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Article history: A new quadrupole model is presented to solve the heat transfer equations in a conventional geometry
Received 26 November 2013 used in the measurement of thermal conductivity of thin films by the 3u method. It takes into account
Received in revised form the following aspects often neglected in the previous works: thermal resistance in the heater, anisotropy
27 May 2014
of the thin film, thermal contact resistances and the limited thickness of the sample. The quadrupole
Accepted 7 June 2014
Available online
model allows us also to compare the Cahill and Duquesne formulas and to find their applicability limits.
The average temperature rise is calculated to validate the quadrupole model, it presents a deviation
lower than 3.5% compared to the numerical simulation in the range of frequency from 1 Hz to 10 KHz.
Keywords:
Quadrupole model
© 2014 Published by Elsevier Masson SAS.
3u method
Thermal conductivity
1. Introduction the heater width. For a film thickness far smaller than the heater
width, Lee et al. [3] has given a formula of temperature drop in the
The thin film and the multilayer thin-film structures are critical film in the cross-plane direction. Duquesne et al. [4] has presented
for a wide range of applications in microelectronics, photonics, an explicit analytical formula for solution of the heat diffusion
microelectromechanical systems and thermoelectrics. It is of great equation obtained under Cahill's hypotheses. Moreover, the 3u
importance to know the thermal conductivity of the thin film. The method has been applied to measure the thermal conductivity of
more popular method to measure the thermal conductivity of thin anisotropic thin films [6e12]. Gurrum et al. [6] has demonstrated
films is the so called 3u technique. It utilizes a micro fabricated that the heat transfer in the metal heater has a significant effect on
metal line deposited on the specimen to act as a resistive heater and the measurement of the film conductivity; especially when the
voltage tester. When an alternative current is applied to the heater material has an anisotropic conductivity. Chien et al. [7] has used a
at a frequency u, the periodic heat generated by Joule effect in the heaterethermometer separated system to measure thermal con-
metal heat is of frequency 2u, which leads to a third harmonic in ductivity of anisotropic material. Besides the anisotropy of the
the voltage waveform. This 3u signal can be measured through the material, Borca-Tasciuc et al. [9] have considered the finite sub-
heater and used to estimate the thermal conductivity of the test strate thickness, the anisotropy of the substrate, the existence of the
material. thermal capacity of heater and of a thermal contact resistance. They
Thanks to its advantages of easily building and insensitivity to proposed a differential method instead of a slope method to esti-
the radial heat loss, it is widely used to investigate the dielectric mate the thermal conductivity and investigated the range of
solids, films and also lines at an appropriate dimension [1e14]. The applicability of the slope method as a function of the penetration
analytical expression of 3u method was originally given by Cahill depth and the heater width. Olson [10] applied the thermal
[1,2], who employed the third harmonic of the voltage along a impedance in terms of experimentally measured 3u quantities to
metal line, deposited on top of a dielectric solid to estimate its each component for a multilayered structure, and used the mini-
thermal conductivity. Following to this work, the 3u method was mization algorithm to find the approximate thermal conductivity,
applied to layered structures when the film is much thicker than which removes many limitations of the analytical method. Con-
cerning the measurement frequency, Wang et al. [12] have revealed
that there is a limited frequency range for thermal conductivity
de Lorraine, LEMTA, UMR 7563, Vandoeuvre-
measurement neglecting the heater thickness by a new analytical
* Corresponding author. Universite
s-Nancy F-54500, France.
le solution of the heat conduction equations. The increase of heater
E-mail address: yves.jannot@ensem-inpl.fr (Y. Jannot). thickness reduces the frequency range. Besides the generally
http://dx.doi.org/10.1016/j.ijthermalsci.2014.06.010
1290-0729/© 2014 Published by Elsevier Masson SAS.
T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324 315
referred parameters, heater thermal mass, boundary conditions, The voltage drop along the heater thus can be expressed by the
anisotropy and contact resistance, the influence of some other formula:
parameters on the temperature rise such as the finite heater length
[13] and the measurement pads [14] have been studied to reveal 1
VðtÞ ¼ R0 I0 ð1 þ aR DTDC ÞcosðutÞ þ R0 I0 aR DTAC cosðut þ jÞ
the limits or improve the Cahill analytical model. The approach was 2
extended to nanofluids and nanowires by several authors [15e17]. 1
Although the method was extended to more complex samples, þ R0 I0 aR DTAC cosð3ut þ jÞ
2
most of the analytical expressions are based on the Cahill formula, (3)
taking some of these hypotheses as the thermal mass of the heater
is null, semi-infinite length of the specimen and no thermal resis- The third harmonic of the voltage is
tance inside the metal strip. It would be of great interest to predict
the conditions for which case the Cahill's analytical formula is 1
V3u ðtÞ ¼ R I a DT cosð3ut þ jÞ (4)
appropriate and to improve it to implemented for real size sample 2 0 0 R AC
and limited experimental conditions. In addition, the need of pre- It can be extracted from the voltage waveform using a lock-in
cise measurement of the thin film properties imposes to work with amplifier and also calculated by use of the model of the tempera-
a more precise model. ture rise DTAC which is a function of the thermal properties.
In this paper, we will present a complete model which can be Considering the following hypotheses:
used as a tool to verify the applicability of the simple formulas
(Cahill and Duquesne) to real measurement and to find for example - Semi-infinite thin film (es infinite, Fig. 1)
the range of frequencies in which they are valid. This complete - Infinite width of the substrate (Ls infinite, Fig. 1)
model takes into account the geometry and the finite thickness of - Thermal capacity and the thermal resistance of heater are null
the specimen, the heat transfer in the metal heater, the boundary - No thermal contact resistance between the heater and the film
conditions and the contact resistances. To our knowledge, there is - No heat transfer by convection on the heater
no model taking simultaneously into account all these physical - Uniform heat transfer on the length of the heater
phenomena.
Cahill [1] described the mean temperature of the heater source
2. The 3u method and simplified Cahill model on the surface of test bulk material:
Moreover, Duquesne et al. [4] have presented the exact solution vTr
of the Equation (5): lr ¼ 0 when 0 < y < e0 ; x ¼ 0 and x ¼ b (14)
vx
P0 1 1 iub2 vT1
T¼ Meijer G 0; ; ½ ; ½0; 0; ; 1 ; (8) l1x ¼ 0 when e0 < y < e0 þ e1 ; x ¼ 0 and x ¼ Ls (15)
4plLz 2 2 a vx
Tr ¼ Ar expði2utÞ (26) contact resistance between the heater and thin film (Equation (20))
can be written by the following expressions:
q1 ¼ A1 cos bsn xdx; bsn Ls ¼ np (33) And solve the problem on each side independently:
0
The Fourier transform of the heat fluxes transferred by con- where Zs, M and N are known impedances, refer to Appendix 1.
vection on the heater (Equation (17)) and through the thermal The inverse Fourier transformation in the real space gives:
Fig. 2. Two sides of the system separated at the interface of the heater and the film.
318 T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324
qrse0 0 X ∞
qrse0 n formula (7), the Duquesne formula (8), the proposed quadrupole
Ar ðx; e0 Þ ¼ þ cosðbn xÞ for 0 < x < b (41) model (45) and two different numerical simulations by the soft-
b n¼1
b=2
ware COMSOL:
q1e0 0 X ∞
q1e0 n - A first one in which the supplied electrical power density g0 is
A1 ðx; e0 Þ ¼ þ cosðbsn xÞ for 0 < x < Ls (42) constant: the problem is then linear and corresponds to the
Ls L =2
n¼1 s
quadrupole model.
One can write the equality of the real temperatures for obtaining - A second one in which the supplied current amplitude I0 is
the equations enabling the calculation of 4(x): constant: real case without approximation.
8
> q X∞ q q1e 0 X ∞ q
> rse0 0 þ
> rse0 n
¼ 0
þ
1e0 n
cosðbsn xÞ for 0 < x < b
>
> cosðb n xÞ
< b n¼1
b=2 Ls n¼1
Ls =2
(43)
>
> q1e 0 X ∞ q
>
> 1 0 1e0 n
>
: ¼ þ cosðbsn xÞ for b < x < Ls
hs 4ðxÞ Ls n¼1
L s =2
If 4(x) is known, the coefficients qrse0 0 ; qrse0 n ; q1e0 0 ; q1e0 n can be The thermal characteristics and the dimension parameters are
derived from relation (35) to relation (38). listed in Table 1. The average heater temperature rise Tr , known as
The solution of the Equation (43) can be obtained convention- the 3u component in the voltage calculation (T3u), has been
ally by a finite differences method. The structure of our problem calculated over a range of frequencies varying from 1 to 104 Hz
enables a simplified solution. In fact, the flux density between b and without considering the thermal contact resistance.
Ls is very small compared to the flux density between 0 and b, and The grid size was chosen such that a refined grid leads to the
may therefore be considered uniform. Similarly, the flux density same solution. No convergence problem has been encountered in
between 0 and b is substantially uniform except near b. the test frequency range.
An approximated solution consists in taking the flux density It can be noticed in Figs. 3 and 4 that the simulation considering
4(x) constant on three intervals, such as: g0 constant instead of I0 constant leads to a difference up to 3.5% at
8 the lower frequency. The difference between the quadrupole model
< 41 0<x<a and the COMSOL simulation with g0 constant is lower than 1%. The
4ðxÞ ¼ 42 a<x<b (44) Duquesne model gives a closer value to COMSOL simulation than
:
43 b < x < Ls the Cahill model when the frequency is higher than 100 Hz.
However, these two models present a significant deviation to the
The equation verified by f(x) is then transformed into a linear
COMSOL simulation especially at low frequency. The difference can
system of 3 equations with 3 unknown parameters by writing the
be explained by the hypothesis of the semi-infinite medium
equality of the average temperature on the three intervals [0, a], [a,
considered for the film.
b] and [b, Ls] (cf. Appendix).
The optimum value of a has been chosen by realizing simula-
tions of the analytical model for several values between 0 and 1. 5. Limits of the Cahill model
These analytical results have then been compared to numerical
simulations realized with COMSOL considering a constant value for 5.1. Film thickness e1
g0. It was found that the value a ¼ 0.6b minimizes the differences
between the two simulations. Fig. 5 represents the real part of the 3u component of the
The average temperature rise in the metal strip is consequently temperature rise for different layers thickness calculated with our
obtained by complete system: analytical model and with the Cahill formula with the assumption
of the semi-infinite substrate for three different values of the film
41 a þ 42 ðb aÞ sinhðg0 e0 Þ sinh2 ðg0 e0 Þ thermal conductivity l1 ¼ 1 W m1 K1, l1 ¼ 10 W m1 K1 and
Tr ¼ M0 þ M0 g0
b g0 e0 g20 e0 l1 ¼ 100 W m1 K1.
!
g sinhðg0 e0 Þ
þ 02 1 expði2utÞ Table 1
lr g0 g0 e0 Thermal characteristics and dimension parameters of the system.
Fig. 3. Amplitude of T3u and its deviation from the COMSOL simulation with I0 constant.
Fig. 4. Real part of T3u and its deviation from the COMSOL simulation with I0 constant.
For each thickness of the film, relation (6) enables the calcula- formula with the same input electrical power for two films
tion of the frequency such as the penetration depth is exactly equal with thermal conductivity l1 ¼ 1 W m1 K1 and
to the film thickness. These frequencies have been represented by a l1 ¼ 100 W m1 K1.
point on Fig. 5. It is also the lower frequency enabling the use of Fig. 6 shows that the Cahill model leads to a satisfying repre-
Cahill formula to estimate the thermal conductivity according to sentation of T3u only if the heater thickness is lower than 200 nm
the hypothesis of semi-infinite substrate. for l1 ¼ 1 W m1 K1 and lower than 2 mm if l1 ¼ 100 W m1 K1.
Fig. 5 shows that:
- For the film lower than certain thickness, the slope method 5.3. Effect of the heater half width b
based on Cahill formula cannot be used to estimate the thermal
conductivity since the linear zone becomes very short and may The real part of the T3u for different heater width, 1 mm, 10 mm
even disappear for the lower thicknesses. and 100 mm is also studied applying our quadrupole model and the
- Relation (6) enables a rather good prediction of the beginning of Cahill formula with the same input electrical power for two
the linear zone and can be used to calculate the lower value of different values of film thermal conductivity as described before.
the frequency that can be used when applying the Cahill Fig. 7 shows that:
formula.
- The lower limit of the frequency interval on which the tem-
perature is a linear function of the frequency does not depend
5.2. Heater thickness e0 on the strip width.
- The upper limit of this interval decreases when the strip width
Fig. 6 represents the real part of T3u for different heater thick- increases. A too large strip will not permit the use of the Cahill's
nesses calculated from our quadrupole model and the Cahill model for thermal conductivity estimation.
Fig. 5. Real part of T3u for different film thicknesses and conductivities.
320 T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324
5.4. Influence of the contact resistance Rrc 5.5. Estimation error using Cahill model
Fig. 8 represents the temperature rise in the heater for different Fig. 9 represents the real part of a COMSOL simulated curve T3u
values of the contact resistances between the heater and the thin on the frequency interval 0.01 Hze1 MHz, where the reference
film. value of the film is l1 ¼ 1 W m1 K1. The thermal conductivity has
Fig. 8 shows that: been estimated from the slope of different frequency interval
(Cahill method) and also by minimization of the quadratic errors
- For a film thermal conductivity l1 ¼ 1 W m1 K1, T3u is between the experimental values and the values calculated by the
insensitive to the thermal contact resistance if it is lower than Duquesne's formula. The estimated values of the thermal conduc-
107 K W1 m2. tivity for each interval are reported in Fig. 9.
- For a layer thermal conductivity near l1 ¼ 100 W m1 K1, T3u is The first point is the lower frequency limit to apply the Cahill
insensitive to the thermal contact resistance only if it is lower formula, where the penetration depth equals the film thickness. It
than 108 K W1 m2. Nevertheless, it must be remarked than shows that in this particular case the estimation error on l using the
the slope remains the same. Cahill model may reach 30% even on a frequency interval on which
Fig. 8. Real part of T3u for different values of the contact resistance Rrc.
T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324 321
sinhðgn e0 Þ
F* ¼ Y ¼ G0 (A3)
gn
and
8
>
> Zb
>
> sinhðg0 e0 Þ sinhðg0 e0 Þ
>
> F*0 ¼ g0 dx ¼ g0 b
>
> g g0
< 0
0
(A4)
>
> Zb
>
> sinhðgn e0 Þ
>
>
>
> F*n ¼ g0 cos bn xdx ¼ 0
: gn
0
Fig. 9. Thermal conductivities (W m1 K1) estimated by the Cahill and Duquesne
2. Connections of the quadrupole relationship on two sides
formulas on different frequency intervals.
where qrse0 0 and qrse0 n are the abbreviations of qrse0 ð0; e0 Þ and The parameter A is equal on the two sides and therefore:
qrse0 ðbn ; e0 Þ.
On the substrate side, the Fourier transformation of the heat
flux is:
8
>
> ZLs
>
>
>
> F ¼ 4ðxÞdx ¼ 41 a þ 42 ðb aÞ þ 43 ðLs bÞ
>
>
s0
< 0
(A12)
>
>
>
> ZLs
>
> sinðan aÞ sinðan bÞ sinðan aÞ sinðan bÞ
>
> F ¼ 4ðxÞcosðan xÞdx ¼ 41 þ 42 43
: sn an an an
0
" #
a aðM0 þ N0 Þ X ∞
2Zsn sin2 ðan aÞ X ∞
2ðM þ NÞsin2 ðbn aÞ
41 Zs0 þ þ þ þ
Ls b n¼1 a2n aLs n¼1 b2n ab
" #
X∞ 2Zsn sinðan bÞsinðan aÞ sin2 ðan aÞ X∞
b a ðb aÞðM0 þ N0 Þ 2ðM þ NÞsin2 ðbn aÞ (A15)
42 Zs0 þ þ þ
Ls b n¼1 a2n aLs n¼1 b2n ab
" #
Ls b X ∞
2 sinðan bÞsinðan aÞ M F
43 Zs0 Zsn 2
¼ 0 *0
Ls n¼1 an aLs b
" #
∞ 2Zsn sinðan bÞsinðan aÞ sin2 ðan aÞ
a aðM0 þ N0 Þ X X∞
2ðM þ NÞsin2 ðbn aÞ
41 Zs0 þ þ þ
Ls b n¼1 a2n Ls ðb aÞ n¼1 b2n bðb aÞ
" #
Z ðb aÞ ðb aÞðM0 þ N0 Þ X ∞
2Zsn ðsinðan bÞ sinðan aÞÞ2 X ∞
2ðM þ NÞsin2 ðbn aÞ
42 s0 þ þ þ þ (A16)
Ls b n¼1 a2n Ls ðb aÞ n¼1 b2n bðb aÞ
" #
∞ 2Zsn sinðan aÞsinðan bÞ sin2 ðan bÞ
Ls b X M F
43 Zs0 þ 2
¼ 0 *0
Ls n¼1 a n L s ðb aÞ b
T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324 323
" # Ze0
1 sinhðgn e0 Þ coshðgn e0 Þ 1
a X ∞
2sn sinðan aÞsinðan bÞ qr ¼ qr dy ¼ k1 þ k2 þS (A23)
41 Zs0 þ e0 gn e0 gn e0
Ls n¼0 a2n Ls ðLs bÞ 0
" #
Substituting k1 and k2 to (A23):
ba X ∞ 2Zsn sinðan aÞsinðan bÞ sin2 ðan bÞ
42 Zs0 þ Zsn þ
Ls a2n Ls ðLs bÞ sinhðgn e0 Þ coshðgn e0 Þ 1 sinhðgn e0 Þ
n¼1 qr ¼ qr0 Fr0 þ S 1
" # gn e0 lgn e0
2 gn e0
Ls b 1 X ∞
2Zsn sin2 ðan bÞ
43 Zs0 þ þ ¼0 (A24)
Ls hs n¼1 a2n Ls ðLs bÞ
Substituting (A5) and the definition of S to (A24):
(A17)
The following parameters are defined to simplify the Equations sinhðgn e0 Þ 1 sinhðgn e0 Þ
qr ¼ qm þ 1 G0 (A25)
(A15), (A16) and (A17). gn e0 lr gn
2 gn e0
The above three equations become: where qm0 and qmn are the zero and n order of the expression qm.
For the expression of qm0 and qmn, they can derive from the
A* a* ðM0 þ N0 Þ * 1
Equation (A5):
41 Zs0 a* þ * þ þ D þ 4 2 Zs0 b* a*
a b* a* =b* 8
>
> sinhðg0 e0 Þ
C * A* a* * 1 < qm0 ¼ M0 ð41 a þ 42 ðb aÞÞ þ M0 g0 b
>
þ þ 1 ðM 0 þ N 0 Þ D g0
a* b* a* =b* (A27)
>
> sinðbn aÞ
C * M F >
: qmn ¼ Mn ð41 42 Þ
þ 43 Zs0 1 b* * ¼ 0 *0 bn
a b
(A18)
The inverse transformation of qr can be calculated by:
C * A* a* ðM0 þ N0 Þ D* qr 0 X ∞
qr n
41 Zs0 a* þ * *
þ *
Ar ¼ þ cosðbn xÞ (A28)
b a b 1 a* =b* b b=2
n¼0
a* B* þ A* 2C *
þ 42 Zs0 b* a* þ 1 * ðM0 þ N0 Þ þ The average temperature on 0 < x < b can be calculated:
b b* a*
D*
C B
* * M F !
þ þ 43 Zs0 1 b* þ * ¼ 0 *0 Zb Zb
1 a* =b* b a* b 1 1 qr0 X ∞
qrn qr
Ar ¼ Ar dx ¼ þ cosðbn xÞ dx ¼ 0
(A19) b b b n¼0
b=2 b
0 0
(A29)
* C*
C * B*
41 Zs0 a *
þ 42 Zs0 b* a* þ * Substituting (A26) and (A27) to (A29), the average temperature
1b 1b
*
(A20) coefficient can be obtained:
1 B
þ 43 Zs0 1 b* þ þ ¼0
hs 1 b*
41 a þ 42 ðb aÞ sinhðg0 e0 Þ
Solving the Equations (A18), (A19) and (A20) we can have the Ar ¼ M0 þ M0 g0
b g0 e0
expression for 41, 42 and f3 .
The average temperature and the heat flux can be derived from
the Equations (30) and (31).
qr ðbn ; 0Þ ¼ k1 þ S
(A21)
Fr ðbn ; 0Þ ¼ lr gn k2
Therefore,
F
k1 ¼ qr0 S; k2 ¼ r0 (A22)
l r gn
The average value of qr between 0 and e0 is: Fig. A1. Simplified quadrupole schema for the heater.
324 T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324
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Nomenclature
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