INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 15, No. 1, pp.

105-110 JANUARY 2014 / 105

DOI: 10.1007/s12541-013-0311-8

Coefficient of Thermal Expansion Measurements for

Freestanding Nanocrystalline Ultra-Thin Gold Films

Alexander Elceario Mag-isa1, Bongkyun Jang2, Jae-Hyun Kim2, Hak-Joo Lee2, and Chung-Seog Oh3,#
1 Department of Mechanical Engineering, Kumoh National Institute of Technology, 61, Daehak-ro, Gumi, Gyeongbuk, South Korea, 730-701
2 Department of Nanomechanics, Korea Institute of Machinery and Materials, 156, Gajeongbuk-ro, Yuseong-gu, Daejeon, South Korea, 305-343
3 Department of Mechanical System Engineering, Kumoh National Institute of Technology, 61, Daehak-ro, Gumi, Gyeongbuk, South Korea, 730-701
# Corresponding Author / E-mail: ocs@kumoh.ac.kr, TEL: +82-54-478-7323, FAX: +82-54-478-7319

KEYWORDS: Coefficient of thermal expansion, Freestanding, Gold film, Grain size, Nanocrystalline, Thermal bulge method

The out-of-plane coefficient of thermal expansion (CTE) measurement method, which is named the thermal bulge method, was used
to measure the linear CTE values for freestanding nanocrystalline ultra-thin gold films with thicknesses ranging from 115 to 1200
nm. White light interferometry was used to determine the out-of-plane thermal deformation as a function of temperature. The thermal
strain showed a linear behavior in the temperature range of 20 to 100oC, but varied with the thickness (or grain size) of the specimen.
The grain sizes, which were measured by transmission electron microscopy (TEM), showed a strong correlation with the CTE:
Specimens with larger grain sizes (44 to 98 nm) had greater CTE values (9.6 to 13.6 ppm/oC). Starting from the CTE values for fine-
grained materials, the CTE of nanocrystalline gold films increased with increasing grain size and approached the CTE of bulk gold.
The thermal bulge method, which was previously developed by the authors, allowed for direct, repetitive, reliable, and quick
measurement of the CTE values of ultra-thin gold films.

Manuscript received: September 15, 2013 / Accepted: November 22, 2013

electrical conductivity and chemical inertness. However, the films must

NOMENCLATURE
become progressively smaller and thinner to keep pace with
miniaturization and integration.
d = average grain size Most solid materials expand and contract upon heating and cooling,
t = average film thickness respectively. Thermal deformation can induce thermal stresses and
T = temperature warpage in multi-layered devices or components.4,5 The temperature-
αav = average linear CTE of a film dependent deformation or stress of a device can be characterized and
αBulk = CTE of bulk material predicted via the coefficient of thermal expansion (CTE). To fully
αS = CTE of substrate account for the contribution or effect of thermal expansion on device
αtrue = true CTE of a film operation and performance, the CTE should be accurately measured
based on the material, size, and fabrication process used to manufacture
the devices.
In general, theoretical studies6 agree that, starting from the values
1. Introduction for coarse-grained materials, the CTE values of nanocrystalline materials
increase with decreasing crystallite size (i.e., increasing volume fraction
Thin solid films are used in many types of engineering systems and of grain boundaries). However, diverse and contradictory results have
have been adapted to fulfill a wide variety of functions.1 In particular, been obtained in experimental studies.7 Several factors affect the CTE
they are commonly applied in metallization and as interconnects in the measurements for thin films and become increasingly prevalent for
semiconductor industry2 and as structural elements in micro electro ultra-thin films. The substrate is one of the key factors that hinder
mechanical system (MEMS) devices.3 Gold thin films are undoubtedly accurate CTE measurements. Residual stresses are inherently formed
one of the most frequently used materials because they have excellent during deposition at high temperatures due to the mismatch in the CTE

© KSPE and Springer 2014

 106 / JANUARY 2014 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 15, No. 1

values of the film and substrate. The residual stresses and their variation
with temperature significantly affect the measurement results.8 In
addition, the Young’s moduli and Poisson’s ratios of the constituent
layers must be known to calculate the CTE of a film using Stoney’s
equation.9 Furthermore, accurate determinations of the elastic constants
are challenging. Thus, an accurate and direct CTE measurement method
is needed to alleviate these problems.
Recently, an out-of-plane linear CTE measurement method, which
is named the thermal bulge method (TBM),10 was developed after a
review of many state-of-the-art techniques. The TBM that incorporates
a zero-CTE or known-CTE substrate has proven to be a convenient and
straightforward method that can be applied to freestanding thin films
with thicknesses greater than 500 nm. The effect of residual stresses
can be completely excluded by using a freestanding film instead of a
constrained one. In addition, this method does not require any material
properties to obtain the CTE of the target film. Fig. 1 (a) (100) Si die (top) holding 6 freestanding Au specimens (224
In this work, we applied the TBM to measure the linear CTE of nm thick and 20 µm wide) and a magnification (bottom); (b) transferred
nanocrystalline ultra-thin gold films varying in thickness from 115 to specimen onto the Zerodur® substrate (top) having a gap of 500 µm
1200 nm and investigated the effect of the thickness (or grain size) on and a magnification (bottom)
the CTE.

2. Experimental Procedure

2.1 Specimen preparation

Freestanding Au specimens were fabricated through sequential
sputtering deposition, photolithography, and bulk etching from the
backside of a (100) Si wafer.11 Four kinds of specimens with different
thicknesses were fabricated by altering the deposition time while
holding the other conditions constant. The die with 6 specimens and a
magnification of one of the specimens are shown in Fig. 1(a). The Fig. 2 (a) Cross section exposed by FIB cut and the enlarged view (b)
specimen was 20 µm wide and 1 mm long. One of the freestanding of the section for the 543 nm thick specimen
straight portions shown in Fig. 1(a) was removed from the die and
transferred to Zerodur® substrate12 for the CTE measurements of the Si
substrate and Au film. The specimen handling procedures to transfer
the film from the Si die to Zerodur® substrate were described in detail
in our previous paper.10 One of the prepared Au films on Zerodur®
substrate is shown in Fig. 1(b).

2.2 Thickness and grain size measurements

The actual thicknesses of the as-fabricated films were measured on
small sections of the specimens that were exposed by cuts made using
a focused ion beam (FIB; FEI’s Nova NanoLab™ 600). The average
thicknesses of the specimens were 115, 224, 543, and 1200 nm. FIB
images of the 543 nm thick specimen are shown in Fig. 2.
The grain size was measured using a transmission electron
microscope (TEM; JEOL’s JEM-2100F); the images are shown in Fig.
3 and the results are tabulated in Table 1. The 115 nm thick specimen
had the smallest grains (44 nm) while the thickest film had the largest
Fig. 3 TEM images of (a) 115 nm, (b) 224 nm, (c) 543 nm, and (d)
grains (98 nm). TEM analysis revealed that the thinner films had smaller
1200 nm thick Au specimens
grains. The relationship between the grain size and thickness is shown
in Fig. 4. For gold, it has been reported13,14 that the variation of the
grain size with respect to thickness is governed by three dimensional require prolonged deposition, they are more susceptible to secondary
(3D) nanometric grains, which form normal grains for relatively thin grain growth, which usually results in larger grains.15
films and large grains in thicker films. In addition, since thicker films
 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 15, No. 1
Fig. 4 Dependence of grain size on film thickness
Fig. 5 Thermal bulge measurement apparatus and schematic diagrams
illustrating setting up of a specimen and curve fitting
2.3 CTE measurement procedures
For the CTE measurements, the specimens were seated in a small
furnace, heated to the desired temperature at a rate of 1oC/min, and held
there for five minutes to achieve thermal equilibrium. Starting from room
temperature, the specimen was heated up to 100oC with measurements
taken at 5oC intervals. The 100oC temperature limit was chosen to
eliminate the effect of other factors such as creep and relaxation in our
test.
The entire procedure, i.e., from the out-of-plane thermal deformation
measurements to the average linear CTE calculations, were followed
by the TBM.10 The actual test setup and an overview of the key test
procedures, such as heating and curve fitting, are presented in Fig. 5.
A white-light interferometric microscope (WLIM) was used to measure
the out-of-plane displacement caused by thermal strain induced on a
freestanding specimen heated inside a miniature furnace with a quartz
glass window. Since the specimen is freestanding and initially buckles
with both ends fixed, the overall length change causes out-of-plane
deformation that can be easily detected and captured by scanning and
obtaining the 3D surface topology of the thermally deformed specimen.
JANUARY 2014 / 107
Fig. 6 Successive shape changes of a specimen (1200 nm thick) on
Zerodur® substrate when heated from 20oC to 100oC at 5oC intervals
The WLIM has an independent sub-nanometer out-of-plane resolution.
The supporting substrate also experiences thermal strain and expands
in-plane along the length of the film; thus, it affects the measured CTE
of the gold films. It was shown that it is easy to compensate for the
effect of the substrate on the measured CTE and the true CTE for the
gold film is simply the sum of the measured CTEs of the gold film and
substrate, which was silicon10 in this study. To accurately account for
the substrate effect, the CTE was also measured on freestanding gold
films supported by a substrate with negligible CTE. The results of this
test provide the CTE value of the substrate in order to account for the
substrate effect on all other specimens.
3. Results and Discussion
The successive shape changes of a film as it underwent thermal
expansion upon heating from room temperature to 100oC were measured
at 5oC intervals using the WLIM; the results are presented in Fig. 6. It
is clearly evident that the height increases monotonically with
increasing temperature. Figs. 7(a) and (b) show the thermal deformation
profiles for silicon and Zerodur® substrates. The six-parameter beta
function was adopted for curve fitting of all the deformation profiles.10
On both substrates, the films bulge consistently upon increasing the
temperature; however, the height increment for the Zerodur® substrate
is greater than that for the silicon substrate. This is attributed to the in-
plane thermal deformation of the Si substrate itself, which reduced the
amount of out-of-plane thermal bulge. Thermal strain versus temperature
plots for both substrates were obtained from the fitted curves of the
corresponding profiles and are shown in Fig. 8. The CTE values were
obtained from the slope of the linear trend lines of the plots. The data
is linear, which is evident from the correlation coefficient value (r2) of
greater than 0.98, up to 100oC. It can be clearly seen that the CTE value
with the Zerodur® substrate (~12.9 ppm/oC) is higher than that with the
Si substrate (~10.1 ppm/oC). The difference between the two (2.8 ppm/
o
C) is unsurprisingly almost equal to the CTE of silicon (3~3.5 ppm/
o
C).10 Note that this step was only performed once and is only needed
if the actual effect of the substrate is important. This particular value
(αS) can be added to all the CTE values (αav) obtained in the proceeding
steps in order to get the true value (αtrue) of a film using Eq. (1) as long
 108 / JANUARY 2014
Fig. 7 Out-of-plane deformation of a Au film when heated from 20oC
to 100oC for (a) silicon and (b) Zerodur® supported substrates
Fig. 8 Thermal strain versus temperature plots for Au films on silicon
and Zerodur® substrates
as the films are supported on the same kind of substrate.
∆ε
α true = -------T- + α S = α av + α S (1)
∆T
Thermal strain versus temperature plots for the four Au thin films
INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 15, No. 1
Fig. 9 Thermal strain versus temperature plots for Au films of 4
different thicknesses on silicon substrates
with different thicknesses are shown in Fig 9. It is interesting to note
that the four fitted lines appear to be grouped into two with one group
having a slope lower than the other. The CTEs of the 115 and 224 nm
films are quite similar, even though there is a significant difference in
the thickness. This is even more pronounced for the 543 and 1200 nm
films, which have a greater difference in thickness and only a slight
difference in CTE values. This clearly indicates that the measured CTE
is not linearly affected by the thickness of the film. In order to determine
the parameter that affects the CTE more significantly, the CTE values
were also correlated with the grain size. For comparison, the CTEs as
a function of thickness and grain size are illustrated in Fig 10 and
tabulated in Table 1. It is evident that there is a stronger relationship
between the CTE and average grain size. Since the grain sizes of the
115 and 224 nm films are relatively close, differing by only 6 nm, their
CTEs are almost the same. The significant difference in the grain sizes
of the 224 and 543 nm films is reflected by a large difference in the
magnitude of thermal expansion: A 50% increase in the average grain
size resulted in a 25% increase in the CTE. In the case of the 543 and
the 1200 nm films, both have larger grains and very similar CTE values.
It is clear that the CTEs of the thin films are remarkably affected by
the film thickness (or grain size). This trend is different from that
reported by Daniel et al.,6 but similar to that reported by Hwang and
Kim.16 It has also been reported that the CTEs of some thin films, such
as those of aluminum and titanium, increase or decrease as the films
thickness increases.17 Overall, the measured CTEs, especially that of the
1200 nm film, are similar to those reported in literature.18 In fact, at
1200 nm, the measured value of 13.6 ppm/oC corresponds well with that
of 14.4 ppm/oC of a bulk material within the same temperature range.
However, at the sub-micron thickness range, other factors, such as grain
size in this study, become more dominant and the CTE value deviates
from that of the bulk. It is also noted that the measurement errors
increase with decreasing thickness; this is mainly due to the high bulge
profile measurement errors of the thinner specimens. They have narrower
width, which makes the specimen edges curled and so hinders the
accurate alignment and scan.
The CTE data, which is shown in Fig. 10(b), was rearranged as a
function of the reciprocal of the square root of the average grain size
(d) and represented in Fig. 11. It is very interesting that the CTE
 INTERNATIONAL JOURNAL OF PRECISION ENGINEERING AND MANUFACTURING Vol. 15, No. 1 JANUARY 2014 / 109

Fig. 11 Linearization of the CTE difference with a new parameter

which also has an FCC structure. On the other hand, body-centered-cubic

(BCC) metals like Cr6 show the reverse trend. It would be premature
to discuss the exact mechanism now. However, the TBM will be used
to measure the intrinsic CTEs of ultra-thin films and thus identify the
underlying mechanisms in the near future.

4. Conclusions

It was demonstrated that the thermal bulge method is effective for

measuring the CTE values of ultra-thin films with thicknesses in the sub-
micron range with significant accuracy and simplicity. The effect of the
substrate on the CTE measurement can be readily determined and easily
Fig. 10 Measured CTE values for the various thicknesses (a) and their
compensated for. Measurement of the CTE values of gold films with
corresponding grain sizes (b) of gold films
thicknesses ranging from 115 to 1200 nm reveals that the grain size,
rather than the thickness, affects the magnitude of thermal expansion:
Table 1 Average thickness, width, grain size, and CTE of Au specimens Specimens with larger grain sizes (44 to 98 nm) had greater CTE values
Thickness, t Width, w Grain Size, d CTE, αtrue (mean±SD) (9.6 to 13.6 ppm/oC). The CTE difference between the bulk and its
[nm] [µm] [nm] [ppm/°C] corresponding films is proportional to the parameter of 1/√d.
115 20~25 44 9.6±1.4
224 20~25 50 10.6±1.2
543 50~55 78 12.9±0.3 ACKNOWLEDGEMENT
1200 50~55 98 13.6±0.2
This paper was supported by the Research Fund of the Kumoh
difference between the bulk material and its corresponding films has a National Institute of Technology.
strong linear relationship with the new parameter. As a result, the CTE
values of the Au films in our study can be described and predicted
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