TW202234962A - Manufacturing circuit board circuit structure with through hole and circuit board circuit structure with through hole manufactured thereof - Google Patents

Abstract

A manufacturing method of circuit board circuit structure with through hole includes providing a substrate. The substrate includes a substrate layer and a copper layer. The substrate layer has opposite first and second surfaces. Each copper layer is formed on the first surface and the second surface of the substrate layer; cover the two photoresist layers on the surface of the two copper layers, and through exposure, make each photoresist layer chemical resistant; drill holes from the surface of the photoresist layer on one side of the first surface to form holes, which lead to the second surface of the substrate layer; a metallized layer is formed by chemical method, which covers the surface of the hole and the surface of the photoresist layer on one side of the first surface; a copper clad layer is formed by electroplating, which covers the surface of the hole and extends to the surface of the photoresist layer on one side of the first surface; removal of the copper-clad layer exceeding the height of the copper layer by etching; and the two photoresist layers are removed to complete the subsequent circuit pattern.

Description

Manufacturing method of circuit board circuit structure with via holes and circuit board circuit structure with via holes

A method for manufacturing a circuit board with via holes, in particular a method for fabricating a circuit board structure and the manufactured circuit board structure with via holes.

The traditional method of plating selection is to perform metallization after drilling and hole cleaning, and then use dry film masking, exposure and development to expose the metallized holes, and then perform electroplating. Because both the drilling process and the exposure process exist The problem of process tolerance, so in the dry film opening process, the hole must be drilled according to the position of the drill hole, and a device with automatic alignment (CCD exposure machine or digital direct drawing exposure machine) must be used, and due to the progressive tolerance problem. The size of the hole must be enlarged, and a protrusion is formed around the hole after electroplating. During circuit fabrication, in order to effectively cover the protruding portion, the selected thickness of the photoresist cannot be thinned, which results in limited resolution and etching molding, and affects the fabrication of thin circuits in the circuit structure of the circuit board.

In view of this, according to an embodiment, a method for fabricating a circuit board circuit structure with a via hole is provided, which includes providing a substrate, the substrate includes a base material layer and a copper layer, the base material layer has opposite first and second surfaces, and each copper layer forming on the first surface and the second surface of the base material layer; covering the two first photoresist layers on the surfaces of the two copper layers, and making each first photoresist layer have chemical resistance through full exposure; The surface of the first photoresist layer on one side is drilled to form holes, and the holes are connected to the second surface of the substrate layer; a metallization layer is formed by chemical means, and the metallization layer covers the surface of the holes and is located on the first surface. The surface of the first photoresist layer on one side; a copper clad layer is formed by electroplating, and the copper clad layer covers the surface of the hole and extends to the surface of the first photoresist layer on one side of the first surface; through chemical etching removing part of the copper clad layer exceeding the height of the copper layer; removing two first photoresist layers; covering two second photoresist layers on the surfaces of the two copper layers, and exposing and developing the two second photoresist layers to form circuit patterns structure; performing an etching process to remove the surface of each copper layer not covered by each second photoresist layer; and removing two second photoresist layers.

In some embodiments, at least one hole penetrates the substrate.

In some embodiments, the photoresist layer is a dry film photoresist.

In some embodiments, the holes are formed by laser drilling.

In some embodiments, the metallization layer is formed through a neutral or weakly acidic metallization system.

In some embodiments, the two first photoresist layers include thin films, and the thin films are removed after the two first photoresist layers are fully exposed.

In some embodiments, the two first photoresist layers comprise thin films, and the thin films are removed after drilling holes on the surface of the first photoresist layers on one side of the first surface.

In some embodiments, the hole has a recess surrounding the opening of the hole.

In some embodiments, the copper clad layer extends along the recess to cover the exposed surface of the copper layer on one side of the first surface.

In addition, according to an embodiment, a circuit board circuit structure with via holes is provided, which is a circuit board circuit structure manufactured by the manufacturing methods of the above-mentioned embodiments.

In summary, the metallization and electroplating range is increased by the first photoresist layer. During the electroplating process, the copper clad layer extends to the surface of the first photoresist layer, and then the excess of the first photoresist layer is removed together. The copper clad layer within the height range of the layer and the removal of the first photoresist layer make the height of the electroplating layer and the copper layer roughly the same, which avoids the problem that the electroplating layer overflows the hole and forms a protrusion around the hole when the hole is electroplated.

Please refer to FIGS. 1 to 7b and 12 first. FIGS. 1 to 7b are schematic structural diagrams (1) to (9) of a method for fabricating a circuit board circuit structure with vias according to an embodiment of the present invention, and FIG. 12 is a A flowchart (1) of a method for fabricating a circuit board circuit structure with vias according to an embodiment of the present invention. As shown in FIG. 1 and FIG. 12 , the manufacturing method of the circuit board circuit structure 100 with via holes in this embodiment includes providing a substrate 10 (step S10 ). The substrate 10 includes a substrate layer 11 and two copper layers 12 . The substrate layer 11 has a first surface 111 and a second surface 112 opposite to each other, and two copper layers 12 are respectively formed on the first surface 111 and the second surface 112 of the base material layer 11 . That is, the first surface 111 and the second surface 112 of the substrate layer 11 can be used to manufacture the circuit board structure 100 of the same or different specifications at the same time, or only one side surface can be used to manufacture the circuit board structure 100 . In this embodiment, the circuit board circuit structure 100 is fabricated on a single side surface as an example, but not limited thereto.

As shown in FIG. 2 and FIG. 12 , the surfaces of the two first photoresist layers 13 are covered on the two copper layers 12 , and the first photoresist layers 13 have chemical resistance through full exposure (step S11 ); wherein, the covering The first photoresist layer 13 is fully exposed by using the existing process, such as applied to the circuit board photolithography process, forming a photoresist layer by laminating a dry film photoresist or forming a photoresist layer by coating a wet film photoresist. In this embodiment, taking the dry film photoresist as an example, the photoresist is formed into a state of chemical resistance by means of full exposure.

As shown in FIG. 3 and FIG. 12 , for the convenience of the subsequent description, the first photoresist layer on the side of the first surface 111 is represented by the first photoresist layer 13 a, and the first photoresist layer on the side of the second surface 112 is represented by the first photoresist layer 13 a. The first photoresist layer 13b is illustrated. The copper layer formed on the side of the first surface 111 is represented by the copper layer 12a, and the copper layer on the side of the second surface 112 is represented by the copper layer 12b. Drilling is performed from the surface of the first photoresist layer 13 a on one side of the first surface 111 (step S12 ) to form holes 20 , and the holes 20 are connected to the second surface 112 of the substrate layer 11 . In this embodiment, the hole 20 is formed by means of laser drilling. Here, two holes 20 are taken as an example, but not limited thereto. The holes 20 are formed from the first photoresist layer 13a on one side of the first surface 111 to the copper layer 12b on one side of the second surface 112 through the first photoresist layer 13a, the copper layer 12a and the base material layer 11 in sequence. pilot hole. The hole 20 includes a hole wall 21 and a hole bottom 22 , and the hole wall 21 includes the side surfaces of the first photoresist layer 13 a , the copper layer 12 a and the base material layer 11 exposed by drilling. The hole bottom 22 includes the surface of the copper layer 12b that is bonded to the second surface 112 .

As shown in FIG. 4 and FIG. 12 , the metallization layer 14 is chemically formed (step S13 ). The metallization layer 14 covers the surface of the hole 20 and the surfaces of the two first photoresist layers 13 . In this embodiment, the photoresist layer is formed by using dry film photoresist. Traditional dry film photoresist, such as metallization system in contact with alkali, will cause the structure of dry film photoresist to be damaged or even fall off. For example, the metallization layer 14 is formed by a neutral or weakly acidic metallization system. In this embodiment, the surfaces of the holes 20 and the surfaces of the two first photoresist layers 13 are formed and covered by a chemically neutral or weakly acidic metallization system. That is to say, the metallization layer 14 covers the surface of the first photoresist layer 13 a on one side of the first surface 111 and the surface of the first photoresist layer 13 b on one side of the second surface 112 . Generally speaking, the coverage of the metallization layer 14 does not include parts of metal materials, such as the side surface of the copper layer 12a exposed by the drilling and the surface of the copper layer 12b exposed by the drilling.

As shown in FIG. 5 and FIG. 12 , after the metallization layer 14 is formed, a copper clad layer 15 is formed by electroplating (step S14 ). The copper clad layer 15 covers the surface of the hole 20 and extends to the first surface 111 on one side A surface of the photoresist layer 13a. In this embodiment, the surfaces of the holes 20 , ie the side surfaces of the first photoresist layer 13 a , the copper layer 12 a and the base material layer 11 exposed by drilling are formed and covered by electroplating. In addition, in this embodiment, because of the copper layer 12b on the side of the second surface 112, the copper clad layer 15 is extended to the surface of the first photoresist layer 13a on the side of the first surface 111.

As shown in FIG. 6 and FIG. 12 , after the electroplating is completed, the copper clad layer 15 that exceeds the height of the copper layer 12 a on one side of the first surface 111 is removed by chemical etching (step S15 ). For example, in this embodiment, in order to make the heights of the copper clad layer 15 and the copper layer 12a approximately equal, the copper clad layer 15 that exceeds the copper layer 12a on one side of the first surface 111 is removed by chemical etching, The height of the copper clad layer 15 is higher than that of the copper layer 12a and lower than that of the first photoresist layer 13a. As shown in FIG. 7 and FIG. 12 , after the chemical etching is completed, the two first photoresist layers 13 are removed (step S16 ), and the patterning of subsequent lines is continued. 7a, 7b and 12, the two second photoresist layers 16 are covered on the surfaces of the two copper layers 12, and through exposure and development, the two second photoresist layers 16 are formed into a circuit pattern structure 161 (step S17). An etching process is performed to remove the surfaces of the copper layers 12 not covered by the second photoresist layers 16 (step S18 ). Next, the two second photoresist layers 16 are removed (step S19 ) to complete the circuit board structure 100 .

Specifically, the metallization and electroplating range is increased by the two first photoresist layers 13. During the electroplating process, the copper clad layer 15 extends to the surface of the first photoresist layer 13a, and then removes more than the first photoresist layer 13a. A copper clad layer 15 within the height range of the photoresist layer 13a and the two first photoresist layers 13 are removed so that the heights of the copper clad layer 15 and the copper layer 12a are approximately the same, so as to prevent the electroplating layer from overflowing the holes and surrounding the holes during electroplating The problem of forming the bulge.

In addition, please refer to Fig. 2a, Fig. 12a and Fig. 12b. FIG. 2a is a schematic diagram of a thin film of a circuit board circuit structure with via holes according to an embodiment. FIG. 12a is a flowchart (2) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. FIG. 12b is a flowchart (3) of a method for fabricating a circuit board structure with vias according to an embodiment. Generally speaking, there is a layer of optical grade polyethylene terephthalate (PET) film on the surface of the dry film, which can protect the dry film from contact with air and react. The PET film will be removed. As shown in FIG. 12a, in this embodiment, the substrate 10 is fully exposed but not developed, so the substrate 10 is covering the surfaces of the two first photoresist layers 13 and the two copper layers 12, and through the overall exposure, the first photoresist layers 13 are After the photoresist layer 13 has chemical resistance (step S11 ), the polyethylene terephthalate film 131 is removed (step S11 ′), and then the first photoresist layer 13 a on one side of the first surface 111 is removed from the first photoresist layer 13 a Drilling is performed on the surface (step S12 ), but not limited thereto. As shown in FIG. 12b , in another embodiment, the substrate 10 covers the surfaces of the two first photoresist layers 13 on the two copper layers 12 and exposes the surface of the two first photoresist layers 13 to make the first photoresist layers 13 have chemical resistance. After (step S11 ), drilling is performed from the polyethylene terephthalate film 131 on the surface of the first photoresist layer 13 a on one side of the first surface 111 (step S12 a ), and then the polyethylene terephthalate is removed Glycol film 131 (step S12a'). In yet another embodiment, taking the wet film photoresist as an example, since the wet film photoresist does not have a PET film, the action of removing the PET film is not required.

In addition, in this embodiment, the circuit board structure 100 is suitable for, for example, an initial inner board of a double-sided or multi-layered board. Here, a double-sided board with one substrate layer 11 and two copper layers 12 is used as an example. Specifically, in this embodiment, a neutral or weakly acidic metallization system is used for metallization. For example, neutral or weakly acidic metallization is performed, and the bottom layer of the substrate needs to be fully conductive. layer stacking. When making the outer board of the multilayer board, the bottom layer of the inner board cannot be fully conductive because the inner board has been fabricated. Therefore, the circuit board circuit structure 100 of this embodiment is suitable for, for example, the inner board of a double-sided or multi-layer board. In this embodiment, the base material layer 11 may be any pure metal material or composite metal material.

See Figure 8. FIG. 8 is a schematic structural diagram (1) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. In another embodiment, the hole 20 has a concave portion 201 , and the concave portion 201 surrounds the opening of the hole 20 . For example, during the laser processing, the first photoresist layer 13a may shrink inward due to the thermal effect of laser processing, or the aperture of the first photoresist layer 13a may be deliberately made larger than the aperture of the hole 20. At this time, the copper A stepped structure is formed between the layer 12a and the first photoresist layer 13a. See Figure 9. FIG. 9 is a schematic structural diagram (2) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. After the metallization layer 14 is formed, the copper clad layer 15 is formed by electroplating (step S14 ). The copper clad layer 15 covers the surface of the hole 20, that is, the side surfaces of the first photoresist layer 13a, the copper layer 12a and the base material layer 11 exposed due to drilling, and also covers the first photoresist layer 13a due to laser processing. The surface of the copper layer 12a which is retracted and exposed. After the electroplating is completed, the copper clad layer 15 that exceeds the copper layer 12a on one side of the first surface 111 is removed by chemical etching, so that the height of the copper clad layer 15 is higher than that of the copper layer 12a and lower than the height of the first photoresist layer 13a (step S15). As shown in FIG. 9 , the copper clad layer 15 forms ears around the opening of the hole 20 , which increases the contact area between the copper clad layer 15 and the copper layer 12 a and enhances the reliability performance.

Please refer to FIG. 10 , FIG. 10 a and FIG. 11 . FIG. 10 is a schematic structural diagram (1) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. FIG. 10a is a schematic structural diagram (2) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. FIG. 11 is a schematic structural diagram (3) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. In yet another embodiment, at least one hole 30 penetrates the substrate 10 to form a through hole. Parts that are the same as those in the above-mentioned embodiments will not be repeated, and only some differences will be described. As shown in FIG. 10 , the holes 30 are formed by laser drilling, and the holes 30 pass through the first photoresist layer 13 a on one side of the first surface 111 to the first photoresist layer 13 b on one side of the second surface 112 in sequence. The first photoresist layer 13a, the copper layer 12a, the base material layer 11, the copper layer 12b, and the first photoresist layer 13b are formed. The hole 30 includes a hole wall 31, and the hole wall 31 includes the first photoresist layer 13a, the copper layer 12a, the substrate layer 11, the copper layer 12b and the side surfaces of the first photoresist layer 13b exposed by drilling. The metallization layer 14 covers the surface of the hole 30 , the surface of the first photoresist layer 13 a on one side of the first surface 111 and the surface of the first photoresist layer 13 b on one side of the second surface 112 . Generally speaking, the coverage of the metallization layer 14 does not include the part of the metal material, such as the side surface of the copper layer 12a exposed by the drilling and the side surface of the copper layer 12b exposed by the drilling. As shown in FIG. 10 a , in the electroplating stage, the copper clad layer 15 covers the surface of the hole 30 and extends to the surface of the first photoresist layer 13 a on one side of the first surface 111 and the first photoresist layer 13 a on one side of the second surface 112 the surface of the photoresist layer 13b. 11 , the copper clad layer 15 that partially exceeds the height of the copper layer 12 a located on one side of the first surface 111 and the copper clad layer 15 that partially exceeds the height of the copper layer 12 b located on one side of the second surface 112 are removed by chemical etching. Copper layer 15 . After the first photoresist layer 13 is removed, the substrate 10 with through holes as shown in FIG. 11 is completed.

To sum up, according to an embodiment of a method for fabricating a circuit board structure with via holes, the metallization and electroplating range is increased by the two first photoresist layers 13. During the electroplating process, the copper clad layer is 15 extends to the surface of the first photoresist layer 13a, then the copper clad layer 15 exceeding the height range of the first photoresist layer 13a and the two first photoresist layers 13 are removed together, so that the copper clad layer 15 and the copper layer 12a are removed together The heights are approximately the same, which prevents the electroplating layer from overflowing the holes and forming protrusions around the holes when the holes are plated, which affects the fabrication of the circuit board structure 100 . The circuit board circuit structure 100 with via holes completed by the method of one embodiment of the present application includes a base material layer 11 , two copper layers 12 and a copper clad layer 15 . The copper clad layer 15 covers the hole 20 and is at the opening of the hole 20 There are relatively flat copper clad layers 15 around, so that the overall surface of the substrate 10 is flatter. In addition, the circuit board circuit structure 100 with via holes completed by the method of another embodiment of the present application includes a substrate layer 11 , two copper layers 12 and a copper clad layer 15 , the copper clad layer 15 covers the hole 20 , and the copper clad layer 15 extends to the opening of the hole 20, and forms ears around the opening of the hole 20. The concave part 201 of the hole 20 increases the contact area between the copper clad layer 15 and the copper layer 12a, and enhances the performance of reliability.

Although the technical content of this case has been disclosed above with preferred embodiments, it is not intended to limit this case. Anyone who is familiar with this technique, any changes and modifications made without departing from the spirit of this case should be covered within the scope of this case. Therefore, the scope of protection in this case should be determined by the scope of the appended patent application.

100: Circuit board structure 10: Substrate 11: Substrate layer 111: First surface 112: Second Surface 12: Copper layer 12a: Copper layer 12b: Copper layer 13: The first photoresist layer 13a: first photoresist layer 13b: first photoresist layer 131: polyethylene terephthalate film 14: Metallization layer 15: Copper Clad Layer 16: Second photoresist layer 161: Circuit pattern structure 20: Holes 201: Recess 21: Hole Wall 22: Bottom of the hole 30: Holes 31: Hole Wall Step S10: providing a substrate Step S11: Covering the surfaces of the two first photoresist layers on the two copper layers, and exposing the entire surface to make the first photoresist layers have chemical resistance Step S11': remove polyethylene terephthalate film Step S12: Drill holes from the surface of the first photoresist layer on one side of the first surface Step S12a: Drill holes from the polyethylene terephthalate film on the surface of the first photoresist layer on one side of the first surface Step S12a': remove polyethylene terephthalate film Step S13: chemically forming a metallization layer Step S14: forming a copper clad layer through electroplating Step S15: removing part of the copper clad layer that exceeds the height of the copper layer on one side of the first surface by chemical etching Step S16: removing two first photoresist layers Step S17: Covering the surfaces of the two second photoresist layers on the two copper layers, and exposing and developing the two second photoresist layers to form a circuit pattern structure Step S18: performing an etching process to remove the surfaces of the copper layers not covered by the second photoresist layers Step S19: removing two second photoresist layers

[FIG. 1] is a schematic structural diagram (1) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. FIG. 2 is a schematic structural diagram (2) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. [ FIG. 2 a ] is a schematic diagram of a thin film of a circuit board circuit structure with via holes according to an embodiment. [FIG. 3] is a schematic structural diagram (3) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. FIG. 4 is a schematic structural diagram (4) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. FIG. 5 is a schematic structural diagram (5) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. FIG. 6 is a schematic structural diagram (6) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. FIG. 7 is a schematic structural diagram (7) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. 7a is a schematic structural diagram (8) of a method for fabricating a circuit board circuit structure with via holes according to an embodiment. [FIG. 7b] is a schematic structural diagram (9) of a method for fabricating a circuit board circuit structure with vias according to an embodiment. 8 is a schematic structural diagram (1) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. FIG. 9 is a schematic structural diagram (2) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. FIG. 10 is a schematic structural diagram (1) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. [FIG. 10a] is a schematic structural diagram (2) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. FIG. 11 is a schematic structural diagram (3) of a method for fabricating a circuit board circuit structure with via holes according to another embodiment. FIG. 12 is a flowchart (1) of a method for fabricating a circuit board structure with vias according to an embodiment. [ FIG. 12 a ] is a flowchart (2) of a method for fabricating a circuit board circuit structure with vias according to an embodiment. [FIG. 12b] is a flowchart (3) of a method for fabricating a circuit board circuit structure with vias according to an embodiment.

Step S10: providing a substrate

Step S11: Covering the surfaces of the two first photoresist layers on the two copper layers, and exposing the entire surface to make the first photoresist layers have chemical resistance

Step S12: Drill holes from the surface of the first photoresist layer on one side of the first surface

Step S13: chemically forming a metallization layer

Step S14: forming a copper clad layer through electroplating

Step S15: removing part of the copper clad layer that exceeds the height of the copper layer on one side of the first surface by chemical etching

Step S16: removing two first photoresist layers

Step S17: Covering the surfaces of the two second photoresist layers on the two copper layers, and exposing and developing the two second photoresist layers to form a circuit pattern structure

Step S18: performing an etching process to remove the surfaces of the copper layers not covered by the second photoresist layers

Step S19: removing two second photoresist layers

Claims (10)

A method for fabricating a circuit board circuit structure with a via hole, comprising: A substrate is provided, the substrate includes a base material layer and two copper layers, the base material layer has a first surface and a second surface opposite to each other, and each of the copper layers is formed on the first surface and the second surface of the base material layer second surface; Covering two first photoresist layers on the surfaces of the two copper layers, and exposing the entire surface to make each of the first photoresist layers have chemical resistance; Drilling is performed from the surface of the first photoresist layer on one side of the first surface to form at least one hole, and the at least one hole is connected to the second surface of the base material layer; forming a metallization layer by chemical means, and the metallization layer covers the surface of the at least one hole and the surface of the two first photoresist layers; forming a copper clad layer through electroplating, the copper clad layer covering the surface of the at least one hole and extending to the surface of the first photoresist layer on one side of the first surface; removing part of the copper clad layer exceeding the height of the copper layer by chemical etching; removing the two first photoresist layers; Covering two second photoresist layers on the surfaces of the two copper layers, and through exposure and development, the two second photoresist layers form a circuit pattern structure; performing an etching process to remove the surface of each of the copper layers not covered by each of the second photoresist layers; and The two second photoresist layers are removed. The method for fabricating a circuit board circuit structure with vias as claimed in claim 1, wherein the at least one hole penetrates the substrate. The method for fabricating a circuit board circuit structure with via holes according to claim 1, wherein the first photoresist layer and the second photoresist layer are dry film photoresist. The method for fabricating a circuit board circuit structure with via holes as claimed in claim 1, wherein the at least one hole is formed by a laser drilling method. The method for fabricating a circuit board circuit structure with via holes as claimed in claim 1, wherein the metallization layer is formed through a neutral or weakly acidic metallization system. The method for fabricating a circuit board circuit structure with via holes according to claim 3, wherein the two first photoresist layers comprise a thin film, and the thin film is removed after the two first photoresist layers are fully exposed. The method for fabricating a circuit board circuit structure with via holes as claimed in claim 3, wherein the two first photoresist layers comprise a thin film, and after drilling the surface of the first photoresist layer on one side of the first surface , remove the film. The method for fabricating a circuit board circuit structure with via holes as claimed in claim 1, wherein the at least one hole has a concave portion, and the concave portion surrounds the opening of the at least one hole. The method for fabricating a circuit board circuit structure with via holes as claimed in claim 8, wherein the copper clad layer extends along the concave portion to cover the exposed surface of the copper layer on one side of the first surface direction. A circuit board circuit structure manufactured by the method for manufacturing a circuit board circuit structure with vias according to any one of claims 1 to 9.

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