Fabrication of High Aspect-Ratio Surface Micro Patterns On Stainless Steel Using High-Speed Direct Laser Interference Patterning
Fabrication of High Aspect-Ratio Surface Micro Patterns On Stainless Steel Using High-Speed Direct Laser Interference Patterning
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Adv. Eng. Mater. 2019, 1900151 1900151 (1 of 9) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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The use of short pulse lasers (pulse duration >1 ns) results 2. Experimental Section
in a considerable amount of melting of the substrate material
2.1. Materials
due to heat diffusion. As a result, the topographies achievable
with DLIP using ns-pulsed lasers are generally limited in
their aspect ratios (ratio between structure depth and spatial Stainless steel substrates (1.4031, X5CrNi18-10) with a thickness
period) to up to 0.5.[36] While high-aspect-ratio structures are of 0.9 mm were electro-polished obtaining a surface roughness
already possible using ps pulsed lasers in combination with (Sa) of 53 nm. Before the laser experiments, the metallic
the DLIP technology,[37] ns laser sources are still very substrates were cleaned using a lint-free cellulose paper with
interesting for industrial high-speed structuring applications isopropyl alcohol.
due to the lower invest costs and higher available laser
powers. Thus, there is a demand for structuring solutions to
structure metals with higher aspect ratios using DLIP with 2.2. Direct Laser Interference Patterning
ns-pulsed lasers.
This work focuses on the high-speed structuring of stainless The laser experiments were carried out using a nanosecond
steel employing ns-pulsed laser radiation using DLIP. In pulsed slab-shaped solid-state laser (Edgewave IS400) operating
addition, for the first time, heat accumulation during the DLIP at its fundamental wavelength λ of 1064 nm. This system
process is investigated when utilizing ns laser pulses. permits to change the repetition rate from single pulse to
Rectangular shaped laser spots permit high surface processing 10 kHz, with a maximum average power of 150 W (@ 10 kHz
rates by enabling the treatment of larger surface areas per laser repetition rate). The pulse duration τ was 10 ns. In the performed
pulse.[38,39] Therefore, an optical DLIP setup is designed, experiments, the laser fluence was kept constant at 3.2 J cm2.
permitting to form the interfering laser beams into a This can be done by setting the pulse energy to 16 mJ (at the
rectangular shape containing a well-defined interference materials’ surface) considering that the area which is irradiated
pattern. A similar approach has been already successfully by each laser pulse is 0.1 5 mm2. In consequence, depending
applied to achieve exceptionally high structuring speeds close to on the used repetition rate, the laser power level was adjusted in
1 m2 min1.[40] By using different optical elements, the spatial order to keep this value constant, considering optical losses in
period of the micro-structures was set to 8 and 19 μm. The the beam path of 33% (0.1 kHz: 2.4 W, 1 kHz: 24.2 W, 2 kHz:
influence of the processing parameters (laser fluence, repeti- 48.4 W, 5 kHz: 121 W).
tion rate, feed speed) on the morphology of the produced The interference patterns were generated using an optical
patterns is investigated. Additionally, the melt flow character- assembly developed by Fraunhofer IWS (see Figure 1). By using
istics as a result of heat accumulation as well as the amount of two bi-prisms, the laser beam is split into two sub-beams which
molten material are taken in account. The obtained surfaces are are overlapped on the sample surface. Additionally, the laser
examined by Confocal Microscopy (CFM) and Scanning beams are formed into a rectangular shape of 5 mm x 100 μm on
Electron Microscopy (SEM). Moreover, energy dispersive X- the sample surface by first expanding the laser beam in one
ray spectroscopy (EDX) measurements are also performed in spatial direction with a cylindrical telescope, and secondly
order to determine possible changes in the chemistry of the focusing the sub-beams one-dimensionally with an additional
treated surface. cylindrical lens (see Figure 1). The intersection angle between
Figure 1. Experimental setup (center) illustrating the optical assembly (right side) that forms the line-like shaped irradiation area containing a two beam
interference pattern and the areal scanning strategy (left side).
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the overlapping sub-beams is defined by the wedge angles of the of material composition in near-surface layers, it can provide
bi-prisms. In this work, the spatial periods Λ of 8 μm and 19 μm useful information for the determination of qualitative changes
were used, which corresponds to intersection angles α of 7.6 and across periodic patterns as has been previously shown.[42] For
3.1, respectively. performing the EDX analysis, the acceleration voltage was set to
In order to structure larger areas, the relative movement 15 kV. The line-scans were realized with a resolution of 284
between the laser irradiated area (which contains the interfer- points/100 μm, corresponding to a separation distance of
ence pattern) and the sample surface was performed using a 352 nm between two data points.
linear stage. The surface processing rate A0 is determined by the
length l of the laser irradiated area per pulse and the feed rate v,
as shown in Equation (2). 3. Results and Discussion
The DLIP approach was used to produce periodic surface
A0 ¼ v l ð2Þ
structures on stainless steel with spatial periods of 8 μm and
19 μm. The influence of the pulse-to-pulse (PTP) overlap on the
resulting structure height was investigated. Figure 2 shows SEM
images of structured samples spatial periods of 19 μm
2.2.1. Surface Characterization (Figure 2a,b) and 8 μm (Figure 2c,d) employing a low PTP
overlap (Figure 2a,c) and high PTP overlap (Figure 2b,d),
The topographies of the patterned surfaces were characterized respectively. Figure 2a,c show the topography when using a
using a scanning electron microscope (Philips ESEM). The 40 μm PTP feed (60% overlap) while Figure 2b and d show the
structure heights were investigated by measuring the structure sample surface when utilizing a PTP feed (99% overlap) of only
height hst at different positions on the substrates using confocal 1 μm. As expected, the DLIP micro-structures become more
microscopy (Sensofar S-Neox).[41]The structure height of the pronounced with increasing the number of pulses.
patterns was evaluated using the step height definition, The individual pulses are still visible for large PTP feeds (see
representing the standard type A1 in the norm ISO5436-1.[41] Figure 2a and c), while they cannot be distinguished in the
Areas of 200 200 μm2 and 100 100 μm2 for the spatial surface profile contour for very small feeds (high overlaps, see
periods of Λ ¼ 19 μm and Λ ¼ 8 μm, respectively, were divided Figure 2b and d). Particularly, it can be seen in Figure 2a, that the
into a series of 18 profiles (cross-sections of the interference molten material at the interference maxima positions forms two
pattern). These profiles were used to calculate the average values independent melt fronts which follow the thermal gradient
as well as the standard errors for each measurement. In order to perpendicular to the line-like laser intensity distribution. These
determine the effect of the laser treatment on the surface two fronts of molten material merge with the material release
chemistry, the treated surfaces were examined with Energy- from the neighboring interference maxima at the interference
dispersive X-ray spectroscopy (EDX, Philips ESEM). Although minima regions when increasing the pulse overlap (Figure 2b),
EDX is of limited use for the precise quantitative determination especially for shorter spatial periods due to the reduced
Figure 2. SEM images of treated steel surfaces (X5CrNi18-10/1.4301) with spatial periods of a) Λ ¼19 μm and 80 % PTP overlap, b) Λ ¼ 19 μm and 99 %
PTP overlap, b) Λ ¼ 8 μm and 80% overlap and c) Λ ¼ 8 μm and 99% PTP overlap. The used laser fluence was 3.2 J cm2 in all cases.
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geometrical distance (Figure 2c). At high PTP overlaps (short the structure height evolution for patterns with spatial periods of
PTP feeds), the melt fronts convergence in combination with the Λ ¼ 19 μm, while Figure 4c and d show the structure height
large amount of molten material resulting in a significant evolutions for spatial periods of Λ ¼ 8 μm. In addition,
increase in the structure height, as shown in Figure 2b and d. Figure 4a and c show the influence of different pulse-to-pulse
Figure 3 shows the confocal microscope images of the same feeds between 1 μm and 20 μm (corresponding to pulse overlaps
line-like structures as in Figure 2. With shorter PTP feed (higher between 99 % and 80 %, respectively) using the same pulse
PTP overlap), considerably deeper structure heights of 8.7 μm repetition rate of 5 kHz. Figure 4b and d also show the influence
and 18.5 μm were achieved for the 8 and 19 μm spatial periods, of different pulse repetition rates based on the results obtained
respectively (see Figure 3b,d). In comparison, the heights of the with pulse repetition rates from 0.1 kHz to 5 kHz at a fixed pulse-
periodic structures formed with larger PTP feed (lower overlap) to-pulse feed of 2 μm.
reached only structure heights of 3.4 μm and 1.5 μm for the From Figure 4a is visible, that with increasing PTP overlap the
spatial periods of 8 μm and 19 μm, respectively (see Figure 3a,c). structure height increases as well. For high pulse overlaps higher
The aspect ratios for both periods are very similar when using than 98%, maximum structure heights of more than 20 μm
high overlap conditions (AR of 1.09 and 0.97 for 8 μm and 19 μm (corresponding to aspect ratios of more than 1) are achieved. In
period, respectively), at 99% overlap and 3.2 J cm2 laser fluence all cases, the structure height is always lower at the beginning of
per pulse (see Figure 3c,d). For low overlap conditions the aspect the process and gradually increases with increasing distance
ratios for both periods differ (AR of 0.42 and 0.08 for 8 μm and relative to the process starting point (infeed) until either a steady
19 μm period, respectively) at 80% overlap at same laser fluence state condition is reached or even a reduction of the structure
(see Figure 3a,c). height occurs. Different mechanisms can be responsible of the
Based on the topographic analysis, the steadiness of structure changes in the structure height observed during the process.
height of the produced patterns was investigated by evaluating One possible reason is the heat accumulation which is produced
the structure height during the course of the laser process. Since during the laser treatment, meaning that the irradiated steel
the substrate is moved relative to the DLIP head during the substrates are heated up.[43,44] Additionally, the produced surface
process, the structure height development was determined by structures on the substrate can have a significant influence on
measurements at different positions on the processed area on the optical absorption of the laser radiation due to multi-
the substrates. The structure heights were measured at the reflections in the generated trenches, which means that a higher
beginning of the process (infeed) and at subsequent positions amount of energy is coupled in the material as the structure is
(dx ¼ 0.5, 1, 2, 3, 4, 5, 10, 20, and 50 mm). formed.[45,46] The effect of heat accumulation is further
Figure 4 shows the development of the position-dependent promoted by incubation effects during multi-shot laser
structure height during the DLIP process. Figure 4a and b show ablation.[47] It has been also reported that rippled surface
Figure 3. Confocal Microscope images of treated steel substrates (X5CrNi18-10/1.4301) with interference periods of a) Λ ¼ 19 μm at pulse overlap of
80%, b) Λ ¼ 19 μm at pulse overlap of 99%, c) Λ ¼ 8 μm at pulse overlap of 80% and d) Λ ¼ 8 μm at pulse overlap of 99%. The used laser fluence per
pulse was 3.2 J cm2.
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where QnD is the residual heat introduced into the material, ρ is 2 Q Heat =A NP Θ t N1
X fL
the mass density of the material, cp its specific heat capacity, T Sum;nD ðtÞ ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi ð4Þ
ρ cp ð4 π κÞ N¼1 t N1
κ ¼ λth (ρ cp)1 is the diffusivity, λth the heat conductivity, t is fL
time, r the coordinate of space, fL the laser repetition rate and NP
the number of pulses. where QHeat is the residual heat and A is the irradiated area.
Due to the elongated shape of the laser irradiated area, the Three different pulse repetition rates of 5 kHz, 1 kHz, and
solution of the 1D heat flow can be assumed, which gives nD ¼ 1 0.1 kHz were used in the calculations with a constant laser
for the indicator of the dimension. By further setting the volume fluence of 3.2 J cm2. Figure 5 shows the calculated temporal
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evolution of the surface temperature for each of the investigated schema shows that the molten material at the interference
pulse repetition rates. It can be seen that even at repetition rates maxima positions moves from the hot to the colder peripheral
of 1 kHz, an important accumulation of heat is observed, areas due to surface tension gradients induced by the
reaching a temperature increase of 600 K after 100 pulses. A temperature differences. Later, the fronts of molten metal start
further increase of the rep. rate to 5 kHz produces an increase of to merge at the interference minima locations. The application
1500 K, also after 100 pulses. The calculated temperature of subsequent laser pulses (with the interference intensity
evolutions demonstrate that heat accumulation is possible also at distribution) which is in particular more relevant when using
relative low repetition rates (KHz range), what in the case of ps high PTP overlaps results in additional melt leading to patterns
laser sources is observed at significantly higher frequencies (e.g., with higher aspect ratios. While the structure height can be
of some MHz).[54,55] This simple calculation clearly demon- significantly boosted especially for the larger spatial periods due
strates that the heat accumulation effects can take place in the to stacking of molten material, a stronger increase of the PTP
process used in the experiments and can also explain the overlap result in a reduction of the structure height for smaller
variation of the height during the DLIP process. periods due to material over melting (Figure 6c). Overmelting
Figure 6a shows the development of the average aspect ratios leads to a local collapse of the structures and thus to the
of the structure heights for the larger (Λ ¼ 19 μm) and smaller emergence of overhang structures (see for example the SEM
(Λ ¼ 8 μm) interference periods as a function of the number of image of Figure 2d). This would be in accordance with known
accumulated laser pulses per area. The aspect ratios are phenomena in the wake of Marangoni convection, such as the
calculated as the quotient of the average structure height (from humping phenomenon in laser welding.[58–60] This effect was
Figure 4) and the corresponding interference period. The not observed for larger periods, as in the latter case a larger
observed differences in the structure heights depending on the amount of melt is required due to the longer distances that have
spatial period and PTP overlap can be interpreted as a result of to be covered. In fact, overhang structures can be seen as an
the melt displacement which is increased due to the accumula- advantage compared to simple structures. For instance, micro-
tion of heat. A generally accepted theory for near-surface melt textures with overhang structures can enable to obtain super-
dynamics during laser processes is provided by Marangoni hydrophobic surfaces, even in materials which are intrinsically
convection.[56] Furthermore, D’Alessandria et al.[57] have already hydrophilic.[61,62]
reported on the different regimes responsible for the pattern These considerations explain that heat accumulation has
formation in DLIP when using ns pulses depending on the similar effect on smaller and larger interference periods, but that
applied pulse fluence, which are either Marangoni convection or for smaller periods the results obtained exceed the state of
the recoil pressure. In both cases, the obtained molten metal is maximum structure height, whereas this is not the case for the
driven towards the minima positions. However, the here larger periods.
presented results demonstrate for the first time the possibility In addition to the topography analysis, EDX measurements
of reaching structure heights in the same order of the spatial were performed for verifying the above described structuring
period (or aspect ratios slightly higher than one).[57] A scheme of mechanism. Figure 7 shows the results of an EDX line-scan
the possible structuring mechanism applying the Marangoni measured across a DLIP-structure (perpendicular to the
convection model for the DLIP using multiple pulses is shown in interference lines) for iron, oxygen, chromium, and carbon
Figure 6b and c, for long and short periods, respectively. The elements. The absolute response of the material during EDX
Figure 5. Temporal evolution of the temperature increase ΔTSum,1D on the surface of a semi-infinite body of stainless steel at the location of a one-
dimensional source for different repetition rates (5 kHz, 1 kHz, and 0.1 kHz) with equal heat source energy of 16 mJ per laser pulse with pulse durations
of τ ¼ 10 ns.
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Figure 6. a) Average Structure Height Aspect Ratio as function of Pulse Overlap PO for Λ ¼ 19 μm and Λ ¼ 8 μm patterns; Schematic representation of
the structuring mechanism showing the melt flow in the DLIP processes for b) large and c) short interference periods.
measurements varies very strongly depending on whether the concentration at the interference minima positions. This
sensing spot strikes in the trenches or on the ridges of the periodic modulation of the material composition underlines
topography. For this reason, for each measurement point of the the movement of the melt flow from the interference maxima to
line scan, the individual percentages of the measured elements minima positions, since the molten metal is longer exposed to
were calculated. The gray bars in the background of Figure 7 the air atmosphere and thus allowing the diffusion of oxygen and
represent the interference maxima positions which correspond finally forming oxides. Both composition distributions for iron
to the locations of the trenches in the produced surface pattern. and oxygen also show slight double periodic peaks, which is in
The image shows that both iron and chromium elements agreement with the previous explanation and represent the two
(corresponding to stainless steel) have a higher concentration at fronts of molten metal which are finally merged at the
the interference maxima positions. Differently, the oxygen interference minima. These effects have been also investigated
content shows a opposite distribution, having a maximal in the past on steel surfaces which were irradiated using ns pulse
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Figure 7. Ratio of the proportions of the most important elements determined as a line diagonally over the cross section of the DLIP trench structures,
based on EDX measurement.
DLIP by Rosenkranz et. Al.[63] Using XPS in combination with explained due to the accumulation of the heat, in particular for
Ar ion etching as well as atom probe tomography, a sharp repetitions rates of few kHz. Thus, this research work permitted
interface for transition between the oxidic and metallic state was to show for the first time heat accumulation processes using
found for the unpatterned sample, whereas for the laser- Direct Laser Interference Patterning with ns laser pulses.
irradiated specimens, not only a mixed oxidic state was observed Depending on the process parameters, aspect ratios slightly
but also an increase of the oxide layer thickness. In addition, this higher than one could be realized, which has not been previously
layer consisted on an iron oxide layer on top followed by achieved using DLIP with ns-pulsed lasers. Particularly for the
chromium oxide.[63] smaller periods, the melt flow impairs pattern formation due to
the overmelting of the material (humping). Finally, a mechanism
for the structure formation was presented, which was verified by
4. Conclusions EDX analyses.
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Adv. Eng. Mater. 2019, 1900151 1900151 (9 of 9) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim