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Highly Thermal Conductive and Electrically Insulated Graphene Based Thermal

Interface Material with Long-Term Reliability

Conference Paper · May 2019

DOI: 10.1109/ECTC.2019.00240

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 2019 IEEE 69th Electronic Components and Technology Conference (ECTC)
Highly Thermal Conductive and Electrically Insulated Graphene Based Thermal
Interface Material with Long-term Reliability
Nan Wang
SHT Smart High Tech AB
Gothenburg, Sweden
Nan.wang@sht-tek.com
Ya Liu
Department of Microtechnology and Nanoscience
Chalmers University of Technology
Gothenburg, Sweden
yaliu@chalmers.se
Shujing Chen
School of Automation and Mechanical Engineering
Shanghai University
Shanghai, China
csj427@i.shu.edu.cn
Abstract—Thermal management in high power devices are
becoming more and more challenging due to the high density
packaging as well as dramatically increased transistor
integration. The conventional TIMs that are widely used in the
microelectronic industry today are experiencing more and
more stress due to their limited thermal performance and poor
reliability. Composed by particle laden polymer matrix,
conventional TIMs have thermal conductivity (K) values in the
range of 1-5 W/mK, and such values can be even lower for
electrically insulated TIMs. Conventional TIMs also suffer
from severe pump-out and dry-out failures, which brought
great threat to the performance and lifetime of the electronic
devices. Here, we address these problems by utilizing a highly
thermally conductive, electrically insulated and reliable
graphene enhanced TIMs (I-GTs). Composed by vertical-
aligned graphene layers, I-GTs provide a direct heat pathway
from top to bottom, which enables superfast heat dissipation at
through-plane direction. The highest bulk thermal
conductivity of the conductive body at the through-plane
direction is over 1000 W/mK, which is 100 times higher than
conventional TIMs. I-GT also possesses good flexibility and
can be easily compressed over 100% at Z direction upon small
applied pressures. Therefore, fully contact between two
surfaces can be achieved by using I-GT as gap fillers. The
minimum thermal resistance measured for I-GTs reaches
about 30 Kmm2/W, which is much lower than most of the
conventional TIMs. To ensure fully electrical insulation, a
smooth and soft adhesive layer with a thickness of few microns
was coated on the surface of I-GT. The breakdown voltage of I-
GT reaches up to 950 V. Thermal cycling test shows the highly
stable nature of I-GT. The good compressibility and elasticity
of I-GT ensures continued proper TIM contact with substrates,
which counteracts the effect of internal stress induced by the
mismatch of coefficient of thermal expansion (CTE) during
temperature cycling. In addition, the I-GT has the advantages
2377-5726/19/$31.00 ©2019 IEEE
DOI 10.1109/ECTC.2019.00240
Lilei Ye
SHT Smart High Tech AB
Gothenburg, Sweden
lilei.ye@sht-tek.com
Johan Liu
Department of Microtechnology and Nanoscience
Chalmers University of Technology
Gothenburg, Sweden
johan.liu@chalmers.se
of low density and good maintainability. The resulting I-GTs
thus offers new solutions for addressing thermal management
issues in high power electronics and other systems with small
form-factor.
Keywords- graphene, reliability, insulation, compressibility,
bonding strength
I. INTRODUCTION
The development of electronic industry towards
miniaturization and higher performance leads to enormous
thermal management challenges. To minimize adverse
effects of such challenges both on the user’s health and
device’s reliability and performance, efficient thermal
management in high power density electronic products
becomes highly essential. As a key element in thermal
management, thermal interface materials (TIMs) act as a
bridge to link the hotspot with cooling system to bring down
the junction temperature of power modules in electronic
devices [1]. Today, the widely used TIMs in the electronics
industry are composed of high thermal conductive filler
enhanced polymer matrix, Such formulas have the great
advantages of high reliability, cost efficient and ease to use
[2], [3]. However, their thermal conductivity (K) at through-
plane direction is usually limited within 10 W/mK, and in
most cases, is about 4 or 5 W/mK. Such low thermal
conductivity of the conventional TIMs is strongly related to
the large thermal contact resistance formed between
individual particle fillers of TIMs [4]. Therefore, it is highly
essential to develop new solutions to address the fast
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growing thermal management issues in modern power
devices.
Many studies have been carried out to solve above
problems. For example, increasing the amount of fillers in
polymer matrix is the most common strategy to improve
thermal performance of TIMs [5]. However, high filler
contents can inevitably lead to the increase of material’s
hardness and make the composites difficult to conform to
surface roughness, which results in relatively high contact
thermal resistance. Moreover, the substantial filler particles
can sacrifice the mechanical strength of polymer resin and
increase the density of composites [6], [7]. Therefore, it
becomes highly essential to investigate new approaches for
improving thermal conductivity of TIM whilst maintaining
low contact thermal resistance.
Here, a highly thermally conductive, electrically
insulated, compressible and light-weighted graphene
enhanced TIMs (I-GTs) were developed to achieve above
goals. The conductive body of I-GT is composed by
vertical-aligned graphene layers, which can provide a
continuous highway for fast heat dissipation at the vertical
direction. Therefore, excellent thermal properties can be
achieved along the heat flow direction in I-GT. The highest
thermal conductivity of the conductive body was found to
be up to 1000 W/mK at the vertical direction. Such a value
is over 100 times higher than conventional TIMs. I-GT also
possesses good flexibility and can be easily compressed
over 100% at Z direction upon small applied pressures (İ
400 KPa). The minimum thermal resistance measured for I-
GTs is about 30 Kmm2/W, which is much lower than most
of the conventional TIMs. To ensure fully electrical
insulation, a smooth and soft adhesive layer with a thickness
of 4 m was coated on the surface of I-GT. The breakdown
voltage of I-GT reaches up to 950 V. Thermal cycling test
shows the highly stable nature of I-GT. The good
compressibility and elasticity of I-GT ensures continued
proper TIM contact with substrates, which counteracts the
effect of internal stress induced by the mismatch of
coefficient of thermal expansion (CTE) during temperature
cycling. In addition, I-GT has the advantages of low density
and good maintainability. The resulting I-GTs thus offers
new solutions for addressing thermal management issues in
high power electronics and other systems with small form-
factor.
II. EXPERIMENTS
I-GTs were fabricated and provided by SHT Smart High
Tech AB. Thermal conductivity of I-GTs at through-plane
direction and thermal resistance of I-GT between two copper
substrates were measured by LFA 447 instrument.
Compression ratios of I-GT at different pressures and
thermal resistance of I-GTs were tested by INSTRON
ASTM. Bonding strength of I-GT was measured by a shear
tester (Dage 4000 Bondtester, Nordson). Thermal reliability
of I-GT was evaluated at the temperature range of -20oC to
1565
I-GT (VG = 75%)
1500
I-GT (VG = 65%)
Thermal conductivity (W/mK)
I-GT (VG = 30%)
1000
500
0
20 40 60 80 100
o
Temperature ( C)
Figure 1. thermal conductivity changes of I-GT with different VG
proportions at the through-plane direction upon different temperatures.
125oC in a thermal cycling oven upon nitrogen atmosphere.
Heat dissipation performance of I-GTs at the through-plane
direction was shown by using a home-made testing platform.
A heater and a heat sink equipped with a cooling fan were
used to create temperature gradient. I-GTs was mounted
between the heater and heatsink. The heater’s working
voltage is 23 V (power 3.57 W). Temperature change on the
surface of heater was recorded by using a thermal imaging
camera (Therm CAM PM595 NTSC) after the system
reaches to the equilibrium state. A thin graphite coating
layer was applied on the surface of heater to improve the
accuracy of temperature recorded by IR camera.
III. RESULTS AND DISCUSSION
The graphene volumatic ratios (VG) play a key role on
determine the through-plane thermal conductivity and
contact thermal resistance of I-GTs. Here, I-GT samples with
varied VG ratios (30%, 65%, and 75%) were fabricated and
tested. As illustrated in Figure 1, the raising of VG ratios
from 30% to 65% led to significant increase of through-plane
thermal conductivity of I-GT samples from 167 ± 9 W/mK
to 637 ± 31 W/mK. Further increase of VG to 75% showed
the highest thermal conductivity (1379 ± 138 W/mK). Such
value is over 100 times and over 3 times higher than
conventional TIMs and copper, respectively. The superior
thermal properties of I-GTs are related to its unique structure
composed by vertically aligned graphene layers.
Contact thermal resistance induced by surface roughness
plays a key role in determining the final heat dissipation
performance of TIMs. Therefore, good compressibility is
highly essential for TIMs to decrease the contact thermal
resistance. Figure 2a shows the change of deformation
behavior of I-GTs at different VG proportions. For I-GT
with a large VG proportion above than 65%, it showed a
linearly increase of the compression ratio when the applied
pressure increased, and the material recovered to its original
thickness completely after the pressure releasing. The
a 200 a
I-GT (VG = 30%) 1000 950 V
I-GT (VG = 65%)
Compression ratio (%)

150

Voltage (V)
100 500

50

0
0 0 500 1000 1500 2000 2500 3000 3500
0 200 400 600 800 Time (S)
Applied pressure (KPa)

b 400 b 3
I-GT (VG = 30%)
Thermal resistance (Kmm2/W)

I-GT (VG = 65%)

2.3 MPa
300

Shear strength (MPa)

2

200

1
100

0
0 50 100 150 200 250 300 350 400 450 0
0 2 4 6 8 10
Applied pressure (KPa) Time (s)
Figure 2. (a) Compression ratio changes of I-GT with different VG
Figure 3. (a) Breakdown voltage of the I-GT film. (b) Shear strength curve
proportions as a funtion of pressures. (b) Thermal resistance change of I-
of the I-GT film.
GT with different VG propotions at different pressures

results showed that the composite is highly elastic at the
through-plane direction. However, electronic devices have
limitations on the applied pressures for TIM bonding (400
KPa) to prevent the functional components from damages.
The compression ratio of I-GT samples with a large VG
proportion above than 65% is less than 20% within 400 KPa,
which is difficult to reduce thermal contact resistance at
interfaces. As a comparison, I-GT (VG = 30%) exhibits high
softness and shows a large compression ratio around 100%
in the pressure range of 400KPa. After releasing the
pressure, the sample thickness can be recovered partially till
to 80% of original thickness. We believe that the 20% of
permanent structural deformation of I-GT (VG = 30%) was
caused by the spontaneously bending and folding processes
of the vertical graphene structure in the first pressing.
Thermal resistance of I-GT samples with different VG
proportions were measured by using ASTM D5470
equipment. The thickness of all measured samples is 2 mm.
The applied pressure was varied in the range of 450 KPa. As
shown in Figure 2b, the I-GT sample with a large VG
proportion of 65% exhibited a large thermal resistance value
of 358 Kmm2/W before pressing, which was about 4 times
higher than that of I-GT (VG = 30%) (96 Kmm2/W). With
the applied pressure increased, both samples showed a
significant decrease of thermal resistance. When pressure
reached to 425 KPa, the resistance values of I-GT (VG =
65%) and I-GT (VG = 30%) are 94 Kmm2/W and 30
Kmm2/W, respectively. The small thermal resistance value
of I-GT (VG = 30%) in the measured pressure range was
attributed to the high softness of I-GT structure which
enabled the composite to decrease the contact thermal
resistance significantly at interfacial areas.
T o a vo id p o te n t ia l r i s k s o f s ho r t c ir c u it a nd
contaminations, the surface of I-GT film needs to be
protected by insulation layers. To meet this goal, a thermal
plastic polymer was coated on the surface of I-GT. It has the
advantages of highly electrical insulation, strong bonding
and good elasticity. The thickness of the protective layer is
4m. Figure 3a shows the breakdown voltage of the I-GT
film. The maximum breakdown voltage that the I-GT film

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a a
Figure 4. (a) Thermal reliability curve of I-GT in 500 cycles of thermal
cycling tests. (b) Pump-out demonstrators of different thermal interface
materials, including thermal pad, thermal grease and I-GT.
can stand reaches to 950V. By increasing the temperature
above than 100oC, the protective layer can form bonding
with variety of substrates, including ceramic, metal, glass,
and polymer. Figure 3b shows the bonding strength of the I-
GT between two pieces of copper substrates. Shear strength
was measured by using a shear tester. The maximum shear
strength that the protective layer can provide is about2.3
MPa, which reaches the same level of mechanical
performance as the commonly used acrylic double-side
tapes.
Thermal reliability of the I-GT was investigated further in
a thermal cycling oven at the temperature range of -20oC to
125oC. To simulate the actual application environment, the
I-GT sample with a thickness of 200 m was used as a TIM
layer between two pieces of copper plates (shown in the
insert image of Fig. 5a). Thermal resistance was measured
by using laser-flash equipment. Figure 4a shows the thermal
resistance variation of FSCs in total 500 thermal cycles.
Notably, the thermal resistance remained constant around 15
Kmm 2 /W. It shows the excellent thermal-mechanical
stability of I-GT during the temperature cycling test. The
good stability of I-GT is mainly attributed to the flexible
nature of the material which benefits on absorbing the inner
stress caused by the mismatch of coefficient of thermal
expansion (CTE). In addition, the unique vertical graphene
structure of I-GT benefits on solving the pump-out and dry-
out failures existing in most of common TIMs. As shown in
Figure 4b, thermal pad and thermal paste exhibited obvious
extrusion phenomenons upon pressing. In electronic devices,
1567
Figure 5. (a) The sketch of the home-made thermal testing platform (b) IR
images of the working temperature of the heater by using different TIMs,
including direct contact, thermal pad, thermal grease and I-GT.
repeated powering up and down processes during the usage
can also generate a similar effect as the above motions
which lead to the increase of thermal resistance and reduce
the lifetime of the power modules. However, with the same
pressure, I-GT did not show any structural change at the in-
plane directions. The main structural deformation of I-GT
was only taken place at the vertical directions in the forms
of bending and folding of the vertical graphene structures.
This advantage of I-GT can benefit improving the long-term
thermal reliability of power devices and thereby improving
their lifetime.
Light weight is another important advantage of I-GT
material compared to most of commercial TIMs, The
density of I-GT (VG = 30%) was measured to be 0.6 g/cm3,
It is only half of the common paste TIMs and also one-
fifteenth of copper.
A thermal testing platform was built to demonstrate the
heat dissipation performance of I-GTs. Two types of
commercial TIMs, including thermal pad with a thermal
conductivity of 3 W/mK and thermal grease with a thermal
conductivity of 2 W/mK, were also used as comparisons. A
control group shows the heat dissipation situation of the
thermal testing platform without using any TIMs. As shown
in Fig. 5a. All tested TIMs were added between a heater and
a heatsink equipped with a cooling fan. The operating power
of the heater and cooling fan were 3.57 W and 0.57 W
respectively. The working temperatures of the heater were
recorded by using a thermal imaging camera when the
 testing platform reached to the equilibrium state. As shown [6] Y. Xu, D. D. L. Chung, and C. Mroz, “Thermally conducting
aluminum nitride polymer-matrix composites,” Compos. Part Appl.
in Fig. 5b, the control group that heater had a direct contact
Sci. Manuf., vol. 32, no. 12, pp. 1749–1757, Dec. 2001.
with the heatsink presented the highest surface temperature [7] S.-Y. Fu, X.-Q. Feng, B. Lauke, and Y.-W. Mai, “Effects of particle
of 115oC. Obvious decreases on the working temperature size, particle/matrix interface adhesion and particle loading on
were detected in the rest three samples. In cases of thermal mechanical properties of particulate–polymer composites,” Compos.
Part B Eng., vol. 39, no. 6, pp. 933–961, Sep. 2008.
pad and thermal grease, the working temperatures of heater
were stabilized at 90oC and 44oC respectively. The much
decreased working temperature in the thermal grease sample
was attributed to its much lower contact resistance than the
thermal pad sample. For the I-GT sample, it showed the
lowest working temperature compared to the rest three
samples, which was only 32oC. It is 83oC less than that of
the control group. The temperature difference between the
heater and ambient was only about 7o due to the fast heat
dissipation property of I-GTs.

IV. CONCLUSIONS
In summary, I-GT was developed as a novel TIM for
addressing thermal management issues in many high power
density devices. I-GT has the advantages of light-weight,
electrically insulation, good compressibility and high
thermal conductivity. The developed I-GT demonstrated
superior thermal-mechanical stability in long-term reliability
study which is highly essential for prolonging the lifetime of
electronic devices. The resulting I-GTs thus offers new
solutions for addressing thermal management issues in high
power electronics and other systems with small form-factor.
ACKNOWLEDGMENT
We thank for the financial support from the Swedish
Foundation for Strategic Research (SSF) (No SE13-0061),
Swedish National Board for Innovation (Vinnova) Graphene
SIO-Agenda Program, Formas program on graphene
enhanced composite as well as from the Production Area of
Advance at Chalmers University of Technology, Sweden.
Thanks for the financial support from the Ministry of
Science and Technology of China (No: 2017YFB040600)
and Chinese national Science foundation project (No:
51872182)
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