Engineering reversible elasticity in ductile or brittle thin films and products resulting from said engineering
11654609 · 2023-05-23
Assignee
Inventors
- Nicolas Vachicouras (Chambesy, CH)
- Christina Myra Tringides (Ames, IA, US)
- Stephanie P. Lacour (Etoy, CH)
Cpc classification
B32B3/266
PERFORMING OPERATIONS; TRANSPORTING
B32B2535/00
PERFORMING OPERATIONS; TRANSPORTING
B32B15/06
PERFORMING OPERATIONS; TRANSPORTING
B29D28/00
PERFORMING OPERATIONS; TRANSPORTING
B29C59/007
PERFORMING OPERATIONS; TRANSPORTING
B29C55/023
PERFORMING OPERATIONS; TRANSPORTING
B29D7/00
PERFORMING OPERATIONS; TRANSPORTING
B29K2079/08
PERFORMING OPERATIONS; TRANSPORTING
B32B3/26
PERFORMING OPERATIONS; TRANSPORTING
Y02E60/10
GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
B32B27/28
PERFORMING OPERATIONS; TRANSPORTING
B32B7/12
PERFORMING OPERATIONS; TRANSPORTING
International classification
B32B3/26
PERFORMING OPERATIONS; TRANSPORTING
B29C59/00
PERFORMING OPERATIONS; TRANSPORTING
B29D28/00
PERFORMING OPERATIONS; TRANSPORTING
Abstract
The present disclosure relates to how to engineer reversible elasticity in thin films and/or layers and/or substrates, using a repeated Y-shaped motif, which is cut out through the film and/or layer and/or substrate. As an example, using a 75 μm thick polyimide (PI) foil, macroscopic dog-bone shaped structures with a range of geometrical parameters of the Y shape have been prepared according to an embodiment of the present disclosure. The tensile strain response of the film at its point of fracture was then recorded. The structures were also confirmed using finite element modeling. Upon stretching, the PI ligaments locally deflect out of plane, allowing the foil to macroscopically stretch.
Claims
1. A multilayer substrate comprising: at least a bottom layer of electrically isolating, intrinsically non-elastic material and, on said bottom layer, a top layer of electrically conductive, intrinsically non-elastic material, said bottom and top layers forming opposite exposed main surfaces of the multilayer substrate; a plurality of through cuts each extending through a thickness of each of said bottom and top layers, the plurality of through cuts in an unstretched state forming a pattern of open surface areas in the opposite exposed main surfaces of the multilayer substrate; wherein each of said through cuts has projections on the opposite exposed main surfaces of said multilayer substrate, and the projections are shaped so as to comprise at least three branches extending from a common portion, each branch having a length and a width that form said open surface areas.
2. The multilayer substrate as claimed in claim 1, wherein, on said opposite exposed main surfaces of said multilayer substrate, at least two of the branches of at least one of said through cuts are of equal length.
3. The multilayer substrate as claimed in claim 1, wherein, on said opposite exposed main surfaces of said multilayer substrate, at least two of the branches of at least one of said through cuts have equal width.
4. The multilayer substrate as claimed in claim 1, wherein, on said opposite exposed main surfaces of said multilayer substrate, each of the branches of at least one of said through cuts has a width between 100 nm and 1 cm.
5. The multilayer substrate as claimed in claim 1, wherein said multilayer substrate extends along a length direction (X) and a width direction (Y) substantially perpendicular to said length direction (X), and wherein, on said opposite exposed main surfaces of said multilayer substrate, for at least two of said through cuts, two respective branches extend along a direction which is parallel to one of said directions (X) or (Y).
6. The multilayer substrate as claimed in claim 1, wherein, on said opposite exposed main surfaces of said multilayer substrate, the plurality of through cuts includes N through cuts/cm.sup.2, with N ranging from 2 to 100,000,000.
7. The multilayer substrate as claimed in claim 1, wherein the thickness of said bottom layer is comprised between 1 nm and 500 μm.
8. The multilayer substrate as claimed in claim 1, wherein said top layer is formed of a conductive metal oxide.
9. The multilayer substrate as claimed in claim 1, wherein the thickness of said top layer is comprised between 1 nm and 500 μm.
10. The multilayer substrate as claimed in claim 1, wherein the multilayer substrate forms a stretchable electrode.
11. The multilayer substrate as claimed in claim 1, wherein a transparency of the opposite exposed main surfaces of the multilayer substrate, which is a ratio between the open surface areas over a total surface area, ranges from 25% to 90%.
12. A method for engineering elasticity, said method comprising: providing a multilayer substrate comprising at least a bottom layer of electrically isolating, intrinsically non-elastic material and, on said bottom layer, a top layer of electrically conductive, intrinsically non-elastic material, said bottom and top layers forming opposite exposed main surfaces of the multilayer substrate; forming a plurality of through cuts in said multilayer substrate, each through cut extending through a thickness of each of said bottom and top layers, the plurality of through cuts in an unstretched state forming a pattern of open surface areas in the opposite exposed main surfaces of the multilayer substrate; wherein each of said through cuts has projections on the opposite exposed main surfaces of said multilayer substrate and the projections are shaped so as to comprise at least three branches extending from a common portion, each branch having a length and a width that form said open surface areas.
13. The method as claimed in claim 12, wherein forming said plurality of through cuts includes forming at least one through cut having, on said opposite exposed main surfaces of said multilayer substrate, at least two branches of equal length.
14. The method as claimed claim 12, wherein forming said plurality of through cuts includes forming at least one through cut having, on said opposite exposed main surfaces of said multilayer substrate, at least two branches of equal width.
15. The method as claimed in claim 12, wherein said multilayer substrate extends along a length direction (X) and a width direction (Y) substantially perpendicular to said length direction (X), and wherein forming said plurality of through cuts includes forming, on said opposite exposed main surfaces of said multilayer substrate, for at least two of said through cuts, two respective branches extending along a direction which is parallel to one of said directions (X) or (Y).
16. The method as claimed in claim 12, wherein forming the plurality of through cuts includes forming, on said opposite exposed main surfaces of said multilayer substrate, N through cuts/cm.sup.2, with N ranging from 2 to 100,000,000.
17. The method as claimed in claim 12, wherein the thickness of said bottom layer is comprised between 1 nm and 500 μm.
18. The method as claimed in claim 12, wherein said top layer is formed of a conductive metal oxide.
19. The method as claimed in claim 12, wherein the thickness of said top layer is comprised between 1 nm and 500 μm.
20. The method as claimed in claim 12, wherein the multilayer substrate forms a stretchable electrode.
Description
BRIEF DESCRIPTION OF THE SEVERAL VIEWS OF THE DRAWINGS
(1) In the following, description will be given of examples and/or embodiments of the present invention, in particular of the examples and/or embodiments which are depicted in the drawings,
(2) However, the present invention is not limited to the examples and/or embodiments as disclosed in the following and/or as depicted in the drawings, but comprises all variants of same which fall within the scope of the appended claims.
(3) In the drawings:
(4)
(5)
(6)
(7)
(8)
(9)
(10)
(11)
(12)
DETAILED DESCRIPTION
(13)
(14) As depicted in
(15) The cut may be formed according to one of wet and/or dry etching, mechanical punching or the like and extends throughout the thickness of the relevant layer and/or substrate.
(16) For instance, the cut extends throughout the thickness of the layer 100 (between the two main exposed surfaces thereof), as well as throughout the thickness of the substrate 120 (between the two main exposed surfaces thereof), and between the thickness of the layer 100 in
(17) As depicted in each of
(18) As anticipated above, within the meaning of the present invention, layers, films, substrates and even multilayer and/or stacked substrates can be engineered.
(19) As an example, a plurality of stacked materials can be engineered, and the number of stacked materials can vary from one to tens or more, and the kind of materials can vary as well.
(20) For example, a substrate comprising:
(21) a membrane of polyimide
(22) a tri-layer: polyimide/titanium (Ti)/polyimide
(23) 5 layers: polyimide/Ti/platinum (Pt)/Ti/polyimide
(24) 7 layers: SiO2 polyimide/Ti/Pt/Ti/polyimide/SiO2
(25) can be engineered.
(26) The stack may also include polymers such as adhesion promoters, or self-assembled monolayers.
(27) The nature of the materials within the stack may be electrically insulating or conducting or semiconducting.
(28) Still within the scope of the present invention, addition of an elastic encapsulation of the engineered elastic stack and/or layer and/or substrate can be envisaged
(29) As an example, the engineered stack and/or layer and/or film and/or substrate can be embedded within an intrinsically elastic material (e.g. silicone rubber).
(30) Still within the scope of the present invention, a distinction can be made between the one or more carrier elastic materials and the top—encapsulating elastic material. They may be distinct materials (e.g. two types of silicone rubber).
(31) The elastic encapsulation may be a plain membrane but may also contain openings through its thickness so that some pads on the engineered elastic stack become exposed, for instance for the purpose of electrically contacting the exposed layer (when conductive and/or semiconductive).
(32) These openings will be primarily patterned in the top encapsulating elastic material but there could be a scenario where the carrier elastic material also comprises openings and/or vias.
(33) As depicted for instance in
(34) Within the scope of the present invention, the cuts can be dense or thin according to the needs and/or circumstances. Moreover, the dimension (size) and/or orientation of the cuts can be selected as well according to the needs and/or circumstances.
(35) As to both the size of the cuts and their possible orientations examples will be disclosed in the following.
(36) As to the density of the cuts, same may be defined as follows and possible ranges of same may be as follows.
(37) Cuts/cm.sup.2: the ratio can vary from 1 cut/cm.sup.2 to 100 million cuts/cm.sup.2.
(38) Spacing: distance between the 2 centers (center lines of the Y, (see parameter Las disclosed below). L can vary from 1 um to 1 cm (or more); 10-25 um spacing may be preferred.
(39) Transparency: ratio between the open surface area over total surface area. This can range from 25 to 90%. but does not capture the density of cuts.
(40) By changing the density of cuts, it is possible to modulate the resulting elasticity of the engineered elastic layer and/or substrate and/or stack or the like. This is particularly relevant when the elastic stack hosts interconnects linking rigid electronic hardware.
(41) (See
(42) As to the Shapes of the Cuts
(43) Most of the tests as reported herewith have been carried out on layers and/or substrates or the like which were engineered by forming Y-shaped cuts into same. However, within the scope of the present invention, cuts with different shapes may be formed as well.
(44) By way of example, Y-shaped cuts may be replaced by multi-branched cuts (with the minimum number of branches being 3). Moreover, into the same layer and/or substrate or the like, cuts with different shapes may be formed; as an example, according to the present invention, a layer and/or substrate or the like, once engineered, may comprise Y shaped cuts along with four branches and/or five branches cuts and so on.
(45) Furthermore, shape does not need to be an isotropic structure (where all branches are of the same length and separated by an equal angle). Lengths of the branches and/or reciprocal orientation thereof may be selected according to the needs and/or circumstances. As an example, elasticity can also be induced if one of the branches (for instance the vertical branch of the Y shaped cuts) is longer than the other two.
(46) Methods
(47) Sample Fabrication
(48) The PI (polyimide, Kapton® HN—Standard Rolls—610 mm wide) and PET (polyethylene terephthalate, Mylar®) films were purchased from Lohmann Technologies. The Y-shaped patterns were cut into the films with a Plotter Cutter (RoboPro CE5000-40-CRP) using a DXF file generated with a MATLAB (R2015b) script. The contour of a dogbone shape (see for instance
(49) For electrically conductive platinum (Pt) samples, an oxygen activation step was first done to improve adhesion on the PI, and followed by the evaporation of a thin layer of 25 nm titanium (Ti). For indium tin oxide (ITO) samples, 100 nm of the conductive material was sputtered on the PET film. The films of PI and PET had a thickness of 75 um.
(50) The PDMS (poly(dimethylsiloxane)) samples were prepared by coating a silicon (Si) wafer with a self-assembled layer of trichloro(1H,1H,2H,2H-perfluorooctyl)silane (Sigma Aldrich) in a dessicator. PDMS (Sylgard 184, Dow Corning, mixed at 10:1 (w:w) with a pre-polymer crosslinker) was then spin-coated on the Si wafers (750 RPM for 35 seconds) and cured at 80° C. for at least 3 hours in a convection oven. The PDMS was then cut out using the same technique as for the PI and PET films with the Plotter Cutter and released manually from the wafer. This technique was able to reliably pattern the Y-shapes onto the film.
(51) Electromechanical Characterization
(52) All samples, except for the bulk PI, were mounted on two clamps for tensile testing on a uniaxial stretcher (MTS Criterion Model 42, with a load cell of 100N maximum capacity) and using a strain rate of 1 mm/s. The samples were securely fastened to the plates of the stretcher by placing double-sided tape on both sides of the film. When the plates moved apart from one another, the dogbone was stretched at a constant and known rate and displacement. For electrically conductive samples, a piece of conductive copper tape was placed on each end of the dogbone, each on which one cable connected to a source meter was attached. This enabled the recording of resistance as the film stretched. The bulk PI was mounted to another uniaxial stretcher for larger force measurements (100 kN MTS 809 axial-torsional servohydraulic testing machine with a load cell of 10 kN). The force-displacement data was measured at a sampling frequency of 100 Hz using the MTS TestSuite TW software. The data was analyzed using MATLAB (R2015b).
(53) For conductive samples, a copper adhesive was taped on each end of the sample and to a Keithley 2400 source-meter for simultaneous resistance measurements.
(54) For figures of mechanical testing, we reported data only up to the maximum strain where all samples survived.
(55) For long-term cycling, the samples were mounted to a homemade uniaxial stretcher and stretched at 10% of their initial length at 1 Hz (1 stretching cycle per second). The resistance was measured using a 4-probe system and a Keithley 2400 source-meter. The stretcher and source-meter were both controlled using custom made software based on Lab View 2015. The resistance is recorded (sampling rate of 5 Hz) and saved only every 10 cycles per decade of cycles.
(56) Scanning Electron Microscopy
(57) SEM images were acquired with a Zeiss Merlin microscope using an annular detector at beam energy of 1 keV.
(58) Finite Element Analysis
(59) The mechanical simulations were performed on the finite element program ABAQUS (6.14) in order to evaluate the effect of the different geometries' parameter. The standard static procedure was used with a damping factor of 1e-7. The S4R element was used with a global mesh size of 0.15 mm and no dependence on the mesh size was observed. Two steps were created with a first step of perturbations applied on three random points and in the direction perpendicular to the film's surface. The perturbations' influence was analyzed and no influence on the force-displacement behavior was observed. The second step consists of a clamped boundary condition on one end and a displacement in the stretching direction on the other end while deactivating the perturbations.
(60) The electrical stimulations were performed with COMSOL (2015) in order to estimate the resistance of a 100 nm thick conductive sheet of platinum, which was cutout with various geometries of the Y-shaped pattern. The ground boundary condition was applied on one end of the sheet and a terminal with 1 A was applied on the other hand. The resulting maximum voltage field was used to estimate the resistance by dividing its value by 1 A.
(61) Results and Discussions
(62) To engineer elasticity in stiff materials, a Y-shaped pattern was designed. Each of the three branches of the Y motif are of equal length (parameter “a”) and width (“w”). The Y shapes are spaced such to form a hexagon: the distance between two motif's centers, on the x-axis, is “L” (
(63) First, the Y-shape motif parameters were optimized. 12 different combinations of a, w, and L were cut and then stretched until failure, which was defined as the time at which the first motif broke. There were 4 different ratios of a/L (0.5, 0.6, 0.7, 0.8) and 3 different values of w (0.7 mm, 1.1 mm, 1.5 mm). Each combination was tested three times, to provide error bars to both the displacement and force at break. Films of bulk (uncut) Kapton and a film of uncut PDMS were also stretched until failure. Each film was 75 urn thick. All 14 force-displacement curves are plotted in
(64) From these three experiments graphs, it was determined that the optimal geometry for the Y-shapes was that of maximum a/L, 0.8, and second largest value of w, 1.1 mm. To understand the effect of film thickness on the spring constant, films of PI of the above given Y-shape parameters were cut on a varying thickness of PI films (25, 50, 75 um). When plotted logarithmically, it was observed that the spring constant scaled as a function of the film thickness, cubed. For comparison, bulk PI of these same thickness was also stretched. Here, the spring constant scaled as a function of the film thickness, only. When the Y-shapes were simulated on PI of different thicknesses (5, 10, 25, 50, 75, 125 um), the observed scaling law on spring constant matched that observed in the experiment. The difference between bulk and engineered PI is thought to come from the buckling and deflection mechanisms seen by the branches, where the force scales in function of the cube of the thickness. The analytical equations of this behavior are out of the scope of this paper, but the experiments match the simulation predictions and we expect a cubic relationship between the spring constant and the thickness, as the bending stiffness scales cubically with thickness.
(65) Since the Y-shapes have 90° corners at the end of each branch, this causes high local strains at these right angles. It was hypothesized that rounding the ends would decrease this strain and thus increase the displacement of the film; further, if circles with a diameter larger than the width w were added to the ends of the branches, the elongation at break of the film should increase even more. Four branch end geometries were compared: squared, rounded, circles with radius 1.2 mm, and circles with radius 1.3 mm. For the rounded ends, the corners of the squared ends were simply rounded to avoid sharp bends. The circles were added such that the total length of each branch was unchanged, as indicated in a schematic in
(66) Once a mechanical characterization of the PI films was completed, the effects of the Y-shapes on electrical conductivity was explored. First, a ductile metal, platinum (Pt) was evaporated on one side of the Kapton film, after the cracks had been cut (
(67) After evaporation of the Ti/Pt, the dogbone films were still able to stretch and deflect in the same way as with the Kapton (
(68) To demonstrate the effectiveness of this approach to engineer elasticity in brittle films, which typically fail after an applied strain of 5%, indium tin oxide (ITO) was sputtered on the top layer of a PET film, after the Y-shapes had been cut into the polymer (
CONCLUSIONS
(69) In summary, we have demonstrated a novel approach to patterning both single and multi-layer, multi-material foils, to engineer elasticity in these films. We performed a systematic study of the electromechanical effects on ductile and brittle electrically conductive materials, as well as an extensive analysis of different geometrical factors that affect local strain and the out-of-plane deflections. Due to the nature of the Y-shaped motifs, which have parameters that are smaller than those of the overall film design, the motif can be overlaid onto any design. Additionally, the technique of cutting the patterns can be used on virtually any material(s), showing potentials for various applications.
(70) The structures were also confirmed using Finite Element Modeling. Upon stretching, the PI ligaments locally deflect out of plane, allowing the foil to macroscopically stretch. The effective spring constant of the engineered PI can be reduced by two orders of magnitude allowing us to nearly match the spring constant of a silicone elastomer of equivalent thickness (75 μm). The engineered films demonstrated no preferential direction of stretching. We applied our motif to ductile platinum (Pt) films on PI foils and brittle ITO (indium tin oxide) films on PET (Polyethylene Terephthalate) foils. The Pt/PI system maintained stable electrical conduction when stretched up to an engineered strain of up to 70%. Moreover, it withstood 100,000 stretch cycles at 10% applied strain, without undergoing electromechanical fatigue. Similarly, the ITO/PET structure stretched up to a maximum 50% uniaxial strain, and kept its electrically and mechanically integrity after a 10000 stretch cycle at 10% applied strain. The proposed design is versatile and compatible with thin-film processing. We anticipate the patterned motifs can be scaled down to offer a wider range of elastic electronic materials to be used in stretchable electronics and soft bioelectronics.
(71) The invention offers a generic design and associated processes and materials enabling in a hexagonal pattern reversible elasticity in films or membranes that are initially inextensible. The distribution of repeated through-hole patterns within a non-elastic multilayered membrane programs reversible elasticity within the said initially inextensible membrane. The through-hole patterns are replicated 2D (planar) closed shapes open in the multilayered membrane. Upon mechanical loading, the contour of the through-hole patterns deforms by moving out of its initial plane thereby enabling substantial mechanical deformation. This method can be applied to a single material and uniform membrane but also to multilayered, multi-material stacks.
(72) The design is valid across scales (macro-to nanoscale) and compatible with any materials, which can be initially laid or manufactured into a film i.e. a uniform planar membrane for which one of its three dimensions is several orders of magnitude smaller than the other two. Examples of such materials include plastics, paper, metals, elastomers, semiconductors. The design is suitable for both ductile (e.g. Platinum) and brittle (e.g. indium-tin oxide—ITO) materials.
(73) An example of a suitable through-hole motif is a “Y” or tri-branched, equidistant shape. See
(74) The through-hole pattern and distribution are further optimized against the structure stiffness and electrical properties. Multilayered structure consisting of at least three layers where the outer layers are electrically insulating polymers and at least one layer is a film of electrically conductive or semiconducting material. The structure may be freestanding or bonded to or embedded in an elastic carrier. Each layer is well bonded to its neighboring ones. An adhesion layer or coating may be deposited on each side of the structure to ensure irreversible bonding with the elastic carrier. The structure is patterned with a myriad of tri-branched through-the-thickness openings, which are not connected to each other. The shape of the tri-branched unit cell is characterized by the branch width and length. See
(75) It has therefore been demonstrated with the above description that the present invention allow to obtain the wished results, thus overcoming the drawbacks affecting the prior art.
(76) While the present invention has been clarified by means of the above description of some embodiments, the present invention is not limited to the embodiments depicted in the drawings and/or described above.