Suppression of the Rayleigh-Plateau instability on a vertical fibre

coated with wormlike micelle solutions

F. Boulogne1,2 , M.A. Fardin3,4 , S. Lerouge3,4 ,
L. Pauchard1 , F. Giorgiutti-Dauphine1
June 18, 2013

arXiv:1306.3811v1 [cond-mat.soft] 17 Jun 2013

UPMC Univ Paris 06, Univ Paris-Sud, CNRS, F-91405. Lab FAST, Bat 502, Campus Univ, Orsay,
F-91405, France.
2
boulogne@fast.u-psud.fr
3
Laboratoire Mati`ere et Syst`emes Complexes, CNRS UMR 7057, Universite Paris Diderot, 10 rue Alice
Domon et Leonie Duquet, 75205 Paris Cedex 13, France.
4
The Academy of Bradylogists
Abstract
We report on the Rayleigh-Plateau instability in films of giant micelles solutions coating a vertical
fibre. We observe that the dynamics of thin films coating the fibre could be very different from the
Newtonian or standard Non-Newtonian cases. By varying the concentration of the components of
the solutions and depending on the film thickness, we show for the first time that the RayleighPlateau instability can be stabilized using surfactant solutions. Using global rheology and optical
visualisations, we show that the development of shear-induced structures is required to stabilize the
micellar film along the fibre. Assuming that the viscoelastic properties of the shear-induced state
can be described by a simple model, we suggest that, in addition to the presence of shear-induced
structures, the latter must have an elastic modulus greater than a critical value evaluated from a
linear stability analysis. Finally, our analysis provides a way of estimating the bulk elasticity of the
shear-induced state.

Introduction

When a liquid film is coating a fibre, it undergoes spatial thickness variations. The mechanism of this
instability has been understood by Lord Rayleigh in the 19th century[33]. Due to the energetic cost of
free surfaces (surface tension), the liquid tends to minimize its surface area by breaking a cylinder into
a serie of regularly spaced droplets. This instability can be observed on free falling jets and it underlies
many natural phenomena, like the dew drops on coweb [7]. The coating of fibres has been extensively
studied by Quere et al. in the situation where the fibre is drawn out of a bath [31]. They compared
their measurements with theoretical predictions from Landau, Levich and Derjaguin on the film thickness
[23, 12].
In the case of a Newtonian fluid flowing down a vertical fibre, flow regimes have been depicted as a
function of physical parameters. For high flow rates and/or fibre radii, the flow is dominated by inertia
and the nature of the instability is convective [14]. On the contrary, when the fibre size is smaller than
the capillary length and for creeping flow (low Reynolds number), the instability is absolute and the
physics is dominated by surface tension [14]. In such absolute regimes, we recently studied the flow of
polymer solutions [6]. We investigated experimentally the influence of two non-Newtonian properties,
shear-thinning effect and first normal stress difference, on the growth rate of the instability and on the
morphology of the drops. The pattern is globally the same as in the case of Newtonian fluids: the first
normal stress difference just tends to slightly decrease the growth rate and to smooth the drop shape.
Beside polymers, a broad variety of molecules assemble to form non-Newtonian fluids. For instance, it
is well-known that above a Critical Micellar Concentration (CMC), surfactant molecules can self-assemble
to form aggregates called micelles. The size and the shape of the micelles depend on the structure of
the surfactant molecule, on the surfactant concentration and on the presence of additives like simple or
organic salts [21]. In some range of parameters, the micelles are giant worms often called living polymers
because thay can entangle like polymers but they can also break and fuse continuously. Solutions of wormlike micelles present remarkable rheological properties such as shear-thickening or shear-banding effects,
Accepted

in Soft Matter. DOI:10.1039/C3SM27940E

extensively studied by theoreticians and experimentalists [2, 8]. These non-linear properties are often
associated with the development of out of equilibrium structures induced by the shear flow. These shearinduced structures present strong viscoelastic properties leading to specific behaviors like the oscillation
of a falling sphere [22] or the incomplete retraction of a filament after a pinch-off [36]. These examples
highlight the consequence of the viscoelastic properties of the flow-induced phases.
In this paper, we investigate the flow, at low Reynolds number, along a vertical fibre of semi-dilute
giant micelles solutions. By varying the concentration of the chemical compounds of the solutions and
the thickness of the film along the fibre, we observe different morphologies for the micellar film. In some
conditions, the film exhibits the expected Rayleigh-Plateau instability, as it has been observed so far, in
Newtonian fluids or viscoelastic polymer solutions while for other conditions, remarkably, the micellar film
remains stable. Using global rheology and optical visualisations, we demonstrate that the stabilisation
process along the fibre is connected with the development, above a characteristic shear stress, of shearinduced structures. We also show that the development of shear-induced structures is necessary but not
sufficient to stabilize the micellar film. Using a simple viscoelastic model (Kelvin-Voigt) to describe the
viscoelastic properties of the shear-induced state, we suggest that the elastic modulus characterizing the
shear-induced structures has to be greater than a critical value provided by the linear stability analysis.
The paper is organized as follows. In Section 2, we present the experimental setup and the chemical
system. In Section 3, we report different flow regimes depending on surfactant and/or salt concentrations
and film thicknesses. In Section 4, we present the rheological behavior of our micellar systems and we
visualize the material under shear to confirm the presence of shear-induced structures. The next two
Sections are devoted to the conditions required to stabilize the micellar film on the fibre. Section 5 focus
on the stress applied to the film by gravity and its relation with the rheological behaviour of the solution
and Section 6 studies the role of the shear-induced film elasticity on the Rayleigh-Plateau instability.

2
2.1

Experimental details
Experimental setups

The experimental setup used for the study of the Rayleigh-Plateau instability is depicted in Figure 1(a).
An upper tank, of diameter 14 cm, is connected to a valve. This valve is composed of two axisymmetric
cones. The adjustment of the gap between these cones controls the flow rate i.e. the film thickness on
the fibre. Guided by a nozzle, the liquid flows along a vertical nylon fibre. The fibre is about 60 cm long
and has a radius R = 0.28 mm. Vertical position and centering of the nozzle are crucial to ensure an
axisymmetric coating. This position is adjusted using an optical support with a precision of 2.4 arc sec
(Model U200-A2K, Newport). Observations are done with a telecentric lens and a high speed camera
(about 500 images/s) delivering a resolution of 0.024 mm/pixel (Fig. 1(b-c)).
The rheological properties of the samples have been characterized using a stress-controlled rheometer
(Anton Paar, MCR 501) at 20.00 0.01 C. The temperature was adjusted with a Peltier plate. We used
a cone and plate geometry (radius 49.988mm, angle 0.484 ). A solvent trap was used to limit evaporation
during the measurements. Rheological protocol consists in applying stress sweep, the stress value being
imposed during 1000 s at each step. The flow curve is obtained by averaging the shear rate response over
the last 100 s of each step.
The global rheological measurements have been complemented by rheo-optical observations of the
flow performed in a Taylor-Couette (TC) flow geometry (gap: 1.13 mm, length: 4 cm), adapted to the
shaft of a stress-controlled rheometer (Anton Paar MCR 301). The inner cylinder is rotating while the
outer transparent cylinder is fixed in the laboratory frame. Direct visualizations were made in the plane
velocity gradient/vorticity (i.e. the plane made by the radial direction and the cylinders axis), the gap
of the TC cell being illuminated with white light. Images of the gap were collected using a CCD camera.
The rheological signal was recorded simultaneously, allowing direct correlation with optical visualizations
[25, 16]. Note that similar rheograms were obtained with TC and cone and plate geometries.

2.2

Materials

We focus on aqueous micellar solutions made of cetyltrimethylammonium bromide (CTAB) and sodium
salicylate (NaSal) purchased from Sigma-Aldrich and used without further purification. NaSal is an
organic salt, sometimes designated as a co-surfactant since it participates to the micellar structure by
taking place in-between the polar head groups of surfactant molecules [32]. The addition of this salt
also screens repulsive electrostatic interactions between CTA+ groups and it reduces the spontaneous
curvature of the system [26]. As a result, the micellar uniaxial growth is promoted because of the large
energetic cost of hemispherical endcaps. All the solutions investigated range in the semi-dilute regime.
For the range of concentration chosen here, the micelles are locally cylindrical and slightly entangled [2].
2

Tank
r

Nozzle
Flat film
Droplet

h(z, t)
Fiber

Weight

(a)

(b)

(c)

(d)

Figure 1: (a) Notations and schematic view of the vertical fibre and the injection device. (b-d) Pictures
illustrating the different morphologies of the film flowing along the fibre: (b) Unstable morphology
which corresponds to drops sliding on a quasi static liquid film. (c) Stable film. (d) Film morphology
corresponding to a gel-like block moving down the fibre. The diameter of the fibre is 0.56 mm.

To prepare chemical solutions, we mixed in pure water (milliQ quality, resistivity: 18 M.cm) the
weight percentages of NaSal and CTAB until a complete dissolution. Samples were stored at rest at 23 C
in darkness to avoid any degradation. The solutions were allowed to reach equilibrium for at least three
days in these conditions before experiments were performed. We carefully checked the homogeneity of
solutions before any measurement. All measurements along the fibre were carried out at T = 20.00.5 C.
The equilibrium surface tension of the solutions studied in this paper is 36.0 0.5 mN/m (Wilhelmy
plate method with a Kr
uss tensiometer), a value consistent with measurements reported in the literature
for solutions above the critical micellar concentration [11].

Morphologies of the liquid film along a vertical fibre

We focused on low Reynolds number flows (Re . 1) dominated by surface tension (R < lc =

= 1.9

mm), for which the flow is absolutely unstable [14]. We studied the flow along the vertical fibre of a large
set of wormlike micelles solutions. Depending at once on the surfactant concentration [CTAB], the salt
concentration [NaSal] and the film thickness h, we observe three possible morphologies of the film along
the fibre as displayed in Fig. 1(b-d):
The film can be unstable with respect to the Rayleigh-Plateau instability. The associated morphology corresponds to drops sliding on a quasi-static liquid film (Fig. 1(b)).
The film can be stable and in this case, the associated morphology corresponds to a flat film
(Fig. 1(c)).
The film can be subjected to some kind of fracture leading to separate blocks moving down the
fiber (Fig. 1(d)). The morphology is essentially flat but the film is discontinuous.
In order to illustrate the effect of the various parameters on the flow along the fibre, we construct a
flow-phase diagram (see Fig. 2a) in the plane ([CTAB], [NaSal]), allowing to identify different domains.
At low NaSal concentrations, the apparent viscosity is low (. 50 mPa.s) which corresponds to inertial
regimes [14]. At high NaSal concentrations, due to a high zero shear viscosity (> 100 Pa.s), the fluid
hardly or could not flow though our experimental device (No flow domain). These two domains
are excluded from the present study which, focuses on the intermediate range of NaSal concentrations,
typically between 0.2 and 0.5 wt.%. In this intermediate range, three domains, denoted by A, B and
C, can be distinguished according to the sequence of morphologies observed as a function of the film
thickness.
Domain A

In this domain, the micellar solutions behave as usual Newtonian fluids [14] or polymer solutions
[6] for all the film thicknesses accessible with our experiment: the film is first flat and then, the
Rayleigh-Plateau instability develops (Fig. 1(b)).

Domain B

In this domain, regardless of the film thickness, the micellar solutions do not exhibit the RayleighPlateau instability. For sufficiently small thicknesses (i.e. low flow rates), the film remains flat and
continuous over the whole fibre extent (about 60 cm). From this stable morphology, an increase
of the film thickness leads to a breaking of the liquid thread into blocks of a few centimeters long,
sliding along the fibre (Fig. 1 (d)). Note that, visually the blocks seem to have a gel-like character
with a large elasticity, in contrast to the solutions at rest. Similar viscoelastic threads were observed
in the case of pinch-off and filament retraction in extensional flow of wormlike micelles [36, 3].

Domain C

In between the two domains A and B, the domain C is characterized by the existence of the three
morphologies (see Fig. 1(b-d)). For small thicknesses, the films are destabilized by the RayleighPlateau instability with patterns similar to those described in domain A. As its thickness is increased, the film adopts a stable morphology corresponding to a flat continuous liquid thread.
Finally, for sufficiently large thicknesses, the flat and continuous liquid thread breaks into gel-like
blocks as described in domain B.

The different sequences of morphologies described above and observed respectively in the domains A,
B and C are schematized in Fig. 2(b).
When a stable morphology is observed, we have noticed that if we tilt the fibre horizontally, after a
few seconds, drops can appear (figure 3). This observation suggests that the flow under the action of
4

(a)

3.5

12

16

NaSal (mM)
20
24
28

32

36

100
Inertial domain

90

3
wt.% CTAB

40

80
70

2.5

60

No flow

50

1.5

CTAB (mM)

40
30

1
0.5
(b)

Domain

20
10
0.1

0.2

0.3
0.4
wt.% NaSal
Film thickness

0.6

Morphology
Fig. 1(b)

0.5

Fig. 1(c)

Thin

Thick

Fig. 1(d)

Thin

Fig. 1(b)

Intermediate

Fig. 1(c)

Thick

Fig. 1(d)

Figure 2: (a): Flow-phase diagram showing domains depending on surfactant (CTAB) and cosurfactant
(NaSal) concentrations. Five domains are identified: Inertial (green +), No flow (magenta ), A
(blue 4), B (red ) and C (orange ). (b): Schematic representations of the different sequences of film
morphologies as a function of the film thickness associated with the different domains A, B and C in the
flow-phase diagram.

~g

Stable film

Flow

Tilting of the fiber

Figure 3: From a vertical fibre where a stable film is flowing down, we tilt the fibre horizontaly leading
to the development of the Rayleigh-Plateau instability.
gravity is necessary to stabilize the film. Particularly, this shows that the flow properties of the micellar
solutions are involved.
Note that this effect is different from the stabilizing process depicted by Quere [30] with Newtonian
fluids. In his experiments, stable films flowing down a vertical fibre were obtained by saturating the
Rayleigh-Plateau instability thanks to the advection of the flows. This saturation (i.e. flat film) occurs
3
if the film thickness is smaller than hc = Rl2 . In our experiment, hc = 6m while h > 200m, and the
c
flow is absolutely unstable .

Rheo-optical properties under simple shear flow

In contrast to the free jets dominated by extensionnal flow [9, 15, 4], the flow along the fibre is dominated
by shear. We thus performed rheological experiments under simple shear flow in order to characterize
the rheological properties of the micellar solutions used in this study. The measurement of the flow
properties is combined with direct optical visualisations of the samples illuminated with white light in
order to detect possible changes in the structure of the micellar fluid. In the different domains A, B and C
identified in the flow-phase diagram, we observe the same type of flow behaviour. Figure 4(a) displays a
representative flow curve gathered from a sample belonging to domain C and obtained in stress-controlled
mode. The choice of this mode has been motivated by the fact that the maximum stress in the liquid
flowing down the fibre can be easily estimated (See Section 5). The response of the samples to simple
shear flow is highly nonlinear, with successive transitions, from shear-thickening to different degrees of
shear-thinning. Such complex evolution of the shear stress as a function of the shear rate has already
been observed for dilute micellar solutions, well-known to exhibit a shear-thickening transition [20, 19].
Following Refs. [20, 19], we divide the flow curve into four distinct regimes, defined by critical shear
stresses, denoted c , s and f .
Regime I ( < c )
This regime corresponds to the primary response of the micellar solution to exceedingly low shear
stresses. For dilute systems, we expect a linear increase of the shear stress as a function of the
shear rate, associated with a Newtonian behaviour while for semi-dilute systems, a slight decrease
of the viscosity as a function of the shear rate is usually observed, due to partial alignment of the
micelles by the flow [18, 20]. Unfortunately, reaching this regime requires shear stresses that cannot
be imposed by the rheometer, what leads to the lack of experimental data points in Fig. 4. Note
that in these conditions, c is only roughly defined.
Regime II (c < < s )
This regime is characterized by a shear-thickening transition, the apparent viscosity of the material
increasing with the shear rate (see Fig. 4). This transition is associated with a re-entrant behavior
of the flow curve since the shear rate first decreases and then increases with the shear stress in
this regime. Due to the re-entrant character of the transition, this regime can only be observed at
imposed stress. The upper boundary of this regime is noted s and corresponds to the shear stress
for which the apparent viscosity reaches a maximum. Images of the sample in the shear-thickening
regime do not exihibit any changes compared to the situation at rest. The gap of the TC cell
6

appears homogeneous suggesting that the changes in the structure of the fluid associated with the
shear-thickening transition, occur at sub-micronic scale.
Regime III (s < < f )
In this range of applied stresses, the flow becomes shear-thinning and direct visualisations show
that the gap of the TC cell remains homogeneous (see Fig. 6 (a-c)).
Regime IV ( > f )
This regime is characterized by a strong degree of shear-thinning associated with the existence of
a stress plateau, the onset of which is denoted by a critical shear stress f . The stress plateau
generates a jump in the shear rate resulting in a sharp decrease of the apparent viscosity. The
stress f is determined by increasing the shear stress step by step with an appropriate sampling as
illustrated in Fig. 5. The plateau is characterized by a large jump in the shear rate at imposed stress,
or equivalently a strong increase of the shear rate versus time at fixed stress (see inset in Fig. 5)
and a large increase of the first normal stress difference N1 , indicative of nonlinear viscolelastic
properties of the material under shear. Note that below or above f , variations of the shear rate
are lower than 10% over the duration of the measure (1000 s). For the sample in Fig. 5, we estimate
f = 4.10.3 Pa. In this regime, direct visualisations in the TC geometry reveal a drastic change in
the structure of the fluid (see Fig.6 (d-e)). A fraction of the sample becomes slightly turbid leading
to variations in the refraction index observable with visible light. These observations suggest that,
for > f , a new phase characterized by a length scale in the order of a few microns nucleates in the
gap of the TC device [35]. We observed that the nucleation occurs from the edges of the cylinders
and progressively extends along the inner cylinder, the growth being favoured at the bottom of the
cell which has a conic shape. At fixed stress, the turbidity fluctuations observed on the pictures
evolve in time with a complex dynamics. The proportion of the induced phase increases with the
imposed shear stress, and for sufficiently high shear stresses, the induced phase invades the whole
gap (see Fig.6 (f-g)). This scenario is reminiscent of the shear-banding transition even if there is
no clear evidence for an organisation into two bands separated by a well-defined interface [24]. By
monitoring the shear-rate as a function of time, we noticed that the appearance of the induced
phase is correlated with the presence of a kink in the (t)

curve which appears sooner as the stress

increases. This kink is also observed in the cone-plate geometry for > f (See inset in Figure 5)
and is then the signature for the appearance of the induced phase.
Beyond this purely phenomenological description, our observations deserve further comments. As
mentioned above, similar complex succession of rheological transitions in the flow curve have already been
observed in dilute micellar solutions of TTAA/NaSal [20, 19]. However, the direct observations reported
by the authors largely differ from the present study: Indeed, in the shear-thickening regime (regime II),
the fluid phase of regime I was found to coexist with a viscous phase of gel-like shear-induced structures
while in regime III, the induced gel-like phase invaded the whole gap of the flow geometry. Furthermore,
the rheological response in regime III was also different, the apparent viscosity being constant, while
in our case the system is shear-thinning. This behaviour was ascribed to the existence of a plug flow
with slip at the walls. Finally, above f , fracture of the gel-like phase followed by flow instabilities were
observed.
Here we do not observe any phase coexistence in regime II. However, this does not rule out the fact
that the shear-thickening transition is associated with a change of the structure of the system but rather
suggests that this change of the structure occurs at sub-micronic scale which prevents direct visualisation.
Our situation could correspond to the minimal scenario for the shear-thickening transition in micellar
systems, namely the uniaxial growth of the micelles [1, 29, 27, 24]. On the other hand, we clearly observe
a phase coexistence in regime IV, above f , the induced phase being characterized by a large first-normal
stress difference. Note that, at equilibrium, the samples under investigation are only weakly entangled:
their concentration is associated with the very beginning of the semi-dilute regime, in a transition range
where the rheological behaviour is between pure shear-thickening of dilute rod-like micellar systems, and
pure shear-banding of strongly entangled wormlike micelles [17, 24]. In this context, the shear-bandinglike behaviour observed in the present study is likely to correspond to a transition from the state induced
during the shear-thickening regime (regime II) towards another induced phase structured at larger scale
(regime IV).
Note that in the literature on wormlike micelles, the shear-induced state associated with the shearthickening transition was called SIS for shear-induced structure [28], or SIP for shear-induced phase [5]
interchangeably. Recent studies [37] have also used FISP to denote irreversible flow-induced structured
phase obtained in extensional flow. However, in the present paper, we make no distinction between the
expressions shear-induced structures and shear-induced phase and in the following we will refer to
SIS as the reversible structures (or phase) induced at larger scale in regime IV.
7

102

Regime IV

101
f

(Pa)

100
10

Regime III

102

Regime II

103
10

10

c
5

Regime I
3

10
101
1
(s )

103

103

101
101
1
(s )

103

10

101

(Pa.s)

100
101
102
103
105

Figure 4: (a): Shear stress and (b): apparent viscosity as a function of the shear rate for a solution
of CTAB (2.55 wt%) and NaSal (0.32wt.%). The temperature is T=20.00 0.01 C. The rheological
protocol consists in stress sweep experiment: at each step, the shear stress is kept fixed during 1000 s.
The resulting shear rate (t)

reaches a stationnary value after a time period that depends on the applied
shear stress. The flow curve is obtained by averaging the measured shear rate over the last 100 s of each
step. c , s and f denotes characteristic shear stresses that delimit different regimes in the flow curve.

10

1250

100

500
10

0.1

0.1

750

Apparition
of SIS

10
100
Time (s)

10
(s1 )

100

N1 (Pa)

1000

(s1 )

(Pa)

1000
250

0
1000

Figure 5: Determination of the stress plateau value (f ). Stress (red +) and first normal stress difference
N1 (green ) versus shear rate for 2.55wt.% CTAB and 0.32wt.% NaSal (T=20.00 0.01 C). At each
step, the shear stress is imposed during 1000 s and the measured shear rate results from the average over
the last 100 s of each step. Inset: Time evolution of the shear rate for a fresh sample at = 4.5 Pa.
The black arrow indicates the signature linked to the apparition of SIS.

~ v,
~ ~v ))
Figure 6: Views of the gap of a Couette cell in the plane velocity gradient/vorticity (noted (~
for different applied shear stresses. Each image is taken after a time t 1000 s. The solution is composed
of 2.55wt.% CTAB and 0.32wt.% NaSal. The top and bottom sides correspond to the outer and inner
wall respectively. For > f = 4 Pa, structures appear near the inner wall. Arrows indicate some
turbidity fluctuations indicative of SIS with micronic characteristic length scale.

h (mm)

1
0.9
0.8
0.7
0.6
0.5
0.4
0.3
0.2
0.1

Unstable
Stable
Blocks
f /(g)

1.6 1.8

2.2 2.4 2.6 2.8

[CTAB] (%)

3.2 3.4

Figure 7: Film morphologies for different film thicknesses and various surfactant concentrations ([NaSal] =
0.32wt.%). The black line is a fit of film thicknesses hf = f /(g) () related to stress plateau values.
It separates unstable and stable flow regimes.

Stress induced by gravity and development of shear-induced

structures

As described in section 3, the film morphology depends on the film thickness h. Our working hypothesis is
that the transition between unstable to stable morphologies along the fibre might be linked to the presence
of the SIS. To clarify and to go further on that point, we will focus on solutions in domain C. This choice
is motivated by the fact that solutions which belong to this domain present all three morphologies. We
first study the influence of the CTAB concentration. We use a set of chemical solutions for which CTAB
concentration is in the range [1.8, 3.2]wt.% keeping [NaSal] = 0.32wt.% constant. For each solution, we
keep increasing the flow rate. The results are reported in figure 7 where we observe successively unstable,
stable and block morphologies as the film thickness increases.
To explain this transition between stable and unstable morphologies, and since the rheology is controlled by the applied shear stress, we compare the stress plateau f extracted from the rheological curves
to the gravitational stress g applied on the film. This stress g = gh ranges between 2 and 8 Pa in our
experiments and is then comparable to the value of the stress plateau f . We define the film thickness
hf related to the stress plateau f as hf = f /(g).
Figure 7 illustrates the succession of film morphologies as a function of the film thickness h for different
surfactant concentrations and a fixed salt concentration. We also report, for each sample, the value
hf = f /(g) gathered from the rheological experiments. Remarkably, the unstable-stable transition is
found to occur as h ' hf . Thus, we can conclude that the condition g > f is necessary to stabilize the
film. This suggests that the stabilization of the film is connected to the presence of the SIS as f is the
characteristic stress value for the development of these structures.
Consequently, the SIS are able to be formed, before the Rayleigh-Plateau instability acts, if > f .
This fixes the first condition to stabilize the film. As we will see in the next section, this condition is
necessary but not sufficient.

Effect of the SIS elasticity on the instability growth rate

In this section, we study a second set of chemical solutions in order to complete our understanding. The
question we attempt to answer is: why do films become suddenly always unstable if the concentrations
are slightly changed near the border between domains A and C? To cross these two domains, we work
with a constant CTAB concentration ([CTAB] = 2.55wt.%) while NaSal concentrations vary in the range
[0.25, 0.4]wt.%. Figure 8 displays the film morphology as a function of the thickness for different salt
concentrations covering domains A and C at fixed surfactant concentration. Based on rheological data,
the thickness of the film f /(g) beyond which the SIS are likely to develop is also reported. A good
agreement is again observed in domain C between the expected thickness computed from rheological
results and the effective thickness above which the films are stable. However, there is a discrepancy for
solutions in domain A since films thicker than hf are unstable. According to our analysis, the SIS still
develop but they do not stabilize the film.
To understand these observations, we focus on two effects: the surface tension which is responsible
for the instability and the bulk elasticity which tends to slow down the film deformations.

10

h (mm)

1
0.9
0.8
0.7
0.6
0.5
0.4
0.3
0.2
0.1

Unstable
Stable
Blocks
f /(g)

Domain C

Domain A

0.26 0.28 0.3 0.32 0.34 0.36 0.38 0.4 0.42

[NaSal] (%)

Figure 8: Film morphologies for different film thicknesses and various salt concentrations ([CTAB] =
2.55wt.%). The black line is a fit of film thicknesses hf = f /(g) related to stress plateau values.
It is worth noting that the constitutive relation describing the SIS is still unknown. Since SIS present
strong elastic properties, we attempt a description of the SIS by a simple Kelvin-Voigt model allowing
analytic calculations [34, 10]. The Kelvin-Voigt model takes into account the viscous dissipation at short
time scales and elasticity at long time scales. The stress tensor ij is function of two parameters: viscosity
0 and elastic modulus G0 :
ij (t) = G0 ij + 0 ij

(1)

where ij is the strain and the dot represents the time derivative.
To obtain the dispersion relation for this constitutive equation, we perform a linear stability calculation. The Fourier transform of the expression (1) reduces the equation to
ij () = ()ij ()

(2)

iG0

+ 0 .
where is a complex frequency and with () =
Experimentally, we observe that the film thicknesses h(z) and the fibre radius R have the same order
of magnitude. Under this consideration, we can calculate the dispersion relation in our geometry[13].
In the cylindrical reference frame (r, , z) (See figure 1(a)), the z-component of the momentum balance,
taking into account the lubrication approximation, becomes:

g z p + r (rr u) = 0
r

(3)

where u is the fluid velocity along the fibre (z direction). The boundary conditions are: no-slip on
the fibre (u(r = R) = 0) and zero tangential stress at the liquid-air interface (r u(r = R + h) = 0).
The pressure gradient
 is caused by surface curvatures and it is expressed from Laplaces law: z p =
z h
(R+h)
+

h
(assuming z h  1). Solving this equation, the fluid velocity profile is u(r) =
2
zzz
 2


z pg
2
(r R ) 2(R + h)2 ln Rr .
4
Incompressibility leads to:
h q
+
=0
(4)
t
z
R R+h
1
where the flow rate per unit length is q = 2(R+h)
u(r)2rdr.
R
To conduct a linear stability analysis, we develop the film thickness as h = h0 + h1 ei(kzt) where k
is the real wave number. Thus, we derive the following dispersion relation


gR2 ()
Rh30 ()
k2
i
k4
(5)
=k
16()
3()(R + h0 )
(R + h0 )2
with = h0 /R. Two dimensionless functions reflect the geometry:
4
ln(1+x)
(x) = x(2+x)(6+5x(2+x))+12(1+x)
and
(1+x)2
4

(x) = 3(4(x+1) ln(x+1)x(x+2)(3x(x+2)+2))

16x3
The imaginary part of corresponds to the instability growth rate noted (k):


Rh30 ()
k2
G0
4
(k) =
k

30 (R + h0 )
(R + h0 )2
0
11

(6)


> 0, unstable

G0 = 0

kmax
k

G0
< 0, stable

Figure 9: Growth rate of the instability vs the wave number k from the Kelvin-Voigt model illustrating
the stabilizing effect of the bulk elasticity G0 . The case G0 = 0 (in green) is the marginal stability curve
for Newtonian fluids (viscosity 0 ). As G0 increases, the marginal curves (in blue) is shifted to the
negative growth rate domain.
For (k) < 0, the system is stable, whereas for (k) > 0 the system is unstable. If G0 = 0, the solution
for Newtonian fluids is recovered. The evolution of the growth rate with k is plotted in figure 9.
We observe that the bulk elasticity (G0 ) plays a stabilizing effect on the film as illustrated in figure 9:
the marginal stability curve is shifted to the negative . If max() = (kmax ) < 0 (blue curve in figure
9), all modes are damped by the elasticity resulting in a stable film.
1
Note that, in this model, the wave number for the maximum of the growth rate is kmax = 2(R+h
0)
and is independent of the elastic modulus.
Solving the condition (kmax ) = 0 defines a critical elastic modulus Gc0 :
Gc0 (h) =

h3 R(h/R)
12(R + h)5

(7)

Experimentally, we can estimate Gc0 from the border between domains A and C. From the data
presented in figure 8, we can evaluate for [CTAB] ' 2.55wt.% ' 70mM, [NaSal] ' 0.33wt.% ' 20mM:
G0 ' Gc0 (hf ) = 1.0 Pa (with h = hf = 0.4 mm).
Thus the bulk elasticity of the SIS has to be sufficient to shift the curve of the growth rate to the
negative values, in order to stabilize the film. To summarize, we have shown that the elastic shear induced
structures are developed in our flow if gh > f . If this condition is fulfilled, we expect a stable film
only if the bulk elasticity is greater than Gc0 . As the result, we can explain the apparent discrepancy
of the unstable region in figure 8. From the transient zone to the unstable one (i.e. increasing salt
concentration), the bulk elasticity decreases such as G0 < Gc0 .
The value Gc0 = 1 Pa can be compared to oscillatory shear flow tests. As suggested by the flow
curve in figure 4, the linear regime could not be reached with our rheometer. The first test consists in the
measurement of the elastic modulus versus time for a shear stress amplitude of 5 104 Pa at a frequency
f = 1Hz. The elastic modulus increases in time from 102 Pa to a few Pascal ([CTAB] = 2.55 wt.%
and [NaSal] = 0.32 wt.%). In a second test, a constant shear stress > f is applied to the sample
followed by an oscillating stress of small amplitude. Even if the SIS has time to partially relax, such
experiments can provide a reasonnable order of magnitude of the moduli (G0 and G) of the SIS at high
angular velocities. We found a value for the elastic modulus around 1.5 Pa, consistent with the value
Gc0 = 1 Pa gathered from the flow along the fibre and considering that the viscoelastic properties of
the SIS can be modelled by a Kelvin-Voigt model. Our results suggest that the elastic modulus of the
solutions under shear is larger than the one for the solution at rest and that the value required to stabilize
the flow could be deduced from the Kelvin-Voigt model.

Conclusion

In this paper, we studied the flow of CTAB/NaSal solutions on a vertical fibre. Structure modifications
occuring from the chemical composition and the shear flow provides a large variety of flowing regimes.
The flow on the fiber can actually be unstable and similar to the flow of newtonian fluids: the capillary
driven Rayleigh-Plateau instability produces drops sliding on the fibre. For another set of solutions, the
film can stay uniform along the fiber provided the film thickness satisfies h > hf = f /(g). From
12

rheo-optical measurements, we found that the condition for stabilizing the flow is that the characteristic
stress on the film should be larger than a critical stress f . This critical stress has been identified as the
onset of emergence of micronic structures induced by the shear-flow, i.e., shear-induced structures (SIS).
A last flowing regime is observed for high film thicknesses and in a given range of concentrations: in this
last regime, the film breaks in a series of gel-like blocks sliding along the fibre.
Our analysis suggests that the bulk elasticity of the SIS is responsible for the decrease of the instability
growth rate until inhibited the Rayleigh-Plateau instability for a negative growth rate. Two conditions
are required to prevent the destabilization of the film: the presence of the SIS and a sufficient elasticity
of theses structures to inhibit the instability driven by the surface tension. A linear analysis of stability
assuming a Kelvin-Voigt model for SIS, evidences a stable flow provided the elastic modulus of the SIS
is higher than a critical value. By comparing with experimental results on systems which can go through
an unstable to stable regime, we can estimate the value of the elastic modulus value of these SIS. In the
future, the inspection of the micronic SIS can provide a better understanding of the micellar structure
inducing the bulk elasticity.

Acknowledgment

The authors thank Triangle de la Physique for the rheometer (Anton Paar, MCR 501) and Federation
Paris VI for the high-speed camera. Also, thanks to Jerome Delacotte, Christophe Clanet and Marina
Moreno Luna for discussions.

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