Composite Structures 232 (2020) 111559

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Composite Structures
journal homepage: www.elsevier.com/locate/compstruct

Shear strength of bonded joints of carbon fiber reinforced plastic (CFRP) T

laminates enhanced by a two-step laser surface treatment
⁎
Yingxi Xie, Binbin Yang, Longsheng Lu , Zhenping Wan, Xiaokang Liu
School of Mechanical & Automotive Engineering, South China University of Technology, 381# Wushan Road, Guangzhou 510641, China

A R T I C LE I N FO A B S T R A C T

Keywords: The apparent shear strength of single-lap bonded joints of carbon fiber reinforced plastic (CFRP) can be en-
Laser processing hanced by laser surface treatment. In this work, a two-step laser surface treatment was used to improve the
Bonded joints single-lap bonded joint performance of CFRP-laminates. STEP-1, the resin at the outer surface of laminates was
Shear strength completely removed by an optimal laser etching process to provide neat carbon fiber fabric. STEP-2, the as-
CFRP
obtained exposed carbon fiber fabric was further irradiated to produce a series of mini-grooves on its surface.
Groove etching
Surface treatment
Laser scanning parameters, i.e., spot distance, scanning angles, groove distance and patterns, were investigated
to analyze their effects on the morphologies of generated grooves. Single-lap shear tests were also carried out to
assess the mechanical performance of these laser processing bonded joints. Experimental results indicated that
crossed grooves significantly enhanced the shear strength of the CFRP-laminates. Failure morphologies of shear
tests were observed to analyze the strengthening mechanism of grooved-CFRP by laser surface treatment. Using
optimal processing parameters during laser surface treatment, the apparent shear strength of single-lap bonded
joints of CFRP-laminates reached 18.58 MPa, implying a 40.8% enhancement compared with smooth laminates.

1. Introduction strengths. To address these critical strength requirements in primary

Carbon fiber reinforced plastic (CFRP) is a promising candidate for
use in airplanes and vehicles because of its extremely lightweight and
energy conservation properties. An outstanding type of CFRP, weaved
carbon fiber reinforced plastic laminate (i.e., CFRP-laminate), has been
widely applied as critical components in aerospace fields [1]. Normally,
joining processes were unavoidable in manufacturing CFRP-laminate
components, especially those with complex geometries or large sizes
[2].
Bolted connection and riveted connection, as two widespread
joining techniques for a long history, are still selected to joint composite
parts in many primary industrial fields [3]. However, both the bolted
and riveted joints exhibited several substantial disadvantages, including
increased localized stresses, time-consuming processes, and inherently
non-lightweight designs [4,5]. Additionally, through-holes drilled using
these joining techniques was more likely to result in adverse effects on
structural integrity of CFRP-laminates, including burrs, tearing and
delamination at top and bottom layers [6,7].
Adhesive bonded connections represented a promising alternative
to the aforementioned mechanical connections for CFRP-laminate
joining due to lighter and higher compact structures [8]. However,
prepared traditional bonding joints have not exhibited strong shear
load-bearing applications, mechanical joints (bolted or riveted joints)
are always utilized in addition to bonding joints [9,10]. However, these
complex joints, i.e., bonding joint combined with mechanical joint are
still overstaffed. To identify pure adhesive bonded connections adap-
table for complex composite components, researchers [11] have looked
for methods to enhance the apparent shear strength of bonding joints.
Generally, the shear strength of a CFRP-laminate bonding joint was
strongly dependent on its adhesive thickness and nature, joint geo-
metry, and surface treatments [8]. For designed CFRP-laminate joints,
surface treatments can be used as posttreatment processes to further
enhance bonding strengths. Therefore, surface treatments of CFRP-la-
minate bonding joints have gradually gained popularity. As reported by
Sun et al. [12], the surface treatments of CFRP-laminates can be clas-
sified into chemical and mechanical treatments. Balart et al. [13] and
Jölly et al. [14] utilized photografting and surface functionalization
techniques to improve the fracture toughness and shear strength of
composite joints by promoting covalent bonding, respectively. How-
ever, these chemical treatments have negative environmental impacts
due to their chemical waste. Moreover, these methods are difficult to
automate in industry. Kanerva et al. [15] and Khan et al. [16] used
peel-ply and grit-blasting techniques to control surface roughness and
remove laminate contaminants, respectively. Unfortunately, these

⁎
Corresponding author.
E-mail address: meluls@scut.edu.cn (L. Lu).

https://doi.org/10.1016/j.compstruct.2019.111559
Received 11 June 2019; Received in revised form 23 September 2019; Accepted 9 October 2019
Available online 12 October 2019
0263-8223/ © 2019 Elsevier Ltd. All rights reserved.
Y. Xie, et al.
Table 1
Pertinent characteristics of the applied laser engraving machine (provided by the manufacturer).
Characteristic Output power (W) Scanning speed (mm/s)
Value 0–20 0–2000
mechanical treatments were time-consuming, hard to machine, and
resulted in surface overstretching and material contamination. In recent
years, laser treatment was considered as an appropriate alternative to
the aforementioned treatments to process the surfaces of CFRP-lami-
nates, which was easy to operate and could be used to simultaneously
modify surface chemistry and morphology [17–20].
Fischer et al. [21] investigated the physical morphologies of CFRP
surfaces treated with various types of laser sources. Regardless of the
laser source, most laser treatments increased the adhesive bonding
strength of CFRPs. Leone et al. [8] reported positive effects of Yb:YAG
fiber laser treatment on the joint strength of CFRP-laminates obtained
by direct co-bonding. Tao et al. [22] evaluated the effect of CO2 laser
surface treatment on the fracture toughness of adhesively bonded
composite joints. Their investigations suggested that increased bonding
strengths of CFRPs after laser treatment were primarily due to the loss
of surface resin matrix and the exposure of fresh carbon fiber (CF) tows,
which increased the contact area and adhesive capacity between CFs
and bonding agents. However, the surface resin distribution of a CFRP-
laminate on the unit area was uneven, i.e., resins were found in
abundant concentrations in weaving junctions but less so in CF tows.
This uneven resin distribution would lead to processing challenges
during surface laser treatment. For instance, in our pre-experiments,
many cross-shaped resin particles were tightly located at most weaving
junctions, whereas all resins located above CF tows were removed by
laser irradiation. Therefore, it is a technical challenge to completely
remove the resin matrix without apparently damaging CF tows during
the laser etching of CFRP-laminates [23–25].
Interestingly, any mechanics structures generated on a bonded
surface can significantly enhance the shear strength of adhesive
bonding joints. Tsuka et al. [26] investigated the effects of laser groove
treatments on the shear strength of plastic PEEK joints. They claimed
that the bonding specimens exhibited significantly reinforced apparent
shear strength after fabricating grooves on bonding interfaces. Moroni
et al. [27] successfully employed a microscale textured surface on a
metal plate via laser processing to improve the shear property of
bonding joints. Da Silva et al. [28] evaluated the function of groove
patterns distributed on the metal substrate surface during the adhesive
bonding process. They revealed that the failure mode of bonded joints
was significantly related to groove patterns. Garcia et al. [10] adopted a
3-dimensional (3D) printing technology to impart textured structures
onto composite bonding joints. The results indicated that the apparent
shear strength of composite joints was significantly enhanced. Based on
these prior studies, the bonding performance of CFRP-laminate parts
can be further enhanced by introducing mechanical structures in the
carbon fiber fabric after removing resin matrix from the surface.
In this work, a two-step laser surface treatment is proposed to en-
hance the bonding strength of CFRP-laminates. In the first step, resin
material on the bonding interface of CFRP-laminate was completely
removed under optimal laser processing parameters. In the second step,
a series of grooves with different patterns were etched on the exposed
weaving CF fabric with further laser processing. Finally, single-lap
shear tests of CFRP-laminate joints bonded by thermoplastic poly-
carbonate (PC) film [29–31] were carried out to evaluate the effects of
these laser treated surface. Failure images and apparent shear strengths
were carefully analyzed.
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Composite Structures 232 (2020) 111559
Repetition frequency (kHz) Pulse duration (ns) Laser spot (μm)
20 100 50
2. Experimental procedures
2.1. Materials and laser equipment
CFRP-laminates were purchased from Zhongfu Carbon Fiber
Corporation (Jiangsu, China), which consisted of 5 layers of poly-
acrylonitrile (PAN)-based T700 balanced weaving carbon fiber fabric
(3 K, Toray Industries, Japan). Bisphenol-A epoxy resin (NPEL-128) was
used as the polymer matrix, and its volume content was controlled from
30% to 35%.
The PC film was purchased from the LEXAN SABIC Company, Saudi
Arabia. The company provided material specifications for the PC film
are: 0.25 mm thick, 1200 kg/m3 density, 65 MPa tensile strength,
2506 MPa tensile modulus, 153 °C glass transition temperature and
approximately 220 °C melt onset temperature, as measured with a dif-
ferential scanning calorimeter (Model 214, NETZSCH, Germany). No
further processing was applied.
A diode-pumped Nd:YAG solid pulsed laser engraving machine
(QSFL-20 A, Shenzhen Super Laser Technology Co., Ltd., China) was
used. Pertinent detailed characteristics of the laser system are listed in
Table 1. To prolong the life of the laser engraving machine, the max-
imum power was limited to 16 W (80%).
2.2. Laser surface treatment of CFRP-laminates
The laser beam irradiation mechanism of CFRP-laminates can be
briefly described as follows [8]. The majority of laser radiation is ab-
sorbed by CF tows because the resin matrix is transparent to the near-IR
radiation of the Nd:YAG laser. As a result, the as-irradiated CFs rapidly
heat up. After received thermal energy, some amount of thermal energy
is transferred from CFs to the nearby resin matrix through heat con-
duction. Due to the high thermal concentration of laser beam, the resin
at heat affected zone will be evaporated and fresh CFs will be exposed.
Fig. 1(a) depicts a schematic of the two-step laser surface treatment,
which consists of surface resin removal (STEP-1) and groove etching
(STEP-2) of CFRP-laminates. There are many parameters involved in
laser processing, such as output power, scanning speed, hatch distance,
repetition frequency and scanning patterns. The scanning speed and
repetition frequency affect the overlapping factor, which is a critical
factor for pulsed laser applications [8]. To better control this factor,
several preliminary experiments investigating laser spot position were
designed, including overlapping, ± 45° tangential, 0/90° tangential and
separation. Fig. 1(b) shows the laser spot arrangement of these pre-
experiments, as well as specific scanning speeds and corresponding spot
center distances. During the groove etching process, the groove depth
was determined by repetition processing numbers. Scanning angles
were introduced to investigate the effects of heat affected zones on final
groove morphologies. The scanning angle is defined as the intersection
angle between the axial direction of surface CFs and the laser scanning
direction. The heat conductivity coefficient of a CF tow showed ani-
sotropy, which was largest at an axial direction and smallest in a ver-
tical direction [32,33]. Therefore, three scanning angles, 0°, 45° and
90°, were studied in this work as shown in Fig. 1(c).
2.3. Single-lap bonded joint tests
A thermoplastic PC film (0.25-mm thick) was set as an adhesive
agent to make a single-lap joint by hot-press technique. Hot-press
parameters included a sub-210 °C molding temperature, 6 MPa molding
Y. Xie, et al.
Fig. 1. (a) The schematic diagram of the two-step laser surface treatment of CFRP-laminate; (b) four typical spot positions arrangement; (c) three typical scanning
angles distribution and (d) the size of a single-lap shear test specimen.
pressure and a 3.5-min holding time [29]. Considering the convenience
of processing and observation, the size of a CFRP-laminate was selected
as 51 × 12.5 × 1 mm3 (length × width × thickness) for single-lap joint
tests which was half the size recommended by ASTM D1002 standards
[34]. All specimens were cut into the designed shape by a CNC milling
machine (Guangzhou Machine Tool Works Co., Ltd., China). A uni-
versal material testing machine (Model Z100, Zwick/Roell, Germany)
with a maximum capacity of 100 kN, was used to test the shear strength
of these single-lap joints based on ASTM D5868 standards [35]. A
special fixture was designed to guarantee the precise positional re-
lationship between two CFRP-laminates and a PC film. All shear tests
were conducted at a set speed of 1.3 mm/min. To eliminate asymmetry
in the tests, a testing specimen and two alignment tabs of
25 × 25 × 1 mm3 were clamped together as described by Lambiase
et al. [30]. The load-bearing capacity of each shear test was determined
over five replicate tests. Each test did not show relative slipping phe-
nomena between clamping fixture and specimen.
2.4. Other characteristics
The morphologies of the laser-processed surfaces and failure posi-
tions of CFRP-laminate were observed by scanning electron microscopy
(SEM) (Hitachi S-3700N, Hitachi High-Technologies Corporation,
Japan). The 3D profiles of specimen surfaces were analyzed by a digital
optical microscope (VH-Z100R, Keyence Corp., Japan).
3. Results and discussion
3.1. Processing parameter optimization of STEP-1
For the two-step laser surface treatment, STEP-1 was used to etch
the resin layer on the bonding interface of a CFRP-laminate joint. In this
step, a parallel laser scanning strategy was adopted, as most previous
studies did [23,25,36].
3.1.1. Output power selection
Fig. 2(a) depicts two typical laser scanning methods which are Z-
shaped and S-shaped scanning paths (named Z-mode and S-mode, re-
spectively). Due to the effect of return time, Z-mode requires more the
total processing time than that of S-mode, thereby reducing processing
efficiency. Therefore, the S-mode of laser scanning was adopted in this
work. To ensure the consistency of laser energy density in the warp and
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Composite Structures 232 (2020) 111559
weft directions of CFRP-laminates, the laser spot and hatch distances
were set equal.
As illustrated in Fig. 2(b), some cross-shaped resin particles are
clearly shown to locate tightly on the weaving junctions of CFRP-la-
minate, whereas most resins above the CF tows were removed without
optimal laser processing parameters. These resin particles may cause
negative effects to the bonding combination of connection joints, such
as delamination, weak bonding, and insufficient wettability of bonding
agents. A series of morphologies laser-treated with different spot dis-
tances (d) and output powers (Po) was used to investigate the effects of
laser parameters on resin removal results. The output powers of all
specimens started from 1 to 8 W at increments of 1 W. As shown in
Fig. 2(c), as the output power increased, all specimens presented a si-
milar tendency, i.e., the resin on weaving junctions was gradually re-
duced. Interestingly, there was a threshold output power to completely
remove the surface resin on CFRP-laminate. The spot distance and the
output power affected the quantity of residual resin remaining on the
surface. The spot distance and the output power are involved in the
Energy density (E) of laser processing, whose mathematical description
can be calculated as:
Ep n Ep (l/ d )2 Po
E= = =
A l2 fd 2 (1)
where Ep is the laser pulse energy determined by output power Po, n is
the total pulse number in the processing area A, d is the spot distance, f
is the repetition frequency of laser pulse, and l is the side length of this
area.
To validate the applicability of energy density, the threshold output
power and spot distance of each experiment were substituted into Eq.
(1) as listed in Table 2. The energy density E decreased as the spot
distance increased, i.e., the energy density required to completely re-
move surface resin was reduced. Therefore, the resin removal of CFRP-
laminate on the weaving junction is not fully dependent on the energy
density. For short spot and hatch distances, the heat generated by ad-
jacent laser spots and adjacent scanning paths may affect each other.
When a laser pulse leaves a certain position, the resin of this position
begins to cool down until the next pulse in the adjacent scanning path
reheats the region. Therefore, the scanning frequency fs directly influ-
ences the resin vaporization effect, which should be accounted in the
calculation. The scanning frequency can be described as follow:
Y. Xie, et al. Composite Structures 232 (2020) 111559

Fig. 2. (a) the schematic diagrams of two typical scanning modes; (b) the resin residual phenomenon of a CFRP-laminate laser treated by 35.3 μm spot distance and
3 W output power; (c) the effect of output powers on the processing results with different spot distances; (d) the pictures of a CFRP-laminate laser treated by 75 μm
spot distance and 12 W output power; (e) the relationship between output power and scanning length.

Table 2 75 μm spot distance and 12 W output power as calculated by the the-

Threshold output powers with different spot distances and their energy density oretical threshold value of Pc. There were resin particles and film ob-
and continue power density in calculation. served between spots. An increased laser power could not eliminate the
Spot distance d Threshold output Energy density Continue power influence of increased spot distance when the spots were separated. In
(μm) power Po (W) E (J/mm2) density Pc (W/mm2) addition, high pulse energy also caused CF breakup. Thus, it is in-
appropriate to adopt separated spot distances.
12.5 2 0.64 16k
Besides spot distance, Eq. (4) indicates that the threshold output
25.0 4 0.32 16k
35.3 6 0.24 17k power is also related to the processing length in the weft direction but is
50.0 8 0.16 16k independent of the processing length in the warp direction. As Fig. 2(e)
shows, resin particles can be observed with a slight distance increase in
the weft direction. Because the distance increase in weft length in-
l warp l warp v fd creased the next arrival time in adjacent paths, the heating frequency
fs = = lwarp·lweft
= =
dt d l weft l weft reduced and cooling time increased. When the output power was ad-
dv (2)
justed to 9, 12 and 15 W, corresponding to the 15, 20 and 25 mm spot
where v is the scanning speed, t is the total processing time, and lwarp distances as calculated by Eq. (4), the residual resin disappeared. In
and lweft are the scanning lengths in their specific areas. Combining fs addition, specimens treated at 6 W output power under 35.3 μm spot
and E, an designed equation named as continue power density (Pc) can distance did not show difference with increases in the warp direction.
be calculated as follow: Therefore, parameter Pc can be used to explain the resin removal
phenomena in the laser etching processing and can be considered an
Pc = kfs E (3) empirical equation in actual applications.
where k is a scale factor. Substituting Eqs. (1) and (2) into Eq. (3), we Therefore, instead of simply increasing output power, a modular
arrive at: laser processing method is preferably used in the laser surface treat-
ment of CFRP-laminates with large areas. Modular laser processing
kPo maintains processing efficiency and avoids disadvantages due to high
Pc =
dl weft (4) output power, such as high power consumption and possibly broken
CFs.
The calculated Pc of different spot distances are listed in Table 2 and
are consistent with each other except at the 35.3 μm spot distance. This
is because the output power was first set as an integer value. Assuming 3.1.2. Spot distance selection
16 k is the theoretical threshold value of Pc for completely removing the In addition to addressing surface resin removal, a relatively com-
resin, the theoretical threshold output power of 35.3 μm spot distance plete CF morphology must also be considered in CFRP laminate surface
should be 5.6 W, which was validated by additional experiments. laser treatment. Different spot distances can be used to achieve surface
However, the application of Pc was also limited by overlapping laser resin removal at different output power levels. Thus, STEP-1 processing
spots. Fig. 2(d) presents the morphologies of a specimen laser-treated at parameters cannot be optimized by considering only Pc. We

4
Y. Xie, et al.
Fig. 3. SEM images show the morphology of CFRP-laminates laser treated at different spot distances with corresponding threshold output power levels: (a) 75 μm; (b)
50 μm; (c) 35.3 μm; (d) 25 μm and (e) 12.5 μm. (f) shows a partially enlarged picture of (e).
investigated the effects of different spot distances according to corre-
sponding threshold output power levels on the processing morphology
of CFRP-laminates. The specimens shown in Fig. 3 have the same Pc
values. However, the degree of broken CFs gradually increased as the
spot distance decreased. Especially at 12.5 μm spot distance, CFs pre-
sented with severe fractures. As the spot distance decreased from 50 to
12.5 μm, E values rapidly accelerated, which was consistent with var-
iations in morphology. The energy density seemed to significantly affect
the CF morphology due to the CF tow directly absorbing thermal energy
from the laser pulse. In this work, based on the effects of energy density
(E) and continue power density (Pc), laser spot distances from 25 to
50 μm in STEP-1 are optimal. At these distances, a qualified processing
morphology with fewer broken CFs and full surface resin removal can
be obtained.
Fig. 4 shows the effect of spot distance on the apparent shear
strength of CFRP-laminate joints. The shear strength increased as the
spot distance increased from 12.5 to 25 μm, remained constant from 25
to 50 μm, and declined from 50 to 75 μm. These results were consistent
with the results of previous surface morphology investigations. For the
Fig. 4. Shear strengths of CFRP-laminate joints laser treated at different spot
distances and corresponding threshold output power levels.
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Composite Structures 232 (2020) 111559
12.5 μm specimen, a large number of broken CFs resulted in early joint
failure under low shear loads. The 75 μm specimen displayed resin
particles on the CF surface and residual resins on the weaving junction.
These residual resins hindered the impregnation of PC film into CF
leading to weak adhesive joints [36]. These two specimens had rela-
tively lower apparent shear strengths than others. Specimens laser
treated at spot distances ranging from 25 to 50 μm had similar complete
CF morphology, and their shear strengths values were also similar.
Based on processing efficiency and shear strength, a spot distance at
35.3 μm was adopted for resin removal; and a shear strength of
13.20 MPa was used for comparisons subsequent shear tests.
3.2. Processing parameter optimization of STEP-2
All specimens were pretreated by STEP-1 laser surface treatment
with optimal processing parameters, i.e., at 35.3 μm spot distance and
6 W output power.
In STEP-2, two types of groove patterns, i.e., parallel and crossed,
were used to etch grooves for comparison, as performed by Da Silva’s
research [28]. Two scanning orientations at 0° and 45° were conducted.
Due to the weaving properties of CF fabric, three groove angles were
obtained: 0°, 45° and 90°. Unlike surface resin removal, groove etching
requires relatively high energies. Therefore, the output power was set to
10 W. Due to output power limitations of the laser equipment, each
groove was reprocessed 8 times. Under these conditions, grooves were
etched to a depth nearly equivalent to the thickness of a CF tow (about
0.08 to 0.1 mm) in the adopted CFPR-laminate. The as-fabricated
grooves in the CF fabric were intended to have as much surface area as
possible to provide a greater anchoring effect during the bonding pro-
cess.
3.2.1. Spot distance selection
The spot distance of the STEP-2 laser processing was first in-
vestigated to determine its effect on the smoothness of the groove
profile. Because a laser spot was 50 μm in diameter, two spot distances
of 50 and 25 μm, corresponding to an entire and a half of a spot dia-
meter, respectively, were compared. Fig. 5(a) and (b) show the
morphologies of as-prepared grooves at the two spot distances under a
90° scanning angle. The grooves prepared at 50 μm spot distance ex-
hibited serrated edges. The grooves prepared at 25 μm spot distance
Y. Xie, et al.
Fig. 5. The groove morphologies of CFRP-laminate laser treated by STEP-2 at different spot distances and scanning angles: (a) 50 μm and 90°; (b) 25 μm and 90°; (c)
25 μm and 45° and (d) 25 μm and 0°. (e) shows schematic diagrams of the heat affected zone of CFRP-laminate laser treated by STEP-2 at different scanning angles.
exhibited smooth and linear profiles. In addition to the 90° scanning
angle, the effectiveness of the 25 μm spot distance was validated at 45°
and 0° scanning angles as shown in Fig. 5(c) and (d), respectively. To
obtain an optimal groove profile, a 25 μm spot distance was preferred
and was adopted in subsequent groove etching experiments.
While thermal effects can be minimized using a pulsed laser beam,
they cannot be entirely avoided [37]. Dong et al. [38] indicated that a
weaving carbon fabric showed a better thermal diffusion along its axial
direction. Therefore, polymer matrices close to grooves were strongly
affected and eventually vaporized upon laser beam etching, thereby
producing some extruded CFs. The volumes of as-vaporized polymer
matrix are determined by the areas of heat affected zone. Fig. 5(e)
displays the effect of groove angles on the heat affected zone. Because
the amounts of resin vaporized along the CF axial direction were the
same for all scanning angles, the final layer thickness of heat affected
zone can be readily calculated accordance with the Pythagorean the-
orem. This conclusion can be validated by SEM observations shown in
Fig. 5(b)–(d).
3.2.2. Groove distance and scanning angle selection of parallel laser
scanning
Generally, the groove distance of a bonded joint will directly affect
the contact area of the bonding interface. Therefore, the groove dis-
tance is a critical factor that should be considered when a grooved
bonded joint is designed. The morphologies of CFRP-laminate laser
treated by STEP-2 with different scanning angle grooves (varying from
0° to 90°) and groove distance (varying from 50 to 150 μm) are shown
in Fig. 6(a)–(i). At a 50 μm groove distance for all scanning angles, the
CF tows on the outer surface were severely damaged, exposing the CF
tows in the bottom layer. During groove etching processes, a short
groove distance generates excessive energy. Due to the overlapping
heat affected zone, grooves cannot be successfully manufactured. In-
stead, most CFs on the outer layers of CFRP-laminates become dis-
continuous and collapse. Therefore, a short groove distance would be
inappropriate for groove etching on CF fabric. As groove distance in-
creases, the groove morphology improves. At a 100 μm groove distance,
continuous grooves were observed, and a complete surface CF layer was
maintained.
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Composite Structures 232 (2020) 111559
The scanning angle of laser treatments also affects groove mor-
phology as Fig. 6(b), (e) and (h) show. The grooves prepared at 0°
scanning angle maintained relatively good morphology even at short
groove distances due to the minimum heat affected zone at a 0° scan-
ning angle. While at a 90° scanning angle at short groove distances, only
shallow, poor morphology grooves were formed. Because the heat af-
fected zone at a 90° scanning angle was at a maximum, most resins
between adjacent grooves were vaporized, inducing severe CF shed-
ding. The groove morphology prepared at a 45° scanning angle ex-
pectedly showed a mix of morphologies, i.e., both CF shedding and
deep grooves were observed.
Considering the comprehensive effect of groove distance and scan-
ning angle, a 150 μm groove distance seems to be a good choice to
obtain clear grooves at all scanning angles. As shown in Fig. 6(c), (f)
and (i), when the groove distance increased to 150 μm, ideal groove
morphology with complete surfaces and deep grooves were observed.
3.2.3. Groove distance selection of crossed laser scanning
The effect of groove distance on crossed grooves was also in-
vestigated, as shown in Fig. 7. Because a 50 μm groove distance was
validated as inappropriate for the aforementioned parallel groove
etching, groove distances from 100 to 200 μm with increments of 50 μm
in crossed groove etchings were examined. To simplify the study, the
groove distances in the two scanning orientations were kept the same.
When the groove distance was set to 100 μm, most of the CFs on the
surface layer were severely damaged, similar to that observed for the
50 μm parallel grooves. Because all crossed grooves have two etching
direction, the 100 μm-distance crossed grooves have the same groove
number as the 50 μm-distance parallel grooves in a unit area, indicating
that they were irradiated by similar laser energy densities. When
comparing the scanning angles of 0/90° and ± 45°, the crossed grooves
prepared at ± 45° scanning angle appeared at more shallow depths.
This is because the parallel grooves at 45° scanning angle and 100 μm
groove distance has appeared slight CF shedding.
As the groove distance reached 150 and 200 μm, the surface CFs and
grooves integrated and flattened out. The crossed grooves accom-
modated twice as many grooves as the parallel grooves at 150 and
200 μm groove distances and still maintained complete groove
Y. Xie, et al. Composite Structures 232 (2020) 111559

Fig. 6. Groove morphologies of parallel grooves of CFRP-laminates laser treated by STEP-2 at different scanning angles and groove distances: (a) 90° and 50 μm; (b)
90° and 100 μm; (c) 90° and 150 μm; (d) 45° and 50 μm; (e) 45° and 100 μm; (f) 45° and 150 μm; (g) 0° and 50 μm; (h) 0° and 100 μm and (i) 0° and 150 μm.

morphology. This indicated that crossed grooves advantageously in- appears as hexagon patterned surfaces. It is due to that the CFs near the
creased the surface contact area. The shape of CFRP-laminates laser groove intersections equally peeled off as the heat affected zones in the
treated with 0/90° crossed etching appears as classical rectangular −45° and +45° scanning angle directions.
patterned surfaces, whereas that treated with ± 45° crossed etching

Fig. 7. Groove morphologies of crossed groove specimens laser treated by different crossed groove patterns and hatch distance in STEP-2: (a) 0/90° and 100 μm; (b)
0/90° and 150 μm; (c) 0/90° and 200 μm; (d) ± 45° and 100 μm; (e) ± 45° and 150 μm; (f) ± 45° and 200 μm.

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Y. Xie, et al. Composite Structures 232 (2020) 111559

Fig. 8. Depths of grooves generated by different scanning angles and patterns: (a) depth bars of different grooves; (b)-(f) are 3D pictures of specimens prepared at 90°,
0°, 45°, 0/90° and ± 45° scanning angles, respectively.

Table 3 scanning direction, resulting in a gradual dissipation of thermal energy

Groove etching parameters. and a linear decrease in groove depth. As Fig. 8(b)–(d) demonstrate, the
Objection Groove distance (μm) Reprocessing times
45° and 90° grooves were flat, whereas the presence of CF fragments
resulted in depth fluctuations in the 0° grooves. Crossed grooves pre-
0° Parallel grooves 200 2 sented the same depths at 45° and 90° directions with parallel grooves.
200 4 However, the depth of crossed grooves obtained at a 0° scanning angle
200 6
200 8
direction further increased compared with that obtained with 0° par-
50 8 allel grooves, from 61.43 to 89.33 μm. Liang et al. [39] indicated that
100 8 there was an impact effect in the pulse laser. Due to this effect, the
150 8 additional 90° scanning of 0/90° etching pattern likely reduced the CFs
250 8
on the surface of 0° grooves, deepening the groove depth. However, the
45° Parallel grooves 200 8
0°/90° Crossed grooves 200 8 0° grooves had nearly no effect on the 90° grooves due to their weak CF
± 45° Crossed grooves 200 8 heat conduction property in the 90° direction.

3.2.4. Groove depth analysis of crossed laser scanning
To provide a specific groove size for reference, the depths of grooves
laser etched on CFRP-laminates by different scanning angles and pat-
terns were measured. In this section, a 200 μm groove distance and 8
reprocessing times were adopted. To minimize errors, each depth was
calculated using native software of the digital optical microscope with
ten repeated measurements in different positions.
As shown in Fig. 8(a), the depths of grooves prepared at 0°, 45° and
90° scanning angles in parallel mode were 61.43, 50.17 and 38.67 μm,
respectively. When the scanning direction was parallel to the CF tow,
the laser energy was concentrated along the axial direction of the CFs,
producing the deepest grooves. As the scanning angle increased, the
heat conduction of the CFRP-laminate started to deviate along the
3.3. Single-lap shear tests and failure analysis
To assess the effect of groove etching parameters (i.e., groove depth,
distance and patterns) on the mechanical properties of as-fabricated
bonded joints, a series of single-lap shear tests was conducted. Table 3
lists detailed information on the groove etching parameters of the dif-
ferent tests. The groove depth variations were achieved by controlling
the number of repetitions of laser scanning. For comparison, a single-
lap shear strength of a smooth CFRP joint was used as reference. This
smooth CFRP joint was also laser pretreated by STEP-1 (otherwise, the
smooth CFRP joint could not be bonded together).
Fig. 9(a) displays the apparent shear strengths of the parallel
grooved-CFRP at 0° scanning angle prepared with different processing

8
Y. Xie, et al.
Fig. 9. Apparent shear strengths of single-lap joints laser treated by different processing parameters in STEP-2: (a) groove depth; (b) groove distance; (c) groove
pattern. (d) shows the optimized results of shear strength.
repetitions, i.e., they were laser treated to obtain different groove
depths. To eliminate the influence of CF shedding, a 200 μm groove
distance was adopted. Because the interface grooves of a bonding joint
increases the contact area between two bonded specimens and provides
an anchoring effect to the bonding agent, the shear strengths of most
grooved-CFRPs were enhanced by employing grooves. However, the 2-
repetition grooved-CFRP was slightly weaker than smooth CFRP. After
etching on the surface, the CF layer was rendered discontinuous, which
may have deteriorated the CFRP shear performance. So the shear
strength variations of grooved-CFRP is the comprehensive result of
enhancement and attenuation brought by the interface grooves. At
shallow depths, the attenuation effects of the grooves were dominant.
Therefore, the bonding strength of 2-repetition grooved-CFRP was even
worse than that of smooth CFRP. As the groove depth increased, the
shear strength of grooved-CFRP steadily increased and reached a
maximum value at 6 repetitions. Then, the shear strength decreased
with subsequent repetitions. This variation was due to variations in the
anchoring effects of grooves. As the groove depth increased, the heat
affected zone region gradually expanded, i.e., the length of extruded
CFs increased, which potentially decreased the tensile strength between
the microstructure layer and composite matrix. Therefore, the con-
nective interface of the microstructure layer may be a short slab in
shear tests. Due to the cask effect, the shear strength declined after
reaching a maximum. Greater groove depths may have also captured air
in unfilled spaces during the binding process. This leads to a weakened
combination between melted PC film and extruded CFs during hot
9
Composite Structures 232 (2020) 111559
press, which negatively affected shear property [36].
Fig. 9(b) shows the effects of groove distance on shear strength of 0°
parallel grooved-CFRPs. Groove numbers were also calculated. When
the groove distance increased from 50 to 100 μm, the shear strength of
0° parallel grooved-CFRP sharply increased. As previously observed, the
morphology of 0° parallel grooved-CFRP with a 50 μm groove distance
exhibited damaged CFs and fewer grooves, indicating a critical at-
tenuation effect of the laser surface treatment. When the groove dis-
tance increased to 100 μm, uniformly distributed grooves were gener-
ated, providing the expected strengthening effect. However, the shear
strength of 0° parallel grooved-CFRP gradually decreased as the groove
distance increased from 100 to 250 μm. This trend correlated with
groove number variation. For a constant area, the groove number and
groove distance were inversely proportional.
Fig. 9(c) shows the shear strength of grooved-CFRPs with different
groove patterns, including 0° parallel, 45° parallel, 0/90° crossed
and ± 45° crossed patterns. The shear strength of the 0° parallel
grooved-CFRP was slightly improved compared with the smooth CFRP
because of the increased contact area after groove etching. When
compared with the smooth CFRP reference sample, the shear strength
of the 45° parallel grooved-CFRP decreased by 11%. Along the tensile
direction, the shear stress of this grooved-CFRP was asymmetric under a
load, indicating that the shear stress was divided in the 45° direction,
generating an additional torque under tensile load. For a bonding
connection, torque loads more likely damages the structure. Compared
with parallel grooved-CFRPs with same groove distances, the shear
Y. Xie, et al.
strengths of crossed grooves were apparently increased. Unlike the 45°
parallel grooved-CFRP, the shear strength of the ± 45° crossed grooves
was 18.6% higher than that of the smooth-CFRP. The ± 45° crossed
grooved-CFRP had a symmetrical structure, thereby eliminating the
influence of asymmetric shear stress observed in the 45° parallel
grooved-CFRP. Compared with the ± 45° crossed pattern, the 0/90°
crossed grooved-CFRP appeared to have a slightly higher shear
strength. This was likely due to the differences in their generated
groove appearances resulting from their different heat affected areas.
Because the above experimental groups were relatively in-
dependent, the optimal processing parameters would be dependent on
the combination of the aforementioned optimized results. Therefore,
additional experiments were performed to validate the prior analyses.
Based on the integrality of grooves, the crossed grooved-CFRPs scanned
at a 150 μm groove distance for 6 repetitions with 0/90° and ± 45°
groove patterns were tested. As shown in Fig. 9(d), the shear perfor-
mances of these crossed grooved-CFRPs improved when compared with
all other results. The shear strengths of 0/90° and ± 45° crossed
grooved-CFRPs were 18.58 and 17.77 MPa, which represented 40.8%
and 34.6% increased rates compared with smooth-CFRP, respectively.
3.4. Single-lap shear failure analysis of grooved-CFRP
To analyze the shear mechanism of CFRP bonding joints enhanced
by laser surface treatment, typical images of failure grooved-CFRPs
were captured. Fig. 10(a) shows two observation positions of two se-
parated parts in a shear test, which reflects the bonding phenomena
between the adhesive agent and CFRP-laminates. In this work, two
common failure modes for a grooved-CFRP joint were observed: (i) the
separation between CFRP-laminates and adhesive agents, and (ii) the
stripping of CFs from CFRP-laminates.
Fig. 10(b) and (c) show the failure images of CFRP-laminates pre-
pared at three parallel scanning angles (0°, 45° and 90°). CF segments
were tightly adhered to the failure surface of PC film in the vertical
direction of the groove orientation for specimens laser treated at 45°
and 90° scanning angles. However, few CF segments were observed on
Fig. 10. (a) Macro failure images of a single-lap CFRP-laminate joint. the micro failure images of grooved-CFRPs laser treated by different groove patterns: (b) 0° and
90° parallel grooves; (c) 45° parallel grooves; (d) 0/90° crossed grooves.; (e) ± 45° crossed grooves. All specimens were prepared at 200 μm groove distance, 8 times
repetition processing.
10
Composite Structures 232 (2020) 111559
the surface of failure PC films treated at 0° scanning angle. These results
indicated that the adhesive agent (PC film) of grooved-CFRP at 45° and
90° scanning angles infiltrated into CFs forming strong CF-PC bonding
connections. The bond strengths were even larger than the stripping
strengths of CFs from CFRP-laminates. However, the CF-PC bonding
strength of the grooved-CFRP at 0° scanning angle was weak. No ob-
vious heat affected zones were observed due to a weak heat transfer
coefficient in the transverse direction of CF tows; thus, no apparent CF-
PC composite was generated at groove interfaces. Additionally, CF
blocks at 0° scanning angle were continuous, which presented stronger
load resistances than discontinuous CF blocks at a 90° scanning angle.
Fig. 10(d) and (e) display the effects of the shear failure experiments
of CFRP-laminates treated at two crossed scanning angles (0/90°
and ± 45°). For these crossed grooved-CFRPs, regardless of the scan-
ning angle, numerous CF segments were stripped from grooved-CFRPs
and adhered to the bonding agent of PC film, suggesting good im-
pregnation between exposed CFs and the PC film. After introducing
crossed laser surface treatment, the as-produced crossed grooves pro-
vided efficient anchoring effects for the bonding agent. Thus, the
crossed groove patterns presented better adhesive surfaces than the
parallel groove patterns.
The mechanism for the observed enhanced shear strength of
grooved CFRP-laminate joints can be explained via a schematic diagram
as shown in Fig. 11. Two main bonding phenomena were evident for
laser treated crossed grooved-CFRP joint surfaces: physical bonding
between CFRP and the bonding agent and anchoring bonding between
the grooves and the bonding agent. The physical bonding primarily
occurred at the interface between CFRP and PC film and was enhanced
by the STEP-1 surface laser treatment. The anchoring bonding occurred
at grooves and proximal heat affected zones and was controlled by the
STEP-2 surface laser treatment. Compound bonding between exposed
CFs and bonding agent at the heat affected zone significantly enhanced
the anchoring bonding. Under the combined action of these two
bonding mechanisms, the apparently shear strengths of CFRP bonded
joints could be enhanced efficiently by the two-step laser surface
treatment.
Y. Xie, et al.
Fig. 11. Schematic diagram of shear strength enhancement of grooved-CFRP
joints.
4. Conclusions
A two-step laser surface treatment was conducted on CFRP lami-
nates using a Nd:YAG solid pulsed laser to improve the shear strengths
of bonded joints. The results are limited to the adopted laser process
parameters and the PC film in our work. Several conclusions were
made:
(1) During the STEP-1 laser processing, there was a threshold output
power for different spot distances that completely removed surface
resins of a CFRP-laminate. The threshold output power can be
calculated based on an index of continue power density. Instead of
increasing output power under a certain spot distance, a modular
laser processing method is preferred in the STEP-1 laser surface
treatment of CFRP-laminates for large areas. The spot distance of
laser surface treatments in STEP-1 should be carefully selected due
to its influence on surface morphology and joint bonding strength.
A moderate range was suggested for resin removal.
(2) Irrespectively laser scanning pattern and scanning angle selection,
in STEP-2 of laser surface treatment, a large groove distance is
preferred to acquire grooves with complete appearance and high
shear strength of its grooved-CFRP bonding joint. The groove dis-
tance should be maintained below a maximum value; otherwise, the
shear strengths of groove-CFRP joints would decline due to in-
sufficient groove area enhancement.
(3) The shear strength variation of grooved-CFRP bonding joint is the
comprehensive result of enhancement and attenuation brought by
interface grooves. The enhancements were attributed to increased
contact areas between bonded specimens and to the anchoring ef-
fects of the bonding agent. The attenuation effects were attributed
to interrupted continuity of CFs due to laser cutting and to de-
creased shear strength between microstructure layer and composite
matrix.
(4) Using optimal processing parameters, the two-step laser surface
treatment can enhance the shear strength of grooved-CFRP bonded
joints. Generally, a bonding joint with crossed grooves had better
shear strength than a bonding joint with parallel grooves and
smooth surfaces. Furthermore, 0/90° crossed grooves showed
11
Composite Structures 232 (2020) 111559
higher enhancement than ± 45° crossed grooves on grooved-CFRP
bonding joints. In this work, the optimal processing parameters
were 150 μm groove distance, 6 reprocessing times, and 0/90°
grooves. These grooved-CFRP bonded joints showed 40.8% in-
creased shear strength compared with smooth-CFRP.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgements
The current study was supported by the National Natural Science
Foundation of China (Nos. 51775197 and U1601203), and the Science
and Technology Planning Project of Guangdong Province, China (No.
2018A050506007).
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