j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

Available online at www.sciencedirect.com

journal homepage: www.elsevier.com/locate/jmrt

Original Article

Size effects on IMC growth of Cu/Ni/Sn-3.5Ag

microbump joints during isothermal aging and
prediction of shear strength using ANN

Chu Tang, Zhuo Chen*, Mingang Fang, Xiaoyu Xiao, Gui Chen,
Wenhui Zhu**
State Key Laboratory of High Performance Complex Manufacturing, College of Mechanical and Electrical Engineering,
Central South University, Changsha, China

article info abstract

Article history: Significant downsizing trend is currently directing the advanced microelectronic packaging
Received 28 October 2021 industry, which poses new challenges to the manufacturing process and reliability of high-
Accepted 17 March 2022 density chip interconnections. In this paper, to investigate the size effect of microbump
Available online 22 March 2022 joints on the interfacial structure and bonding strength, the chip-to-chip bonding joints
fabricated by microbumps of same Cu/Ni/Sn-3.5Ag construction but of various sizes were
Keywords: experimentally examined. After thermocompression bonding process to fabricate the chip-
Interfacial reactions to-chip microbump interconnections, the intermetallic compound (IMC) growth on the Ni/
Shear strength Sn-3.5Ag interface during 150
C isothermal aging was compared for joints of 100, 40 and
Size effect 25 mm in diameter as well as 35, 25 and 15 mm in solder layer height, using field emission
Intermetallics electron microscopy and electron probe microanalysis. A clear size effect on the thickness
Artificial neural network and morphology of Ni3Sn4 IMC was observed, showing thicker IMC in joints of smaller
Microbump interconnection diameter and lower height. The Ni concentration distribution in the solder layer was
verified to be dependent on the joint size, with possible reasons being enhanced sidewall
diffusion and grain boundary diffusion through IMC grains in small-diametered joints, as
well as shorter diffusion path in lower joints. The shear strength of chip-to-chip bonding
vehicles was also found to be size-dependent. In addition, artificial neural network (ANN)
approach was applied to establish the numerical correlation of structural factors and
bonding strength. It was found that a properly constructed ANN model can successfully
predict the influence of the complex combinations of geometric and interfacial factors with
highly accurate output, providing an effective tool for design and optimization of micro-
bump interconnection structures and processes.
© 2022 The Author(s). Published by Elsevier B.V. This is an open access article under the CC
BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

* Corresponding author.
** Corresponding author.
E-mail addresses: zhuochen@csu.edu.cn (Z. Chen), zhuwenhui@csu.edu.cn (W. Zhu).
https://doi.org/10.1016/j.jmrt.2022.03.110
2238-7854/© 2022 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).
1866 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
1. Introduction
Facing the urgent need to improve the performance of elec-
tronic products and chip process scaling, three-dimensional
integrated circuit (3D IC) technology, which significantly pro-
motes the off-chip Input/Output (I/O) performance by using
stacked silicon chips, has gained interests rapidly [1,2].
Microbump technology is the key for mechanical and elec-
trical connections between stacked chips. Today, the size of
micro interconnection joints for stacked chips is approaching
10 mm level [1,3]. As a consequence, the amount of solder in a
micro interconnect is very small and is prone to be fully
transformed to brittle intermetallic compounds (IMCs) during
bonding process and final product service life. Excessive
amounts of brittle IMC are thermally mismatched to the sol-
der and the substrate, predisposing the solder joint to weak-
ening and fatigue failure [4]. Industrial applications typically
use a Ni barrier layer inserted between Cu metallization and
Sn-based solder to retard the IMC growth in a joint [5].
In order to study the growth characteristics of IMC and the
method of inhibiting its overgrowth, many studies [2,6,7] have
been conducted previously to explore new Sn-based alloy
solders. The basic systems of Sn-Cu, Sn-Ag and Sn-Ag-Cu
have become the front-runners to replace Sn-Pb solders
[2,6]. Among them, the Sn-Ag solder is considered most suit-
able for the small sized and Cu pillar-based joints, since the
Sn-Ag eutectic alloy can be easily prepared through electro-
plating after the Cu pillar, and Ag was found effective in
slowing the IMC growth [7].
Many studies [8e10] have shown that solder joint size is a
sensitive factor affecting the joint strength. For relatively large
joints, the shear strength exhibited an increase followed by a
decrease when the solder joint height was reduced from 500 to
100 mm [8,9]. In addition, a study found that the strength of
solder joints continued to increase as the diameter of solder
joints decreased from 600 to 200 mm, exhibiting a size effect
[10]. Previous studies have concluded from the theoretical
analysis [11,12] and experimental combined simulation [13]
Table 1 e Size effect of the microsolder joint on shear strength and IMCs thickness.
Ref Sample size range
Qin et al. [11] 100e500 mm (height)
Li et al. [12]
Tian et al. [13] 200e600 mm (diameter)
Qin et al. [16] 300 mm (diameter), 25e100 mm (height)
Wang et al. [22] 1000 mm (diameter), 10e100 mm (height)
Zhu et al. [23] 10e50 mm (height)
Wang et al. [27] 50e2000 mm (height)
Magnien et al. [28] 50e800 mm (height)
Huang et al. [24] 200e500 mm (diameter)
Wang et al. [25] 6e11 mm (diameter)
Wong et al. [26] 40e250 mm (diameter)
a
Increase ¼ [，decrease ¼ Y, Increase first and then decrease ¼ [þY.
that the smaller the height/radius ratio (h/r) of the solder joint,
the higher the strength of the solder joint. Another factor that
has a significant impact on the strength of solder joints is the
interfacial IMC thickness. Aging [14e17] and multiple reflows
[18] increase the IMC thickness and thus reduce the strength
of the solder joint. The growth of IMC is also strongly affected
by the size of the solder joints. Reducing the solder joint height
[19,20] and solder joint diameter [21e23] leads to faster growth
of IMC. It has also been studied that Cu/SAC305 (sandwich) in
liquid thermal aging (300
C) found that the interfacial IMC
thickness decreased with decreasing solder joint height, while
solid-state thermal aging (210
C) found that the interfacial
IMC thickness increased with decreasing solder joint height
[24]. Magnien et al. [25] studied Cu/Sn3.5Ag0.75Cu thermal
aging (150
C) interface found that the IMC growth rate
decreased with decreasing solder joint height. Table 1 sum-
marizes the previously reported effects of solder joint size on
the interfacial IMC thickness and shear strength. It can be
seen that previous studies [11e13,24,26] have mainly focused
on the size effect in large size ball grid array (BGA) solder joints
or sandwich structures, and the impact of microbump joint
(100 mm) size on shear strength as well as IMC growth are not
explored deeply enough and not clear, which can only be
clarified by the side-by-side comparison of joints with
different size, under the same fabrication process and aging
condition.
Developing a physical model to accurately predict the
mechanical properties and reliability of microbump joints is
difficult because the strength of microbump joints is influ-
enced by multiple factors. Some researchers [26,27] have
attempted to develop predictive models based on experi-
mental data, but these models consider relatively few influ-
encing factors. Artificial neural network (ANN) modeling
techniques are a promising artificial intelligence tool that has
been widely used to solve various scientific problems with
classification and prediction capabilities [28,29]. ANN
modeling techniques have applications in reflow soldering
processes, the mechanical strength of solder joints and IMC
layer thickness of Sn-5Sb-xCNT/Cu composite solder joints
Joint/Reaction type Shear strength with
reduced solder joint sizea
Cu/SAC305(BGA) [þY（250
CReflow）
Cu/SAC305(BGA) [（150
CAging）
Ni/SAC305(sandwich) [（250
CReflow）
IMCs thickness with
reduced solder joint sizea
Cu/Sn(sandwich) [（260
CReflow）
Cu/Sn(sandwich) [（160
CAging）
Cu/SAC305(sandwich) Y（300
CAging）
[（210
CAging）
Cu/Sn3.5Ag0.75Cu (sandwich) Y（150
CAging）
Cu/Sn-xAg-yCu(BGA) [（250
CReflow）
Cu/Ni/Sn-3.5Ag(CPB) [（150
CAging）
Ni/Sn-3.8Ag-0.7Cu (BGA) [（150
CAging）
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
[30e32]. However, a prediction model is lacking for the me-
chanical strength of Cu/Ni/Sn-3.5Ag microbump joints of
different sizes (100 mm) after aging. Similarly, the growth
prediction model for IMC rarely considers the effect of size
pffiffiffiffiffiffi
and mainly uses the diffusion equation (x ¼ x0 þ Dt) to
calculate it [33e37].
In this paper, we experimentally characterized the IMC
layer and shear strength of isothermally aged Cu/Ni/Sn-3.5Ag
microsolder joints of same configuration but different in size.
Moreover, the Ni concentration distribution in solder joints
was measured and the growth mechanism of IMC affected by
the joint size during isothermal aging was explored. Finally, to
extend the scope of computational intelligence-based
methods for developing prediction models in engineering
applications, ANN models were successfully deployed to
predict the mechanical properties of microbump joints by
back-propagation convergence techniques. To verify the re-
sults of the developed model, confirmatory experiments were
conducted.
2. Material and methods
2.1. Materials
The test vehicles consist of top and bottom chip with Cu/Ni/
Sn-3.5Ag microbumps and daisy chain circuits for electrical
test. Figure 1 shows the design drawing of bottom chips with
different size microbumps. All chips were fabricated through
a standard bumping process patterned by photolithography,
including first lithography for Cu trace etching, second
lithography for defining the microbump area, and sequential
electroplating of Cu, Ni, and Sn-3.5Ag in the photoresist-
defined holes. The Ni barrier layer between the Cu pillar and
the Sn-3.5Ag layers was 2 mm for all chips. Table 2 shows the
Fig. 1 e Graphics of chip design pattern with different size microbumps ((a) 25 mm diameter and (b) 100 mm diameter) on the
bottom chip.
1867
geometric designs of different size Cu/Ni/Sn-3.5Ag pillar
bumps. For chips with 100 mm diameter microbumps, the Sn-
3.5Ag layers heights of both the top and bottom chips are
available in 15 and 25 mm, and the desired height of the
microbumps can be obtained by controlling the gap during the
thermocompression bonding process. The Sn-3.5Ag layer is
reflowed into a ball shape after electroplating. The thickness
of both chips is the same, 0.5 mm. For the chips containing 25
and 40 mm diameter microbumps, the Sn-3.5Ag layers height
was 15 mm for both the top and bottom chips. Figure 2(a)
shows the cross-sectional schematic of the microbump joints.
Figure 2(b) and (c) show the fabrication of 100 mm diameter Cu/
Ni/Sn-3.5Ag pillar bumps for the top and bottom chip. Sam-
ples used in this article were provided by National Center for
Advanced Packaging Co., Ltd. (NCAP China), which were
fabricated after a series of standard manufacturing processes
including but not limited to photolithography, electroplating
and etching.
2.2. Experimental setup and characterization
The chip-on-chip bonding was carried out through thermo-
compression bonding process by an Athlete CB-600 flip chip
bonding machine. Five microbump joint sizes were designed
for the test, 100 mm in diameter and 15, 25 and 35 mm in height.
25 and 40 mm diameter samples were also prepared for the
15 mm joint height, respectively. The substrate is heated to a
constant temperature of 150
C during the entire bonding pro-
cess. The bonding parameters were optimized and finally
determined to be a bonding temperature of 325
C, a bonding
pressure of 2 N, and a bonding time maintained between 6 and
10 s. The bonding time is slightly longer for samples with higher
solder joint heights. Before bonding, the microbumps on the
top and bottom chips were coated with flux. The height of the
solder joint is controlled by adjusting the compression distance
1868 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

Table 2 e Geometric designs of Cu/Ni/Sn-3.5Ag pillar bumps.

Layer Pillar structure Bump diameter (mm) Bump height (mm) Cu/Ni/Sn-3.5Ag Thickness (mm)
Bump Top chip Cu/Ni/Sn-3.5Ag 25 15 23/2/15
40 15 30/2/15
100 15 20/2/15
100 25 20/2/15
100 35 20/2/25
Bottom chip Cu/Ni/Sn-3.5Ag 25 15 8/2/15
40 15 8/2/15
100 15 15/2/15
100 25 15/2/25
100 35 15/2/25

Fig. 2 e Schematic diagram (a) SEM micrographs, (b) top chip, (c) bottom chip of Cu/Ni/Sn pillar bumps.

of the welding head during the thermocompression bonding.
After bonding, isothermal aging tests were performed in a non-
vacuum oven at 150
C for 0, 100, 200 and 400 h. Die shear tests
were performed using a global bond test (Dage 4000). As shown
in Fig. 3, the conditions for the low-speed shear test included a
height of 30 mm and a shear rate of 0.1 mm/s. The shear test was
performed at least three times and the strength values were
averaged. The specimens were fixed with epoxy after bonding
and then sequentially ground to the maximum cross-section of
the microbump joints with 200, 800, 2500 and 4000 # SiC
sandpaper, and then polished with Al2O3 suspension and SiO2
suspension. Finally, sample cross-sections and fracture sur-
faces were analyzed by field emission electron microscopy (FE-
SEM) and energy dispersive X-ray spectrometry (EDS) attached
to the microscope. The concentration distribution of Ni atoms
at different locations in the solder layer was scanned by Elec-
tron probe microanalysis (EPMA) after 400 h of isothermal aging
tests. The concentration values were obtained by averaging
four data points around the measurement locations. The Ni
concentration variation curves were also plotted for micro-
bump joints of different sizes. The image processing software
Photoshop was also used to measure the IMC thickness. The
average thickness of IMC can be obtained by dividing the total
area of IMC by the length of the observed area.
2.3. Artificial neural network (ANN) modelling
ANN is a nonlinear statistical data modeling tool that is well
suited to solve nonlinear stochastic problems. In solving com-
plex problems, researchers value its ability to learn and
generalize reasonable outputs to new inputs that are not
encountered during training [38]. They did this by constructing
input, hidden, and output layers, which were interconnected by
neurons, and by learning and adopting information from the
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5 1869

Fig. 3 e Schematic diagram of the die shear test.

examples. Seventy percent of the sample parameters are used N 

P 2
to train the neural network, and the other 30 percent of the data yipre  yitag
are separated out and used to test and validate the developed R2 ¼ 1  i¼1N  2 (1)
P i
model. In this way, we take care to cover the entire range of ypre  y
i¼1
experiments to develop and test the neural network models.
The ANN model developed in this work uses the Levenberg vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
uN  2
uP i
u
ti¼1 ypre  ytag
Marquardt back-propagation (LMBP) algorithm as the training i

algorithm because it is robust and has the fastest convergence
rate relative to other training algorithms, which is essential for
effective training [39e41]. Previous studies [42,43] have pro-
posed many methods to explore the optimal number of hidden
layers and neurons, but they are not applicable to all research
subjects. In this paper, a supervised trial-and-error method was
used to find that two hidden layers gave the best predictions.
Therefore, the ANN model in this paper determines the number
of hidden layers is two, thus further exploring the optimal
number of neurons. In addition, the network performance and
the degree of fit of the various ANN topologies studied in this
work were analyzed by using two statistical parameters, the
coefficient of determination (R2) and root mean square error
(RMSE) [30,43].
RMSE ¼ (2)
N
where yipre is the predicted output, yitag is the experimental
(target) output, y is the average of the experimental output
and N is the total number of data observation.
3. Results and discussion
3.1. IMC morphological analysis and growth kinetics
Figure 4 shows SEM micrographs of the fracture surfaces, Figs.
5e7 show the cross-sectional microstructure of Cu/Ni/Sn-
3.5Ag sample after isothermal aging at 150
C. As shown in

Fig. 4 e SEM micrographs of the fracture surfaces of 100 mm diameter samples after isothermal aging at 150
C for (a), (e) 0 h,
(b), (f) 100 h, (c), (g) 200 h, (d), (h) 400 h (h ¼ 15).
1870 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
Fig. 5 e Cross-sectional microstructure of Cu/Ni/Sn-3.5Ag sample after isothermal aging at 150
C for (a), (a1) 0 h, (b), (b1)
100 h, (c), (c1) 200 h, (d), (d1) 400 h (d ¼ 100 mm, h ¼ 15 mm).
Figs. 4(e) and 5(a1), a thin layer of scallop-shaped IMC with a
thickness of about 0.72 mm grew at the Ni/Sn-3.5Ag interface
after bonding for a microbump joint of 100 mm diameter and
15 mm height. The EDS analysis showed that the IMC was
Ni3Sn4. Some Ag3Sn particles were also found to precipitate in
the solder near the IMC. When the specimen was isothermally
aged at 150
C, the Ni3Sn4 IMC grew symmetrically at the
upper and lower interfaces of the microbump joints (Fig. 5(b)).
With increasing aging time, the morphology of Ni3Sn4 IMC
changes from scallop type to layer type. The subsequent
microbump joints fracture morphology analysis depict the
growth process of IMC grains with aging time. After aging for
400 h, the thickness of Ni3Sn4 is 2.63 mm, which is 1.91 mm
higher than the original thickness. The Ag3Sn particles were
observed attached to the Ni3Sn4 surface, which was preferred
site for the heterogeneous nucleation Ag3Sn [44]. The IMC
growth in each type of microbump joints was slowing down
with increasing aging time, as shown in Figs. 6 and 7.
Magnien et al. [25] and Kim et al. [45], while studying the
morphology of Cu/Sn-Ag-Cu/Cu microbump joints of different
sizes after isothermal aging, found that the gradual coarsening
of b-Sn grains and Ag3Sn particles was observed with
increasing solder gap size (volume), due to slower cooling rate
in joints with larger solder volume. Figures 8 and 9 show cross-
sectional microstructure of Cu/Ni/Sn-3.5Ag sample after
isothermal aging at 150
C, Figs. 10 and 11 show SEM micro-
graphs of the fracture surfaces. As shown in Figs. 8(a1) and
10(e), the microbump joints shrink from 100 to 40 mm, and
after thermocompression bonding, a thin needle-like IMC layer
is formed at the Ni/Sn-3.5Ag interface, which is more slender
than 100 mm in diameter, with a layer thickness of about
0.75 mm. This may be due to the fact that smaller diameter
microbump joints dissipate heat more quickly during the
cooling phase of thermocompression bonded joints, with
greater subcooling and easier IMC nucleation, resulting in the
formation of more and finer grains. After 100 h aging, the
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
Fig. 6 e Cross-sectional microstructure of Cu/Ni/Sn-3.5Ag sample after isothermal aging at 150
C for (a), (a1) 0 h, (b), (b1)
100 h, (c), (c1) 200 h, (d), (d1) 400 h (d ¼ 100 mm, h ¼ 25 mm).
spaces between the needle-like IMCs are filled by the repreci-
pitated IMCs, causing the IMCs to grow from needle-like to
shell-like. After aging for 200 h, Ni, Sn atoms diffusing through
the IMC layers become less easy, the growth rate slows down,
and the shell-like IMC becomes a flatter layer. The thickness of
Ni3Sn4 is 2.47 mm, which is 1.72 mm higher than the original
thickness. This phenomenon is also seen in 25 mm diameter
microbump joints, as shown in Figs. 9(b) and 11(e). Figure 12
shows a plot of IMC thickness versus aging time for micro-
bump interfaces with diameters of 25, 40 and 100 mm.
Furthermore, the small Ag3Sn grains were observed after
bonding and had the effect of pinning at the IMC/Sn interface
[46] and filling the voids [47], thus increasing the solder joint
shear strength. However, finely dispersed Ag3Sn particles
agglomerated into a few large grains during aging, as shown in
Figs. 7 and 8. As the aging time increases, the pits in the
microbump joint sections are becoming less and deeper, and
the Ni3Sn4 grains are becoming coarser. Also, some of the
1871
adjacent Ni3Sn4 grains have formed holes between them due
to growth shrinkage, which is one of the reasons for the
reduced strength of the microbump joints, as shown in Figs.
4(g), (h), 10(g) and 10(h) [48,49].
Size effects play a role in aging and reflowing microbump
joints [21,46,50]. We found that the IMC thicknesses of the aged
microbump joints were also significantly different for different
sizes. After isothermal aging at 150
C, the IMC thickness of the
microbump joints increases with the reduction of the joint size,
as shown in Fig. 12. Among the microbump joints with a
diameter of 100 mm, the thickness of the IMC is 1.40 mm for the
microbump joints with a height of 35 mm aged for 100 h. The
IMC thickness of the 25 mm height microbump joints is 1.60 mm,
which is 14.3% higher than that of the 35 mm height microbump
joints. When the height of the microbump joints is further
reduced to 15 mm, the thickness of the IMC is 1.76 mm, which is
10% higher than that of the microbump joints with a height of
25 mm. When the height of the microbump joints is constant
1872 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
Fig. 7 e Cross-sectional microstructure of Cu/Ni/Sn-3.5Ag sample after isothermal aging at 150
C for (a), (a1) 0 h, (b), (b1)
100 h, (c), (c1) 200 h, (d), (d1) 400 h (d ¼ 100 mm, h ¼ 35 mm).
and the diameter of the microbump joints is reduced, the IMC
thickness of the microbump joints is increasing. For a micro-
bump joints with a diameter of 25 mm, the thickness of the IMC
after 100 h aging is 1.87 mm, which is 6.3% higher than that of a
100 mm diameter. This shows that the size effect has a greater
influence on the height direction of the microbump joints than
in the diameter direction. A similar effect is manifested
throughout the aging process.
He et al. [36] and Alam et al. [37], while studying the growth
kinetics of Ni3Sn4 in BGA microbump joints at the Sn-3.5Ag
solder/Ni interface, found that the initial growth of Ni3Sn4 is
greatly affected by the grain boundary diffusion, but after the
aging time increases, the grains become coarser and the
number of grain boundaries decreases, so the volume diffu-
sion gradually becomes dominant. Therefore, in order to
study the kinetics of the interfacial reaction layer growth with
time at a particular temperature, it is appropriate to use the
following empirical power law relationship.
pffiffiffiffiffiffi
x ¼ x0 þ Dt (3)
where x is the total thickness of the reaction layer at time t and
x0 is the initial thickness, d is the growth rate constant. The
value of D at a specific temperature can be obtained by
multivariate linear regression analysis.
As seen in Fig. 13, the linear slope is the square root of the
growth rate constant D (h is the solder height and d is the
microbump diameter). The growth constants for different size
microbump joints ranged from 0.0066 to 0.0132, showing a size
effect. The growth rate of IMCs increases with decreasing
height in microbump joints of 100 mm diameter with heights of
15, 25 and 35 mm. The equations for the growth of IMC thick-
ness for different solder heights in a 100 mm diameter micro-
bump are given in (6), (7) and (8).
Figure 13 also shows that the interfacial response increases
and the growth constant D of IMC increases as the diameter of
Cu/Ni/Sn-3.5Ag microbump decreases from 100 to 40 and then
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5 1873

Fig. 8 e Cross-sectional microstructure of Cu/Ni/Sn-3.5Ag sample after isothermal aging at 150
C for (a), (a1) 0 h, (b), (b1)
100 h, (c), (c1) 200 h, (d), (d1) 400 h (d ¼ 40 mm, h ¼ 15 mm).

to 25 mm in the isothermal aging test. The growth of IMC is 3.2. Ni concentration distribution in microbump joints
promoted by the increased grain boundary diffusion due to
the finer initial grain size of 25 mm diameter microbump joints To further clarify the direct cause of size effect on the IMC
during thermocompression bonding. The equations for the growth, the elemental concentration distribution in the
growth of IMC thickness in 25 mm diameter and 40 mm diam- microbump joints was analyzed. As shown in Fig. 14(a), Cu/Ni/
eter microbump are given in (4), (5). Sn-3.5Ag microbump joints (d ¼ 25 mm) formed a very thick
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi IMC layer at the Ni/Sn-3.5Ag interface. As indicated in
x1 ¼ 0:76 þ 0:0132t (4) Fig. 14(b), EPMA analysis shows that the Ni atom concentra-
tion in the solder gradually decreases from the IMC/Sn inter-
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
x2 ¼ 0:75 þ 0:0121t (5) face to the middle of the solder.
As illustrated in Fig. 15, the Ni atom concentration de-
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
x3 ¼ 0:72 þ 0:0104t (6) creases with increasing microbump joints height in micro-
bump joints of 100 mm diameter with three values of
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 0.907 ± 0.12, 0.510 ± 0.06, and 0.419 ± 0.08 wt.%, respectively.
x4 ¼ 0:67 þ 0:0089t (7)
This result is consistent with of Dybkov's diffusion kinetic
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi model: the lower the solder joint height, the faster the Ni
x5 ¼ 0:54 þ 0:0066t (8) barrier dissolves and the higher the Ni concentration in the Sn
1874 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

Fig. 9 e Cross-sectional microstructure of Cu/Ni/Sn-3.5Ag sample after isothermal aging at 150
C for (a), (b) 0 h, (c), (d) 100 h,
(e), (f) 200 h, (g), (h) 400 h (d ¼ 25 mm, h ¼ 15 mm).
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5 1875

Fig. 10 e SEM micrographs of the fracture surfaces of 40 mm diameter samples after isothermal aging at 150
C for (a), (e) 0 h,
(b), (f) 100 h, (c), (g) 200 h, (d), (h) 400 h (h ¼ 15).

Fig. 11 e SEM micrographs of the fracture surfaces of 25 mm diameter samples after isothermal aging at 150
C for (a), (e) 0 h,
(b), (f) 100 h, (c), (g) 200 h, (d), (h) 400 h (h ¼ 15).

solder [51]. Furthermore, when the height of the microbump
joints was kept constant and the diameter was reduced to 40
and 25 mm, we found that the average Ni concentration
increased from 0.907 ± 0.12 to 1.008 ± 0.18 and
1.060 ± 0.15 wt.%, respectively. It can be deduced that the high
Ni atom concentration in smaller sized microbump joints has
a positive effect on the oversaturation of Ni in the Sn solder.
Figure 16 depicts the effect of diffusion on Ni atoms in
microbump joints of different sizes. The smaller the size of the
microbump joints, the higher the concentration of Ni atoms.
To explain the Ni atom concentration distribution in different
size microbump joints, we suspected that on one hand, as the
aging time increases, the IMC thickens, so that the volume
diffusion path and the time required for Ni atoms to diffuse
through the IMC layer increases. Meanwhile, Ni atoms could
also diffuse from the sidewall surface through the surface
diffusion, bypass the volume diffusion path in IMC and diffuse
into the solder layer from the side to react with Sn, which has
1876 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

become an important driving force for the growth of IMC [52].

This proportion of surface diffusion increases when the
microbump joints diameter is reduced, so promoting the
growth of IMC [22]. On the other hand, as shown in Figs. 4(e)
and 11(e), during bonding, the smaller diameter microbump
joints dissipate heat faster and have higher subcooling, so
more IMC nucleation and finer IMC grains are produced. The
fine IMC grains increase the grain boundary diffusion of Ni
atoms, which enhances the Ni atom concentration in the
solder and promotes IMC growth. The grain boundary diffu-
sion is faster than the bulk diffusion and the IMC usually
grows along the grain boundary [33,53,54]. Another possible
reason is the thermal gradient as an additional driving force of
diffusion, or generally known as thermomigration, which is
higher in small diameter microbump joints [23]. Similarly, for
low height microbump joints, on the one hand, the low vol-
ume of solder and the fast heat dissipation during the ther-
Fig. 12 e Variation of average thickness of Ni3Sn4 IMC as a mocompression bonding promote solideliquid diffusion [20].
function of time. On the other hand Ni atoms have reduced diffusion paths and
tend to aggregate at the IMC/Sn-3.5Ag interface, both
increasing the Ni atom concentration and accelerating the
IMC generation.
During the aging process, the Ni barrier layer inhibits the
interdiffusion of Cu and Sn atoms significantly. The compo-
sition of the solder joints after isothermal aging at 150
C for 0,
100, 200 and 400 h was analyzed by EDS line scan. According to
Fig. 17, the Ni barrier layer thins with increasing aging time
but is always present. Meanwhile, as shown in Fig. 18, the EDS
element mapping of the microbump joints after isothermal
aging for 400 h shows that the Ni barrier layer remains
continuous and is not depleted or penetrated. In addition, an
EDS analysis of the specific composition of the IMC was per-
formed. The atomic ratios of the different compositions show
that the IMC is (NixCu1-x)3Sn4, as shown in Table 3. The con-
tent of Cu atoms in the IMC was 6.31 at.% after bonding and
increased to 9.10 at.% after 100 h of aging. The Ag content was
less than 0.1 at.% and was not included in the statistics.
Fig. 13 e Variation in the IMC thickness with the square Therefore, the strength of microbump joints in this paper is
root of the aging time. mainly influenced by the Ni3Sn4-structured IMC.

Fig. 14 e (a) Cross-section SEM images of the Cu/Ni/Sn-3.5Ag layers joint after aging 400 h and (b) concentration gradient of
Ni between the solder layers.
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
Fig. 15 e Relationship between the concentration of Ni and
different size of bumps after aging 400 h.
3.3. Shear strength analysis
Figure 19 shows the shear strength of thermocompression
bonded and aged microbump joints of different sizes studied
in this paper. When the microbump joints size decreases in
the height dimension, it shows a size effect, an increase in
shear strength. When decreasing the diameter dimension, the
shear strength decreases. The shear strength of a 100 mm
diameter microbump joints with a height of 15 mm after
bonding is 71.3 MPa, which is about 1.82 times higher than
that with a height of 25 mm, 39.2 MPa. The shear strengths of
Fig. 16 e Size effect of microsolder joints on Ni diffusion for (a) d¼ 100 mm, h ¼ 35 mm, (b) d ¼ 100 mm, h ¼ 25 mm, (c) d ¼ 100
mm, h ¼ 15 mm, (d) d ¼ 40 mm, h ¼ 15 mm, (e) d ¼ 25 mm, h ¼ 15 mm.
1877
height 25 and 35 mm are close, larger than that with a height of
35 mm by 5.8 Mpa.
After 100 hours of aging, the strength of all microbump
joints decreased significantly. In the microbump joints with a
diameter of 100 mm, the shear strength of the joint with a
height of 15 mm dropped from 71.3 to 42.0 Mpa, and the shear
strength loss was 41.1%. The shear strength of microbump
joints of different sizes has a similar trend after aging. How-
ever, after 400 hours of aging, only the 100 mm diameter
microbump joints with a height of 15 mm have the largest
decrease in strength, 15.2 Mpa.
It can also be seen from Fig. 19 that when the microbump
joints height remains unchanged and the diameter is reduced
from 100 to 25 mm, the strength of the microbump joints after
bonding decreased from 71.3 to 26.0 Mpa, 63.5% shear strength
loss. After aging 400 h, the 25 mm diameter microbump joints
strength was slowly decreased to 22.8 MPa. It is close to the
strength (25.7 Mpa) of the microbump joints with a diameter
of 100 mm, both at a lower level.
Many previous studies [8,12,13] have shown that the solder
volume/substrate area ratio (V/A) or the microbump joints
height/substrate radius ratio (h/r) has a significant effect on
the interfacial IMC growth and microbump joints strength.
Wong et al. [23] found that the solder ball strength decreases
with decreasing pad diameter in the push ball test of Cu/Ni/
SAC solder balls. It is generally believed that the thinner the
microbump joints are during aging, the faster the IMC growth
and the faster the microbump joint's strength decreases. In
this paper, the experimental analysis concluded that the ge-
ometry of the microbump joints plays a dominant role in the
strength of the microbump joints after bonding. The h/r value
1878 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

Fig. 17 e (a), (c), (e) and (g) show SEM images of the Cu/Ni/Sn-3.5Ag interfaces, respectively; (b), (d), (f) and (h) show line-scan
results of elemental compositions at the Cu/Ni/Sn-3.5Ag interfaces, respectively.(d ¼ 40 mm, h ¼ 15 mm).
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5 1879

Fig. 18 e Element Mapping of Solder Joint after isothermal aging at 150
C for 400 h: Electron back scattered diffraction (BSE)
image(a) and EDS mappings of Ni(b), Cu(c), Sn(d) and mixed elements distributions (e).(d ¼ 40 mm, h ¼ 15 mm).

is smaller the higher the strength. However, after isothermal ductileebrittle combination, while in the others fractures all
aging at 150
C, the IMC increases linearly with the 0.5 th occurred in the soldered region and had dimple structures at
power of time. After aging for 100 h, the thickness of IMC the fracture site, indicating ductile fracture characteristics.
increased by about 1 mm for different sizes of microbump After 100 h of aging, in the 100 mm diameter joints, with the
joints. The weakening effect of IMC on the strength of height decreasing from 35 to 25 and then to 15 mm, the pits
microbump joints is obvious. The shear strength of the containing Ni3Sn4 particles are increasing, the fracture form is
microbump joints still shows a size effect. However, after ductileebrittle combination, but the brittle fracture constituent
400 h of aging, the average increase in the thickness of IMC of increases with the decrease of the height of the microbump
different sizes of joints was 1.89 mm. At this time, the weak-
ening of IMC on shear strength dominated, and the strength of
different sizes of joints was reduced to about 26.1 MPa. The
size effect of the shear strength of the microbump joints is not
obvious anymore.
To investigate the relationship between the shear fracture
pattern and the shear strength of the microbump joints, the
fracture morphology of the samples was observed by SEM, as
shown in Figs. 4, 20 and 21. After bonding, the fracture form of
the sample with 100 mm diameter and 15 mm height was a

Table 3 e Compositions of the IMCs marked by the red

box in Fig. 17 (d ¼ 40 mm，h ¼ 15 mm).
Aging Sn Ni Cu IMC type
time (h) (at.%) (at.%) (at.%)
0 54.77 38.92 6.31 (Ni0.86,Cu0.14)3Sn4
100 54.20 36.70 9.10 (Ni0.80,Cu0.20)3Sn4
200 53.74 36.96 9.30 (Ni0.80,Cu0.20)3Sn4 Fig. 19 e Shear strengths of the Cu/Ni/Sn-3.5Ag
400 55.79 34.79 9.42 (Ni0.79,Cu0.21)3Sn4
microbumps as functions of the aging time.
1880 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

Fig. 20 e SEM micrographs of the fracture surfaces of 100 mm diameter samples after isothermal aging at 150
C for (a), (e) 0 h,
(b), (f) 100 h, (c), (g) 200 h, (d), (h) 400 h (h ¼ 25).

Fig. 21 e SEM micrographs of the fracture surfaces of 100 mm diameter samples after isothermal aging at 150
C for (a), (e) 0 h,
(b), (f) 100 h, (c), (g) 200 h, (d), (h) 400 h (h ¼ 35).

joints. After aging for 200 and 400 h, the fracture form of
microbump with a diameter of 100 mm and a height of 25 and
35 mm is still a ductileebrittle combination, but the brittle
fracture component is increasing with time. The number of pits
on their fracture surfaces is increasing and the Ni3Sn4 particles
at the bottom of the pits are becoming thicker. This all causes
the strength of the microbump joints to decrease as well. For a
microbump with a diameter of 100 mm and a height of 15 mm,
after the aging time was increased from 200 to 400 h, almost
only dense Ni3Sn4 particles remained on the fracture surface.
The fractured form changes from a ductileebrittle combination
to a nearly complete brittle fracture, with the strength of the
microbump joints dropping to 1/5 of that after bonding.
An interesting phenomenon can also be found in the
fracture morphology. The Ni3Sn4 grains located in the frac-
ture surface of microbump joints follow a growth pattern of
fine grains growth after bonding (Fig. 4(e)), and coarsening
after aging for 100 h (Fig. 4(f)). The Ni3Sn4 grains grew into
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5 1881

Table 4 e Shear strength of samples.

Factors Shear strength (Mpa)
Solder diameter (mm) Solder height (mm) IMC thickness (mm) Trial1 Trial2 Trial3
25 15 0.76 25.0 26.2 26.8
25 15 1.87 24.4 25.6 25.9
25 15 2.61 25.5 25.8 22.8
25 15 2.91 22.1 24.3 22.0
40 15 0.75 42.6 41.0 42.7
40 15 1.82 36.6 39.6 36.3
40 15 2.47 36.2 32.4 34.3
40 15 2.85 25.3 24.4 27.4
100 15 0.72 70.3 73.1 70.5
100 15 1.76 42.8 42.4 40.8
100 15 2.32 36.9 37.0 34.7
100 15 2.63 25.1 28.4 26.9
100 25 0.67 38.7 38.6 40.3
100 25 1.6 32.7 29.6 32.2
100 25 2.14 28.3 30.7 30.7
100 25 2.47 28.7 28.6 27.3
100 35 0.54 32.2 33.8 34.2
100 35 1.4 31.8 30.9 27.9
100 35 1.8 30.6 27.5 29.2
100 35 2.07 28.8 27.4 25.9

relatively independent large grains after aging for 200 h are expected to solve this problem with the help of artificial
(Fig. 4(g)). After aging continued to 400 h, small grains of neural network models.
Ni3Sn4 grew on the independent Ni3Sn4 large grains (Fig. 4(h)) 60 sets of experiments were done to maximize the effect of
and grew toward the adjacent grains until fusion. In addition, input factors on the shear strength of Cu/Ni/Sn-3.5Ag micro-
three states of grain growth are found in Fig. 4(h); the first one bump joints by varying the geometry of the microbump joints
is that the small grains on adjacent large grains grow toward and the IMC thickness. The experimental results are shown in
each other (red arrow a, b); the second one is that the small Table 4. In this study, an artificial neural network model with
grains on adjacent large grains have grown together and microbump joints height, diameter and IMC thickness as
formed a “bridge” (red arrow c); the third one is that the input parameters and shear strength as the characterization
adjacent grains have fused together and grown into larger result was developed. The optimal structure was determined
particles (red arrow d). by using several ANN topologies to train the network and by
As shown in Fig. 10, for a microbump with a diameter of adjusting the number of neurons in the two hidden layers.
40 mm and a height of 15 mm after bonding, most of the fracture Table 5 lists the ANN topologies (hidden neuron structures)
surface is Sn-3.5Ag solder, with a few long pits having tiny used to develop the ANN models and their respective network
particles, which are still mainly ductile fractures at this time. performance. Figure 22 shows a visual representation of the
As the aging time increases, the fracture appears as a pit developed model. Approximately 9 independent ANN topol-
containing Ni3Sn4 particles, and the Ni3Sn4 particles become ogies were systematically examined by varying the number of
bigger with increasing aging time. The form of fracture is a neurons in the hidden layer in the range of 2e16. As can be
ductileebrittle combination, and the shear strength decreases seen from the group of “*” markers in Table 5, 16-4 (20
continuously as a result. In general, 40 mm diameter micro-
bump joints have lower shear strength than 100 mm diameter
joints due to the smaller volume of the solder. A similar Table 5 e Summary of ANN topologies used in the
pattern occurs in microbump joints with a diameter of 25 mm, development of the ANN model.
as illustrated in Fig. 11. The only difference is that the IMC Hidden Training Validation Test
particles are coarser in the fracture at the same aging time, neurons 2 2 2
R RMSE R RMSE R RMSE
and the shear strength is diminished even more.
2e2 0.9036 0.1241 0.6790 0.1364 0.9312 0.1473
4e2 0.9901 0.0469 0.9247 0.0632 0.8470 0.0774
3.4. ANN model development for shear strength 4e4 0.9892 0.0436 0.9868 0.0608 0.9229 0.0812
5e5 0.9790 0.0583 0.8977 0.0592 0.9778 0.0938
Through the above example, we found that the specific 8e2 0.9830 0.0608 0.9651 0.0539 0.6598 0.1334
structure of the microbump joints determines the growth of 8e4 0.9849 0.0735 0.8977 0.0714 0.9853 0.0917
16e4a 0.9843 0.0424 0.9919 0.0583 0.9903 0.0721
IMC. The IMC growth and microbump joints structure
12e10 0.9888 0.0520 0.9698 0.0624 0.8475 0.1015
together determine the shear strength of the microbump
16e8 0.9883 0.0436 0.9632 0.1204 0.9408 0.0837
joints. Therefore, there are too many factors that affect the
a
Optimum model on the basis of the training, validation and test
shear strength of microbump joints, so that it is difficult for us
data.
to decouple them into a series of single factors. In this case, we
1882 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5

Fig. 22 e Schematic of artificial neural network (ANN) layers.

neurons) is clearly the best structure for the hidden layer due
to the largest correlation coefficient R2 and the smallest root
mean square error RMSE value. Therefore, the 3-16-4-1 com-
bination is the optimal ANN structure for predicting shear
strength. The activation functions used for convergence are
the hyperbolic tangent “tansig” in the hidden layer and the
linear transfer function “purelin” in the output layer. The
training performance curve of the neural network is shown in
Fig. 23, and convergence to the mean square error of
3.4233  103 is achieved in 7 iterations or epochs. Figure 24
shows a comparative plot of the experimental and predicted
values of the shear strength of Cu/Ni/Sn-3.5Ag microbump
joints.
It can be seen from the figure that the developed ANN
model performs satisfactorily by using the model with the
best ANN topology to obtain a good fit between the predicted
results and the experimental results. The overall correlation
coefficient R2 between the predicted and measured values is
0.99266, indicating a significant correlation with the actual
values. This finding is very different in the field of microbump
joints interconnection and reliability than previous studies
[30,31] on bonding process on microbump joints reliability

Fig. 23 e MSE convergence during training of the ANN model 3-16-4-1 for the shear strength.
 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
Fig. 24 e Comparison of the ANN model simulation results with the experimental results for shear strength.
prediction and can fill the blanks of microbump joints size and
IMC thickness on microbump joints strength prediction very
well. This shear strength prediction model integrates the
microbump structure, especially the IMC thickness. It results
in a more accurate prediction of the strength of microbump
joints and a wider adaptation to the situation. It is possible to
adequately control the selection of dimensions (microbump
joints height and diameter), optimize the service parameters
(isothermal aging time and IMC thickness), and predict the
shear strength of Cu/Ni/Sn-3.5Ag microbump joints with
small errors.
4. Conclusion
In this study, the intermetallic compound growth in Cu/Ni/Sn-
3.5Ag microbump joints of different diameters from 100 to
25 mm, and solder layer heights from 35 to 15 mm, was sys-
tematically investigated under isothermal aging condition to
1883
reveal the size effect on the interfacial Ni3Sn4 IMC growth
kinetics and the resulting chip-to-chip bonding strength. It
was found that the IMC morphology and thickness were
dependent on the joint size, joints with smaller diameter and
solder layer height produced thicker Ni3Sn4, as well as a
transition from scallop shape to needle-like shape of Ni3Sn4
was observed when downsizing the microbump joint from 100
to 25 mm. EPMA analyses showed the Ni concentration distri-
bution in the Sn-3.5Ag solder matrix was indeed higher in
smaller or lower joints. A phenomenon directly linked to the
higher diffusion coefficient and enhanced IMC growth, due to
the reason of increased proportion of sidewall Ni diffusion and
higher IMC grain boundary density, as well as shorter diffu-
sion path. The die shear strength was also size-dependent,
joints with larger diameter and thinner solder layer showed
higher strength. To deal with the complex influence of various
factors including the joint diameter, height and IMC thick-
ness, an artificial neural network model with a 3-16-4-1 layer
structure was applied to generate accurate predictions on the
1884 j o u r n a l o f m a t e r i a l s r e s e a r c h a n d t e c h n o l o g y 2 0 2 2 ; 1 8 : 1 8 6 5 e1 8 8 5
bonding strength of chip-to-chip bonding samples, providing
a practical tool for the design and optimization of joint
structure with highly complex factor combinations.
CRediT authorship contribution statement
Chu Tang: Data curation, Writing - original draft. Zhuo Chen:
Methodology, Writing-review and editing, Supervision. Min-
gang Fang: Investigation, Validation. Xiaoyu Xiao: Methodol-
ogy, Investigation. Gui Chen: Methodology, Investigation.
Wenhui Zhu: Conceptualization, Methodology.
Declaration of Competing Interest
The authors declare there are no conflict of interest.
Acknowledgments
This work is supported by National Natural Science Founda-
tion of China (Grant No. U20A6004), the Fundamental
Research Funds for the Central Universities of Central South
University, China, (Grant 2021zzts0144), Natural Science
Foundation of Hunan Province (Grant No. 2021JJ40734), State
Key Laboratory of High Performance Complex Manufacturing
(Grant No. ZZYJKT2020-08), the Innovation-Driven Project of
CSU (Grant No. 2020CX005). Key Project of Science and Tech-
nology of Changsha (kq2102005).
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