Surfaces and Interfaces 46 (2024) 103905

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Surfaces and Interfaces

journal homepage: www.sciencedirect.com/journal/surfaces-and-interfaces

Improvement of interfacial thermal resistance between TIMs and copper for

better thermal management
Xiaoyu Fan a, Ying Sun a, Leyi Huang a, Jiaqiu Xie a, Xiaoliang Zeng b, Chenhan Liu c, Lifa Zhang a,
Yunshan Zhao a, *
a
Phonon Engineering Research Center of Jiangsu Province, Center for Quantum Transport and Thermal Energy Science, Institute of Physics Frontiers and Interdisciplinary
Sciences, School of Physics and Technology, Nanjing Normal University, Nanjing 210023, China
b
Shenzhen Institute of Advanced Electronic Materials, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
c
Micro- and Nano-scale Thermal Measurement and Thermal Management Laboratory, School of Energy and Mechanical Engineering and Jiangsu Key Laboratory for
Numerical Simulation of Large-Scale Complex Systems, Nanjing Normal University, Nanjing 210023, China

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

Keywords: Due to the increasing power consumption of modern electronic devices and rapid rise in heat generation, how to
Thermal contact resistance (TCR) efficiently manage the heat dissipation becomes a challenge. The previous studies have shown the importance of
Graphite-copper interface interface treatment for better thermal management while the mechanism is lacking yet. Here, we study the
Thermal interface materials
interface thermal transport between the thermal interface materials (TIMs) and the copper substrate using both
COMSOL simulation
experimental measurements and theoretical calculations. The results show that after interface treatment, the
thermal contact resistance between the graphite materials and copper decreases from 87.96K ⋅ mm2 ⋅ W− 1 to
20.26K ⋅ mm2 ⋅ W− 1. For the practical testing, a difference up to 7 C is demonstrated between the treated and
○

untreated samples, indicating the potential of reduction of thermal contact resistance for the heat dissipation in
electronic devices, which is verified in our theoretical calculation as well. Our study provides an applicable
approach to enhancing the thermal stability in electronic devices by investigating the impact of the interfacial
thermal resistance on heat dissipation.

1. Introduction
With the rapid development of 5 G technology, the integration and
miniaturization of electronic devices become dominant, leading to the
continuous rise in power consumption and the issue of heat concentra­
tion. [1] High operating temperature can lead to the deterioration in the
stability, performance and lifetime of the electronic devices, so how to
achieve an efficient heat removal becomes a key issue. In general, a
typical thermal dissipation setup consists of a chip, heat sink, a cooling
system, thermal interface materials(TIMs) and a temperature controller,
[2] and the heat dissipation across each of these components relies
primarily on the contact heat exchange. If the electronic devices and
heat sink are directly connected, their actual contact area is small, due to
its uneven surface microscopically, and the rest are air gaps, etc.
Considering that the air is a poor conductor of heat and has a thermal
conductivity around 0.026W ⋅ m− 1 ⋅ K− 1, [3] there is a ultra-high ther­
mal contact resistance (TCR) resulting from the rest 90 % air gap. [4]
Therefore, for the Integrated Circuit (IC) packaging, the electronic heat
dissipation materials, TIMs are commonly used. TIMs are mainly used to
fill the micro-gaps and uneven surface gap when two materials are
contacted, which are essential in the thermal management of electronic
devices. [5–7]
Typically, TIMs have properties of good heat dissipation, electrical
insulation and easy processability etc., which enable the generated heat
to be dissipated efficiently, resulting in lower operating temperatures
and longer service life. [8,9] Guo et al. prepared YDH-151 functional­
ized multi-walled carbon nanotubes and blended them into PVDF, which
significantly improved the interfacial compatibility with PVDF and
hence the thermal conductivity. [10] Qiu et al. obtained DLC/TiN coated
VACNT arrays by using the chemical vapor deposition methods,
resulting in a 50-fold reduction in the TCR from 15K ⋅ mm2 ⋅ W− 1 to 0.3K
⋅ mm2 ⋅ W− 1. [11] Ye et al. fabricated Cu@rGO@Al2O3 microspheres by
heating graphene oxide nanosheet-coated Cu microspheres with an Al
(OH)3 outer layer under H2/Ar atmosphere. Compared to the bare Cu
microsphere filler, the new material shows an increased thermal con­
ductivity by up to 1.5 times. [12] Further studies show that an

* Corresponding author.
E-mail address: yunshan12241@gmail.com (Y. Zhao).

https://doi.org/10.1016/j.surfin.2024.103905
Received 20 November 2023; Received in revised form 2 January 2024; Accepted 13 January 2024
Available online 14 January 2024
2468-0230/© 2024 Elsevier B.V. All rights reserved.
X. Fan et al.
introduction of novel materials like BN, [10,13,14] CNT [15] and
TMDCs [16] into TIMs would improve their heat dissipation
performances.
Recently, the graphene composites are studied and considered to be
potential TIMs. Graphene has almost the highest thermal conductivity of
all known materials, [17] and it has a wide range of applications in
thermal management. [18–20] Guo et al. used fused deposition model­
ling to prepare graphene filled thermoplastic polyurethane composites,
which have excellent interfacial thermal conductivity (12W ⋅ m− 1 ⋅ K− 1).
[21] Naghibi et al. reported the first preparation of a graphene thermal
paste with high thermal conductivity (7.1W ⋅ m− 1 ⋅ K− 1) without the use
of commercial TIMs and other fillers. [22] Usually, graphene is added
into polymers to improve the thermal conductivity of composites. Dai
et al. developed a dual-assembled graphene frame­
work/polydimethylsiloxane composite with highly aligned graphene in
the vertical direction and low interfacial thermal resistance (ITR) of
adjacent graphene sheets, which exhibited excellent in-plane (24.8W ⋅
m− 1 ⋅ K− 1) and through-plane thermal conductivity (62.4W ⋅ m− 1 ⋅ K− 1).
[23] Bai et al. have developed highly thermally conductive graph­
ite/copper composites that can achieve a maximum thermal conduc­
tivity of 676W ⋅ m− 1 ⋅ K− 1 when the volume fraction of graphite is 70 %,
which is 180 % of that of copper. [24].
In addition, the thermal transport in the through-plane direction is
also an important issue for thermal management. [25,26] Li et al. pre­
pared a super flexible and foldable graphene/polyimide flexible carbon
film, where the through-plane thermal conductivity (150 ± 7W ⋅ m− 1 ⋅
K− 1) was improved while ensuring ultra-high in-plane thermal con­
ductivity (1428 ± 64W ⋅ m− 1 ⋅ K− 1). [27] A bridge structure consisting
of loosely stacked horizontal large graphene sheets with randomly ori­
ented small graphene sheets resulted in a hierarchically structured
graphene paper with excellent in-plane thermal conductivity (12.6W ⋅
m− 1 ⋅ K− 1). [28] Song et al. developed a highly thermally conductive
polypropylene/graphene composite with a 3D graphene framework,
which exhibits a fairly high through-plane thermal conductivity of
10.93W ⋅ m− 1 ⋅ K− 1. [29] However, even these graphene-based com­
posites show improved intrinsic thermal conductivity, while the thermal
contact interface between the composites and the substrates would be
another dominant factor to achieve an excellent heat dissipation per­
formance. [30,31]
Normally the total thermal resistance includes two parts, the TCR, Rc
and the intrinsic thermal resistance of TIM, RTIM, where RTIM can be
calculated by the equation
l
RTIM = (1)
κ
l is the thickness of TIM and κ is the intrinsic thermal conductivity of
TIM. As discussed above, the previous studies focused on increasing κ to
reduce RTIM, thus reducing RTotal. However, in the practical application
of integrated chips, the weak thermal coupling between graphene and
substrate leads to high TCR at the interface. [32,33] As a result, it re­
mains unclear that how much the TCR can be improved, and how to
further reduce the TCR.
In this study, we probe the impact of the interface treatment between
TIMs and copper substrate on through-plane thermal transport by tuning
the TCR via different thermal pastes. The thermal contact conductance
between two copper substrates is carried out to verify the reliability of
our equipment. By comparing the graphite composites and the com­
mercial thermal pads, it was observed that the proportion of TCR in total
thermal resistance can reach to 33.14 % before the interface treatment.
And TCR decreases from 87.96K ⋅ mm2 ⋅ W− 1 to 20.26K ⋅ mm2 ⋅ W− 1
after the application of thermal paste. Moreover, a thermal test platform
is set up to demonstrate the superior practical cooling performance by
using the graphite TIMs. Further COMSOL simulation is carried out as
well to verify the substance of the interface treatment. Our work would
provide a practical direction for realizing the efficient heat dissipation in
modern electronic devices.
2
Surfaces and Interfaces 46 (2024) 103905
2. Results and discussions
The thermal conductivity measurements have been performed ac­
cording to the ASTM D5470 standard as shown in Fig. 1(a). Two high
thermal conductivity pure copper bars, 10mm × 10mm square in the
cross-sectional area and80mm in the length, are fixed between the
heating module and the cooling module. All the copper bars surfaces are
sanded to obtain a flat and even surface. On the same side of each copper
bars, four small holes with a diameter of about 1mm are located at 6mm,
26mm, 46mm, and 66mm away from the position of the measured
sample. The hole is about 5mm deep into the copper bars and reaches
the center of the copper bars. Eight thermocouples with a diameter of
1mm are inserted into the holes to collect temperature data. The data
acquisition system (DAQ6510) consists of Keithley Instruments and can
simultaneously monitor up to eight thermocouple signals.
The heating module at the top consists of ceramic heating plates that
operate at a stable output voltage, while the cooling module at the
bottom is composed of inverted "U" shaped square copper block, which is
immersed in a container of ice water. The ball joint is used to facilitate
the sample alignment with the upper and lower copper bars. An
adjustable mechanical pressure is applied at the top of the device, which
is visualized by a coaxial pressure sensor mounted at the bottom. The
schematic diagram of the device is shown in Fig. 1(a).
For the data acquisition, the readings from the eight thermocouples
are recorded and we take the average of three readings for each ther­
mocouple. The measured data are plotted in Fig. 1(b), where it can be
seen that the temperature of the eight thermocouples tends to be satu­
rated with time. As shown in Fig. 1(c), the temperature difference ΔT
between the upper and lower surfaces of the copper bars in contact with
TIM can be obtained by linear fitting the temperature data once the eight
thermocouples are stabilized, with the details discussed in the
Methodology.
Metals like copper, have wide applications in both electronic and
heat transfer devices. For metals, many factors would affect their ther­
mal contact conductance, such as the surface roughness, the tempera­
ture near interface, the external pressure and the contact area, etc. [34,
35] Here, we firstly measure the thermal contact conductance between
two copper bars used in our measurement setup. In our work, the
pressure applied to the equipment is chosen as a variable. As is shown in
Fig. 2(a), it has been presented that when the pressure increases from
1.15 to 7.40 MPa, TCR between two flat copper surfaces has an evident
linear increase from 6.95kW/K ⋅ m2, finally reaching 17.82kW/K ⋅ m2,
almost three times of the original value, which coincides with the results
by Tariq et al. [36]
As it is known, TIMs can fill the gaps and removes the air between the
components and the heat sink, thus creating an effective heat transfer
path and significantly reducing the TCR. [37,38] Here a commercial
thermal pad (Laird’s Tflex HD90000) is chosen. As shown in Fig. 2(b),
the application of thermal paste (Cooler MasterGel PRO) significantly
improves the contact at the interface between the commercial thermal
pad and the heat sink, where an approximately 25 % reduction in the
total thermal resistance is observed and the TCR decreases from 77.96K ⋅
mm2 ⋅ W− 1 to 58.30K ⋅ mm2 ⋅ W− 1, indicating the role of interface
treatment in facilitating the heat transfer at the interface between the
pad and the heat sink. [11]
To further improve the heat dissipation at the interface, the graphite
composites are employed considering its ultrahigh thermal conductivity.
Herein, a kind of vertically oriented graphite/polybutadiene (V-GP/PB)
TIM is selected in this work due to its excellent elastic compliance and
high through-plane thermal conductivity, [39] and the detailed fabri­
cations are discussed in the Methodology. Before investigating its ther­
mal property, we characterize the structure by Raman spectrometer. As
shown in Fig. 3(a), for graphite composites, two Raman sensitive peaks
are observed, which are G peak and 2D peak, located around 1580cm− 1
and 2700cm− 1, respectively. [40] Moreover, the D peak around
1330cm− 1 is shown, indicating the existence of defects and disorder in
X. Fan et al. Surfaces and Interfaces 46 (2024) 103905

Fig. 1. (a) The schematic diagram of the measurement setup. (b) Images of temperature changing over time at various points of the measured sample recorded for a
total of 1 hour, and T1-T8 represent the readings of eight thermocouples. (c) A set of temperature data obtained after a certain measurement.

Fig. 2. (a) The contact thermal conductance of Cu-Cu interface as a function of the applied pressure. (b) Thermal resistance and thermal conductivity of commercial
thermal pad before and after using the thermal paste.

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X. Fan et al. Surfaces and Interfaces 46 (2024) 103905

Fig. 3. (a) Raman spectra of the graphite composites under 5mW laser excitation. The inset is the optical image of the samples. (b) Thickness-dependent thermal
resistance of V-GP/PB TIMs.

the composites. [41] to the equation:

Fig. 3(b) shows the total thermal resistance variations with the
different thicknesses of TIMs, and the linear fitting actually correspond

Fig. 4. (a)An illustration of the thermal test platform. (b) The surface temperature recorded at different time for different TIMs. (c)(d)(e) are for the surface
temperature images measured at 0 s, 20 s and 120 s, respectively, which are taken by an infrared thermal camera.

4
X. Fan et al. Surfaces and Interfaces 46 (2024) 103905

l keep the temperature at the bottom of the TIMs consistent, which was
Rtotal = Rc + (2)
κ realized by setting the output power of the ceramic heating plate con­
which means that there is a linear relationship between the whole
thermal resistance and TIM thickness if the TCR keeps constant, and Rc is
the intercept of fitting line on the coordinate. As shown in Fig. 3(b), the
slopes of these two curves are approximately equal and consistent with
theoretical values. [9,42] And the TCR between copper and V-GP/PB
TIMs, which can be calculated by the vertical intercept mentioned
before, drops from 87.96K ⋅ mm2 ⋅ W− 1 to 20.26K ⋅ mm2 ⋅ W− 1. It is
worth mentioning that before the interface treatment, the measured
thermal conductance of V-GP/PB TIMs is close to that of HD90000
owing to the high TCR, which could be improved by the thermal paste to
fill the air gap at the interface. Moreover, it is shown that the TCR plays
an increasing important role with the decrease of TIMs thickness. Before
the surface treatment, the TCR accounts for 18.87 % of the total thermal
resistance when the thickness of TIM is 3.75mm, and this value will raise
to 33.14 % when the thickness is 1.2mm. After the treatment of the
thermal paste, the TCR for the thickness of 3.75mm decreases to 6.61 %.
It should be noted that the TIMs that we selected have a generally larger
thickness than that used in practical applications. [31] Therefore, the
actual proportion of TCR can be predicted to be even larger when the
thickness of TIMs reaches the order of micrometers. [43]
Moreover, we home-designed a thermal test platform to further
demonstrate the effectiveness the interface treatment for heat dissipa­
tion, as shown in Fig. 4(a). The commercial thermal pad mentioned
before (HD90000) with a high through-plane thermal conductivity of
7.5W ⋅ m− 1 ⋅ K− 1 is used here for comparison. Cooler MasterGel PRO was
selected as the thermal paste, and the calibrated thermal conductivity
was 8W ⋅ m− 1 ⋅ K− 1.
When testing the heat dissipation performance of the V-GP/PB TIMs,
we compared it to the HD90000 TIMs with the same size while different
thickness. Both TIMs were placed on a ceramic heating plate and further
placed on top of the substrate. During measurement, it was critical to
stant at 20 W. Thermocouples were placed above the TIMs to measure
the temperature, and the temperature changes over time were plotted in
Fig. 4(b). For V-GP/PB TIMs, the use of the thermal paste significantly
accelerates the heating process, and the top temperature becomes sta­
bilized after approximately 120s. However, it takes around 200s for the
temperature stabilization without the thermal paste. The steady-state
surface temperature of V-GP/PB TIMs treated with the thermal paste
reaches 64◦ C, which is higher than the temperature without thermal
paste (57◦ C). The cyan and yellow triangles in Fig. 4(b) are for the
surface temperature of HD90000 with and without thermal paste
treatment, reaching the steady-state temperatures of 59◦ C and 55◦ C,
respectively. Therefore, the heat dissipation performance of TIMs is
significantly improved after the surface treatment with the thermal
paste. Fig. 4(c), (d) and (e) show the surface temperature distributions of
V-GP/PB TIMs during measurement. It is evident that the surface tem­
perature distribution of TIMs becomes more uniform over time. The
abrupt temperature change in the middle of the TIM is due to the
presence of thermocouples for measuring, which are placed on the top of
device during measurement.
In order to better show the importance of the interface treatment, a
finite element simulation is performed by using a multi-physical field
simulation software (COMSOL). As shown in Fig. 5(a), the heater and
TIM with the size of 2.5cm × 2.5cm and the thickness of 0.8mm are
stacked on a large enough heat sink. For comparison, the thermal pad
used before (HD90000), treated and untreated V-GP/PB TIMs are
applied as TIMs in this simulation. The testing conditions including
heating power (50W ⋅ cm− 2) and ambient temperature (25◦ C) are kept
identical as shown in Fig. 5(a) and Fig. 5(b). Obviously, when the
thermal pad (HD90000) and untreated V-GP/PB TIMs are used as TIMs,
the heater temperature between these two cases is only 1.24◦ C, although
the intrinsic thermal conductivity of V-GP/PB TIMs is larger than that of
HD90000. While after treating the interface between TIM and the

Fig. 5. Finite element simulation of (a) Schematic configuration of COMSOL simulation. (b) Temperature profiles under different configurations. Vertical tem­
perature change profile of HD90000 (c), untreated V-GP/PB TIMs (d) and treated V-GP/PB TIMs (e).

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X. Fan et al. Surfaces and Interfaces 46 (2024) 103905

heater, the TCR will decrease from 87.96K ⋅ mm2 ⋅ W− 1 to 20.26K ⋅ mm2 ⋅ ( )
Qupper + Qlower
W− 1, causing the temperature drop rapidly climbing to 66.45◦ C, which Q= (5)
2
is nearly 50 times higher than that of the untreated TIMs. Vertical
temperature distribution for these three TIMs is shown in Fig. 5(c), (d) ΔT
and (e). It is demonstrated that when applying treated V-GP/PB TIMs, RTIM = (6)
Q
the entire cooling system has a uniform temperature profile, which
means a more excellent ability of heat dissipation. Where κ and A is the thermal conductivity and the cross-sectional
area of the pure copper bar, dT dZ
is the temperature gradient of the
3. Conclusion upper and lower copper bars under steady state, which can be obtained
from measured data. According to the heat conduction formula, the heat
In summary, we studied the interface thermal transport between the through the upper and lower copper bars per unit time can be obtained.
copper substrate and TIMs to further explore the mechanism of interface When the system reaches a steady state, it is Qupper = Qlower. The dif­
treatment in heat transfer. It is experimentally confirmed that after ference between the interface temperature on the upper and lower
treated by thermal paste, the TCR between graphite films and copper copper bars can be acquired by deducing the bars temperature at 8
substrate drops from 87.96K ⋅ mm2 ⋅ W− 1 to 20.26K ⋅ mm2 ⋅ W− 1, thermocouples to the contact interface. When determining whether the
implying the role of surface treatment for the interfacial thermal temperature of the whole system reaches a steady state in the mea­
transport. Besides, in our thermal test platform, the treated TIMs can surement process, if the absolute difference between the heat flux J of
show a more efficient cooling performance than untreated ones by the upper and lower copper bar is controlled within 10 %, we believe
achieving a temperature difference of 7◦ C, which is demonstrated by that the stable state can be approximately reached. The heat flux can be
finite element simulation performed in this study. Our work aids to the calculated by Fourier’s Law:
thermal design in microelectronic circuits by studying the TCR across dT
various interfaces. J = − κ⋅ (7)
dZ

4. Methodology Fig. 1(c) shows that the steady-state temperature data at eight
thermocouples. By linear fitting these 8 data and calculating the tem­
Materials: Polybutadiene adducted with maleic anhydride (Ricon perature at the junction of the upper and lower copper bars, the tem­
130MA8) and hydroxyl terminated polybutadiene (Poly bd® R45V) perature gradient inside the upper and lower copper bars along the Z
were purchased from Cray Valley, France. Graphite films with 25μm axis and the temperature difference at their interface can be obtained.
thickness were provided by Hefei Aoqi Electronic Technology Co., Ltd., The thermal conductivity κ of the sample can be calculated as follows:
China. The coupling agent, dodecyltrimethoxysilane, was offered by d
κsample = (8)
Qufu Chenguang Chemical Co., Ltd., China. The antioxidant, 3-(3, 5- RTIM
ditert‑butyl‑4‑hydroxy-phenyl)-propionate (BASF 1010), was offered by
And d is the sample thickness.
BASF, Germany. All other materials were used with received.
Preparation of the Vertically Oriented Graphite/ Polybutadiene TIMs: A
CRediT authorship contribution statement
certain amount of Poly bd® R45V, Ricon 130MA8, and antioxidant
(3:1:0.024 wt/wt) were mixed, followed by a speed Mixer (Song chong)
Xiaoyu Fan: Methodology, Investigation. Ying Sun: Methodology,
for 1 min under atmospheric pressure (1500 rmp/min) and 3 min under
Data curation. Leyi Huang: Methodology, Investigation. Jiaqiu Xie:
vacuum (1500rmp/min) to get uniformly mixed polymer matrix. The
Software, Methodology. Xiaoliang Zeng: Methodology. Chenhan Liu:
polymer matrix was uniformly coated on the functionalized graphite
Project administration. Lifa Zhang: Writing – review & editing, Inves­
films by vacuum adsorption coater (KJ-6017B) and then placed in the
tigation. Yunshan Zhao: Writing – review & editing, Supervision,
mold for cross stacking. The cross-stacked samples were vacuumed at 25
Investigation, Funding acquisition, Conceptualization.
◦
C for 3 h to remove bubbles and cured at 150 ◦ C for 5 h. Several groups
of samples with different graphite content were prepared by controlling
Declaration of competing interest
the coating thickness of the polymer matrix.
Thermal transport measurement: The top heating module consists of
The authors declare the following financial interests/personal re­
ceramic heating plates. Operating at an externally stable output voltage,
lationships which may be considered as potential competing interests:
a stable heat flow can be generated over the copper bars and TIM. The
Yunshan Zhao reports financial support was provided by National
cooling module at the bottom consists of an inverted "U" shaped square
Natural Science Foundation of China.
copper block immersed in a container of ice water. During the entire
measurement process, the cooling module needs to keep the tempera­
Data availability
ture low, so that the copper bars have a clear temperature gradient. The
ball joint is used to facilitate the sample alignment with the upper and
Data will be made available on request.
lower copper bars. An adjustable mechanical pressure is applied at the
top of the device, which is visualized by a coaxial pressure sensor
mounted at the bottom. Under the action of mechanical pressure, the
Acknowledgements
Heater and upper copper bars can slide freely and vertically on three
fixed posts by linear bearings.
This work was supported by the National Natural Science Foundation
The thermal resistance RTIM of the sample can be obtained by the
of China (Grants No. 12204244) and the Natural Science Foundation of
following formula:
Jiangsu Province (Grant No. BK20210556) and Department of Science
( )
dT and Technology of Jiangsu Province (Grant No. BK20220032). Z.Y.S.
Q1 = − κ⋅A⋅ (3)
dZ upper acknowledges support from the Jiangsu Specially-Appointed Professor
Program and the open funding of the State Key Laboratory of Artificial
( )
dT Microstructure and Mesoscopic Physics.
Q2 = − κ⋅A⋅ (4)
dZ lower

6
X. Fan et al. Surfaces and Interfaces 46 (2024) 103905

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