JP2006120730A - Wiring structure using multilayered carbon nanotube for interlayer wiring, and its manufacturing method - Google Patents

Wiring structure using multilayered carbon nanotube for interlayer wiring, and its manufacturing method Download PDF

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JP2006120730A
JP2006120730A JP2004304667A JP2004304667A JP2006120730A JP 2006120730 A JP2006120730 A JP 2006120730A JP 2004304667 A JP2004304667 A JP 2004304667A JP 2004304667 A JP2004304667 A JP 2004304667A JP 2006120730 A JP2006120730 A JP 2006120730A
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Daiyu Kondo
大雄 近藤
Mizuhisa Nihei
瑞久 二瓶
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Fujitsu Ltd
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<P>PROBLEM TO BE SOLVED: To obtain a wiring structure capable of turning into low resistance, where a multilayered carbon nanotube (CNT) is used for interlayer wiring of two or more conductive layers. <P>SOLUTION: In the wiring structure, the multilayered CNT is used for the interlayer wiring of two or more conductive layers. A plurality of annular cut areas formed in concentric circular states by a graphene sheet contained in the multilayered CNT at the end of the CNT on the side far from the growing base point of the CNT is respectively brought into contact with the conductive layers. Since the conductive layers and graphene sheet are brought into contact with each other, without going through the intermediary of the portion of the cap layer of the CNT, the contact resistances between the conductive layers and graphene sheet become smaller than those of the conventional types. <P>COPYRIGHT: (C)2006,JPO&NCIPI

Description

本発明は、ナノカーボンを用いた半導体製造技術に関し、特に層間配線に多層カーボンナノチューブ（多層ＣＮＴ）を用いる配線構造及びその製造方法に関する。   The present invention relates to a semiconductor manufacturing technology using nanocarbon, and more particularly to a wiring structure using multi-walled carbon nanotubes (multi-walled CNT) for interlayer wiring and a manufacturing method thereof.

この種の技術分野では、今後のデバイスの微細化を実現するために、ナノカーボンを利用することが有望視されている。特に、多層ＣＮＴは、単層ＣＮＴとは異なり、優れた導電性を示し、集積回路の配線に使用することが期待されている（このようなＣＮＴについては、例えば特許文献１参照。）。   In this kind of technical field, it is considered promising to use nanocarbon in order to realize future miniaturization of devices. In particular, multi-walled CNTs, unlike single-walled CNTs, exhibit excellent conductivity and are expected to be used for wiring of integrated circuits (see, for example, Patent Document 1 for such CNTs).

図１は、２つの導電層の層間配線に多層ＣＮＴを用いる配線構造を製造するためのいくつかの工程を示す。図１（Ａ）に示される工程では、例えば銅（Ｃｕ）など１種類以上の金属元素より成る第１の導電層１２に、層間絶縁膜１４が成膜される。図１（Ｂ）に示される工程では、層間絶縁膜１４の所定の部分にビア１３が形成され、第１の導電層１２が露出するようにする。露出した導電層１２の部分には、例えばニッケル（Ｎｉ）のような触媒金属１５が設けられる。図１（Ｃ）に示される工程では、例えば５００℃程度の雰囲気でアセチレンガス等が反応炉内に供給される。これにより、触媒金属１５を基点にして、多層ＣＮＴがビア１３に沿って成長する。触媒金属１５の種類、熱処理の温度等を制御することで、成長するＣＮＴの種類や大きさ等を調整することができる。図１（Ｄ）に示される工程では、層間絶縁膜１４及び多層ＣＮＴ１６上に、例えば銅など１種類以上の金属元素より成る第２の導電層１８が成膜される。こうして、第１及び第２の導電層１２，１８の層間配線に多層ＣＮＴ１６を用いた配線構造を得ることができる（この種の配線構造については、例えば非特許文献１参照。）。
特開２００３−８１６２１号公報 Ｍ．Ｎｉｈｅｉ，ｅｔ ａｌ．，“Ｓｉｍｕｌｔａｎｅｏｕｓ Ｆｏｒｍａｔｉｏｎ ｏｆ Ｍｕｌｔｉｗａｌｌ Ｃａｒｂｏｎ Ｎａｎｏｔｕｂｅｓ ａｎｄ ｔｈｅｉｒ Ｅｎｄ−Ｂｏｎｄｅｄ Ｏｈｍｉｃ Ｃｏｎｔａｃｔｓ ｔｏ Ｔｉ Ｅｌｅｃｔｒｏｄｅｓ ｆｏｒ Ｆｕｔｕｒｅ ＵＬＳＩ Ｉｎｔｅｒｃｏｎｎｅｃｔｉｏｎｓ”，Ｊａｐａｎｅｓｅ Ｊｏｕｒｎａｌ ｏｆ Ａｐｐｌｉｅｄ Ｐｈｙｓｉｃｓ，Ｖｏｌ．４３，Ｎｏ．４Ｂ，２００４，ｐｐ．１８５６−１８５９ FIG. 1 shows several steps for manufacturing a wiring structure using multilayer CNTs for interlayer wiring of two conductive layers. In the step shown in FIG. 1A, an interlayer insulating film 14 is formed on the first conductive layer 12 made of one or more metal elements such as copper (Cu). In the step shown in FIG. 1B, a via 13 is formed in a predetermined portion of the interlayer insulating film 14 so that the first conductive layer 12 is exposed. A catalytic metal 15 such as nickel (Ni) is provided on the exposed portion of the conductive layer 12. In the step shown in FIG. 1C, acetylene gas or the like is supplied into the reactor in an atmosphere of about 500 ° C., for example. Thereby, the multilayer CNT grows along the via 13 with the catalyst metal 15 as a base point. By controlling the type of catalyst metal 15 and the temperature of the heat treatment, the type and size of the growing CNT can be adjusted. In the step shown in FIG. 1D, a second conductive layer 18 made of one or more kinds of metal elements such as copper is formed on the interlayer insulating film 14 and the multilayer CNT 16. In this way, it is possible to obtain a wiring structure using the multilayer CNT 16 for the interlayer wiring of the first and second conductive layers 12 and 18 (see, for example, Non-Patent Document 1 for this type of wiring structure).
JP 2003-81621 A M.M. Nihei, et al. , “Simultaneous Formation of Multiwall Carbon Nanotubes and the End End-Bonded Ohmic Contacts to Ti Electrodes for Future Amplitudes, Japan, USA”. 43, no. 4B, 2004, pp. 1856-1859

ところで、ＣＮＴは、グラフェンシートと呼ばれる側壁と、キャップ層と呼ばれる先端部分を有する。多層ＣＮＴでは、グラフェンシート及びキャップ層が入れ子状に幾層にも重なった構造が形成される。このような多層ＣＮＴは、それ自体は導電性を有するが、それが層間配線に利用される場合には、導電層との間の接触抵抗が大きくなるという問題がある。この場合に、非特許文献１記載発明は、成長基点側の導電層１２にチタニウム（Ｔｉ）のような所定の金属より成る層を形成し、そこに触媒金属を設けて多層ＣＮＴを成長させることで、多層ＣＮＴ１６と導電層１２との間の接触抵抗を減少させようとしている。しかしながら、上部の導電層１８側との間では、主にキャップ層と導電層１８との間の接触抵抗が大きいことに起因して、配線構造全体としての抵抗値が大きくなってしまうことが懸念される。   By the way, CNT has a side wall called a graphene sheet and a tip part called a cap layer. In multi-walled CNTs, a structure in which graphene sheets and cap layers are nested and overlapped is formed. Such multi-walled CNTs themselves have conductivity, but when they are used for interlayer wiring, there is a problem that the contact resistance with the conductive layer increases. In this case, according to the invention described in Non-Patent Document 1, a layer made of a predetermined metal such as titanium (Ti) is formed on the conductive layer 12 on the growth base side, and a catalyst metal is provided thereon to grow a multilayer CNT. Thus, the contact resistance between the multilayer CNT 16 and the conductive layer 12 is to be reduced. However, there is a concern that the resistance value of the entire wiring structure may increase due to the large contact resistance between the cap layer and the conductive layer 18 between the upper conductive layer 18 side. Is done.

また、ＣＮＴの成長の際に、プロセス条件に依存して、図１（Ｄ）右側の拡大図に示されるように、ＣＮＴの周囲にアモルファスカーボンが付着することがある。更には、このようなアモルファスカーボンが、ＣＮＴの多くの部分を包囲してしまうこともある。アモルファスカーボンの導電性は低いので、そのような余分な物質がＣＮＴに付着すると、導電層１８との間の抵抗値が大きくなってしまう。特許文献１記載発明は、ＣＮＴに付着したアモルファスカーボンを除去する技術を開示している。しかし、特許文献１記載発明は、ＣＮＴを乳鉢に入れて物理的機械的にＣＮＴに付着した余分な物質を除去するので、ビアの中に成長させたＣＮＴに対する余分な物質の除去には使用できない。   Further, during the growth of CNTs, depending on the process conditions, amorphous carbon may adhere around the CNTs as shown in the enlarged view on the right side of FIG. Furthermore, such amorphous carbon may surround many parts of the CNT. Since the conductivity of amorphous carbon is low, if such extra material adheres to the CNTs, the resistance value with respect to the conductive layer 18 increases. The invention described in Patent Document 1 discloses a technique for removing amorphous carbon adhering to CNTs. However, the invention described in Patent Document 1 cannot be used to remove excess material from CNT grown in vias because CNT is placed in a mortar and mechanically and mechanically attached to CNT is removed. .

本発明は、上記の問題点に鑑みてなされたものであり、その課題は、２以上の導線層の層間配線に多層ＣＮＴが使用される配線構造の低抵抗化を図ることの可能な配線構造及びその製造方法を提供することである。   The present invention has been made in view of the above-mentioned problems, and its problem is a wiring structure capable of reducing the resistance of a wiring structure in which a multilayer CNT is used for an interlayer wiring of two or more conductor layers. And a method of manufacturing the same.

本発明では、２以上の導電層の層間配線に多層カーボンナノチューブが使用される配線構造が使用される。前記多層カーボンナノチューブに含まれるグラフェンシートにより形成され且つ前記多層カーボンナノチューブの成長基点から遠い側の端部に同心状に形成される複数の環状の切り口が、導電層にそれぞれ接触する。   In the present invention, a wiring structure in which multi-walled carbon nanotubes are used for interlayer wiring of two or more conductive layers is used. A plurality of annular cuts formed by a graphene sheet contained in the multi-walled carbon nanotube and concentrically formed at an end portion far from the growth base point of the multi-walled carbon nanotube are in contact with the conductive layer.

本発明によれば、２以上の導線層の層間配線に多層ＣＮＴが使用される配線構造の低抵抗化を図ることができる。   According to the present invention, it is possible to reduce the resistance of a wiring structure in which a multilayer CNT is used for an interlayer wiring of two or more conductor layers.

本発明の一態様によれば、
第１の導電層上に設けられた絶縁層に、前記第１の導電層に至るビアが形成され、
前記ビアを貫通する多層ＣＮＴが形成され、
前記多層ＣＮＴを含む構造が、酸素を含む雰囲気で加熱され、
前記絶縁層及び前記多層ＣＮＴ上に第２の導電層が成膜されることで、配線構造が作成される。 According to one aspect of the invention,
Vias reaching the first conductive layer are formed in the insulating layer provided on the first conductive layer,
A multilayer CNT penetrating the via is formed,
The structure including the multilayer CNT is heated in an atmosphere including oxygen,
A wiring structure is created by forming a second conductive layer on the insulating layer and the multilayer CNT.

前記多層ＣＮＴを含む構造が、酸素を含む雰囲気で加熱されると、多層ＣＮＴの先端部分と酸素が反応し、その先端部分が開端され、グラフェンシートにより形成される複数の環状の端部が露出する。この複数の環状の端部に接触するように第２の導電層が成膜される。第２の導電層は、ＣＮＴのキャップ層の部分を介さずにチューブのグラフェンシート側に接するので、導電層とＣＮＴとの接触抵抗は従来よりも小さくなる。また、この開端の工程にて、多層ＣＮＴに付着した余分な物質（アモルファスカーボン）も、酸素と反応することで除去される。   When the structure including the multi-walled CNT is heated in an atmosphere containing oxygen, the front-end portion of the multi-walled CNT reacts with oxygen, the front-end portion is opened, and a plurality of annular ends formed by the graphene sheet are exposed. To do. A second conductive layer is formed so as to be in contact with the plurality of annular ends. Since the second conductive layer is in contact with the graphene sheet side of the tube without passing through the cap layer portion of the CNT, the contact resistance between the conductive layer and the CNT is smaller than in the conventional case. Also, in this open end step, excess substances (amorphous carbon) adhering to the multi-walled CNT are also removed by reacting with oxygen.

本発明の一態様によれば、前記多層ＣＮＴの内部に、所定の導電性物質より成る層間配線部材が設けられる。本発明の一態様では、その所定の導電性物質は、フラーレン又は金属元素より成る。チューブの中空部分に導電性物質が充填されることで、導電層とＣＮＴとの間の電気抵抗を更に小さくすることができる。   According to one aspect of the present invention, an interlayer wiring member made of a predetermined conductive material is provided in the multilayer CNT. In one embodiment of the present invention, the predetermined conductive material is made of fullerene or a metal element. By filling the hollow portion of the tube with the conductive material, the electrical resistance between the conductive layer and the CNT can be further reduced.

本発明の一態様によれば、前記多層カーボンナノチューブの成長基点側とは異なる端部側の導電層が、所定の金属元素より成るコンタクト層と、コンタクト層とは異なる導電性の層より成る。本発明の一態様によれば、所定の金属元素は、チタニウム、モリブデン、タンタル、パラジウム、ルテニウム、アルミニウム、白金、金及び銅を含む群から選択された少なくとも１つの元素を含む。これにより、ＣＮＴとの間の電気抵抗を低減することができる。   According to an aspect of the present invention, the conductive layer on the end side different from the growth base point side of the multi-walled carbon nanotube includes a contact layer made of a predetermined metal element and a conductive layer different from the contact layer. According to one aspect of the present invention, the predetermined metal element includes at least one element selected from the group including titanium, molybdenum, tantalum, palladium, ruthenium, aluminum, platinum, gold, and copper. Thereby, the electrical resistance between CNTs can be reduced.

本発明の一態様によれば、前記コンタクト層が、多層に形成される。本発明の一態様によれば、前記コンタクト層が、タンタル及びチタニウムより成る２層から形成される。これにより、例えば、高温の製造工程中に、導電層中の元素がコンタクト層側に拡散することを抑制することが可能になる。   According to an aspect of the present invention, the contact layer is formed in multiple layers. According to an aspect of the present invention, the contact layer is formed of two layers made of tantalum and titanium. Thereby, for example, it becomes possible to suppress diffusion of elements in the conductive layer to the contact layer side during a high-temperature manufacturing process.

本発明の一態様によれば、前記熱処理を施す前に、水素雰囲気中で、前記多層カーボンナノチューブを含む構造に熱処理が施される。これにより、ＣＮＴに与える影響を少なくしつつ、余分なアモルファスカーボンを除去することができる。   According to one aspect of the present invention, the heat treatment is performed on the structure including the multi-walled carbon nanotubes in a hydrogen atmosphere before the heat treatment. Thereby, excess amorphous carbon can be removed while reducing the influence on CNTs.

図２は、２つの導電層の層間配線に多層ＣＮＴを用いる配線構造を製造する方法におけるいくつかの工程を示す。簡単のため、上下２層の導電層に対する層間配線構造が説明されるが、更に多くの導電層を有する配線構造に本発明を使用することもできる。図２（Ａ）に示される工程では、第１の導電層２０２に、層間絶縁膜２０４が成膜される。第１の導電層２０２は、用途に応じて、例えば銅（Ｃｕ）、金（Ａｕ）その他任意の導電性物質から構成することができる。   FIG. 2 shows several steps in a method of manufacturing a wiring structure using multilayer CNTs for interlayer wiring of two conductive layers. For simplicity, an interlayer wiring structure for two upper and lower conductive layers is described, but the present invention can also be used for a wiring structure having more conductive layers. In the step shown in FIG. 2A, an interlayer insulating film 204 is formed over the first conductive layer 202. The first conductive layer 202 can be made of, for example, copper (Cu), gold (Au), or any other conductive material depending on the application.

図２（Ｂ）に示される工程では、層間絶縁膜２０４の所定の部分にビア２０６が形成され、第１の導電層２０２が露出するようにする。ビア２０６は、フォトリソグラフィ法のような既存の技術を用いて形成することができる。導電層２０２の露出した部分には、例えばニッケル（Ｎｉ）、コバルト（Ｃｏ）、鉄（Ｆｅ）のような触媒金属２０８が設けられる。このような触媒金属２０８は、ビア２０６を形成した後に設けてもよいし、ビア２０６を形成する前に事前に設けておいてもよい。後者の場合は、第１の導電層２０２に層間絶縁膜２０４が形成される前に、第１の導電層２０２に触媒金属が設けられることになる。本実施例では、銅より成る第１の導電層２０２上にタンタル（Ｔａ）及びチタニウム（Ｔｉ）より成る層（図示せず）が成膜され、さらにそのチタニウム層に触媒金属が設けられる。タンタル層により第１の導電層２０２を構成する銅の拡散が防止される。また、後に形成される多層ＣＮＴと第１の導電層２０２との間にチタニウム層が介在することによって、多層ＣＮＴ及び第１の導電層２０２間の電気抵抗が小さく抑制される。   In the step shown in FIG. 2B, a via 206 is formed in a predetermined portion of the interlayer insulating film 204 so that the first conductive layer 202 is exposed. The via 206 can be formed using an existing technique such as a photolithography method. The exposed portion of the conductive layer 202 is provided with a catalytic metal 208 such as nickel (Ni), cobalt (Co), or iron (Fe). Such a catalyst metal 208 may be provided after the via 206 is formed, or may be provided in advance before the via 206 is formed. In the latter case, a catalyst metal is provided on the first conductive layer 202 before the interlayer insulating film 204 is formed on the first conductive layer 202. In this embodiment, a layer (not shown) made of tantalum (Ta) and titanium (Ti) is formed on the first conductive layer 202 made of copper, and a catalyst metal is further provided on the titanium layer. The diffusion of copper constituting the first conductive layer 202 is prevented by the tantalum layer. Further, since the titanium layer is interposed between the multilayer CNT formed later and the first conductive layer 202, the electrical resistance between the multilayer CNT and the first conductive layer 202 is suppressed to be small.

図２（Ｃ）に示される工程では、例えば５００℃程度の雰囲気でアセチレンガス（Ｃ２Ｈ２）等が反応炉内に供給される。これにより、触媒金属２０８は微粒子状になり、その微粒子に炭素が吸収される。微粒子による炭素の吸収が飽和すると、微粒子を基点にして、多層ＣＮＴがビアに沿って成長する。触媒金属２０８の種類、熱処理の温度、触媒金属の下地層（チタニウム層）の膜厚等を制御することで、成長するＣＮＴの種類や大きさ等を調整することができる。本実施例では、最も外側の直径が５乃至２０ｎｍ程度の多層ＣＮＴがビア２０６内に多数形成される。図示の例では、６つの多層ＣＮＴが模式的に描かれている。ＣＮＴの成長を促進させる工程は、多層ＣＮＴ２１０が層間絶縁膜２０４の膜厚程度に成長するまで継続される。 In the step shown in FIG. 2C, acetylene gas (C 2 H 2 ) or the like is supplied into the reactor in an atmosphere of about 500 ° C., for example. As a result, the catalytic metal 208 is in the form of fine particles, and carbon is absorbed by the fine particles. When the absorption of carbon by the fine particles is saturated, the multi-walled CNT grows along the vias starting from the fine particles. By controlling the type of catalyst metal 208, the temperature of the heat treatment, the thickness of the underlayer (titanium layer) of the catalyst metal, the type and size of the grown CNTs can be adjusted. In this embodiment, a number of multi-walled CNTs having an outermost diameter of about 5 to 20 nm are formed in the via 206. In the illustrated example, six multilayer CNTs are schematically drawn. The process of promoting the growth of CNT is continued until the multilayer CNT 210 is grown to the thickness of the interlayer insulating film 204.

図２（Ｄ）に示される工程では、所定のプロセス条件の下で熱処理が行われる。この工程は、例えば、５００℃程度の温度で、真空排気後に反応炉に導入された１キロパスカル程度の酸素の雰囲気中で、５分乃至１０分間行われる。これにより、多層ＣＮＴ２１０の先端部分（キャップ層）が、酸素と反応して除去され、構造的に閉じているＣＮＴの端部が開端される（図３参照）。ＣＮＴの先端部分は、６員環で安定的に構成される側壁部（グラフェンシート）とは異なり、５員環を含む比較的不安定な構造を有する。従って、酸素と反応する際には、先端部分が優先して反応し、最外殻から最内殻まで順に開端されてゆく。開端された後の多層ＣＮＴは、図２（Ｄ）右側の拡大図に模式的に示されるような形状を有する。   In the step shown in FIG. 2D, heat treatment is performed under predetermined process conditions. This step is performed, for example, at a temperature of about 500 ° C. for 5 to 10 minutes in an atmosphere of oxygen of about 1 kilopascal introduced into the reactor after evacuation. Thereby, the front-end | tip part (cap layer) of multilayer CNT210 reacts with oxygen, is removed, and the edge part of CNT structurally closed is opened (refer FIG. 3). Unlike the side wall portion (graphene sheet) that is stably composed of a 6-membered ring, the tip portion of the CNT has a relatively unstable structure including a 5-membered ring. Therefore, when reacting with oxygen, the tip portion reacts preferentially, and the ends are sequentially opened from the outermost shell to the innermost shell. The multilayer CNT after being opened has a shape as schematically shown in the enlarged view on the right side of FIG.

図２（Ｅ）に示される工程では、層間絶縁膜２０４及び多層ＣＮＴ２１０上に、例えば銅より成る第２の導電層２１２が成膜される。導電層の成膜は、例えばスパッタリング法を用いて行うことができる。こうして、第１及び第２の導電層２０２，２１２の層間配線に多層ＣＮＴ２１０を用いた配線構造を得ることができる。   In the step shown in FIG. 2E, a second conductive layer 212 made of, for example, copper is formed on the interlayer insulating film 204 and the multilayer CNT 210. The conductive layer can be formed by using, for example, a sputtering method. Thus, a wiring structure using the multilayer CNT 210 for the interlayer wiring between the first and second conductive layers 202 and 212 can be obtained.

本実施例によれば、図２（Ｄ）右側に示されるような、複数の環状の端部が第２の導電層２１２にそれぞれ接触するので、最外殻の先端部分のみが導電層に接触していた従来例よりも低い接触抵抗が得られる。   According to the present embodiment, as shown in the right side of FIG. 2D, a plurality of annular ends are in contact with the second conductive layer 212, respectively, so that only the tip portion of the outermost shell is in contact with the conductive layer. The contact resistance is lower than that of the conventional example.

ところで、背景技術の図１（Ｄ）に関連して説明されたように、ビアに沿って成長したＣＮＴには、余分な物質（アモルファスカーボン）が付着していることがある。しかしながら、本実施例では、図２（Ｄ）の酸化工程にて、そのようなアモルファスカーボンが除去される。アモルファスカーボンはＣＮＴよりも不安定な構造を有し、酸素と反応しやすいからである。従って、図２（Ｄ）の酸化工程では、多層ＣＮＴが開端されることに加えて、アモルファスカーボンの除去も行われる。アモルファスカーボンを除去する観点からは、上記のように、酸素雰囲気中で製造途中の配線構造を加熱してもよいし、或いは配線構造を酸素プラズマにさらしてもよい。前者は配線構造自体を高温に加熱しなければならないが、後者は室温で行うことができる。従って、配線構造に与える熱的な影響を少なくする観点からは、後者の酸素プラズマを用いる方が有利であろう。   By the way, as described with reference to FIG. 1D of the background art, an extra substance (amorphous carbon) may be attached to the CNT grown along the via. However, in this embodiment, such amorphous carbon is removed in the oxidation step of FIG. This is because amorphous carbon has a more unstable structure than CNT and easily reacts with oxygen. Therefore, in the oxidation process of FIG. 2D, in addition to the opening of the multi-layer CNT, the removal of amorphous carbon is also performed. From the viewpoint of removing amorphous carbon, the wiring structure being manufactured may be heated in an oxygen atmosphere as described above, or the wiring structure may be exposed to oxygen plasma. The former has to heat the wiring structure itself to a high temperature, while the latter can be performed at room temperature. Therefore, it is more advantageous to use the latter oxygen plasma from the viewpoint of reducing the thermal influence on the wiring structure.

また、図２（Ｃ）及び（Ｄ）に示される工程の間に、例えば５００乃至６００℃の温度で、真空排気後に反応炉に導入された１キロパスカル程度の水素の雰囲気中で熱処理を行うことで、アモルファスカーボンを除去してもよい。アモルファスカーボンは、水素とも反応しやすいからである。但し、ＣＮＴの先端部分との反応性に関しては、水素は酸素より弱い反応性を示すので、水素を用いるこの工程でＣＮＴのキャップ層部分を除去することは困難であろう。従って、この工程は、多層ＣＮＴにさほど影響を与えずに、余分な物質を除去する観点からは好都合であろう。   Also, during the steps shown in FIGS. 2C and 2D, heat treatment is performed in a hydrogen atmosphere of about 1 kilopascal introduced into the reaction furnace after evacuation at a temperature of 500 to 600 ° C., for example. Thus, amorphous carbon may be removed. This is because amorphous carbon easily reacts with hydrogen. However, regarding the reactivity with the tip portion of the CNT, since hydrogen shows a weaker reactivity than oxygen, it will be difficult to remove the cap layer portion of the CNT in this process using hydrogen. Therefore, this step may be advantageous from the viewpoint of removing excess material without significantly affecting the multi-walled CNTs.

上述したように、多層ＣＮＴは、筒状のチューブが幾重にも重なった構造を有するので、最も内側のＣＮＴの内部は中空である。本発明の第２実施例では、この中空の領域に、導電性の電流経路が設けられる。   As described above, the multi-walled CNT has a structure in which the cylindrical tubes overlap each other, so that the inside of the innermost CNT is hollow. In the second embodiment of the present invention, a conductive current path is provided in this hollow region.

図４の左側の図は、多層ＣＮＴの一端（終端側）が開端された直後の様子を示し、これは図２（Ｄ）の工程が終了した時点の様子に相当する。次に、最も内側のＣＮＴ内部の中空の領域内に、銅のような導電性物質が導入される。導電性物質の導入は、分子線エピタキシ（ＭＢＥ）、気相成長法等の手法を用いて行うことができる。中空の領域内は構造的に安定で低エネルギ状態であり、雰囲気中に漂う導電性物質はその領域内に入りやすいからである。その結果、図４右側に示されるように、最も内側のＣＮＴ内部を導電性物質で充填することができる。以後、図２（Ｅ）に示されるような工程を行うことで、配線構造が完成する。なお、スパッタリング等により第２の導電層を成膜する際に多層ＣＮＴ上に飛来する導電性物質は、多層ＣＮＴの直径より大きな塊状の物質であるので、そのような物質は多層ＣＮＴの中空領域には内包されにくいであろう。   The diagram on the left side of FIG. 4 shows a state immediately after one end (terminal side) of the multilayer CNT is opened, which corresponds to the state at the time when the step of FIG. Next, a conductive material such as copper is introduced into a hollow region inside the innermost CNT. The introduction of the conductive substance can be performed using a technique such as molecular beam epitaxy (MBE) or vapor phase epitaxy. This is because the hollow region is structurally stable and has a low energy state, and the conductive substance floating in the atmosphere tends to enter the region. As a result, as shown on the right side of FIG. 4, the innermost CNT can be filled with the conductive material. Thereafter, the wiring structure is completed by performing the steps as shown in FIG. Note that the conductive material flying on the multi-walled CNT when the second conductive layer is formed by sputtering or the like is a massive material larger than the diameter of the multi-walled CNT. Therefore, such a material is a hollow region of the multi-walled CNT. It will be difficult to enclose.

本実施例によれば、筒状のＣＮＴ構造内に、芯のような導電性経路を設けるので、第１及び第２の導電層間の抵抗を更に低くすることができる。ＣＮＴに充填する導電性物質としては、用途に応じて任意の原子及び分子を使用することができる。例えば、直径１０ｎｍ程度の筒状中空部分に直径１ｎｍ未満の微小球のフラーレン（例えば、Ｃ６０等）が多数充填されてもよい。 According to the present embodiment, since a conductive path such as a core is provided in the cylindrical CNT structure, the resistance between the first and second conductive layers can be further reduced. Arbitrary atoms and molecules can be used as the conductive material filled in the CNTs depending on the application. For example, the fullerene of the microspheres having a diameter of less than 1nm to the cylindrical hollow portion having a diameter of about 10 nm (e.g., C 60, etc.) may be filled many.

図５は、ＣＮＴに導電性物質を内包させていない場合（内包前）及び内包させた場合（内包後）のＣＮＴの導電性を示す。図中横軸はＣＮＴの両端にかかる電圧を示し、縦軸はＣＮＴに沿って流れる電流を示す。図示されているように、ＣＮＴに導電性物質を内包させることで、グラフの傾きを更に急峻にし、ＣＮＴの電気抵抗を低減できることが分かる。   FIG. 5 shows the conductivity of CNTs when the conductive material is not encapsulated in CNT (before encapsulation) and when encapsulated (after encapsulation). In the figure, the horizontal axis indicates the voltage applied to both ends of the CNT, and the vertical axis indicates the current flowing along the CNT. As shown in the figure, it can be seen that the inclusion of a conductive substance in the CNTs can make the slope of the graph more steep and reduce the electrical resistance of the CNTs.

図６は、本発明の一実施例による配線構造を示す。第１実施例で説明済みの要素（図２）には同様な参照番号が付されている。図６左側に示されるように、本実施例では、多層ＣＮＴ２１０上に、チタニウム（Ｔｉ）より成るコンタクト層２２０が設けられ、そのコンタクト層２２０上に第２の導電層２１２が設けられている。そのようなコンタクト層は、例えば、室温におけるスパッタリングで成膜し、場合によっては加熱することにより形成される。コンタクト層２２０中のチタニウムは、ＣＮＴ側との間でチタニウムカーバイト（ＴｉＣ）を形成し、電気的に良好な接合部を形成する。従って、本実施例によれば、配線構造の低抵抗化を更に促すことができる。コンタクト層２２０は、チタニウムだけでなく、タンタル（Ｔａ）、モリブデン（Ｍｏ）、パラジウム（Ｐｄ）、ルテニウム（Ｒｕ）、アルミニウム（Ａｌ）、白金（Ｐｔ）、金（Ａｕ）、銅（Ｃｕ）等の導電性物質で構成してもよい。コンタクト層２２０の形成は、第２の導電層２１２を成膜する前に行われる。具体的には、図２（Ｄ）の工程と図２（Ｅ）の工程の間に行われる。コンタクト層２２０は、単一の材料層としてもよいし、多層の材料層としてもよい。なお、図６右側に示されるように、コンタクト層２２０をビアの外に設けてもよい。   FIG. 6 shows a wiring structure according to an embodiment of the present invention. Elements already described in the first embodiment (FIG. 2) have similar reference numbers. As shown on the left side of FIG. 6, in this embodiment, a contact layer 220 made of titanium (Ti) is provided on the multilayer CNT 210, and a second conductive layer 212 is provided on the contact layer 220. Such a contact layer is formed, for example, by sputtering at room temperature and in some cases by heating. Titanium in the contact layer 220 forms titanium carbide (TiC) with the CNT side to form an electrically good junction. Therefore, according to this embodiment, the resistance of the wiring structure can be further reduced. The contact layer 220 is not only titanium but also tantalum (Ta), molybdenum (Mo), palladium (Pd), ruthenium (Ru), aluminum (Al), platinum (Pt), gold (Au), copper (Cu), etc. The conductive material may be used. The contact layer 220 is formed before the second conductive layer 212 is formed. Specifically, it is performed between the step of FIG. 2D and the step of FIG. The contact layer 220 may be a single material layer or a multilayer material layer. As shown on the right side of FIG. 6, the contact layer 220 may be provided outside the via.

図７は、コンタクト層２２０を多層の材料層で形成した場合の一例を示す。図７左側に示される例では、コンタクト層２２０が、チタニウムより成る第１層２２２と、その上に設けられたタンタルより成る第２層２２４とを含む。一般に、銅は高温の環境下では隣接する層内に拡散する性質を有する。タンタルの第２層２２４を設けることで、銅がチタニウムの第１層２２２側に拡散することを抑制することができる。この例についても、図７右側に示されるように、コンタクト層２２０を構成する第１層２２２及び第２層２２４を、ビアの外に設けてもよい。   FIG. 7 shows an example in which the contact layer 220 is formed of multiple material layers. In the example shown on the left side of FIG. 7, the contact layer 220 includes a first layer 222 made of titanium and a second layer 224 made of tantalum provided thereon. In general, copper has the property of diffusing into adjacent layers in high temperature environments. By providing the second layer 224 of tantalum, it is possible to suppress the diffusion of copper to the first layer 222 side of titanium. Also in this example, as shown on the right side of FIG. 7, the first layer 222 and the second layer 224 constituting the contact layer 220 may be provided outside the via.

以下、本発明により教示される手段を例示的に列挙する。   Hereinafter, the means taught by the present invention will be listed as an example.

（付記１）
２以上の導電層の層間配線に多層カーボンナノチューブが使用される配線構造であって、
前記多層カーボンナノチューブに含まれるグラフェンシートにより形成され且つ前記多層カーボンナノチューブの成長基点から遠い側の端部に同心状に形成される複数の環状の切り口が、導電層にそれぞれ接触する
ことを特徴とする配線構造。 (Appendix 1)
A wiring structure in which multi-walled carbon nanotubes are used for interlayer wiring of two or more conductive layers,
A plurality of annular cuts formed by a graphene sheet contained in the multi-walled carbon nanotube and concentrically formed at an end far from the growth base point of the multi-walled carbon nanotube are in contact with the conductive layer, respectively. Wiring structure.

（付記２）
前記多層カーボンナノチューブの内部に、所定の導電性物質より成る層間配線部材が設けられる
ことを特徴とする付記１記載の配線構造。 (Appendix 2)
The wiring structure according to appendix 1, wherein an interlayer wiring member made of a predetermined conductive material is provided inside the multi-walled carbon nanotube.

（付記３）
前記所定の導電性物質が、フラーレンなどの分子又は金属元素より成る
ことを特徴とする付記２記載の配線構造。 (Appendix 3)
The wiring structure according to appendix 2, wherein the predetermined conductive material is made of a molecule such as fullerene or a metal element.

（付記４）
前記多層カーボンナノチューブの成長基点から遠い側に設けられる導電層が、所定の金属元素より成るコンタクト層と、コンタクト層とは異なる導電性の層より成る
ことを特徴とする付記１記載の配線構造。 (Appendix 4)
The wiring structure according to claim 1, wherein the conductive layer provided on the side far from the growth base point of the multi-walled carbon nanotube includes a contact layer made of a predetermined metal element and a conductive layer different from the contact layer.

（付記５）
前記所定の金属元素が、チタニウム、モリブデン、タンタル、パラジウム、ルテニウム、アルミニウム、白金、金及び銅を含む群から選択された少なくとも１つの元素を含む
ことを特徴とする付記４記載の配線構造。 (Appendix 5)
The wiring structure according to claim 4, wherein the predetermined metal element includes at least one element selected from the group including titanium, molybdenum, tantalum, palladium, ruthenium, aluminum, platinum, gold, and copper.

（付記６）
前記コンタクト層が、多層に形成される
ことを特徴とする付記４記載の配線構造。 (Appendix 6)
The wiring structure according to appendix 4, wherein the contact layer is formed in multiple layers.

（付記７）
前記コンタクト層が、銅、タンタル及びチタニウムより成る３層から形成される
ことを特徴とする付記６記載の配線構造。 (Appendix 7)
The wiring structure according to appendix 6, wherein the contact layer is formed of three layers made of copper, tantalum, and titanium.

（付記８）
第１の導電層上に設けられた絶縁層に、前記第１の導電層に至るビアを形成し、
前記ビアを貫通する多層カーボンナノチューブを成長させ、
酸素を含む雰囲気で、前記多層カーボンナノチューブを含む構造に熱処理もしくはプラズマ処理を施し、
前記絶縁層及び前記多層カーボンナノチューブ上に第２の導電層を成膜する
ことを特徴とする配線構造の製造方法。 (Appendix 8)
Forming a via leading to the first conductive layer in an insulating layer provided on the first conductive layer;
Growing multi-walled carbon nanotubes through the vias;
In an atmosphere containing oxygen, the structure containing the multi-walled carbon nanotubes is subjected to heat treatment or plasma treatment,
A method of manufacturing a wiring structure, comprising forming a second conductive layer on the insulating layer and the multi-walled carbon nanotube.

（付記９）
前記第２の導電層を成膜する前に、開端された多層カーボンナノチューブの筒状の中空部分に導電性物質を導入する
ことを特徴とする付記８記載の製造方法。 (Appendix 9)
The manufacturing method according to appendix 8, wherein a conductive substance is introduced into the cylindrical hollow portion of the opened multi-walled carbon nanotube before forming the second conductive layer.

（付記１０）
前記導電性物質が、フラーレンなどの分子又は金属元素より成る
ことを特徴とする付記８記載の製造方法。 (Appendix 10)
The manufacturing method according to appendix 8, wherein the conductive substance is made of a molecule such as fullerene or a metal element.

（付記１１）
前記第２の導電層を成膜する前に、少なくとも前記多層カーボンナノチューブ上に所定の金属元素より成るコンタクト層を成膜する
ことを特徴とする付記８記載の製造方法。 (Appendix 11)
9. The manufacturing method according to appendix 8, wherein a contact layer made of a predetermined metal element is formed on at least the multi-walled carbon nanotube before forming the second conductive layer.

（付記１２）
前記コンタクト層を多層に形成する
ことを特徴とする付記１１記載の製造方法。 (Appendix 12)
The manufacturing method according to appendix 11, wherein the contact layer is formed in multiple layers.

（付記１３）
前記熱処理を施す前に、水素を含む雰囲気で、前記多層カーボンナノチューブを含む構造に熱処理を施す
ことを特徴とする付記８記載の製造方法。 (Appendix 13)
The manufacturing method according to appendix 8, wherein the structure including the multi-walled carbon nanotubes is subjected to a heat treatment in an atmosphere containing hydrogen before the heat treatment.

従来の配線構造を製造する主要な工程の概略断面図を示す。The schematic sectional drawing of the main processes which manufacture the conventional wiring structure is shown. 本発明の一実施例による配線構造を製造する主要な工程の概略断面図を示す。The schematic sectional drawing of the main processes which manufacture the wiring structure by one Example of this invention is shown. 開端される多層ＣＮＴを示す図である。It is a figure which shows the multilayer CNT opened. 多層ＣＮＴに導電性物質が充填される様子を示す図である。It is a figure which shows a mode that a conductive material is filled into multilayer CNT. 多層ＣＮＴの導電性を示すグラフである。It is a graph which shows the electroconductivity of multilayer CNT. 本発明の一実施例による配線構造を示す図である。It is a figure which shows the wiring structure by one Example of this invention. 本発明の一実施例による配線構造を示す図である。It is a figure which shows the wiring structure by one Example of this invention.

符号の説明Explanation of symbols

１２，１８ 導電層； １３ビア； １４ 層間絶縁膜； １５ 触媒金属； １６ 多層ＣＮＴ；
２０２，２１２ 導電層； ２０４ 層間絶縁膜； ２０６ ビア； ２０８ 触媒金属； ２１０ 多層ＣＮＴ； ２２０ コンタクト層 12, 18 conductive layer; 13 vias; 14 interlayer insulating film; 15 catalytic metal; 16 multilayer CNT;
202, 212 Conductive layer; 204 Interlayer insulating film; 206 Via; 208 Catalytic metal; 210 Multi-layer CNT; 220 Contact layer

Claims (5)

２以上の導電層の層間配線に多層カーボンナノチューブが使用される配線構造であって、
前記多層カーボンナノチューブに含まれるグラフェンシートにより形成され且つ前記多層カーボンナノチューブの成長基点から遠い側の端部に同心状に形成される複数の環状の切り口が、導電層にそれぞれ接触する
ことを特徴とする配線構造。 A wiring structure in which multi-walled carbon nanotubes are used for interlayer wiring of two or more conductive layers,
A plurality of annular cuts formed by a graphene sheet contained in the multi-walled carbon nanotube and concentrically formed at an end far from the growth base point of the multi-walled carbon nanotube are in contact with the conductive layer, respectively. Wiring structure. 前記多層カーボンナノチューブの内部に、所定の導電性物質より成る層間配線部材が設けられる
ことを特徴とする請求項１記載の配線構造。 The wiring structure according to claim 1, wherein an interlayer wiring member made of a predetermined conductive material is provided inside the multi-walled carbon nanotube. 前記多層カーボンナノチューブの成長基点から遠い側に設けられる導電層が、所定の金属元素より成るコンタクト層と、コンタクト層とは異なる導電性の層より成る
ことを特徴とする請求項１記載の配線構造。 The wiring structure according to claim 1, wherein the conductive layer provided on the side far from the growth base point of the multi-walled carbon nanotube includes a contact layer made of a predetermined metal element and a conductive layer different from the contact layer. . 第１の導電層上に設けられた絶縁層に、前記第１の導電層に至るビアを形成し、
前記ビアを貫通する多層カーボンナノチューブを成長させ、
酸素を含む雰囲気で、前記多層カーボンナノチューブを含む構造に熱処理もしくはプラズマ処理を施し、
前記絶縁層及び前記多層カーボンナノチューブ上に第２の導電層を成膜する
ことを特徴とする配線構造の製造方法。 Forming a via leading to the first conductive layer in an insulating layer provided on the first conductive layer;
Growing multi-walled carbon nanotubes through the vias;
In an atmosphere containing oxygen, the structure containing the multi-walled carbon nanotubes is subjected to heat treatment or plasma treatment,
A method of manufacturing a wiring structure, comprising forming a second conductive layer on the insulating layer and the multi-walled carbon nanotube. 前記第２の導電層を成膜する前に、開端された多層カーボンナノチューブの筒状の中空部分に導電性物質を導入する
ことを特徴とする請求項６記載の製造方法。
The manufacturing method according to claim 6, wherein a conductive substance is introduced into the cylindrical hollow portion of the opened multi-walled carbon nanotube before forming the second conductive layer.
JP2004304667A 2004-10-19 2004-10-19 Wiring structure using multilayered carbon nanotube for interlayer wiring, and its manufacturing method Pending JP2006120730A (en)

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