JPS58125690A - Synthesis of diamond - Google Patents
Synthesis of diamondInfo
- Publication number
- JPS58125690A JPS58125690A JP57004226A JP422682A JPS58125690A JP S58125690 A JPS58125690 A JP S58125690A JP 57004226 A JP57004226 A JP 57004226A JP 422682 A JP422682 A JP 422682A JP S58125690 A JPS58125690 A JP S58125690A
- Authority
- JP
- Japan
- Prior art keywords
- carbon
- metal
- crystal
- seed crystal
- diamond
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J3/00—Processes of utilising sub-atmospheric or super-atmospheric pressure to effect chemical or physical change of matter; Apparatus therefor
- B01J3/06—Processes using ultra-high pressure, e.g. for the formation of diamonds; Apparatus therefor, e.g. moulds or dies
- B01J3/062—Processes using ultra-high pressure, e.g. for the formation of diamonds; Apparatus therefor, e.g. moulds or dies characterised by the composition of the materials to be processed
-
- C—CHEMISTRY; METALLURGY
- C30—CRYSTAL GROWTH
- C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
- C30B13/00—Single-crystal growth by zone-melting; Refining by zone-melting
- C30B13/02—Zone-melting with a solvent, e.g. travelling solvent process
-
- C—CHEMISTRY; METALLURGY
- C30—CRYSTAL GROWTH
- C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
- C30B29/00—Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape
- C30B29/02—Elements
- C30B29/04—Diamond
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2203/00—Processes utilising sub- or super atmospheric pressure
- B01J2203/06—High pressure synthesis
- B01J2203/065—Composition of the material produced
- B01J2203/0655—Diamond
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2203/00—Processes utilising sub- or super atmospheric pressure
- B01J2203/06—High pressure synthesis
- B01J2203/0675—Structural or physico-chemical features of the materials processed
- B01J2203/068—Crystal growth
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Crystallography & Structural Chemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Crystals, And After-Treatments Of Crystals (AREA)
- Carbon And Carbon Compounds (AREA)
Abstract
Description
【発明の詳細な説明】 るものである。[Detailed description of the invention] It is something that
従来のダイヤモンド合成方法は第１図（イ）に示すよう
な反応室を用いて、ダイヤモンドを高温高１ト：下で種
結晶より合成する方法が知られている。第１図（イ）は
円板状反応室の軸方向中央断面図で、１は種結晶，２は
溶媒金属（ ＦｅＩ Ｎ ’ ｌ ｃｏ＋ ｃ ｒ ＋
Ｍｎ ｌ ’Ｉ”ａまたはこれらを含む合金）、ろは
炭素供給源，５は円筒状ヒーターである。一般にこのよ
うな反応室の構成では軸方向中央部と溶媒金属底部との
間に第１図（口）のような湿度差Ａｔが生じ、これによ
る溶媒金属への炭素の溶解度差を利用して種結晶１上に
ダイヤモンドを成長させる。なお４および６はそれぞれ
Ｎａｉｌ 、パイロフィライトなどの圧力媒体である。A conventional diamond synthesis method is known in which diamond is synthesized from a seed crystal at a high temperature and under 100 mph using a reaction chamber as shown in FIG. 1(a). FIG. 1(a) is an axial center cross-sectional view of a disc-shaped reaction chamber, where 1 is a seed crystal, 2 is a solvent metal (FeI N'l co+ cr +
5 is a cylindrical heater.Generally, in such a reaction chamber configuration, a first A humidity difference At occurs as shown in the figure (mouth), and diamond is grown on the seed crystal 1 using the resulting difference in the solubility of carbon in the solvent metal. Note that 4 and 6 are Nail, pyrophyllite, etc., respectively. It is a pressure medium.
さらに説明を加えると、従来の方法ではダイヤモンド結
晶が成長するにつれてその先端部と溶媒との温度差が小
さくなる。従って大型の高品質製品を合成する場合、成
長初期には成長速度が早く結晶が成長するに従い成長速
度が遅くなるため、（１） 在来の構成の反応室では
溶媒等の不純物か含有され易く、特に種結晶に近い結晶
の底面付近で暑しい。このため不純物の極めて少ない高
品質の結晶を合成するには成長速度を遅くしなければな
らず経済的でない。To explain further, in the conventional method, as the diamond crystal grows, the temperature difference between its tip and the solvent decreases. Therefore, when synthesizing large-scale, high-quality products, the growth rate is fast in the initial stage of growth, and as the crystal grows, the growth rate slows down. , especially near the bottom of the crystal near the seed crystal. Therefore, in order to synthesize high-quality crystals with extremely few impurities, the growth rate must be slowed down, which is not economical.
（２） 高圧容器の下半分しか使うことができない。(2) Only the lower half of the high-pressure vessel can be used.
（３） 合成できる結晶の大きさに制限かある。(3) There are limits to the size of crystals that can be synthesized.
等の欠点かある。There are some drawbacks such as.
本発明は上記の点に鑑みなされたダイヤモンド合成方法
を提供するものでその特徴は、炭素または金属からなる
円筒形ヒーターの一部の利質または形状を変えることに
より結晶成長領域の温度を均一にし、かつ炭素供給源と
種結晶の間に温度差を持たせ、これによる溶媒金属への
炭素の溶解度差を利用して種結晶からダイヤモンドを成
長させることにある。The present invention provides a diamond synthesis method devised in view of the above points, and its feature is that the temperature in the crystal growth region is made uniform by changing the quality or shape of a part of the cylindrical heater made of carbon or metal. , and to create a temperature difference between the carbon supply source and the seed crystal, and to grow diamond from the seed crystal by utilizing the resulting difference in the solubility of carbon in the solvent metal.
以下本発明を図面を用いて説明する。The present invention will be explained below using the drawings.
第２図（イ）に示す円筒形ヒーターにおいて、抵抗大の
部分７と抵抗小の部分８を設け、８の発熱量を７に較べ
て小さくすることにより溶媒金属２の下の部分（結晶の
成長領域）の温度分布を第２図（ロ）のように均一にす
る。In the cylindrical heater shown in FIG. 2(a), a portion 7 with high resistance and a portion 8 with low resistance are provided, and by making the calorific value of 8 smaller than that of 7, the portion under the solvent metal 2 (the part of the crystal) The temperature distribution in the growth region) is made uniform as shown in Figure 2 (b).
または、第３図（イ）のように溶媒金属２と炭素供給源
ろとの間にＮａＣｌ等の熱伝導の低い物質でできた開口
部を有する断熱層９を設ける。この断熱層９により開口
部内の溶媒金属２または炭素供給源６の温度勾配を大き
くし、相対的に溶媒金属２の下の部分の温度勾配を第３
図（ロ）のように小さくする。Alternatively, as shown in FIG. 3(A), a heat insulating layer 9 having an opening made of a substance with low thermal conductivity such as NaCl is provided between the solvent metal 2 and the carbon supply source. This heat insulating layer 9 increases the temperature gradient of the solvent metal 2 or the carbon supply source 6 within the opening, and relatively reduces the temperature gradient of the portion below the solvent metal 2 to a third level.
Make it smaller as shown in figure (b).
本発明のダイヤモンド合成方法の利点は、（１） 従
来の方法では炭素供給源を位置させるべき最高温部が反
応室の軸方向中心にあり、合成に利用できる範囲は下半
分に限られ、上半分は対流等により良質の結晶合成には
適していないが、本発明の方法ならば反応室に任意の温
度分布を与えることができるので、反応室全体を翁効に
使うことが可能になる。The advantages of the diamond synthesis method of the present invention are as follows: (1) In the conventional method, the highest temperature area where the carbon source should be located is in the axial center of the reaction chamber, and the area available for synthesis is limited to the lower half; Half of the reaction chamber is not suitable for synthesizing high-quality crystals due to convection, etc., but the method of the present invention makes it possible to provide an arbitrary temperature distribution to the reaction chamber, making it possible to use the entire reaction chamber efficiently.
（２） 反応室内の結晶成長領域の温度が均一である
ため成長の条件が一定に保たれ、溶媒等の不純物の混入
が少ないため、高品質の結晶を合成することかできる。(2) Since the temperature of the crystal growth region in the reaction chamber is uniform, the growth conditions are kept constant and there is little contamination of impurities such as solvents, making it possible to synthesize high-quality crystals.
（３１＋１１の理由に加えて、従来の方法では結晶は温
良差の小さくなる方向へ成長してゆき、次第に成長速度
か小さくなるか、本発明の方法ではそのようなことは起
らないので、直径数ｍｍ以上の大型単結晶でも効率よく
合成することができる。(In addition to the reason for 31+11, in the conventional method, the crystal grows in the direction of decreasing temperature difference, and the growth rate gradually decreases, but in the method of the present invention, such a thing does not occur, so the diameter Even large single crystals of several mm or more can be efficiently synthesized.
等である。etc.
反応室は第４図に示すような構成とし、ヒーターとして
外径２’１ｍｍ ｌ内径、：ｌ、：１ｍｍの黒鉛円筒を
用い、その一部をＭＯの円筒とした。その円筒における
配置は」二から黒鉛７’、 Ｍｏ ｇ’、黒鉛７′の順
でその長さの比は３：２：３とした。その内側に外径／
ｇｍｍのｐｅ−１，２Ｎｉ型の円柱を溶媒金属２として
配置し、その上に炭素供給源６として３２３／’１００
メツシコーの合成ダイヤモンドと人造黒鉛粉末を重量比
で３：／に混合した粉末を配置した。この周囲には圧力
媒体４としてＮａＣ１を配置し、溶媒金属２の底面にあ
たる部分に種結晶１として３３／ｌｌｏメツシユの合成
ダイヤモンドを埋め込んだ。The reaction chamber was constructed as shown in FIG. 4, and a graphite cylinder with an outer diameter of 2'1 mm and an inner diameter of 1 mm was used as a heater, and part of the cylinder was made of MO. The arrangement in the cylinder was from graphite 7' to Mog' to graphite 7' in this order, with a length ratio of 3:2:3. Outside diameter/
A pe-1,2 Ni type cylinder of gmm is placed as the solvent metal 2, and a carbon source 6 of 323/'100 is placed on top of it as the solvent metal 2.
A powder made by mixing Metsushiko's synthetic diamond and artificial graphite powder at a weight ratio of 3:/ was placed. NaCl was placed around this as a pressure medium 4, and a 33/llo mesh synthetic diamond was embedded as a seed crystal 1 in the bottom of the solvent metal 2.
この構成体をガードル型超高圧装置を用いて加ＩＥ Ｌ
ｊｊ ｋ ｂの圧力を加え、次いでヒーターに通電し
炭素供給源乙の温度か７５００°Ｃになるよう加熱した
。This structure was subjected to IEL using a girdle-type ultra-high pressure device.
A pressure of jj k b was applied, and then electricity was applied to the heater to heat the carbon supply source B to 7500°C.
この条件をぶ０時間保持した後加熱を停止し、減圧後に
試別を取り出したところ／１１０ ｍｙの溶媒等の不純
物かほとんど混入していない単結晶か種結晶」二に成長
していた。After maintaining these conditions for 0 hours, the heating was stopped and the sample was taken out after reducing the pressure. When the sample was taken out, it was found that a single crystal or seed crystal of 110 mm had grown with almost no impurities such as solvent mixed in.
比較のため、均一の黒鉛円筒ヒーターを用い、その他の
条件を同一にした実験では８０＝−１の単結晶か得られ
たが、その内部特に種結晶の近辺にかなりの不純物が含
まれていた。For comparison, in an experiment using a homogeneous graphite cylindrical heater and keeping the other conditions the same, a single crystal of 80 = -1 was obtained, but it contained a considerable amount of impurities, especially in the vicinity of the seed crystal. .
第５図に示すような構成で、炭素供給＃＋３とｐｅ −
１７，２Ｎｉ溶媒金属２との間に直径３ ｍｍの穴をあ
げたＮａＣｌ板４を断熱層として配置し、ヒーター５に
黒鉛円筒を用いて実施例／と同じ条件で実験を行ったと
ころ／７０％ｌの溶媒等の不純物が極めて少ない良質の
単結晶が得られた。With the configuration shown in FIG. 5, carbon supply #+3 and pe −
An experiment was conducted under the same conditions as in Example/70 by placing a NaCl plate 4 with a 3 mm diameter hole between it and the 17,2Ni solvent metal 2 as a heat insulating layer and using a graphite cylinder as the heater 5. A high-quality single crystal containing very few impurities such as solvent was obtained.
第１図は従来のダイヤモンド合成方法の説明図で（イ）
は反応室の軸方向中央断面図、（ロ）は（イ）の反応室
のすｑ１１方向中央部と」ユ下端部との間のｌ晶度差状
況説明図、第２図および第３図はいずれも本発明の説明
図で（イ）は反応室の軸方向中央断面図、（ロ）は（イ
）の反ＩＩ；室の軸方向中央部と−１−下゛端部との間
の洗１【度差状況説明図、第４ ＋ｆｆｌおよび第５図
はいずれも本発明のそれぞれ異なる実施例の説明図であ
る。
１・・種結晶、２・・溶媒金属、６・・・炭素供給源、
４ ・−ＮａＣｌ （圧力媒体）、４′・ＮａＣ１板、
５・・・円筒状ヒーター、６・・・パイロフィライト（
Ｅカ媒体）、７・・抵抗穴の部分、７′・黒鉛、８・・
・抵抗小の部分、８′・・・ＭＯ１９・・・断熱層、４
ｔ・・ヒーターの軸方向中央部と浴媒金属底部との温良
差。
芳１閏
汀４図 所５閏Figure 1 is an explanatory diagram of the conventional diamond synthesis method (a)
1 is an axial center sectional view of the reaction chamber, (b) is an explanatory diagram of the difference in crystallinity between the central part in the square direction of the reaction chamber in (a) and the lower end of the reaction chamber, FIGS. 2 and 3. Both are explanatory views of the present invention, and (a) is a cross-sectional view of the reaction chamber in the axial direction, and (b) is the opposite view of (a); between the axial center of the chamber and the -1-lower end. FIG. 4 +ffl and FIG. 5 are explanatory diagrams of different embodiments of the present invention. 1... Seed crystal, 2... Solvent metal, 6... Carbon source,
4 ・-NaCl (pressure medium), 4′・NaCl1 plate,
5... Cylindrical heater, 6... Pyrophyllite (
E media), 7...Resistance hole part, 7', graphite, 8...
・Low resistance part, 8'...MO19...insulation layer, 4
t...Difference in temperature between the axial center of the heater and the bottom of the bath metal. Fang 1 Leap 4 Figure Toko 5 Lean
Claims (1)
材質または形状を変えることにより結晶成長領域の流度
を均一にし、かつ炭素供給源と種結晶の間に温度差を持
たせ、これによる溶媒金属への炭素の溶解度差を利用し
て種結晶からダイヤモンドを成長させることを特徴とす
るダイヤモンド合成方法。 ２、 円筒形ヒーターの一部の材質を元の材質に対し０
〜ＳＯ％の抵抗の材質に変えた特許請求の範囲第１項記
載のダイヤモンド合成方法。 ６、 円筒形ヒーターの一部の厚さを他の部分に酸ベア
、５倍以上にした特許請求の範囲第１項または第２項記
載のダイヤモンド合成方法。 ４、炭素供給源または金属溶媒の外径に対し、そのＨ〜
％の開口部を有する断熱層を設けた特許請求の範囲第１
項、第２項または第３項記載のダイヤモンド合成方法。[Claims] 1. By changing the material or shape of a part of the cylindrical heater made of carbon or metal, the flow rate in the crystal growth region can be made uniform, and the temperature difference between the carbon source and the seed crystal can be reduced. A diamond synthesis method characterized by growing diamond from a seed crystal by using the difference in solubility of carbon in a solvent metal. 2. Change the material of some of the cylindrical heaters to 0 compared to the original material.
The diamond synthesis method according to claim 1, wherein the material has a resistance of ~SO%. 6. The diamond synthesis method according to claim 1 or 2, wherein the thickness of a part of the cylindrical heater is 5 times or more thicker than that of the other part. 4. With respect to the outer diameter of the carbon source or metal solvent, its H~
Claim 1, which is provided with a heat insulating layer having an opening of %
The diamond synthesis method according to item 2, item 3, or item 3.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57004226A JPS58125690A (en) | 1982-01-14 | 1982-01-14 | Synthesis of diamond |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57004226A JPS58125690A (en) | 1982-01-14 | 1982-01-14 | Synthesis of diamond |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS58125690A true JPS58125690A (en) | 1983-07-26 |
Family
ID=11578662
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP57004226A Granted JPS58125690A (en) | 1982-01-14 | 1982-01-14 | Synthesis of diamond |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS58125690A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2016203950A1 (en) * | 2015-06-19 | 2016-12-22 | 住友電気工業株式会社 | Diamond single crystal, tool, and method for manufacturing diamond single crystal |
-
1982
- 1982-01-14 JP JP57004226A patent/JPS58125690A/en active Granted
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2016203950A1 (en) * | 2015-06-19 | 2016-12-22 | 住友電気工業株式会社 | Diamond single crystal, tool, and method for manufacturing diamond single crystal |
| JP2017007887A (en) * | 2015-06-19 | 2017-01-12 | 住友電気工業株式会社 | Diamond single crystal, tool, and manufacturing method of diamond single crystal |
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