JP3291804B2 - Method of synthesizing diamond single crystal - Google Patents
Method of synthesizing diamond single crystalInfo
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- JP3291804B2 JP3291804B2 JP00905893A JP905893A JP3291804B2 JP 3291804 B2 JP3291804 B2 JP 3291804B2 JP 00905893 A JP00905893 A JP 00905893A JP 905893 A JP905893 A JP 905893A JP 3291804 B2 JP3291804 B2 JP 3291804B2
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- diamond
- weight
- crystal
- solvent
- powder
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Description
【０００１】[0001]
【産業上の利用分野】本発明は装飾用途や光学部品など
に用いられる無色で透明なダイヤモンド単結晶の合成方
法に関するものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for synthesizing a colorless and transparent diamond single crystal used for decorative purposes and optical parts.
【０００２】[0002]
【従来の技術】現在市販されている装飾用ダイヤモンド
は、主に南アフリカ、ロシアより産出されるものの中か
ら、無色透明で内部欠陥の少ないものを選別して用いら
れている。天然装飾用ダイヤモンドは宝石の中でも最も
販売量が多い。また、ダイヤモンドを用いた光学部品と
して、レーザー窓やＩＲアンビルセルなどがあるが、い
ずれも天然原石の中から赤外領域に光の吸収のない透明
なダイヤモンド（IIａ型とよばれる）が選ばれて用いら
れている。しかし、無色透明な原石の産出は極めて少な
く、安定供給や価格に問題がある。2. Description of the Related Art Currently, commercially available decorative diamonds are mainly selected from those produced in South Africa and Russia, and those which are colorless and transparent and have few internal defects are used. Natural ornamental diamonds have the highest sales volume among gemstones. As optical components using diamond, there are a laser window, an IR anvil cell, and the like. In each case, a transparent diamond (called type IIa) having no light absorption in the infrared region is selected from natural rough. Used. However, the production of colorless and transparent rough is extremely low, and there is a problem in stable supply and price.
【０００３】一方、人工合成によるダイヤモンドは通
常、超高圧高温下で合成する際に溶媒中の窒素が結晶格
子内に取り込まれるために黄色く着色してしまうが、溶
媒中に窒素ゲッターを添加することで無色透明のダイヤ
モンドを得ることができる。この窒素ゲッターとして
は、たとえば、The Journal of Physical Chemistry, v
ol.75, No.12 (1971) p1838 に示されているように、Ａ
ｌがよく知られている。具体的には、米国特許第４０３
４０６６号明細書には、Ｆｅ溶媒にＡｌを３〜５重量％
添加することにより宝石級の無色透明なダイヤモンド単
結晶が得られると記載されている。Ａｌ以外の窒素ゲッ
ターを用いた例として、たとえば無機材質研究所研究報
告書第３９号（１９８４）、ｐ１６〜１９項にＴｉやＺ
ｒを溶媒金属に添加することにより、結晶中の窒素が除
去されたという報告がある。[0003] On the other hand, artificially synthesized diamond is usually colored yellow because nitrogen in a solvent is taken into a crystal lattice when synthesized under ultra-high pressure and high temperature. However, it is necessary to add a nitrogen getter to the solvent. To obtain a colorless and transparent diamond. Examples of this nitrogen getter include, for example, The Journal of Physical Chemistry, v
ol. 75, No. 12 (1971) p1838.
l is well known. Specifically, U.S. Pat.
No. 4066 describes that 3 to 5% by weight of Al is added to an Fe solvent.
It is described that a colorless and transparent gem-grade diamond single crystal can be obtained by the addition. Examples of the use of nitrogen getters other than Al include, for example, Ti and Z, p.
There is a report that nitrogen in the crystal was removed by adding r to the solvent metal.
【０００４】[0004]
【発明が解決しようとする課題】しかし、特に無色透明
の合成ダイヤモンドは合成コストが天然ダイヤモンドよ
りはるかに高くなるため工業生産は行われていない。こ
の理由は、合成には高価で特殊な装置が必要である上
に、Ａｌなどを窒素ゲッターとして添加した場合、その
添加量の増加に従って、溶媒が結晶中に取り込まれ（以
下インクルージョンと呼ぶ）て、不良結晶となることが
多くなるため、良質な結晶とするためには成長速度を大
幅に下げる必要があるからである。とくにＴｉやＺｒを
窒素ゲッターとして用いた場合は、合成中に溶媒中に生
成したＴｉＣやＺｒＣなどの炭化物が原因でより多くの
インクルージョンが結晶中に取り込まれるようになる。However, in particular, colorless and transparent synthetic diamond has not been produced industrially because the synthesis cost is much higher than that of natural diamond. The reason is that the synthesis requires expensive and special equipment, and when Al or the like is added as a nitrogen getter, the solvent is taken into the crystal as the amount of addition increases (hereinafter referred to as inclusion). This is because the number of defective crystals increases, and it is necessary to greatly reduce the growth rate to obtain high-quality crystals. In particular, when Ti or Zr is used as a nitrogen getter, more inclusions are incorporated into the crystal due to carbides such as TiC and ZrC generated in the solvent during the synthesis.
【０００５】本発明者らが行った実験による結果では、
窒素ゲッターとしてＡｌを用い、溶媒金属に均一混合し
た場合、無色透明なダイヤモンド結晶を合成するために
は、その添加量は溶媒に対し少なくとも４重量％（約１
２体積％）必要であるが、この場合インクルージョンの
巻き込みなしに結晶成長させるためには成長速度を１ｍ
ｇ／ｈｒ以下にする必要がある。この場合、たとえば１
カラット（２００ｍｇ）の結晶を合成するには２００時
間以上の合成時間を要し、製造コストは膨大なものとな
る。また、Ｔｉ、Ｚｒなど、Ａｌより窒素との反応性の
高い物質を窒素ゲッターとして溶媒に均一添加した場
合、添加量は１重量％でも無色透明な結晶となる。しか
し、これらは炭化物を形成しやすく、成長速度を大幅に
低下させたとしてもＴｉＣやＺｒＣなどの炭化物の影響
で、良質な結晶は殆ど得られない。すなわち、ＴｉＣや
ＺｒＣなどの炭化物自体がダイヤモンド結晶中へ混入し
たり、また、これらの炭化物が溶媒中の炭素の拡散を妨
げて、炭素の結晶表面への供給量が低下し、その結果、
溶媒が結晶中に巻き込まれやすくなる。本発明はかかる
問題点を解決し、無色透明でインクルージョのほとんど
ない結晶を、安価にしかも安定して合成できる新規な製
法を提供し、人工合成ダイヤモンドの装飾用途又は光学
部品用途への使用を可能にすることを意図するものであ
る。[0005] According to the results of experiments performed by the inventors,
When Al is used as a nitrogen getter and uniformly mixed with a solvent metal, the amount of addition is at least 4% by weight (about 1%) based on the solvent in order to synthesize a colorless and transparent diamond crystal.
2% by volume), but in this case, in order to grow the crystal without involving inclusion, the growth rate is 1 m.
g / hr or less. In this case, for example, 1
Synthesizing a carat (200 mg) crystal requires a synthesis time of 200 hours or more, and the production cost is enormous. When a substance having a higher reactivity with nitrogen than Al, such as Ti or Zr, is uniformly added to the solvent as a nitrogen getter, colorless and transparent crystals are obtained even if the added amount is 1% by weight. However, these tend to form carbides, and even if the growth rate is significantly reduced, good quality crystals are hardly obtained due to the influence of carbides such as TiC and ZrC. That is, carbides such as TiC and ZrC themselves are mixed into the diamond crystal, and these carbides prevent the diffusion of carbon in the solvent, thereby reducing the amount of carbon supplied to the crystal surface.
The solvent is likely to be involved in the crystal. The present invention solves the above problems, and provides a novel production method capable of inexpensively and stably synthesizing a colorless and transparent crystal having almost no inclusions. It is intended to be possible.
【０００６】[0006]
【課題を解決するための手段】上記の問題を解決するた
め、本発明者らは、溶媒中に窒素ゲッターとして、Ｔ
ｉ、Ｚｒ、Ｈｆなどの、窒素との反応性の高い元素を添
加し、同時にＣｕ、Ａｇ、Ａｕ、Ｚｎ、などを添加すれ
ば、窒素の除去効率が上がり、また、ＴｉＣやＺｒＣな
どの炭化物が合成中に溶媒中に生成することが少なくな
り、炭化物のダイヤ結晶中への混入や、溶媒の巻き込み
によるインクルージョンが大幅に少なくなり、その結
果、窒素不純物やインクルージョンをほとんど含まない
高純度なIIａタイプのダイヤモンド結晶が、比較的はや
い成長速度でも得られることを見いだした。さらに検討
を重ねたところ、Ｔｉ、Ｚｒ、Ｈｆなどの元素とＣｕ、
Ａｇ、Ａｕなどの元素からなる合金もしくは金属間化合
物を窒素ゲッターとして溶媒中に添加すれば、より効果
的であることが判った。Means for Solving the Problems To solve the above-mentioned problems, the present inventors have proposed a method in which a nitrogen getter is used as a nitrogen getter in a solvent.
Addition of elements having high reactivity with nitrogen, such as i, Zr, Hf, and at the same time, addition of Cu, Ag, Au, Zn, etc., increase the nitrogen removal efficiency, and also provide carbides such as TiC and ZrC. Is reduced in the solvent during the synthesis, and the inclusion of carbides in the diamond crystal and the inclusion due to the entrainment of the solvent are significantly reduced. As a result, high-purity IIa containing almost no nitrogen impurities and inclusions It has been found that a type of diamond crystal can be obtained even at a relatively high growth rate. After further studies, elements such as Ti, Zr and Hf and Cu,
It has been found that it is more effective to add an alloy or an intermetallic compound made of an element such as Ag or Au to a solvent as a nitrogen getter.
【０００７】すなわち、本発明は温度差法によるダイヤ
モンド結晶合成において、溶媒金属に、窒素ゲッターと
してＴｉ，Ｚｒ，Ｈｆ，Ｖ，Ｎｂ，Ｔａから選ばれる一
種もしくは二種以上の金属を添加し、かつ、Ｔｉ、Ｚ
ｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａの炭化物を分解する物質を添
加することを特徴とするものである。ここで、Ｔｉ、Ｚ
ｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａの炭化物を分解する物質がＣ
ｕ、Ａｇ、Ａｕ、Ｚｎ、Ｃｄから選ばれる金属であるこ
とを特徴とするものである。窒素ゲッターとして添加す
るＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａから選ばれる一種
もしくは二種以上の金属の添加量は、溶媒に対して、
０．１重量％以上、５重量％以下が好ましく、かつ、Ｔ
ｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａの炭化物を分解する物
質の添加量が溶媒に対して、０．１重量％以上２０重量
％以下であることが好ましい。That is, in the present invention, in the diamond crystal synthesis by the temperature difference method, one or more metals selected from Ti, Zr, Hf, V, Nb and Ta are added to a solvent metal as a nitrogen getter, and , Ti, Z
It is characterized by adding a substance that decomposes carbides of r, Hf, V, Nb and Ta. Where Ti, Z
The substance that decomposes carbides of r, Hf, V, Nb, Ta is C
It is a metal selected from u, Ag, Au, Zn, and Cd. The amount of one or more metals selected from Ti, Zr, Hf, V, Nb and Ta to be added as a nitrogen getter is
0.1% by weight or more and 5% by weight or less, and T
It is preferable that the amount of the substance that decomposes carbides of i, Zr, Hf, V, Nb, and Ta be 0.1% by weight or more and 20% by weight or less based on the solvent.
【０００８】また、本発明は温度差法によるダイヤモン
ド結晶合成において、溶媒金属にＸ−Ｙ系の合金もしく
は金属間化合物（ここで、ＸはＴｉ、Ｚｒ、Ｈｆ、Ｖ、
Ｎｂ、Ｔａから選ばれる元素、ＹはＣｕ、Ａｇ、Ａｕ、
Ｚｎ、Ｃｄから選ばれる元素）を添加することを特徴と
するものである。ここで、前記、Ｘ−Ｙ系の合金もしく
は金属間化合物（ここで、ＸはＴｉ、Ｚｒ、Ｈｆ、Ｖ、
Ｎｂ、Ｔａから選ばれる元素、ＹはＣｕ、Ａｇ、Ａｕ、
Ｚｎ、Ｃｄから選ばれる元素）の添加量は、溶媒に対し
て、０．１重量％以上、１０重量％以下であることが好
ましい。さらに、本発明において、溶媒金属は、Ｆｅ，
Ｃｏ，Ｎｉ，Ｍｎ，Ｃｒの中から選ばれる一種もしくは
二種以上からなり、且つ０．１〜６．０重量％の炭素を
含むことが好ましい。In the present invention, in the synthesis of diamond crystals by the temperature difference method, an XY-based alloy or intermetallic compound (where X is Ti, Zr, Hf, V,
An element selected from Nb and Ta, and Y is Cu, Ag, Au,
(Elements selected from Zn and Cd). Here, the XY-based alloy or intermetallic compound (where X is Ti, Zr, Hf, V,
An element selected from Nb and Ta, and Y is Cu, Ag, Au,
The addition amount of the element selected from Zn and Cd) is preferably 0.1% by weight or more and 10% by weight or less based on the solvent. Further, in the present invention, the solvent metal is Fe,
It is preferable that it is composed of one or more selected from Co, Ni, Mn, and Cr and contains 0.1 to 6.0% by weight of carbon.
【０００９】図１は本発明の一具体例であって、ダイヤ
モンド結晶合成用の試料室構成を示す図であり、溶媒金
属２中に、窒素ゲッターとしてＴｉ、Ｚｒ、Ｈｆ、Ｖ、
Ｎｂ、Ｔａから選ばれる一種もしくは二種以上の金属を
添加すると同時に、Ｔｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａ
の炭化物を分解する物質としてＣｕ、Ａｇ、Ａｕ、Ｚ
ｎ、Ｃｄから選ばれる金属を添加する。窒素ゲッターと
して添加するＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａから選
ばれる一種もしくは二種以上の金属の添加量は、溶媒に
対して、０．１重量％以上、５重量％以下であることが
好ましい。０．１重量％より少ないと、窒素が十分に除
去されずに結晶が黄色味を帯びてくる。また５重量％を
越えると、結晶中のインクルージョンが多くなり良質な
結晶が得られなくなる。また、Ｔｉ、Ｚｒ、Ｈｆ、Ｖ、
Ｎｂ、Ｔａの炭化物を分解する物質の添加量は溶媒に対
して、０．１重量％以上２０重量％以下であることが好
ましい。０．１重量％より少ないと炭化物分解の効果が
不十分で、２０重量％をこえると多結晶化や自然核発
生、インクルージョンが多くなり良質な結晶が得られな
くなる。FIG. 1 shows an embodiment of the present invention, showing a sample chamber configuration for diamond crystal synthesis. In a solvent metal 2, Ti, Zr, Hf, V,
At the same time as adding one or more metals selected from Nb and Ta, Ti, Zr, Hf, V, Nb, Ta
Cu, Ag, Au, Z as substances that decompose carbides
A metal selected from n and Cd is added. The amount of one or more metals selected from Ti, Zr, Hf, V, Nb and Ta to be added as a nitrogen getter is 0.1% by weight or more and 5% by weight or less based on the solvent. Is preferred. If the amount is less than 0.1% by weight, nitrogen is not sufficiently removed and the crystals take on a yellow tint. On the other hand, if it exceeds 5% by weight, the inclusion in the crystal increases, and a good quality crystal cannot be obtained. Also, Ti, Zr, Hf, V,
The amount of the substance that decomposes carbides of Nb and Ta is preferably 0.1% by weight or more and 20% by weight or less based on the solvent. If it is less than 0.1% by weight, the effect of carbide decomposition is insufficient, and if it exceeds 20% by weight, polycrystallization, generation of natural nuclei and inclusion increase, so that good quality crystals cannot be obtained.
【００１０】また、本発明の別の方法では、前記溶媒金
属２中にＸ−Ｙ系の合金もしくは金属間化合物（ここ
で、ＸはＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａから選ばれ
る元素、ＹはＣｕ、Ａｇ、Ａｕ、Ｚｎ、Ｃｄから選ばれ
る元素）を添加する。たとえばＴｉ−Ｃｕ合金の例とし
ては２５Ｔｉ−７５Ｃｕ合金（重量比、以下同じ）、５
０Ｔｉ−５０Ｃｕ合金、７５Ｔｉ−２５Ｃｕなどが挙げ
られる。また、たとえばＴｉ−Ｃｕ系金属間化合物の例
としては、Ｃｕ2 Ｔｉ（原子比、以下同じ）、ＣｕＴ
ｉ、ＣｕＴｉ2 、Ｃｕ3 Ｔｉ2 などが、Ｃｕ−Ｚｒ系の
金属間化合物としては、Ｃｕ3 Ｚｒ、Ｃｕ3 Ｚｒ2 、Ｃ
ｕＺｒ、ＣｕＺｒ2 などが挙げられる。このＸ−Ｙ系の
合金もしくは金属間化合物の添加量は溶媒に対して、
０．１重量％以上、１０重量％以下であることが好まし
い。０．１重量％より少ないと窒素が十分に除去されず
に結晶が黄色味を帯びてくる。１０重量％をこえると多
結晶化や自然核発生、インクルージョンが多くなり良質
な結晶が得られなくなる。In another method of the present invention, in the solvent metal 2, an XY-based alloy or an intermetallic compound (where X is an element selected from Ti, Zr, Hf, V, Nb and Ta) , Y is an element selected from Cu, Ag, Au, Zn, and Cd). For example, as an example of the Ti-Cu alloy, 25Ti-75Cu alloy (weight ratio, the same applies hereinafter), 5
0Ti-50Cu alloy, 75Ti-25Cu and the like. Examples of Ti-Cu intermetallic compounds include Cu 2 Ti (atomic ratio, the same applies hereinafter), CuT
i, CuTi 2 , Cu 3 Ti 2, and the like are Cu—Zr-based intermetallic compounds such as Cu 3 Zr, Cu 3 Zr 2 , C
uZr, CuZr 2 and the like. The amount of the XY alloy or intermetallic compound added to the solvent is
It is preferable that the content be 0.1% by weight or more and 10% by weight or less. If the amount is less than 0.1% by weight, nitrogen is not sufficiently removed, and the crystals take on a yellow tint. If the content exceeds 10% by weight, polycrystallization, generation of natural nuclei, and inclusion increase, and high-quality crystals cannot be obtained.
【００１１】ここで、図１の２の溶媒金属は一般にはＦ
ｅ，Ｃｏ，Ｎｉ，Ｍｎ，Ｃｒの中から選ばれる一種もし
くは二種以上からなる金属であり、種結晶溶解防止のた
め０．１〜６．０重量％の炭素をあらかじめ添加してお
くのが好ましい。炭素添加量が０．１重量％未満もしく
は炭素を含まない溶媒金属を用いた場合、種結晶上にＰ
ｔなどの種結晶溶解防止材を配置する必要があるが、こ
のような種結晶溶解防止材を配置することは、多結晶化
やインクルージョンの巻き込みの原因となり好ましくな
い。また、炭素添加量が６重量％をこえると、自然核発
生がおこりやすくなり、種結晶以外の部所より結晶成長
するため結晶同士が干渉し、良質な結晶が得られなくな
る。Here, the solvent metal of 2 in FIG.
e, Co, Ni, Mn, and Cr are metals selected from one or more selected from the group consisting of 0.1 to 6.0% by weight of carbon to prevent dissolution of seed crystals. preferable. When a solvent metal containing less than 0.1% by weight of carbon or containing no carbon is used, P
It is necessary to dispose a seed crystal dissolution preventing material such as t, but disposing such a seed crystal dissolution preventing material is not preferable because it causes polycrystallization and inclusion inclusion. On the other hand, if the amount of carbon exceeds 6% by weight, natural nuclei are likely to be generated, and crystals grow from a portion other than the seed crystal, so that the crystals interfere with each other and a good quality crystal cannot be obtained.
【００１２】本発明に用いる種結晶、炭素源等はこの種
の技術分野で公知のものを用いることができる。また、
温度差法による合成の条件等は適宜選択することができ
る。具体的な例は後記する実施例に挙げられる。As the seed crystal, carbon source and the like used in the present invention, those known in the technical field of this type can be used. Also,
Conditions for synthesis by the temperature difference method and the like can be appropriately selected. A specific example will be described in Examples described later.
【００１３】[0013]
【作用】本発明によるダイヤモンド合成方法によると、
溶媒金属に窒素ゲッターとしてＴｉ，Ｚｒ，Ｈｆ，Ｖ，
Ｎｂ，Ｔａから選ばれる一種もしくは二種以上の金属を
添加し、かつ、Ｔｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａの炭
化物を分解する物質たとえばＣｕ、Ａｇ、Ａｕ、Ｚｎ、
Ｃｄから選ばれる金属を添加する、あるいは、溶媒金属
にＸ−Ｙ系の合金もしくは金属間化合物（ここで、Ｘは
Ｔｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａから選ばれる元素、
ＹはＣｕ、Ａｇ、Ａｕ、Ｚｎ、Ｃｄから選ばれる元素）
を添加するため、窒素の除去効率が高く、また、ＴｉＣ
やＺｒＣなどの炭化物の結晶中への混入や、溶媒の巻き
込みによるインクルージョンが大幅に少なくなり、その
結果、窒素不純物やインクルージョンをほとんど含まな
い高純度なIIａタイプのダイヤモンド結晶が、従来より
かなり速い成長速度でも得られるようになる。According to the diamond synthesis method of the present invention,
Ti, Zr, Hf, V,
A substance which adds one or more metals selected from Nb and Ta and decomposes carbides of Ti, Zr, Hf, V, Nb and Ta, for example, Cu, Ag, Au, Zn,
A metal selected from Cd is added, or an XY-based alloy or intermetallic compound (where X is an element selected from Ti, Zr, Hf, V, Nb, Ta,
Y is an element selected from Cu, Ag, Au, Zn, and Cd)
, The nitrogen removal efficiency is high, and TiC
Inclusion due to the incorporation of carbides such as ZrC and ZrC into the crystal and entrainment of the solvent is greatly reduced, and as a result, a high-purity IIa type diamond crystal containing almost no nitrogen impurities and inclusions grows much faster than before. You can also get at speed.
【００１４】この理由について、次に具体的に述べる。
先にも述べたように、Ｔｉのみを窒素ゲッターとして用
いた場合、窒素との反応性が高いので添加量は〜１重量
％という微量でも無色透明なダイヤモンド結晶となる
が、ＴｉＣが溶媒中に多量に生成する。そのため結晶成
長が阻害されたり、また結晶の成長速度を大幅に低下さ
せたとしても、このＴｉＣが結晶中に取り込まれたりし
て、良質な結晶は殆ど得られない。しかし、窒素ゲッタ
ーとしてＴｉを添加するとともに、炭化物を形成せず、
しかもＴｉＣを溶解・分解する働きのあるＣｕを同時に
添加することにより、溶媒中のＴｉＣの影響によるイン
クルージョンの混入を抑えることができる。さらにＴｉ
とＣｕからなる合金又は金属間化合物、例えばＣｕＴｉ
などを添加した場合、より効果的であり、良質な結晶が
かなり得やすくなる。また、窒素の除去効率も、Ｔｉと
同程度で、１重量％程度の微量の添加でも殆ど窒素が除
去される。以上のように、窒素ゲッター及び炭化物分解
性物質を併用することにより、ＡｌやＴｉなどの従来の
窒素ゲッターを用いる場合より、速い成長速度で無色透
明でインクルージョンのない良質なIIａダイヤモンド結
晶を合成することが可能となる。具体的には例えばＣｕ
とＴｉをＣｕＴｉ金属間化合物の形で溶媒金属に対し１
重量％添加した場合、成長速度２．５ｍｇ／ｈｒでも、
無色透明な良質なIIａダイヤモンド結晶が得られる。Next, the reason for this will be specifically described.
As described above, when only Ti is used as a nitrogen getter, a colorless and transparent diamond crystal can be obtained with a small amount of up to 1% by weight because of high reactivity with nitrogen, but TiC is contained in the solvent. Generates in large quantities. Therefore, even if the crystal growth is inhibited or the growth rate of the crystal is significantly reduced, the TiC is taken into the crystal and almost no high-quality crystal is obtained. However, while adding Ti as a nitrogen getter, without forming carbides,
In addition, by simultaneously adding Cu having a function of dissolving and decomposing TiC, the inclusion of inclusion due to the influence of TiC in the solvent can be suppressed. Further Ti
Alloy or intermetallic compound consisting of Cu and Cu, such as CuTi
When such is added, it is more effective, and it becomes easier to obtain a good quality crystal. In addition, the nitrogen removal efficiency is almost the same as that of Ti, and almost even nitrogen is removed by a small amount of about 1% by weight. As described above, by using a nitrogen getter and a carbide decomposable substance together, a high-quality IIa diamond crystal that is colorless, transparent, and free of inclusions is synthesized at a higher growth rate than when a conventional nitrogen getter such as Al or Ti is used. It becomes possible. Specifically, for example, Cu
And Ti in the form of CuTi intermetallic compound with respect to the solvent metal
Weight%, the growth rate is 2.5 mg / hr,
A colorless and transparent high-quality IIa diamond crystal is obtained.
【００１５】[0015]
【実施例】以下、本発明を実施例により具体的に説明す
るが、本発明はこれに限定されるものではない。 実施例１ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｃｏ粉末、グラファイト粉末を用い、 Ｆｅ：Ｃｏ：Ｃ＝６０：４０：４．５（重量比） となるように配合した。これに、さらに平均粒径５０ミ
クロンのＴｉ粉末と、平均粒径５０ミクロンのＣｕ粉末
をいずれも溶媒金属量（グラファイトを除く）に対し
１．５重量％添加し、十分に混合した。この混合粉末を
型押し成形し、脱ガス、焼成したもの（直径２０ｍｍ、
厚み１０ｍｍ）を溶媒とした。図１に示す試料室構成で
炭素源（１）にはダイヤモンドの粉末、種結晶（３）に
は直径５００ミクロンのダイヤモンド結晶３個を用い
た。そして、炭素源（１）と種結晶（３）部に約３０℃
の温度差がつくように加熱ヒーター（５）内にセットし
た。これを超高圧発生装置を用いて、圧力５．５ＧＰ
ａ、温度１３００℃で７０時間保持し、ダイヤモンドの
合成を行った。その結果０．７〜０．９カラットの無色
透明な、インクルージョンのほとんどない良質なIIａ型
のダイヤモンド結晶が得られた。ＥＳＲにより、結晶中
の窒素濃度を測定するといずれも０．１ｐｐｍ以下であ
った。磁気天秤によりインクルージョン量を測定すると
いずれも０．５重量％以下であった。EXAMPLES The present invention will be described below in more detail with reference to examples, but the present invention is not limited to these examples. Example 1 High purity F having a particle size of 50 to 100 microns as a raw material of a solvent
e powder, Co powder, and graphite powder were blended so that Fe: Co: C = 60: 40: 4.5 (weight ratio). Further, 1.5 wt% of a Ti powder having an average particle diameter of 50 μm and a Cu powder having an average particle diameter of 50 μm were added to the amount of the solvent metal (excluding graphite) by 1.5% by weight and mixed well. This mixed powder was stamped, degassed and fired (diameter 20 mm,
(Thickness 10 mm) was used as a solvent. In the sample chamber configuration shown in FIG. 1, diamond powder was used for the carbon source (1), and three diamond crystals having a diameter of 500 μm were used for the seed crystal (3). Then, about 30 ° C. was applied to the carbon source (1) and the seed crystal (3).
Was set in the heater (5) so that the temperature difference was obtained. This was converted to a pressure of 5.5 GP using an ultra-high pressure generator.
a, The temperature was maintained at 1300 ° C. for 70 hours to synthesize diamond. As a result, a colorless and transparent, good quality IIa type diamond crystal having almost no inclusions of 0.7 to 0.9 carats was obtained. The nitrogen concentration in the crystals measured by ESR was 0.1 ppm or less in all cases. The inclusion amount was measured by a magnetic balance and found to be 0.5% by weight or less in all cases.
【００１６】実施例２〜８ ＴｉとＣｕの添加量を重量％で（Ｔｉ，Ｃｕ）＝（０．
５，０．５）、（１，１）、（１，２）、（１，３）、
（１，５）、（２，２）、（２，３）と変えた他は実施
例１と同様にして、ダイヤモンド合成を行った。いずれ
も０．８カラット前後の良質なIIａ型ダイヤモンド結晶
が得られた。いずれの結晶も窒素濃度は０．２ｐｐｍ以
下、インクルージョン量は０．７重量％以下であった。Examples 2 to 8 The addition amounts of Ti and Cu are expressed by weight% (Ti, Cu) = (0.
5,0.5), (1,1), (1,2), (1,3),
Diamond synthesis was performed in the same manner as in Example 1 except that (1, 5), (2, 2), and (2, 3) were changed. In each case, good quality IIa type diamond crystals of about 0.8 carats were obtained. Each of the crystals had a nitrogen concentration of 0.2 ppm or less and an inclusion amount of 0.7% by weight or less.
【００１７】実施例９ Ｔｉの代わりにＺｒを用いた他は実施例１と同様に、ダ
イヤモンド結晶を合成した。その結果、実施例１と殆ど
同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 9 A diamond crystal was synthesized in the same manner as in Example 1 except that Zr was used instead of Ti. As a result, a high-quality IIa diamond crystal almost the same as that of Example 1 was obtained.
【００１８】実施例１０ Ｃｕの代わりにＡｇを用いた他は実施例１と同様に、ダ
イヤモンド結晶を合成した。その結果、実施例１と殆ど
同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 10 A diamond crystal was synthesized in the same manner as in Example 1 except that Ag was used instead of Cu. As a result, a high-quality IIa diamond crystal almost the same as that of Example 1 was obtained.
【００１９】実施例１１ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｃｏ粉末、グラファイト粉末を用い、 Ｆｅ：Ｃｏ：Ｃ＝６０：４０：４．５（重量比） となるように配合した。これに、さらに添加材として平
均粒径５０ミクロンの５０Ｔｉ−５０Ｃｕ合金粉末（重
量比）を、溶媒金属量（グラファイトを除く）に対し３
重量％添加し、十分に混合した。この混合粉末を型押し
成形し、脱ガス、焼成したもの（直径２０ｍｍ、厚み１
０ｍｍ）を溶媒とした。図１に示す試料室構成で炭素源
（１）にはダイヤモンドの粉末、種結晶（３）には直径
５００ミクロンのダイヤモンド結晶３個を用いた。そし
て、炭素源（１）と種結晶（３）部に約３０℃の温度差
がつくように加熱ヒーター（５）内にセットした。これ
を超高圧発生装置を用いて、圧力５．５ＧＰａ、温度１
３００℃で７０時間保持し、ダイヤモンドの合成を行っ
た。その結果０．７〜０．９カラットの無色透明な、イ
ンクルージョンのほとんどない良質なIIａ型のダイヤモ
ンド結晶が得られた。ＥＳＲにより、結晶中の窒素濃度
を測定するといずれも０．１ｐｐｍ以下であった。磁気
天秤によりインクルージョン量を測定するといずれも
０．３重量％以下であった。Example 11 A high purity F having a particle size of 50 to 100 microns was used as a solvent raw material.
e powder, Co powder, and graphite powder were blended so that Fe: Co: C = 60: 40: 4.5 (weight ratio). Further, 50Ti-50Cu alloy powder (weight ratio) having an average particle size of 50 microns as an additive was added to the solvent metal amount (excluding graphite) in an amount of 3%.
% By weight and mixed well. This mixed powder was stamped, degassed, and fired (diameter 20 mm, thickness 1).
0 mm) was used as a solvent. In the sample chamber configuration shown in FIG. 1, diamond powder was used for the carbon source (1), and three diamond crystals having a diameter of 500 μm were used for the seed crystal (3). Then, the carbon source (1) and the seed crystal (3) were set in the heater (5) so that a temperature difference of about 30 ° C. was obtained. Using an ultra-high pressure generator, the pressure was 5.5 GPa and the temperature was 1
The temperature was maintained at 300 ° C. for 70 hours to synthesize diamond. As a result, a colorless and transparent, good quality IIa type diamond crystal having almost no inclusions of 0.7 to 0.9 carats was obtained. The nitrogen concentration in the crystals measured by ESR was 0.1 ppm or less in all cases. The inclusion amount was measured by a magnetic balance and found to be 0.3% by weight or less in all cases.
【００２０】実施例１２〜１６ ５０Ｔｉ−５０Ｃｕ合金粉末の添加量を溶媒金属量（グ
ラファイトを除く）に対し０．５、１．０、２．０、
５．０、８．０重量％と変えた他は実施例１１と同様に
してダイヤモンド合成を行った。いずれも、０．８カラ
ット前後の良質なIIａ型ダイヤモンド結晶が得られた。
いずれの結晶も窒素量０．２ｐｐｍ以下、インクルージ
ョン量は０．３重量％以下であった。Examples 12 to 16 The addition amount of 50Ti-50Cu alloy powder was set to 0.5, 1.0, 2.0, and 0.5 with respect to the amount of solvent metal (excluding graphite).
Diamond synthesis was performed in the same manner as in Example 11 except that the weight was changed to 5.0 and 8.0% by weight. In each case, good quality IIa type diamond crystals of about 0.8 carats were obtained.
Each crystal had a nitrogen amount of 0.2 ppm or less and an inclusion amount of 0.3% by weight or less.
【００２１】実施例１７ 添加材として、７０Ｔｉ−３０Ｃｕ（重量比）合金粉末
を、２重量％添加した他は実施例１１と同様にしてダイ
ヤモンド結晶を合成した。その結果、実施例１１と殆ど
同じ、良質なIIａ型ダイヤモンド結晶が得られた。Example 17 A diamond crystal was synthesized in the same manner as in Example 11, except that 2 wt% of 70Ti-30Cu (weight ratio) alloy powder was added as an additive. As a result, a high-quality IIa type diamond crystal almost the same as that of Example 11 was obtained.
【００２２】実施例１８ 添加材として、２５Ｔｉ−７５Ｃｕ（重量比）合金粉末
を、４重量％添加した他は実施例１１と同様にしてダイ
ヤモンド結晶を合成した。その結果、実施例１１と殆ど
同じ、良質なIIａ型ダイヤモンド結晶が得られた。Example 18 Diamond crystals were synthesized in the same manner as in Example 11 except that 4 wt% of 25Ti-75Cu (weight ratio) alloy powder was added as an additive. As a result, a high-quality IIa type diamond crystal almost the same as that of Example 11 was obtained.
【００２３】実施例１９ 添加材として、１０Ｔｉ−９０Ｃｕ（重量比）合金粉末
を、８重量％添加した他は実施例１１と同様にしてダイ
ヤモンド結晶を合成した。その結果、実施例１１と殆ど
同じ、良質なIIａ型ダイヤモンド結晶が得られた。Example 19 Diamond crystals were synthesized in the same manner as in Example 11 except that 8 wt% of 10Ti-90Cu (weight ratio) alloy powder was added as an additive. As a result, a high-quality IIa type diamond crystal almost the same as that of Example 11 was obtained.
【００２４】実施例２０ 添加材として、７０Ｔｉ−３０Ａｇ（重量比）合金粉末
を、３重量％添加した他は実施例１１と同様にしてダイ
ヤモンド結晶を合成した。その結果、実施例１１と殆ど
同じ、良質なIIａ型ダイヤモンド結晶が得られた。Example 20 A diamond crystal was synthesized in the same manner as in Example 11 except that 3 wt% of 70Ti-30Ag (weight ratio) alloy powder was added as an additive. As a result, a high-quality IIa type diamond crystal almost the same as that of Example 11 was obtained.
【００２５】実施例２１ 添加材として、５０Ｔｉ−５０Ａｇ（重量比）合金粉末
を、２重量％添加した他は実施例１１と同様にしてダイ
ヤモンド結晶を合成した。その結果、実施例１１と殆ど
同じ、良質なIIａ型ダイヤモンド結晶が得られた。Example 21 A diamond crystal was synthesized in the same manner as in Example 11, except that 2 wt% of 50Ti-50Ag (weight ratio) alloy powder was added as an additive. As a result, a high-quality IIa type diamond crystal almost the same as that of Example 11 was obtained.
【００２６】実施例２２〜２６ 添加材として、ＣｕＴｉ金属間化合物合金粉末を用い、
その添加量を０．５，１．０，２．０，４．０，８．０
重量％とした他は実施例１１と同様にしてダイヤモンド
結晶を合成した。その結果、実施例１１と殆ど同じ、
０．８カラット前後の良質なIIａ型ダイヤモンド結晶が
得られた。いずれの結晶も窒素量０．２ｐｐｍ以下、イ
ンクルージョン０．３重量％以下であった。Examples 22 to 26 Using CuTi intermetallic compound alloy powder as an additive,
0.5, 1.0, 2.0, 4.0, 8.0
A diamond crystal was synthesized in the same manner as in Example 11 except that the content was changed to% by weight. As a result, almost the same as Example 11,
A good quality IIa type diamond crystal of about 0.8 carat was obtained. Each of the crystals had a nitrogen content of 0.2 ppm or less and an inclusion of 0.3% by weight or less.
【００２７】実施例２７ 添加材として、ＣｕＴｉ2 金属間化合物粉末を、１重量
％添加した他は実施例２２と同様にしてダイヤモンド結
晶を合成した。その結果、実施例２２と殆ど同じ、良質
なIIａ型ダイヤモンド結晶が得られた。Example 27 A diamond crystal was synthesized in the same manner as in Example 22, except that 1% by weight of CuTi 2 intermetallic compound powder was added as an additive. As a result, a high-quality IIa-type diamond crystal almost identical to that of Example 22 was obtained.
【００２８】実施例２８ 添加材として、ＣｕＺｒ金属間化合物粉末を、４重量％
添加した他は実施例２２と同様にしてダイヤモンド結晶
を合成した。その結果、実施例２２と殆ど同じ、良質な
IIａ型ダイヤモンド結晶が得られた。Example 28 4% by weight of CuZr intermetallic compound powder as an additive
A diamond crystal was synthesized in the same manner as in Example 22 except that it was added. As a result, almost the same high-quality
A type IIa diamond crystal was obtained.
【００２９】実施例２９ 添加材として、ＣｕＺｒ2 金属間化合物粉末を、２重量
％添加した他は実施例２２と同様にしてダイヤモンド結
晶を合成した。その結果、実施例２２と殆ど同じ、良質
なIIａ型ダイヤモンド結晶が得られた。Example 29 A diamond crystal was synthesized in the same manner as in Example 22 except that 2 % by weight of CuZr 2 intermetallic compound powder was added as an additive. As a result, a high-quality IIa-type diamond crystal almost identical to that of Example 22 was obtained.
【００３０】実施例３０ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｎｉ粉末、Ｃｏ粉末、グラファイト粉末を用
い、 Ｆｅ：Ｎｉ：Ｃｏ：Ｃ＝６０：３０：１０：４．２（重
量比） となるように配合した他は実施例１１と同様にしてダイ
ヤモンドの合成を行った。その結果、実施例１とほとん
ど同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 30 A high purity F having a particle size of 50 to 100 microns was used as a solvent raw material.
e powder, Ni powder, Co powder, and graphite powder were used in the same manner as in Example 11 except that Fe: Ni: Co: C was blended so as to be 60: 30: 10: 4.2 (weight ratio). Synthesis of diamond was performed. As a result, a high-quality IIa type diamond crystal almost the same as that of Example 1 was obtained.
【００３１】実施例３１ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｎｉ粉末、Ｍｎ粉末、グラファイト粉末を用
い、 Ｆｅ：Ｎｉ：Ｍｎ：Ｃ＝６０：３０：１０：４（重量
比） となるように配合した他は実施例１１と同様にしてダイ
ヤモンドの合成を行った。その結果、実施例１１とほと
んど同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 31 As a solvent raw material, high-purity F having a particle size of 50 to 100 microns was used.
e powder, Ni powder, Mn powder, and graphite powder, and were blended in the same manner as in Example 11 except that Fe: Ni: Mn: C was blended so as to be 60: 30: 10: 4 (weight ratio). Synthesis was performed. As a result, a high-quality IIa diamond crystal almost the same as that of Example 11 was obtained.
【００３２】実施例３２ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｎｉ粉末、グラファイト粉末を用い、 Ｆｅ：Ｎｉ：Ｃ＝７０：３０：３．５（重量比） となるように配合した他は実施例１１と同様にしてダイ
ヤモンドの合成を行った。その結果、実施例１１とほと
んど同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 32 As a solvent raw material, high-purity F having a particle size of 50 to 100 microns was used.
A diamond was synthesized in the same manner as in Example 11, except that e powder, Ni powder, and graphite powder were used and Fe: Ni: C was mixed so as to be 70: 30: 3.5 (weight ratio). As a result, a high-quality IIa diamond crystal almost the same as that of Example 11 was obtained.
【００３３】実施例３３ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｃ
ｏ粉末、グラファイト粉末を用い、 Ｃｏ：Ｃ＝１００：４．７（重量比） となるように配合した他は実施例１１と同様にしてダイ
ヤモンドの合成を行った。その結果、実施例１１とほと
んど同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 33 As a solvent raw material, high-purity C having a particle size of 50 to 100 microns.
A diamond was synthesized in the same manner as in Example 11 except that o: powder and graphite powder were used and blended so that Co: C = 100: 4.7 (weight ratio). As a result, a high-quality IIa diamond crystal almost the same as that of Example 11 was obtained.
【００３４】実施例３４ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｎ
ｉ粉末、グラファイト粉末を用い、 Ｎｉ：Ｃ＝１００：４．２（重量比） となるように配合した他は実施例１１と同様にしてダイ
ヤモンドの合成を行った。その結果、実施例１１とほと
んど同じ良質なIIａ型ダイヤモンド結晶が得られた。Example 34 A high purity N having a particle size of 50 to 100 microns was used as a solvent raw material.
A diamond was synthesized in the same manner as in Example 11, except that i: powder and graphite powder were used and Ni: C was blended so as to be 100: 4.2 (weight ratio). As a result, a high-quality IIa diamond crystal almost the same as that of Example 11 was obtained.
【００３５】比較例１ Ｃｕを添加せずに、Ｔｉのみ添加（１．５重量％）した
他は実施例１と同様にしてダイヤモンド結晶の合成を試
みた。窒素量が約０．２ｐｐｍと少ない結晶が得られた
が成長量は一個あたり０．３カラットと少なく、また多
くのＴｉＣが結晶中に見られ、溶媒の巻き込みも約１．
３重量％と多く、良質な結晶は得られなかった。Comparative Example 1 A diamond crystal was synthesized in the same manner as in Example 1 except that only Ti was added (1.5% by weight) without adding Cu. Crystals with a low nitrogen content of about 0.2 ppm were obtained, but the growth amount was as low as 0.3 carats per piece, a large amount of TiC was found in the crystals, and the entrainment of the solvent was about 1.
As high as 3% by weight, good quality crystals could not be obtained.
【００３６】比較例２ ５０Ｔｉ−５０Ｃｕ合金粉末の添加量を１５重量％とし
た他は実施例１１と同様にダイヤモンドの合成を試み
た。種結晶から成長した結晶は多結晶化しており、良質
な結晶は得られなかった。Comparative Example 2 Diamond synthesis was attempted in the same manner as in Example 11 except that the amount of the 50Ti-50Cu alloy powder was changed to 15% by weight. The crystal grown from the seed crystal was polycrystallized, and no good quality crystal was obtained.
【００３７】比較例３ 窒素ゲッターとして溶媒に添加するＴｉの量を１５重量
％とした他は実施例１と同様にダイヤモンドの合成を試
みた。種結晶から成長した結晶は多結晶化しており、良
質な単結晶は得られなかった。、また、自然核発生も多
数みられた。Comparative Example 3 Synthesis of diamond was attempted in the same manner as in Example 1 except that the amount of Ti added to the solvent as a nitrogen getter was changed to 15% by weight. The crystal grown from the seed crystal was polycrystallized, and a good single crystal was not obtained. In addition, many natural nuclei were observed.
【００３８】比較例４ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｎｉ粉末、Ｃｏ粉末を用い、 Ｆｅ：Ｎｉ：Ｃｏ＝６０：３０：１０（重量比） となるように配合し、グラファイトを添加しなかった他
は実施例１１と同様にしてダイヤモンドの合成を行っ
た。その結果、種結晶は溶媒中に溶解して消失してしま
い、ダイヤモンドの成長は認められなかった。COMPARATIVE EXAMPLE 4 As a solvent raw material, high-purity F having a particle size of 50 to 100 microns was used.
e powder, Ni powder, and Co powder, and blended so that Fe: Ni: Co = 60: 30: 10 (weight ratio), except that graphite was not added. Synthesis was performed. As a result, the seed crystal was dissolved in the solvent and disappeared, and no diamond growth was observed.
【００３９】比較例５ 溶媒の原料として粒径５０〜１００ミクロンの高純度Ｆ
ｅ粉末、Ｎｉ粉末、Ｃｏ粉末、グラファイト粉末を用
い、 Ｆｅ：Ｎｉ：Ｃｏ：Ｃ＝６０：３０：１０：７（重量
比） となるように配合した他は実施例１１と同様にしてダイ
ヤモンドの合成を行った。その結果、種結晶以外の所よ
りダイヤモンドが多数自然核発生し、このため結晶同士
が干渉し、良質なダイヤモンド結晶はほとんど得られな
かった。Comparative Example 5 High purity F having a particle size of 50 to 100 μm was used as a solvent raw material.
e powder, Ni powder, Co powder, and graphite powder were mixed in the same manner as in Example 11 except that Fe: Ni: Co: C was blended so as to be 60: 30: 10: 7 (weight ratio). Synthesis was performed. As a result, many natural nuclei of diamond were generated from places other than the seed crystal, and the crystals interfered with each other, so that almost no high-quality diamond crystal was obtained.
【００４０】[0040]
【発明の効果】以上説明したように、本発明によれば、
無色透明でインクルージョンのほとんどないダイヤモン
ド結晶を、安価に安定して合成できる。本方法によって
合成ダイヤモンドを装飾用途、光学部品などに利用する
ことが可能である。As described above, according to the present invention,
A colorless and transparent diamond crystal having almost no inclusion can be stably synthesized at low cost. By this method, synthetic diamond can be used for decorative purposes, optical components, and the like.
【図１】本発明の一具体例における結晶合成用の試料室
構成を示す概略説明図である。FIG. 1 is a schematic explanatory view showing a configuration of a sample chamber for crystal synthesis according to a specific example of the present invention.
１ 炭素源 ２ 溶媒金属 ３ 種結晶 ４ 絶縁体 ５ 黒鉛ヒーター ６ 圧力媒体 DESCRIPTION OF SYMBOLS 1 Carbon source 2 Solvent metal 3 Seed crystal 4 Insulator 5 Graphite heater 6 Pressure medium
───────────────────────────────────────────────────── フロントページの続き (58)調査した分野(Int.Cl.7，ＤＢ名) B01J 3/06 C01B 31/06 C30B 29/04 ──────────────────────────────────────────────────続 き Continued on the front page (58) Field surveyed (Int.Cl. 7 , DB name) B01J 3/06 C01B 31/06 C30B 29/04
Claims (6)
おいて、溶媒金属に窒素ゲッターとしてＴｉ、Ｚｒ、Ｈ
ｆ、Ｖ、Ｎｂ、Ｔａから選ばれる一種もしくは二種以上
の金属を添加し、かつ、Ｔｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、
Ｔａの炭化物を分解する物質を添加することを特徴とす
るダイヤモンド単結晶の合成方法。1. In a diamond crystal synthesis by a temperature difference method, Ti, Zr, H is used as a nitrogen getter as a solvent metal.
One, two or more metals selected from f, V, Nb and Ta are added, and Ti, Zr, Hf, V, Nb,
A method for synthesizing a diamond single crystal, comprising adding a substance that decomposes carbide of Ta.
化物を分解する物質がＣｕ、Ａｇ、Ａｕ、Ｚｎ、Ｃｄか
ら選ばれる金属であることを特徴とする請求項１記載の
ダイヤモンド単結晶の合成方法。2. The diamond element according to claim 1, wherein the substance that decomposes carbides of Ti, Zr, Hf, V, Nb, and Ta is a metal selected from Cu, Ag, Au, Zn, and Cd. Crystal synthesis method.
ｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａから選ばれる一種もしくは二
種以上の金属の添加量が溶媒に対して、０．１重量％以
上、５重量％以下であり、かつ、Ｔｉ、Ｚｒ、Ｈｆ、
Ｖ、Ｎｂ、Ｔａの炭化物を分解する物質の添加量が溶媒
に対して、０．１重量％以上２０重量％以下であること
を特徴とする請求項１または２記載のダイヤモンド単結
晶の合成方法。3. Ti, Z added as a nitrogen getter
The amount of one or more metals selected from the group consisting of r, Hf, V, Nb and Ta is 0.1% by weight or more and 5% by weight or less with respect to the solvent, and Ti, Zr, Hf,
3. The method for synthesizing a diamond single crystal according to claim 1, wherein the amount of the substance that decomposes carbides of V, Nb and Ta is 0.1% by weight or more and 20% by weight or less based on the solvent. .
おいて、溶媒金属にＸ−Ｙ系の合金もしくは金属間化合
物（ここで、ＸはＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａか
ら選ばれる元素、ＹはＣｕ、Ａｇ、Ａｕ、Ｚｎ、Ｃｄか
ら選ばれる元素）を添加することを特徴とするダイヤモ
ンド単結晶の合成方法。4. In a diamond crystal synthesis by a temperature difference method, an XY-based alloy or an intermetallic compound (where X is an element selected from Ti, Zr, Hf, V, Nb and Ta, and Y Is an element selected from the group consisting of Cu, Ag, Au, Zn, and Cd).
合物（ここで、ＸはＴｉ、Ｚｒ、Ｈｆ、Ｖ、Ｎｂ、Ｔａ
から選ばれる元素、ＹはＣｕ、Ａｇ、Ａｕ、Ｚｎ、Ｃｄ
から選ばれる元素）の添加量が溶媒に対して、０．１重
量％以上、１０重量％以下であることを特徴とる請求項
４記載のダイヤモンド単結晶の合成方法。5. The XY-based alloy or intermetallic compound (where X is Ti, Zr, Hf, V, Nb, Ta)
Y is Cu, Ag, Au, Zn, Cd
5. The method for synthesizing a single crystal diamond according to claim 4, wherein the amount of the element selected from the group consisting of (a) and (b) is 0.1% by weight or more and 10% by weight or less based on the solvent.
ｎ，Ｃｒの中から選ばれる一種もしくは二種以上からな
り、且つ０．１〜６．０重量％の炭素を含むことを特徴
とする請求項１、２、３、４、または５記載のダイヤモ
ンド単結晶の合成方法。6. The solvent metal is Fe, Co, Ni, M
The diamond according to any one of claims 1, 2, 3, 4, and 5, comprising one or more kinds selected from n and Cr, and containing 0.1 to 6.0% by weight of carbon. A method for synthesizing a single crystal.
Priority Applications (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP00905893A JP3291804B2 (en) | 1992-04-03 | 1993-01-22 | Method of synthesizing diamond single crystal |
| KR1019930013401A KR940014144A (en) | 1992-01-22 | 1993-07-16 | Manufacturing method of diamond single crystal |
| EP93306785A EP0603995A1 (en) | 1992-12-22 | 1993-08-26 | Process for the synthesising diamond single crystals |
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4-82142 | 1992-04-03 | ||
| JP8214292 | 1992-04-03 | ||
| JP00905893A JP3291804B2 (en) | 1992-04-03 | 1993-01-22 | Method of synthesizing diamond single crystal |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH05329356A JPH05329356A (en) | 1993-12-14 |
| JP3291804B2 true JP3291804B2 (en) | 2002-06-17 |
Family
ID=13766186
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP00905893A Expired - Fee Related JP3291804B2 (en) | 1992-01-22 | 1993-01-22 | Method of synthesizing diamond single crystal |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3291804B2 (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0603995A1 (en) * | 1992-12-22 | 1994-06-29 | Sumitomo Electric Industries, Limited | Process for the synthesising diamond single crystals |
| US7404399B2 (en) | 2003-10-10 | 2008-07-29 | Sumitomo Electric Industries, Ltd. | Diamond tool, synthetic single crystal diamond and method of synthesizing single crystal diamond, and diamond jewelry |
| EP4067540A4 (en) * | 2019-11-26 | 2022-12-28 | Sumitomo Electric Industries, Ltd. | Synthetic single crystal diamond, tool equipped with same, and synthetic single crystal diamond production method |
-
1993
- 1993-01-22 JP JP00905893A patent/JP3291804B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH05329356A (en) | 1993-12-14 |
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