1. Introduction
Flexible inorganic electronic devices, which are prepared by integrating ultrathin functional elements based on traditional inorganic semiconductor materials with flexible substrates, have shown attractive application prospects in the fields of the optical/electronic industry and medical treatment due to their good electronic properties and unique flexibility [
1]. One key step in the fabrication of flexible inorganic electronic devices is the epitaxial growth of inorganic thin films [
2]. To meet this processing requirement, multiple thin film transfer techniques have been developed, such as temporary wafer bonding [
3] and transfer printing methods [
4]. Among these techniques, microtransfer printing is one of the most widely used transfer printing methods due to the advantages of environment-independent temperature/corrosion properties, repeatability, and high precision [
5]. The principle of the microtransfer printing technique is to transfer thin film components prefabricated on donor substrate (i.e., inorganic semiconductor substrate) to target substrate (i.e., flexible substrate) using a flexible stamp. Two steps including picking-up and printing are commonly involved in this technique. In the picking-up step, the stamp is brought into contact with the thin film and then peeled away to remove the film from the donor substrate, while in the printing step, the inked stamp contacts the target substrate and is retrieved to print the film onto the target substrate. The interfacial adhesion caused by van der Waals interactions at the micro scale is the pivotal factor influencing these two steps [
5]. Successful microtransfer printing requires that the adhesion at the stamp/film interface is stronger than that at the film/donor substrate interface to delaminate the film and the donor substrate in the picking-up step, while it is weaker than that at the film/target substrate interface to delaminate the film and the stamp in the printing step [
6]. However, the above requirements cannot always be satisfied, and controls of adhesion and delamination at interfaces, especially the stamp/film interface, still have difficulties [
7,
8]. To date, obtaining a high fabrication yield remains challenging [
5,
9,
10], and thus the industrial application of microtransfer printing is delayed [
1]. To optimize the existing microtransfer printing technologies and develop new efficient methods, many efforts have been made to develop methods for regulating the adhesion between stamp and film [
1,
5]. Evaluating the feasibility of adhesion regulation methods primarily requires prediction of the mechanical behaviors of the stamp/film interface.
As far as the numerical techniques for predicting the adhesion/delamination characteristics of the stamp/film interface are concerned, three kinds of mechanical models including a model based on J-integral theory, a model based on the virtual crack closure technique (VCCT), and a model based on the cohesive zone method (CZM) are mainly used. Both the model based on J-integral theory and that based on the VCCT treat the interface adhesion/delamination in the microtransfer printing process as a crack propagation problem and evaluate the adhesion or delamination state of the interface according to the energy release rate, defined as the energy per area necessary to cause the crack to propagate [
7,
11]. The J-integral is an energy contour integral proposed to quantitatively characterize the strength of the stress and strain field around a crack tip, which equals the energy release rate for linear elastic fracture problems [
12]. Based on the J-integral method, Tucker et al. [
7] established a mechanical model of the stamp-film-substrate system and calculated the energy release rate by introducing initial cracks at the interface and using finite element simulation. Effects of the initial crack length and interface toughness on the interface adhesion/delamination behaviors were investigated. However, the stamp was modeled as an elastic solid. Cheng et al. [
13] abandoned the elastic assumption of the stamp and proposed a viscoelastic model for calculating the energy release rate at the stamp/film interface from the J-integral. The pull-off force required to fail the interface was obtained by setting the energy release rate equal to the interface toughness, and the superiority of the finite element model to the analytical model in revealing the relationship between pull-off force and pulling speed was demonstrated. Similar to the J-integral method, the VCCT method, which was proposed based on the Irwin energy theory [
14], is another commonly used technique to calculate the energy release rate. This method assumes that the strain energy released upon an increment of crack growth is equal to the energy required upon the same increment of crack closure. Based on the VCCT method, Carlson et al. [
15] illustrated influences of the shear displacement of the stamp on the energy release rate by establishing and solving a finite element model of the stamp–film system containing an interfacial preset crack. Simulation results of the pull-off force reflected similar trends to the experimental ones even though the preset crack length was arbitrary. Furthermore, the VCCT method was also adopted by Kim-Lee et al. [
11] and Minsky et al. [
16] to examine the effects of different factors on the adhesion behavior at the stamp/film interface and provide understanding of the mechanics of interface delamination. However, in the above three studies, the material of the stamp was assumed to be linear elastic. Different from the J-integral method and VCCT method, the model based on the CZM treats the interface adhesion/delamination in the microtransfer printing process as an interface damage problem and evaluates the adhesion or delamination state of the interface according to the cohesive law [
17]. In this method, a cohesive interface is defined at the stamp/film interface and the cohesive law characterizing the interface traction force–separation displacement relationship is used to describe the non-linear nature of the interface strength. Using the CZM approach, Jiang et al. [
17] modeled the viscoelastic stamp/film interface and investigated the effects of the viscoelastic modulus and relaxation time of the stamp on the area of retrieved film in the stamp through finite element simulations. Subsequently, Al-okaily et al. [
18] adopted the CZM approach to model the stamp/film interface thermo-mechanical delamination in the laser microtransfer printing technique and demonstrated the capabilities of this approach. Both of the above studies applied the bilinear cohesive law to represent the degradation and failure of the stamp/film interface.
Although the above mechanical models provide methods for predicting the interface adhesion/delamination behavior, their applicability is not clear as they are used separately in different studies. In order to determine the suitability of these three numerical calculation models, this paper intends to compare the results of these models and determine the most proper one. To achieve this, the layout of this paper is arranged as follows. First, interface mechanical models based on the J-integral theory, VCCT, and CZM are established for the microtransfer printing problem of a thin film by a flat stamp using the classical kinetically controlled operation mode. Then, these three models are solved separately by adopting the commercial finite element package Abaqus to obtain the adhesion/delamination behavior of the stamp/film interface. Their results are compared and analyzed to assess the applicability of different models and determine the most suitable model. Finally, the influences of the microtransfer printing technological parameters and material interface parameters on the mechanical behavior of the stamp/film interface are investigated. For the convenience of analysis, the materials of the film and stamp are selected to be silicon and polydimethylsiloxane (PDMS), respectively, which were adopted in most of the previous studies [
7,
11,
15,
16,
17,
18]. For other materials, the simulation approaches and calculation methods presented in this paper can also be applied.
2. Stamp/Film Interface Mechanical Models
Figure 1 shows the schematic diagram of the stamp, film, and interface, in which the film thickness
hfilm is much smaller than the stamp thickness and the film width
wfilm is much smaller than its length. Therefore, the film and stamp can be taken to deform under the plane strain conditions. To predict the adhesion/delamination mechanical behaviors of the stamp/film interface, the models based on J-integral theory, the VCCT, and the CZM are established in this section and an energy-based criterion for crack propagation is used. The Griffith criterion [
19] is a simple and effective fracture criterion selected in J-integral theory and VCCT [
7,
11].The crack propagation condition given by the Griffith criterion is
G >
Γ0, in which
G denotes the energy release rate and
Γ0 is the interface toughness measured by experiments. In J-integral theory, the J-integral value is equivalent to the energy release rate for linear elastic materials, which were assumed in previous studies [
7,
11]. The VCCT is a method proposed based on the Griffith criterion [
20]. Furthermore, in the cohesive zone model, an energy-based crack propagation criterion in which the area enclosed under the traction–separation curve equals the critical energy release rate is often utilized [
17]. Therefore, through the parameter energy release rate, the models based on the J-integral, VCCT, and CZM can be linked and compared. Brief introductions of the establishing methods for these three models are presented as follows.
2.1. Mechanical Model Based on J-Integral Theory for the Stamp/Film Interface
The J-integral denotes the path-independent contour integral around the crack tip [
12], which is proposed based on the energy conservation principle and can evaluate the available energy to delaminate the given interface. Under the linear elastic fracture mechanics assumption, the J-integral value equals the energy release rate, and its definition for two-dimensional problems can be expressed as [
12]
where
and
.
ui denotes the displacement vector, d
s is the increment of length along the integral path,
τ represents the path around the crack tip,
w is the strain energy density, and
Ti denotes the stress component at any point along the integral path.
σij and
εij are the stress and strain tensors, respectively, and
nj is the unit normal vector along the integral path.
In order to use the finite element method to calculate the J-integral at the crack tip of the stamp/film interface, cracks with length
c at both ends of the interface need to be preset, as shown in
Figure 2a. The two-dimensional finite element model established in Abaqus software [
21] is shown in
Figure 2b. The mesh elements near the crack tip are locally refined to improve the accuracy of calculation. Swept mesh is adopted in the refinement zone and generated along the sweep path to improve the mesh quality.
2.2. Mechanical Model Based on the VCCT for the Stamp/Film Interface
In the virtual crack closure technique (VCCT), the energy release rate is evaluated according to the force at the node of the crack tip and the displacement at the node behind the crack tip. For the two-dimensional problem, the energy release rate
G for four-noded elements is calculated as [
22]
where
GI and
GII are components of the energy release rate under crack-opening mode I and in-plane shear mode II, respectively.
B is the thickness of the cracked body, Δ
a is the micro-increment of crack,
Fx1 and
Fy1 are the force components acting on node 1 of crack tip, and Δ
v3,4 is the opening displacement between nodes 3 and 4 behind crack tip.
In order to calculate the energy release rate at the crack tip of stamp/film interface by combining the VCCT and finite element method, initial defects, i.e., cracks, should be specified at the interface. As shown in
Figure 3a, the introduction of initial cracks with length
c in the unbonded area at both ends of the interface can be realized by setting bonding units in the middle area of the interface. The two-dimensional finite element model established in Abaqus is shown in
Figure 3b.
2.3. Mechanical Model Based on the CZM for the Stamp/Film Interface
The cohesive zone method (CZM) is a widely used theory based on damage mechanics for predicting crack initiation and propagation [
23]. It regards the vicinity of the crack tip as a crack process zone [
24], and the cohesive damage zone is formed by introducing the degradation mechanism (that is, the material softening or weakening) in front of the crack. The constitutive relationship between surface traction force and relative separation displacement at the interface in the cohesive zone, which is known as the traction–separation law or cohesive law, is used to describe the adhesion between materials. The form of the traction–separation law, such as the commonly encountered Dugdale law, bilinear law, and exponential law, as shown in
Figure 4, is crucial to the effectiveness of simulating the interface [
25]. The essence of the traction–separation law is to characterize the interaction between atoms or molecules of the material [
26]. For the microtransfer printing technique, it is usually carried out in dry and uncharged environments, and the van der Waals force is the main source of the interaction between atoms or molecules. Therefore, the normal interaction at the stamp/film interface can be characterized by the Lennard–Jones surface force law derived from the intermolecular pair potential, which is written as [
27]
where
Tn is the normal adhesive force per unit area between two surfaces, Δ
n denotes the surface relative displacement, Δ
γ is the work of adhesion, and
ε denotes the equilibrium distance between two flat surfaces.
Comparisons between the Lennard–Jones surface force law and three commonly used traction–separation laws are depicted in
Figure 4, in which
Tmax denotes the maximum traction force and
δn is the characteristic length in the normal direction. It can be seen that the traction–separation displacement relationship described by the exponential law is close to that described by the Lennard–Jones surface force law, which can be used to analyze the adhesion/delamination problem at the stamp/film interface.
The control equations of the exponential law in the two-dimensional plane state [
28] are
where
Tn and
Tt are normal and tangential tractions across the surface, respectively.
ϕn is the fracture energy of normal separation.
σmax is the normal strength at the cohesive surface, that is, the maximum stress. Δ
n and Δ
t are the interface separation displacements in the normal and tangential directions, respectively, and
δn and
δt are the corresponding characteristic lengths.
q =
ϕt/
ϕn and
r = Δ
n*/
δn are the coupling constants between the normal and tangential directions.
ϕt is the fracture energy of tangential separation. Δ
n* is the normal displacement after complete shear separation under
Tn = 0.
In order to analyze the interface adhesion/delamination problem by combining the CZM with the finite element method, cohesive elements with properties following the traction–separation law should be preset along the interface, as shown in
Figure 5a. In addition, the model shown in
Figure 5b, which introduces initial cracks with length
c at both ends of the interface through inserting cohesive elements only in the middle region of the stamp/film interface, is also established. This model is used to compare with the model based on the VCCT and investigate the influence of initial cracks on the mechanical behaviors of the interface. The two-dimensional finite element models established in Abaqus are shown in
Figure 5c,d. Since the exponential law represented by Equations (4) and (5) is not available as cohesive elements in commercial finite element software, the user subroutine approach [
29] is used in the present analysis to develop user-defined cohesive zone elements at the stamp/film interface.
In the above three kinds of finite element models, the stamp and film are simulated by the plane strain reduction integral element (CPE8R), and the number of elements and nodes are determined by the mesh-independent analysis. The boundary conditions are that the bottom boundary of the film is constrained and the displacement load is applied on the top boundary of the stamp.
4. Conclusions
Mechanical models based on J-integral theory, the VCCT, and the CZM for predicting adhesion/delamination behaviors at the stamp/film interface were developed and simulated through finite element modeling in this study. The pull-off force required to fail the interface were extracted from the results of these three models, and its variations with the preset crack length were presented. Through comparing between the simulation results and previous experimental results, the choice of a priority mechanical model was determined. Furthermore, to provide insight into the mechanical characteristics at the stamp/film interface, the effects of the microtransfer printing technological parameter and interface material parameters on the pull-off force were inspected based on the priority model. The main conclusions are as follows.
The major disadvantage for models based on J-integral theory and the VCCT was the introduction of initial fictitious cracks which made the delamination behaviors of the stamp/film interface change with the preset crack length. The model based on the CZM could not only predict results that were close to the model based on the VCCT in the presence of fictitious cracks, but also predict the initiation and propagation of interface delamination without presetting initial cracks. Furthermore, the simulation results of the model based on the CZM are closer to the previous experimental data, exhibiting its suitability in analyzing the adhesion/delamination behavior of the stamp/film interface.
Simulation results of the model based on the CZM without presetting initial cracks indicated that the stamp/film interface adhesion strength characterized by the pull-off force was independent of the pulling speed under the elastic assumption of the stamp, while it increased with the pulling speed when accounting for the viscoelastic properties of the stamp. Furthermore, the pull-off force of the viscoelastic stamp/film interface tended to increase with increases in the normal strength and the normal fracture energy, which was beneficial to the success of the picking-up process in microtransfer printing.