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International Journal of Thermal Sciences 86 (2014) 314e324

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International Journal of Thermal Sciences


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

Theoretical study of the limits of the 3u method using a new complete


quadrupole model
Tingting Ding a, b, Yves Jannot a, b, *, Alain Degiovanni a, b
a
Universit
e de Lorraine, LEMTA, UMR 7563, Vandoeuvre-l
es-Nancy F-54500, France
b
CNRS, LEMTA, UMR 7563, Vandoeuvre-l es-Nancy F-54500, France

a r t i c l e i n f o a b s t r a c t

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:

Considering the device in Fig. 1, a thin metal strip of length Lz, of Z∞


P0 sin2 ðabÞ 1
width 2b and of thickness e0 is deposited onto the thin film surface T¼ qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
 da (5)
plbLz a2 b a2 þ i2u a
to act as both a heater and a temperature sensor. An AC current is 0
supplied to the strip with the angular modulation frequency u and
the amplitude I0. Heat is generated in the heater by Joule effect, and where P0 the electrical power produced in the heater, l and a are
the temperature rise is proportional to the electrical power, it the thermal conductivity and the thermal diffusivity of the
contains a constant part and a sinusoidal part: measured material, b is the half width of the heater.
The penetration depth can be calculated by:
DTðtÞ ¼ DTDC þ DTAC cosð2ut þ jÞ (1)
pffiffiffiffiffiffiffiffiffiffiffi
ep ¼ a=2u (6)
where DTDC and DTAC are respectively the two temperature am-
plitudes due to the constant and sinusoidal parts. j is the phase if it is much larger than the heater half width, the solution of
shift between the current and the temperature. Equation (5) can be written approximately as [1]:
Since the strip resistance varies linearly with the temperature, it
can be written as: " rffiffiffiffiffiffi ! #
P0 2u p
Tz ln b þhi (7)
RðtÞ ¼ R0 ð1 þ aR DTÞ ¼ R0 ½1 þ aR DTDC þ aR DTAC cosð2ut þ jÞ plLz a 4
(2)
where h is a constant. Duquesne et al. [4] have further demon-
where aR is the temperature coefficient of the heater. strated that h ¼ 0.923.

Fig. 1. Experimental device used for the 3u method.


316 T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324

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

Equation (7) is the commonly used expression by the other vTs


authors for the thermal conductivity estimation, although it has ls ¼ 0 when e0 þ e1 < y < ∞; x ¼ 0 and x ¼ Ls (16)
vx
much more limits to implement compared to Equation (8). We will
call the Equations (7) and (8) respectively the Cahill formula and On the heater surface and the thin film surface, the heat transfer
the Duquesne formula in the following sections. is described by:
If the penetration depth is further larger than the half heater
vTr
width, Duquesne et al. [4] suggest approximating the relation (8) lr ¼ hr ðTr  Text Þ 0 < x < b; y ¼ 0 (17)
vy
as:
rffiffiffiffiffiffi ! !
P 2u 3 p vT1
Tz 0 ln b þ  0:5772  i for u/0 (9) l1y ¼ hs ðT1  Text Þ b < x < Ls ; y ¼ e0 (18)
plLz a 2 4 vy
The constancy of the heat transfer coefficient may be assumed
P0 as a simplification in relation (17) and (18). It is acceptable when
Tz qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
 ð1  iÞ for u/∞ (10) forced convection is assumed, and it may be acceptable also for
2lLz 2iub2 a natural convection and radiative exchange if the surface tempera-
ture variations are relatively small.
It can be seen that the approximated relation (9) is similar to On the interface between the heater and the thin film, the heat
the Cahill formula (7) for low frequency. Theoretically the thermal flux is continuous but not the temperature due to thermal contact
conductivity can be estimated either by the real part or imaginary resistance Rrc.
part of the temperature rise (relation (7) or (9)). More often, the so
called “slope method” based on the linear relation between the vTr vT
lr ¼ l1y 1 0 < x < b; y ¼ e0 (19)
real part of the temperature rise and ln(u) is used to estimate the vy vy
thermal conductivity of the film. Despite the corrections to the
 
slope method, i.e. differential technique [8], these relations can vT1
Tr  T1 ¼ Rrc  l1y 0 < x < b; y ¼ e0 (20)
only be applied for infinite thickness samples and for narrow metal vy
heater. Furthermore, they did not consider the heater specific heat
and thermal conductivity or the thermal contact resistance On the interface between the thin film and the substrate, there is
simultaneously. A more precise model is required to take these also a thermal contact resistance Rsc.
properties into account, which we will present in the following
vT1 vTs
section. l1y ¼ l2 0 < x < Ls ; y ¼ e0 þ e1 (21)
vy vy
 
3. Quadrupole model vT1
T1  Ts ¼ Rsc  l1y 0 < x < Ls ; y ¼ e0 þ e1 (22)
vy
A complete model has been developed, which takes into account On the bottom of the substrate:
the heat transfer in the heater, the anisotropy of the film and its
finite thickness as well as the thermal contact resistances. y/∞ 0 < x < Ls (23)
The temperature distributions in the heater, in the thin film and
in the substrate are firstly calculated using the two-dimensional The initial temperature is:
heat equations. Since the length is much larger than the width of
T ¼ Text t¼0 (24)
the heater, it can be considered as a two-dimensional problem in
the Cartesian coordinates shown in Fig. 1. The governing equations where Tr, T1 and T2 are the temperatures in the heater, the film and
for heat conduction in the heater, thin film and the substrate are the substrate, respectively, ar, a1 and a2 are their thermal diffusivity,
given by and l1x and l1y are the thermal conductivities in direction x and y of
an anisotropic thin film .
v2 Tr v2 Tr 1 1 vTr
þ 2 þ g¼ (11) The heat source can be written:
vx2 vy lr ar vt
1
P ¼ R0 I02 cos2 ðutÞ ¼ R I 2 ð1 þ cosð2utÞÞ (25)
l1x v2 T1 v2 T1 1 vT1 2 00
þ ¼ (12)
l1y vx2 vy2 a1 vt The solution of the linear problem is the sum of a transient
problem and a periodic problem, whose sources are P0 ¼ 1=2R0 I02
v2 Ts v2 Ts 1 vTs and P0cos(2ut) respectively. The volumetric power density consists
þ 2 ¼ (13) consequently in two terms g0 and g0cos(2ut).
vx2 vy as vt
The solution of the system (11e13) for the steady periodic
Only the right part of the geometry (x  0) is considered for regime can be obtained by associating an imaginary problem with a
calculation due to its symmetry. On the symmetry axis and on the source ig0sin(2ut). The global complex source to be considered is
right border of the structure, an adiabatic condition is applied. then g0exp(i2ut). The complex solution can thus be written in the
The boundary conditions for the proposed structure are: following form:
T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324 317

Tr ¼ Ar expði2utÞ (26) contact resistance between the heater and thin film (Equation (20))
can be written by the following expressions:

T1 ¼ A1 expði2utÞ (27) Fr0 ¼ hr qr0 (35)

Ts ¼ As expði2utÞ (28) qre0  qrse0 ¼ Rrc Fre0 (36)

where Ar ¼ jTrjexp(i4r), A1 ¼ jT1jexp(i41) and As ¼j Tsjexp(i4s).


where hr is the convection coefficient on the heater.
To solve the Equation (11) for the heater, we will use the cosine
The quadrupole schema represent the whole system is
Fourier transformation:
shown in Fig. 2, where the volumetric power density g0 is sup-
posed to be uniform and time independent (cf. x1 in the
Zb
Appendix).
qr ¼ Ar cos bn xdx; bn b ¼ np (29) In Fig. 2, Z1 ¼ A  1/C, Z2 ¼ Z1, Z3 ¼ 1/C;qr0 and Fr0 are the ab-
0 breviations of qr(bn,0,u) and Fr(bn,0,u) respectively; qre0 and Fre0
The solution of Equation (11) becomes: are the abbreviations of qr(bn,e0,u) and Fr(bn,e0,u) respectively;
Z11 ¼ cosh(ane1)  1/l1ansinh(ane1); Z12 ¼ Z11; Z13 ¼ 1/
qr ðbn ; y; uÞ ¼ k1 coshðgn yÞ þ k2 sinhðgn yÞ þ S (30) l1ransinh(ane1); Z∞ ¼ 1/l2a2n ; where bsn ¼ np/Ls,
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi a1n ¼ b2sn þ i2u=a1 , a2n ¼ b2sn þ i2u=a2 .
where S ¼ 1=g2n 1=lr G0 , gn ¼ b2n þ ði2u=ar ÞG0 is the Fourier
q1e0 and Fse0 are the abbreviations of q1(b1n,e0,u) and
transformation of g0
Fs(b1n,e0,u).
And the heat flux is expressed by:
For the Equation (11), the Fourier transform was realized on [0,
b] on the x coordinate to obtain the quadrupolar relationship
Fr ðbn ; y; uÞ ¼ lr gn ðk1 sinhðgn yÞ þ k2 coshðgn yÞÞ (31)
between the temperature and the heat flux in the heater. It is
The relationship between these two formulas can be written in a different from that on the substrate side carried out along the x
quadrupole form according to the approach proposed by Maillet direction from 0 to Ls. We can't connect the two sides by the
et al. [11]: quadrupole schemas because they have two Fourier trans-
formations with different eigenvalues: bn s bsn and thus
      
qr ðbn ; 0; uÞ A B qr ðbn ; e0 ; uÞ X qrse0 sq10 .
¼  (32) In order to solve this problem, we will use the heat flux method,
Fr ðbn ; 0; uÞ C D Fr ðbn ; e0 ; uÞ Y
which supposes the flux density f(x) at y ¼ e0 is known between
whereA ¼ D ¼ cosh(gne0), C ¼ lrgnsinh(gne0), B ¼ sinh(gne0)/lrgn , 0 and Ls. We can thus calculate the integral transformations of f(x)
X ¼ G0 coshðgn e0 Þ  1=lr g2n , Y ¼ G0sinh(gne0)/gn respectively. at the heater and the film sides:
In the quadrupole model, the effect of the heater thermal
characteristics and dimension is described by several impedances Zb
as a function of frequency instead of neglecting it in the Cahill and Fre0 ¼ 4ðxÞcosðbn xÞdx (37)
Duquesne formulas. 0
The Equations (12) and (13) for the thin film and substrate can
be solved using Equations (27) and (28) and then applying cosine ZLs
Fourier transformation:
Fse0 ¼ 4ðxÞcosðbsn xÞdx (38)
ZLs 0

q1 ¼ A1 cos bsn xdx; bsn Ls ¼ np (33) And solve the problem on each side independently:
0

qrse0 ¼ MF0  ðM þ NÞFre0 (39)


ZLs
qs ¼ As cos bsn xdx; bsn Ls ¼ np (34) q1e0 ¼ Zs Fse0  ðM þ NÞFre0 (40)
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.

(45) Parameters Symbols Values

Thermal conductivity of nickel (W m1 K1) lr 87.8


The detailed calculation this temperature and the expression of
Thermal conductivity of SiO2 film (W m1 K1) l1 1.38
M0 can be found in the Appendix. Thermal conductivity of Si substrate (W m1 K1) l2 126
Volume thermal capacity of nickel (J m3 K1) rcpr 3.9  106
4. Comparison with other models Volume thermal capacity of SiO2 (J m3 K1) rcp1 1.639  106
Volume thermal capacity of Si (J m3 K1) rcp2 1.638  106
Width of metal strip (nm) e0 200
To validate our model, we have calculated the temperature rises Width of film (mm) e1 100
with a heater, film and substrate structure using expression (45). Half width of the metal strip (mm) b 10
We have considered a heater in nickel, a film in SiO2 and a substrate Half width of substrate (mm) Ls 5
in Si, as done by Jacquot et al. [13]. The comparison is carried out by Convection coefficient on strip (W m2 K1) h0 5
Convection coefficient on film (W m2 K1) hs 5
comparing the temperature rise with four methods: the Cahill
T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324 319

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

Fig. 6. Real part of T3u for different heater thicknesses.

Fig. 7. Real part of T3u for different heater widths.

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.

Fig. 5a can be simplified as shown in Fig. A2.


The expressions of qm and qrse0 are derived:
the curve seems to be rather linear such as the one used for (
calculating l14. At high frequency, the Duquesne formula is much qm ¼ MðFre0  F* Þ
(A5)
more precise than the Cahill's one. qm ¼ NFre0 þ qrse0

qrse0 ¼ MF*  ðM þ NÞFre0 (A6)


6. Conclusion
where M ¼ 1=ðð1=Z3 Þ þ ð1=Z1 þ 1=hr ÞÞ; N ¼ Z2 þ Rrc :
This new quadrupole model allows us to calculate the temper-
Therefore,
ature rise showing a deviation lower than 3.5% compared to the
values calculated by COMSOL simulation considering the temper-
(
qrse0 ð0; e0 Þ ¼ M0 F*0  ðM0 þ N0 ÞFre0 ð0; e0 Þ
ature coefficient of resistance on the full range of frequency. The (A7)
qrse0 ðbn ; e0 Þ ¼ ðM þ NÞFre0 ðbn ; e0 Þ
largest part of the error comes from the approximation g0 constant.
The error is less than 1% when comparing our model results with
the COMSOL results neglecting the temperature coefficient in the where M0, N0 are the zero order of the impedance M and N.
power density calculation. This proves that dividing the heat flux The complete impedance on the film and substrate side shown
into three parts on the interface of the heater and thin film to Fig. 5b can be rewritten:
connect the quadrupole solutions of the two sides leads to a good
1
precision and reduces significantly the time calculation. Zs ¼ Zs1 þ 1
(A8)
This quadrupole model has been used to highlight the limits of Zs3 þ Zs2 þR1sc þZ∞
the Cahill model and to show that for high frequencies the
The heat flux between the heater and the film on the domain [0,
Duquesne relation is much more precise than the Cahill one. It may
Ls] can be rewritten with three values:
further be used to obtain a more precise estimation of the film
8
thermal conductivity than with the slope method based on Cahill's < 41 0<x<a
model. 4ðxÞ ¼ 42 a<x<b (A9)
:
43 b < x < Ls

Appendix The Fourier transformation on the heater side can be written:


8
1. Establishment of the quadrupole relation with uniform internal >
> Zb
>
>
source >
> Fr0 ¼ fðxÞdx ¼ f1 a þ f2 ðb  aÞ ¼ Fre0 ð0; e0 Þ
>
>
< 0
A simplified schema for the heater is possibly presented by >
> Zb
>
> ðf  f2 Þsinðbn aÞ
Fig. A1. >
>
> Frn ¼
> fðxÞcosðbn xÞdx ¼ 1 ¼ Fre0 ðbn ; e0 Þ
The qr0 and Fr0 are calculated from: : bn
0
8    
> Z1 Z1 Z2 (A10)
> q
> r0 ¼ 1 þ q þ Z þ Z þ Fre0  Z1 F*
< Z3 re0 1 2
Z3 We can calculate the A on the heater side:
  (A1)
>
> 1 Z
>
:Fr0 ¼ qre0 þ 1 þ 2 Fre0  F*
Z3 Z3 8
> qrse 0 X ∞ q
rse0 n sinðbn aÞ
>
> Ar 0;a ¼ 0
þ
       >
>
qr0 A B qre0 Z1 F* < b n¼1
b=2 bn a
¼  (A2) (A11)
Fr0 C D Fre0 F* > qrse 0 X ∞ q
>
> rse0 n sinðbn aÞ
>
> A ¼ 0

Comparing the Equation (12) in the paper to (A2), we can : r a;b
b b=2 bn ðb  aÞ
n¼1
deduce:
322 T. Ding et al. / International Journal of Thermal Sciences 86 (2014) 314e324

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

We can calculate the A on the substrate side: 8


>
> Ar 0;a ¼ A10;a
>
>
>
>
8 <
> q X∞
q1n sinðan aÞ Ar a;b ¼ A1a;b (A14)
>
> A10;a ¼ 10 þ >
>
> >
>
>
> L s Ls =2 an a >
> 1
>
> n¼1
: hs 4 ¼ A1 b; Ls
>
>
>
< q X∞
q1n sinðan bÞ  sinðan aÞ
3
A1a;b ¼ 10 þ (A13)
>
> L s n¼1 s
L =2 an ðb  aÞ
>
>
>
>
>
> q10 X q1n sinðan bÞ

>
>
: A1 b; Ls ¼ Ls 
>
Ls =2 an ðLs  bÞ
Substituting (A11) and (A13) for the
n¼1 Ar 0;a ; A10;a ; Ar a;b ; A1a;b and A1b;Ls , we will have the following
equations:
where q10 ¼ Zs0Fs0; q1n ¼ ZsnFsn. Zs0 and Zsn are the zero and n order
of the impedance Zs.

" #
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 zero and n order expression of qr can be rewritten:


a * b X∞
2 sin2 ðan aÞ X∞
2 sin2 ðan bÞ
a* ¼ ; b ¼ ; A* ¼ Zsn ; B* ¼ Zsn ; 8  
Ls Ls ðan Ls Þ2
ðan Ls Þ2 >
> sinhðg0 e0 Þ 1 sinhðg0 e0 Þ
n¼0 n¼0 >
> q ¼ q þ 1  G00
< r0 g0 e0 m0
lr g20 g0 e0
>   (A26)
X

2 sinðan aÞsinðan bÞ X∞
2ðM þ NÞsin2 ðbn aÞ >
> sinhðgn e0 Þ 1 sinhðgn e0 Þ
*
C ¼ Zsn ; D* ¼ > q
: rn ¼ qmn þ 1  G0n
2 gn e0 lr g2n gn e0
n¼0 ðan Ls Þ n¼0 b2n b2

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 .

3.. Calculation of the average temperature in the heater

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

[14] Zh.X. Zong, Zh.J. Qiu, Sh.L. Zhang, R. Streiter, R. Liu, A generalized 3u method
for extraction of thermal conductivity in thin films, J. Appl. Phys. 109 (2011)
063502.
[15] L. Qiu, D.W. Tang, X.H. Zheng, G.P. Su, The freestanding sensor-based 3u
technique for measuring thermal conductivity of solids: principle and ex-
amination, Rev. Sci. Instrum. 82 (2011) 045106.
[16] H.F. Lee, B.A. Samuel, M.A. Haque, In-plane thermal conductance measure-
ment of one-dimensional nanostructures, J. Therm. Anal. Calorim. 99 (2010)
495e500.
[17] M.M. Rojo, S. Grauby, J.M. Rampnoux, O. Caballero-Calero, Fabrication of
Bi2Te3 nanorwire arrays and thermal conductivity measurement by 3u-
scanning thermal microscopy, J. Appl. Phys. 113 (2013) 054308.

Fig. A2. Advanced simplified quadrupole schema the heater.

Nomenclature
References
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