JP4892723B2 - Magnetic metal-encapsulated carbon nanotube device - Google Patents

Magnetic metal-encapsulated carbon nanotube device Download PDF

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JP4892723B2
JP4892723B2 JP2006107470A JP2006107470A JP4892723B2 JP 4892723 B2 JP4892723 B2 JP 4892723B2 JP 2006107470 A JP2006107470 A JP 2006107470A JP 2006107470 A JP2006107470 A JP 2006107470A JP 4892723 B2 JP4892723 B2 JP 4892723B2
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靖彦 林
知春 徳永
武志 藤田
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国立大学法人 名古屋工業大学
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本発明は、強磁性金属充填カーボンナノチューブ素子及びそれを用いたデバイスに関する。   The present invention relates to a ferromagnetic metal-filled carbon nanotube element and a device using the same.

従来、特許文献１のカーボンナノチューブの製造方法が開示されている。特許文献１は、金属を内包するカーボンナノチューブの製造方法に関する特許であり、磁気抵抗効果（以下「TMR」という。）を利用した磁気ランダムアクセスメモリ（以下「MRAM」という。）の応用が示されているが，内包された金属の磁性特性が明らかにされていなかった。また、特許文献２においては、内包もしくは充填する金属が一種類であった。非特許文献１は、2層金属内包に関する論文であり、非特許文献２、３は、Fe内包カーボンナノチューブの電子線ホログラフィーに関する論文である。
特開平６−２２７８０６号公報 特開２００５−１０４８１４公報 “Production and Characterization of Single-Crystal FeCo Nanowires Inside Carbon Nanotubes”, A. L. Elias, J. A. Rodriguez-Manzo, M. R. McCartney, D. Golberg, A. Zamudio, S. E. Baltazar, F. Lopez-Urias, E. Munoz-Sandoval, L. Gu, C. C. Tang, D. J. Smith, Y. Bando, H. Terrones, and M. Terrones, Nano Lett. 5, 467 - 472 (2005). “Magnetic properties of aligned Fe-filled carbon nanotubes”, T. Muhl, D. Elefant, A. Graff, R. Kozhuharova, A. Leonhardt, I. Monch, M. Ritschel, P. Simon, S. Groudeva-Zotova, and C. M. Schneider, J. Appl. Phys. 93, 7894-7896 (2003). “Synthesis and properties of filled carbon nanotubes”, A. Leonhardt, M. Ritschel, R. Kozhuharova, A. Graff, T. Muhl, R. Huhle, I. Monch, D. Elefant and C. M. Schneider, Diamond Relat. Mater. 12, 790-793 (2003). Conventionally, the manufacturing method of the carbon nanotube of patent document 1 is disclosed. Patent Document 1 is a patent relating to a method for producing a carbon nanotube containing metal, and shows an application of a magnetic random access memory (hereinafter referred to as “MRAM”) using a magnetoresistive effect (hereinafter referred to as “TMR”). However, the magnetic properties of the encapsulated metal were not clarified. In Patent Document 2, there is one kind of metal to be included or filled. Non-Patent Document 1 is a paper on double-layer metal encapsulation, and Non-Patent Documents 2 and 3 are papers on electron holography of Fe-encapsulated carbon nanotubes.
JP-A-6-227806 JP 2005-104814 A “Production and Characterization of Single-Crystal FeCo Nanowires Inside Carbon Nanotubes”, AL Elias, JA Rodriguez-Manzo, MR McCartney, D. Golberg, A. Zamudio, SE Baltazar, F. Lopez-Urias, E. Munoz-Sandoval, L Gu, CC Tang, DJ Smith, Y. Bando, H. Terrones, and M. Terrones, Nano Lett. 5, 467-472 (2005). “Magnetic properties of aligned Fe-filled carbon nanotubes”, T. Muhl, D. Elefant, A. Graff, R. Kozhuharova, A. Leonhardt, I. Monch, M. Ritschel, P. Simon, S. Groudeva-Zotova, and CM Schneider, J. Appl. Phys. 93, 7894-7896 (2003). “Synthesis and properties of filled carbon nanotubes”, A. Leonhardt, M. Ritschel, R. Kozhuharova, A. Graff, T. Muhl, R. Huhle, I. Monch, D. Elefant and CM Schneider, Diamond Relat. Mater. 12, 790-793 (2003).

しかし、上記従来技術では、これまでに、単一のカーボンナノチューブに充填もしくは内包した金属からの磁性特性を得られていない。また、二種類以上の磁性金属を含む金属全般を内包もしくは充填する技術は確立されていない。
本発明は、上記従来の実情に鑑みてなされたものであって、磁性金属をチューブ内に完全に充填もしくは、チューブ先端に内包するナノチューブ素子を作製し、磁性特性の評価を行い、本素子を用いた磁気センサー等のデバイスを提供することを解決すべき課題としている。 However, in the above prior art, magnetic properties from a metal filled or encapsulated in a single carbon nanotube have not been obtained so far. In addition, a technique for enclosing or filling all metals including two or more kinds of magnetic metals has not been established.
The present invention has been made in view of the above-described conventional situation, and a nanotube element in which a magnetic metal is completely filled in a tube or encapsulated in a tube tip is manufactured, and magnetic characteristics are evaluated. Providing a device such as a magnetic sensor used is an issue to be solved.

第１発明の強磁性金属充填カーボンナノチューブ素子は、単層・多層カーボンナノチューブに二種類以上の磁性金属を含む金属を内包もしくは充填することを特徴とする。
第２発明の強磁性金属充填カーボンナノチューブ素子は、第１発明の磁性金属を含む金属が，単層・多層カーボンナノチューブ内で合金もしくは分離して内包もしくは充填することを特徴とする。
第３発明のバーコードタイプ強磁性金属充填カーボンナノチューブ素子は、第１発明のの磁性金属を含む金属が，単層・多層カーボンナノチューブ内でそれぞれの金属ごとに分離して内包もしくは充填することを特徴とする。
第４発明の磁気ランダムアクセスメモリデバイスは、第１又は第２発明のカーボンナノチューブ素子を用い磁気抵抗効果を利用することを特徴とする。
第５発明の磁気力顕微鏡（MFM）探針及び第６発明の磁気センサーは、第１又は第２発明のカーボンナノチューブ素子を用いることを特徴とする。 The ferromagnetic metal-filled carbon nanotube element of the first invention is characterized in that single-walled / multi-walled carbon nanotubes are encapsulated or filled with a metal containing two or more kinds of magnetic metals.
The ferromagnetic metal-filled carbon nanotube element of the second invention is characterized in that the metal containing the magnetic metal of the first invention is alloyed or separated and enclosed or filled in the single-walled / multi-walled carbon nanotube.
The barcode type ferromagnetic metal-filled carbon nanotube element of the third invention is such that the metal containing the magnetic metal of the first invention is separately encapsulated or filled in each single-walled / multi-walled carbon nanotube. Features.
A magnetic random access memory device according to a fourth aspect of the invention is characterized in that the carbon nanotube element according to the first or second aspect of the invention is used and the magnetoresistive effect is utilized.
The magnetic force microscope (MFM) probe of the fifth invention and the magnetic sensor of the sixth invention use the carbon nanotube element of the first or second invention.

図1に示すように、一種類以上の磁性金属を含む金属全般を内包もしくは充填するために、基板に内包もしくは充填する金属薄膜を積層する。   As shown in FIG. 1, in order to encapsulate or fill all metals including one or more kinds of magnetic metals, a metal thin film to be encapsulated or filled is laminated on a substrate.

金属を内包もしくは充填する金属を積層した基板を用いてナノチューブを成長することで，成長と同時にこれらの金属内包もしくは充填する．成長条件を制御することで，チューブ内の金属を分離して内包もしくは充填することができる。   Nanotubes are grown using a substrate on which a metal that contains or fills metal is laminated, and these metals are included or filled simultaneously with the growth. By controlling the growth conditions, the metal in the tube can be separated and encapsulated or filled.

金属を内包もしくは充填した単一のナノチューブからの磁性特性を，電子線ホログラフィー法により明らかにし，磁気センサーなどの有効なことを示した。
従来一種類もしくは二種類の金属を内包するナノチューブの報告があるが，本発明により多数の金属をチューブ内に内包もしくは充填することが可能となった。
カーボンナノチューブ内に合金を内包もしくは充填するだけでなく，金属を分離して内包もしくは充填することに成功した．これにより，ナノスケールでバーコードのようなデバイスを作成することが可能となった。
金属を内包もしくは充填した単一のナノチューブからの磁性特性を電子線ホログラフィー法で観察することで，金属からの明らかな磁気力線を確認することができ，磁気センサーなどの磁気デバイスへの応用が可能となった。また，金属はナノチューブの中に閉じこめられているため，直接大気に触れることがなく，金属の酸化などから防ぐことができ，磁気センサーなどに応用した場合には安定した特性が得られる。 The magnetic properties of single nanotubes containing or filled with metal were clarified by electron holography, and it was shown that they were effective for magnetic sensors.
Conventionally, there have been reports of nanotubes containing one or two kinds of metals, but according to the present invention, it has become possible to enclose or fill a tube with a large number of metals.
In addition to encapsulating or filling alloys in carbon nanotubes, we succeeded in separating and encapsulating metals. This made it possible to create barcode-like devices on the nanoscale.
By observing the magnetic properties of a single nanotube encapsulating or filling a metal with an electron holography method, it is possible to confirm the clear magnetic lines of force from the metal, which can be applied to magnetic devices such as magnetic sensors. It has become possible. In addition, since the metal is confined in the nanotube, it is not directly exposed to the atmosphere and can be prevented from oxidation of the metal, and stable characteristics can be obtained when applied to a magnetic sensor or the like.

単層・多層カーボンナノチューブに二種類以上の磁性金属を含む金属を内包もしくは充填することが可能となる。   It becomes possible to enclose or fill a single- or multi-walled carbon nanotube with a metal containing two or more kinds of magnetic metals.

カーボンナノチューブ内に合金を内包もしくは充填するだけでなく，金属を分離して内包もしくは充填するバーコードタイプ強磁性金属充填カーボンナノチューブも可能となる。   In addition to including or filling an alloy in a carbon nanotube, a barcode-type ferromagnetic metal-filled carbon nanotube that separates and encapsulates a metal is also possible.

磁気センサーに応用する際，磁性金属を含む金属はカーボンナノチューブ内に内包もしくは充填しているため，大気などに暴露されることがないため安定したデバイスが作製可能となる。   When applied to a magnetic sensor, a metal containing a magnetic metal is encapsulated or filled in carbon nanotubes, so that it is not exposed to the atmosphere and a stable device can be produced.

以下、本発明を具体化した実施例を図面を参照しつつ説明する。 DESCRIPTION OF THE PREFERRED EMBODIMENTS Embodiments embodying the present invention will be described below with reference to the drawings.

図1に示すように、一種類以上の磁性金属を含む金属を内包もしくは充填するために、基板に内包もしくは充填する金属薄膜を積層する。
図１は二層及び多層構造カーボンナノチューブで、１（部品番号１）は基板、例えばシリコン基板、金属基板を示す。２（部品番号２）は、前記部品番号１がシリコン基板の場合は、SiO2，SiNx，Mo，Wなどであり、前記部品番号１が金属基板の場合では、Mo，Wなどの高融点金属である。３（部品番号３）及び４（部品番号４）は、内包する金属を２（部品番号２）の上に積層する．図1では，２種類の金属の場合で，例えば，３（部品番号３）はPd（非磁性金属），部品番号４はCo（強磁性金属）のような組み合わせである．内包もしくは充填する金属の種類により部品数を増やすことができる．
図２は、多層カーボンナノチューブ内でPdとCoを分離して内包する実施例を示す写真である。５（部品番号５）は、多層カーボンナノチューブ内でPdとCoを分離して内包し、６（部品番号６）はPd金属であり、７（部品番号７）はCo金属を示す。
図３は、多層カーボンナノチューブ内でPdとCoが合金として充填している実施例を示す写真である。 As shown in FIG. 1, in order to enclose or fill a metal containing one or more kinds of magnetic metals, a metal thin film to be encapsulated or filled is laminated on a substrate.
FIG. 1 shows double-walled and multi-walled carbon nanotubes, and 1 (part number 1) denotes a substrate, for example, a silicon substrate or a metal substrate. 2 (part number 2) is SiO 2 , SiN x , Mo, W or the like when the part number 1 is a silicon substrate, and high melting point such as Mo or W when the part number 1 is a metal substrate It is a metal. In 3 (part number 3) and 4 (part number 4), the encapsulating metal is laminated on 2 (part number 2). In FIG. 1, there are two types of metals. For example, 3 (part number 3) is a combination such as Pd (nonmagnetic metal) and part number 4 is Co (ferromagnetic metal). The number of parts can be increased depending on the type of metal to be included or filled.
FIG. 2 is a photograph showing an example in which Pd and Co are separated and included in a multi-walled carbon nanotube. 5 (part number 5) separates and encloses Pd and Co in the multi-walled carbon nanotube, 6 (part number 6) is Pd metal, and 7 (part number 7) indicates Co metal.
FIG. 3 is a photograph showing an example in which Pd and Co are filled as an alloy in a multi-walled carbon nanotube.

図４は、電子線ホログラフィー法により観察したカーボンナノチューブ単一に内包したCo金属からの磁気誘導を示す図である。   FIG. 4 is a diagram showing magnetic induction from a Co metal encapsulated in a single carbon nanotube observed by an electron holography method.

本発明の強磁性金属充填カーボンナノチューブ素子及びそれを用いたデバイスは磁気センサー等に利用可能である。   The ferromagnetic metal filled carbon nanotube element of the present invention and a device using the same can be used for a magnetic sensor or the like.

二層及び多層構造カーボンナノチューブを示す説明図である。It is explanatory drawing which shows a double-layer and a multilayer structure carbon nanotube. 多層カーボンナノチューブ内でPdとCoを分離して内包する実施例を示す写真である。It is a photograph which shows the Example which isolate | separates and encloses Pd and Co in a multi-walled carbon nanotube. 多層カーボンナノチューブ内でPdとCoが合金として充填している実施例を示す写真である。It is a photograph which shows the Example which has filled Pd and Co as an alloy in a multi-walled carbon nanotube. 電子線ホログラフィー法により観察したカーボンナノチューブ単一に内包したCo金属からの磁気誘導を示す図である。It is a figure which shows the magnetic induction from the Co metal included in the carbon nanotube single observation observed by the electron beam holography method.

Claims (5)

多層カーボンナノチューブにニ種類以上の金属が内包もしくは充填され、該金属が磁性金属および非磁性金属からなり、磁性金属と非磁性金属とが分離されて内包もしくは充填されていることを特徴とするカーボンナノチューブ素子。 Multi layer two or more metals are contained or packed in a carbon nanotube, and characterized in that said metal is made of a magnetic metal and nonmagnetic metal, and a magnetic metal and nonmagnetic metal are encapsulated or filled separated to Luke over carbon nanotube element. 前記磁性金属と非磁性金属がバーコード状に配置されたバーコードタイプの請求項１に記載のカーボンナノチューブ素子。The carbon nanotube device according to claim 1, wherein the magnetic metal and the nonmagnetic metal are in a barcode type in which the magnetic metal and the nonmagnetic metal are arranged in a barcode. 磁気抵抗効果を利用した磁気ランダムアクセスメモリデバイスに用いられる請求項１または２に記載のカーボンナノチューブ素子。The carbon nanotube device according to claim 1 or 2, which is used for a magnetic random access memory device utilizing a magnetoresistive effect. 磁気力顕微鏡（ＭＦＭ）探針に用いられる請求項１または２に記載のカーボンナノチューブ素子。The carbon nanotube device according to claim 1 or 2, which is used for a magnetic force microscope (MFM) probe. 磁気センサーに用いられる請求項１または２に記載のカーボンナノチューブ素子。The carbon nanotube element according to claim 1 or 2 used for a magnetic sensor.
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