How Does Tack Depend on Time of Contact

and Contact Pressure?

COSTANTINO CRETON’* and LUDWIK LElBLER*

’Laboratoire de Physico-Chimie Structurale et Macromol6culaire, URA CNRS 278, ESPCI, 10 Rue Vauquelin, 75231
Paris C6dex 05, France; ’Laboratoire de Physico-Chimie Thborique, URA CNRS 1382, ESPCI, 10 Rue Vauquelin,
75231 Paris C6dex 05, France

SYNOPSIS

The tack of polymer melts on rigid substrates under conditions of short contact times and
low pressures is examined. The substrate is modeled as a random rough surface with a
distribution of asperities heights. The true contact area between the adhesive and the
substrate is calculated for a given total load and elastic modulus of the substrate. The
dependence of tack on contact time is accounted for by introducing the relaxation of the
adhesive through a time-dependent elastic modulus. For relatively high pressures the tack
is predicted to scale with 1/E so that for short contact times, tc, the tack is predicted to
scale with (&/T~)”’, where T, is the entanglement time. For lower pressures this simple
scaling law is no longer valid and we predict a complex variation of tack with contact time
and molecular parameters. 0 1996 John Wiley & Sons, Inc.
Keywords: adhesion pressure-sensitive adhesive contact mechanics theory contact
time pressure tack

INTRODUCTION However, even when debonding conditions are

It is a common experience to touch a sticky sub-
stance with a finger. When removing the finger, one
measures tack. The question is then how to quantify
the feeling of tackiness. And in particular what is a
good reproducible experiment to measure this effect?
Clearly two stages have to be distinguished the
bonding process (applying the finger) and the de-
bonding stage (removing the finger).
The relevant parameter to measure tack may be
the energy dissipated in the process of debonding.
This energy can be several orders of magnitude
larger than the thermodynamic work of adhesion,
W ,resulting from the rupture of the Van der Waals
bonds a t the interface.’-3 For polymer melts and
elastomers, the viscoelastic effects or the cavitation
and fibrillation of the adhesive are responsible for
a large energy dissipation and strong adhesion.
Hence, this energy is dependent on both the tem-
perature and the debonding rate.
* To whom correspondence should he addressed.
Journal of Polymer Science: Part B: Polymer Physics, Vol. 34,545-554 (1996)
0 1996 John Wiley & Sons, Inc. CCC 0887-6266/96/030545- 10
kept the same, the measured energy of adhesion may
depend on bonding conditions such as the applied
pressure and time of contact under p r e ~ s u r e .This
~.~
typically occurs at low pressures and/or short con-
tact times.
We refer to this regime, where adhesion is de-
pendent on these bonding conditions, as “tack.” The
goal of this article is to understand the dependence
of tack on the pressure and contact time and to relate
quantitatively our results to the molecular structure
of the adhesive and the roughness of the substrate
to bring a unifying approach to the interpretation
of the experimental results.
This problem of how tack depends on contact
time and contact pressure is important in many ap-
plications, namely for the design of pressure-sen-
sitive adhesives (PSA). In practice, the tackiness is
tested by the following procedure: the adhesive film
is deposited on a rigid backing and a stainless steel
probe is brought into contact with the adhesive,
maintained in contact under a constant pressure
(typically i04 Pa) for a given time (typically 1 s),
and finally removed a t a constant velocity. The
maximum force necessary to debond the adhesive is

545
546 CRETON AND LEIBLER

measured a s a function of the time of contact and

contact pressure. Typical results are shown in Figure loo0 3
l a and b for two different pressure-sensitive adhe-
sives on stainless steeL6
Although such a qualitative behavior has long
been known, it seems that no unified picture has
emerged in the literature about what controls quan-
titatively the contact time and pressure dependence
of t a ~ k . In
~ , certain
~ conditions tack is reportedly
nearly independent of contact pressure whereas in
others it is strongly dependent and the same is true
of the effect of the time of contact. 0.1I I I I I I I
-40 -20 0 20 40 60 80
The short contact times may be the origin of very
subtle effects. As a n illustration, consider the tem- T ("C)
perature dependence of the adhesion energy for two Figure 2. Probe tack results showing the adhesion en-
different times of contact, a very short and very long ergy G under short time, low pressure conditions (for t,
one (Fig. 2). Clearly, for short times of contact, the = 1.6 X lo2 s and p = 8 X lo3 Pa) and the maximum
adhesion energy, G , shows a pronounced maximum, adhesion energy (for t, = 1000 s and high pressure). The
polymer is a polyisobutylene (data from ref. 5).

approximately a t 50°C above the glass transition

temperature of the adhesive. This maximum is sup-
pressed, however, when the time of contact is in-
- creased.
N

.
E
z_
T h e explanations found in the literature t o ac-
m count for the decrease in adhesion a t short contact
E times and low pressures are all based on the same
;;
general argument of the decrease in real area of con-
tact between the adhesive and the probe. The rea-
sons given for this decrease in contact area vary,
however, a t least in the terminology, and one can
0.1 1 10 100 find lack of viscous flow;5 incomplete wetting;' too
time of contact 1s) high elastic modulus of the adhesive.l0." This last
effect also has been evoked for the more complicated
case of self-adhesion of polymers where interdiffu-
sion of chains can occur." In a typical tack experi-
ment, the experimental time, which is of the order
of a second, is much shorter than the terminal re-
laxation time of the polymers used for PSAs so that
there cannot be any substantial amount of viscous
flow.
We propose t o consider the adhesive as a visco-
elastic material with a time-dependent modulus and
t o treat the bonding process in the framework of
contact mechanics. More specifically, we model the
substrate as a random rough surface with asperities
lo3 lo4 lo5
of constant radius of curvature and a distribution
Pressure (Nlm ') of asperity heights relative to a reference plane. This
Figure 1. Probe tack results showing the maximum problem of contact of a random rough surface on a n
stress as a function of the time of contact (a) and contact elastic half-plane has been treated p r e v i ~ u s l y ' ~for
,'~
pressure (b) for two commercial pressure-sensitive ad- the case of adhesion of rubber on a rough substrate
hesives. The contact pressure is lo4Pa in (a) and the time but was never applied to the specific case of the
of contact is 1 s in (b) (data from ref. 6). measurement of tack for which viscoelastic effects

t<O O<t<t, t > t,
Figure 3. Schematics of the probe tack experiment.
are important. In particular, what characterizes the
tack measurement are the short time of contact and
even shorter debonding time. The central idea of
our approach is that the bond formation between
the viscoelastic half-plane and the rough substrate
occurs under conditions where elastic contact me-
chanics is applicable. The instantaneous area of
contact, A ( p , t,), can then be calculated as a function
of the time of contact, t,, applied pressure, p , and
molecular characteristics of the viscoelastic adhe-
sive.
We argue that this area is the relevant quantity
to be considered for the debonding process because
no substantial reduction in contact area (dewetting)
can occur during the very rapid release of the applied
pressure. This important statement is based on the
seminal work of Maugis and Barquins,15 who con-
sidered the case of the contact between an elasto-
meric sphere and a plane and who found that the
simple release of the applied pressure does not cause
the contact area to change very rapidly. Only the
application of a negative pressure will cause rapid
debonding. Alternatively, this amounts to saying
that the released elastic energy upon removal of the
pressure is much smaller than the viscoelastic losses
required for debonding at normal operating speeds.
Therefore, when comparing tack measurements
made at the same debonding rate, we argue that the
tack should be proportional to the true area of con-
tact established during the bonding step.
In this context, an important issue to discuss per-
tains to the details of the debonding process. Our
goal here is to set the framework for a better un-
derstanding of the bond formation and its influence
on tack in the regime where it is contact limited. In
our analysis of the influence of the bonding process
we implicitly assume that the debonding conditions
are kept constant and that the increase in area of
contact does not have any effect on the occurrence
of cavitation and fibrillation in the adhesive during
debonding nor does it cause a transition from ad-
hesive to cohesive separation. The validity of this
assumption and some further possible developments
will be discussed in the concluding remarks.
The next paragraphs will consider in more detail
how to calculate this true area of contact, first for
TACK OF POLYMER MELTS 547
large pressures relative to those due to Van der
Waals forces (Hertzian case), and then for smaller
pressures where surface forces become important.
In this latter case we follow closely the seminal work
of Fuller and Tabor.14 Within this framework, it is
easy to incorporate the characteristics of the ad-
hesive and to examine the role of the contact time
and contact pressure.
LARGE PRESSURES
We first consider the case of large pressures as de-
fined in the preceding paragraph. A further as-
sumption is that the time of contact between the
adhesive and the substrate is much shorter than the
terminal relaxation time of the adhesive so that no
viscous flow takes place. Under those conditions,
the process of adhesion can be seen as shown sche-
matically in Figure 3.
In a first stage, the adhesive film is brought into
contact with the substrate at a certain rate. This rate
being fast, the film acts as if it was elastic. Then a
constant pressure is maintained for a time t,. During
this time under constant pressure the melt relaxes
and the film behaves as if its modulus was lower. The
contact area at t = t, is therefore larger than at t =
0 and is governed by the viscoelastic relaxation mod-
ulus, E ( t,) , which could be obtained experimentally
in a creep experiment after a time t,.
One way to represent the contact between two
surfaces is to consider one of the surfaces as a model
rough surface. To calculate the true area of contact
between our model rough surface and a flat surface,
it is useful to consider first the contact of a single
asperity and then introduce the distribution.
If the problem is treated as an elastic problem,
the area of contact between one asperity and the
flat surface can be calculated by contact mechanics
and is given by the classic Hertz solution if surface
forces are neglected.16
As described in Figure 4,when a sphere is brought
in contact with a flat plane under a force, P , the
P I
-
I 2a I
Figure 4. Schematics of the contact between a spherical
cap and a plane.
548 CRETON AND LEIBLER

relationships between the radius of contact, a , the
applied force P , and the vertical displacement, 6,
are given by
These results are valid provided the modulus of the
sphere and the plane are very different so that the
modulus E in eq. ( 2 ) is that of the more deformable
material. In our case, we describe in the following
sections the physical picture of the hard asperity
indenting in a soft elastic plane. The opposite sit-
uation (i.e., a soft asperity on a hard plane) would
A model for a random rough surface has been
proposed by Greenwood and Williamson, l3 who
represented the surface as a series of asperities of
constant radius of curvature, R , but with a distri-
bution of heights relative to a mean plane, and a
density of asperities per unit surface, 2. If a flat
plane is brought in contact with such a surface, when
their two reference planes are separated by a dis-
tance, d , there will be contact with any asperity
whose height was originally greater than d . The
probability of this contact is given by
r x
prob(z > d ) = J cp(z) dz (3)
d

give exactly the same results provided that the mod-

ulus of the asperity was used in the calculations. and the total number of such contacts will be
A real rough surface has a distribution of asper-
ities heights and radii of curvature of the asperities.
The type of the distribution depends on the specific n = N r cp(z) dz (4)
mechanical surface treatment and is discussed in
more detail by Johnson.lfi If the surface has been
obtained by sand-blasting it is nearly random and where N is the total number of asperities.
the distribution of asperities heights follows a The total area of contact can be found by com-
Gaussian distribution, as shown in Figure 5. Al- bining eqs. ( 1) and (4) to give
though further surface treatment such as polishing
will modify the randomness of the surface, it is a
Atot = N R cp(z)(z - d ) dz (5)
good starting point.

200pm

L I I 1
I -4 -2 0 2 4
Height in pm

Figure 5. Schematics of a real rough surface and height distribution of asperities for a
sand-blasted surface of aluminium plotted in a normal probability scale. The y-axis on a
normal probability graph is scaled numerically so that a Gaussian distribution of asperities
will fall on a straight line (data from ref. 16).

whereas the total load, PtOt,
is given by combining
eqs. ( 2 ) and (4)
Although the distribution of heights of random
surfaces is better approximated by a Gaussian, the
significant results for high pressures can be obtained
analytically by using an exponential distribution and
this approach is chosen here. The distribution cp( z )
is then given by
With this distribution, the total area of contact and
the total load are given by
A,,, = naR (8)
P,,, = nEa3/'R'/'. (9)
From these two expressions, one can easily obtain
the relationship between load and area:
which gives the well-known Greenwood result that
the area of contact and the applied pressure are pro-
portional to each other.13The important result that
should be emphasized in our context is that for a
given surface, A is inversely proportional to the
elastic modulus E and proportional to the applied
pressure. In our problem of tack, the longer the con-
tact time, the more relaxed is the PSA and the lower
its modulus E ( t,) .
This result can then be used to develop a molec-
ular interpretation of the tack properties. The sim-
plest but instructive case is that of a monodisperse
high molecular weight polymer above its glass tran-
sition temperature. Its modulus E ( t , ) vs. log t, is
shown schematically in Figure 6. The "softening"
of the melt is related to the relaxation of deformed
chains. The entanglements impose topological con-
straints on the motion of chains and control the
relaxation processes. According to the reptation
picture, there are two characteristic time scales that
define three different regime~.'~
The entanglement time, T,, is defined as
TACK OF POLYMER MELTS 549
I I
I
I
I
I
I
'
)
Int
zt? zd
I
I I
Rouse f plateau f terminal
I
Figure 6. Young's modulus E of a high molecular weight
monodisperse polymer as a function of time in a creep
experiment.
where N , is the number of monomers in a strand
c0
between two entanglements, denotes the monomer
friction coefficient, and b is the monomer length.
The disentanglement time T d scales as
with Z being the polymerization index. For short
time scales (t, < T,), the relaxation occurs on short
distance scales and is due to Rouse-like motions. As
a result, the modulus decreases according to a simple
power law:
where EE) denotes the plateau modulus. For inter-
mediate times (7,< t, < T d ) , the modulus practically
does not change. Relaxation requires the disentan-
glement of chains from their original tubes and times
longer than T d . Thus, only at contact times longer
than the disentanglement time T d does the adhesive
deform by viscous flow so that E decreases again
with t.
It is important to consider these molecular ar-
guments in the context of a tack experiment. We
propose that the relevant transition for PSAs is from
the Rouse domain to the plateau region and is con-
trolled by 7,. Combining eqs. (10) and (13),a t times
shorter than T,, the area of contact A,,, is expected
to increase as t:/' and to level off when t, > 7,.The
entanglement time 7,can be measured directly from
dynamical mechanical spectroscopy. Furthermore,
the crossover contact time at which tack levels off
should be strongly dependent on temperature as it
scales with the monomer friction coefficient lo.On
550 CRETON AND LEIBLER
the other hand, this crossover time should be in-
dependent of the molecular weight of the chains
provided they are entangled.
This result seems consistent with experiments of
Zosel on the tack as a function of temperature of
two samples of polyisobutylene of different molec-
ular weight^.^ The critical temperature below which
tack starts to decrease is independent of molecular
weight, implying therefore that the entanglement
time T, rather than the terminal relaxation time Td
is controlling the loss of tack.
A viscous flow explanation would imply, on the
other hand, that the transition between good and
bad tack is controlled by the disentanglement time:
a t t, > T d the adhesive flows and tack is good whereas
a t shorter times there is not enough viscous flow t o
ensure a good contact. If this hypothesis was true,
the critical contact time for good tack would have a
strong molecular weight dependence.
SMALL APPLIED PRESSURES
Clearly, the universal law presented in the preceding
section cannot be true when surface forces become
of the order of the external applied force.
The situation for the contact of a single asperity
when surface forces are important has been analyzed
by Johnson et al. in their classic J K R approximation
for the contact of two soft solids." The surface forces
appear as a n apparent additional force on the sur-
face, which would give the same contact area using
the Hertzian analysis. The J K R approximation gives
in particular a nonzero contact area, even under zero
applied force. This area, Ao, and the corresponding
radius of the contact area, ao, are approximately
given by
where W is the thermodynamic work of adhesion.
The corresponding apparent Hertz load is given by
Po - WR (15)
and the resulting indentation is given by
T h e quantitative analysis of the J K R situation
brings two complications in the calculation of the
true area of contact and the load as a function of
the indentation. First, the radius of the area of con-
tact and the force of contact can no longer be ex-
plicitly expressed as a function of the indentation 6
but need to be evaluated numerically. Second, in
this low force regime the results are sensitive to the
tail end of the distribution of asperities and the more
realistic Gaussian distribution must be used rather
than the simpler exponential one.
We recall here briefly the approach of Fuller and
Tabor.'* The first step in the calculation is to express
6 and a 3 as a function of P . If a , P , and 6 are nor
malized by a,,, Po, and tio,as defined in eqs. ( 14)
( 1 6 ) ,one obtains
and
From these analytic expressions, we can extract
numerically the ratios P / P o andA/Ao as a function
of (6/6,). This finally gives, in normalized param-
eters, for the average area and the average force per
asperity:
At''
-- -
N
A, = a; [a( $)
X exp( - 21 ( h + A ) 2
.(
P, Po
- -
ptot
N
- N
$)
X ex,( - 51 ( h + A)'
where h = d / a , A = 6/a, A, = &,/a, 9 is obtained
numerically from eq. ( 1 7 ) and @ is obtained nu-
merically by combining eqs. 17 and 18.
The evaluation of the integral (20) a s a function
of A, and h gives the average force P I per asperity
for a given normalized separation h between the
plane of the adhesive and the midplane of the rough
substrate. Conversely, the separation h can be ob-
tained for a given average force P1.
Once h is known, the average area of contact per
asperity Al for a force P I can then be obtained from
eq. ( 1 9 ) .

Within this framework, it is now interesting t o
examine more quantitatively certain experimental
conditions and in particular the transition from the
regime where the true area of contact is controlled
by surface forces and the regime where i t is con-
trolled by the external applied force.
h = 0 and P1 = 0
This corresponds to the situation where perfect
contact can be attained between the two surfaces
under no external applied force. Although this sit-
uation is not realistic, as it assumes t h a t the plane
is already in contact with the substrate, it is nev-
ertheless interesting to give a lower bound for the
critical modulus for perfect contact. Numerically,
the critical modulus is obtained by determining for
which value of A, one obtains complete contact (i.e.,
h = 0 ) for zero applied pressure ( P1= 0 ) . Replacing
the critical value of A, = 6,/a in eq. ( 1 7 ) , this gives
for the critical modulus E* at P1= 0
This result could also have been obtained in the sin-
gle asperity case by a physical argument that pro-
vides more insight. T h e excess free energy of the
system due to the indentation 6 of the sphere is
given, under zero applied load, by
AFt,, N -WR6 +E
(Y
- a3
where ( 6 / a ) ' is the elastic deformation that takes
place over a volume of the order of a 3 . T h e radius
of contact a is roughly equal t o % so that by sub-
stituting a in eq. ( 2 2 ) , minimizing F,,, relative to 6,
and finally setting 6 = (for complete contact on
average), one obtains eq. ( 21 ) .
It is worthwhile t o do some numerical estimates
of what this critical modulus should be. Taking W
= 50 m J / m 2 , R = 100 pm, and cr = 2 pm typical of
a machined metal surface, one obtains E* N 0.2
MPa. The physical meaning of this value is to put
a lower bound below which, regardless of the applied
pressure, there will be good contact. It is remarkable
that for a realistic degree of roughness it is in good
agreement with what is experimentally known a s
the Dahlquist's criterion ( i.e., the critical modulus
above which there is substantial loss of tack). T h e
value of E* is, however, very sensitive to the nominal
roughness, which should provide a n easy way t o test
these conclusions experimentally.
TACK OF POLYMER MELTS 551
h = 0, E as a Function of PI
After considering the case where the applied force
is zero, it is interesting t o examine how does E*
evolve when the applied force is increased. In the
limiting case of high pressures, the Hertz situation
is recovered and as A l cc P, / E , one expects E * t o
increase linearly with the applied pressure with a
slope proportional t o ( R /cr ) 1'2.
A , ( € ) for Different Values of P l / W R
In Figure 7 we consider the case where the contact
area is calculated as a function of the elastic modulus
for different values of the nominal force per asperity.
T h e average area of contact per asperity Al is nor-
malized by A *, defined a s the result of integral ( 19)
for h = 0 (i.e., the maximum area of contact within
the framework of our model). What is apparent from
the curves is t h a t whereas a t zero applied force, the
decrease of A l with E is nearly exponential, as soon
as PI > 0, the curve must have a limiting behavior
a t high moduli of Al cc 1/ E matching the Hertzian
result. This curve could be used to predict the con-
tact area a s a function of the time of contact t,
through the relaxation of the modulus E = E ( t,) .
In this regime the dependence of the contact area
on the time of contact will not follow a universal
law but will depend on the relative importance of
surface forces and elastic forces, and this is consis-
tent with experimental results that show a variety
of functional dependencies of the tack with the time
of contact.
1
0.1
0.01
0.001
E/E*
Figure 7 . True normalized area of contact AJA* as a
function of the normalized elastic modulus E/E* for var-
ious values of the average force per asperity P I /WR. The
relationship between the nominal pressure p and the av-
erage pressure per asperity PI is given by: p = P,/Rc.
552 CRETON AND LEIBLER

.
-
.,
E
01 L3
15

0.01 2 2
3 4 5 6 7 8 9 3 4 5 6 789 0.001 0.01 0.1 1 10 100
0.1 1 10
P,MR t, (s)
Figure 8. True normalized area of contact AJA* as a Figure 9. Probe tack results showing the adhesion en-
function of the normalized force per asperity P,/ WR for ergy G as a function of the time of contact t, for a nominal
various values of the elastic modulus E/E*. The relation- pressure p = 2 X lo5 Pa (data from ref. 4).
ship between the nominal pressure p and the average
pressure per asperity P1 is given by: p = PJRo.
x W / IJ.Numerically, if we take the same values as
in the previous section, this gives p * = 0.025 MPa
A,(P) for Different Values of €/€* or for a 1 cm2 surface, a force of 2.5N.
The physical interpretation ofp* is the nominal
Another natural extension of the calculation is to
pressure on the sample below which surface forces
investigate the dependence of A l with the applied
become important and must be incorporated in the
force for a range of different moduli. In this case a s
calculation.
well, the limiting behavior a t large values of E/E*
Zose14 measured the tack G a s a function of the
must be Hertzian but when E is closer to E*, the
contact time t, of a sample of polyethylhexyl ac-
slope of the curve of Al/A* decreases and becomes
rylate on a stainless steel probe under a pressure
closer to A l cc Pi’*, as illustrated in Figure 8.
of 0.2 M P a and of the contact pressure p with a
fixed contact time of 1 s. These results, shown in
Figures 9 and 10, allow us t o check for the self-
C O M P A R I S O N WITH EXPERIENCE
consistency of our arguments. In the time-depen-
dence experiment Zosel found that G increased with
After obtaining the trends and scaling laws in the
tEl2a t low values oft, and reached a constant value
different regimes for the true area of contact as a
for t, > 1s. In the pressure-dependence experiment,
function of the applied force and the time of contact,
it is interesting to make some more quantitative
2
comparisons with experimental results to test the 0 1
validity of the model. The difficulty lies in the lack
of quantitative simultaneous measurements of both
tackiness and roughness. We must therefore rely on
estimates of roughnesses for typical probes and ad-
hesives. First, we need to estimate the areal density
of asperities. The main results contained in eqs. ( 19)
and ( 2 0 ) give the average area per asperity A l and
the average force per asperity P I as a function of a
mean separation between the adhesive and the sub-
strate. If the average radius R and the mean asperity
height u are known, the areal density of asperities 10
0.01 0.1 1 10
L: is not a n independent variable but can be esti-
mated roughly. The average diameter of a n asperity p (MPa)
is of the order of 6 so that the areal density of Figure 10. Probe tack results showing the adhesion
asperities is of the order of 1/Ra. Therefore, a n av- energy G as a function of the contact pressure for a contact
erage force P, = WR corresponds to a pressure p* time of 1 s (data from ref. 4).

he found an increase of G with p1/2and a leveling
off f o r p > 0.3 MPa.
If we take p* = 0.025 MPa as estimated above,
the experimental contact pressure of Zosel, p = 0.2
MPa, is about eight times greater than p * . We can
then extract the predicted functional dependence of
the contact area with E from Figure 7 with PI
= 8 W R . In this regime we expect the area to vary
with 1 / E and therefore, from the arguments pro-
posed in the Large Pressures Section, the tack
should increase with t E / 2 , in very good agreement
with experimental data.
The question is whether the time scale at which
the saturation occurs is consistent with our predic-
tions. As we do not have precise information on the
frequency dependence of the modulus, we cannot
compare directly the saturation time and 7,. How-
ever, a value of 7, of about l s seems quite plausible
for poly (ethylhexyl acrylate) at room temperature.
The pressure dependence of tack, as shown in
Figure 10, is harder to compare quantitatively to our
model in the absence of detailed roughness data. We
have shown that the apparent exponent of the tack
dependence on pressure varies with the ratio E / E * .
This critical modulus E* depends itself both on the
average height ~7and on the average radius of the
asperities R .
The experimentally determined exponent N 3
would correspond from Figure 8 to E / E * N 2.5.
Therefore, the tack should become independent of
pressure at a pressure higher than p c N 3 W / u. Typ-
ically, for a value of csof a few microns, p c should be
of the order of 104-105 Pa, which is slightly lower
than the experimentally determined value from Fig-
ure 10.
Another confirmation of the influence of applied
pressure, Hammond’s results in Figure Ib show ex-
ponents from 0.7 to 0.4 when the adhesive goes from
rough to smooth. These results should be compared
with Figure 8 showing the effect of the contact pres-
sure at a given modulus and are consistent with a
decrease in the exponent when the contact surface
is made smoother.
A different experimental observation, which
reinforces the present analysis, is the dependence
of the measured tack on temperature. Experimen-
tally, tack goes through a maximum with tempera-
t ~ r e The
. ~ high temperature side of the maximum
is controlled by the viscoelastic losses whereas the
low temperature side may be controlled by the area
of contact. Zosel measured, on the same systems,
the tack and the elastic modulus at a time corre-
sponding to the time of contact t,. His results, shown
in Figure 11, are consistent with W cc 1 / E , implying
TACK OF POLYMER MELTS 553
lo 2 loo0
n
T (“C)
Figure 11. Probe tack adhesion energy G (0)and elastic
compliance 1 / E (-) for polyisobutylene as a function of
temperature. In the contact-limited regime, G cc 1 / E and
when 1/E reaches a plateau, the tack is controlled by
the viscoelastic losses and decreases with T (data from
ref. 10).
that we are in a regime where the modulus is much
higher than E* and the area of contact decreases as
1 / E , as predicted by our model.
CONCLUDING REMARKS
Our model is in very good qualitative agreement with
the available experimental results. In particular, the
scaling laws successfully predict all the trends of the
influence of the pressure and of the time of contact
in the regimes where adhesion is contact limited.
Roughness effects seem to be qualitatively well ac-
counted for in our picture as well. The more quan-
titative comparisons based on molecular arguments
would require simultaneous measurements of stress
relaxation and tack on well-characterized substrates
and adhesives. In particular, it will be interesting to
study how the temperature does affect the pressure
and time dependence of tack.
We assumed in our analysis that the measured
tack (force or energy) was directly proportional to
the true area of contact. This assumption can only
be valid if two conditions are fulfilled:
1. the debonding conditions, such as tempera-
ture and debonding rate, are kept constant,
2. the variation in contact area does not affect
the debonding mechanism.
Although the first condition is easy to fulfill by a
proper choice of experimental conditions, the second
one implies that there will be no transition from
554 CRETON AND LEIBLER
adhesive to cohesive failure or from nonfibrillar to
fibrillar fracture when the area of contact is in-
creased. Although we do not have observations con-
firming these points, the available experimental re-
sults are consistent with our hypothesis that the
measured tack is proportional to the contact area
and do not show evidence of a sharp transition in
the tack force or energy a t a given value of the area
of contact.
I t is well known that many PSAs cavitate and
form fibrils when they are debonded from the ad-
hesive. The detailed process of fibrillation is likely
to depend on the initial contact area but is not nec-
essarily proportional t o it. However, the fibrillar de-
bonding normally occurs in a regime where the
adhesion is not contact limited but rather controlled
by the amount of viscoelastic losses taking place
during the large deformation involved in the fibril-
lation process.
We assumed implicitly that the specific chemical
interactions between the adhesive and the substrate,
which would affect the thermodynamic energy of
adhesion W, were independent of the time of contact
and pressure, Although this is not true for many
pressure-sensitive adhesives, the increase in adhe-
sion due to W is generally occurring over a much
longer time scale than the viscoelastic effects in-
vestigated in the present model so that we feel that
it is a reasonable assumption to take W as a con-
stant.
As pointed out in the Introduction, the removal
of the force upon debonding is extremely fast in a
typical tack experiment. When a negative pressure
is applied and the two surfaces are still in contact,
the debonding process can be represented as the si-
multaneous propagation of small circular cracks
around each asperity a t a certain speed. The multiple
crack picture had already been suggested by de
Gennes' on a flat surface. T o treat the problem of
debonding quantitatively, it seems necessary to
consider a rough surface and to incorporate existing
experimental ' 'J'and results on crack
propagation in viscoelastic media.
We are grateful to Denis Melot and Michel Glotin (Elf-
ATOCHEM) for stimulating discussions on PSAs.
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Received April 27, 1995
Revised September 22, 1995
Accepted September 27, 1995