Ultramicroscopy 220 (2021) 113161

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Ultramicroscopy
journal homepage: www.elsevier.com/locate/ultramic

Laser ablation sample preparation for atom probe tomography and

transmission electron microscopy
N. White a, K. Eder a, b, J. Byrnes a, J.M. Cairney a, b, I.E. McCarroll a, *
a
Australian Centre for Microscopy and Microanalysis, The University of Sydney, Australia
b
School of Aerospace Mechanical and Mechatronic Engineering, The University of Sydney, Australia

A R T I C L E I N F O A B S T R A C T

Keywords: Laser ablation is capable of removing large volumes of material with micron scale precision at very high speeds.
Laser ablation This makes it an ideal tool for the initial stage of preparation of samples for atom probe and electron microscopy
Atom probe tomography studies. However, the thermal nature of the laser ablation process is such that thermal and mechanical damage is
Transmission electron microscopy
induced in the samples in the form of zones of recrystallisation and stress induced deformation. For the analysis
Silicon wafers
Pure aluminium
of nanometer-sized samples, such as those required for atom probe tomography and transmission electron mi­
Damage characterisation croscopy, it is necessary to ensure that any damage induced during sample preparation will not introduce ar­
tefacts and that specimens are representative of the microstructure of the bulk sample. Here we have undertaken
an analysis of the damage caused during sample preparation through a study of pure aluminium and phos­
phorous doped silicon wafers. Our findings indicate that recrystallisation and stress induced misorientations
occur in pure aluminium at the micron scale, however, no detectable damage is observed in the silicon sample.

1. Introduction
Valuable insights gained by microscopy techniques often rely on the
assumption that isolated areas chosen for characterisation are repre­
sentative of the bulk material and are free of deformation and damage
induced during sample preparation. Mechanical polishing, focused ion
beam (FIB) milling, and electropolishing are all widely used for sample
preparation and yet each introduces a certain amount of damage into the
sample. Mechanical polishing induces deformation and is largely limited
to forming flat planes [1,2]. FIB is ideal for forming nano-scale samples
with 3D geometrical requirements, such as the needles required for atom
probe tomography (APT) or the thin films required for transmission
electron microscopy (TEM). However, the required milling time means
it is limited to the removal of very small amounts of material. Further­
more, penetration of ions into the sample can cause local contamination
and amorphisation of the surface, the extent of which depends on the ion
beam acceleration voltage [3]. Electropolishing is also used to prepare
TEM and APT specimens and is the most time and cost efficient method,
however, it is limited to conductive materials and requires the use of
potentially dangerous chemicals [4].
Laser ablation micromachining is an emerging technique for the
micro-scale shaping of materials [5]. At two to five orders of magnitude
faster than FIB, it is ideal for quick fabrication [6]. Furthermore, laser
ablation systems are largely automated, reducing the user-time neces­
sary to operate the machine and could therefore have important appli­
cations for the fabrication of microscopy specimens, allowing for quick
fabrication of non-conductive samples, which are currently limited to
time-intensive FIB techniques. For example, by preparing a “coarse”
atom probe tip or TEM foil via laser ablation, followed by a final FIB
milling step, FIB lift-out could be circumvented. This would simplify FIB
preparation, reduce the time required on the FIB and remove the need
for a platinum or tungsten weld, which, for atom probe specimens, is
often a point of failure during field evaporation [3].
A limiting factor for preparing representative microscopy samples
using laser ablation is the potential for damage induced by the ablation
process [7]. While laser power and energy vary considerably across in­
struments, the use of this technique is known to produce a heat affected
zone [8]. In order to be able to use laser micro-machining tools for
material specimen preparation, a clear understanding of the damage is
important, especially for thermally-sensitive samples. Here we charac­
terise the damage in the region adjacent to laser ablation cuts that are
designed to mimic the geometries used in APT and TEM analysis. We
have used a 3D-Micromac microPREPTM system that is being marketed
to the microscopy community as a specimen preparation tool.

* Corresponding author.
E-mail address: ingrid.mccarroll@sydney.edu.au (I.E. McCarroll).

https://doi.org/10.1016/j.ultramic.2020.113161
Received 11 June 2020; Received in revised form 28 October 2020; Accepted 1 November 2020
Available online 2 November 2020
0304-3991/© 2020 Elsevier B.V. All rights reserved.
N. White et al.
Aluminium (Al) and silicon (Si) have been studied in order to compare
the difference between the affected zones in materials with different
thermal properties.
Previous laser micro-machining investigations have established that
Si is a good candidate for laser machining [7]. Characterization of the
microstructural changes in the Si will therefore provide a useful
benchmark for the damage that is induced by our micro-machining
system in semiconductors. Metals have very different thermal proper­
ties to semiconductors. For laser micromachining to be widely used on
metal samples, the possible damage mechanisms must first be assessed.
Aluminium (Al) is a relatively soft metal with a high thermal conduc­
tivity and is susceptible to recrystallisation at relatively low tempera­
tures. Thus, observations of laser induced damage in Al can provide a
guide to the maximum damage that one might expect when using laser
micro-machining for sample preparation for higher melting point metals
and alloys.
2. Material & methods
2.1. Material
A 99.9 % pure as-cast Al ingot with a grain size of 100-150 µm was
used, which had large grain size and low recrystallisation temperature,
with recrystallisation expected to occur at 350◦ C [9]. An N-type
Fig. 1. a) Workflow for preparation of the as-cast Al samples for electron backscatter diffraction (EBSD) and laser ablation. b) Scanning electron microscope (SEM)
image of a pillar cut specimen ready for FIB annular milling. c) A SEM image of a trench cut specimen ready for FIB cross-section polishing.
2
Ultramicroscopy 220 (2021) 113161
phosphorus Si prime wafer was also used. Si wafers are able to operate at
temperatures up to 1150◦ C with minimal developments in crystal de­
fects [10]. In both cases, the large grain size should mean that any
recrystallisation of the sample will be easily identifiable.
Three samples were sectioned from the as-cast Al block using an
Accutom-50 diamond saw. Of the three samples, two were polished into
200 µm thin wafers to remove any deformation induced during
sectioning. All polishing was conducted using a RotoPol-22 polishing
wheel. The third sample was mounted into a conductive resin with an as-
cast face exposed for bulk analysis of the microstructure. All surfaces
intended for characterisation or exposure to the laser were finally
chemical-mechanical polished with 0.04 µm colloidal silica. A schematic
of the samples cut from the Al block and their orientation with regard to
laser exposure and final analysis is presented in Fig. 1a. Fig. 1b and c are
representative images of how the specimens look after laser ablation for
both the pillar cuts and trench cuts, respectively.
The Si wafers were cleaved into pieces of smaller than 5 × 5 mm in
order to fit within the various instruments. The wafers were chemical-
mechanical polished with 0.04 µm colloidal silica to minimise surface
damage from handling. Analysis of laser-induced damage in Si has
previously been characterised, both from the microPREPTM and a vari­
ety of other laser systems [5–7].
N. White et al. Ultramicroscopy 220 (2021) 113161

2.2. Laser ablation Table 2

Parameters used to prepare coarse APT tips.
Once polished, samples were placed into the microPREPTM system, a Power Area Dose Dimensions/Inner Outer
490 picosecond pulsed laser ablation tool with a pulse energy of 60 µJ (W) (Pulses/µm2) Diameter (µm) Diameter (µm)
and a laser wavelength of 532 nm. Parameters can be adjusted in order Box 0.1 25 100 × 100 ~300 × 300
to optimise the properties and accuracy of the final laser cuts. In order to Mill
minimise variability in our experiments, the spot diameter, line dis­ Pillar 0.05 5 20 200
tance, pulse distance and use of airjets were held constant (Table 1). Mill

Three parameters were varied: (1) average power (W), which is calcu­
lated as the pulse energy multiplied by the repetition rate, (2) area dose
(pulses/µm2), the total number of pulses given to a unit area, and (3) the Table 3
focus shift, letting the laser focus shift during the ablation process, so Parameters used for the trench cuts.
that it focuses on the new surface as material is removed. Trench Power Area Dose (Pulses/ Focus Shift
Name (W) µm2)
2.2.1. APT sample preparation T3 3 200 No
APT samples are required to have a needle-like shape with a final tip T1 1 200 No
diameter of < 200 nm. The microPREPTM is equipped with an annular T0.1 0.1 200 No
T0.05 0.05 5 Yes, 100 layers, total depth
milling function, capable of producing needle shaped samples. To
100 µm
explore the applicability of this function to the initial preparation of APT
tips and the extent of damage induced within the manufactured pillars,
APT samples were prepared from Al and Si. Samples were initially the saturation levels and orientation edited for clarity.
prepared using the microPREPTM ‘box mill’ function to form a square
pillar of ~100 × 100 µm with a 300 µm moat around the pillar. The 3. Results
initial material was removed to provide the clearance and visibility
necessary for a successful APT experiment. From this square pillar a 3.1. Sample preparation time
‘coarse’ tip was milled using the pillar mill function, which ablates
material in successive rings from the inner diameter to the outer diam­ Sample preparation time for the coarse APT tips can be separated
eter. The relevant laser parameters and dimensions for both the box mill into three stages: 1) initial sample polishing, 2) laser ablation of the
and pillar mill are recorded in Table 2. These parameters were selected outer pillar, 3) and the final ablation step that produces the coarse APT
to produce shapes with dimensions best reflecting APT tips: the smallest tip. The tip can be prepared in under 1.5 hours, with the breakdown of
possible tip diameter without losing height, and the lowest possible time spent at each stage presented in Table 4. It is relevant to note that
shank angle. The focus shift functionality of the laser ablation system multiple tips can be produced from a single polished sample reducing
was used as it produced the steepest shank angles. From these coarse the average time per tip.
APT tips smooth cross-sections were prepared for EBSD by using a Zeiss
Auriga FIB/SEM. Initial FIB milling was conducted using a 10 nA current
3.2. Coarse APT tips
followed by a 5 nA polish to minimise surface curtaining. The final cross-
section was produced roughly along the axis of the tips.
Secondary electron images of the FIB-milled tip cross sections from
Al and Si are shown in Fig. 2a and d, respectively. The end radii of both
2.2.2. Laser parameter study
tips are roughly the same size, ~15 µm, however, the shank angle of the
In order to understand the effects of laser power and area dose on the
Al tip is visibly larger than that of the Si tip. Initial observation of the
damage, an Al wafer was prepared for ‘trench’ cuts, as illustrated in
EBSD maps presented in Fig. 2b and e, would appear to reveal very little
Fig. 1. Table 3 records the parameters that were varied between cuts and
damage caused by the laser ablation process. The EBSD map of the Al tip,
a naming scheme is provided. The trench cut provides a simple cross-
Fig. 2b, shows a small amount, roughly 1-2 µm, of laser-induced
section that can be easily analysed, providing information that is rele­
recrystallisation at the edges of the sample. However, further investi­
vant for both TEM and atom probe specimen preparation. After laser
gation of the Al sample, in the form of a misorientation study, Fig. 2c,
ablation, the wafer’s edge was mechanically polished with a Leica TXP
reveals that significant laser-induced damage has occurred. Fig. 2c
to expose cross-sections. The sample was then further polished using the
shows two types of data: misorientation between neighbouring points
FIB to produce flat cross-sections adjacent to the trench. An area >1 mm
along line A to B, where large spikes in this data indicates grain
away from the laser cut was also prepared using the FIB to expose a non-
boundaries, and a comparison of each point along the line with point B,
laser affected zone for comparison to the areas adjacent to the cuts.
where point B is selected to be representative of the original orientation.
The neighbouring points analysis indicates that a number of low angle
2.3. Characterisation grain boundaries are present within the first 15 µm. The misorientation
across these boundaries is less than 3 degrees. The misorientation rela­
Secondary electron images and electron backscatter diffraction tive to point B, shows that the damage extends deeper into the sample,
(EBSD) maps were captured for all samples by using a Zeiss Ultra with a gradual increase in misorientation when moving along the line in
scanning electron microscope equipped with an Oxford Instruments Fig. 2b from point B to A. The misorientation analysis relating to Si,
Aztec-integrated EBSD system and a Nordlys-nano EBSD detector. All Fig. 2e, indicates that there has been no recrystallisation of the Si tip at
EBSD maps were cleaned, processed and analysed using Channel 5 and all. All misorientations within the bulk of the sample are approximately
Tango. ‘Wild’ spikes were removed, and zero solutions were extrapo­
lated from 4 neighbours using iteration. Images have been cropped and
Table 4
Processing times for APT sample preparation stages.
Table 1
Mechanical Ablation - Ablation - FIB annular
Parameter constants for all trenches and atom probe tips.
polishing Outer Pillar Coarse APT Tip milling
Spot Diameter Line Distance Pulse Distance Air Jets on?
Time 45-60 <20 5 30-40
12 µm 5 µm 5 µm No (min)

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N. White et al. Ultramicroscopy 220 (2021) 113161

Fig. 2. Results from the preparation of coarse APT tips using laser ablation. The scale bar in the bottom left corner is representative of all images in this figure. a)
Secondary electron image of FIB cut cross-section of an Al tip, the face smoothed by FIB milling has been highlighted with a dashed white line. b) IPF Z EBSD Map
produced from the area in the preceding secondary electron image. On the EBSD map red lines are grain boundaries of >10◦ , black are grain boundaries of >5◦ and
yellow are grain boundaries of >2◦ . c) Misorientations along the line marked on the preceding EBSD maps. The number in brackets indicates the misorientation value
for that particular bar of the histogram, which currently exceeds the limits of the plot. d) Secondary electron image of FIB cut cross-section of a Si tip. e) IPF Z EBSD
Map produced from the area in the preceding secondary electron image. f) Misorientations along the line marked on the preceding EBSD maps. (For interpretation of
the references to color in this figure legend, the reader is referred to the web version of this article.).

one degree or smaller. The observed asymmetry of both tips is thought to
be related to either laser drift or as a result of the use of focus shift.
To determine if the gradual change in misorientation observed in the
Al tip, Fig. 2c, is indicative of damage caused during laser ablation or if it
is a feature of the underlying material, the as-cast microstructure is
presented, Fig. 3. A typical region, presented in Fig. 3a, shows that the
bulk sample is composed of large grains with high-angle grain
boundaries (grain boundary misorientations are indicated in brackets in
Fig. 3b). While there are large misorientations at grain boundaries,
misorientations within a grain are small, less than one degree of dif­
ference in a point-to-point analysis and approximately two degrees of
overall misorientation difference within a single grain. The orientation
profiles obtained from the Al tips in Fig. 2c vary significantly from the
bulk sample, indicating that the damage was induced during sample

Fig. 3. a) an IPF Z EBSD map from the as-cast Al alloy. b) Misorientation profile from A-B, as indicated in a). This profile indicates that the original as-cast sample
contains large grains with high-angle grain boundaries. This profile indicates that only a small degree of misorientation (< 2 degrees) is expected within the grains.

4
N. White et al. Ultramicroscopy 220 (2021) 113161

preparation and that the extent of damage extends to 30 µm. Damage of
this scale is significant for the preparation of nm sized samples, even if
the final preparation steps are undertaken by FIB.
3.3. As-cast Al trenches
Laser-assisted preparation of Al atom probe tips has shown laser-
induced damage. To understand the effects of the laser operating
parameters on the degree of damage caused, four trenches were ablated
with different laser powers and, in one instance, a different area dose.
The area dose was changed for the final trench to match the parameters
used for the preparation of the coarse tips. The laser parameters used for
the trenches are listed in Table 3. Secondary electron images and EBSD
maps are provided in Fig. 4, where the trench cut is the vertical face on
the left hand side in all images. Misorientation line profiles are provided
in Fig. 5.

Fig. 4. a), c), e) and f): Secondary electron image of a FIB cross-section prepared directly adjacent to T3, T1, T0.1 and T0.05 trenches, respectively. The boundary
between the trench cut and the FIBed flat surface is identified by a white dashed line. A horizontal white dashed line also indicates the location of the crater rim in a),
c) and e). b), e), h) and k): IPF Z EBSD maps produced from the same areas. Red lines indicate grain boundaries with misorientations >10◦ , black boundaries are
between 5 and 10◦ , and yellow boundaries are between 2 and 5◦ . The line AB has been placed 20 µm below the uppermost part of each sample and is 40 µm in length.
(For interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.).

5
N. White et al.
Fig. 5. Two plots of misorientation. Left: a plot of misorientation with respect to the crystal orientation at point B on the EBSD images shown in Fig. 4. Right:
Misorientation relative to the adjacent point.
In all cases the EBSD maps show damage to the Al sample. Recrys­
tallisation has occurred at the edges of the sample, with a mixture of low
and high angle grain boundaries present in this region. More gradual
changes to the crystal orientation continue inwards. T3 and T1 have a
large rim (a crater rim) at the corner of the trench, identified in the SEM
images by a horizontal white dashed line. A smaller rim is present in
T0.1 and no rim is observed near the T0.05 cut. Rim formation has
previously been attributed to melt ejection from the ablated region [11].
A fine-grained region is present at the top edge of the T3 and T1 samples,
and to a lesser extent, T0.1. These areas are poorly indexed in the EBSD
maps. Close inspection of the secondary electron images indicate that his
area is somewhat porous. This is most apparent in Fig. 4c. These porous
areas are thought to be the result of melt ejection.
The microstructure of the three samples prepared using an area dose
of 200 pulses/µm2 (T3, T1, and T0.1) is different in character to that of
the sample prepared with an area dose of 5 pulses/µm2 (T0.05). The top
surface of T0.05 contains a thick layer of fine grains with high angle
grain boundaries (~ 7 µm thick on the right hand side of the image),
while the laser ablated edge (vertical edge) also contains a layer of fine
grains that is thicker than that seen for the other three samples.
Although no crater rim has formed at the corner of the laser cut, sig­
nificant recrystallisation has occurred at this corner. The observed dif­
ferences between the results may have been caused by the use of the
focus shift for this particular trench. Further exploration of these dif­
ferences will be presented in the discussion.
Samples T3, T1, and T0.1 all contain a fine-grained structure at the
very edge of the laser cut. As described earlier, the outer part of this
layer is attributed to redposited molten matter, but there is also a dense
layer of small grains on the edge of the sample that could be attributed to
recrystallisation, similar to the recrystallised later observed in the coarse
tip sample. Misorientation plots, provided in Fig. 5, have been preared
from the region indicated by the line from point A to point B in the EBSD
maps in Fig. 4. Across all laser powers, the first few microns from the
laser ablated edge contain large misorientations, consistent with
recrystallisation. Beyond this region the material has been heavily
deformed, but does not conatin high angle grain boundaries. This in­
dicates that this damage is the result of strain that occurs as a result of
stress induced during laser ablation. This sub-surface deformation is
similar to that observed in the Al atom probe tip and extends up to 40 µm
into the sample.
The top surface of all samples has a layer of small grains, roughly 1-3
6
Ultramicroscopy 220 (2021) 113161
µm in diameter, with high angle grain boundaries between them. This
layer is thicker for sample T0.05. As this is a polished surface it is
possible that the small grains on the surface are induced by mechanical
damage during polishing. To test if this is indeed the case an EBSD image
is provided in Fig. 6 from a FIB prepared area at a distance >1 mm from
the laser affected surface. Indeed, a layer of fine grains, comparable to
those seen on samples T3, T1, and T0.1, is present on the area unaffected
by the laser. There are two possible explanations. One is that the layer is
the result of stress-induced recrystallisation caused during mechanical
polishing [12]. Another is that it is redeposited material from the laser
ablation process, this was not ruled out in the current work by testing a
non laser ablated sample. It is not, however, a product of thermal
damage.
4. Discussion
4.1. APT sample preparation
The main aim of this work is to reduce sample preparation time for
TEM and APT by using laser ablation in the sample preparation process,
but it is also neccessary to ensure that the process results in undamaged
samples that are representative of the bulk material. In terms of the time
required to prepare samples for atom probe tips, the use of laser ablation
for the first stage significantly reduces sample preparation time and its
implementation would reduce the degree of expertise required to pre­
pare appropriate atom probe tips. Initial results indicate that coarse, FIB-
ready, atom probe tips can be prepared from a pre-polished surface for
final annular milling in under 30 min per tip, as opposed to hours [3,13].
The final shape of the coarse APT tips varies depending on the material
under consideration, with some materials resulting in a shallower shank
angle than others. The final dimensions at the apex of the coarse APT tips
tend to be on the order of 20 µm, therefore, annular FIB milling is a
necessary step to reduce the tip diameter to 200 nm or less. This process
takes between 30 to 40 minutes to complete depending on the starting
shank angle. This is roughly the same amount of time that it takes to
annular mill an atom probe tip from a FIB prepared post [14] or for an
in-situ xenon plasma-FIB approach [15]. Laser ablation removes the
need for lift-out of non-site-specific samples, significantly reducing the
time required to reach the annular milling stage and without signifi­
cantly adding to the time required for the final annular milling step.
Understanding the damage caused by laser ablation is less
N. White et al.
Fig. 6. EBSD image of an area of the sample a significant distance from the laser ablation cuts.
straightforward. Previously, damage has been treated differently by
different authors: in some studies, recrystallised/amorphous zones are
considered [7,16], while other studies only consider induced stresses
[17]. In the context of whether a sample prepared for microstructural
analysis is representative of the bulk sample, a stringent perspective on
damage is required. In the case of APT and TEM, stress induced zones
can be significant enough to cause changes to the local chemistry and
crystal orientation. Thus, in the current study both recrystallised zones
and zones of induced strain have been considered as damage.
EBSD results using laser ablation in the preparation process for APT
samples indicated very little damage in the Si wafer. This suggests that
ablation may be a good method for the preparation of electronic mate­
rials. Another possible thermal affect that may be considered is the
redistribution of impurities. Given the current evidence that no signifi­
cant crystal damage occurs to the Si wafer, APT becomes the perfect
platform for investigating impurity redistribution and segregation
occurring as a result of the sample preparation process [18]. For the
as-cast Al, a thin recrystallisaed layer at the very edges of the needle
might be expected to be removed during the final FIB annual milling
step, however, the misorientation profiles indicated that significant
deformation occurred in the form of a gradual change in orientation
from the edge of the sample inwards, of more than several tens of
micrometres. Care would be needed with the interpretation of atom
probe or TEM results from these samples.
4.2. Laser induced damage
Laser ablation with a 490 ps pulsed laser proceeds as a largely
thermal process, and laser-induced recrystallisation has previously been
reported as a bi-product of this process [19]. To induce recrystallisation,
the thermal energy must exceed the given material’s recrystallisation
temperature. The absence of a recrystallisation zone in the Si wafer
suggests that the temperatures reached at the edge of the laser ablated
region are less than would be required to cause recrystallisation. For the
Al sample the presence of recrystallisation suggests that the tempera­
tures reached during laser ablation are greater than 250◦ C, the lower
range of the as-cast Al recrystallisation temperature [20]. An increase in
the width of the recrystallisation zone for the 0.05 W trench may be
linked to the use of the focus shift. Focus shift was used for the 0.05 W
trench to imitate the process used to create the coarse atom probe tips.
The choice to use the focus shift for the atom probe tips was made based
on an observed improvement in the atom probe tip shape.
In an attempt to understand the effects of laser power on the extent of
damage in the Al sample, a number of laser powers were tested. To
change the effective laser power, the laser repetition rate is changed,
with an increased repetition rate linked to increased laser power. Pre­
vious studies have linked repetition rates to the formation of crater rims,
for lasers with an average power in the range of 60 W, with lower
repetition rates, therefore lower powers, linked to the observation of
smaller crater rims [21]. The current results support this finding for
significantly lower powers, identifying that a decrease in power corre­
sponds to the formation of smaller crater rims. Although a crater rim was
not observed for the lowest power, 0.05 W, a significant amount of
7
Ultramicroscopy 220 (2021) 113161
recrystallisation was observed at the corner of this sample. This suggests
that the thermal energy transferred when using the lower power is
sufficient enough to cause recrystallisation, but is not large enough to
induce thermal deformation of the sample.
While the recrystallised regions could be removed in the FIB step, the
most serious form of damage observed in the results are the zones of
misorientation identified in the vicinity of the laser ablated region. The
depth of the region affected by misorientation is equivalent in all Al
samples regardless of the applied laser power. This suggests that the
observed reorientation of the grains is not caused by thermal effects. It is
therefore proposed that the misorientation profile along A-B is caused by
the presence of mechanical forces in the form of applied pressure. As
material is rapidly heated and vaporised, stress develops within the
trench, leading to the observed deformation behaviour/strain [11,17].
Laser peening, a surface engineering technique, makes use of these high
pressures to purposefully induce residual stress, thereby improving the
material hardness [17,22]. The residual stresses in laser peening are
defined by small misorientations observable with EBSD, which are
comparable to the misorientations visible in Figs. 2, 4, and 5. The same
zone of misorientation was not observed in the Si sample, suggesting
that this material is better able to withstand the applied forces resulting
from the development of vaporisation pressures. This may suggest that
the development of misorientation damage is solely dependent on the
material properties and not on the chosen laser ablation parameters.
4.3. Implications for sample preparation
A comparison between the Al samples prepared in the two different
geometries (i.e. the 0.05 W trench and the 0.05 W Al atom probe tip),
reveals two different microstructures. While both misorientation plots
indicate an equal amount of deformation caused by induced strain, the
coarse APT tip appears to have undergone less recrystallisation than the
trenches. The only difference in the preparation of these samples was the
geometry of the prepared samples and the pattern used to prepare the
samples. In the case of the atom probe tip an annular milling pattern was
used, with the laser moving from the centre of the tip outward. In the
case of the trench, a series of line milling patterns were used. When
conducting an annular milling pattern, a larger surface area to volume of
material is exposed to the atmosphere, providing a larger area for
thermal convection of heat away from the sample. If we assume that
local heating of the sample is responsible for the recrystallisation, then a
reduction in potential for thermal energy transfer to the sample will
reduce the amount of recrystallisation observed. These results suggest
that the pattern used during laser ablation plays a significant role in the
inducement of thermal damage. A reduction of thermal damage due to
changing milling patterns has also been observed in studies of thermal
damage induced in biological samples when prepared using FIB milling
techniques [23]. To account for this in future laser ablation protocols it
is recommended that alternative patterns are used during the ablation
process.
The limited thermally induced recrystallisation in the laser ablation-
prepared Al tips suggests that consideration of thermal damage of these
samples is not necessary for atom probe sample preparation. In contrast,
N. White et al.
unless changes are made to the rastering patterns, it is critical to
consider the thermal properties of the sample when using laser ablation
for TEM sample preparation. For both APT and TEM sample preparation,
the extent of the damage induced by the presence of vaporisation
pressures can be prohibitive to the use of laser ablation as a preparation
method, however, this is dependent on the material chosen. In the
current study it is evident that the pressures present during laser abla­
tion do not lead to deformation in the preparation of Si wafers, with very
little to no damage observed in the results. The opposite is the case with
the Al samples, with the stress-induced misorientation largely prohib­
iting the use of this technique for the preparation of Al APT and TEM
samples by laser ablation processes.
5. Conclusion
We have explored the potential to use laser ablation as a preparation
method for APT and TEM samples. The use of laser ablation as an initial
‘bulk milling’ process has significantly reduced the time required for
APT sample preparation and removes the need for the highly-skilled ‘lift-
out’ step and the local platinum weld. However, initial results indicate
that the successful use of this preparation method is dependent on the
material under investigation. As a guide to choosing an appropriate
material for sample preparation, two mechanisms that influence the
degree of damage have been identified:
1 Thermally induced recrystallisation at the edge of the sample
exposed to the laser
2 Deformation caused by stress during vaporisation
Thermally-induced effects such as the development of crater rims at
the corners of the samples can be reduced by reducing the laser power.
Reduction of the laser power, however, increases the observed recrys­
tallisation zone, suggesting that an increased amount of thermal energy
transfer to the sample at lower laser powers is significant enough to
induce recrystallisation but that the stress generated during ablation is
insufficient to cause deformation of the sample. An alternative method
for minimising recrystallisation has been suggested, which takes into
consideration the laser scanning pattern. For samples such as Si, the
current APT sample preparation process does not induce significant
thermal damage.
Modification of the laser power does not influence the depth of the
misorientation zone, suggesting that this is a purely mechanical process.
Therefore, stress-induced misorientation appears to be the key limiting
factor in regards to which materials are appropriate for sample prepa­
ration via the laser ablation process.
In an initial analysis of N-type phosphorous -doped Si we found no
damage in the sample, either in the form of recrystallisation or strain-
induced misorientation. Furthermore, the preparation time and skills
required for sample preparation are significantly reduced through the
utilisation of the laser ablation process. In conculsion, the laser ablation
technique presents as a possible alternative sample preparation method
to FIB lift-out, however, close attention must be paid to the material
chosen for analysis.
Declaration of Competing Interest
None.
Ultramicroscopy 220 (2021) 113161
Acknowledgement
The authors acknowledge the instruments and scientific and tech­
nical assistance of Microscopy Australia at the Australian Centre for
Microscopy and Microanalysis, The University of Sydney, a facility that
is funded by the University, and State and Federal Governments.
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