High Temperatures ^ High Pressures, 2001, volume 33, pages 17 ^ 25

15 ECTP Proceedings pages 689 ^ 697

DOI:10.1068/htwu184

An estimation of thermophysical properties of layered

materials by the laser-flash method

Wolfgang Hohenauer
Austrian Research Centre Seibersdorf, A-2444 Seibersdorf, Austria; fax: +43 2254 780 3366;
email: wolfgang.hohenauer@arcs.ac.at
Libor Vozär
Constantine the Philosopher University, Tr. A Hlinku 1, SK-94974 Nitra, Slovakia; fax:
+421 87 6511243; email: vozar@uvt.uniag.sk
Presented at the 15th European Conference on Thermophysical Properties, Wu«rzburg, Germany,
5 ^ 9 September 1999

Abstract. An investigation of two-layered and three-layered systems by the flash method has
been carried out. Because of the behaviour of the material analysed, the theory considers two-
layered and three-layered composites with the ideal thermal contact described by zero thermal
contact resistance. The data reduction algorithm is introduced and results are given of an estima-
tion of the thermal diffusivity of alumina (aluminium oxide, Al2 O3) on copper/alumina layers.
An estimation of the thermal diffusivity of one layer requires, besides the knowledge of other
relevant properties (density, heat capacity, and thickness of components), knowledge of the thermal
diffusivity of the remaining layer(s). The way the error in the known thermal diffusivity influences
the error in the unknown thermal diffusivity estimation is analysed. The proposed approach, which
indicates error propagation and estimates the accuracy limits, is applied to a two-layered system.

1 Introduction
The use of layered materials, especially coatings on substrates, has increased in a number
of applications, such as thermal barriers, emissivity controls, electric insulation and
wear, and erosion and corrosion resistance protection. Because such systems have been
utilised under different thermal conditions, knowledge of their thermophysical properties
is of great importance. One may study contact thermal resistance between layers, indicat-
ing the quality of the layered composite. In-situ measurements on layered systems allow
one to test how the thermophysical properties (the thermal conductivity and the thermal
diffusivity) of components differ from the values received for bulk materials.
On the other hand, for several practical reasons, it is necessary to form a layered
composite during a photothermal measurement. An additional layer may be placed on a
homogeneous sample to limit the temperature rise of the exposed face and to improve
absorption ability, or to prevent direct penetration of the heat-pulse radiation energy in the
case of semitransparent media. Some measurements, such as the study of liquids, powders,
and melts, involve the use of a cell as a sample holder, which should be considered during
data analysis.
It has been demonstrated that the laser-flash technique (Parker et al 1961), primarily
developed for the measurement of the thermal diffusivity of homogeneous materials, is
suitable for studying layered structures (Balageas 1989; Maglic̈ and Taylor 1992). In the
flash method, the front face of a disk-shaped sample is subjected to a pulse of radiant
energy coming from a laser. If the material boundaries are flat and parallel to the sample
front and rear surfaces and if there are no heat losses from the radial surface, one-dimen-
sional heat transfer occurs across the sample. By analysis of the resulting temperature rise
on the opposite (rear) face of the sample any thermophysical property (thermal diffusiv-
ity of one layer, or the thermal contact resistance) can be computed.
We present measurements of the thermal diffusivity on two-layered and three-layered
copper/alumina composites using the flash method. Data reduction and estimation of
18 W Hohenauer, L Vozär
15 ECTP Proceedings page 690

the desired thermal diffusivity of one layer were performed by means of a nonlinear
least-squares fit of the recorded rear-face temperature rise versus time data by an
appropriate theoretical curve.
The determination of the thermal diffusivity of a component on layered systems is a
dependent measurement. An estimation of the thermal diffusivity of one layer requires in
addition knowledge of other relevant properties (density, heat capacity, and thickness of
components) in order to determine the thermal diffusivity of the remaining layer(s). Errors
in the measurement of these additional parameters are propagated through the data
reduction and result in error in the thermal diffusivity determination. Our objective was
to analyse how the inaccuracy of the known thermal diffusivity influences the accuracy of
the unknown thermal diffusivity estimation. Here we propose an approach for estimating
measurement limits. The proposed methodology is applied to copper/alumina two-layered
systems and some quantitative results are given here.

2 Theory
2.1 Two-layered composite
The model assumes one-dimensional heat flow through the two-layered sample that con-
sists of layers of thicknesses e1 and e2 (figure 1). We consider good thermal contact
between the layers: zero thermal contact resistance, uniform and constant thermal prop-
erties and densities of both layers, and that the front face (at x ˆ ÿe1) is uniformly
subjected to the instantaneous heat pulse with the heat Q supplied to the unit area. If the
sample is thermally insulated one may utilise the theory described in detail elsewhere
(Lee H J 1975; Lee T Y R 1977). In the case of non-ideal experimental conditions, ie
when heat losses from the front and rear faces should be taken into account, appropriate
boundary conditions include a heat flux term with the heat transfer coefficients h1 and
h2 . The expression for the transient temperature rise, T ˆ T(x, t), in the sample can be
obtained by solving the heat conduction equation for each layer:
q2 Ti …x, t† 1 qTi …x, t†
ˆ , i ˆ 1, 2 , (1)
qx 2 ai qt
with the initial value
Ti …x, 0† ˆ 0 , (2)
and the boundary conditions
qT1 …ÿe1 , t†
ÿk1 ˆ Qd…0† ÿ h1 T1 …ÿe1 , t† , (3)
qx
T1 …0, t† ˆ T2 …0, t† , (4)

qT1 …0, t† qT …0, t†

k1 ˆ k2 2 , (5)
qx qx
qT2 …e2 , t†
k2 ˆ ÿh2 T2 …e2 , t† . (6)
qx

ÿx ÿe1 0 e2 x

h1 h2 Figure 1. Diagram of two-layered sample.

Thermophysical properties of layered materials 19
15 ECTP Proceedings page 691

The problem [equations (1) ^ (6)] is negotiable by the Green's function approach, as
well as by utilising the Laplace transform technique (Oëzisik 1980) where, following Lee's
notation (Lee 1975), the dimensionless temperature rise at the rear face can be written
in the following form (Sweet 1989):  
g2k t
X1 exp ÿ
T…e2 , t† o21 Z22
y…t† ˆ ˆ 2…1 ‡ PU† . (7)
T1 kˆ1
d0 ‡ de
Here T1 is the adiabatic limit temperature, which is the temperature the sample would
have received under ideal adiabatic conditions (for other parameters see the Appendix).
2.2 Three-layered composite
The sample consists of three layers of thicknesses e1, e2, and e3 (figure 2). If we consider the
same properties and experimental conditions as in the case of a two-layered composite
the transient temperature field governs the heat conduction equation (1) for each layer,
i ˆ 1, 2, and 3, with the initial [equation (2)] and the boundary conditions [equations (3) ^
(5)] and the following:
T2 …e2 , t† ˆ T3 …e2 , t† , (8)

qT2 …e2 , t† qT …e , t†
k2 ˆ k3 3 2 , (9)
qx qx

qT3 …e2 ‡ e3 , t†
k3 ˆ ÿh2 T3 …e2 ‡ e3 , t† . (10)
qx

ÿx ÿe1 0 e2 e2 ‡ e3 x

h1 h2
Figure 2. Diagram of three-layered sample.

If we take the quadrupole formalism of the Laplace transform technique (Degiovanni

1988) the problem can be expressed in matrix form:
        

yf 
y X11 X12 
yr 
y
ˆX r ˆ ˆ H1 M1 M2 M3 H2 r . (11)
Q 0 X21 X22 0 0
Here y and 
f y are the Laplace transforms of the sample front and rear face temper-
r
atures, respectively,
… defined as:
1

yi ˆ 
yi …p† ˆ exp…ÿpt†Ti …t† dt , (12)
0

and Hi and Mi are the boundary (heat loss) and transfer matrices,
 
1 0
Hi ˆ , (13)
hi 1
8  1=2  1=2
9
>
> p sinh‰…p=ai † ei Š >
>
>
> cosh ei >
>
< ai ki …p=ai †
1=2 =
Mi ˆ  1=2  1=2  . (14)
>
> >
>
>
> p p >
>
: ki sinh ei cosh…ki ei † ;
ai ai
 20 W Hohenauer, L Vozär
15 ECTP Proceedings page 692

The Laplace transform of the rear face temperature can be expressed as

 Q
yf ˆ . (15)
X21
The dimensionless temperature rise at the sample rear face gives an inverse Laplace
transform of 
yr. Our experience shows that the numerical algorithm proposed by Stehfest
(1970) works well.

3 Data reduction
An original software package for experimental `flash method' data processing has been
developed. The software currently allows the study of two-layered materials with zero
or non-zero thermal contact resistance, respectively, as well as three-layered materials
with ideal thermal contact (uniform: zero thermal contact resistance). The applied theory
considers ideal adiabatic boundary conditions, and heat losses can also be taken into
account.
Provided that we have a case with ideal thermal contact between the layers the data
reduction and estimation of the thermal diffusivity of one layer require knowledge of
the thickness, the density, and the specific heat of all the components and the thermal
diffusivities of the remaining layers. The data reduction consists of a least-squares fit of
the measured temperature rise versus time evolution. Because we have semilinear fitting
tasks, ie the working expressions linearly depend on the normalisation factor, adiabatic
limit temperature T1, the algorithm described elsewhere (Gembarovic­ et al 1990; Vozär
and Sírämkovä 1997) that shifts the fitting to solving a set of algebraic equations can be
reliably utilised.
Results of sensitivity analysis of the ideal two-layered composite show that normal-
ised sensitivity…1† to front layer diffusivity, Sa , and sensitivity to rear layer diffusivity, Sa ,
1 2

versus time curves are close to being linearly dependent (figure 3) so these parameters
cannot be estimated simultaneously in a simple flash-method experiment. The sensitivity
to Biot number, SBi, and the temperature rise curve, T(t), which is equal to the sensitivity to
the adiabatic limit temperature T1, have different shapes. This confirms that a simulta-
neous unique estimation of the adiabatic limit temperature T1, of the Biot number, Bi,
and one of the thermal diffusivities a1 or a2, respectively, can be performed successfully.
The maximum sensitivity to thermal diffusivities a1 or a2 lies around the half-time,…2† t0:5 .
This part of the data is the most suitable for the data reduction. Similar results were

T(t)
Sensitivity arb. units

Sa1

1
Sa


SBi

0.00 0.02 0.04 0.06 0.08 0.10


Time s
Figure 3. Normalised sensitivity versus time curvesöa two-layered model.

…1†
The sensitivity Sa is normalised sensitivity, defined as: Sa ˆ a1 qT (t)=qa1 .
1 1

…2†
The half-time, t0:5, corresponds to the time at which the temperature rise reaches half its
maximum value under ideal adiabatic conditions.
 Thermophysical properties of layered materials 21
15 ECTP Proceedings page 693

obtained for a three-layered composite. A unique simultaneous estimation can be

performed for the thermal diffusivity of only one layer with additional nuisance param-
eters T1 and Bi.
Here we note that Biot numbers of the front and rear faces enter the theory in a
similar way and their sensitivities are linearly dependent. Therefore, it is reasonable to
assume equal heat losses from the front and rear faces governed by the same Biot
number, Bi, or heat transfer coefficient, h, respectively.
A determination of the thermal diffusivity of a component on a two-layered and
three-layered system is a dependent measurement. The accuracy of an estimation of the
thermal diffusivity of one layer depends on the error and magnitude of other relevant
properties. In the present case the accuracy depends especially on the thermal diffusivity
of the remaining layer(s) and on the geometry of the sample and the ratio(s) of the layer
thicknesses. It was experimentally demonstrated that an estimation of the thermal diffu-
sivity of a thin layer is extremely sensitive to changes in the half-time t0:5 (Lee et al 1978)
that the data are based on. They stated that it was not practical to measure the thermal
diffusivity of a thin relatively highly thermally conductive layer deposited on a thick
poorly conductive substrate.
In order to investigate conditions for the thermal diffusivity determination and accu-
racy limits the following analyses were performed. We took the two-layered model and
calculated various simulated temperature rise versus time curves. We assumed we had
copper and alumina layers with their relevant (bulk) properties and we considered ran-
dom heat losses at a level corresponding to a real laser-flash experiment. We calculated
the curves for various thickness ratios, eCu =(eCu ‡ ealumina ), while we considered the total
thickness, e ˆ eCu ‡ ealumina, to be constant. Figure 4 presents the thermal diffusivity
results obtained. We see that the inaccuracy of the thermal diffusivity estimation for
copper rapidly increases with decreasing copper layer thickness. On the other hand the
dispersion of results of the thermal diffusivity estimation for alumina is relatively low.
The presented `apparent' thermal diffusivity values are those results obtained by the use
of the analytical model that considers the sample as a homogeneous medium. To summa-
rise the results we can say that in the case of a thin copper layer, information about the
thermal diffusivity of copper is insufficient for any reliable data reduction.
Then we analysed how the estimation of the thermal diffusivity of one layer is sensitive
to error in the knowledge of the thermal diffusivity of the second layer. Figure 5 (figure 6)
presents results of the variation of an estimation of the thermal diffusivity of alumina
(copper in figure 6) when the thermal diffusivity of the supplementary component copper
(or alumina) changes in the range of 1% ^ 3%. We see that in general the accuracy of the
determination of the thermal diffusivity of the material of lower thermal conductivity

100
106 a m2 sÿ1


50

0
0.0 0.2 0.4 0.6 0.8 1.0

eCu (eCu ‡ ealumina )

Figure 4. Comparison of estimated thermal diffusivity of copper (6) and alumina (~) (two-layered
model) and apparent (&) thermal diffusivity values (homogeneous media assumption model) ver-
sus thickness ratio.
 22 W Hohenauer, L Vozär
15 ECTP Proceedings page 694

20
aalumina

1.01aalumina
10
1.02aalumina
daCu aCu

0 1.03aalumina


0.99aalumina
ÿ10 0.98aalumina
0.97aalumina
ÿ20
0.0 0.2 0.4 0.6 0.8 1.0
eCu =(eCu ‡ ealumina )
Figure 5. Variation of the thermal diffusivity of copper versus the thickness ratio as a result of devi-
ation in the thermal diffusivity of alumina (3%).

2
aCu

1 1.01aCu
1.02aCu
daalumina aalumina

0 1.03aCu


0.99aCu
ÿ1 0.98aCu
0.97aCu
ÿ2
0.0 0.2 0.4 0.6 0.8 1.0
eCu =(eCu ‡ ealumina )

Figure 6.Variation of thermal diffusivity of alumina versus the thickness ratio as a result of deviation
in the thermal diffusivity of copper (3%).

1.0

0.8
eCu (eCu ‡ ealumina)

0.6

0.4


0.2

0.0
0 5  10 15
aCu aalumina

Figure 7. Estimation accuracy limit curves: ^, alumina; &, copper.

(alumina) is much higher than the determination of the higher conductive component.
The analysis also gives quantitative relationships between the accuracy of the thermal
diffusivity estimation and the thickness ratio of the layers. Figure 6 indicates that when
the error in the thermal diffusivity of copper is less than 3%, an accuracy of the estima-
tion of the thermal diffusivity of alumina better than 1% can be achieved only when the
condition eCu =(eCu ‡ ealumina ) < 0:72 is fulfilled. By performing similar analyses for differ-
ent thermal diffusivity ratios, the accuracy limit curves may be calculated, as illustrated
in figure 7. These curves limit the thickness ratio interval for reliable estimation of the
thermal diffusivity of a component on a two-layered sample as a function of the ratio of
the thermal diffusivity of the components.
 Thermophysical properties of layered materials 23
15 ECTP Proceedings page 695

Here we note that the results achieved can be generalised only with great care. In
our analyses, we have not considered variation of the density and the heat capacity.
Because of a strong correlation between the thermal diffusivity and the product of heat
capacity and density in a layered model (Koski 1985) the accuracy limit curves achieved
should be slightly modified. Although other disturbing phenomena were not taken into
account, the results achieved are a suitable basis for the predetermination of real estima-
tion accuracy limits.

4 Experimental results
Experiments were carried out with the home-made laser-flash apparatus installed at the
Materials Research Division of the Austrian Research Centre in Seibersdorf, described in
detail elsewhere (Vozär and Hohenauer 2000). Various test measurements on standard
materials allow us to guess the accuracy of the thermal diffusivity measurement to 3% ^
5%. For the test measurements we prepared samples from sintered-copper plasma-sprayed
layers on alumina substrate. These Cu/alumina/Cu three-layered sheets are regularly
utilised as electronic components. From the material we prepared three-layered samples
as well as two-layered ones, obtained by subtracting one copper layer. For comparison
we prepared and measured samples from the alumina substrate. The values of heat
capacity of both components were taken from the literature (Touloukian and Boyco
1970a, 1970b) and the densities were measured by the use of the weight principle.
In accordance with previous analytical results, we estimated the thermal diffusivity
of alumina on various samples. We measured a pure alumina layer, as well as two-layered
and three-layered Cu/alumina composites. The thickness of the alumina layer was 0.63 mm,
and the copper had thicknesses 0.035 mm and 0.063 mm, for the two-layered and three-
layered samples, respectively. The results obtained are summarised in table 1 and figure 8.
We see that there are no significant differences between results obtained on different

7
106 a m2 sÿ1

6


4
0 50 100 150

Temperature 8C

Figure 8. Comparison of experimental results of thermal diffusivity of alumina obtained on different

samples: ^, homogeneous sample; &, two-layered sample; ~, three-layered sample.

Table 1. Results of thermal diffusivity measurements of alumina on a homogeneous sample (a),

and two-layered (a2L ) and three-layered (a3L ) Cu/alumina composites.

T 106 a 106 a2L (a2L ÿ a)=a 106 a3L (a3L ÿ a)=a

8C 2
m s ÿ1
m s 2 ÿ1
% m2 sÿ1 %

30 7.21 7.14 ÿ0:90 7.15 ÿ0:83

60 6.29 6.26 ÿ0:69 6.28 ÿ0:23
90 5.56 5.61 0.96 5.63 1.34
120 5.01 5.08 1.37 5.07 1.12
150 4.52 4.57 1.06 4.60 1.81
24 W Hohenauer, L Vozär
15 ECTP Proceedings page 696

samples and analytical models. The dispersion of results is fully covered by the range we
stated for the accuracy and the reproducibility of the apparatus. On the other hand our
results are in very good agreement among values obtained in different laboratories as
summarised by Touloukian et al (1973).

5 Conclusion
We have shown that in the case of a study of thermal properties of a thin copper layer
deposited on a thick alumina layer, information about the thermal diffusivity of copper
obtained by the laser-flash method is insufficient for a reliable data reduction. The
proposed approach gives the possibility to relate quantitatively the accuracy of the
thermal diffusivity estimation of one layer on a layered composite to the thickness ratio
of the layers. Although other disturbing phenomena were not taken into account (varia-
tion of the density and the heat capacity, noise, etc) the results obtained give a suitable
basis for predetermination of real estimation accuracy limits.
Acknowledgements. The authors wish to thank the Hertha Firnberg Foundation of the ARC
Seibersdorf and the Slovak Science Grant Agency for financial support.
References
Balageas D L, 1989 High Temp. ^ High Press. 21 85 ^ 96
Degiovanni A, 1988 Int. J. Heat Mass Transf. 31 553 ^ 557
Gembarovic­ J, Vozär L, Majern|¨ k V, 1990 Int. J. Heat Mass Transf. 33 1563 ^ 1565
Koski J A, 1985, in Thermal Conductivity 18 Eds T Ashworth, D R Smith (New York: Plenum)
pp 525 ^ 536
Lee H J, 1975 Thermal Diffusivity in Layered and Dispersed Composites doctoral thesis, Purdue
University, Lafayette, IN, USA
Lee T Y R, 1977 Thermal Diffusivity of Dispersed and Layered Composites doctoral thesis, Purdue
University, Lafayette, IN, USA
Lee T Y R, Donaldson A B, Taylor R E, 1978, in Thermal Conductivity 15 Ed. V V Mirkovich
(New York: Plenum) pp 135 ^ 148
Maglic̈ K D, Taylor R E, 1992, in Recommended Measurement Techniques and Practices volume
2 of Compendium of Thermophysical Property Measurement Methods Eds K D Maglic̈, A
Cezairliyan, V E Peletsky (New York: Plenum) pp 281 ^ 314
Parker W J, Jenkins R J, Butler C P, Abbott G L, 1961 J. Appl. Phys. 32 1679 ^ 1684
Oëzisik M N, 1980 Heat Conduction (New York: John Wiley) p. 294
Stehfest H, 1970 Commun. ACM 13 47 ^ 49, 624
Sweet J N, 1989, in Thermal Conductivity 20 Eds D P H Hasselman, J R Thomas (New York:
Plenum) pp 287 ^ 304
Touloukian Y S, Boyco E H (Eds), 1970a Thermal Conductivity: Nonmetallic Solids volume 2 of
Thermophysical Properties of Matter Eds Y S Touloukian, C Y Ho (New York: IFI/Plenum)
Touloukian Y S, Boyco E H (Eds), 1970b Specific Heat: Metallic Solids volume 4 of Thermophys-
ical Properties of Matter Eds Y S Touloukian, C Y Ho (New York: IFI/Plenum)
Touloukian Y S, Powell R W, Ho C Y, Nicolaou M C (Eds), 1973 Thermal Diffusivity volume 10 of
Thermophysical Properties of Matter Eds Y S Touloukian, C Y Ho (New York: IFI/Plenum)
Vozär L, Hohenauer W, 2000 High Temp. ^ High Press. (accepted)
Vozär L, Sírämkovä T, 1997 Int. J. Heat Mass Transf. 40 1647 ^ 1655
Thermophysical properties of layered materials 25
15 ECTP Proceedings page 697

APPENDIX
Lee (1975) defined the following parameters:
Hi ˆ Ari ci ei ,
ei
Zi ˆ 1=2
,
…ai †
where A is the cross-sectional area of the sample, ri the density, ci the heat capacity,
and ei the thickness of layer i. Then,
d0 ˆ cos…gk † ‡ PU cos…Ugk † ,

o1 o
de ˆ ‰Y sin…gk † ‡ PUY2 sin…Ugk †Š ‡ 21 ‰Y1 cos…gk † ‡ PY2 cos…Ugk †Š ‡ . . .
gk 1 gk

Zo21
... ‡ f2‰sin…gk † ÿ P sin…Ugk †Š ÿ gk ‰cos…gk † ÿ PU cos…Ugk †Šg ,
gk3
and gk is the kth positive root of
 
o1 Zo1
sin…g† ‡ P sin…Ug† ÿ Y1 cos…g† ‡ PY2 cos…Ug† ‡ ‰sin…g† ÿ P sin…g†Š ˆ 0 ,
g g
where
Hi
Hi=j ˆ ,
Hj
Z2
Z2=1 ˆ ,
Z1

X1 ˆ H1=2 Z2=1 ‡ 1 ,
X2 ˆ H1=2 Z2=1 ÿ 1 ,
o2 ˆ Z1=2 ÿ 1 ,
o1 ˆ Z1=2 ‡ 1 ,

X2
Pˆ ,
X1
o2
Uˆ ,
o1
hi ei
Bii ˆ ,
ai ci ri

Bi1
Bi1=2 ˆ ,
Bi2
 
Bi1=2
Y1 ˆ Bi2 ‡1 ,
Z1=2
 
Bi1=2
Y2 ˆ Bi2 ÿ1 ,
Z1=2
Bi1=2
Z ˆ Bi22 .
Z1=2
ß 2001 a Pion publication printed in Great Britain