Guided template based electrokinetic microassembly (TEA)
11840769 · 2023-12-12
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Abstract
The present invention is directed to devices and methods for assembling particulates through the use of non-contact electrokinetic forces applied to polymeric, organic, non-organic, and metallic micro- and nano-particulates in an aqueous solution. The present invention features an electrode comprising a conductive substrate with a layer of photosensitive polymer disposed on it with a plurality of windows etched into the layer. The plurality of windows expose certain portions of the conductive substrate. Applying electric signals to the conductive substrate (e.g. by a function generator) causes materials to attract to only the exposed portions of the conductive substrate. The materials may comprise a plurality of organic, non-organic, and metallic micro- and nano-particulates disposed in an aqueous solution.
Claims
1. A system for assembling particulates through the use of electrokinetic means, the system comprising: a. a conductive substrate (10) comprising a plurality of electrodes disposed side-by-side, each electrode comprising; a layer of photosensitive polymer (20) disposed on top of each electrode; wherein each layer of photosensitive polymer (20) is patterned with a plurality of windows (25) exposing the electrode underneath; wherein, for each electrode, a bottom of each window of the plurality of windows (25) is made up entirely of the electrode; c. a solution comprising a plurality of particulates and contacting the conductive substrate; and d. a function generator (30) configured to apply a non-uniform AC signal to the plurality of electrodes such that the non-uniform AC signal causes the plurality of particulates in the solution to move and attach to the plurality of electrodes through the plurality of windows (25).
2. The system of claim 1, wherein the AC signal is configured to cause electroosmosis or dielectrophoresis.
3. The system of claim 2, wherein the system is configured to use a combination of electroosmosis and dielectrophoresis to guide the plurality of particles to the plurality of electrodes.
4. The system of claim 1, wherein the particulates are microparticulates, nanoparticulates, or a combination thereof.
5. The system of claim 1, wherein the particulates are organic particulates, non-organic particulates, metallic particulates, or a combination thereof.
6. The system of claim 1, wherein the system is configured to sort the plurality of particulates based on size, shape, density, conductivity, material composition, or permeability.
7. A method for fabricating an electrode array (100) used for assembling particulates through the use of electrokinetic means, the method comprising: a. providing a conductive substrate (10) comprising a plurality of electrodes disposed side-by-side; b. spin-coating a layer of photosensitive polymer (20) on top of each electrode of the plurality of electrodes; and c. patterning each layer of photosensitive polymer (20) to form a plurality of windows (25) in each layer of photosensitive polymer (20) and expose the electrode underneath; wherein, for each electrode, a bottom of each window of the plurality of windows (25) is made up entirely of the electrode; wherein each electrode (100) is connected to a function generator (30), wherein the function generator (30) is configured to generate non-uniform electric signals to attract particulates in a solution to the plurality of electrodes through the plurality of windows (25).
8. The method of claim 7 further comprising soft baking each layer of photosensitive polymer (20) after spin-coating it onto the electrode.
9. The method of claim 8 further comprising hard baking the conductive substrate (10) after soft baking each layer of photosensitive polymer (20).
10. A method for assembling particulates through the use of electrokinetic means, the method comprising: a. providing a conductive substrate (10) comprising: i. a plurality of electrodes disposed side-by-side, each electrode comprising a layer of photosensitive polymer (20) disposed on top of each electrode, wherein each layer of photosensitive polymer (20) is patterned with a plurality of windows (25) to expose the electrode underneath; wherein, for each electrode, a bottom of each window of the plurality of windows (25) is made up entirely of the electrode; b. providing an aqueous solution comprising a plurality of particulates and contacting each layer of photosensitive polymer (20) and each electrode; and c. applying non-uniform electrical signals to the plurality of electrodes (100), wherein the electrical signals cause the plurality of particulates to attract towards each electrode exposed by the plurality of windows (25).
11. The method of claim 10, wherein the method sorts the particulates by size, shape, density, conductivity, material composition, or permeability.
12. The method of claim 11, wherein the particulates are guided to each electrode by a combination of electroosmosis and dielectrophoresis.
13. The method of claim 10, wherein the particulates are microparticulates, nanoparticulates, or a combination thereof.
14. The method of claim 10, wherein the particulates are organic particulates, non-organic particulates, metallic particulates, or a combination thereof.
15. The method of claim 10, wherein the electrical signals are applied by a function generator (30).
16. The method of claim 10, wherein the method further comprises entrapping the plurality of particulates attracted to each electrode via electropolymerization.
17. The method of claim 10, wherein the electropolymerization comprises: a. providing a polymerization solution; b. mixing the polymerization solution with a particulate suspension; c. depositing the polymerization solution and the particulate suspension over each electrode; d. covering each electrode; and e. applying a non-uniform DC offset to each electrode (100) to entrap the plurality of particulates in place.
18. The method of claim 17, wherein the polymerization solution comprises an electropolymerization monomer and an ionic surfactant.
Description
BRIEF DESCRIPTION OF THE SEVERAL VIEWS OF THE DRAWINGS
(1) The patent application or application file contains at least one drawing executed in color. Copies of this patent or patent application publication with color drawings will be provided by the Office upon request and payment of the necessary fee.
(2) The features and advantages of the present invention will become apparent from a consideration of the following detailed description presented in connection with the accompanying drawings in which:
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DETAILED DESCRIPTION OF THE INVENTION
(13) Following is a list of elements corresponding to a particular element referred to herein: 10 conductive substrate 20 layer of photosensitive polymer 25 windows 30 function generator 100 electrode
(14) As used herein, the term electroosmosis (EO) refers to the motion of liquid containing the dissolved ions induced by an applied potential across a porous material, capillary tube, membrane, microchannel, or any other fluid conduit. The frequency range within which EO is active is typically between 1 and 10,000 Hz.
(15) As used herein, the term dielectrophoresis (DEP) refers to a phenomenon in which a force is exerted on a dielectric particle when it is subjected to a non-uniform electric field. This force does not require the particle to be charged. All particles exhibit dielectrophoretic activity in the presence of electric fields. However, the strength of the force depends strongly on the medium and particles' electrical properties, on the particles' shape and size, as well as on the frequency of the electric field. Consequently, fields of a particular frequency can manipulate particles with great selectivity. The frequency range for negative DEP and positive DEP highly depends on the nature of the particle and the media. It is typical for polystyrene particles suspended in deionized water to experience positive DEP and lower frequencies than negative DEP.
(16) As used herein, the term “function generator” refers to a piece of electronic test equipment or software used to generate different types of electrical waveforms over a wide range of frequencies. Non-limiting examples of electrical waveforms include sine waves, square waves, triangular waves, or sawtooth waves. The waveforms may be repetitive or single-shot.
(17) Referring now to
(18) In some embodiments, the function generator (30) is configured to apply an AC signal to the conductive substrate (10). Applying an AC signal to the conductive substrate (10) may cause the plurality of particulates in the solution to move and attach to the conductive substrate (10) through the plurality of windows (25) in the layer of photosensitive polymer (20). In some embodiments, the AC signal is configured to cause electroosmosis or dielectrophoresis. In other embodiments, the system is configured to use a combination of electroosmosis and dielectrophoresis to guide the plurality of particles to the conductive substrate.
(19) Non-limiting examples of the conductive substrate (10) include regions of doped silicon wafer, layers of polysilicon, traces of gold, silver, or copper, and a layer of pyrolyzed carbon. Examples of the photosensitive polymer (20) include, but are not limited to, SU-8 photoresist, Shipley or AZ resist lines and others, dry resin, or any non-conductive layer such as cardboard or tape with windows cut in these layers could be utilized. In other embodiments, the solution may comprise organic, non-organic, metallic particulates, or a combination thereof. In further embodiments, the particulates may be microparticulates, nanoparticulates, or a combination thereof. Non-limiting examples of the particulates include organic molecules, carbon nanotubes, cells, inorganic silicone chips, or polysilicone microparticles. In some embodiments, the solution may comprise carboxyl modified latex polystyrene beads in deionized water.
(20) In further embodiments, the system may combine particle assembly and sorting. The particulates whose physical properties such as electrical conductivity and permeability are affected by particle size and material composition will experience positive and negative DEP at different ranges of frequencies. Thus it is possible to select a specific frequency range when one type of particle will experience positive DEP, while another type of particle will experience negative DEP and therefore, only the particles experiencing the positive DEP will be assembled at the electrodes. In this embodiment, the plurality of particulates may be guided to the conductive substrate (10) using a combination of electroosmosis and dielectrophoresis. The combination of AC electroosmosis (EO) and dielectrophoretic (DEP) forces applied at certain frequencies may sort the particulates. As a non-limiting example, the particulates may settle in the aqueous solution to bring the particulates closer to the conductive substrate (10). EO may be used to bring all particulates in the aqueous solution closer to the conductive substrate (10). All of the particulates may be collected at the conductive substrate (10) using only EO. In other embodiments, most of the particulates may be collected at the conductive substrate (10) using EO, then by using negative DEP to collect the remaining particulates. In some embodiments, for larger particulates, negative DEP may be used to repel the particulates to a region of the conductive substrate (10), then positive DEP may be used to attract the particulates to the conductive substrate. In yet another embodiment, smaller particulates may be attracted to the conductive substrate (10) by using EO only. Examples of properties that may be used to sort the particulates include, but are not limited to, size, shape, density, material composition, permeability, or conductivity.
(21) As a non-limiting example, when 1 μm and 5 μm diameter polystyrene beads were used, at an applied frequency of 1 kHz, 1 micron beads were quickly gathered inside the wells under positive DEP conditions. However, when the identical conditions were used on 5 micron microbead suspension placed onto electrode arrays, most of the microbeads would not move towards the wells. Without wishing to limit the present invention to any theory or mechanism, the viscous drag for larger 5 micron beads may be significantly greater than that for smaller 1 micron beads, as seen from Stokes law describing the viscous drag that is experienced by spherical particles of radius moving through the media.
(22) Referring now to
(23) In some embodiments, the conductive substrate (10) may comprise a silicon wafer covered with a layer of thermal oxide. Other non-limiting examples of the conductive substrate (10) include regions of doped silicon wafer, layers of polysilicon, traces of gold, silver, or copper, and a layer of pyrolyzed carbon. Examples of the photosensitive polymer (20) include, but are not limited to, SU-8 photoresist, Shipley or AZ resist lines and others, dry resin, or any non-conductive layer such as cardboard or tape with windows cut in these layers could be utilized. The method may further comprise soft baking the layer of photosensitive polymer (20) after spin-coating it onto the conductive substrate (10). The method may further comprise hard baking the conductive substrate (10) after soft baking the layer of photosensitive polymer (20). In some embodiments, the electrode (100) is connected to a function generator (30). The function generator (30) may be configured to generate electric signals to attract particulates in a solution to the conductive substrate (10) through the plurality of windows (25).
(24) Referring now to
(25) In some embodiments, the conductive substrate (10) may comprise a silicon wafer covered with a layer of thermal oxide. Other non-limiting examples of the conductive substrate (10) include regions of doped silicon wafer, layers of polysilicon, traces of gold, silver, or copper, and a layer of pyrolyzed carbon. Examples of the photosensitive polymer (20) include, but are not limited to, SU-8 photoresist, Shipley or AZ resist lines and others, dry resin, or any non-conductive layer such as cardboard or tape with windows cut in these layers could be utilized. In some embodiments, the solution may comprise carboxyl modified latex polystyrene beads in deionized water. In some embodiments, the electrical signals may be applied by a function generator (30).
(26) The electropolymerization may comprise providing a polymerization solution, mixing the solution with a particulate suspension, depositing the solution and the particulate suspension over the electrode, covering the electrode, and applying a DC offset to the electrode (100) to entrap the plurality of particulates in place. In some embodiments, the polymerization solution may comprise a polymerization monomer and an ionic surfactant. Examples of polymerization monomers include, but are not limited to, pyrrole or aniline. A non-limiting example of an ionic surfactant is NaDBS.
(27) The plurality of particulates may comprise organic particulates, non-organic particulates, and metallic particulates. In other embodiments, the particulates may be microparticulates, nanoparticulates, or a combination thereof. In some embodiments, the method may sort the particulates by a certain property of the particulates. Examples of properties that may be used to sort the particulates include, but are not limited to, size, shape, density, material composition, permeability, or conductivity. In preferred embodiments, the particulates are guided to the conductive substrate (10) by a combination of electroosmosis and dielectrophoresis.
(28) Assembly of particulates from constitutive parts presently relies on slow serial steps of direct assembly such as pick-and-place operations. The guided non-contact assembly of microparticulates achieved through Template Electrokinetic Assembly (TEA) described in this work presents a promising alternative to serial assembly process. This work studies an electrokinetic dielectrophoretic and electroosmotic assembly of polymer microparticulates onto specific locations on glassy carbon interdigitated electrode arrays (IDEAs). The IDEAs are coated with a layer of lithographically patterned resist. When the AC electric field is applied to the IDEA, the microparticulates suspended in an aqueous solution above the electrodes are attracted to the open regions of the electrodes not covered by the photoresist. The combination of AC electroosmosis and dielectrophoretic forces guide 1 μm and 5 μm diameter microparticulates to assemble in wells opened in the photoresist atop the electrodes. Permanent entrapment of the microparticulates is demonstrated via the electropolymerization process of the conducting polymer polypyrrole.
EXAMPLE
(29) The following is a non-limiting example of the present invention. It is to be understood that said example is not intended to limit the present invention in any way. Equivalents or substitutes are within the scope of the present invention.
(30) The goal of the Template Electrokinetic Assembly (TEA) process under study is to collect 1 micron and 5 micron polystyrene microbeads into specific locations, so-called “wells,” the windows opened in the photoresist layer on top of microelectrodes as seen in
(31) To minimize the drag experienced by the 5 micron particles during the micro-assembly, a two-step process is implemented. In the first step, negative DEP is applied to the beads using 1 MHz applied frequency and 4 Vpp (peak-to-peak). Under these conditions, the initially homogeneous suspension of 5 m particles is forced into three areas: the trenches between the electrodes, the gaps between the wells (i.e. windows opened in the photoresist), and the centers of the wells as seen in
(32) Once the nDEP step was performed, the frequency was lowered to 1 kHz where the beads experience a positive DEP. At this point, the 5 micron particles located in the trenches and gaps moved towards the edges of the electrodes and were subsequently pulled into the centers of the wells, joining the cluster of particles initially located there, as the sequence of pictures in
(33) The formation of the initial nDEP pattern of 5 micron beads can be explained by the fact that the electric field lines are concentrated around dielectrics and insulators in a process called insulator DEP (iDEP). Therefore, strong negative DEP forces will be produced around the photoresist edges that cover the electrodes. Some 5 micron beads will settle to the bottom of the electrode chip, including into the wells. Once nDEP is applied, the beads already located inside the wells will be pushed together into the center of each well away from the well sides, while beads between the wells (on top of the resist) will be pushed away by this nDEP force forming the lines in the gaps between wells, and similarly the beads will be pushed away from the resist-covered edges of the electrodes, forming the lines in the trenches between the electrodes as seen in
(34) When the applied frequency is lowered to 1 kHz and the microbeads start to experience positive DEP, the edges of the resist and the growing clusters of microbeads inside the wells serve as the points of the highest electric field gradient and subsequently as the areas of microbead assembly. From the sequence of pictures in
(35) For 1 micron beads, the DEP force is too weak due to the beads' small size to be comparable to the ACEO flow, and consequently the beads can act as tracers to reveal the nature of the ACEO flow. It has been proven in other works that electroosmosis-driven vortices are induced at the edges of coplanar bar electrodes as well as over the surface of the electrodes. For the patterned electrodes, these EO vortices are generated above the wells at frequencies of 10 kHz and lower where EO is strong.
(36) 1 micron beads influenced by electroosmotic flow will fill the windows if the applied frequency is below 10 kHz. Meanwhile, 5 micron beads under that range of frequencies will aggregate at the edges of the windows under the influence of the positive iDEP forces, rather than in the windows since larger beads are more inertial and less influenced by the flow streamlines and more influenced by DEP forces that depend on the cube of particle radius.
(37) Thus, in order to fill the windows in the resist with 5 micron beads, deposit the bead suspension, wait several minutes for gravitational sedimentation to take place and then apply 1 MHz frequency to utilize negative DEP (
(38) An alternative strategy exists for attracting 5 micron beads into the windows if a homogeneous suspension of beads is used and gravitational sedimentation isn't utilized. Adding 1 micron beads to the suspension of 5 micron beads and applying 1 kHz frequency, causes the 1 micron beads to start filling the windows under the influence of ACEO. The clusters of these 1 micron beads serve as areas of the high electric field and will cause positive DEP for 5 micron beads.
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(40) The guided electrokinetic microassembly of polystyrene microparticles onto specific locations of patterned carbon microelectrodes was presented. The assembly sequence is divided into two steps: guided deposition of microparticles, followed by their permanent entrapment via electropolymerization of the conductive polymer, polypyrrole. Experimental evidence and numerical simulations presented demonstrate the process of the guided assembly of microparticles under the combined influence of dielectrophoretic and electroosmotic forces. The demonstrated guided electrokinetic assembly technique has the potential to be utilized for massively parallel micro-assembly processes for devices employed in a wide range of fields from biotechnology to micro- and nano-electronics and with microparts to be assembled made out of a variety of materials such as organic matter, dielectric, insulators, or metals.
(41) Although there has been shown and described the preferred embodiment of the present invention, it will be readily apparent to those skilled in the art that modifications may be made thereto which do not exceed the scope of the appended claims. Therefore, the scope of the invention is only to be limited by the following claims. In some embodiments, the figures presented in this patent application are drawn to scale, including the angles, ratios of dimensions, etc. In some embodiments, the figures are representative only and the claims are not limited by the dimensions of the figures. In some embodiments, descriptions of the inventions described herein using the phrase “comprising” includes embodiments that could be described as “consisting essentially of” or “consisting of”, and as such the written description requirement for claiming one or more embodiments of the present invention using the phrase “consisting essentially of” or “consisting of” is met.
(42) The reference numbers recited in the below claims are solely for ease of examination of this patent application, and are exemplary, and are not intended in any way to limit the scope of the claims to the particular features having the corresponding reference numbers in the drawings.