CN110975761A - Method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure - Google Patents
Method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure Download PDFInfo
- Publication number
- CN110975761A CN110975761A CN201911290356.2A CN201911290356A CN110975761A CN 110975761 A CN110975761 A CN 110975761A CN 201911290356 A CN201911290356 A CN 201911290356A CN 110975761 A CN110975761 A CN 110975761A
- Authority
- CN
- China
- Prior art keywords
- crystal
- diamond
- seed
- seed crystal
- synthesizing
- 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.)
- Pending
Links
Images
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
-
- 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
-
- 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
- B01J3/065—Presses for the formation of diamonds or boronitrides
-
- 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
- B01J2203/0605—Composition of the material to be processed
- B01J2203/062—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
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Crystals, And After-Treatments Of Crystals (AREA)
- Carbon And Carbon Compounds (AREA)
Abstract
The invention discloses a method for synthesizing a diamond single crystal by using special-shaped {100} seed crystals at high temperature and high pressure, belonging to the technical field of diamond single crystal growth in crystal growth. The method mainly comprises the steps of obtaining seed crystals, determining synthesis process parameters, assembling a cavity, synthesizing diamond at high temperature and high pressure and the like. The method has simple steps and high repeatability, can still obtain the conventional diamond crystal by using the unconventional seed crystal, greatly reduces the difficulty of obtaining the seed crystal, has good quality of the synthesized diamond crystal, and can grow the diamond with different shapes according to the requirement.
Description
Technical Field
The invention belongs to the technical field of diamond single crystal growth in crystal growth, and particularly relates to a method for synthesizing a diamond single crystal by using special-shaped {100} seed crystals.
Background
Diamond is a high-quality material with good physical and chemical properties, has great mechanical hardness, is a potential candidate material for realizing the operation of high and new devices under extreme conditions, and has wide application in other fields. With the development of artificial diamond synthesis technology in recent years, the synthesis of gem grade diamond is no longer difficult, but has the disadvantage of over-high threshold.
At present, the methods for synthesizing diamond mainly include the following two methods: chemical Vapor Deposition (CVD) and high temperature High Pressure (HPHT) processes. The CVD method can synthesize large-size diamond single crystals with few impurities, but has high requirements on seed crystals, only can select the seed crystals with the {100} crystal faces to realize two-dimensional growth, and is not very suitable for the trend of industrial production of diamond. The HPHT method for synthesizing the diamond can realize three-dimensional growth, and the crystal form is complete. Seed selection is also loose, and diamond of gem grade can be synthesized by using a millimeter-grade diamond 100 surface as a seed surface without pretreatment. Therefore, the HPHT method has great advantages in industrial production for synthesizing diamond single crystals.
The threshold for selecting the seed crystal is reduced, so that the production efficiency of the crystal can be continuously improved, the cost is reduced, and the waste is reduced. Therefore, it is one of the objectives of researchers to find new types of usable seed crystals.
Disclosure of Invention
The invention aims to overcome the defects in the prior art, find a new available seed crystal type, reduce the waste of seed crystals and crystals, reduce the use threshold of the seed crystals and reduce the cost of industrially synthesizing diamond.
The invention is characterized in that micron-sized industrial diamond is not directly used as a seed crystal, but the seed crystal is obtained by cutting any direction and shape on a common diamond {100} surface by laser. The cut seed crystals with different shapes are used for growth, because the diamond crystals are finally grown according to the crystal orientation information when the original crystal planes are cut under the influence of the crystal orientation factors, and the standard {100} high-quality crystals are finally grown.
The technical scheme adopted by the invention is as follows:
a method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure comprises the following specific steps:
1) obtaining seed crystals, selecting a diamond single crystal, cutting a {100} plane into a diamond sheet with the thickness of 1mm by using laser parallel to the plane, and cutting the diamond sheet into diamond sheets with the area of 0.4-2.3 mm by using laser vertical to the crystal plane2To obtain heterotype {100} seed crystal;
2) determining synthesis process parameters, setting the pressure of chain type six-side-top high-pressure equipment to be 4-6 GPa, and the temperature to be 1200-1350 ℃;
3) assembling a cavity, placing a graphite carbon source 7 at the high-temperature end of a synthesis cavity of a chain type six-anvil high-pressure device, placing a crystal bed 10 at the low-temperature end, placing a catalyst 8 between the carbon source 7 and the crystal bed 10, placing a seed crystal 3 at the center of the crystal bed, wherein the upper crystal face of the seed crystal 3 is flush with the surface of the crystal bed 10, and the pressure transfer media wrapping the cavity are a ceramic pressure transfer medium 4, dolomite 2 and pyrophyllite 1 in sequence from inside to outside;
4) and (3) synthesizing diamond, namely synthesizing the assembled cavity in a chain type six-side-top high-pressure device for 6-30 hours at high temperature and high pressure according to the parameters set in the step 2), so as to obtain the diamond.
Wherein, the geometric shapes in the step 1) include but are not limited to squares, rectangles, equilateral triangles, isosceles right triangles and drop shapes.
In the step 1), the included angle between the symmetry axis of the cut shape and the symmetry axis of the original crystal face is 0-90 degrees.
Has the advantages that:
1. compared with other prior art, the method has the characteristics of simple steps and high repeatability.
2. The invention is not limited to the use of micron-sized industrial diamond as the seed crystal, and the {100} surface of any crystal can be used as the seed crystal through cutting, thereby greatly reducing the threshold of using the seed crystal. And also reduces waste, several seeds can be cut from one diamond 100 plane.
3. Even if the shape of the seed crystal is irregular, the growth of the crystal is not influenced, and the finally synthesized crystal has good quality and is typical type Ib diamond.
Description of the drawings:
FIG. 1 is an assembly view of diamond single crystal synthesized by the high-temperature high-pressure temperature gradient method of the present invention.
Fig. 2 is an optical microscope photograph of a square seed synthesized diamond of example 1.
Fig. 3 is an optical microscope photograph of the rectangular seed-synthesized diamond of example 2.
Fig. 4 is an optical microscope photograph of the isosceles right triangle seed-synthesized diamond of example 3.
Fig. 5 is an optical microscope photograph of the equilateral triangular seed-synthesized diamond of example 4.
Fig. 6 is an optical microscope photograph of the seed-synthesized diamond in the form of a droplet of example 5.
Detailed Description
The diamond synthesis process in the examples is as follows:
1) and (4) obtaining seed crystals. Several diamond single crystals were selected and laser light parallel to the 100 planes was used to cut these planes into a diamond sheet 1mm thick. Then the laser is perpendicular to the crystal faces and cut into square, rectangle, isosceles right triangle, equilateral triangle and drop shape respectively, so as to obtain five kinds of heterotype {100} seed crystals with different shapes.
2) And determining synthesis process parameters. The pressure required by synthesis is 4-6 GPa, and the temperature is 1200-1350 ℃.
3) And assembling the cavity. The assembled chamber structure is shown in fig. 1. A graphite carbon source 7 is placed at the high-temperature end of the synthesis cavity, a crystal bed 10 is placed at the low-temperature end, and a catalyst 8 is placed between the carbon source 7 and the crystal bed 10. The seed crystal 3 is placed at the center of the crystal bed, the upper crystal face of the seed crystal 3 is flush with the face of the crystal bed 10, and the pressure transmission medium wrapping the cavity sequentially comprises a ceramic pressure transmission medium 4, dolomite 2 and pyrophyllite 1 from inside to outside; in addition, a steel cap 5, a graphite sheet 6 and a graphite tube 9 jointly form a conductive path penetrating through the upper part and the lower part of the cavity, and the graphite tube 9 is a main heat source.
4) And (4) synthesizing diamond. Diamond was synthesized using a chain cubic apparatus.
EXAMPLE 1 Square seed Synthesis of Diamond
The area of the seed crystal surface is 1mm2The {100} square seed crystal is synthesized for 8 hours under the conditions of 5.0GPa and 1240 ℃ temperature. The obtained optical microscope photo of the diamond is shown in figure 2, the upper left corner is a schematic diagram of the relative position relationship between the seed crystal and the original crystal during cutting, the symmetry axis of the seed crystal is superposed with the symmetry axis of the original crystal face, and the dotted line area is the position of the seed crystal after growth.
EXAMPLE 2 Synthesis of Diamond with rectangular seed crystals
The area of the seed crystal surface is 1mm2{100} rectangular seed crystal of (A), strip at 1270 ℃ pressure of 5.3GPaThe synthesis was carried out for 11 h. The obtained optical microscope photo of the diamond is shown in figure 3, the upper left corner is a schematic diagram of the relative position relationship between the seed crystal and the original crystal during cutting, the symmetry axis of the seed crystal is superposed with the symmetry axis of the original crystal face, and the dotted line area is the position of the seed crystal after growth.
Example 3 Synthesis of diamond from isosceles Right triangle seed
The area of the seed crystal surface is 2mm2The {100} isosceles right triangle seed crystal is synthesized for 11 hours under the conditions of 5.4GPa pressure and 1260 ℃ temperature. The obtained optical microscope photo of the diamond is shown in figure 4, the upper left corner is a schematic diagram of the relative position relation between the seed crystal and the original crystal during cutting, the included angle between the symmetry axis of the seed crystal and the symmetry axis of the original crystal face is about 30 degrees, and the dotted line area is the position of the grown seed crystal.
EXAMPLE 4 equilateral triangular seed Synthesis of Diamond
The area of the seed crystal surface is 0.6mm2The {100} equilateral triangle seed crystal is synthesized for 12 hours under the conditions of 5.0GPa and 1310 ℃ temperature. The obtained optical microscope photo of the diamond is shown in figure 5, the upper left corner is a schematic diagram of the relative position relationship between the seed crystal and the original crystal during cutting, the symmetry axis of the seed crystal is superposed with the symmetry axis of the original crystal face, and the dotted line area is the position of the seed crystal after growth.
EXAMPLE 5 Synthesis of Diamond by Water droplet-shaped seed Crystal
The area of the seed crystal surface is 1.6mm2The {100} square seed crystal is synthesized for 12 hours under the conditions of 4.9GPa pressure and 1230 ℃ temperature. The obtained optical microscope photo of the diamond is shown in figure 6, the upper left corner is a schematic diagram of the relative position relationship between the seed crystal and the original crystal during cutting, the included angle between the symmetry axis of the seed crystal and the symmetry axis of the original crystal face is 90 degrees, and the dotted line area is the position of the grown seed crystal.
As can be seen from the above examples, even though the cutting angles of the seed crystals are different and the shapes of the seed crystals are also quite different, the diamond synthesized under the HPHT condition has excellent quality and the appearance is consistent with that of the conventional {100} crystal, and the requirement of the method on the seed crystals is verified to be very low. And the seed crystal has wider source, and the synthesized undesirable crystal can be cut into the {100} surface to obtain the seed crystal, so that the cyclic utilization is realized, the waste of raw materials is reduced, and the cost is reduced.
Claims (3)
1. A method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure comprises the following specific steps:
1) obtaining seed crystals, selecting a diamond single crystal, cutting a {100} plane into a diamond sheet with the thickness of 1mm by using laser parallel to the plane, and cutting the diamond sheet into diamond sheets with the area of 0.4-2.3 mm by using laser vertical to the crystal plane2To obtain heterotype {100} seed crystal;
2) determining synthesis process parameters, setting the pressure of chain type six-side-top high-pressure equipment to be 4-6 GPa, and the temperature to be 1200-1350 ℃;
3) assembling a cavity, placing a graphite carbon source 7 at the high-temperature end of a synthesis cavity of a chain type six-anvil high-pressure device, placing a crystal bed 10 at the low-temperature end, placing a catalyst 8 between the carbon source 7 and the crystal bed 10, placing a seed crystal 3 at the center of the crystal bed, wherein the upper crystal face of the seed crystal 3 is flush with the surface of the crystal bed 10, and the pressure transfer media wrapping the cavity are a ceramic pressure transfer medium 4, dolomite 2 and pyrophyllite 1 in sequence from inside to outside;
4) and (3) synthesizing diamond, namely synthesizing the assembled cavity in a chain type six-side-top high-pressure device for 6-30 hours at high temperature and high pressure according to the parameters set in the step 2), so as to obtain the diamond.
2. A method for synthesizing a diamond monocrystal by using a special-shaped {100} seed crystal at high temperature and high pressure according to claim 1, wherein the geometric shape in the step 1) is a square, a rectangle, an equilateral triangle, an isosceles right triangle or a water drop.
3. The method for synthesizing the diamond single crystal by using the special-shaped {100} seed crystal at high temperature and high pressure as claimed in claim 1, wherein in the step 1), the included angle between the symmetry axis of the cut shape and the symmetry axis of the original crystal plane is 0-90 °.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911290356.2A CN110975761A (en) | 2019-12-16 | 2019-12-16 | Method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911290356.2A CN110975761A (en) | 2019-12-16 | 2019-12-16 | Method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN110975761A true CN110975761A (en) | 2020-04-10 |
Family
ID=70093891
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201911290356.2A Pending CN110975761A (en) | 2019-12-16 | 2019-12-16 | Method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN110975761A (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111763986A (en) * | 2020-07-08 | 2020-10-13 | 彭伟华 | Method for preparing diamond |
| CN112064120A (en) * | 2020-08-13 | 2020-12-11 | 中南钻石有限公司 | Seed crystal for large-size cultivation of diamond and preparation method thereof |
| CN112844233A (en) * | 2021-01-19 | 2021-05-28 | 吉林大学 | Method for regulating and controlling appearance of diamond single crystal under high temperature and high pressure |
-
2019
- 2019-12-16 CN CN201911290356.2A patent/CN110975761A/en active Pending
Non-Patent Citations (1)
| Title |
|---|
| 王遥等: "籽晶100面形状对高温高压合成金刚石大单晶的影响", 《高压物理学报》 * |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111763986A (en) * | 2020-07-08 | 2020-10-13 | 彭伟华 | Method for preparing diamond |
| CN112064120A (en) * | 2020-08-13 | 2020-12-11 | 中南钻石有限公司 | Seed crystal for large-size cultivation of diamond and preparation method thereof |
| CN112064120B (en) * | 2020-08-13 | 2021-09-03 | 中南钻石有限公司 | Seed crystal for large-size cultivation of diamond and preparation method thereof |
| CN112844233A (en) * | 2021-01-19 | 2021-05-28 | 吉林大学 | Method for regulating and controlling appearance of diamond single crystal under high temperature and high pressure |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN110975761A (en) | Method for synthesizing diamond single crystal by using special-shaped {100} seed crystal at high temperature and high pressure | |
| EP0780153B1 (en) | Diamond synthesis | |
| US7713507B2 (en) | Tough diamonds and method of making thereof | |
| US6805745B2 (en) | Large size single crystal seed crystal fabrication by intergrowth of tiled seed crystals | |
| JP5269605B2 (en) | New diamond applications / uses based on single crystal CVD diamond produced at high growth rates | |
| CN101023028A (en) | Ultratough cvd single crystal diamond and three dimensional growth thereof | |
| JP2008512342A5 (en) | ||
| KR20110104562A (en) | High pressure high temperature (hpht) method for the production of single crystal diamonds | |
| CN111020698A (en) | Method for synthesizing diamond single crystal by using special-shaped {111} seed crystals | |
| CN110055585A (en) | A kind of method of artificial synthesized column diamond large single crystal | |
| CN110639432B (en) | Square flaky diamond large single crystal and preparation equipment and preparation method thereof | |
| JPH0687691A (en) | Production of diamond and diamond single crystal substrate used in the same | |
| US7294198B2 (en) | Process for producing single-crystal gallium nitride | |
| CN217068784U (en) | Gem-grade diamond synthesis device with large cavity | |
| JPH05221791A (en) | Method for synthesizing diamond by combustion | |
| KR20090124111A (en) | Process for growing single crystal diamond | |
| GB2535572A (en) | A method of fabricating single crystal synthetic diamond products and single crystal synthetic diamond products fabricated using said method | |
| JPH0393695A (en) | Polycrystal diamond and production thereof | |
| CN111659318B (en) | Assembled block for high-temperature high-pressure modification of CVD cultivated diamond and modification method | |
| CN117552097A (en) | Substrate for single crystal diamond growth and method for producing single crystal diamond | |
| RU2162734C2 (en) | Reaction cell of high-pressure gang-punch apparatus for growing asymmetrically zonal diamond monocrystals | |
| CN112844233A (en) | Method for regulating and controlling appearance of diamond single crystal under high temperature and high pressure | |
| JP2023511395A (en) | how to grow a big diamond | |
| CN112899776A (en) | Method for synthesizing boron-hydrogen co-doped diamond single crystal | |
| JPH0380533B2 (en) |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| WD01 | Invention patent application deemed withdrawn after publication |
Application publication date: 20200410 |
|
| WD01 | Invention patent application deemed withdrawn after publication |