiple femtosecond laser pulses with different laser energy densities on a Ti6Al4V surface. In this work, a set of partial differential equations calculating the electron and lattice temperature variations, followed by coupling with an electric field, is used to analyze the evolution of the periodic surface structure induced by the interaction of the femtosecond laser with the material. As the number of pulses increases, the surface structure of the material changes from none to produce LIPSS structure and from low spatial frequency LIPSS (LSFL) structure to high spatial frequency LIPSS (HSFL) structure. In order to compare the results, single-point laser scanning ablation experiments were carried out at femtosecond laser energy. The experimental results are consistent with the simulation results.

Electron backscatter diffraction (EBSD) data yield plentiful information on microstructure and texture of natural as well as experimentally produced mineral and rock samples. For instance, the characterization of microstructures and textures by EBSD allows for the evaluation of phase equilibria. Furthermore, determination of the preferred orientations of crystals using EBSD yields constraints on deformation mechanisms and history of the minerals/rocks. The latter affects bulk-rock properites, for example, through the relation between lattice preferred orientation and electrical conductivity and seismic anisotropy. EBSD is also applied to advance our understanding of various phenomena such as seismic wave attenuation in the Earth deep interior and its relation to the presence of interfacial small degrees of melt fractions, or free fluid phases. In standard EBSD software solutions, the original EBSD patterns are rarely saved and indexing routines result in many artifacts, such as pseudo-symmetry or unindexed pixels at interfaces that may be misinterpreted as amorphous material, such as a melt. Here we report the first application of the dictionary indexing (DI) approach proposed by Chen et al. (2015), an alternative indexing routine, which we extended to be applicable to multiphase geologic materials. The DI method is independent of the EBSD system, and thus of the used detector/software. The DI routine generates simulated EBSD patterns for all possible crystal orientations, taking the sample composition and experimental setups into account. The resulting pattern database is called a dictionary. The experimental electron backscattering pattern (EBSP) images are indexed by comparing them to the dictionary using a dot-product algorithm. We evaluate the new DI method in comparison to standard routines and highlight advantages and disadvantages. To test and compare the DI’s reliability and performance, we apply the routine to two scientifically challenging samples: (1) A nominally anhydrous (“dry”) residual eclogite composed of garnet (cubic), clinopyroxene (monoclinic) and an amorphous melt, where the different degrees of hardness of the phases cause surface topology; and (2) a pure forsterite (olivine) polycrystalline sample produced by vacuum sintering. The acquired EBSD patterns are of low quality for the latter as a result of fast data acquisition to reduce the on-line machine time. We conclude that the new DI method is highly precise and surpasses the performance of previously available methods, while being computer time and computer memory consuming. We find that the DI method is free of pseudo-symmetry-related problems. Interpolation of data becomes obsolete and high reproducibility is obtained, which minimizes the operator impact on the final data set. The latter is often caused by applying several cleaning steps on EBSD maps with low indexing fraction. Finally, much higher scientific integrity is ensured by image collections as described above, which requires that all patterns are saved. This in turn allows later re-analyses if required. The DI routine will help to achieve more reliable information on interface properties of geological samples, including amorphous materials, and thus in the long run help to improve the accuracy of large-scale Earth mantle process models.

While electron backscatter diffraction (EBSD) patterns are often used to present two-dimensional information about a material microstructure, they are in fact a product of the three-dimensional electron interaction volume. Consequently, 3D spatial information exists in EBSD images, which is generally not accessed. Specifically, the inclination of the grain boundary plane may be observed in EBSD patterns taken near grain boundaries. If, at the same time, the shape of an electron interaction volume in the material is known, a grain boundary plane normal direction can be obtained from a sequence of EBSD images taken stepwise in a line crossing the grain boundary. Here, these two principles are used for demonstrating the determination of grain boundary normal vectors from EBSD images. Coherent twin boundaries and focused ion beam serial scan data are used for validation. Results indicate a mean error for this approach of 3 deg with a standard deviation of 3.8 deg.

Laser-induced periodic surface structures (LIPSS) on chalcogenide glassy semiconductors are of great interest in relation with creating polarization-sensitive optical elements. This study investigates the formation of LIPSS on the surface of As 50 Se 50 amorphous film, fabricated by thermal vacuum deposition, under femtosecond laser irradiation in the wavelength range from 400 to 800 nm. The periods of various LIPSS types depend linearly on the laser wavelength. The measured birefringence of so-called low spatial frequency LIPSS, formed by different irradiation wavelengths, are in the 10–85 nm range. The maximum birefringence of 85 nm was obtained for structures irradiated at a 480 nm wavelength. A significant decrease in birefringence was observed at a wavelength of 800 nm, which may be due to the formation of a less pronounced and more disordered surface relief caused by less effective absorption of modifying laser radiation with photon energy lower than optical band gap of As 50 Se 50 . Decreased optical absorption observed in As 50 Se 50 films with LIPSS is caused by increased light scattering on the surface relief.

Dynamics of the formation of laser-induced periodic surface structures (LIPSS) upon femtosecond two-color double-pulse irradiation of metals, semiconductors, and dielectrics

The formation of laser-induced periodic surface structures (LIPSS) upon irradiation of semiconductors and dielectrics by linearly polarized high-intensity Ti:sapphire fs-laser pulses (τ ~100 fs, λ ~800 nm) is studied experimentally and theoretically. In the experiments, two different types of LIPSS exhibiting very different spatial periods are observed (socalled LSFL - low spatial frequency LIPSS, and HSFL - high spatial frequency LIPSS), both having a different dependence on the incident laser fluence and pulse number per spot. The experimental results are analyzed by means of a new theoretical approach, which combines the generally accepted LIPSS theory of J. E. Sipe and co-workers [Phys. Rev. B 27, 1141-1154 (1983)] with a Drude model, in order to account for transient changes of the optical properties of the irradiated materials. The joint Sipe-Drude model is capable of explaining numerous aspects of fs-LIPSS formation, i.e., the orientation of the LIPSS, their fluence dependence as well as their spatial periods. The latter aspect is specifically demonstrated for silicon crystals, which show experimental LSFL periods Λ somewhat smaller than λ. This behaviour is caused by the excitation of surface plasmon polaritons, SPP, (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 fields with that of the incident laser beam, resulting in a spatially modulated energy deposition at the surface. Upon multi-pulse irradiation, a feedback mechanism, caused by the redshift of the resonance in a grating-assisted SPP excitation, is further reducing the LSFL spatial periods. The SPP-based mechanism of LSFL successfully explains the remarkably large range of LSFL periods between ~0.6 λ and λ.

Electron backscatter diffraction (EBSD) is a powerful tool to automatically and quantitatively characterize the orientation of grains and phases of ceramic and composite materials [1]. EBSD ultra‐fast pattern acquisition, i.e., patterns streaming to hard disk (HD) and later pattern indexing, becomes an interesting technique to investigate a series of large‐scale ceramic, which can quickly provide phase distribution information for further improving ceramic production. However at the same time, it becomes more and more important to handle the huge offline EBSD raw data efficiently and correctly. In this project, we already reported the EBSD characterisation results of the polymorphs of a solid state sintered silicon carbide component based on Densitec 15, a ready to press powder‐made by Saint Gobain Ceramic Materials AS [2]. The pre‐sintered powder was produced using the Acheson process and would typically consist of the 4H‐ and 6H‐polytypes, with small amounts of 3C and sometimes traces of 15R. The offline EBSD raw data collection was carried out in a Hitachi SU‐6600 FESEM and the patterns were acquired by using NORDIF UF‐1100 EBSD detector and written directly to HD. The previous results only identified 4H‐ and 6H‐phases in the sample, consistent with the expected transformation of 3C‐crystals that takes place at temperatures significantly lower than the sintering temperature of 2110°C. In this abstract further detailed phase identification of silicon carbide 3C by the new developed NORDIF EBSD Extraction Software is carried out. Figure 1 is the overview for the new developed NORDIF EBSD Extraction Software, where the indexed phase map of the present silicon carbide sample shows partly on the right part of the figure. Offline EBSD indexing reveals that the content of the silicon carbide 3C phase is below 0.5% in the sample. By using the point analysis tool (+) in the program, the individual EBSD patterns from the silicon carbide 3C phase can be retrieved from HD with auto contrast and background subtraction corrections. Representative 3C‐SiC EBSD patterns shown in Fig. 2 together with the corresponding internal coordinations (x,y), where the pattern (6,59) is exactly the same retrieved pattern shown that in Fig. 1. Further detailed 3C‐SiC pattern indexing is performed. Under the system optimized calibration settings, the best confidence indexes (CIs) in Fig. 2 are all below 0.03, and the representative indexing result shows in Fig. 3. As checking back and comparing that in Fig. 1, it can be concluded that the indexed 0.5% 3C‐SiC phases are mostly located at the boundaries among different grains, phases and pores, which resulted those EBSD patterns mis‐indexed as 3C‐SiC phase. Offline EBSD together with its Extraction Software is hence an excellent tool to study not only the crystallographic texture and phase distribution, but also fully confirmed that the 3C‐SiC recrystallisation and phase transformations processes taking place during sintering of ceramic materials. It also reveals that the present EBSD Extraction Software is good practice to carefully view the offline EBSD raw data before applying further processing algorithms.

In this paper, we perform experimental and numerical study of the formation of femtosecond laser-induced periodic surface structures on metals, Cu, Ag, and Al. Under identical experimental conditions, laser-induced surface structures show distinctly different level of morphological clearness on the three different metals. The structures differences are explained by numerical calculations depending the improved two-temperature model. The calculation results confirm our experimental work on femtosecond laser induced periodic surface structures on metals, where electron-phonon energy coupling and hot electron diffusion are believed to play the dominant role.

In this research, the formation of laser-induced periodic surface structures (LIPSS) on the stainless steel surface by femtosecond laser pulses was investigated under static irradiation and line-scanning experiment. In the experiment, we used a commercial amplified Ti:sapphire laser system that generated 164 fs laser pulses with a maximum pulse energy (Ep) of 1 mJ at a 1 kHz repetition rate and with a central wavelength λ = 780 nm. To obtain a fine periodic ordering of surface nanostructures, the laser beam, through a 0.2 mm pinhole aperture positioned near the 5× objective lens, was focused onto the sample. The samples were mounted on an XYZ-translation stage and irradiated in static and line-scanning experiment. The morphology of the induced periodic structure was examined by scanning electron microscopy. The surface profile was measured by atomic force microscopy. High-spatial-frequency LIPSS (HSFL) with a period of 255 ± 21 nm were obtained over the entire ablated area. HSFL were found to form on low-spatial-frequency LIPSS (LSFL). From our results we elucidated the relationship between the formation of LSFL and HSFL to obtain an enhanced understanding of the mechanism of HSFL formation by femtosecond laser pulses. A large number of applications have been proposed, such as improvement of the optical properties of the surface, new cutting tool development and hard diamond. More applications could be found as the spatial period of HSFL on different materials comes into sub-100 nm.

Bulk metallic glasses (BMG) are amorphous metal alloys known for their unique physical and mechanical properties. In the present study, the formation of femtosecond (fs) laser-induced periodic surface structures (LIPSS) on the Zr-based BMGs Zr46Cu46Al8, Zr61Cu25Al12Ti2, Zr52.5Cu17.9Al10Ni14.6Ti5 (Vit105) and Zr57Cu15.4Al10Ni12.6Nb5 (Vit106) was investigated as a function of their different chemical composition. For this purpose, LIPSS were generated on the sample surfaces in an air environment by fs-laser irradiation (λ = 1025 nm, τ = 300 fs, frep = 100 kHz). The surface topography was characterized by scanning electron microscopy and atomic force microscopy. Moreover, the impact of LIPSS formation on the structure and chemical surface composition was analyzed before and after fs-laser irradiation by X-ray diffraction and X-ray photoelectron spectroscopy as well as by transmission electron microscopy in combination with energy dispersive X-ray spectroscopy. Despite the different chemical composition of the investigated BMGs, the fs-laser irradiation resulted in almost similar properties of the generated LIPSS patterns. In the case of Zr61Cu25Al12Ti2, Vit105 and Vit106, the surface analysis revealed the preservation of the amorphous state of the materials during fs-laser irradiation. The study demonstrated the presence of a native oxide layer on all pristine BMGs. In addition, fs-laser irradiation results in the formation of laser-induced oxide layers of larger thickness consisting of an amorphous ZrAlCu-oxide. The precise laser-structuring of BMG surfaces on the nanoscale provides a versatile alternative to thermoplastic forming of BMG surfaces and is of particular interest for the engineering of functional material surfaces.

Electron backscatter diffraction is a scanning electron microscopy technique used to obtain crystallographic information on materials. It allows the nondestructive mapping of crystal structure, texture, and strain with a lateral and depth resolution on the order of tens of nanometers. Electron backscatter diffraction patterns (EBSPs) are presently acquired using a detector comprising a scintillator coupled to a digital camera, and the crystallographic information obtainable is limited by the conversion of electrons to photons and then back to electrons again. In this article we will report the direct acquisition of energy-filtered EBSPs using a digital complementary metal-oxide-semiconductor hybrid pixel detector, Timepix. We show results from a range of samples with different mass and density, namely diamond, silicon, and GaN. Direct electron detection allows the acquisition of EBSPs at lower (≤5 keV) electron beam energies. This results in a reduction in the depth and lateral extension of the volume of the specimen contributing to the pattern and will lead to a significant improvement in lateral and depth resolution. Direct electron detection together with energy filtering (electrons having energy below a specific value are excluded) also leads to an improvement in spatial resolution but in addition provides an unprecedented increase in the detail in the acquired EBSPs. An increase in contrast and higher-order diffraction features are observed. In addition, excess-deficiency effects appear to be suppressed on energy filtering. This allows the fundamental physics of pattern formation to be interrogated and will enable a step change in the use of electron backscatter diffraction (EBSD) for crystal phase identification and the mapping of strain. The enhancement in the contrast in high-pass energy-filtered EBSD patterns is found to be stronger for lighter, less dense materials. The improved contrast for such materials will enable the application of the EBSD technique to be expanded to materials for which conventional EBSD analysis is not presently practicable.

Electron backscattered diffraction (EBSD) is a widely used technique for both identifying the crystallographic phase and for mapping the orientation of crystalline materials on the micron length scale. Often the operating conditions necessary for phase identification are not suitable for orientation mapping and vice versa. In an effort to optimize the speed involved in the mapping technique, pattern quality is sacrificed and the wealth of information present in an EBSD pattern is compressed to basically 4 values: a matched phase and three Euler angles. However, ab initio identification of phases from EBSD patterns requires high quality patterns and fairly intense computation. Spectrum imaging is an analytical approach that may offer some solutions to the aforementioned problems. Spectrum imaging consists of collecting a whole spectrum at each pixel in a mapping style measurement. This large set of data is then analyzed using multivariate statistical analysis (MSA) techniques such as principle components analysis, multivariate curve resolution, or other least squares based techniques. The result of these calculations is a set of component spectral shapes with corresponding abundances that allow the analyst to extract the greatest amount of physically relevant information from an otherwise enormous data set. Spectrum imaging has been used successfullymore » in EDX microanalysis (both in the SEM and TEM), TOF-SIMS, WDS, and EELS. To examine the potential benefits of the spectrum imaging approach for EBSD data, a series of basic experiments and calculations were run. Test data sets (20 x 20 patterns in .jpeg format) on polycrystalline Al and on the directionally solidified eutectic oxide, CoO/ZrO{sub 2}(CaO), were collected using the HKL Channel 5 system with a Nordlys detector under normal mapping conditions. The data was collected on a FEI dual beam FIB (model DB235) and a Zeiss (Supra 55 VP) SEM at 20keV for Al and CoO/ZrO{sub 2}(CaO), respectively. The data sets were analyzed according to the schematic shown in Figure 1. Each EBSD pattern was hough transformed, unzipped into a 1-D vector of channels with intensities ranging from 0-255, and then added to an overall data matrix. A range of treatments (edge/no edge detection, spatial simplicity/spectral simplicity, etc.) were examined to determine the optimal way of treating the data. The multivariate analyses were performed using the AXSIA code developed at Sandia National Laboratories. The MSA techniques were able to correctly identify individual grains in the Al sample and individual phases in the CoO/ZrO{sub 2}(CaO) sample. For each component EBSD pattern identified from the Al data, a corresponding color map of abundance can be seen which clearly corresponds to a single grain (Figure 2). The success in the CoO/ZrO{sub 2}(CaO) sample is particularly notable due to both phases sharing the Fm-3m space group which would confuse most autoindexing routines. The range of analytical treatments identified two extremes in results: a minimal number of components (patterns) with only kikuchi line positions present or a larger number of components with full intensity information present. The further application of these results to phase mapping will be discussed.« less