JP2010232667A - Thermolysis mutual fusion method for heat decomposable particle using high-frequency electromagnetic wave irradiation, and its application to product - Google Patents
Thermolysis mutual fusion method for heat decomposable particle using high-frequency electromagnetic wave irradiation, and its application to product Download PDFInfo
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Abstract
Description
本発明はプリント配線基板等の電子実装部品製造における、導電部品(導電路、バンプ等)およびアンテナパターンの形成方法に関する。 The present invention relates to a method for forming conductive parts (conductive paths, bumps, etc.) and an antenna pattern in the manufacture of electronic mounting parts such as printed wiring boards.
金属(金属酸化物)微細粒子の製造技術、独立分散技術、さらには、超微量インクジェット、精密スクリーン印刷、ナノプリンティング、ナノインプリンティングによる微細配線パターニング技術の近年の著しい発展に伴い、それら技術を応用した直接回路描画法が次世代の電子実装部品形成技術として大いに注目されている。 With the recent remarkable development of fine wiring patterning technology by metal (metal oxide) fine particle manufacturing technology, independent dispersion technology, ultra-micro inkjet, precision screen printing, nanoprinting and nanoimprinting, these technologies are applied. The direct circuit drawing method has attracted a great deal of attention as a next-generation electronic packaging component forming technology.
この直接回路描画法は、それまでリゾグラフィーやエッチングといった複雑な工程を経て製造されていた電子実装部品を、金属(金属酸化物)粒子の直接描画→焼成→相互融着→導電化によって製造するという手法であり、その詳細については非特許文献1第71頁に記載されている。この手法の確立により、導電回路パターン、バンプ、パッド、ビア、アンテナパターンといった電子実装部品を、安価かつ簡便に製造することが可能となると期待される。
In this direct circuit drawing method, an electronic packaging component that has been manufactured through complicated processes such as lithography and etching is manufactured by direct drawing of metal (metal oxide) particles → firing → mutual fusion → conducting. The details are described in page 71 of Non-Patent
この直接回路描画法の重要な工程の一つに、金属(金属酸化物)粒子をパターニングした回路基板を熱処理し、粒子を相互融着させ、粒子によって構成された回路パターンを導電化する工程がある。 One of the important steps of this direct circuit drawing method is a step of heat-treating a circuit board on which metal (metal oxide) particles are patterned, mutually fusing the particles, and making a circuit pattern constituted by the particles conductive. is there.
これまでに提案されている直接回路描画法においては、この粒子を相互融着させる熱処理工程に、熱風やスチームもしくは電熱線を用いた加熱炉によって、金属(金属酸化物)粒子によって構成された回路パターン部分と下地基板部分の実装部品全体を、150℃から210℃で加熱処理することが特許文献1の実施例に、また同じく実装部品全体を150℃で加熱処理することが特許文献2の実施例に記載されている。
In the direct circuit drawing method proposed so far, a circuit composed of metal (metal oxide) particles by a heating furnace using hot air, steam, or heating wire in the heat treatment process for mutual fusion of the particles. The entire mounting component of the pattern portion and the base substrate portion is heat-treated at 150 ° C. to 210 ° C. in the embodiment of
しかしながら、この従来提案されていた熱処理方法では、粒子によって構成された回路パターンと共に下地基板部分も同等に等しく加熱されるため、使用可能な下地基板がこの熱処理時の保持温度よりも耐熱温度の高い材料に限定されるという問題があった。特に次世代の超高速電子デバイスにおいて不可欠な低抵抗の電子実装部品を作成する場合、この熱処理条件を高温・長時間に設定する必要があり、その意味で使用可能な基板材料は大きく限定されるものであった。 However, in this conventionally proposed heat treatment method, since the base substrate portion is heated equally and together with the circuit pattern constituted by the particles, the usable base substrate has a heat resistant temperature higher than the holding temperature during this heat treatment. There was a problem that it was limited to materials. Especially when creating electronic components with low resistance, which are indispensable for next-generation ultra-high-speed electronic devices, it is necessary to set the heat treatment conditions at high temperature and long time. In this sense, usable substrate materials are greatly limited. It was a thing.
さらに、この従来提案されていた熱処理方法では、加熱に数十分の時間を要し、生産性も低いことなどか特許文献1の実施例に記載されている。 Further, in this conventionally proposed heat treatment method, heating takes several tens of minutes, and productivity is low.
金属(金属酸化物)粒子を用いた直接回路描画法において、使用可能な下地基板が耐熱温度の高い材料に限定されるともに、基板の加熱処理に時間がかかり生産性が低いという問題があった。そこで、本発明は耐熱性の低い基板材料においても低抵抗の実装部品を短時間に作成することが可能な、新しい技術手法を提供することを目的とする。 In the direct circuit drawing method using metal (metal oxide) particles, there are problems that the usable base substrate is limited to a material having a high heat-resistant temperature and that the heat treatment of the substrate takes time and productivity is low. . Accordingly, an object of the present invention is to provide a new technical method that can produce a low-resistance mounting component in a short time even on a substrate material having low heat resistance.
請求項1に記載の発明は、熱分解性を有し且つ高周波電磁波を吸収する粒子を、各種基板上に表面塗布を行った後に、高周波電磁波照射を行うことで、熱分解性粒子を選択的に加熱することを特徴とする、熱分解性粒子の加熱分解方法である。 The invention according to claim 1 selectively selects the thermally decomposable particles by performing high frequency electromagnetic wave irradiation after the surface of the particles having thermal decomposability and absorbing high frequency electromagnetic waves is applied on various substrates. It is a method for thermally decomposing thermally decomposable particles, characterized by heating to a temperature.
請求項2に記載の発明は、熱分解性を有し且つ高周波電磁波を吸収する粒子を、各種基板上に表面塗布を行った後に、高周波電磁波照射を行うことで、熱分解性粒子を選択的に加熱することを特徴とする、熱分解性粒子の加熱分解相互融着方法である。 According to the second aspect of the present invention, the particles having heat decomposability and absorbing high-frequency electromagnetic waves are selectively applied to the thermally decomposable particles by performing high-frequency electromagnetic wave irradiation after surface coating on various substrates. It is a method for thermally decomposing and thermally decomposing thermally decomposable particles, characterized by heating to a temperature.
請求項3に記載の発明は、熱分解性を有し且つ高周波電磁波を吸収する粒子を、各種基板上に回路パターニングを行った後に、高周波電磁波照射を行うことで、熱分解性粒子を選択的に加熱することを特徴とする、熱分解性粒子の加熱分解相互融着方法である。 The invention according to claim 3 selectively selects the thermally decomposable particles by irradiating the particles having heat decomposability and absorbing high frequency electromagnetic waves on a variety of substrates after circuit patterning. It is a method for thermally decomposing and thermally decomposing thermally decomposable particles, characterized by heating to a temperature.
請求項4に記載の発明は、高周波電磁波照射によって、基板上に塗布もしくは回路パターニングされた熱分解性粒子を選択的に加熱し、さらにこの照射にともなう昇温によって熱分解性粒子の熱分解−相互融着が引き起こされた後は、加熱効果が自発的に停止することを特徴とした請求項2乃至請求項3に記載の熱分解性粒子の加熱分解相互融着法である。
The invention according to claim 4 selectively heats the thermally decomposable particles coated or circuit-patterned on the substrate by high-frequency electromagnetic wave irradiation, and further thermally decomposes the thermally decomposable particles by increasing the temperature accompanying this irradiation. 4. The thermal decomposition mutual fusion method of thermally decomposable particles according to
請求項5に記載の発明は、表面塗布された熱分解性粒子が、フェノール樹脂、エポキシ樹脂をはじめとする高分子樹脂と熱分解性粒子を混合したペースト状混合物の形で表面塗布されることを特徴とする請求項2乃至請求項4に記載の熱分解性粒子の加熱分解相互融着方法である。
In the invention according to
請求項6に記載の発明は、熱分解性粒子に照射する電磁波が1MHz<f<300GHzの範囲の高周波電磁波であることを特徴とする請求項2乃至請求項5に記載の熱分解性粒子の加熱分解相互融着方法である。 The invention according to claim 6 is characterized in that the electromagnetic wave applied to the thermally decomposable particles is a high frequency electromagnetic wave in a range of 1 MHz <f <300 GHz. This is a thermal decomposition mutual fusion method.
請求項7に記載の発明は、熱分解性粒子に照射する電磁波が300MHz<f<300GHzの範囲の高周波電磁波であることを特徴とする請求項2乃至請求項5に記載の熱分解性粒子の加熱分解相互融着方法である。
The invention according to
請求項8に記載の発明は、前記熱分解性粒子が、金属−酸素結合を持つ無機及び有機金属化合物、金属−窒素結合を持つ無機及び有機金属化合物、金属−炭素結合を持つ無機及び有機金属化合物、金属−ハロゲン結合を持つ無機及び有機金属ハロゲン化物のいずれかであること特徴とする、請求項2乃至請求項7に記載の粒子熱分解相互融着法である。
The invention according to claim 8 is characterized in that the thermally decomposable particles are inorganic and organometallic compounds having metal-oxygen bonds, inorganic and organometallic compounds having metal-nitrogen bonds, and inorganic and organometallics having metal-carbon bonds. The particle pyrolysis mutual fusion method according to any one of
請求項9に記載の発明は前記熱分解性粒子が、酸化銀、窒化銀、ハロゲン化銀のいずれかであることを特徴とする、請求項8に記載の粒子熱分解相互融着法である。 The invention according to claim 9 is the grain pyrolysis mutual fusion method according to claim 8, wherein the thermally decomposable grains are any one of silver oxide, silver nitride, and silver halide. .
請求項10に記載の発明は、各種基板上にパターニングした高周波電磁波を吸収する熱分解性を有する粒子を、高周波電磁波照射を行うことで選択的に加熱し、熱分解性粒子を加熱分解相互融着して作成した導電路と基板の両者を含むことを特徴とする電子実装部品である。 The invention according to claim 10 selectively heats the thermally decomposable particles that absorb high frequency electromagnetic waves patterned on various substrates by irradiating the high frequency electromagnetic waves, and thermally decomposes the particles by thermal decomposition and mutual fusion. An electronic mounting component including both a conductive path and a substrate formed by wearing.
本発明は、前記粒子熱分解相互融着法を用いることを特徴とする導電材の形成方法である。 The present invention is a method for forming a conductive material, wherein the particle pyrolysis mutual fusion method is used.
本発明は、前記粒子熱分解相互融着法を用いることを特徴とする導電路の形成方法である。 The present invention is a method for forming a conductive path using the particle pyrolysis mutual fusion method.
本発明の導電路の形成方法において、回路パターンの形成方法がインクジェット法によることを特徴とする導電路の形成方法である。 In the method for forming a conductive path according to the present invention, the method for forming a circuit pattern is an ink-jet method.
本発明の導電路の形成方法において、回路パターンの形成方法がナノプリンティング法によることを特徴とする導電路の形成方法である。 In the method for forming a conductive path according to the present invention, the method for forming a circuit pattern is based on a nanoprinting method.
本発明の導電路の形成方法において、回路パターンの形成方法がナノインプリンティング法によることを特徴とする導電路の形成方法である。 In the method for forming a conductive path according to the present invention, the circuit pattern is formed by a nano-imprinting method.
本発明は、各種基板上にパターニングした高周波電磁波を吸収する熱分解性を有する粒子を、高周波電磁波照射を行うことで選択的に加熱し、熱分解性粒子を加熱分解相互融着して作成した導電路である。 The present invention was produced by selectively heating particles having thermal decomposability that absorb high frequency electromagnetic waves patterned on various substrates by performing high frequency electromagnetic wave irradiation, and thermally decomposing the particles by thermal decomposition and mutual fusion. It is a conductive path.
本発明は、各種基板上にパターニングした高周波電磁波を吸収する熱分解性を有する粒子を、高周波電磁波照射を行うことで選択的に加熱し、熱分解性粒子を加熱分解相互融着して作成したアンテナである。 The present invention was produced by selectively heating particles having thermal decomposability that absorb high frequency electromagnetic waves patterned on various substrates by performing high frequency electromagnetic wave irradiation, and thermally decomposing the particles by thermal decomposition and mutual fusion. It is an antenna.
本発明は、各種基板上にパターニングした高周波電磁波を吸収する熱分解性を有する粒子を、高周波電磁波照射を行うことで選択的に加熱し、熱分解性粒子を加熱分解相互融着して作成したバンプである。 The present invention was produced by selectively heating particles having thermal decomposability that absorb high frequency electromagnetic waves patterned on various substrates by performing high frequency electromagnetic wave irradiation, and thermally decomposing the particles by thermal decomposition and mutual fusion. It is a bump.
本発明は、各種基板上にパターニングした高周波電磁波を吸収する熱分解性を有する粒子を、高周波電磁波照射を行うことで選択的に加熱し、熱分解性粒子を加熱分解相互融着して作成したパッドである。 The present invention was produced by selectively heating particles having thermal decomposability that absorb high frequency electromagnetic waves patterned on various substrates by performing high frequency electromagnetic wave irradiation, and thermally decomposing the particles by thermal decomposition and mutual fusion. It is a pad.
本発明は、各種基板上にパターニングした高周波電磁波を吸収する熱分解性を有する粒子を、高周波電磁波照射を行うことで選択的に加熱し、熱分解性粒子を加熱分解相互融着して作成したビアである。 The present invention was produced by selectively heating particles having thermal decomposability that absorb high frequency electromagnetic waves patterned on various substrates by performing high frequency electromagnetic wave irradiation, and thermally decomposing the particles by thermal decomposition and mutual fusion. Beer.
本発明の方法を用いて、熱分解性を有する粒子を基板上に表面塗布又はパターニング後、所定の周波数の高周波電磁波を照射して選択加熱することにより、複雑な電子実装部品を、熱分解性を有する粒子を熱分解後相互融着させて形成することができる。この方法を用いることにより、基板上に導電路やアンテナ、バンプ、パッド、ビア等を含む電子部品を実装した電子基板を形成できる。このとき、電子部品形成部を選択的に加熱することから、電子部品実装基板には耐熱性を有する基板のみでなく、耐熱性の低い樹脂基板等を用いることが可能となる。 Using the method of the present invention, a thermally decomposable particle is coated on a substrate or patterned, and then irradiated with a high-frequency electromagnetic wave of a predetermined frequency to selectively heat a complex electronic packaging component to be thermally decomposable. It can be formed by thermally fusing the particles having a thermal decomposition. By using this method, it is possible to form an electronic substrate on which electronic components including conductive paths, antennas, bumps, pads, vias, and the like are mounted on the substrate. At this time, since the electronic component forming portion is selectively heated, not only a substrate having heat resistance but also a resin substrate having low heat resistance can be used as the electronic component mounting substrate.
以下に本発明の高周波電磁波照射を利用した熱分解粒子の加熱分解相互融着方法の詳細について説明する。導電路もしくはバンプ等の実装部品を構成する粒子材料として、熱分解性を有し且つ高周波電磁波を吸収する粒子を用い、その粒子を各種基板上に表面塗布もしくは表面パターニングを行う。基板上の表面塗布又はパターンニング法としては、インクジェット法、ナノプリンティング法、ナノインプリンティング法等の各種回路パターニング方法がある。ここで、導電路とは、そこに電流が流れたり、電磁誘導により電流が誘起されたりするもの等も含むものとし、閉回路も開回路も含み、さらに回路の形状やパターニングによる制約を受けないものとする。本願における回路も同様の意味で使用しているので、必ずしも閉回路に限らない。 The details of the thermal decomposition mutual fusion method of thermal decomposition particles using high frequency electromagnetic wave irradiation of the present invention will be described below. As a particle material constituting a mounting part such as a conductive path or a bump, particles having heat decomposability and absorbing high-frequency electromagnetic waves are used, and the particles are subjected to surface coating or surface patterning on various substrates. Examples of surface coating or patterning methods on a substrate include various circuit patterning methods such as an ink jet method, a nanoprinting method, and a nanoimprinting method. Here, the conductive path includes a current flowing therethrough or a current induced by electromagnetic induction, including a closed circuit and an open circuit, and not restricted by a circuit shape or patterning. And Since the circuit in this application is also used in the same meaning, it is not necessarily limited to a closed circuit.
また、熱分解性粒子をペースト状にして塗布する時には、目的とする電子部品や導電路の形成部に応じて、ペーストの組成を選択できる。ペーストには、少なくとも高周波電磁波を吸収し、加熱分解・相互融着する粒子が含まれることを必須要件とするが、この他に導電性樹脂又は有機溶媒、導電性樹脂及び有機溶媒を必要に応じて混合する。混合する目的は、高周波電磁波を照射する粒子の分散状態の改善や基板との密着性の改善などのためである。 Further, when applying the thermally decomposable particles in the form of a paste, the composition of the paste can be selected according to the target electronic component and the conductive path forming part. The paste must include at least particles that absorb high-frequency electromagnetic waves and are thermally decomposed and fused together. In addition to this, a conductive resin or an organic solvent, a conductive resin, and an organic solvent are used as necessary. And mix. The purpose of mixing is to improve the dispersion state of particles irradiated with high-frequency electromagnetic waves, improve the adhesion to the substrate, and the like.
高周波電磁波を吸収する熱分解性粒子として、金属−酸素結合を持つ無機及び有機金属化合物、金属−窒素結合を持つ無機及び有機金属化合物、金属−炭素結合を持つ無機及び有機金属化合物、金属−ハロゲン結合を持つ無機及び有機金属化合物の少なくとも一つを用いることができる。また、第1ステップの熱分解性粒子として、酸化銀、窒化銀、ハロゲン化銀の少なくとも一つを用いる。 As thermally decomposable particles that absorb high-frequency electromagnetic waves, inorganic and organometallic compounds having metal-oxygen bonds, inorganic and organometallic compounds having metal-nitrogen bonds, inorganic and organometallic compounds having metal-carbon bonds, metal-halogens At least one of an inorganic and organic metal compound having a bond can be used. In addition, at least one of silver oxide, silver nitride, and silver halide is used as the thermally decomposable grain in the first step.
次に、作成した熱分解性の粒子が塗布もしくは回路パターニングされた実装基板に対し、高周波電磁波照射を行うことで、熱分解性粒子を選択的に加熱し、この熱分解性粒子を加熱分解相互融着させる。この熱分解性粒子の加熱分解相互融着によって各種基板上に導電性部品を形成する。 Next, the thermally decomposable particles are selectively heated by irradiating the mounted substrate on which the thermally decomposable particles are coated or circuit-patterned with high frequency electromagnetic waves, and the thermally decomposable particles are thermally decomposed. Fuse. Conductive components are formed on various substrates by thermal decomposition mutual fusion of the thermally decomposable particles.
本発明の最も特記すべき特徴は次の二つである。一つは、金属(金属酸化物)微細粒子を用いた直接回路描画法において、その熱処理(粒子相互融着)工程に、加熱炉ではなく、高周波電磁波照射装置を用いた点であり、もう一つは、それに使用する粒子として、熱分解性でかつ高周波電磁波吸収性の材料を用いた点である。 The most notable features of the present invention are the following two. One is that, in the direct circuit drawing method using fine metal (metal oxide) particles, a high-frequency electromagnetic wave irradiation device is used instead of a heating furnace in the heat treatment (particle mutual fusion) process. One is that a thermally decomposable and high-frequency electromagnetic wave absorbing material is used as the particles used for the particles.
高周波電磁波照射による物質加熱は、高周波電磁波の物質内部での誘電現象に起因する。すなわち、誘電損失の大きい(高周波電磁波吸収性の)材料に照射された高周波電磁波は、材料を構成する分子を回転・衝突・振動・摩擦させ、エネルギーを失いながら物質内部を伝搬する。この時生じた分子の運動により材料が加熱される。 Material heating by high-frequency electromagnetic wave irradiation is caused by a dielectric phenomenon inside the substance of high-frequency electromagnetic wave. That is, the high frequency electromagnetic wave irradiated to the material with high dielectric loss (high frequency electromagnetic wave absorbing property) rotates, collides, vibrates and rubs the molecules constituting the material, and propagates inside the substance while losing energy. The material is heated by the movement of molecules generated at this time.
従来提案されていた熱風やスチームもしくは電熱線を用いた加熱炉による熱処理とこの高周波電磁波加熱との最も大きな相違点は、前者では外部から熱伝導によって材料によらず均一に熱が伝えられるのに対し、後者では、目的とする材料が直接加熱され、さらにこの加熱特性が物質により異なることに起因し、目的とする物質のみを選択的に加熱することが可能であるという点にある。 The biggest difference between the heat treatment by a heating furnace using hot air, steam or heating wire, which has been proposed in the past, and this high-frequency electromagnetic wave heating is that heat is transmitted uniformly from the outside by heat conduction regardless of the material. On the other hand, in the latter, the target material is directly heated, and furthermore, this heating characteristic varies depending on the substance, so that only the target substance can be selectively heated.
ここで高周波電磁波による加熱特性の物質による相違について説明する。高周波電磁波が誘電性物質の中で単位面積あたり熱となって消費されるエネルギー(P)は次式で表される。 Here, the difference between the heating characteristics due to the high-frequency electromagnetic wave due to the substance will be described. Energy (P) consumed by the high frequency electromagnetic wave as heat per unit area in the dielectric material is expressed by the following equation.
従って、高周波電磁波による物質の加熱され易さは、それぞれ物質固有の誘電率と誘電損失角の積(誘電損失係数)によって決まる。つまり、誘電損失係数が高い物質では、高周波電子波によって物質が高効率に加熱されるのに対し、誘電損失係数が低い物質では、ほとんど加熱されない。この誘電損失係数の値は、温度、周波数によって変化するが、一般に誘電損失係数の高い材料としては、水、エチレングリコール、遷移金属酸化物などが知られ、また誘電損失係数の低い材料としては、石英ガラス、ポリスチレン、ポリカーボネート、ポリイミド、テフロン(登録商標)などが知られている。 Therefore, the ease with which a substance is heated by high-frequency electromagnetic waves is determined by the product (dielectric loss coefficient) of the dielectric constant and dielectric loss angle inherent to the substance. That is, a substance having a high dielectric loss coefficient is heated with high efficiency by a high-frequency electron wave, whereas a substance having a low dielectric loss coefficient is hardly heated. The value of this dielectric loss coefficient varies depending on the temperature and frequency. Generally, water, ethylene glycol, transition metal oxide, etc. are known as materials having a high dielectric loss coefficient, and materials having a low dielectric loss coefficient are Quartz glass, polystyrene, polycarbonate, polyimide, Teflon (registered trademark), and the like are known.
本発明では、使用する粒子材料として誘電損失係数の高い遷移金属酸化物などの材料を用い、さらに下地基板として誘電損失係数の低いポリカーボネートなどの材料を選択することで、粒子に対する選択的加熱を実現している。 In the present invention, a material such as a transition metal oxide having a high dielectric loss coefficient is used as the particle material to be used, and a material such as polycarbonate having a low dielectric loss coefficient is selected as the base substrate, thereby realizing selective heating of the particles. is doing.
次に、本発明において、使用する粒子の材料として酸化銀(Ag2O)をはじめとする熱分解性の材料を選択したことによって期待される、自発的過剰加熱防止効果について説明する。これは、物質の熱分解による誘電損失係数の変化に着目したものである。例えば、Ag2Oでは約190℃前後で、2Ag2O→4Ag+O2の分解(還元)反応が生じることが知られている。 Next, the spontaneous overheating preventing effect expected by selecting a thermally decomposable material such as silver oxide (Ag 2 O) as the material of the particles used in the present invention will be described. This focuses on the change in the dielectric loss coefficient due to the thermal decomposition of the substance. For example, it is known that a decomposition (reduction) reaction of 2Ag 2 O → 4Ag + O 2 occurs at about 190 ° C. with Ag 2 O.
ここで、遷移金属酸化物であるAg2Oでは誘電損失係数は高く、高周波電磁波の照射により急速に加熱される一方で、高導電性遷移金属であるAgではこの誘電損失係数が極めて小さくほとんど加熱されない。ただし金属の場合、電磁誘導現象によって生じる電流に起因するジュール熱によって加熱されるために、高周波電磁波応答特性は厳密には式(1)では表せない。 Here, Ag 2 O, which is a transition metal oxide, has a high dielectric loss coefficient and is rapidly heated by irradiation with high-frequency electromagnetic waves, whereas Ag, which is a highly conductive transition metal, has an extremely small dielectric loss coefficient and is almost heated. Not. However, in the case of metal, since it is heated by Joule heat caused by the current generated by the electromagnetic induction phenomenon, the high-frequency electromagnetic wave response characteristic cannot be expressed strictly by Equation (1).
従って、Ag2O粒子に対して高周波電磁波を照射した場合、まずAg2Oが選択的に急速に加熱され、その加熱によりAg2Oが熱分解してAgに変化した後は、ほとんど加熱されないとい
う、自発的な過剰加熱防止機構が働くことになる。本発明におけるこの自発的過剰加熱防止機構は、実装回路材料の直接回路描画法において、耐熱温度の低い基板材料の使用を可能とするための重要な特徴の一つであると考えられる。
Therefore, when high frequency electromagnetic waves are irradiated to Ag 2 O particles, Ag 2 O is first selectively heated rapidly, and after heating, Ag 2 O is thermally decomposed and changed to Ag, it is hardly heated. That is, a spontaneous overheating prevention mechanism works. This spontaneous overheating prevention mechanism in the present invention is considered to be one of the important features for enabling the use of a substrate material having a low heat resistance temperature in the direct circuit drawing method of the mounted circuit material.
次に、本発明に使用する高周波電磁波の周波数fの影響について説明する。本発明で使用する照射する高周波電磁波として、周波数が1MHz<f<300GHzの範囲の高周波電磁波を用いる。これは電磁波照射により物質内部に誘電損失現象が生じると考えられる範囲である。適用周波数を1MHz<f<300GHzとするのは、周波数1MHz以下では、誘電損失効果自体がほとんど生じないからであり、また周波数300GHz以上では、照射された電磁波は極表面で減衰し、物質内部まで侵入しないためである。なお、この周波数範囲の高周波電磁波の中で、周波数範囲が300MHz<f<300GHzの範囲のものは、波長が短く、空間を自由に伝搬できることから、使用する電磁波としてより適していると考えられる。 Next, the influence of the frequency f of the high frequency electromagnetic wave used in the present invention will be described. The high frequency electromagnetic wave to be used in the present invention is a high frequency electromagnetic wave having a frequency in the range of 1 MHz <f <300 GHz. This is a range where dielectric loss phenomenon is considered to occur inside the substance due to electromagnetic wave irradiation. The reason why the applied frequency is 1 MHz <f <300 GHz is that the dielectric loss effect itself hardly occurs when the frequency is 1 MHz or less. Further, when the frequency is 300 GHz or more, the irradiated electromagnetic wave is attenuated on the pole surface and reaches the inside of the substance. This is to prevent intrusion. Of the high frequency electromagnetic waves in this frequency range, those having a frequency range of 300 MHz <f <300 GHz are considered to be more suitable as electromagnetic waves to be used because they have a short wavelength and can freely propagate in space.
さらに式(1)より、高周波電磁波が誘電性物質の中で単位面積あたり熱となって消費されるエネルギー(P)は、照射する周波数(f)の二乗に比例することが分かる。その意味からは、周波数が高いほど、物質表面の急速加熱には適していると言える。しかしながら、その一方で、高周波電磁波は物質内部では減衰する。入射電磁波が物質内で半減する深さ(D)は次式で表される。 Furthermore, it can be seen from the formula (1) that the energy (P) consumed by the high frequency electromagnetic wave as heat per unit area in the dielectric material is proportional to the square of the frequency (f) to be irradiated. In that sense, it can be said that the higher the frequency, the more suitable for rapid heating of the material surface. However, on the other hand, high-frequency electromagnetic waves are attenuated inside the substance. The depth (D) at which the incident electromagnetic wave is halved in the substance is expressed by the following equation.
この式から、照射電磁波の周波数が高くなるにつれて、物質内部への高周波電磁波の減衰距離は短くなることが分かる。従って、本発明では、作成する実装部品のサイズ(厚み)に応じて、照射する電磁波の周波数を調整すればよい。 From this equation, it can be seen that the attenuation distance of the high frequency electromagnetic wave into the substance becomes shorter as the frequency of the irradiated electromagnetic wave becomes higher. Therefore, in the present invention, the frequency of the electromagnetic wave to be irradiated may be adjusted according to the size (thickness) of the mounted component to be created.
次に、本発明に用いる粒子材料について説明する。本発明に使用する粒子の必要要件は、熱分解性でかつ高周波電磁波吸収特性のある材料であり、その要件を満たすものであれば、粒子の種類を問わないため、熱分解性粒子が、金属−酸素結合を持つ無機及び有機金属化合物、金属−窒素結合を持つ無機及び有機金属化合物、金属−炭素結合を持つ無機及び有機金属化合物、金属−ハロゲン結合を持つ無機及び有機金属ハロゲン化物等を用いることができる。さらに具体的には、Ag化合物を例にとると、熱分解性粒子としては酸化銀、窒化銀、ハロゲン化銀等を用いることができる。その中でも酸化銀(Ag2O)などは、比較的低温(約190℃)での熱分解性が報告されており、その意味でより適当であると考えられる。 Next, the particulate material used in the present invention will be described. The necessary requirements for the particles used in the present invention are materials that are thermally decomposable and have high-frequency electromagnetic wave absorption characteristics, and any type of particles can be used as long as they satisfy the requirements. -Inorganic and organometallic compounds having oxygen bonds, inorganic and organometallic compounds having metal-nitrogen bonds, inorganic and organometallic compounds having metal-carbon bonds, inorganic and organometallic halides having metal-halogen bonds, etc. be able to. More specifically, taking an Ag compound as an example, silver oxide, silver nitride, silver halide or the like can be used as the thermally decomposable particles. Among them, silver oxide (Ag 2 O) and the like have been reported to be thermally decomposable at a relatively low temperature (about 190 ° C.) and are considered to be more suitable in that sense.
ここで、熱分解特性を有する粒子のサイズに関して、特に制限は設けない。本発明の目的とする電子実装部品の作成、特に次世代高密度電子デバイスに対応した微細実装部品の作成という観点からは、平均粒径50μm以下のものが適当である。粒子径が大きいと、粒子充点率が低下し、その結果抵抗率が増加する。さらに、粒子の界面エネルギー、粒径減少による融点の低下、さらには高周波電磁波の浸透深さを考慮すると、粒子サイズはより小さい方が好ましく、例えば、平均粒径1nm〜100nmであると特に好ましいと考えられる。 Here, no particular limitation is imposed on the size of the particles having thermal decomposition characteristics. From the viewpoint of producing an electronic mounting component, which is the object of the present invention, particularly a fine mounting component corresponding to the next-generation high-density electronic device, those having an average particle size of 50 μm or less are suitable. When the particle diameter is large, the particle filling rate decreases, and as a result, the resistivity increases. Furthermore, considering the interfacial energy of the particles, the lowering of the melting point due to the reduction of the particle size, and the penetration depth of the high frequency electromagnetic wave, the particle size is preferably smaller, for example, the average particle size is particularly preferably 1 nm to 100 nm. Conceivable.
以下に本発明の実施例について説明する。 Examples of the present invention will be described below.
高周波電磁波を照射した場合の熱分解性物質(Ag2O)の選択加熱性、および過剰発熱防止効果について、以下の実験により確認した。熱分解性で且つ高周波電磁波を吸収する物質の一例として、Ag2Oナノ粒子ペースト(平均粒径50nm、藤倉化成(株)製)を準備した。次にこのAg2Oナノ粒子ペーストを一般的なポリイミド基板上に部分的に塗布した(図1参照)。なお塗布部分の膜厚は約50μmであった。 The selective heating property and the effect of preventing excessive heat generation of the thermally decomposable substance (Ag 2 O) when irradiated with high frequency electromagnetic waves were confirmed by the following experiment. As an example of a substance that is thermally decomposable and absorbs high-frequency electromagnetic waves, an Ag 2 O nanoparticle paste (average particle size 50 nm, manufactured by Fujikura Kasei Co., Ltd.) was prepared. Next, this Ag 2 O nanoparticle paste was partially applied onto a general polyimide substrate (see FIG. 1). The applied portion had a thickness of about 50 μm.
なお、本実施例では、熱分解性かつ高周波電磁波吸収性の粒子として、ペースト化したAg2Oナノ粒子を用いて実験を行ったが、本発明においては用いる粒子は必ずしもこのようなペースト状である必要はない。しかしながら、ペースト化した粒子を用いることで、ペーストに基板との密着性を高めることが可能となるため、高周波電磁波照射後に形成された導電材と基板との密着性が向上することが期待される。 In this example, the experiment was performed using the pasted Ag 2 O nanoparticles as the thermally decomposable and high frequency electromagnetic wave absorbing particles. However, the particles used in the present invention are not necessarily in such a paste form. There is no need. However, by using the pasted particles, it becomes possible to improve the adhesion between the paste and the substrate, so that it is expected that the adhesion between the conductive material formed after the high-frequency electromagnetic wave irradiation and the substrate is improved. .
次に、このAg2Oナノ粒子ペーストを部分的に塗布したポリイミド基板に対し、図2に示す低周波電磁波照射装置により、出力500Wにて、周波数(f)=1000Hzの低周波電磁波を発生させ、低周波電磁波の照射、および図3に示す高周波電磁波照射装置により出力500Wにて、周波数(f)=2.45GHzの高周波電磁波を発生させ、高周波電磁波の照射をそれぞれ行い、それら照射にともなう基板各部(A部〜E部)の温度変化を、サーモグラフィー(日本アビオニクス社製、型式:TVS−8500)を用いて測定した結果を図1に示す。但し、電磁波照射容器内にサーモグラフィーを設置することが不可能であったため、温度の測定はそれぞれ設定時間の電磁波照射後すぐに電磁波防護用扉を開放することで行った。測定結果を表1、表2に示す。 Next, a low-frequency electromagnetic wave having a frequency (f) = 1000 Hz is generated at an output of 500 W by a low-frequency electromagnetic wave irradiation apparatus shown in FIG. 2 on a polyimide substrate partially coated with this Ag 2 O nanoparticle paste. The low frequency electromagnetic wave irradiation and the high frequency electromagnetic wave irradiation apparatus shown in FIG. 3 generate a high frequency electromagnetic wave of frequency (f) = 2.45 GHz at an output of 500 W, and perform the irradiation of the high frequency electromagnetic wave, respectively. The result of measuring the temperature change of each part (A part-E part) using thermography (Nippon Avionics make, model: TVS-8500) is shown in FIG. However, since it was impossible to install the thermography in the electromagnetic wave irradiation container, the temperature was measured by opening the electromagnetic wave protection door immediately after the electromagnetic wave irradiation for a set time. The measurement results are shown in Tables 1 and 2.
先ず、表1(a)から、周波数(f)=1000Hzの電磁波を照射した場合、50sec照射後においても、Ag2O塗布部分の温度上昇は5℃以下であり、この周波数の電磁波照射においてAg2O粒子がほとんど加熱されないことが確認された。この結果は、低周波の電磁波照射は、本発明の目的とする熱分解性粒子の加熱分解相互融着には不適であることを示唆するものである。 First, from Table 1 (a), when an electromagnetic wave having a frequency (f) = 1000 Hz is irradiated, the temperature rise of the Ag 2 O coated portion is 5 ° C. or less even after 50 seconds of irradiation. It was confirmed that 2 O particles were hardly heated. This result suggests that low frequency electromagnetic wave irradiation is unsuitable for the thermal decomposition mutual fusion of the thermally decomposable particles as the object of the present invention.
一方で、表2より、周波数(f)=2.45GHzの高周波電磁波を照射した場合、Ag2O粒子を塗布した領域の顕著な温度上昇が確認された。この結果は、高周波電磁波を照射した場合の熱分解性物質(Ag2O)の選択的加熱性を示唆するものである。また同じく表2から、高周波電磁波照射に伴う熱分解性物質の温度上昇は190℃近傍で止まり、それ以上は加熱されないことも確認された。この結果は、加熱に伴うAg2Oの分解反応(2Ag2O→2Ag+O2)の進行により、電磁波の吸収量が減少したことに起因するものと考えられる。 On the other hand, from Table 2, the frequency (f) = when irradiated with 2.45GHz high frequency electromagnetic waves, significant temperature rise in the region coated with Ag 2 O particles was confirmed. This result suggests the selective heating property of the thermally decomposable substance (Ag 2 O) when irradiated with high-frequency electromagnetic waves. Similarly, from Table 2, it was confirmed that the temperature increase of the thermally decomposable substance accompanying high-frequency electromagnetic wave irradiation stopped at around 190 ° C. and no further heating was performed. This result is considered to be due to the decrease in the amount of electromagnetic waves absorbed due to the progress of the decomposition reaction of Ag 2 O accompanying heating (2Ag 2 O → 2Ag + O 2 ).
このように、この高周波電磁波の照射対象として、酸化銀をはじめとする各種熱分解性で且つ高周波電磁波を吸収する粒子を用いることにより、粒子のみを選択的に加熱され、
さらに加熱による熱分解の進行後過度の昇温が自発的に防止されることを確認した。
As described above, by using particles that absorb various high-frequency electromagnetic waves, such as silver oxide, as the irradiation target of the high-frequency electromagnetic waves, only the particles are selectively heated,
Furthermore, it was confirmed that excessive heating was prevented spontaneously after the progress of thermal decomposition by heating.
また、上記実験と同様に、図3に示す高周波電磁波の照射装置を用いて、Ag2Oナノ粒子ペーストを(部分的に)塗布したポリイミド基板に対し、出力500Wにて、周波数(f)=500GHzの超高周波電磁波を発生させ、超高周波電磁波の照射実験も行った。このサンプルに関しても、50sec照射後、サンプルのAg2Oナノ粒子ペースト領域が、相互融着していることが確認された。 Further, similarly to the above-described experiment, the frequency (f) = frequency was applied to a polyimide substrate on which the Ag 2 O nanoparticle paste was applied (partially) using the high-frequency electromagnetic wave irradiation apparatus shown in FIG. A 500 GHz ultra-high frequency electromagnetic wave was generated, and an irradiation experiment of the super-high frequency electromagnetic wave was also conducted. Also for this sample, it was confirmed that the Ag 2 O nanoparticle paste region of the sample was mutually fused after irradiation for 50 seconds.
高周波電磁波の照射による熱分解性物質(Ag2O)の加熱分解−粒子相互融着効果について、下記の実験により確認した。まず、上記の高周波電磁波照射実験終了後の各サンプルについて、ZRD(粉末X線回折装置、株式会社リガク製)によって、結晶構造の同定を行った。周波数(f)=1000Hzの電磁波を照射したサンプルについては、照射時間によらず、Ag2Oのみの存在を示すピークが確認された。これは、周波数(f)=1000Hzの低周波電磁波の照射では、加熱分解が進行しなかったことを示唆するものである。 The effect of thermal decomposition of the thermally decomposable substance (Ag 2 O) by irradiation with high frequency electromagnetic waves and particle mutual fusion was confirmed by the following experiment. First, about each sample after completion | finish of said high frequency electromagnetic wave irradiation experiment, the crystal structure was identified by ZRD (powder X-ray-diffraction apparatus, Rigaku Corporation make). For samples irradiated with an electromagnetic wave of frequency (f) = 1000 Hz does not depend on the irradiation time, the peak indicating the presence of Ag 2 O only was confirmed. This suggests that the thermal decomposition did not proceed with the irradiation of the low frequency electromagnetic wave having the frequency (f) = 1000 Hz.
次に周波数(f)=2.45GHzの電磁波を照射したサンプルについては、照射時間によって得られるX線回折でのピークの位置が変化した。照射時間0secおよび10secのサンプルについては、Ag2Oのみの存在を示すピークが確認されたのに対し、照射時間20secのサンプルについては、Ag2OおよびAgのピークが確認され、さらに、照射時間30sec以上のサンプルについては、Agのピークのみが確認された。この結果は、高周波電磁波照射にともなう加熱によって、熱分解性物質(Ag2O)の加熱分解が進行するという事実を示唆するものである。 Next, for the sample irradiated with the electromagnetic wave having the frequency (f) = 2.45 GHz, the peak position in the X-ray diffraction obtained by the irradiation time changed. For samples with an irradiation time of 0 sec and 10 sec, a peak indicating the presence of only Ag 2 O was confirmed, whereas for a sample with an irradiation time of 20 sec, Ag 2 O and Ag peaks were confirmed. Only the Ag peak was confirmed for the samples of 30 sec or longer. This result suggests the fact that the thermal decomposition of the thermally decomposable substance (Ag 2 O) proceeds by the heating accompanying the high frequency electromagnetic wave irradiation.
さらに周波数(f)=500GHzの電磁波を50sec照射したサンプルについては、Ag2OおよびAgのピークが確認された。これは部分的(表面)においてのみAg2Oの熱分解が進行したものによると考えられる。 Furthermore, Ag 2 O and Ag peaks were confirmed for the sample irradiated with electromagnetic waves of frequency (f) = 500 GHz for 50 seconds. This is considered to be due to the fact that the thermal decomposition of Ag 2 O progressed only partially (surface).
さらに、加熱にともなう粒子相互融着効果を確認することを目的に、周波数(f)=2.45GHzの電磁波を照射したサンプル(照射時間50sec)について電気抵抗測定を行った。測定は、デジタルマルチメータ(Keithley社製、型式:DMM2000)、直流安定化電源(ケンウッド社製、形式:PAR20−4H)を用いて、直流四端子法によって行った。 Furthermore, for the purpose of confirming the effect of particle mutual fusion accompanying heating, electrical resistance measurement was performed on a sample (irradiation time 50 sec) irradiated with an electromagnetic wave having a frequency (f) = 2.45 GHz. The measurement was performed by a DC four-terminal method using a digital multimeter (Keithley, model: DMM2000) and a DC stabilized power supply (Kenwood, model: PAR20-4H).
その結果、この周波数(f)=2.45GHzの電磁波を50sec照射したサンプルに対しては、ρ=5.0μΩ・cmという高い導電性が確認された。この結果は、高周波電磁波の照射によりAg2Oの加熱分解(還元)粒子相互融着効果が進行し、Agの低抵抗の導電膜が形成されるという事実を示唆するものである。 As a result, a high conductivity of ρ = 5.0 μΩ · cm was confirmed for the sample irradiated with the electromagnetic wave having the frequency (f) = 2.45 GHz for 50 seconds. This result suggests the fact that the thermal decomposition (reduction) particle mutual fusion effect of Ag 2 O proceeds by irradiation with high-frequency electromagnetic waves, and a low-resistance conductive film of Ag is formed.
なお、同様の効果は同じくポリイミド基板上にバンプ状に形成した円柱突起(円柱状、高さ約1mm、直径2mm)においても確認され、形状によらず本方法が適用出来ることが分かった。 The same effect was also confirmed in a cylindrical protrusion (cylindrical shape, height of about 1 mm, diameter of 2 mm) formed in a bump shape on the polyimide substrate, and it was found that this method can be applied regardless of the shape.
さらに、ポリイミド基板上に形成したAg2Oナノ粒子ペーストを用いてパッド、ビア等を形成し、効果を確認したところ高い導電性が得られ、これらについても同様の効果が確認された。 Furthermore, pads, vias, and the like were formed using an Ag 2 O nanoparticle paste formed on a polyimide substrate, and when the effects were confirmed, high conductivity was obtained, and similar effects were confirmed for these.
1.ポリイミド基板
2.Ag2O粒子を塗布した領域
3.電磁波照射容器
4.導線
5.加熱電極
6.ターンテーブル
7.電磁波
1. 1. polyimide substrate 2. Area where Ag 2 O particles are applied 3. Electromagnetic wave
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