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of Texas Libraries on 18/06/2014 08:40:24. Soft Matter REVIEW View Article Online View Journal Recent advances

Recent advances in wrinkle-based dry adhesion

Cite this: DOI: 10.1039/c4sm00027g

Received 7th January 2014 Accepted 1st May 2014

DOI: 10.1039/c4sm00027g

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

Surface wrinkles driven by elastic instabilities have attracted signicant interest in the eld 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 di erent methods to prepare wrinkle surfaces, we focus on the investigation of dry adhesion mechanisms in di erent material systems. By exploiting wrinkle dimension, morphology, modulus, curvature, and di erent contacting surfaces (at, 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.

1 Introduction

Surface textures have profound impact on adhesion properties, which are crucial to bioorganisms, 1 4 synthetic structural adhesives 5 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 eect 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 insects 1,2 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:

b Center for Convergence Advanced Materials, Surya University, Jl. Scientia Boulevard Blok U/7, Summarecon Serpong, Tangerang, 15810 Indonesia

structures normally involves costly and time-consuming multi- step processing in photolithography and so lithography. 7,21 Furthermore, the fabricated high-aspect-ratio brillar-like structures are oen 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 di erence 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 side 29,30,57 62 or on both sides 63 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 di erent 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 eect of the aforementioned structural parameters. We further discuss the role of materials properties, including modulus, surface energy and viscoelas- ticity. The e ect 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 di erent 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 connement, 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 15). Among di erent 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 13). The

on a compliant substrate (see Schemes 1 – 3). The Fig. 1 Components and parameters in

Fig. 1 Components and parameters in the wrinkle structure. The dierence 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

l ¼ 2p t "

1 v s 2 E c

E s # 1=3

3 1 v c 2


Here, t is the hard skin layer thickness, E s and E c are Young's moduli, and v s and v c are Poisson's ratios of the substrate and the thin coating, respectively. The critical compressive strain to induce wrinkling 3 c and the amplitude A are given by 36,44,96,97

3 c z 0: 52 " 1 v c 2 1 v s 2

E s

E c # 2 =3

A z l







when E s / E c 1, where 3 is the applied compressive strain ( 3>3 c ). eqn (1) shows that the wrinkle wavelength increases with the lm thickness, or the di erence 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 W adh , de ned as 98,99

W adh ¼ W 12 ¼ g 1 + g 2 g 12


Here g is the surface energy, and g 12 is the interfacial energy of components 1 and 2. When the two components are of the same material with surface energy g , W adh ¼ 2 g . Here W adh 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


Schematic illustration


  36, 37, 51, 67, 68, 72, 73, 75, 76 and 93

36, 37, 51, 67, 68, 72, 73, 75, 76 and 93

A mechanically or thermally stressed bilayer system

Swelling of a

laterally conned bilayer or a graded polymer


Drying of a solgel lm

Skin: metal, siliceous lms, foundation: elastomer, compressive stress: externally induced from modulus mismatch or external force

Skin: polymer or oxide of a higher or lower modulus than the foundation material, foundation:

a compliant or glassy

polymer, compressive stress:

osmotic pressure-induced stress release

Skin: a gelated lm or segregated lm by external stimuli, foundation: sol or a pre-polymer solution, compressive stress: modulus mismatch due to solvent evaporation

Scheme 1. Metal deposited on a sosubstrate

evaporation Scheme 1. Metal deposited on a so  substrate 26, 41, 52, 80, 83 –

26, 41, 52, 80, 8386, 94 and 95

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

of oxygen plasma or UVO-treated elastomeric sheet 69 and 112 Scheme 3. UV or ion beam

69 and 112

Scheme 3. UV or ion beam bombardment or corona discharge-induced wrinkling

ion beam bombardment or corona discharge-induced wrinkling 42, 56, 79 and 81 Scheme 4. Swelling of

42, 56, 79 and 81

Scheme 4. Swelling of a laterally conned polymer lm

4. Swelling of a laterally con  ned polymer  lm 91, 92 Scheme 5. Drying

91, 92

Scheme 5. Drying of a solgel lm

thermodynamic value due to dissipative energy away from the interface. For non-equilibrium contact, the critical strain energy release rate G c should be used by compensating the nature of contact (e.g. the contact area). It is given by 57 P f

W adh ¼ G c ¼


8pE * a p 3


Here, P f is the maximum separation force of a at surface, E * is e ective modulus, which will be de ned later and a p is the

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radius of the test probe. G c 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 by 99

W adh ¼ W 12


2 h g d g




0: 5 ð g p


g p Þ 0: 5 i



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 innite 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

the Hertz equation as a 3 ¼ 3RF . Here, R is the radius of a


E *

hemisphere, E * is the e ective modulus of the system given

E 2 ð 1 v 1 2 Þ E 1 þ E E 1 ð 1 v 2 2 Þ and F is the compressive

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 KendallRobert (JKR)

as 101,102

by E * ¼


a 3 ¼ 4E 3R * F þ 3p Rg þ 6p R gF þ ð 3 pR g Þ 2 1= 2


Here, the elastic stress at the edge of the contact is assumed to be innite, and the adhesion force could deform hemi- spherical surfaces into the equilibrium contact area. The result is a nite pull-o force as

F JKR ¼ (3/2) p RG c


When the contacting surface is sti, 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-o force using the Hertzian contact area, which is given by F DMT ¼ 2p RG c . 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 e ective Young's modulus E e of HAR brillars can be calculated as 16

E eff ¼

3EI r sin b

L 2 cos 2 b½ 1 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 coe cient 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-o force in eqn (8) should be modied to accommodate the geometry e ect. The modied-JKR adhesion model based on contact line is 104

F ModJKR ¼ 3.16( KG c 2 r ) 1/3 L


where r is the radius of brillars, and K ¼ 4 E */3. When a wrinkled surface is in contact with a substrate ( at, hemispherical, or self-similar wrinkles), adhesion strength can be enhanced or reduced. Dierent wrinkle-based dry adhesion systems are summarized in Table 2 (see Schemes 68).

3.1. Wrinkles in contact with a at surface

The pull-o 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 r t , with the

total splitting protrusion N ¼ R / r t . 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 becomes 6,105

F t




N 2 p RG c



Therefore, it is apparent that the advantage of splitting contact points into smaller discrete contact points is to generate 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 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 k 1 l and contact width l /2. Here, k 1 is a geometry constant rendering the average contact length in respect to its wavelength. 39 The number of




wrinkles per unit area of the test probe is n ¼ p zl , where a p is

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 s s,s : 30

s s ;s ¼ 8p E * G c a p 3 1= 2

p a p 2

¼ 8E * G c


a p

1 =2


Therefore, adhesion strength enhancement due to n number of wrinkles per unit area of the test probe is given by 30

s s; w ¼

zl ð G c ð l þ 2z ÞÞ



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Table 2 Summary of adhesion force characteristics in dierent wrinkle systems


Normalized adhesion force to projected area, F

Adhesion force enhancement descriptor, F

projected area, F Adhesion force enhancement descriptor, F F ¼ p a p 2 zl ð



pa p 2


ðG c ðl þ 2z ÞÞ

Scheme 6. Contact splitting wrinkles in contact with a at cylindrical probe surface

in contact with a  at cylindrical probe surface F y a c 2 ð G


y a c 2 ðG c 2 E * R w Þ 1=3


Scheme 7. Non-planar wrinkle to a at contact

1 = 3 l Scheme 7. Non-planar wrinkle to a  at contact F ¼ 6


¼ 6pd 0 3 aA




Scheme 8. Complimentary wrinkles in contact

F 0 ¼

1 þ

2zl p l


a p 3=2

G c




F 0 y

RG c

* 1=3


F 0 ¼ 1 þ

2v v tan 2 1 g Þ q max




þ 2 v v tan 2 1 g Þ q m a x 2 2 2

Fig. 2 A wrinkled poly(n-butyl acrylate) lm in contact with a at test probe. (a) Adhesion strength as a function of wrinkle wavelength. The adhesion strength is increased signicantly by lowering the wrinkle wavelength as the eect of contact splitting. (b) Adhesion strength test setup with a detail simplication 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

While Chan et al. 30 reported enhanced dry adhesion strength in a poly( n -butyl acrylate) (P n BA) 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 inte rfaces, which determine the maximum adhesion force. Case I, low roughness or deep indentation, where 1D ripples are attened in the contact

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(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-o force can be estimated from eqn (8) with slightly modifying the e ective work of adhesion to compensate the energy release U r during indentation, which is a geometry-depen- dent factor:

F ¼

2 3 pR ð G c U r Þ


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of Texas Libraries on 18/06/2014 08:40:24. Soft Matter Fig. 3 Two limiting cases of PDMS microwrinkle

Fig. 3 Two limiting cases of PDMS microwrinkle dry adhesion in 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 each individual ripple during contact (c). (d) Comparison of experi- mentally measured pull-oforce vs. prediction with two limiting cases. Reproduced with permission from ref. 59. Copyright 2008 Royal Society of Chemistry.

For case II, the relation between strain and pull-o 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-o force is given by


F ¼ ð 0


f ð dð r ÞÞ 2p r dr


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-o 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 e ect 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-o force in eqn (8) should be modied 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 R w and lever arm length l avg . The maximum pull-o force in this case is 58

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F max; c ¼l avg


E * a cw


4R w



Here, a cw y


c R




1 =3

is the half-width of an approximated

rectangular contact area at the critical point with the presence of wrinkles. Here, wrinkle geometry is simpli ed to a cylindrical



contact with radius R w y 2p 2 A . By taking R w R , the surface


contact area at the maximum pull-o force is p a . The maximum pull-o force is therefore 58


F max; w y





G c 2 E * R w 1=3


Correspondingly, the adhesion force enhancement is 58

F max ; smooth z


max; w

RG * c 1 =3 z RA G c l

l 2 : A 2 E


* 1 =3


The dependency of adhesion enhancement to the accumu- lative e ect of the radius of curvature of the curvy substrate in addition to the wavelength and the amplitude of the wrinkles as shown in eqn (18) o ers a new pathway to tune the adhesion behavior of smart adhesives.

3.4. Adhesion strength of two complimentary wrinkling


In a single discontinuity surface, the maximum adhesion force, F max , per unit width, a, is given by 106





2 =3




6p d


Here, m is the shear modulus of the adhesive material as a function of the dimensionless lm thickness H ¼ h /(D/12 m) 1/3 , where h is the lm thickness, D is the substrate bending rigidity, A is the Hamaker constant and d 0 is the universal cut-o 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

F max ¼ 3s c


a 12m 1= 3



Here, s c 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-o

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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 arrestingmechanism. When the size of the structure decreases to a characteristic stress-decay

length, 1 k ¼ Dh 12m 1 =6

constant, and the contribution from individual discontinuity 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 o a at PDMS plate from a PDMS adhesive with embedded 1-D channels (channel diameter ¼ 50 800 m m). 107 Microchannel adhesives show signicant 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 aects 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.

, the crack-initiation moment becomes


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

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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, di erent 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 innity 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 G min will

be minimum at a value of q max or G min ¼ G c cos 4 q max . 29 Here,


q max ¼ tan 1 (2p A) is the crack growth angle from the direction



of the maximum energy release rate, where A 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

such as in this system, the energy release rate is related Fig. 4 Schematic illustrations of

Fig. 4 Schematic illustrations of (a) complementarity between two surfaces of the same or di erent 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 (bc) are reprinted with permission from ref. 29. Copyright 2011 John Wiley and Sons.

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18/06/2014 08:40:24. Soft Matter View Article Online Review Fig. 5 Crack growth pro fi le of

Fig. 5 Crack growth prole of two complimentary surfaces. (a) Flat, (b) low-amplitude surfaces and (c) high-amplitude ripple surfaces. The eective 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 e ective work of adhesion as 108 G ¼ G c r (q ¼ 0, n) ¼ G c (n) for both at and rippled interfaces. Here, n is the crack velocity. At any nite n, G c (n) > G (n), W 0 is for a at surface. Therefore, adhesion enhancement in the rippled interface vs. the at interface is given by 29







G cos 4 q max




¼ 1 þ

2 2v v tan 2 ð 1 f Þ q max




Here, f is the parameter that determines the in uence of the phase angle, n is Poisson's ratio of the material (see Scheme 8). Fig. 5 shows the characteristic of crack growth on three di erent complimentary surfaces: at, low-amplitude and high-ampli- tude ripple surfaces. For a perfectly at surface (Fig. 5a), the cracks grow in an apparently smooth and continuous manner until the lms are peeled o from each other. On peeling o low-amplitude ripple surfaces ( A ¼ 1.8 mm), the cracks grow relatively steadily in an orthogonal direction from the main crack (see Fig. 5b). The cracks halt intermittently with subse- 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 m m) (see Fig. 5c). In this case, peeling oboth 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

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particle donor lm to a receiver lm to pattern the nano- particles using a enrolling-microcontact printing (Em CP)

method (see Fig. 6). 109 First, the 1D PDMS rippled lm is wrapped onto a lint roller, which is then rolled onto a rigid, high surface energy substrate, Si wafer. Because PDMS wets well on both Si wafer and silica nanoparticles, a conformal contact is

formed between PDMS ripples and nanoparticles. When the PDMS wrinkles are rolled onto and removed from the donor substrate very fast, all nanoparticles are transferred onto the ridges of the ripple surface. It has been suggested that the kinetic control of dry adhesion from a at PDMS sheet is critical to transfer printing. 110 The assemblies of nanoparticles on top of the wrinkle ridges is in sharp contrast to the results when dipping or spin-coating the wrinkles with a nanoparticle solu- tion, where the nanoparticles are assembled in the wrinkle trenches driven by capillary force. When enrolling the nano- particle lm at a speed of 1 cm s 1 onto a receiver substrate, nanoparticles are transferred, lines of 10 m m in width are formed, with the same ridge size as the original wrinkle master. This method o ers the advantage of non-contaminant dry

This method o ff ers the advantage of non-contaminant dry Fig. 6 (a) Schematic illustration of

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 E mCP process.

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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 releaseof 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 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 o ers advantages to pick, transfer, and releaseindividual compo- nents with di erent 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 m m 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 O states can be seen in Fig. 8a and b.

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Similar to the on-demand transfer method by Lin et al. , 59 here the adhesion-On and O states are achieved by the stretching and releasing of the underlying adhesive pad (PDMS, thickness 1 mm, size 1 1 cm 2 ). 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 cm 2 and normal adhesion strength up to 11 N cm 2 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-O state (see Fig. 8d), the adhesion strength is reduced to nearly zero and 0.98 N cm 2 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 cm 2 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 O 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 oen suer 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.

cant loss of their adhesion strength, as shown in Fig. 8e. Fig. 7 “ Pick and

Fig. 7 Pick and releaseof a glass sphere using a rippled PDMS lm. (A) 3D surface contour of the ripple surfaces stretched to dierent degrees. (B) Optical images of picking and release of the glass sphere. The sphere is lifted up (a c) when the rippled PDMS lm is stretched at (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 (eg). Insets: Schematic drawing of the status of strain on the PDMS lm. Images are reproduced with permission from ref. 59. Copyright 2008 The Royal Society of Chemistry.

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18/06/2014 08:40:24. Soft Matter View Article Online Review Fig. 8 An on-demand adhesive from hybrid spatula-like

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-O (bottom) states. The adhesion-On state is achieved by stretching the wrinkled substrate into a at condition for the maximum contact of spatula-ended pillars to the counter surface. The adhesion-O 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 di erent 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 di erent 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 suering 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- mers 64,65,93,111 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.

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This work is supported by the National Science Foundation (NSF) GOALI grant (# DMR-1105208).

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