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Recent advances in wrinkle-based dry adhesion

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Cite this: DOI: 10.1039/c4sm00027g

Yudi Rahmawan,ab Chi-Mon Chena and Shu Yang*a

Received 7th January 2014
Accepted 1st May 2014
DOI: 10.1039/c4sm00027g
www.rsc.org/softmatter
Surface wrinkles driven by elastic instabilities have attracted significant interest in the field of materials
science and engineering. They are simple and readily fabricated with various patterns of tunable size,
morphology and surface topography from a wide range of material systems. Recently, they have been
investigated as a new type of dry adhesives. In this review, after a brief introduction of different methods
to prepare wrinkle surfaces, we focus on the investigation of dry adhesion mechanisms in different
material systems. By exploiting wrinkle dimension, morphology, modulus, curvature, and different
contacting surfaces (flat, hemispherical, spherical) and their complementarity, we show adhesion
enhancement, reduction and selectivity. By comparing experimental results with theoretical predictions,
we aim to provide a guideline to design and engineer wrinkle-based dry adhesives. Several examples of
applications of engineered wrinkles are also demonstrated, including pick, release and transfer of
nanoparticles and bulk materials, and gecko-like hybrid adhesives. The review is concluded with
perspectives on the wrinkling technology for smart dry adhesives.

structures normally involves costly and time-consuming multi-

1 Introduction
Surface textures have profound impact on adhesion properties,
which are crucial to bioorganisms,1–4 synthetic structural
adhesives5–7 and robotic locomotion.8,9 It could increase or
decrease the adhesion force depending on the type of contact,
length scale, and compliance of materials.10–13 In general, for a
hard elastic surface with surface textures, the true area of
contact is limited by the asperity to asperity contact, resulting in
a decrease of the adhesion force with the increase of surface
mean square roughness.14,15 It becomes more complicated if at
least one of the surfaces involved is compliant with respect to
the applied stress. The adhesion force in this case depends on
the competition between elastic energy required to deform the
contacting surfaces and the increase in the true area of contact.
In the realm of biology, animals have shown remarkable ways to
reduce elastic penalty while minimizing the effect of contact
area reduction for enhanced dry adhesion. For example, the
hierarchical, high-aspect-ratio (HAR) brillar structures on
gecko toe pads dramatically increase the compliance of its
brillars, leading to enhanced contact when bent.16 Via the
contact splitting mechanism, the brillar structures are insen-
sitive to defects, contact pressure uniformity, surface adapt-
ability and crack re-initiation.2,6 Similar hierarchical structures
are observed from numerous insects1,2 and have been widely
mimicked in synthetic systems for adhesion improvement.7,17–20
Nevertheless, the fabrication of the delicate hierarchical
a
Department of Materials Science and Engineering, University of Pennsylvania, 3231
Walnut Street, Philadelphia, PA 19104, USA. E-mail: shuyang@seas.upenn.edu
b
Center for Convergence Advanced Materials, Surya University, Jl. Scientia Boulevard
Blok U/7, Summarecon Serpong, Tangerang, 15810 Indonesia
step processing in photolithography and so lithography.7,21
Furthermore, the fabricated high-aspect-ratio brillar-like
structures are oen vulnerable to collapse driven by structural
instabilities.22–25
Interestingly, simple patterns such as low-aspect-ratio ridges
found in our ngerprints, palms and toes have been shown to
increase adhesion, to permit grabbing things and to amplify the
signal of sensory neurons in body parts.26–28 Meanwhile, wrin-
kles with smooth and shallow surface undulations are robust
and relatively easy to fabricate. They have been used to control
surface properties, including adhesion,29–31 wetting and
biofouling,18,32,33 and to create novel electronic and optical
devices.27,34,35
Wrinkles can be generated by compressing a composite lm
with a modulus difference along the lm thickness and a
monolithic beam or sheet rested on a so foundation or
conned on one side.26,36–44 The further increase of compression
could lead to a transition of surface wrinkling to surface
folds.43,45–48 Here, we focus on the discussion of dry adhesion
from wrinkles that are typically fabricated from composite
lms. The wrinkle wavelength and amplitude can be ne-tuned
by varying the lm thickness, modulus and strain level,26,35–41
whereas wrinkle morphology is ruled by the boundary condi-
tions, magnitude of the strain, lm crosslinking density and
thickness.26,42,49–56 This versatility and controllability renders
wrinkles an ideal platform to tune surface roughness for
adhesion study. Recent studies have shown that the adhesion
strength between two surfaces in the presence of wrinkles
on one side29,30,57–62 or on both sides63 can be either enhanced
or reduced comparing to their at counterparts. The
adhesion strength depends on parameters, including wrinkle

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geometry,30,57,59,61 material's intrinsic properties,62,64,65 surface
curvature,58 complementarity,29,61 and types of adhesion tests.
By varying some of these parameters in real time, it is also
possible to dynamically tune the dry adhesion strength.59 In this
review, we start with a brief summary of different methods to
prepare wrinkle surfaces in various material systems, followed
by the discussion of wrinkle-based dry adhesion studies in the
recent decade to elucidate the effect of the aforementioned
structural parameters. We further discuss the role of materials
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properties, including modulus, surface energy and viscoelas-
ticity. The effect of contact geometry is also examined. We
compare the experimental investigation with theoretical
predictions with an aim to provide a guideline to design and
engineer wrinkle-based dry adhesives.
2 Fabrication of wrinkle surfaces in
different material systems
Wrinkles are undulation or wavy patterns formed on so,
continuous base materials or simply undulations spanning on
entire thickness of a sheet.35,36,44,66 While wrinkles are typically
random under isotropic force, they can be ordered into one-
dimensional (1-D) ripples, 2-dimensional (2-D) herringbone
and highly ordered zigzag structures.41,53,67–71 Under anisotropic
strain or surface connement, more complex structures that are
out-of-phase or in-phase with a pre-pattern are possible.56
On a bilayer or graded thin lms of dissimilar mechanical
properties and crosslinking density, residual stress can be
induced or released by heating,36,37,51,72–77 solvent
swelling,42,47,70,71,78–82 mechanical stretching/compres-
sion,26,41,52,83–86 UV or thermal curing,55,87,88 capillarity,89,90 and
drying of a sol–gel lm.91,92 On a compliant substrate, with a
skin layer of dissimilar mechanical properties, wrinkles are
formed when compressive stress acted on them exceed a critical
value (see Fig. 1) to achieve an equilibrium state of minimal
energy. Since the general mechanism of wrinkle formation has
been well reviewed in the literature,27,34,35 here we only briey
summarize several commonly used wrinkling systems and their
fabrication (see Table 1 and Schemes 1–5).
Among different wrinkling approaches, the most common
ones for adhesion studies are thermally or mechanically
induced wrinkling of bilayer systems consisting of a hard thin
skin deposited on a compliant substrate (see Schemes 1–3). The
Fig. 1 Components and parameters in the wrinkle structure. The
difference in elastic moduli between layered materials produced
instabilities on the surface when compressive stress is presented.
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hard skin can be thermally deposited metals,36,37,52,72,73,75,76,93
glassy polymers,40 and a siliceous thin lm generated by oxygen
treatment or UV ozonolysis,26,41,52,80,83–86,94,95 The compliant
substrates usually are elastomers (e.g. polydimethylsiloxane,
PDMS), thermoplastics (e.g. polystyrene) or shape memory
polymers, which become soened when heated above the glass
transition or ow temperature. Wrinkle morphology (ordering
and orientation) can be controlled using a template, the
sequential application of mechanical force or a programmed
ion beam. For example, by sequential stretching and releasing
of an oxygen plasma-treated PDMS lm via controlling strain
and timing, we maneuvered winkle generation from 1D ripples
gradually in transition to ripple with bifurcation, a ripple/
herringbone mixed structure, and highly ordered zig-zag-based
2D herringbone structures.41
In the bilayer system, when the strain is small the wrinkle
wavelength l is predicted from linear stability analysis on a
compressed lm lying on an elastic substrate, assuming that
both top and bottom layers are elastic, and the bottom layer is
semi-innite,37,38,41
"  #1=3
1  vs 2 Ec
l ¼ 2pt   (1)
3 1  vc 2 Es
Here, t is the hard skin layer thickness, Es and Ec are Young's
moduli, and vs and vc are Poisson's ratios of the substrate and
the thin coating, respectively. The critical compressive strain to
induce wrinkling 3c and the amplitude A are given by36,44,96,97
"  #2=3
1  vc 2 Es
3c z 0:52   (2)
1  vs 2 Ec
l pffiffi
Az 3 (3)
p
when Es/Ec1, where 3 is the applied compressive strain (3>3c).
eqn (1) shows that the wrinkle wavelength increases with the
lm thickness, or the difference between the elastic moduli of
the substrate and thin layer increases.
3 Wrinkle dry adhesion
Before discussing the adhesion in wrinkle structures, it is
important to revisit the mechanism of general adhesion. From a
physical viewpoint, adhesion is an attraction between surfaces
when they are kept adjacent to each other. The energy required
to separate two at surfaces is the thermodynamic work of
adhesion Wadh, dened as98,99
Wadh ¼ W12 ¼ g1 + g2  g12 (4)
Here g is the surface energy, and g12 is the interfacial energy
of components 1 and 2. When the two components are of the
same material with surface energy g, Wadh ¼ 2g. Here Wadh in
eqn (4) is for the equilibrium reversible contact of two solid
surfaces. Therefore, it can be used as the lower limit for adhe-
sion. In most polymer systems, adhesion exceeds the
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Table 1 Exemplary wrinkling systems

System Schematic illustration Ref.

36, 37, 51, 67, 68,

72, 73, 75, 76 and 93
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Scheme 1. Metal deposited on a so substrate

Skin: metal, siliceous

A mechanically or lms, foundation: elastomer, 26, 41, 52, 80,
thermally stressed compressive stress: externally 83–86, 94 and 95
bilayer system induced from modulus
mismatch or external force

Scheme 2. Stretching/release of oxygen plasma or UVO-treated

elastomeric sheet

69 and 112

Scheme 3. UV or ion beam bombardment or corona

discharge-induced wrinkling
Skin: polymer or oxide of a
higher or lower modulus
Swelling of a
than the foundation
laterally conned
material, foundation:
bilayer or a 42, 56, 79 and 81
a compliant or glassy
graded polymer
polymer, compressive stress:
lm
osmotic pressure-induced
stress release Scheme 4. Swelling of a laterally conned polymer lm

Skin: a gelated lm or

segregated lm by external
stimuli, foundation: sol or a
Drying of a
pre-polymer solution, 91, 92
sol–gel lm
compressive stress: modulus
mismatch due to solvent
evaporation
Scheme 5. Drying of a sol–gel lm

thermodynamic value due to dissipative energy away from the
interface. For non-equilibrium contact, the critical strain energy
release rate Gc should be used by compensating the nature of
contact (e.g. the contact area). It is given by57
Pf 2
Wadh ¼ Gc ¼ (5)
8pE * ap 3
Here, Pf is the maximum separation force of a at surface, E*
is effective modulus, which will be dened later and ap is the
radius of the test probe. Gc is typically considered as the upper
limit of work of adhesion for polymeric adhesives and is used
throughout this paper.
The adhesion strength of the same surface can be enhanced
almost linearly with the increase of surface energy g.5 Since g is
an intrinsic characteristic of two contacting materials, the rst
principle to design a dry adhesive should consider this factor.
However, the precise measurement of the surface energy of
solids can be a challenge since the intermolecular forces

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normally need to be solved numerically.100 According to Fowkes'
theory of additivity on surface forces, the surface energy is a
sum of intermolecular forces, including dipole–dipole interac-
tions, ion–dipole interactions, van der Waals forces and
hydrogen bonding. The surface forces can be further simplied
into polar and non-polar forces, which can be measured
experimentally, and expressed by99
h 0:5 i
0:5
Wadh ¼ W12 ¼ 2 gd1 gd2 ðgp1 gp2 Þ (6)
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Here, superscripts d and p represent the dispersive and polar
components, respectively.
To dene a nite boundary of equilibrium contact area
between two surfaces, hemispherical contacts are normally
modeled instead of innite at-to-at contact. This system is
also found to have wide applicability to many biological struc-
tures.2,4 When two hemispherical elastic materials are in
contact, the equilibrium contact area of both solids dened by
3RF
the Hertz equation as a3 ¼ . Here, R is the radius of a
4E*
hemisphere, E* is the effective modulus of the system given
E1 E2
by E* ¼ and F is the compressive
E2 ð1  v1 2 Þ þ E1 ð1  v2 2 Þ
pressure to make contact. E and n with subscripts 1 and 2 are the
Young's modulus and Poisson's ratio of 1 and 2, respectively.
The extension of the Hertz equation by considering surface
forces has been proposed by Johnson–Kendall–Robert (JKR)
as101,102
  1=2 
3R 2
a3 ¼ F þ 3pRg þ 6pRgF þ ð3pRgÞ
4E *
Here, the elastic stress at the edge of the contact is assumed
to be innite, and the adhesion force could deform hemi-
spherical surfaces into the equilibrium contact area. The result
is a nite pull-off force as
FJKR ¼ (3/2)pRGc
When the contacting surface is stiff, i.e. adhesion force could
not deform the surface, it is apparent that the contact radius
can be relatively small. Therefore, Derjaguin et al.103 estimated
the pull-off force using the Hertzian contact area, which is given
by FDMT ¼ 2pRGc.
It is also important to point out that natural dry adhesives
are typically hierarchical HAR brillars arranged in an angle
geometry with at or curved end tips.2,4 Such a design will not
only improve the locomotion for easy detachment, but also
increase compliance for enhanced adhesion strength upon
contact. The effective Young's modulus Eeff of HAR brillars can
be calculated as16
3EIr sin b
Eeff ¼
L2 cos2 b½1  m tan b
where E is the intrinsic Young's modulus of the adhesive
material, I is the moment intertia, r is the density of brillars, L
is the side contact length, m is the friction coefficient and b is
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the tilting angle. Furthermore, when the contact of the adhesive
pad is mainly due to the side contact perimeter, the pull-off
force in eqn (8) should be modied to accommodate the
geometry effect. The modied-JKR adhesion model based on
contact line is104
FMod–JKR ¼ 3.16(KGc2r)1/3L (10)
where r is the radius of brillars, and K ¼ 4E*/3.
When a wrinkled surface is in contact with a substrate (at,
hemispherical, or self-similar wrinkles), adhesion strength can
be enhanced or reduced. Different wrinkle-based dry adhesion
systems are summarized in Table 2 (see Schemes 6–8).
3.1. Wrinkles in contact with a at surface
The pull-off force based on the JKR model in eqn (8) is for the
hemispherical contact of elastic solids. When the contact tip is
split into smaller contact elements, the initial contact radius R
can be divided into a smaller protrusion of radius rt, with the
total splitting protrusion N ¼ R/rt. By self-similarity principles,
where the radius of contact scales with the contact size s, the
enhancement of adhesion force due to this contact splitting
becomes6,105
 
pffiffiffiffiffi 3
Ft ¼ N pRGc (11)
2
Therefore, it is apparent that the advantage of splitting
contact points into smaller discrete contact points is to generate
(7) more total force of interaction. The enhancement of adhesion
due to splitting the contact elements into smaller ones is called
“contact splitting”. It is also applicable in wrinkled surfaces
with the contact perimeter as contributors. Chan et al.
demonstrated that the smaller wrinkle wavelength led to higher
adhesion strength compared to the smooth surface, as shown in
Fig. 2.30 Here, adhesion strength enhancement is not due to
increasing contact area during preloading. Instead, it is due to
(8) increasing contact perimeter similar to the contact splitting
mechanism observed from gecko foot hairs. During contact
with a at surface, the wrinkle interface can be depicted as a
cylindrical contact with a contact length z ¼ k1l and contact
width l/2. Here, k1 is a geometry constant rendering the average
contact length in respect to its wavelength.39 The number of
a2p
wrinkles per unit area of the test probe is n ¼ p , where ap is
zl
the radius of the test probe (see Scheme 6). eqn (11) can be
rearranged and normalized into the adhesion force per unit
area or the adhesion strength ss,s :30
 1=2  * 1=2
8pE * Gc ap 3 8E Gc
ss;s ¼ ¼ (12)
pap 2 pap
(9)
Therefore, adhesion strength enhancement due to n number
of wrinkles per unit area of the test probe is given by30
 
1
ss;w ¼ ðGc ðl þ 2zÞÞ (13)
zl
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Table 2 Summary of adhesion force characteristics in different wrinkle systems

System Normalized adhesion force to projected area, F Adhesion force enhancement descriptor, F

      1=2
pap 2 1 p Gc
F¼ ðGc ðl þ 2zÞÞ F0 ¼ 1þ ap 3=2
zl 2zl l E*
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Scheme 6. Contact splitting wrinkles in contact

with a at cylindrical probe surface

 2  
ac RGc 1=3
Fy ðGc 2 E * Rw Þ1=3 F 0y *
l lAE

Scheme 7. Non-planar wrinkle to a at contact

 

6pd0 3 12m 2=3 0 2v  qmax

F¼ F ¼1 þ tan2 1  gÞ
aA D 2  2v 2

Scheme 8. Complimentary wrinkles in contact

Fig. 2 A wrinkled poly(n-butyl acrylate) film in contact with a flat test probe. (a) Adhesion strength as a function of wrinkle wavelength. The
adhesion strength is increased significantly by lowering the wrinkle wavelength as the effect of contact splitting. (b) Adhesion strength test setup
with a detail simplification of wrinkle contact (c) Reproduced with permission from ref. 30. Copyright 2008 John Wiley and Sons.

3.2. Wrinkles in contact with a spherical probe
30
While Chan et al. reported enhanced dry adhesion strength
in a poly(n-butyl acrylate) (PnBA) elastomer when decreasing
wrinkle wavelength (typically in hundreds of microns), Lin
et al.59 observed totally opposite adhesion strength behavior
when PDMS wrinkles with wavelength in submicron to a few
microns are brought in contact with a spherical probe; that
is, the wrinkled surface has lower adhesion strength
compared to a at surface. It is suggested that there are two
limiting cases at wrinkle interfaces, which determine the
maximum adhesion force. Case I, low roughness or deep
indentation, where 1D ripples are attened in the contact
(Fig. 3a). Case II, high roughness or shallow indentation,
where the ripples are slightly attened because of the
change in the contact area of all individual ripples during
indentation (Fig. 3b). For case I, the pull-off force can be
estimated from eqn (8) with slightly modifying the
effective work of adhesion to compensate the energy
release Ur during indentation, which is a geometry-depen-
dent factor:
3
F¼ pRðGc  Ur Þ (14)
2

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!
pE * acw 2
Fmax;c ¼lavg (16)
4Rw

 1=3
Gc R2w
Here, acw y is the half-width of an approximated
E
rectangular contact area at the critical point with the presence
of wrinkles. Here, wrinkle geometry is simplied to a cylindrical
l2
contact with radius Rw y 2 . By taking Rw  R, the surface
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2p A
contact area at the maximum pull-off force is pa2c. The
maximum pull-off force is therefore58
 2
ac  2 * 1=3
Fmax;w y Gc E Rw (17)
l

Correspondingly, the adhesion force enhancement is58

 1=3  1=3
Fmax;w RGc RA Gc l
z z 2
: (18)
Fig. 3 Two limiting cases of PDMS microwrinkle dry adhesion in Fmax; smooth AE * l A2 E *
contact with a spherical probe. (a) Case I, low roughness or deep
indentation. (b) Case II, high roughness or shallow indentation. For
case II, the total adhesion force should consider the integration of The dependency of adhesion enhancement to the accumu-
each individual ripple during contact (c). (d) Comparison of experi- lative effect of the radius of curvature of the curvy substrate in
mentally measured pull-off force vs. prediction with two limiting cases. addition to the wavelength and the amplitude of the wrinkles as
Reproduced with permission from ref. 59. Copyright 2008 Royal shown in eqn (18) offers a new pathway to tune the adhesion
Society of Chemistry.
behavior of smart adhesives.

3.4. Adhesion strength of two complimentary wrinkling

For case II, the relation between strain and pull-off force is
more complicated since one should integrate the deection d of
each individual ripple during indentation, as shown in Fig. 3c.
The total pull-off force is given by
ð rmax
F¼ f ðdðrÞÞ2prdr (15)
0 D
and should be calculated numerically. Fig. 3d compares exper-
imental results with predictions from the two limiting cases.
For a small strain (<4%), the small-roughness model is accurate
due to the energy penalty to completely atten ripples that grow
very rapidly with increasing amplitude. The partial contact
model is accurate for an intermediate strain (4–13%) with a
characteristic strong decay in the pull-off force at large strain.
This may be due to the large energy loss associated with the
large deformation in the ripples. Nevertheless, the two models
have captured the effect of strain on adhesion at small and
moderate strain levels.
3.3. Curvy wrinkles in contact with a at probe surface
For the case when wrinkles are fabricated on a curved substrate,
Kundu et al. studied the adhesion behavior of a non-planar
wrinkle surface in contact with a at surface, as shown in
Scheme 7 in Table 2.58 In this system, the JKR pull-off force in
eqn (8) should be modied to accommodate the curvy contact of
the wrinkle surface. To simplify the model, the contact is started
by considering a cylindrical contact to a at surface with radius
Rw and lever arm length lavg. The maximum pull-off force in this
case is58
surfaces
In a single discontinuity surface, the maximum adhesion force,
Fmax, per unit width, a, is given by106
 2=3
12m
Fmax¼ (19)
aA
6pd03
Here, m is the shear modulus of the adhesive material as a
function of the dimensionless lm thickness H ¼ h/(D/12m)1/3,
where h is the lm thickness, D is the substrate bending rigidity,
A is the Hamaker constant and d0 is the universal cut-off
distance (0.15 nm).
On the other hand, when the adhesive material is dis-
continued, the maximum force to dissociate the surface
becomes much larger because of the requirement to initiate
crack formation behind the contact line:106
 1=3
h D
Fmax ¼ 3sc (20)
a 12m
Here, sc is the critical stress associated with crack nucle-
ation, and h is lm thickness.
The role of surface discontinuity is to pin the contact line and
prevent the crack from propagating until a threshold stress is
achieved. The maximum adhesion force per single discontinuity
is therefore started from crack nucleation at the incision and
vanishes at the other side of the incision. This adhesion pull-off

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force is then repeated to the next discontinuities presented on
the surface. Crack initiation requires much higher stress than
crack propagation on a smooth surface. The enhancement of
adhesion force due to the crack initiation on a discontinuous
surface is called the “crack arresting” mechanism. When the size
of the structure decreases to a characteristic stress-decay
 3 1=6
1 Dh
length, ¼ , the crack-initiation moment becomes
k 12m
constant, and the contribution from individual discontinuity
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can no longer be felt.107
Adhesion enhancement by the crack arrest mechanism has
been transferred into engineered surfaces by arresting the
propagation of the crack to the perpendicular direction by using
1-D channels or wrinkle structures. Majumdeer et al. rst
reported the observation of crack arresting when peeling off a
at PDMS plate from a PDMS adhesive with embedded 1-D
channels (channel diameter ¼ 50–800 mm).107 Microchannel
adhesives show signicant enhancement of adhesion (up to 30
times of smooth PDMS) as a result of crack arresting together
with capillary force. When the channels are lled with air or oil,
compressive stress is exerted on the elastic channel wall,
resulting in the buckling and bugling of the channel wall, which
affects the contact between the plate and channels. It is noted
that the adhesive surface is elastic, unlike the conventional
adhesive where adhesion enhancement is achieved by visco-
elasticity. In turn, the stress concentration and adhesive energy
during separation can be either enhanced or reduced depend-
ing on channel diameter, spacing and lm thickness.
Vajpayee et al.29 reported enhanced adhesion and selectivity
between two complimentary 1D ripple surfaces vs. the non-
complimentary ones (see schematic in Fig. 4a). To create the
complimentary ripples, rst, a rippled PDMS lm is fabricated
from the uniaxial stretching of a at PDMS strip, followed by
UVO treatment and releasing. The rippled PDMS strip is then
used as a master for replica molding the ones used in the
Fig. 4 Schematic illustrations of (a) complementarity between two surfaces of the same or different depth of grooves, and (b) sample fabrication
process. (c) Experimental setup for measuring adhesion (t ¼ 0.5 mm; d ¼ 170 mm). An exaggerated internal rippled interface is shown to guide the
eye. Images (b–c) are reprinted with permission from ref. 29. Copyright 2011 John Wiley and Sons.
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experiment. This way, the contribution of pre-stress and the
hard thin skin in the originally wrinkled lm are no longer a
concern. The molded PDMS strip is then treated with uo-
rosilane as a releasing agent, and the complementary one is
molded on top of it (see Fig. 4b). To control the amplitude of
rippled surfaces, different strains were applied to fabricate the
master ripples. Adhesion strength is measured from its corre-
lation to the crack length observed by an inverted microscope
when a cover slip was inserted between the two surfaces, as
shown in Fig. 4c.
It is important to point out that the enhanced adhesion
strength is highly dependent on the complementarity of rippled
surfaces. When the rippled surfaces are not complementary, e.g.
the counter ripple surface is with lower amplitude or at
compared to the ripple surface, the crack length grows to
innity until both surfaces are separated. There is a critical
threshold value to stop the crack growth rate, and it gives a
measure of the threshold of adhesion. Therefore, the determi-
nation of the optimum geometry to stop crack growth is key in
designing smart wrinkle-based dry adhesives e.g. with selec-
tively or fully adherent surfaces.
In an engaged pair of complementary, rippled surfaces with
wavelength l and amplitude A, the energy release rate Gmin will
 
qmax 29
be minimum at a value of qmax or Gmin ¼ Gc cos4 . Here,
2
1
qmax ¼ tan (2pĀ) is the crack growth angle from the direction
of the maximum energy release rate, where Ā is the normalized
ripple amplitude by ripple wavelength. Similar to adhesion in a
discontinued surface that we discussed before, a periodic vari-
ation in the energy release rate with crack length is observed
when separating two complementary ripple surfaces, leading to
crack arrest, followed by unstable propagation to the next point
of crack arrest. Such a rate dependence of the work of adhesion
removes the instability in crack growth. For mixed-mode
loading such as in this system, the energy release rate is related
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Fig. 5 Crack growth profile of two complimentary surfaces. (a) Flat, (b) low-amplitude surfaces and (c) high-amplitude ripple surfaces. The
effective work of adhesion of complimentary ripple surfaces as a function of amplitude. Reproduced with permission from ref. 29. Copyright
2010 John Wiley and Sons.

to the effective work of adhesion as108 G ¼ Grc(q ¼ 0, n) ¼ Gc(n) for particle “donor” lm to a “receiver” lm to pattern the nano-
both at and rippled interfaces. Here, n is the crack velocity. At particles using a enrolling-microcontact printing (EmCP)
any nite n, Gc(n) > G0c(n), W0c is for a at surface. Therefore, method (see Fig. 6).109 First, the 1D PDMS rippled lm is
adhesion enhancement in the rippled interface vs. the at wrapped onto a lint roller, which is then rolled onto a rigid, high
interface is given by29 surface energy substrate, Si wafer. Because PDMS wets well on

both Si wafer and silica nanoparticles, a conformal contact is
Gcr 2v qmax
  ¼1þ tan2 ð1  fÞ (21) formed between PDMS ripples and nanoparticles. When the
qmax 2  2v 2
Gc0 cos4 PDMS wrinkles are rolled onto and removed from the donor
2
substrate very fast, all nanoparticles are transferred onto the
ridges of the ripple surface. It has been suggested that the
Here, f is the parameter that determines the inuence of the kinetic control of dry adhesion from a at PDMS sheet is critical
phase angle, n is Poisson's ratio of the material (see Scheme 8). to transfer printing.110 The assemblies of nanoparticles on top
Fig. 5 shows the characteristic of crack growth on three different of the wrinkle ridges is in sharp contrast to the results when
complimentary surfaces: at, low-amplitude and high-ampli- dipping or spin-coating the wrinkles with a nanoparticle solu-
tude ripple surfaces. For a perfectly at surface (Fig. 5a), the tion, where the nanoparticles are assembled in the wrinkle
cracks grow in an apparently smooth and continuous manner trenches driven by capillary force. When enrolling the nano-
until the lms are peeled off from each other. On peeling off particle lm at a speed of 1 cm s1 onto a “receiver” substrate,
low-amplitude ripple surfaces (A ¼ 1.8 mm), the cracks grow nanoparticles are transferred, lines of 10 mm in width are
relatively steadily in an orthogonal direction from the main formed, with the same ridge size as the original wrinkle master.
crack (see Fig. 5b). The cracks halt intermittently with subse- This method offers the advantage of non-contaminant dry
quent growth involving the nucleation of a forward notch, fol-
lowed by its lateral growth to cover the entire length of the next
ripple. A signicant increase in adhesion strength is observed in
high-amplitude ripple surfaces (A ¼ 6.4 mm) (see Fig. 5c). In this
case, peeling off both surfaces requires the formation of inter-
facial cavities ahead of the crack front before merging with the
main crack, leading to signicant adhesion enhancement as
described in eqn (21). The comparison of experiments and
theory of the adhesion enhancement on two complimentary
ripple surfaces is shown in Fig. 5d. It is clear that the amplitude
plays a critical role in the adhesion strength of rippled surfaces.

4. Applications
Given the simplicity in fabrication and rich mechanisms to
manipulate wrinkle dry adhesives, researchers have begun to
exploit their applications. For example, Badre et al. demon-
strated the selective transfer of 100 nm nanoparticles from a
Fig. 6 (a) Schematic illustration of enrolling-microcontact printing
(EmCP) to selectively transfer nanoparticles layers based on the
dimension of the wrinkle surface. (b) SEM images of a PDMS wrinkle
and of transferred nanoparticle assemblies (1D and 2D) from the EmCP
process.

Soft Matter This journal is © The Royal Society of Chemistry 2014


Review
adhesion based on loading and release without the use of any
lithographic steps. The nanoparticles can be printed on both
rigid (e.g. Si) and so (e.g. PDMS) substrates.
Because PDMS is elastomeric, wrinkled PDMS can be
reversibly stretched and released to adjust surface roughness
(see Fig. 7A) and thus adhesive strength. Lin et al. demonstrated
“pick and release” of a glass sphere using a rippled PDMS lm
(see Fig. 7B).59 Here, the wrinkled surface is fabricated from a
siliceous/PDMS bilayer system. The 1D ripple surface is
Published on 06 June 2014. Downloaded by University of Texas Libraries on 18/06/2014 08:40:24.
mechanically stretched to a nearly attened state, achieving
large contact area with the glass bead. When the stretched
surface was released, the at state surface comes back to the
ripple surface with lower adhesion strength to the glass bead,
resulting in the release of the glass bead. Here, the use of
mechanical force to stretch and release the wrinkles offers
advantages to “pick, transfer, and release” individual compo-
nents with different sizes and shapes in real time.
A further exploitation of the wrinkle adhesive is to combine
the wrinkle surface with a spatula-like micropillar array as
demonstrated by Jeong et al. (see Fig. 8).31 The adhesive is made
by replica molding of PDMS from a negative silicon mold of
micropillars array (20 mm in diameter, space, and height) with
at heads. The spatulate at head of pillars is fabricated by the
over etching of the Si lm deposited on a Si-on-insulator (SOI)
wafer. PDMS micropillars with enlarged tips are then exposed to
UVO with a pre-strain of 3%. To prevent undesired surface
oxidation, the PDMS micropillar heads are capped with a thin
layer of poly(urethane acrylate) (PUA) prior to UVO treatment,
which is later removed using a scotch tape. Detailed fabrication
steps with SEM images of the surfaces in adhesion-On and Off
states can be seen in Fig. 8a and b.
Fig. 7 “Pick and release” of a glass sphere using a rippled PDMS film. (A) 3D surface contour of the ripple surfaces stretched to different degrees.
(B) Optical images of picking and release of the glass sphere. The sphere is lifted up (a–c) when the rippled PDMS film is stretched flat (high
adhesion) and dropped (d) as the stretch is released (reduced adhesion). When the sample is unstretched (rippled, low adhesion), the adhesion
force is too low to lift the glass ball (e–g). Insets: Schematic drawing of the status of strain on the PDMS film. Images are reproduced with
permission from ref. 59. Copyright 2008 The Royal Society of Chemistry.
This journal is © The Royal Society of Chemistry 2014
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Soft Matter
Similar to the on-demand transfer method by Lin et al.,59
here the adhesion-On and Off states are achieved by the
stretching and releasing of the underlying adhesive pad (PDMS,
thickness 1 mm, size 1  1 cm2). When the pad is wrinkled, the
micropillars are tilted against the neighboring ones, resulting
in the very small contact point of the pillar heads to the counter
surface. The stretching of the adhesive pad causes the pillars to
revert to the vertical position, where the heads could touch the
counter surface perfectly. Shear adhesion strength up to 15 N
cm2 and normal adhesion strength up to 11 N cm2 are
achieved in this system due to a large contact area of spatula-
like micropillars on the adhesive pad to the counter surface in
the adhesion-On state (see Fig. 8c). Upon releasing the strain in
the adhesion-Off state (see Fig. 8d), the adhesion strength is
reduced to nearly zero and 0.98 N cm2 in the shear and normal
direction, respectively. The conformal contact of spatulate at
heads on the micropillars has contributed signicant increase
in adhesion strengths compared to that of a at PDMS sheet,
which are 2.65 and 2.06 N cm2 in the shear and normal
direction, respectively. Without the at heads, the adhesion
strength is nearly zero since the dimension of micropillars does
not satisfy the contact splitting threshold.6 The high hysteresis
in adhesion strength between the adhesion-On and Off states is
therefore very benecial for the manipulation of the on-demand
adhesives. It is important to note that wrinkle adhesives are very
stable structures due to the relatively small aspect ratio
(amplitude/wavelength, less than 0.3). They do not collapse or
bundle during repeated use, which micropillar adhesives oen
suffer from. Most wrinkle adhesives could sustain the adhesion
performance for more than 100 cycles without signicant loss of
their adhesion strength, as shown in Fig. 8e.
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Fig. 8 An on-demand adhesive from hybrid spatula-like micropillars on a PDMS ripple substrate. (a) Illustration of fabrication steps. (b) SEM
images of the hybrid adhesive with adhesion-On (top) and adhesion-Off (bottom) states. The adhesion-On state is achieved by stretching the
wrinkled substrate into a flat condition for the maximum contact of spatula-ended pillars to the counter surface. The adhesion-Off state is
achieved by releasing the strain. Adhesion strength characteristics are shown in shear (c) and normal (d) directions. (e) Adhesion cycling test.
Reproduced with permission from ref. 31. Copyright 2010 American Chemical Society.

5. Perspectives
Wrinkle adhesives have very unique characteristics for dry
adhesion. It is simple yet versatile to fabricate wrinkles with
different sizes (from hundreds of nanometers to hundreds of
microns) and morphologies in a wide range of material systems.
The adhesion can be enhanced or reduced in comparison to the
smooth surface depending on the wrinkle dimension vs. the
contact surface and whether the contact surface is at, hemi-
spherical, spherical or complementary to the wrinkles, as well
as different materials chemistry and intrinsic properties.
Further, they can be integrated with other type of adhesives,
such as micropillars, to signicantly enhance the adhesive
strength without suffering undesired instabilities. The real-time
application, selectivity, robustness, and on-demand pick,
transfer and release will add important values to the existing dry
adhesive systems for applications such as electronics and
robotics. Although we review several wrinkle adhesive systems,
our understanding and manipulation of wrinkle-based dry
adhesion has just begun. The tuning of materials chemistry and
bulk properties, for example, using shape memory poly-
mers64,65,93,111 and liquid crystal elastomers that can change
modulus or internal strain near the phase transition tempera-
tures coupled with tunable wrinkle topography are yet to be
developed and understood. With all wrinkle adhesion charac-
teristics, it is rational to expect that even more divergent
applications of dry adhesives could evolve.
Acknowledgements
This work is supported by the National Science Foundation
(NSF) GOALI grant (# DMR-1105208).
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