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Nat.Lab.

Unclassified Report 831/99


Date of issue: 01/00

Design of a model system for the determination of adhesion energy at a polymer/metal interface.

Ivan Goudet Supervisor: A.Mavinkurve

Philips Electronics 2000

831/99

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Written by: Supervisor:

Ivan Goudet, WB 3 1. Dr A Mavinkurve, WB 3 11 amar.mavinkurve@philips.com

Philips Electronics N.V. 2000 All rights are reserved. Reproduction in whole or in part is prohibited without the written consent of the copyright owner
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Title: Author(s): Part of project:

Design of a model system for the determination of adhesion energy between a polymer and metal.
Ivan Goudet Polymer-Metal Integration

Customer:

Dr A. Mavinkurve

Keywords:

Adhesion ; interface ; crack ; energy release rate; step lap joint ; Jintegral ; opening mode ; node release. Adhesion between polymers and metal is commonly encountered in various processes (the most typical examples being in injection moulding). The work has consisted of investigating the potential of existing commercial software in modelling delamination in terms of adhesion energy, and designing a model experimental system which would complement the numerical work. A step lap joint was used where a layer of polycarbonate was sandwiched between two polished aluminium or brass bars. Bonding was induced by heating the sample to a temperature in the region of the glass transition of polycarbonate.

Abstract:

Conclusions:

- Heating of polycarbonate to around the glass transition temperature, is the most effective way to induce variable adhesion at the interface without unpredictable changes in the bulk. - The sample dimension has to be optimised to get a stable crack propagation, - No commercial software can directly answer our specific questions, but the node release methode needs to be investigated further.

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Contents
1 Introduction. 2 Theory. 2.1 Factors influencing adhesion between polymer and its substrate. 2.1.1 Mechanical. 2.1.2 Thermodynamic and chemical. 2.1.3 Kinetic. 2.2 An approach encompassing the different factors. 2.3 Basics of linear elastic fracture mechanics. 2.3.1 The energy release rate. 2.3.2 The stress intensity factor. 2.3.3 Opening modes. 2.3.4 Relationship between K and G. 2.3.5 J-integral. 2.4 Why examine G? 2.5 Few words about the software. 2.5.1 MARC. 2.5.2 ZENCRACK. 2.5.3 Software flow chart 3 Experimental. 3.1 Materials. 3.2 Sample preparation. 3.2.1 Problems with drying. 3.2.2 Conclusion. 4 Modelling. 4.1 Model definition. 4.2 Iterative procedure. 4.2.1 First iteration: Arbitrary choice of the dimensions. 4.2.2 Second iteration : Mesh density. 4.2.3 Third iteration : Boundary condition. 4.2.4 Fourth iteration : Size choice. 4.2.5 Fifth iteration: Mesh density. 4.3 Conclusions. 5 The node release method. 5.1 Background theory. 5.2 Numerical technique.

7 9 9 10 10 11 11 13 13 14 15 15 16 16 17 17 18 19 21 21 22 22 23 25 25 26 26 26 28 30 31 34 35 35 36
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5.3

TheBorgmeier and DeVries Method. 5.3.1 Compliance consideration. 5.3.2 Crack closure integral.

37 37 37 39 39 39 39 40 40 40 43 44 44 45 46 48 50 52 52 52 53 54 55 55 55 56 58

6 Conclusions and recommendations for future work. 6.1 Conclusions. 6.1.1 Experiments. 6.1.2 Software. 6.2 Recommendations 6.2.1 Experiment 6.2.2 Node release method. References. Appendix Appendix A: Project proposal. Appendix B: Cleaning procedure. Appendix C: Solvent results. Appendix D: Birefringence. Appendix E: G numerical results. Appendix F: Philips. I. Philips company. II. Philips Research. II-a. A little history. II-b. The Nat.Lab. Appendix G: Material Mechanics and Heat Transfer group. I. Description. II. General Trends. III. Group sub-activities. Acknowledgements.

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List of Symbols
a A b c E F G
g

H J k K K l N p r S r S T u U V W Wa Wd Wp Wt

Crack length Crack surface Crack width Compliance Youngs modulus External force Energy release rate Free energy Enthalpy J-integral Rigidity Stress intensity factor Stiffness matrix Crack movement Nodal force Distributed load Distance from the crack tip Entropy Stress vector Temperature Displacement Potential energy Sample volume Energy density Thermodynamic work of adhesion Energy stored in elastic strain within the sample Plastic work dissipated at the crack tip Work of the external forces Thermal expansion coefficient Strain Surface energy Friction coefficient Poisons ratio Orientation with the crack plane Stress

[m] [m2] [m] [m2/N] [N/m2] [N] [J/m2] [J] [J] [J/m] [N/m2] [N/m3/2] [N/m2] [m] [N] [N/m2] [m] [J/K-1] [N/m2] [K] [m] [J] [m3] [J/m3] [J] [J] [J] [J] [K-1] [-] [J/m2] [-] [-] [rad] [N/m2]

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1 Introduction.
Interaction between polymers and metals is commonly encountered in various industrial processes (the most typical examples being in injection moulding). The work presented here is encompassed in a larger project aiming to gain a better understanding of adhesion concepts between polymer and its substrate. (More details are given in appendix A) This part, still at the very first stages, aims to design a model system to perform experiments and numerical modeling of adhesion fracture (in fracture energy terms). The work consisted mainly of examining the mechanical aspects of the adhesion between polycarbonate and its substrate, first building a numerical model and then optimizing the experimental samples to complement the numerical work. Indeed, the way we choose is iterative. Results presented in this work aim to improve the quality of the experimental samples, themselves further used to valid numerical predictions. Each aspect will counterbalance the other: the present numerical work allows suitable sample choice, these pieces will be used as a model system for the development of a more accurate numerical model for determination of adhesion energy The first step of the project consisted of designing an experimental system to get relevant results that could be linked to the theoretic work. Commercial software already possesses powerful tools to describe crack propagation within homogeneous materials. We investigated if it was possible to use these tools for interfacial delamination. The theory being largely improved within these numerical packages, the problem has been to focus on, how to model an interface between a polymer and its substrate? The first chapter specifies the theoretical aspects necessary to understand the adhesion itself and goes into ways to model it. It summarizes the necessary tools required and assumptions made for the work that. The second chapter gives a brief description of experiments in which we attempted to find the best conditions to get suitable adhesion (i.e. a system conducive to mechanical and numerical modeling). The very first approaches were not effective, the results are therefore limited, but we were able to propose conditions required to carry out future experiments. The next chapter details the building of the model, and specifies the hypotheses used. (in the work done or within the software) for this first building. The result is the best compromise between the theory and the numeric tools. In chapter five, the node release method is explained; its possible applications with the corresponding limitations are specified. Finally, we summarize the results and give recommendations for future work.

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2 Theory.
Various definitions for adhesion have been proposed in literature, but none is completely or/and generally accepted. That, which seems to be more convenient in our case, is proposed by Wu in Polymer interfaces and adhesion: Adhesion refers to the state in which two dissimilar bodies are held together by intimate interfacial contact such that mechanical forces can be transferred across the interface. The interfacial forces holding the two phases together may arise from Van Der Waals forces, chemical bonding electrostatic attraction or mechanical links (physically due to asperity, for example). The adhesion between a polymer and its substrate will be controlled by mechanical chemical and thermodynamic factors. These three aspects are closely linked. It is thus hard to examine each of them separately, but looking for a macroscopic parameter including this set of factors would allow a global approach of the model. The free energy required to separate reversibly two phases from their equilibrium position to infinity at constant temperature and pressure is the thermodynamic work of adhesion Wa, typically of the order of 0.1 to 1 J/m2 for polymers (according to Ref [1] &[4]). But the real adhesive strength in polymers mechanically measured is usually more than an order of magnitude higher. Indeed, a part of the energy is dissipated at the crack tip in plastic deformations occurring during the propagation and other storing and dissipative mechanisms within the material. This work is thus linked to the propagation rate.

2.1 Factors influencing adhesion between polymer and its substrate.


Examining the various factors should give us a good understanding of the adhesion. In a very global view, many of them act on the adhesion between the polymers and their substrate depends on: - Mechanical Macroscopic factors: Inherent stress, or stress introduced by external influences. Microscopic factors: Nature of the contact, surface roughness. - Thermodynamics/chemical Nanoscale phenomena: Polymer adsorption dynamics, chain relaxation, crystallization, surface chemistry. Other phenomena like competitive adsorption of additive, cleanliness. - Kinetic

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2.1.1 Mechanical. Adhesion between polymers and metals is influenced by the surface roughness. The asperity and surface irregularities can intervene as mechanic links between the polymer and the substrates. The bulk polymer can enter the surface irregularities and build a purely mechanical link. Further more, under those conditions the crack propagates on a nonflat surface, which costs more energy because of direction changes. 2.1.2 Thermodynamic and chemical. The main mechanism of adhesion between a smooth substrate and polymer is adsorption. It involves loss of conformational entropy in the polymers; S is linked to the chain length. The available energy used to create the links between the two substrates (H) compensate the entropy loss. This phenomena is controlled by free energy equation: g=H-TS Where: g is the free energy, H the enthalpy, S the entropy, and T the temperature. (1)

Adsorption energy is supplied by secondary interaction between dipoles in the polymer and active sites (AS) on the metallic surface, i.e. oxide or hydroxide (see next figure). The surface has thus to be perfectly clean. (Cleaning procedure detailed in appendix B) Thermal energy allows molecular motion, which cause the polymers to come against the metallic surface to interact with these AS (both oxide and hydroxide) in order to reach equilibrium.

Fig 1: Metallic surface (Purely schematic diagram, no scale has been respected).

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The surface energies of the 2 materials polycarbonate and metal, with the interfacial tension polycarb/metal, are the most influential terms. In a very general sense, the fracture energy i is: i = (polycarbonate + metal + polycarb/metal)+ p + a (2) Where is a factor function of the crack plan orientation, p is the energy stored per surface unit in plastic deformations, a is a term encompassing the other dissipative forms. In our case, these surface energies play an important role (we can here consider that 1 and. p 0) 2.1.3 Kinetic. Another important aspect is the dynamics of the process. Indeed, thermodynamic interactions necessitate time. This could require, for entangled polymers, time scales of the order of the reptation time. The reptation model proposed by De Gennes (Ref [7]), consist of imagining a fixed tube around the polymer (at least the main chain); the reptation time is the time necessary for the molecule to go out of this tube. For interaction between chains and surface, such motions are required. Besides, the penetration of the polymer into the mechanical roughness of the substrate will also take time depending on the viscosity (itself time and temperature dependant), applied pressureetc.

2.2 An approach encompassing the different factors.


Finally, in our conditions, the adhesion is due to a mixture of the previous factors, but they cannot be clearly separated. We have to deal with a mixture of them. The approach being in terms of mechanical work, the experiments will be done with a tensile machine. But the force or the displacement applied during a shear test, is shared within the sample.
Material 1 (E1, 1) Crack Interface Material 2 (E2, 2) Fig 2: Schematic aspect of an interface crack. (More details about our model given furtherly)

Under the load, the two materials tend to deform (each in its own proportions), the energy potentially stored in elastic strain is Wd.

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Some area can deform plastically, even with very small deformations, as soon as a crack appears, its tip is surrounded by a plastic zone.

The work dissipated is Wp.

Fig 3: Plastic zone at the crack tip.

Those quantities are linked by the following equation: Wt = Wd + Wp + Wa (3) Where:Wt is the work done by the tensile machine. 1 1 Wd = ku 2 kiui 2 2 sample k being the rigidity of the material and u the displacement.

Wp =
ij

1 ij ij dV 2V

V being the plastified volume near the crack tip.


Force

Work Displacement Fig 4: Graphic representation of work.

Hypothesis: The adhesion is very weak and then the stress very low (pre-experiments shown the stress before breaking was around 1.01MPa), the plastic deformations are thus assumed negligible Wp = 0 Finally, Wa = Wt - Wd (4) Through the work done by the tensile machine and the potential energy stored in elastic strain, it is possible to get a work encompassing the factors detailed in part 2-1.

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Griffith showed that for an infinitesimal growth of a crack, the decrease of potential energy under a given load, is at least equal to the decrease of the stored elastic energy at a given displacement:

d (WT Wd ) dW a r da Fext =cst da u =cst


dU d or r da Fext = cst da u =cst

(5)

(6)

dWa d But da or da is the work done per increment of propagation of the crack. Irwin defined this value as the energy release rate G. This approach being in terms of energy, we can thus encompass all the aspects discussed in the former part.

2.3 Basics of linear elastic fracture mechanics.

2.3.1 The energy release rate. The energy release rate is defined as follows:
G= dWt dU dA dA

(7)

where dWt is the work done by the external forces during the increase of the crack by an infinitesimal surface area dA, and dU is the increment of the energy stored simultaneously in the body. Their difference corresponds to the energy required to open new surfaces for the crack. Thus defined, G is the available energy to make the crack propagate. This is the crack propagation strength in J/m2. To link G to the experimental data, it can be expressed for example, like: G= 1 F 2 dc 2 b dA

(8)

Where F is the force acting on the body, c is the compliance, b the crack width and A the crack surface. According to the first expression G is the change of potential energy of the body corresponding to an infinitesimal increment of the crack size. G is a function of the elastic constants of the material and the shape of the sample for a given shape, G is proportional to the square of the stress intensity factor K.

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2.3.2 The stress intensity factor.

The tip of a crack in a loaded body is a place with high stress concentration. This concentration can be characterized by means of a stress intensity factor K. Generally this factor is calculated as: K = Y a (9)

Where: - is the nominal stress at the point investigated, -a is the length or other characteristic dimensions of the crack. -Y a geometric factor which depends on the shape and size of both the crack and the body, and on the character of load. The knowledge of the stress intensity factor allows us to predict the stress field around the crack tip: K ij = f ij ( ) r Where r and are defined as follow: (10)

Fig 5: Definition of the coordinate axis ahead a crack tip. (Taken from ref [3].)

Note that the infinite values coming from the above expression for r 0, are not physically reached because of the none zero value of the crack tip radius, and plastic deformations or crazing (for polymers) surrounding the tip and allowing stress relaxation (see Fig 3).

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2.3.3 Opening modes. The propagation of a crack is a complex phenomenon, the propagation of the crack takes place via one of or a mixture of the three the following different modes. These modes are referred with the subscripts I II or III.

Fig 6: The three loading modes (Taken from ref [3].)

2.3.4 Relationship between K and G. Two parameters describing the behavior of cracks have been mentioned so far. The stress intensity factor, according to its definition, is determined by external data (cf. Y definition). It characterizes the stresses strains and displacement near the crack tip. These are local parameters. The energy release rate quantifies the energy changes accompanying an increment of crack extension. This is a global parameter. (Ref [3]) It has been shown that for linear elastic materials K and G are uniquely related:
G I / II = (1 2 ) G III K I2/ II E

K2 = (1 + ) III E

(11)

Where is the Poison ratio and E the Young modulus. Willing to avoid at maximum the plastic deformations, these relations will be acceptable in the present work. As G is a scalar, for a more complex rupture, it is possible to use the additive property:

G = G I + G II + G III =

1 2 E

2 K2 2 K I + K II + III 1

(12)

G turns out to be a global parameter allowing a characterization under mixed modes of failure.

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2.3.5 J-integral. An other important factor is the J-integral, define by Rice as: r r u J = W dy S dl x

(13)

where is a curve leading from one crack surface around its tip to the other surface (fig r r 8), W is the energy density, S the vector of stress acting on the border , and u the vector of the corresponding displacement (ref [2]).

Fig 7: Definition of J-integral.

Generally the J-integral express the changes in potential energy of two body (loaded in the same way), one with a crack of length a, the other with a crack a+da. If the plastic deformations are restricted to the vicinity of the crack tip, the J-integral is identical to G However the J- integral unambiguously describes the state of the body with a crack even if larger plastic deformations have occurred. Another advantage of the J-integral is that it does not depend on the integration path as long as it is closed. The curve is thus chosen so that the calculations are as simple as possible (see 3.5.1)

2.4 Why examine G?


We will see in section 3 that the experimental samples have the shape specified in the next figure:
Polycarbonate Metal piece

Fig 8: Sample shape.

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In our case the energy release rate and J-integral are similar as the plastic deformations are concentrated to the vicinity of the crack. The stress intensity factor can be calculated analytically for simple modes, or can be approached experimentally with the property of birefringence of the polycarbonate. But the analytical determination is very complicated under mixed modes. And in our case, mode I and II are present. The next figures present a simulation of the model shown in the precedent figure:

Fig 9 a: Stress component 11 within the model.

Fig 9 b: Stress component 22 within the model.

Numerical modeling is thus imperative. G is the parameter that we want to obtain from numerical and experimental results to find a way to get criteria for its determination during crack propagation. The examination of the factors has been done in chapter 4.

2.5 Few words about the software.


The package used to make calculations is MARC combined with ZENCRACK. 2.5.1 MARC. In a finite element formulation based on the displacement method, the energy release rate within MARC is calculated as follows:
G= 1 T K u u 2 l

(14)

where u is the nodal displacement vector and K is the change in the stiffness matrix due to propagation of the crack, l is the amount of crack movement. A small propagation of the crack only has influence on a limited number of elements in the vicinity of the crack tip (path independent property). The stiffness change is thus calculated in a small number of elements.

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For an elastic-plastic material, the J-integral is uniquely defined outside the plastic region. The evaluation of the J-integral in MARC is based on node movement and numerical differentiation to obtain the change in the potential energy as a function of nodal positions. It is assumed that node movement does not change the load, so that the only concern is the change in strain energy. Parks (ref [9]) has originally developed this method This is the main MARC package hypothesis we have used in the calculations. Note that the stress intensity factor is not used at all hence.

2.5.2 ZENCRACK. ZENCRACK is used to generate the 3D finite element meshes containing the crack front from an uncracked model, and to calculate the distribution of the energy release rate along the crack front The elements forming the crack front are gathered in different types of Crack Blocks (CB), chosen in function of the crack type to be modeled; these Crack Blocks are constituted of sets of 20 nodded brick elements. A fundamental option for our case allows the control of the midside node position to use a quarter point nodes method to keep the stress singularity (stress peak at the crack tip) in a limited area. The plastic deformations can thus be located in a very limited volume, and be neglected. We needed a CB allowing propagation in a given plane, and with sufficient elements in the thickness to keep only one layer of element in the 3D uncracked model (for simplicity). The chosen type is shown in figure 10:

Fig 10: Crack-block - front and back view. (Ref [11])

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Their insertion in the model occurs as followed:

Fig 11: crack block insertion.

The crack blocks presented in figure 10 is used to model a half crack, the above figure show how two crack blocks are used to model a whole crack. In the model we used, we restricted the crack growth to the interface plan. So, the energy release rate distribution within the crack plane has been used to evaluate the crack growth rather than the local maximum stress intensity factor. 2.5.3 Software flow chart

ZENCRACK user input: crack specifications

MARC user input An existing finite element mesh of an uncracked component (.dat file encompassing boundary conditions)

ZENCRACK Insert the crack within the component by generating the crack finite element mesh.

MARC Finite element analysis (strain, stress, energy release rate)

No

ZENCRACK Analysis of initial crack only?

Yes

ZENCRACK Evaluate crack growth, update crack fronts, geometry and f.e. model.

ZENCRACK stop Output file (report) Output files (.t16 or .t19)


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3 Experimental.
The first part of the experimental work was to see how it was possible to prepare some relevant physical samples to test and model adhesion. we had to determine their shape, their size, and the materials. The global project aims to model adhesion between polymers and metals including the influence of differential thermal contraction. Hence it was appropriate to use shear tests, more precisely step lap joint tests. Indeed, this shape facilitates grasping by tensile test machine cramps, and the way to assemble the different sample pieces is very simple.

Fixed edge

Adhesive Applied displacement or force

Fig 12: Step lap joint.

Indeed, the stress induced in a single lap joint in tension seems to be close to that encountered by the solidified polymer in contact with the colder mould during the injection stage: in the joint, the differential straining of the adherent in the overlap region produces shear stresses, whereas eccentric bending produces tearing (peel test) [1]

Fig 13a: Differential straining. Fig 13b: Bending and tearing in single lap joint.

3.1 Materials.
Polycarbonate is both polar (chemically speaking) and also shows birefringence. It is thus possible to get reasonable adhesion on metal (cf. part 2.1.1) and use birefringence to confirm calculated stress distributions. Grade K486 (construction grade) has been chosen as the adhesive between the metal bases.

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As it is necessary to avoid the primary chemical interactions, metals carrying stable oxide layers such as aluminum and brass have been chosen for the base (the only interaction remaining being thus ones within the timescale of the experiment). Polished surfaces have been used to avoid other influences of a surface roughness.

3.2 Sample preparation.


The aim was to realize adhesion between a polymer and its substrate under simple experimental conditions. Our first attempt involved the use of a volatile solvent working at room temperature to induce local chain mobility without affecting the bulk. The adhesion process at higher temperature is of course perfectly known, but it turned out that the decrease of temperature coming out of the oven, generates such a high induced local stress, that the crack propagated because of the thermal expansion coefficient difference. We will see in paragraph 4.2.3 that stresses generated are of the order of 10MPa. Anyway, we desired to obtain homogeneous adhesion on the whole surface, without neither residual solvent nor water; to be sure the experimental conditions only depend on the materials.

3.2.1 Problems with drying. The first experiments made, showed that the solvent had to be completely removed, to avoid that the polymer was softer near the interface, witch would prevent the crack from propagating into the polymer rather than along the interface.

We first attempted a very volatile solvent to remove it quickly enough to avoid crystallization (a known problem in polycarbonate). 1,2dichloropropane and 1,1,2trichloropropane evaporated at a too slow rate, and crystallized state was reach very quickly. The properties of the crystallized polymer are different of those of the amorphous state. 1,2dichloroethane & dichlororomethane are more volatile but needed a longer time for drying at room temperature.

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To accelerate the process, we chose to heat the samples up to 40C. This revealed the presence of bubbles in the polycarbonate. Two things about the origin of the bubbles. Polycarbonate absorbs water easily. Tests made with undried pieces of PC and pieces dried for 4 hours at 120 C showed that fewer bubbles appeared in dry PC. Diffusion rate of the solvent is low in the material, and at higher temperature conversion to gas is even faster than diffusion. In the presence of solvent, PC is soft enough to allow nucleation and formation of gas bubbles which stay captive within the material and become bigger and bigger. We thus conclude that a longer drying time is necessary with 1,2dichloroethane & dichlororomethane at room temperature (see appendix C to have detailed result) In fact to get better results it was necessary to wait at least 4 days at room temperature and to put the samples for 2 days at 40 C. Even with these last solvents, it was difficult to avoid crystallization. The shortage of time did not allows us to resolve those last points and attention shifted to the approach of using temperature-induced bounding.

3.2.2 Conclusion. The main result of this study is that solvent has to be removed extremely quickly to avoid crystallization. But the phenomenon is controlled by diffusion that is too slow to dry the samples before crystals appear. The increase of temperature is more effective for the molecular motions than on the diffusion rate, so that crystallization is reached before the solvent has been removed. Because of the shortage of time, no more tests have been made, but the pre-tests showed that: 7 days of drying (5 at free atmosphere and 2 in a 40 degrees oven) are necessary. Pieces have to be perfectly clean, to get correct samples. The best approach would be to prepare the samples by inducing bounding in an oven at a temperature around Tg (say 140C) and cooling it by few degrees before testing (135C). At 135C and within the timescale of the experiment, the modulus is still high enough to avoid deformation due to the small forces applied to bring the bodies together, or surface tension. This requires a climatic chamber which can be mounted around the tensile testing machine. This could not be carried out because the oven was not installed.

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Preliminary experiments have shown that significant adhesion was obtained at about 140C within a time scale of the order of magnitude of the relaxation time. This in itself is an interesting subject (adhesion of PC around the Tg).

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4 Modelling.
The modeling will mainly deal with the numerical tools that we have used. We have to elaborate a suitable model, which answer our needs. As the strain energy density, the quantity we want to look at, depends on many parameters, it is important to choose suitable conditions for the experiments and the modeling. A parametric model has thus been built to examine the influence of geometry on the numerical results. The realized model keeps the chosen shape of the experimental pieces, but each dimension can be changed. Likewise the density of the mesh can be modified.

4.1 Model definition.


The chosen shape was the step lap joint:

Figure 14a: Shape of the metal pieces.

Figure 14b: Assembled model.

It allows to get the lap joint configuration (as discussed in part 2) and to be grasped by the clamps. The model has been built with 20 noded brick elements The boundary conditions have been modeled as follow.

Null displacement

Fixed displacement

Fig 15: Boundary conditions.

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This configuration is similar to that used by Borgmeier and DeVries in their analysis of the effects of tapering adherents on the strength of adhesive lap joints. (Ref [4])

Fig 16.

Many parameters have to be taken into account, and each of them is susceptible to influencing the others. The choice of the dimensions and of the mesh type will be taken out of an iterative process (fixing some parameters, then allowing the others to vary, then optimizing the first, then correcting the seconds.).

4.2 Iterative procedure.


4.2.1 First iteration: Arbitrary choice of the dimensions. In order to observe the stress evolution with birefringence, it was decided not to make the samples thicker than 2mm (size already used in former experiments done at the lab). Correct proportions for the sample length and height should be between 2 and 10, and 1 and 5 millimeters, respectively.
Length Height

Fig 17: Dimensional parameters.

We first chose to use a 5 per 2mm model. 4.2.2 Second iteration : Mesh density. The correct density is a compromise between the number of elements (which has to be high enough to get accurate results), and an acceptable CPU time (which is lower when there is few elements).

Fig 18: Different mesh densities.

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The examination of Von Misses stress for different mesh densities showed that in the chosen scale a factor of 2 in the mesh density does not influence results significantly. In the tested solution, we have enough elements to already converge close to physical values. The chart shown below gives the values of Von Misses Stress for different mesh densities. It is given as a xy number of elements (corresponding to length per height) for the polycarbonate piece.

Von Mises stress

Von Mises stress

8.10E+06 8.10E+06

6.10E+06 4.10E+06 2.10E+06

6.10E+06 4.10E+06 2.10E+06 1.00E+05

1.00E+05

5x2

10x4

15x6

20x8

25x10

5x2

10x4 Point A A Point

15x6
Mesh density Mesh density

20x8 Point C Point

25x10

Point B Point B

Point A, B and C a specified on the next picture

The growth of the stress at point B is caused by the corner which generate a stress peak and an increasing gradient (singularity) with the decrease of the mesh density. Nevertheless, this problem will be solved with the presence of the crack in the mesh, which will restrict the singularity to within a small range of elements.

B A

Fig 19: Stress distribution within a mono-material sample presenting the same shape.

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A 10 per 4 element mesh has been kept for the polycarbonate area for the following reasons: The density is thin enough to avoid a very high stress gradient within one element, The aspect ratio (relation between height, width and length of the element) is still good enough to converge (smaller elements would require several layer in thickness, and heavier calculations), The element size is large enough to allow an easy replacement by the crack blocks generated in Zencrack (which contain lots of elements). 4.2.3 Third iteration : Boundary condition. The boundary conditions have to be chosen to stay as close as possible to the experimental data. We want to simulate a stress we will encounter in the futures experiments. The experiments realized to test the adhesion process by heating allowed us to get a rough idea of this stress. We looked at conditions under which the samples broke when we put them out of the oven: the interface bounds were broken with a decrease of 50C, it meant a stress of, 9 6 6 approximately test = E T = 2.5 10 65.10 50 8.1 10 Pa. This value is similar to this of the polycarbonate in numerical simulation which results are presented below. Note that in this scale of temperature (20 to 140C), no significant changes in the elastic constants have been measured in the DMTA (Dynamic Mechanical Thermal Analysis) within the timescale of the experiment.

Polycarbonate piece

Fig 20: Numerical simulation of the induced stress due to a decrease of 50C in a piece of polycarbonate between two aluminum pieces under the assumption of perfect adhesion.

The expected values must thus be of the order of magnitude of 10 MPa.


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Not to be influence by the numerical interaction of the two materials, the choice of the displacement value is determined with a mono-material model having the save shape. We used aluminum, because its higher Young Modulus induced higher stresses (corresponding to the conditions in which the propagation would be the faster). Different simulations have been made, the results are given below.

Fig 21a: Displacements within a mono-material model

Fig 21b : Von Misses stress within a mono-material model.

A maximum value of 10Mpa was reached for displacements of 2m. It is now important to see the influence of the imposed displacement on the numerical results. The same model has been subjected to different displacements, and the energy release rate value has been plotted in function of these ranges.

The values delivered by calculations are thus perfectly linear with the displacement imposed in the boundary conditions. A change of range will not require a recomputation.

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4.2.4 Fourth iteration : Size choice. The geometric parameters looked at are the length and the height (cf. 4.2.1). Different models with different lengths and heights of the P.C. portion have been generated and used to calculate the energy release rate for the considered parameters.

Fig 22: Starting crack at the interface.

The energy release rate has been examined for the middle node (in thickness) not to be influenced by the borders. Results show a regular surface, quite flat with an almost horizontal part. Furthermore, the numerical results are in reasonable agreement with the literature. We saw that energy release rate is of the order of 0.1 to 1 J/m2 for weak interfaces (Ref [6]).Our results give values from 0.05 to 0.79 J/m2. (Details in appendix E)

G (J/m2)

Length (mm) Height (mm)

Fig 23: Energy release rate as a function of the geometric data for a starting crack.

The physical meaning of the flat horizontal part is that the samples of these dimensions will have a stable rate of crack propagation. Suitable samples are thus in the region where the length is grater than 4mm, and the height is greater than 2mm.

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4.2.5 Fifth iteration: Mesh density. Now that the dimensions are restricted to a smaller area, it is possible to make a more accurate choice of the density. The problem is that the mesh, chosen on purely stress criteria should have no influence on the absolute values of the results. Twice coarser and twice denser meshes have thus been examined.

G (J/m2) G (J/m2)

Length(mm) High (mm)

Length (mm) High (mm)

Fig 24: G for a twice-denser mesh.

Fig 25: G for a twice-coarser mesh.

The global aspect is, of course, unchanged (except the problems of too coarse mesh for the smaller models: not enough elements are present in a given surface, these results have not been put in the chart in Fig 25), although each value is not perfectly identical. The next two figures details the difference percentages of the energy release rate between our originally chosen density and (1) a twice denser mesh, (2) a twice coarser mesh.

Length (mm) Height (mm)


Fig 26: Percentage of difference between the values for the initial mesh and a twice-denser mesh.

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Length(mm) Height (mm)

Fig 27: Percentage of difference between the values for the initial mesh and a twice coarser mesh.

First observations: The models with a very larger height/length ratio do not allow very stable results for different densities. It can come from a too large predominance of the shear components within the material. We are not anyway, interested in such configurations. The flat area on the former surface presents the smallest differences from one density to the other. Conclusions. Finally, the 6 per 3 mm model seems to be the best: It is in a flat area of the surface, this avoids that the possible variations of the experimental samples dimensions bring us in a less stable area. The sensitivity of the values of G to the mesh density need to be looked at in more details. Nevertheless, it appears that perfect absolute values can not be determined from the numerical calculations. Here we can talk about the very specific problem encountered in our proceeding. Indeed, the thinner the mesh, the better the results, but above a certain density, the elements are too small to allow the crack block insertion: too many elements are put in too small a volume (Fig 28 & 29).

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Fig 28: Mesh aspect of the model.

Fig 29: Von Mises stress within the model.

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4.3 Conclusions.
The optimized geometry is: a 63 mm polycarbonate piece, a 104 element area, a 2m fixed displacement. Such a configuration allows: a correct shape for observation and manipulation, an interface that is not too large (allowing to avoid macroscopic adhesion non-uniformity), a good stability of propagation,

Zencrack systematically delivers the G and K values for the crack tip nodes. In our model 5 nodes are used in the depth to build the tip, the corresponding numerical results are summarized in the next table: Nodes 1 2 3 4 5 6 Mean Min Max G (J/m2) 0.13E+00 0.16E+00 0.17E+00 0.17E+00 0.16E+00 0.12E+00 0.15E+00 0.13E+00 0.17E+00 K (plane stress assumption) 0.803E+05 0.91E+05 0.93E+05 0.93E+05 0.91E+05 0.80E+05 0.88E+05 0.80E+05 0.93E+05 K (plane strain assumption) 0.87E+05 0.99E+05 0.10E+06 0.10E+06 0.99E+05 0.87E+05 0.96E+05 0.87E+05 0.10E+06

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5 The node release method.


This is another method, which is available in most of the finite element software. It consists of the possibility to separate the coinciding nodes of two bodies previously in contact. In other words, nodes of different pieces, located at the same geometric position during contact will be spatially separated under the action of the resulting normal force coming from the applied conditions.

5.1 Background theory.


Here again, the analysis is limited to linear elastic fracture mechanics. Note that in real materials, some significant plastic deformation can appear near the crack tip, but the energy lost in these dissipations will be encompassed into the term representing the required energy to create a new surface. For a crack being expanded from a length a to a+da, the necessary differential energy is, under constant forces:
Force

Displacement Fig 30: Graphic representation of the strain energy.

dU = 1 / 2 Fa (u a + da u a ) Where:dU is the change in energy, F the applied force, u the bodys displacement. The energy release rate being define as the change in strain energy per unit area :
G= 1 / 2 Fa (u a + da u a ) dA

(15)

(16)

Where:dA is the new crack surface. The expression for a discrete system can be expressed by :
G= Wt U A A

(17)

Where Wt is the change in work input by displacement of applied loads, U the change in the energy stored in the body.

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5.2 Numerical technique.


Marc package delivers the strain energy density. It should thus be possible to get the energy release rate during the propagation. If under given condition, i nodes are released along the interface (work with a 2D mode under plane strain condition is now enough), and if it is possible to find the new criterion under which one more node is released (i.e. i+1 nodes separated), the two values of the strain energy density of these two consecutive steps allow us to calculate the energy release rate:
G= U i +1 U i Vsample da

(18)

Where Ui is the strain energy density in the configuration of i nodes released, da is the length of propagation (here, distance between two nodes) V the sample volume in which the energy is stored. But an important problem comes from the configuration of our model. All the contact and friction options within Marc are based on the value of the normal force acting on the nodal point. If the solution has converged, a check is performed on the normal force acting on the nodal points being in contact. (Ref [10]) Fn Fseparation: solution OK Fn Fn < Fseparation: contacting node A will separate
A

The point is that our interface undergo mainly shear forces, the single normal components arise from the potential bending moment. The numerical technique is thus far from physical reality. It was then assumed this method was not good enough for our purpose. Of course the normal and shear components can be linked, via Coulomb laws or shear friction (Ftangential=Fnormal; distributed load are proportional to the equivalent shear stress: pt=VonMisses/ 3 ) But the friction coefficient is perfectly unknown for our condition and is in fact more or less what we are looking for.

Fig 31: Aspect of the strain energy density in the pre-simulations using the nodes release method.

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5.3 TheBorgmeier and DeVries Method.


P R Borgmeier and K L DeVries programmed their own method. Their work being detailed in ref [4] we will only recall the process here.

5.3.1 Compliance consideration. The energy release rate is calculated under assumption of constant force crack extension. Displacement for a model with a crack of given length a are calculated for a given load Fa ; similar computations are done for a model with a crack length of a+da. Then the energy release rate has been estimated with the equation (15) :
G= 1 / 2 Fa (u a + da u a ) A

(15)

5.3.2 Crack closure integral. Calculations are again under the assumption of constant applied forces. The first run is used to calculate the displacement (or location) of the finite elements nodes at the crack tip for a crack length a. A node is then released, extending the crack to a length a+da, the new nodes displacements are calculated under the same load as previously. A vertical unit force is then applied to the released nodes in the direction needed to bring them back to their initial position. The resulting displacements are the unit force displacements at the crack tip for the length a+da. The fourth step is similar to the preceding one : unit horizontal forces are applied to the released nodes to get their horizontal displacement. Since a linear elastic material was assumed, the total force required to move each node back to its original position can be calculated by scaling of the unit forces by correct factors. Forces and displacement are then used to calculate the necessary energy to close the crack. This force is furthermore divided into its horizontal and vertical components, it is thus possible to get the partition of the energy related to the different modes of crack growth. Energy being a scalar, the results can be added to find the total energy release rate : G=GI+GII

(19)

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Fig 32: Different steps of the crack closure integral.

Those two methods give of course good and coherent results, but need heavier programming that shortage of time did not allow us to do. Nevertheless, in the next chapter, hypothesis for future work is presented.

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6 Conclusions and recommendations for future work.


6.1 Conclusions.
6.1.1 Experiments. The use of solvents is not feasible for such experiments. The use of high temperatures would be the best solution to get a suitable interface. Reasonable adhesion is obtained around Tg (to allow molecular motions). Mechanical testing has to be done in glassy states, it is necessary to cool the samples down. The thermal residual stress must be taken into account during the experiments and modeling. Quality of the surfaces is extremely important. It means that: They have to be perfectly flat, To avoid changes of direction during crack propagation (which consume energy ), To be sure that the whole surface is in contact. They have to be perfectly clean. They must neither be covered with grease nor contain water (It is advisable to dry the samples before using them). One should be careful about the preparation of the polymer pieces. If other materials (like organic solvents) are used to clean or polish them, the polymer properties can be modified. 6.1.2 Software. No commercial software is able to answer our specific problem completely. One way would be to write ones own program (writing ones own program or use subroutines or internal procedures to modify existing software) Nevertheless, under simple modes, it should be possible to get relevant results with the node release method. Contact options implemented within MARC is perfect for mode I, The use of a specific coefficient (Ftangential/Fnormal) should be examined in more details for mixed mode. Discussions will be undertaken with other groups working on ANSYS to see the feasibility of the contact options within that software, in particular the node release method for mixed mode delamination.

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6.2 Recommendations
6.2.1 Experiment

Adhesion between polycarbonate and metal induced around Tg.. Cool by T (to below Tg), avoiding delamination, OR induce delamination by slow cooling. Calculate stress distribution, confirm with birefringence.

Vary time at given temperature to modify adhesion energy (interesting from a fundamental point of view)

Possible control with birefringence

Simpler if all the pieces already clamped in the tensile machine during adhesion process.

Apply force or displacement in tensile machine.

Follow delamination if possible, or find critical force for fracture.

Find G from value of F or u, using the node release method

Comparison with others models.

6.2.2 Node release method. As it has been said, the best way to use the node release method would be to write ones own program, but such work should be done once the project has progressed further and more data is gathered about this specific crack type. An other interesting hypothesis would be to keep the node release method implemented in Marc, and use a coefficient NTangential/NNormal (Nodal force) to work in term of tangential forces although normal forces are taken into account by the software.
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Consider a simple experimental sample. The critical shear stress necessary to start a crack or to break the whole interface, would be generated by a force FTangential.
r FTangential(physical )

Interface
FTangential ( physical )
r

Sample

Fig 33: Shear test on a physical sample

Then the above situation should be modeled, and the necessary nodal force, Nnormal, to break the numerical model in the same way as the experimental one, should be found (by an iterative procedure).
r N Normal

Numerical model

r N Normal

Fig 34: Numerical simulation.

From the experimental results (force applied, sample size) it would also be possible to calculate the nodal tangential force which would appear at the corresponding numerical interface. This would be the tangential nodal force appearing at the fictitious nodes of the interface: NTangential.
NTangential ( fictitious )
r

= FTangential / Number _ of _ nodes

Fictitious nodes Fig 35: Fictitious considerations on physical sample.

Knowing NNormal and NTangential, the coefficient could be determined. To validate it, another simple geometry and its corresponding model could be used. Nevertheless, the coefficient would be based on purely experimental facts. It would thus be important not to use it purely for predictions, but to use it to complement each experiment.

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References.
[1] Souheng Wu, Polymers interface and adhesion, Marcel Dekker, INC (1982). Jaroslav Mencik, Mechanics of Components with Treated or Coated Surfaces, Kluwer academic publishers (1996). T.L.Anderson ,Fracture Mechanics, CRC Press (1995). P R Borger and K L DeVires, A fracture mechanics analysis of the effect of tapering adherents on the strength of adhesive lap joint, J Adhesion Sci. Technol. Vol. 7 No. 9,pp. 967-986 (1993). J.M.G.Cowie, Polymers, Chemistry & physics of modern materials, Blackie academic & professional (1993). Richard P. Wool, David M. Bailey and Anthony D. Friend, The nail solution: adhesion at interface, J Adhesion Sci. Technol. Vol. 10 No. 4,pp. 305-325 (1996). P.G.de Gennes, Scaling Concepts in Polymer Physics, Cornell University Press (1979). R.Wimberger-Friedl and J.G.De Bruin, The time-dependent stress-optical behavior of polycarbonate. Rheologica Acta. Vol. 30,pp.419-429 (1991). MARC users manual, volume A (1994).

[2]

[3] [4]

[5]

[6]

[7]

[8]

[9]

[10] MARC users manual, Enhanced contact, analysis using adaptive techniques (1995). [11] ZENCRACK user manual, appendix A page A-18 [12] Philips intranet website.

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Appendix
Appendix A: Project proposal.
Project proposal: Adhesion energy concepts between a polymer and its substrate. Relevance: Much analytical and numerical work has been done in order to understand and predict (qualitatively and quantitatively) the thermally- and flow-induced stress distribution in injection moulded polymers. It is usually assumed that the adhesion between mould and solidifying polymer is either perfect (the so-called no-slip condition), or entirely absent. Generally, non-zero pressures are taken as conditions that lead to the no-slip condition at the interface. In fact, the adhesion between mould and substrate always has some finite value, depending on the temperature and pressure history, the material combination and the presence of contaminants like additives at the interface. The quality of adhesion would have a significant influence on the properties of the finished product. Description: Adhesion is quantified with the help of a term called adhesion energy. This value for a given interface is defined as the energy required to separate the interface. It comes from fracture mechanics, where energy considerations, rather than stress considerations are used to calculate failure criteria. The quality of adhesion is important in determining the stability of the mould/polymer interface throughout the filling, packing and cooling stages. If the adhesion energy is low, the stresses built up during various stages could be released through slip or premature release of the substrate. This is especially critical when the surface texture takes place during the moulding. Slip or premature release could lead to damage of the surface. On the other hand, after completion of the cooling stage, the product should be capable of being ejected without difficulty, i.e., without damaging the transcribed information. This means that if the adhesion energy were too high, difficulties with release would introduce problems as well. In other words, a critical adhesion window is required to ensure a better moulding process. One must also give due considerations to factors like stresses, which are introduced, at the interface during the cooling cycle. This requires better quantification of adhesion phenomena in injection moulding. A better understanding of adhesion phenomena in the mould may help to improve our estimation of the stresses built up during the various moulding stages. This project aims to introduce some fracture mechanics concepts in the modeling of the injection moulding process. Note that the term adhesion is taken in its broadest sense, and is meant to encompass phenomena like friction, which appears whenever relative movement is required at the metal/polymer interface. In the world of fibre-reinforced composites, numerical fracture mechanics concepts are known to be effective tools in the estimation of adhesion energy or strain energy release rate.

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Appendix B: Cleaning procedure.

1- Cleaning with demineralized water and soap ( 1.5%).

2- Washing off with demineralized water

3 -Rinsing with alcohol (ethanol or isopropanol).

4- Rinsing with heptane.

5- Drying with nitrogen.

6 -Treatment at UV ozone for 10 min.

Steps 1 & 2 aim to remove most of the grease and inorganic, water-soluble impurities. Steps 3 & 4 allow removal of water and other organic material on the surface The last step destroys traces of organic material remaining on the metallic surfaces. This procedure has been used to clean all the samples (for metallic pieces and polymers without step 6) and the glass used in experiments aiming to determine the drying time of the samples.

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Appendix C: Solvent results.

The experimental samples have been prepared on glass (instead of aluminum or brass), which cleaning procedure is detailed in the preceding appendix To confirm that the solvent was completely removed, and to test the samples quality, the pieces have been heated up to 120 C for few minutes. Under such conditions, the remaining solvent would vaporize very quickly, and blisters would be rapidly visible. These were the chosen criteria to judge the interface quality in our very first experiments. As this work consist in preliminary experiments, no quantified criteria have been chosen to characterize the bubbles quantitatively, I only cared about the qualitative aspects. Results are characterized as follow: 0 : No visible bubbles in the samples. * : Few bubbles are visible. ** : Larger amount of bubbles. *** : Interface almost covered with bubbles. The Results column gives the best quality obtained with the specified condition. The last column give the specimen number presenting the indicated quality compared to the total number of tested sample under the given conditions.
Duration of drying At room temperature In the oven in free atmosphere at 40 Celsius degree 5 days 2 days 5 days 2 days 5 days 2 days 5 days 2 days 4 days 4 days 4 days 4 days 3 days 3 days 3 days 3 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days 2 days Adhesion process capillary capillary drop drop capillary capillary drop drop capillary capillary drop drop capillary capillary drop drop Glass cleaning ozone without ozone ozone without ozone ozone without ozone ozone without ozone ozone without ozone ozone without ozone ozone without ozone ozone without ozone Results 0 0 * ** * 0 * 0 0 ** ** *** * ** ** *** Proportion 4/4 3/4 3/3 3/4 2/2 2/4 1/3 3/4 1/3 2/2 2/2 2/2 1/2 2/2 2/2 2/2

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Solvent application Two ways were used to stick the pieces of PC on their substrate. The drop: 1 drop of solvent was rested on the metal and the PC piece was rested on it. This method is good to make sure that the whole surface is covered with solvent, but a larger quantity of liquid is necessary. Longer time is necessary to remove it totally, and crystallization often begins. Capillary: the piece of PC is put on the substrate, and a drop of solvent is allowed to diffuse along the interface by capillary. This method uses a lower quantity of solvent, drying is thus quicker. But it is difficult to have complete surface coverage, and so almost impossible to know the precise adhesion surface. Other ways have been envisaged, but not attempted: Apply solvent with a brush, Use a spray, but the reaction is immediate and rapid, in both cases the surface of PC is affected (deformed, curved). Without taking into account the problems with drying, the best method seems to be the drop technique, because of the possibility to cover the complete surface without damaging it. In future work, it would be interesting to examine the possibility of using of a micropipette and very flat surface (to avoid local solvent accumulation)

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Appendix D: Birefringence.

Birefringence is based on the properties of certain materials which are optically isotropic, but can be made anisotropic under external actions : a stress field for example. Each point behaves like a birefringent strip, where neutral lines correspond to the principal stress direction. Experiment shows that the induced phase difference of light passing through the strip is proportional to the principal stresses difference between the principal stresses at that point. The stressed strip induced an optical path difference :

= en = eC (T , t ) ( x y )
With e : thickness of the strip n : optical index variation C : Stress optical coefficient (Time and temperature dependant in P.C.) (Ref [8]) x and y : principal stress at the given point Further more the phase difference between the ordinary and the extraordinary ray is : 2 = With : optical path difference, : wave length. Thus, for specific phase differences (mainly the destructive ones), some wavelengths are switched off if the sample is placed between crossed polarizer and analyzer. The considered sample area then appears in the complementary color of the extinguished wavelength. A pattern of colored fringes then appears and characterizes the stress state of the piece. This experimental stress pattern, obtained from the stress optical coefficient, can then be compared to the model predictions. One can also use birefringence to follow delamination.

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The next photographs show the fringe pattern due to the stresses generated due to a difference of thermal expansion coefficients during cooling down of a polycarbonate piece which adheres on its substrate. The cooling down leads to delamination which can be clearly observed as shown below.

Crack tip.

Area of still effective adhesion

Pict F1: Use of birefringence to detect delamination. Substrate: Aluminum.

Crack tip.

Delaminated area.

Pict F2: Use of birefringence to detect delamination Substrate: Brass.

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Appendix E: G numerical results.

In the next tables, the height and length of the polycarbonate piece are given in mm; the energy release rate is expressed in J/m2.

Length 2 4 6 8 10

Height

1 0.795 0.465 0.333 0.280 0.258

2 0.319 0.235 0.177 0.148 0.133

3 0.144 0.141 0.115 0.098 0.088

4 0.068 0.091 0.081 0.072 0.065

5 0.034 0.062 0.061 0.055 0.052

Table A: Energy release rate for a sample with a 104 mesh density, under a 2m displacement, and a starting crack.

Length 2 4 6 8 10

Height

1 0.697 0.390 0.277 0.235 0.223

2 0.313 0.220 0.164 0.137 0.125

3 0.154 0.143 0.113 0.096 0.087

4 0.078 0.098 0.084 0.073 0.067

5 0.041 0.069 0.065 0.058 0.048

Table B: Identical conditions to table A with a twice-denser mesh (start crack)

Length

Height 2 4 6 8 10

1 12 16 17 16 13

2 2 7 8 7 6

3 6 1 1 2 1

4 13 7 4 2 2

5 19 12 8 5 7

Table C: Difference in percent between the original mesh and the twice-denser mesh.

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Length 4 6 8

Height

2 0.468 0.243 0.205

3 0.183 0.154 0.132

4 0.112 0.104 0.093

5 0.074 0.075 0.071

Table D: Energy release rate for a sample, with a twice coarser mesh density than case A, and a starting crack.

Length 4 6 8

Height

2 49 35 38

3 24 25 26

4 25 23 23

5 20 20 20

Table E: Percentage difference in percent between the original mesh and the twicecoarser mesh.

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Appendix F: Philips.

I. Philips company. Philips is now among the 10 first electronic groups in the world, its net income in 1998 rose to 13.339 million Dutch Guilders (around 7 million US dollars, 52 million francs). Seven divisions make its products: - Philips Business Electronics, - Philips Components, - Philips Consumer Electronics, - Philips Domestic Appliance and Personal Care, - Philips Lightning, - Philips Medical Systems, - Philips Semiconductors. These divisions are themselves supported by : - the Center for Manufacturing Technology - Philips PMF (Plastics and Metalware Factories) - Philips Machinefabrieken - Philips Design - and of course, Philips Research

II. Philips Research. Founded in Eindhoven, The Netherlands, in 1914, Philips Research has expanded the scale and scope of its activities to become one of the worlds major private research organizations. It has laboratories in six different countries (The Netherlands, England, France, Germany, Taiwan and the United States) and is staffed by around 3,000 people. Its activities have led to the award of over 60,000 patent and design rights, and the publishing of many technical and scientific papers. The annual research budget of Philips Research is slightly less than 1% of Philips Electronicsannual sales, which amounted to more than 76 billion Dutch guilders (about 39 billion US dollars or 228 billion francs) in 1997 Scientists from a wide range of disciplines, from electrical engineering, physics, chemistry, mathematics, mechanics, information technology and software, work in close proximity, influencing and broadening each others views. Philips Research betted on the benefits of synergy and cross-fertilization of ideas. In close co-operation with the Philips Product Divisions, the Philips Research organization generates options for new and improved products and processes, and produces important patents in many fields. These patents are important, because they protect technological achievements and enable Philips to gain access to the knowledge of others.

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II-a. A little history. The Philips Company started in 1891. The technical development of its sole product, the incandescent lamp, was done alongside the factory. In the rest of the world, the concept of a separate industrial research laboratory was only just emerging. In 1913, the decision was taken to open a physics laboratory (the Natuurkundig Laboratorium or Nat.Lab. ). And in 1914, Dr G. Holst became the first true researcher in Philips. Broadly speaking, three periods can be distinguished. These are closely related to the historical development of the Philips Company and the general economic and political situation in the world at the time [12].

From 1914 to 1945 was the period of growth and diversification. A part from improvements to the incandescent lamp, research was carried out into gas discharge lamps as a more efficient way to generate light. At the same time, the bulb technology opened up the way to new products such as the X-ray tube and the radio valve. The invention of the pentode (five-electrode lamp) gave Philips a basic patent in the radio field. In 1923, Philips decided to become a systems supplier instead of a components company . The research organization broadened its scope into work on radio receiving and transmission. Early work was also done into the development of television.

The second period, which started after World War II, was the period of expansion. The research philosophy was characterized by the belief that research always pays off, and that research automatically leads to products. In this period television became a mass-produced consumer good and the research work initiated in the 1930s became a major program. The invention of the transistor by Bell Labs changed the world of electronics forever. Philips had access to the transistor patents through a cross-license agreement between Philips and AT&T. Philips strength was based, among other things, on its strong patent position in magnetic materials. In the field of semiconductor devices, Philips Research contributed a new germanium transistor used in every modern MetalOxide-Semiconductor Integrated Circuit (MOSIC) and developed the Integrated Injection Logic used in the majority of the present bipolar-IC devices. In this period, research laboratories in England, France, Germany and the USA were founded.

In the third period from 1970 to the present time, industrial research has been tied much more closely to industrial activities. The emphasis has been shifted to research on systems; the research into integrated-circuit design and technology has played a very important role. Information processing, storage, transmission and display were and are the main subjects of research. In this period, the field of optical recording was opened up by Philips Research giving rise to such well-known products as Compact Disc Digital Audio, CD-ROM and more recently DVD (the 'Digital Video Disc' or 'Digital Versatile Disc'). Philips Research was, by this time, also heavily involved in medical systems such as magnetic-resonance imaging and ultrasound. In mobile telephony the full-rate GSM speech code is an important Philips Research contribution. Research into components has

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brought a great deal of success. World-class semiconductor lasers are good examples of this. Also, research into polymer Light-Emitting Diodes (LEDs) and plastic electronics show great prospects for new components. New dedicated multi-milliontransistor ICs are designed for digital video coding and decoding and for speech recognition Finding the right balance between dedicated and programmable solutions ('co-design') is one example of the activities in which Philips Research is involved today. II-b. The Nat.Lab. The Nat.Lab. is part of PHILIPS Corporate Research. It is the largest of the PHILIPS Research laboratories and one of the largest industrial research laboratories in the world. It has a staff of about 1700 people at the headquarters in Eindhoven and a research group composed of 15 people in Monza (Italy) [12].

Fig. A1: PHILIPS Natuurkundig Laboratorium, Eindhoven, The Netherlands.

The Nat.Lab. recruits people straight from universities or engineering schools. New employees are involved in research projects. Their stay at the Nat.Lab. is normally limited to a period of four to eight years, in which they work on new phenomena and the development of new processes, devices, systems and applications. After their period at the Nat.Lab., researchers often join a Product Division (often starting in a development group). The PDs welcome them as well trained staff. Because of their previous stay at the Nat.Lab, they are ideal communication partners for Philips Research. By means of this circulation policy, the Nat.Lab achieves its goal of maintaining an enthusiastic crew, eager to find new solutions. Employees who stay at the Nat.Lab. form the scientific backbone of the laboratory. Their presence ensures continuity and training of young staff members. Group leaders are chosen for their scientific reputation and their capacity to coach professionals. The Nat.Lab. consists of eight sectors: the sector Operations & Engineering for internal services and seven sectors for different areas of research . Each sector consists of a number of groups. Some of them are outside of the Corporate Research budget and therefore have the responsibility of generating their own income.

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Appendix G: Material Mechanics and Heat Transfer group.

I. Description. The expertise of the group is in the area of solid mechanics, fluid mechanics and thermal physics. Since these are broad disciplines, areas of applications are found in many of Philips products and related processes. The scope is therefore to provide a disciplinary support for the innovation and to focus on the reliability aspects both with respect to thermal and mechanical failure. The work is theoretical and experimental in character, and often extended by numerical analysis. The experimental facilities include a broad range of apparatus for mechanical characterization of solid materials, liquids and flow of liquids and thermal properties of. For numerical analysis commercial finite element software packages are used (ANSYS, MARC, Fidap, Flotherm, SEPRAN). The majority of the members of the group have a degree in engineering or applied physics, a number of them with a background in fluid mechanics. Because of the horizontal character of the disciplines, co-operation with other groups and laboratories is essential for all of the projects. First of all, many of the group projects form part of larger projects, which run in the business groups themselves, or in system research groups. Formal relations exist to the University of Eindhoven, Leeds and Burgers center. Informal contacts exist to many national and international institutes of fluid dynamics and material mechanics (like INSA in France for example).

II. General Trends. An important trend for Philips is to move the ambition with respect to materials processing to outside suppliers, while focussing internally on cost reduction and optimized processing. A general trend for the group is to re-balance the distribution between analytical type of work and synthetical type of work. The analytical type of work is more involved with understand the problem. Synthetical type of work deals with coming up with new options and solutions. Group intention is to move more to the synthetical side that requires a somewhat different mind setting. The ultimate goal, however, is to improve existing processes and products.

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III. Group sub-activities. Thin Film Mechanics. Description: Tribology and mechanical properties of thin films, structural integrity of brittle materials and plastics, analysis of abrasion machining processes. Present application: Optical recording systems, flat displays, lighting, passive components, possibly semiconductors. Wet coating processes. Description: Innovation of coating techniques; coatings on finite inhomogeneous 3Dsubstrates, formulation of coatings and inks. Present application: Application of optical coatings and phosphor on Cathode Ray Tubes, hydrodynamics of capillary systems. Printing processes. Description: Innovation of printing techniques, including formulation of inks. Present application: Deposition of patterned layers for poly-LED, (plastic) electronics, Printed Circuit Boards. Thermal management. Description: Research on fluid flow and heat transfer in geometrically complex structures and thermal characterization of components: numerical analysis supported by experiments, virtual prototyping, measurement of material properties, performance of cooling. Present application: Electronic power circuits, electronic systems, CRT and flat panel manufacturing, optical recording. Home Care. Description: Study of principles underlying the area of home environmental care for the developments of innovative product concepts. Application: Ironing, garment care, floor care. Polymer processing. Description: Modeling of specific properties of plastic processing and systems such as optical disk mastering and molding, further miniaturization and integration in plastics. Present application: Optical recording, multi technology injection molding. Major trends: Non-isothermal and 3D modeling of flow and solidification of polymer melts for the study of filling extremely small cavities and elongational viscosity of polymer. Miniature integrated modules. Interaction of thin polymer film with organic/inorganic substrates (electrical, heat, optical, crystallization).

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Acknowledgements.
I am thankful to the Material Mechanics and Heat Transfer group for its welcome, and its friendship (Id like to mention Cor Roelandse for his help with my outing tips). I am grateful to Michiel Roersma, Dirk Brokken and Lucien Douven for their advice and help to learn Mentat and Marc software, and to Jurgen Rusch for almost all my computer related problems. Id like also to thank Harm Keunen (Technical University of Eindhoven) for his help in learning Zencrack, and of course Christian Rademaker (from CFT) for his precious advice. But above all, Id like to offer very special thanks to Amar Mavinkurve, my supervisor, for his help, his consideration, his favors and of course, his friendship. He really helped me to stay in the best working conditions. I deeply wish his project would conclude successfully.

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Author(s): Title :

Ivan Goudet Design of a model system for the determination of adhesion energy between a polymer and metal.

Distribution Nat.Lab./PI PRL PRB LEP PFL CP&T Director: Department Head WB-5 Redhill, UK Briarcliff Manor, USA Limeil-Brvannes, France Aachen, Germany WAH J.A. Pals M. Buijs WB-53 WB-12

Abstract Members of group Buijs J.G. de Bruin Nat.Lab. WB-72

Full report C.W. Rademaker U.P. Goossens D.S. Samoy R. Wimberger-Friedl J.M.J. den Toonder P.C.P. Bouten P.J. Slikkerveer D.B. van Dam J.F. Dijksman A.A. Mavinkurve (4X) CFT CFT CCPMF Nat.Lab. Nat.Lab. Nat.Lab. Nat.Lab. Nat.Lab. Nat.Lab. Nat.Lab. SAQ-2 SAQ-2 SEH-2 WB-72 WB-31 WB-31 WB-12 WB-12 WB-12 WB-31

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