WO2020256012A1 - Pilier conducteur - Google Patents

Pilier conducteur Download PDF

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Publication number
WO2020256012A1
WO2020256012A1 PCT/JP2020/023752 JP2020023752W WO2020256012A1 WO 2020256012 A1 WO2020256012 A1 WO 2020256012A1 JP 2020023752 W JP2020023752 W JP 2020023752W WO 2020256012 A1 WO2020256012 A1 WO 2020256012A1
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WIPO (PCT)
Prior art keywords
pillar
conductive pillar
pillars
fine particles
acid
Prior art date
Application number
PCT/JP2020/023752
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English (en)
Japanese (ja)
Inventor
亮太 山口
真 矢田
Original Assignee
Dic株式会社
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Publication date
Application filed by Dic株式会社 filed Critical Dic株式会社
Priority to JP2021526839A priority Critical patent/JP7243827B2/ja
Publication of WO2020256012A1 publication Critical patent/WO2020256012A1/fr

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    • H01L24/16—Structure, shape, material or disposition of the bump connectors after the connecting process of an individual bump connector
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L24/00—Arrangements for connecting or disconnecting semiconductor or solid-state bodies; Methods or apparatus related thereto
    • H01L24/80—Methods for connecting semiconductor or other solid state bodies using means for bonding being attached to, or being formed on, the surface to be connected
    • H01L24/81—Methods for connecting semiconductor or other solid state bodies using means for bonding being attached to, or being formed on, the surface to be connected using a bump connector
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/30—Technical effects
    • H01L2924/35—Mechanical effects
    • H01L2924/351—Thermal stress
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/30—Technical effects
    • H01L2924/35—Mechanical effects
    • H01L2924/351—Thermal stress
    • H01L2924/3512—Cracking

Definitions

  • the present invention relates to a conductive pillar (Pillar), which is a flip chip mounting terminal that is a connection method between a semiconductor chip and a package interposer in a semiconductor package.
  • the present invention is a pillar produced by sintering a paste containing metal fine particles, and is a conductive pillar having a bonding layer.
  • a semiconductor device is manufactured by manufacturing an electronic circuit on a semiconductor chip and connecting an electrode on the semiconductor chip and an electrode on a semiconductor package.
  • an electrode on a semiconductor chip and an electrode on a semiconductor package have been electrically connected by using a bonding wire made of gold or copper.
  • the flip chip method is used as an electrical connection method between a semiconductor chip and a semiconductor package.
  • Gold bumps and solder bumps are known as typical connection methods in the flip chip method.
  • the flip chip mounting method which is attracting attention as a high-density mounting method, involves forming a large number of solder bumps on metal electrode pads arranged on a wafer or substrate, mounting a semiconductor chip on the electrode pads, and then heating the chips.
  • a method of melting solder bumps to perform chip bonding Patent Document 1.
  • solder bumps in the flip chip mounting method includes a method of forming bumps by electrolytic plating, a printing method such as a stencil mask method and a dry film method, a ball mounting method, a vapor deposition method, and an IMS (injection molded solder) method ( This is done by melting (reflowing) the solder supplied on the wafer or substrate according to Patent Documents 2, 3, 4) and the like. At this time, if the solvent contained in the solder is gasified at the time of melting and remains as voids in the bumps, the joint strength and the like are lowered. Therefore, solder bumps having few voids are required.
  • solder material When solder bump bonding is used, the solder material has problems such as inferior heat resistance, high volume resistivity as compared with copper and silver, and small current capacity. Copper pillar bumps are known as materials for solving these problems. Copper as a metal material used for copper pillars is also excellent in terms of heat resistance, low electrical resistance, high current capacity, high electromigration resistance, and the like (Patent Document 5).
  • the electrolytic plating method has a problem of undercutting when etching the seed layer.
  • the plating method has a high equipment installation cost and a large environmental load due to harmful waste liquid.
  • Patent Document 6 A method using metal particles and solder has been reported as a method for forming copper pillars without using the plating method.
  • Patent Document 6 does not describe in detail the particle size of the metal particles that can be used for the pillars and the composition of the conductive paste, and the effect that the present invention aims to achieve could not be obtained.
  • the plating method has a problem that it is necessary to recycle or dispose of a large amount of waste liquid, which has a large environmental load and costs for equipment maintenance.
  • Bulk copper pillars produced by a plating method or the like are three times or more larger than the elastic modulus of the solder material and eight times or more larger than the yield stress of the solder material. Therefore, the thermal stress generated when the chip and the substrate are joined. There was a problem that could not be sufficiently buffered. As a result, the chip is greatly affected by thermal stress, and cracks are likely to occur in the wiring layer that employs a dielectric constant interlayer insulating film with weak mechanical strength, resulting in a decrease in yield.
  • Document 6 discloses a method for producing a conductive pillar using metal particles as described above, but does not describe any composition of the conductive pillar, and what kind of composition is used as a raw material. It was unclear whether suitable conductivity and bonding strength could be obtained.
  • a conductive pillar using metal particles there is a problem that if the particle size of the metal particles is large, it is not possible to manufacture a fine conductive pillar.
  • a pillar (A) produced by sintering a paste containing metal fine particles having a particle size of less than 1 ⁇ m and a protective agent. And a conductive pillar (B) having a bonding layer.
  • the present invention relates to a conductive pillar used as a terminal for mounting a flip chip.
  • the conductive pillars By forming the conductive pillars on the electrode substrate using the paste according to the present invention, the conductive pillars have been made plating-less.
  • the undercut during etching which was a problem with the conventional method, has been solved, and fine copper pillars can be formed.
  • a conductive pillar By forming a conductive pillar on the electrode substrate using the paste according to the present invention, it was possible to produce a conductive pillar composed of metal fine particles and a bonding layer.
  • the obtained conductive pillars had the performance that the conductivity and the bonding strength could withstand the mounting.
  • the protective agent contained in the pillar (A) has at least one functional group among amino group, carbonyl group, thiol group, alkylthio group, alkenylthio group, thioether group and phosphoric acid group, and
  • the conductive pillar (B) according to (1) which is a compound having a molecular weight of 500 or more.
  • the bonding layer is an alloy containing tin, lead, silver, copper or one or more metals selected from these. Conductive pillars.
  • the present invention is a pillar made of metal fine particles and a conductive pillar having a bonding layer, which can be used for flip chip mounting.
  • a conductive pillar made of a paste containing metal fine particles and a protective agent is an opening portion of a resist layer in which the paste is pre-patterned with a squeegee or the like without using the plating technique which is a conventional technique in the manufacturing process. Pillars can be easily formed by filling the paste.
  • the undercut during etching which has been a problem due to the plating method, can be solved, and fine copper pillars can be formed.
  • the conductive pillar of the present invention can solve the problems of the conventional plating method.
  • the metal species that can be used as the metal fine particles of the present invention are those in which the functional groups in the protective agent described later can be physically or chemically adsorbed on the surface of the metal fine particles or chemically bonded (coordinated). If so, there is no particular limitation. However, from the viewpoint of the stability of the metal fine particles, one or more selected from gold, silver, copper and nickel can be preferably used. Particularly preferred are silver and copper.
  • the metal type may be one kind, or may be a mixture of two or more kinds or an alloy as long as it contains the metals listed above.
  • the average primary particle size of the metal fine particles is preferably less than 1 ⁇ m from the viewpoint of filling property and bondability. Further, when a conductive pillar is produced by utilizing the fusion function of fine particles without using a binder resin, it is more preferable to use metal fine particles having an average primary particle diameter of 100 nm or less. As a result, when the resist opening is filled with paste so that the resist opening is less than 100 ⁇ m to form a conductive pillar, the resist opening is densely filled with metal fine particles, and the electrode / pillar is sufficiently connected. It is possible to maintain the bonding strength and ensure the conductivity due to the contact or bonding between the metal fine particles.
  • the pillars When the pillars are formed by the fusion function of the metal, the pillars can be formed with or without the addition amount of the binder resin, and the pillars having excellent heat resistance can be formed.
  • the shape of the metal fine particles is not particularly limited, and spherical or flake-shaped fine particles can be used within a range that does not impair the effects of the present invention, but the average primary particle diameter calculated by the method for calculating the average primary particle diameter Is preferably less than 1 ⁇ m.
  • the average primary particle size can be calculated by observation with a transmission electron microscope (TEM). That is, in the present specification, the average primary particle diameter of the metal fine particles is calculated by taking a photograph of a sample with a transmission electron microscope (TEM) and analyzing the image.
  • TEM transmission electron microscope
  • the prepared metal fine particles are diluted with a good solvent to an arbitrary concentration, and the diluted solution is cast on a carbon film-coated grid and dried to obtain a sample for observation with a transmission electron microscope (TEM).
  • TEM transmission electron microscope
  • 200 fine particles are randomly extracted from the obtained TEM image, the area of each fine particle is obtained, and a value calculated based on the number of particle size when converted into a true sphere is adopted. From the randomly selected particles, those in which two particles overlap are excluded. When a large number of particles are in contact with each other or secondarily aggregated and aggregated, the particles constituting the aggregate are treated as independent particles.
  • each of the five particles constituting the aggregate is a target for calculating the average primary particle diameter of the metal fine particles.
  • the value before sintering is adopted as the average primary particle diameter. That is, the value before fusion occurs due to sintering is adopted.
  • the protective agent of the present invention is not particularly limited as long as it can protect the surface of the metal fine particles with the protective agent and has a functional group and / or a molecular structure having an affinity for the metal fine particles and the dispersion medium. Compounds having the following functional groups / molecular structures can be used.
  • the protective agent to be used can be used regardless of the size of the molecular weight, and high conductivity and dispersion stability can be imparted to the metal fine particles by designing the protective agent according to the metal type to be used and the desired physical properties. Is possible.
  • the characteristics of metal fine particles can be freely changed by selecting a protective agent according to various purposes.
  • a protective agent When a high molecular weight protective agent is used, various properties can be exhibited by changing the number and types of functional groups in the compound.
  • a low molecular weight protective agent When a low molecular weight protective agent is used, various properties can be exhibited by using two or more compounds in combination.
  • the functional group contained in the protective agent of the present invention include a thiol group, an alkylthio group, an alkenylthio group, a carboxy group, an amino group, a hydroxy group, a phosphoric acid group, a phosphoric acid ester group, a sulfonic acid group, and an aromatic group.
  • the family group is mentioned.
  • Dispersion stability can be added to the fine particles by using a protective agent having these functional groups.
  • a low molecular weight compound having a carboxyl group When a low molecular weight compound having a carboxyl group is used as the protective agent, the following substances can be used as specific examples.
  • a low molecular weight compound having an amino group When a low molecular weight compound having an amino group is used as the protective agent, the following substances can be used as specific examples.
  • any molecular structure having an affinity for the dispersion medium can be adopted as the selectable molecular structure.
  • the dispersion medium is a polar solvent such as alcohols or water
  • an organic compound containing a polyethylene oxide structure having 8 to 200 carbon atoms can be preferably used, and a polyethylene oxide structure having 8 to 100 carbon atoms can be preferably used.
  • the containing organic compound can be used more preferably. Since the polyethylene oxide moiety of the protective agent has excellent affinity with an alcohol solvent having a boiling point of 250 ° C. or lower, aggregation of metal fine particles can be strongly suppressed, and metal fine particles can be highly dispersed. As a result, the metal fine particles are packed at a high density, and voids are not generated due to the decomposition and removal of the protective agent and the solvent by the heat treatment, and the high density filling is possible.
  • metal fine particles composite of organic compound and metal fine particles
  • organic compound containing a polyethylene oxide structure having 8 to 200 carbon atoms used in the present invention
  • Japanese Patent No. 4784847 and Japanese Patent Application Laid-Open No. 2013-60637 the metal fine particles described in Japanese Patent No. 5077728 can be mentioned, and can be synthesized by the method described therein.
  • the thioether type (RSR') organic compound has an appropriate affinity adsorption effect on the surface of metal fine particles and a rapid desorption property by heating, and has low temperature fusion characteristics. It has been developed as a metal fine particle showing.
  • metal fine particles in which a polymer compound having a polyethylene oxide moiety having 8 to 200 carbon atoms is composited are included.
  • the polymer compound containing these polyethylene oxide structures can be produced according to the methods described in these publications.
  • the phosphoric acid ester type organic compound containing these polyethylene oxide structures has a thioether skeleton and also has a phosphoric acid ester group, and by having these groups, the surface of the metal fine particles is subjected to. Appropriate affinity adsorption effect and rapid desorption by heating can be added.
  • the concentration of the protective agent in the paste is not particularly limited, but is preferably in the range of 15% or less from the viewpoint of easy fusion of metal fine particles during sintering, conductivity and improvement of bonding strength. Yes, more preferably in the range of 10% or less.
  • the paste according to the present invention is composed of at least metal fine particles and a protective agent.
  • the paste according to the present invention can be produced by protecting the surface of metal fine particles with a protective agent. Any method can be adopted for the preparation of the paste. For example, in addition to the chemical reduction method, the thermal decomposition method and the electrochemical method can be adopted as the wet method, and the evaporation method in gas and the sputtering method can be adopted as the dry method.
  • a method for producing a paste when an organic compound containing a polyethylene oxide structure having 8 to 200 carbon atoms is used as a protective agent will be described.
  • the metal type is copper and / or silver
  • the metal fine particles in which an organic compound containing a polyethylene oxide structure having 8 to 200 carbon atoms is composited are prepared by mixing a divalent copper ion compound or a monovalent silver ion compound with a solvent in the presence of a thioether type organic compound. It can be easily produced by combining with a step of reducing copper ions or silver ions.
  • the divalent copper ion compound a generally available copper compound can be used, and sulfates, nitrates, carboxylates, carbonates, chlorides, acetylacetonate complexes and the like can be used.
  • a complex with zero-valent copper fine particles it may be produced from a divalent compound or a monovalent compound, or may have water or water of crystallization.
  • the divalent copper ion compound CuSO 4 , Cu (NO 3 ) 2 , Cu (OAc) 2 , Cu (CH 3 CH 2 COO) 2 , Cu (HCOO) 2 , CuCO 3 , CuCl 2 , Cu 2 O, C 5 H 7 CuO 2 , and their hydrates and the like can be used.
  • heating the salt, or a basic salt e.g. Cu (OAc) 2 ⁇ CuO obtained by such exposure to a basic atmosphere, Cu (OAc) 2 ⁇ 2CuO , Cu 2 Cl (OH) 3 or the like suitably the Can be used.
  • These basic salts may be prepared in the reaction system, or may be prepared separately outside the reaction system. Further, a general method of adding ammonia or an amine compound to form a complex to secure solubility and then using it for reduction can also be applied.
  • the monovalent silver ion compound generally available silver compounds can be used, such as silver nitrate, silver oxide, silver acetate, silver fluoride, silver acetylacetonate, silver benzoate, silver carbonate, and silver citrate.
  • silver hexafluorophosphate, silver lactate, silver nitrite, silver pentafluoropropionate, hydrates thereof, etc., and silver nitrate or silver oxide can be used from the viewpoint of ease of handling and industrial availability. preferable.
  • These copper and / or silver ion compounds are dissolved or mixed in a solvent in which a thioether type organic compound is dissolved or dispersed in advance.
  • the solvent that can be used at this time depends on the structure of the organic compound used, but alcohols such as ethanol, ethylene glycol, diethylene glycol and glycerin, polar solvents such as water and acetone, and mixtures thereof are preferable. Can be used. Of these, a water-ethylene glycol mixture is particularly preferred.
  • the concentration of the thioether-type organic compound in various solvents is preferably adjusted to the range of 0.3 to 10% from the viewpoint of facilitating the control of the subsequent reduction reaction.
  • Copper and / or silver ion compounds are added collectively or separately to the solvent prepared above and mixed.
  • a poorly soluble solvent When used, it may be dissolved in a small amount of a good solvent in advance and added to the solvent.
  • the mixing ratio of the thioether-type organic compound to be mixed with the copper and / or silver ion compound can be appropriately selected according to the protective ability of the thioether-type organic compound in the reaction solvent.
  • the thioether-type organic compound per 1 mol of the copper and / or silver ion compound is prepared in the range of 1 mmol to 30 mmol, and is particularly preferably used in the range of 15 to 30 mmol.
  • the same can be carried out by using a phosphoric acid ester type organic compound containing a polyethylene oxide structure, and the amount of the organic compound used per 1 mol of the copper and / or silver ion compound is also the same as described above.
  • Reducing agents include hydrazine compounds, hydroxylamines and derivatives thereof, metal hydrides, phosphinates, aldehydes, endiols, hydroxyketones, etc., and reduction of copper and / or silver at a temperature of 80 ° C. or lower from ice-cold temperature. Since the reaction can proceed, it can be preferably used.
  • reducing agents such as hydrazine hydrate, unsymmetrical dimethylhydrazine, aqueous hydroxylamine solution, and sodium borohydride are suitable. These reducing agents can reduce copper compounds to 0 valence, and are suitable for producing a composite of an organic compound and nano-copper particles by using divalent and monovalent copper compounds as reduced copper.
  • the conditions of the reduction reaction can be appropriately set according to the copper compound used as a raw material, the type of reducing agent, the presence or absence of complexation, the solvent, and the type of the thioether type organic compound.
  • copper (II) acetate is reduced with sodium borohydride in an aqueous solvent
  • zero-valent nanocopper particles can be prepared even at an ice-cooled temperature.
  • hydrazine is used, the reaction is slow at room temperature, and a smooth reduction reaction occurs only after heating to about 60 ° C.
  • a reaction time of about 2 hours is required at 60 ° C.
  • a reaction mixture containing a complex of an organic compound and copper-based fine particles is obtained.
  • the copper fine particles prepared in this way can be highly dispersed in the same manner as before drying even when the moisture is completely removed by the effect of the protective agent to obtain a dried body powder and then dispersed in the solvent again. is there.
  • a step of removing metal compound residue, reducing reagent residue, organic compound containing excess polyethylene oxide structure, etc. is provided as necessary.
  • Purification of the complex can be carried out by reprecipitation, centrifugal sedimentation, ultrafiltration, etc., and the above-mentioned impurities are obtained by washing the reaction mixture containing the obtained complex with water, ethanol, acetone and a mixture thereof. Can be washed away.
  • the paste according to the present invention is used for binder components such as resins, antidrying agents, antifoaming agents, adhesion imparting agents to substrates, antioxidants, and for promoting film formation, as long as the effects of the present invention are not impaired.
  • binder components such as resins, antidrying agents, antifoaming agents, adhesion imparting agents to substrates, antioxidants, and for promoting film formation, as long as the effects of the present invention are not impaired.
  • Various catalysts, various surfactants such as silicone-based surfactants and fluorine-based surfactants, leveling agents, mold release accelerators and the like can be added as auxiliary agents.
  • the concentration of the metal fine particles in the paste according to the present invention can be adjusted to an arbitrary concentration by adding a dispersion medium described later.
  • the dispersion medium can be added at the time of paste synthesis or after synthesis.
  • the concentration of the metal fine particles in the paste is not particularly limited, but is preferably in the range of 40 or more and less than 95%, more preferably 60 to 90%, in consideration of the fluidity of the paste and the filling performance in the opening portion. The range.
  • Dispersion medium Water or a solvent as a dispersion medium can be added to the paste containing the metal fine particles and the protective agent of the present invention as long as the effects of the present invention are not impaired.
  • the dispersion medium can be added for the purpose of imparting wettability to the base material and adjusting the concentration of metal fine particles in the paste.
  • the dispersion medium that can be used in the present invention it is desirable that the dispersion medium does not remain inside the pillars after sintering, and it is preferable to use a compound or mixture having a boiling point of 250 ° C. or lower.
  • the dispersion medium is not particularly limited as long as it is a compound having a boiling point of 250 ° C. or lower, and water and / or an organic solvent can be used as the dispersion medium.
  • As the dispersion medium it is preferable to use a good dispersion medium that does not agglomerate metal fine particles in order to produce a paste having a uniform particle size.
  • organic solvents that can be preferably used.
  • examples of the organic solvent containing a hydroxyl group include water, methanol, ethanol, 1-propanol, isopropanol, 1-butanol, isobutanol, sec-butanol, tert-butanol, amyl alcohol, tert-amyl alcohol, 1-hexanol, and cyclo.
  • the pillars in the present invention are not particularly limited in shape, diameter, etc. as long as the effects of the present invention are exhibited.
  • the pillar of the present invention preferably has a columnar shape because the tip bonding is stable, more preferably a substantially columnar shape, and particularly preferably a columnar shape.
  • the diameter of the pillar of the present invention is preferably 100 ⁇ m or less, more preferably 50 ⁇ m or less, and particularly preferably 30 ⁇ m or less, because the chip joining step becomes efficient.
  • the method for forming pillars in the present invention is not particularly limited, but a method for forming pillars by an embedding method will be described in detail below.
  • a resist layer is formed on a substrate having an electrode portion, a pattern (mold) having a plurality of openings is formed in the resist layer, and a paste is filled in the openings of the resist layer.
  • the pillar (A) can be easily produced by sintering.
  • the material of the substrate having the electrodes is not particularly limited, and metals, ceramics, silicon, resins, composite materials thereof and the like can be used.
  • a known method can be adopted for forming a resist layer having an opening portion on a substrate having an electrode.
  • the resin material used is not particularly limited as long as a mold having a desired pattern having an opening can be produced.
  • various dry films such as photoresist (photo-resist), polyimide, epoxy, and epoxy molding compound (EMC) can be used.
  • the resist layer may be removed after the pillar (A) is formed or the conductive pillar is formed, or may be left as a permanent film. When used as a permanent film, there is an advantage that the step of peeling the resin film can be reduced.
  • the method of filling the paste opening into the resist opening is not particularly limited, and squeegee, doctor blade, dispenser, inkjet, press injection, vacuum printing, pressing by pressurization, or the like can be used.
  • the method of filling the opening with the paste using a squeegee is adopted, there are no restrictions on the squeegee material, and a squeegee made of plastic, urethane rubber, other rubber, ceramic, metal, etc. can be used.
  • the thickness and length of the squeegee are not particularly limited.
  • the pressing during coating can be performed with a printing pressure that does not damage the opening pattern of the resist layer. Further, a metal mask or a mask for screen printing may be used.
  • the paste filling operation in the mold can be performed in an inert gas atmosphere or a reducing gas atmosphere.
  • the shape of the pillar to be produced is not particularly limited, and there is no particular limitation as long as a bonding layer can be provided at the tip of the pillar, but a cylinder or a polygonal pillar shape is preferable.
  • the firing temperature and firing time are not particularly limited as long as sufficient values can be obtained for the conductivity and bonding strength of the pillars, but preferably, the firing temperature is 150 to 350 ° C. and the firing time is 1 to 1.
  • the range is 60 minutes. More preferably, the firing temperature is in the range of 200 to 250 ° C. or less and the firing time is in the range of 5 to 15 minutes. If the paste according to the present invention is used, sufficient performance can be exhibited even when baking is performed for a short time. Further, if necessary, it is also possible to perform firing using a temperature profile, such as performing a temporary firing in which the solvent is volatilized at a low temperature and then performing a main firing in the range of 150 to 350 ° C.
  • the firing method for sintering the metal fine particles is not particularly limited as long as the metal fine particles are fused, and the firing method by heat such as a hot plate or a hot air oven, visible light, infrared light, or laser light is used. Plasma treatment such as irradiation, flash lamp, and hydrogen gas may be used.
  • the gas type used during sintering there are no particular restrictions on the gas type used during sintering.
  • a noble metal is used as the metal fine particles
  • sintering is possible not only in an inert gas environment such as nitrogen gas or argon gas but also in the atmosphere.
  • an inert gas such as nitrogen gas or argon gas.
  • a base metal is used for the metal fine particles
  • a forming gas containing hydrogen may be used, or a gas to which a reducing component such as formic acid is added may be used.
  • the shape of the upper part of the cross section is concave. It becomes a cup shape.
  • This cup shape has the effect of increasing the bonding strength of the pillars because (1) the bonding area between the pillars and the bonding layer can be increased. (2) When the linear expansion coefficients of the top chip and the bottom chip are different, distortion occurs in the horizontal direction with respect to the electrode substrate due to the heating / cooling cycle, but the bonding layer / pillar interface exists in the same direction as the strain direction. This has the effect of increasing the joint strength of the pillars. As a result, the effect of dramatically improving the adhesion and the joint strength at the time of the die shear test can be obtained. This effect cannot be realized by the conductive pillars produced by the plating method.
  • the prepared pillars are made by fusing copper particles that are finely packed in a mold and have a structure with voids. Therefore, unlike bulk metals, the stress between the base materials caused by the difference in the coefficient of thermal expansion Has the effect of being able to alleviate. Therefore, it has the effect of improving the durability during environmental tests such as the thermal shock test and improving the joint strength.
  • the conductive pillar (B) according to the present invention can be produced by forming a bonding layer at at least one tip of the pillar (A) produced by the above method (FIG. 1).
  • the conductive pillar (C) according to the present invention can also be manufactured in the same manner as the conductive pillar (B).
  • the conductive pillar (C) is different from the conductive pillar (B) in that it has an intermetallic compound layer at the interface between the pillar (A) and the bonding layer.
  • FIG. 2 shows the difference between the conductive pillars (B) and (C).
  • FIG. 2A shows a schematic view of a top view of the manufactured conductive pillar.
  • 2B and 2C are schematic cross-sectional views taken along the cross section shown by the broken line in FIG. 2A. Each configuration will be described in detail below.
  • solder alloy As the material of the bonding layer according to the present invention, Au, Ag, Cu, Sn, Ni, a solder alloy and the like can be used, and even if it is composed of only a single component, it is composed of a plurality of components. May be good.
  • a solder alloy can be more preferably used as the material of the bonding layer according to the present invention.
  • Sn—Ag alloy, Sn—Pb alloy, Sn—Bi alloy, Sn—Zn alloy, Sn—Sb alloy, Sn—Bi alloy, Sn—In alloy, Sn—Cu alloy, Sn with Au, Ag. , Bi, In and Cu, and alloys to which two elements selected from the group are added can be used.
  • a metal or alloy used for general bonding purposes can be used in addition to Sn, and it can also be used.
  • the material of the bonding layer according to the present invention a material containing no solvent and / or flux component can be more preferably used. If the bonding layer material contains a solvent or a flux component, it may be gasified during melting or reflowing and remain as voids in the bonding layer, resulting in a decrease in bonding strength.
  • the method for forming the bonding layer according to the present invention is not particularly limited as long as the bonding layer can be formed at at least one tip of a pillar made of metal fine particles.
  • the bonding layer can be formed at at least one tip of a pillar made of metal fine particles.
  • printing methods such as stencil mask method and dry film method, ball mounting method, thin film deposition method, IMS method, etc.
  • melting by melting (reflowing) the solder supplied to the tip of the pillar.
  • the IMS method can be more preferably used because the bonding layer can be produced at the tip of the pillar in the state where the bonding layer material is melted and no solvent or flux component is required.
  • the structure of the bonding layer is not particularly limited, and a multilayer structure in which two or more types of bonding layer materials are laminated may be used.
  • the bonding layer is formed at the tip of at least one of the pillars made of fine metal particles.
  • the intermetallic compound layer according to the present invention indicates an alloy layer formed between the pillar (A) and the bonding layer.
  • the composition of the intermetallic compound and its ratio are not particularly limited, and the composition ratio of the alloy varies depending on the metal type and the sintering conditions.
  • the intermetallic compound layer is formed by mutually diffusing the bonding material into the pillar (A) and the metal of the pillar (A) into the bonding material. Pillars made from metal fine particle paste are composed of metal fine particles and have a porous structure. The structure is maintained even when the metal fine particles are fused by sintering.
  • the molten bonding material invades the inside of the pores of the pillar (A) having a porous structure.
  • the impregnated bonding material forms intermetallic compounds with fine metal particles.
  • a material having a porous structure can form a uniform intermetallic compound layer more quickly than a bulk metal because of its large specific surface area.
  • This intermetallic compound layer is formed at the interface between the bonding layer and the pillar (A), and improves the bonding strength of the conductive pillar.
  • the intermetallic compound layer does not exist in parallel with the electrode substrate and has a concave shape. This concave shape improves the strength against the die shear test.
  • the conductive pillars are not particularly limited as long as the chips can be joined, but in order not to impair the conductivity, a cylindrical, triangular prism, or polygonal prism shape is used. It can be preferably used.
  • the diameter of the conductive pillar of the present invention can be calculated as follows.
  • the diameter of the "circle” which is the shape of the bottom surface of the pillar can be calculated as the diameter of the conductive pillar. it can.
  • the height of the "triangle" which is the shape of the bottom surface of the pillar should be calculated as the diameter of the conductive pillar. Can be done.
  • the conductive pillar has a polygonal pillar shape and the connecting surface between the pillar (A) and the electrode substrate is polygonal (excluding triangles), the most diagonal line of the "polygon" which is the shape of the bottom surface of the pillar.
  • the length of the long wire can be calculated as the diameter of the conductive pillar.
  • the aspect ratio of the conductive pillar is not particularly limited, but a conductive pillar having an aspect ratio of 0.5 or more can be preferably used.
  • the "height of the conductive pillar" means the height
  • the resist layer used as a mold in the pillars may be removed.
  • a known method can be used to remove the resist layer used for the mold from the substrate. It is also possible to leave the resist layer as a permanent film without removing it. When a permanent film is used, there is an advantage that the step of peeling the resin film can be reduced.
  • the conductive pillar of the present invention can be used as a mounting terminal for various electronic components / devices including flip chip mounting (Fig. 3).
  • this reaction mixture is circulated in a hollow fiber type ultrafiltration membrane module (HIT-1-FUS1582, 145 cm 2 , fractional molecular weight 150,000) manufactured by Daisen Membrane Systems, Inc., and the same amount as the exuding filtrate.
  • a 0.1% aqueous solution of hydrazine hydrate While adding a 0.1% aqueous solution of hydrazine hydrate, the mixture was circulated and purified until the filtrate from the ultrafiltration module became about 500 mL.
  • an aqueous dispersion of 2.85 g of a complex of a thioether type organic compound and copper fine particles was obtained.
  • the non-volatile content in the aqueous dispersion was 16%.
  • thermogravimetric analysis TG-DTA
  • TG-DTA thermogravimetric analysis
  • the obtained copper fine particles contained an organic substance containing a 3% polyethylene oxide structure.
  • the average primary particle size was measured by transmission electron microscopy (TEM) observation.
  • the prepared metal fine particles are diluted 100-fold with a good solvent (water, terpineol, 1-butanol or ethylene glycol), and the diluted solution is cast on a carbon film-coated grid, dried, and subjected to a transmission electron microscope (equipment). : TEMJEM-1400 (manufactured by JEOL), acceleration voltage: 120 kV).
  • 200 fine particles were randomly extracted from the obtained TEM image, the area of each fine particle was calculated, and the value calculated based on the number of particle size when converted into a true sphere was adopted.
  • the average primary particle diameter of the obtained copper fine particles was 20 nm.
  • the average primary particle size was measured in the same manner as described in Synthesis Example 1. When the obtained fine particles were observed with a transmission electron microscope (TEM), the average primary particle size of the fine particles was 6 nm.
  • TEM transmission electron microscope
  • the average primary particle size was measured in the same manner as described in Synthesis Example 1. When the obtained silver fine particles were observed with a transmission electron microscope (TEM), the average primary particle size of the silver fine particles was 17 nm.
  • TEM transmission electron microscope
  • the average primary particle size was measured in the same manner as described in Synthesis Example 1. When the obtained silver fine particles were observed with a transmission electron microscope (TEM), the average primary particle size of the silver fine particles was 25 nm.
  • TEM transmission electron microscope
  • the paste of this synthetic example is 8.26 g of copper powder (1100Y D50: 1.1 ⁇ m manufactured by Mitsui Metal Mine Co., Ltd.) and 0.190 g of TEGO (registered trademark) VARIPLUSSK (manufactured by Evonik Degussa Japan Co., Ltd.).
  • DISPER BYK-111 (Bick Chemie's phosphate group-containing polymer) 0.05 g, TRIXENE BI 7992 (Baxenden's) 0.660 g, and Denacol® EX-321 (Nagase Chemtex (registered trademark) (Manufactured by Co., Ltd.) 0.207 g, High Solve (registered trademark) MTEM (manufactured by Toho Kagaku Kogyo Co., Ltd.) 0.260 g, Diethylene glycol monobutyl ether acetate 0.323 g, and U-CAT SA 102 (Sun Appro) (Manufactured by Yasuda Seiki Co., Ltd.) was mixed with 0.050 g using an automatic Hoover Marler (manufactured by Yasuda Seiki Seisakusho Co., Ltd.) and dispersed.
  • the average primary particle size was measured in the same manner as described in Synthesis Example 1.
  • the average primary particle size of the copper fine particles was 1.2 ⁇ m.
  • Example 1 ⁇ Manufacturing conductive pillars> (Preparation of electrode substrate and mold) The method of manufacturing the electrode substrate used in the experiment will be described.
  • the substrate was prepared by the following procedure. Ti (thickness 50 nm) was sputtered on a 4-inch silicon wafer provided with an Al electrode, and then Cu (250 nm) was sputtered to prepare an electrode substrate. A resist resin was applied to the sputtered silicon substrate so that the final film thickness was 30 ⁇ m, and patterning was performed.
  • the shape of the resist pattern was a cylindrical shape, the diameter of the opening portion was 30 ⁇ m, and the depth of the opening portion was 30 ⁇ m.
  • the aspect ratio was designed to be 1.0.
  • the pillars were formed by embedding the adjusted paste in a resist opening provided in the prepared electrode substrate and sintering the paste.
  • the paste was filled using a urethane rubber squeegee for screen printing. Printing was done by hand and no printing mask was used. The printing speed at the time of filling was about 10 mm / s.
  • the paste prepared by the method described in Synthesis Example 1 was filled in an opening portion having a diameter of 30 ⁇ m with a urethane squeegee.
  • Example 2 (Example 2) ⁇ Manufacturing conductive pillars> (Preparation of electrode substrate and mold) An electrode substrate was produced in the same manner as in the method described in Example 1.
  • Pillar formation Pillars were formed in the same manner as in Example 1 using the paste prepared by the method described in Synthesis Example 2.
  • a bonding layer was prepared in the same manner as described in Example 1.
  • Example 3 (Preparation of electrode substrate and mold) An electrode substrate was produced in the same manner as in the method described in Example 1.
  • Pillar formation Pillars were formed in the same manner as in Example 1 using the paste prepared by the method described in Synthesis Example 3.
  • a bonding layer was prepared in the same manner as described in Example 1.
  • Example 4 ⁇ Manufacturing conductive pillars> (Preparation of electrode substrate and mold) An electrode substrate was produced in the same manner as in the method described in Example 1.
  • Pillar formation Pillars were formed in the same manner as in Example 1 using the paste prepared by the method described in Synthesis Example 4.
  • a bonding layer was prepared in the same manner as described in Example 1.
  • the electrode substrate used in the experiment was prepared by the following procedure.
  • An electrode substrate was prepared by providing a Ni layer on an Al electrode substrate provided on a 4-inch silicon wafer and laminating Au on the Al electrode substrate to a thickness of 4 ⁇ m by an electroless plating method.
  • the prepared electrode substrate was used in this experiment.
  • a resist resin was applied to a silicon substrate having an Au electrode so that the final film thickness was 30 ⁇ m, and patterning was performed.
  • the shape of the resist pattern was a cylindrical shape, the diameter of the opening portion was 30 ⁇ m, and the depth of the opening portion was 30 ⁇ m.
  • the aspect ratio was designed to be 1.0.
  • Pillar formation Pillars were formed in the same manner as in Example 1 using the paste prepared by the method described in Synthesis Example 1.
  • a bonding layer was prepared in the same manner as described in Example 1.
  • Pillar formation Pillars were formed in the same manner as in Example 1 using the paste prepared by the method described in Synthesis Example 5.
  • a bonding layer was prepared in the same manner as described in Example 1.
  • the prepared electrode substrate was immersed in 5 wt% sulfuric acid to perform a pretreatment for removing the oxide film of the seed layer. After the pretreatment, a copper plating solution consisting of 65 g / L of copper sulfate pentahydrate, 170 g / L of sulfuric acid, and 70 mg / L of sodium chloride was prepared. The prepared electrode substrate was immersed in a copper plating solution and polarized. The exposed cathode electrode surface of the pattern opening portion of the resist layer was plated with copper to prepare pillars. The prepared pillar was columnar, and the pillar height was 20 um.
  • a bonding layer was prepared in the same manner as described in Example 1.
  • Pillars were formed in the resist opening portion by a paste filling or plating method, and SAC305, which is a connecting layer, was formed at the tip of the pillars by the IMS method to obtain a conductive pillar.
  • the prepared conductive pillar had a pillar height (metal fine particle layer) of about 15 to 20 ⁇ m, an intermetallic compound layer of 1 to 5 ⁇ m, and a bonding layer of about 5 to 15 ⁇ m.
  • the resist thin film was removed and the bonding strength was measured. The results of the obtained joint strength measurement are shown in Table 1.
  • the evaluation criteria were as follows. ⁇ : Indicates that the maximum value of the shear strength of the produced conductive pillar is 150 MPa or more. ⁇ : Indicates that the maximum value of the shear strength of the produced conductive pillar is 80 MPa or more. ⁇ : Indicates that the maximum value of the shear strength of the produced conductive pillar is 50 MPa or more. X: Indicates that the maximum value of the shear strength of the produced conductive pillar is less than 50 MPa.
  • the pillars prepared in Examples 1 to 5 showed good bonding strength as compared with those of Comparative Example.
  • the conductive pillars prepared by using the copper paste prepared in Synthesis Example 1 showed very good results.
  • the conductive pillar in which the electrode substrate was made of Au showed a good share strength comparable to that of the copper-plated pillar described in Reference Example 1. It is considered that this is because the surface of the electrode substrate was not affected by oxidation and the bonding between the electrode and the conductive pillar was strengthened. Therefore, it is considered that removing the oxide film on the surface of the electrode substrate improves the bonding strength to the same extent as that described in Reference Example 1 in Examples 1 to 5, and the conductive pillar made of metal fine particles according to the present invention is industrially used. It shows that it can be done.
  • ⁇ Measurement of electrical resistance of conductive pillars The prepared top Si chip having a conductive pillar and the bottom Si chip having a copper electrode substrate were joined, and the electric resistance of the conductive pillar was measured by 4-terminal measurement.
  • the diameter of the conductive pillar used for the measurement was a cylindrical shape of 40 ⁇ m, and the height of the conductive pillar after chip assembly was 25 ⁇ m.
  • the resistance value was measured by joining 80 or 82 conductive pillars in series and measuring the electrical resistance (FIGS. 3 and 4). For the measurement, 16 wirings in which 80 or 82 conductive pillars were connected in series were measured. Based on the resistance value obtained by the measurement, the resistance value per conductive pillar was calculated. Table 2 shows the average value of these resistance values obtained by the measurement.
  • the pillars produced in Examples 1 to 5 showed a good resistance value, that is, conductivity as compared with those of Comparative Example.
  • the conductive pillars prepared by using the copper paste prepared in Synthesis Example 1 showed very good results. Even when compared with SAC305 of Comparative Example 2, the resistance value is about 1/10 to 1/5, which is sufficiently durable for practical use.
  • 80 or 82 conductive pillars were joined in series to evaluate the conductivity, but since this measurement method is possible, the conductive pillars of the present invention are chipped. It has few defects such as chips and has a good yield. In Comparative Example 1, measurement could not be performed due to disconnection.
  • the conductive pillar of the present invention has excellent shear strength and conductivity, and can be used as a terminal for mounting various electronic components and devices including a terminal for mounting a flip chip. Further, since the conductive pillar of the present invention can be manufactured without an etching step or a plating step, the environmental load at the time of manufacturing is small, and a fine structure can be obtained.

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  • Engineering & Computer Science (AREA)
  • Computer Hardware Design (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Power Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Powder Metallurgy (AREA)
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Abstract

La présente invention concerne des piliers conducteurs formés par placage électrolytique, un procédé classique, qui souffrent d'un problème en ce qu'il est difficile de former des piliers de manière fine sans être affecté par une contre-dépouille. De surcroît, des piliers de cuivre dans la masse présentent des modules d'élasticité d'au moins trois fois ceux d'un matériau de brasure et présentent des contraintes de rendement d'au moins huit fois celles d'un matériau de brasure et souffrent ainsi du problème selon lequel une contrainte thermique générée pendant la liaison d'une puce et d'un substrat ne peut pas être suffisamment absorbée. Les inventeurs ont examiné sérieusement des solutions aux problèmes et découvert un pilier conducteur qui contient de fines particules métalliques et comprend une couche d'assemblage. La présente invention est le pilier conducteur qui peut être utilisé en tant que borne d'encapsulation de puce retournée et présente un effet spécial pour les problèmes.
PCT/JP2020/023752 2019-06-18 2020-06-17 Pilier conducteur WO2020256012A1 (fr)

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Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014111800A (ja) * 2012-12-05 2014-06-19 Nippon Handa Kk ペースト状金属微粒子組成物、固形状金属または固形状金属合金の製造方法、金属製部材の接合方法、プリント配線板の製造方法および電気回路接続用バンプの製造方法
US9859241B1 (en) * 2016-09-01 2018-01-02 International Business Machines Corporation Method of forming a solder bump structure

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014111800A (ja) * 2012-12-05 2014-06-19 Nippon Handa Kk ペースト状金属微粒子組成物、固形状金属または固形状金属合金の製造方法、金属製部材の接合方法、プリント配線板の製造方法および電気回路接続用バンプの製造方法
US9859241B1 (en) * 2016-09-01 2018-01-02 International Business Machines Corporation Method of forming a solder bump structure

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