JP2000185920A - Production of oxide polycrystal and apparatus therefor - Google Patents

Production of oxide polycrystal and apparatus therefor

Info

Publication number
JP2000185920A
JP2000185920A JP10368125A JP36812598A JP2000185920A JP 2000185920 A JP2000185920 A JP 2000185920A JP 10368125 A JP10368125 A JP 10368125A JP 36812598 A JP36812598 A JP 36812598A JP 2000185920 A JP2000185920 A JP 2000185920A
Authority
JP
Japan
Prior art keywords
crucible
raw material
oxide polycrystal
container
oxide
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
Application number
JP10368125A
Other languages
Japanese (ja)
Inventor
Yoji Yamashita
洋二 山下
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Toshiba Corp
Original Assignee
Toshiba Corp
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Toshiba Corp filed Critical Toshiba Corp
Priority to JP10368125A priority Critical patent/JP2000185920A/en
Publication of JP2000185920A publication Critical patent/JP2000185920A/en
Pending legal-status Critical Current

Links

Landscapes

  • Inorganic Compounds Of Heavy Metals (AREA)

Abstract

PROBLEM TO BE SOLVED: To provide an oxide polycrystal production unit enabling an oxide polycrystal of a high bulk density to be easily produced in high purity. SOLUTION: For producing an oxide polycrystal, a sintered stock is put into a crucible 1 which is then heated through induction heating coils 8 to effect melting the stock into a melt. By decreasing or stopping electric power supply to the coils 8, the temperature of the crucible 1 falls, resulting in solidification, namely crystallization of the melt in the crucible 1, thereby forming a polycrystalline stock inside the crucible 1. By applying a light shock to the iridium crucible 1, the polycrystalline stock is debonded off the crucible 1; because the diameter of the crucible 1 gets larger toward its opening, the polycrystalline stock can be easily drawn off the crucible 1.

Description

【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION

【０００１】[0001]

【発明の属する技術分野】本発明は、容器を用いて酸化
物多結晶を製造する酸化物多結晶の製造方法およびその
装置に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method and an apparatus for producing polycrystalline oxide using a container.

【０００２】[0002]

【従来の技術】近年、表面弾性波素子や光学素子の基板
に、タンタル酸リチウム単結晶またはニオブ酸リチウム
単結晶などの酸化物単結晶が用いられている。2. Description of the Related Art In recent years, an oxide single crystal such as a lithium tantalate single crystal or a lithium niobate single crystal has been used for a substrate of a surface acoustic wave element or an optical element.

【０００３】そして、タンタル酸リチウムあるいはニオ
ブ酸リチウムなどの酸化物単結晶は融点が高いことか
ら、一般に、白金、白金−ロジウム、イリジウムなどの
貴金属るつぼを用いたチョクラルスキー法で製造されて
いる。Since oxide single crystals such as lithium tantalate and lithium niobate have a high melting point, they are generally produced by the Czochralski method using a noble metal crucible such as platinum, platinum-rhodium and iridium. .

【０００４】また、これら酸化物単結晶の引上げは、る
つぼ内に収容した溶融原料の半分程度の原料を引上げ単
結晶に用い、残りの固化したるつぼ残に引上げで消費し
た分の原料を粉末状の焼結原料で追加して次の引上げを
し、定まった回数引上げした後に、るつぼ残を取り除
き、るつぼ残無しのすべて新しい原料で引上げを再開し
ている。[0004] In addition, in the pulling of these oxide single crystals, about half of the raw material contained in the crucible is used as the pulling single crystal, and the remaining solidified crucible residue is converted into powdery material by the amount consumed by pulling. After additional pulling up with the sintering raw material and pulling up a fixed number of times, the crucible residue is removed, and the pulling is restarted with all new raw materials without crucible residue.

【０００５】そして、新しい原料は、粉末状の焼結原料
のみでは嵩蜜度が低くるつぼ内に焼結原料を一度で充填
しきれないので、２〜３回に分けて追加している。[0005] A new raw material is added in two or three times because a powdery sintering raw material alone cannot fill a crucible having a low bulkiness at a time with a sintering raw material at one time.

【０００６】ところが、一旦、るつぼ内に焼結原料を収
容して溶融、固化させ、さらに、焼結原料を追加すると
いう方法のため、一回日の焼結原料を収容し２回目の焼
結原料の追加まででほぼ１日の時間を要するので、引上
機の稼働率が低下してしまう。However, since the sintering raw material is once stored in a crucible, melted and solidified, and then the sintering raw material is added, the sintering raw material for one day is stored and the second sintering is performed. Since it takes approximately one day to add the raw materials, the operating rate of the pulling machine decreases.

【０００７】一方、原料の全重量の半分程度の結晶状の
原料をるつぼ内に収容することも用いられており、結晶
状の原料としては、スライス工程で生じる結晶ヘッド、
テールなど余品の他、引上結晶の不良品などが充当され
る。On the other hand, it has also been used to accommodate a crystalline raw material of about half of the total weight of the raw material in a crucible. The crystalline raw material includes a crystal head generated in a slicing step,
In addition to surplus items such as tails, defective products such as pulled crystals are used.

【０００８】ところが、結晶状の原料の確保は不良の結
晶が生じることを前提として考えており、結晶歩留まり
が向上すると結晶状の原料が不足してしまう。[0008] However, it is considered that the securing of the crystalline raw material is based on the premise that defective crystals are generated. When the crystal yield is improved, the crystalline raw material becomes insufficient.

【０００９】また、稼働率の問題のみを考えるなら、専
用の結晶状の原料作成機を用意し、るつぼ内での原料の
溶融、固化に専用の結晶状の原料作成機を用いればよ
く、大きなるつぼを用いれば、結晶状の原料作成の効率
も十分に上がる。If only the problem of the operation rate is considered, a dedicated crystal raw material preparation machine may be prepared, and a dedicated crystal raw material preparation machine may be used for melting and solidifying the raw material in the crucible. If a crucible is used, the efficiency of producing a crystalline raw material can be sufficiently increased.

【００１０】[0010]

【発明が解決しようとする課題】しかしながら、専用の
結晶状の原料作成機を用いた場合でも、固化した結晶を
るつぼから抜き取るという作業が必要になり、るつぼ内
の結晶をるつぼから抜き取るには、るつぼ内の結晶を直
接に欠き取らなければならず、結晶状の原料が汚染され
てしまい、引上げ用の原料としては用いることができな
くなる場合が生じるという問題を有している。However, even when a dedicated crystal raw material preparing machine is used, it is necessary to extract the solidified crystal from the crucible. In order to extract the crystal in the crucible from the crucible, The crystal in the crucible must be directly chipped off, and the crystalline raw material is contaminated, which causes a problem that the raw material cannot be used as a raw material for pulling.

【００１１】本発明は、上記問題点に鑑みなされたもの
で、嵩密度の高い酸化物多結晶を容易に容易にかつ高純
度で製造できる酸化物多結晶の製造方法およびその装置
を提供することを目的とする。SUMMARY OF THE INVENTION The present invention has been made in view of the above problems, and provides a method and an apparatus for producing an oxide polycrystal which can easily and easily produce an oxide polycrystal having a high bulk density with high purity. With the goal.

【００１２】[0012]

【課題を解決するための手段】本発明は、貴金属製で上
部の開口方向に向けて径が増大する形状の容器に材料を
入れ、この材料を昇温させて溶融し、この溶融した材料
を降温して固化して酸化物多結晶を生成し、前記容器か
らこの酸化物多結晶を取り出すもので、容器は貴金属製
で上部の開口方向に向けて径が増大する形状のため、容
器から酸化物多結晶を取り出す際にも、容易に酸化物多
結晶を抜き取れる。SUMMARY OF THE INVENTION According to the present invention, a material is placed in a container made of a noble metal and having a shape whose diameter increases toward an upper opening direction, and the material is heated and melted. The polycrystalline oxide is generated by lowering the temperature to produce polycrystalline oxide, and the polycrystalline oxide is taken out of the container. Since the container is made of a noble metal and has a shape whose diameter increases toward the upper opening direction, the container is oxidized. The oxide polycrystal can be easily extracted also when taking out the material polycrystal.

【００１３】また、貴金属は、イリジウムであるので、
容器に接する部分の結晶は非常に細かくなるため、酸化
物多結晶は容易に容器から剥離する。Further, since the noble metal is iridium,
Since the crystal in the portion in contact with the container is very fine, the oxide polycrystal is easily separated from the container.

【００１４】さらに、酸化物多結晶を取り出す前に容器
に衝撃を与え酸化物多結晶を容器から剥離するもので、
簡単に酸化物多結晶が容器から剥離する。Further, before removing the polycrystalline oxide, a shock is applied to the container to separate the polycrystalline oxide from the container.
The oxide polycrystal easily peels from the container.

【００１５】またさらに、容器は、５°以上の角度で径
が増大するもので、酸化物多結晶を容器から抜き取る際
に容易に抜き取れる。Still further, since the diameter of the container increases at an angle of 5 ° or more, the oxide polycrystal can be easily extracted from the container.

【００１６】また、容器の外周に設けられた誘導加熱手
段であるもので、簡単に容器を加熱できる。The induction heating means provided on the outer periphery of the container can easily heat the container.

【００１７】[0017]

【発明の実施の形態】以下、本発明の一実施の形態の酸
化物多結晶の製造装置を図面を参照して説明する。DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS A polycrystalline oxide manufacturing apparatus according to an embodiment of the present invention will be described below with reference to the drawings.

【００１８】図１に示すように、１は容器としてのるつ
ぼで、このるつぼ１は貴金属であるイリジウム（Ｉｒ）
製で、上部が開口され上部に向けてテーパ状に５°以上
の角度で直径が増大した形状である。また、このるつぼ
１上には反射板２が取り付けられ、この反射板２より上
方にはるつぼ１の上部の開口と同径で筒状のアフターヒ
ータ３が設けられている。そして、このるつぼ１は断熱
材４を介して耐火物部材５に収納され、るつぼ１は支持
台６により耐火物部材５に支持されている。As shown in FIG. 1, reference numeral 1 denotes a crucible as a container, and the crucible 1 is made of iridium (Ir) which is a noble metal.
It has a shape whose diameter is increased at an angle of 5 ° or more in a tapered shape toward the upper portion with an open upper portion. A reflecting plate 2 is mounted on the crucible 1, and a cylindrical after heater 3 having the same diameter as the upper opening of the crucible 1 is provided above the reflecting plate 2. The crucible 1 is housed in a refractory member 5 via a heat insulating material 4, and the crucible 1 is supported on the refractory member 5 by a support 6.

【００１９】また、耐火物部材５の周囲には石英管７が
配設され、この石英管７の周囲にはるつぼ１などを加熱
する誘導加熱手段としての誘導加熱コイル８が巻回され
ている。A quartz tube 7 is provided around the refractory member 5, and an induction heating coil 8 is wound around the quartz tube 7 as induction heating means for heating the crucible 1 and the like. .

【００２０】そして、酸化物多結晶を形成する際には、
図２に示すように、るつぼ１のなかに焼結原料11を収容
し、誘導加熱コイル８によりるつぼ１を加熱し、図３に
示すように、焼結原料11が融け融液12となる。ここで、
誘導加熱コイル８への電力を減少あるいは停止すること
により、るつぼ１の温度が下がり、るつぼ１内の融液が
固体化、すなわち結晶化することで、多結晶の結晶状の
原料13がるつぼ１内に形成される。When forming the oxide polycrystal,
As shown in FIG. 2, the sintering raw material 11 is accommodated in the crucible 1 and the crucible 1 is heated by the induction heating coil 8, and as shown in FIG. here,
By reducing or stopping the power to the induction heating coil 8, the temperature of the crucible 1 is lowered, and the melt in the crucible 1 is solidified, that is, crystallized, so that the polycrystalline crystalline raw material 13 is converted into the crucible 1. Formed within.

【００２１】さらに、このるつぼ１に軽い衝撃を加える
ことにより、結晶状の原料13がるつぼ１から剥離し、る
つぼ１は開口部方向に向かって直径が大きくなるので、
結晶の原料13の抜き取りも容易にできる。Further, by applying a light impact to the crucible 1, the crystalline raw material 13 is separated from the crucible 1, and the diameter of the crucible 1 increases toward the opening.
Extraction of the crystal raw material 13 can also be easily performed.

【００２２】そして、チョクラルスキー法により多結晶
を単結晶に成長させるに際し、このるつぼ１の結晶状の
原料13を結晶状の原料として用いる。このように、液引
上機とは別の他の引上機あるいは専用の結晶原料作成機
を用いて、るつぼ１内で焼結原料のような嵩密度の低い
原料を溶融、固体化させることにより、嵩密度の大きい
結晶状の原料を別途に作成し、るつぼ１から容易に結晶
状の原料を容易に抜き取ることができる。When growing a polycrystal into a single crystal by the Czochralski method, the crystalline raw material 13 of the crucible 1 is used as a crystalline raw material. As described above, a material having a low bulk density, such as a sintering material, is melted and solidified in the crucible 1 using another pulling machine different from the liquid pulling machine or a dedicated crystal raw material preparing machine. Thereby, a crystalline raw material having a large bulk density can be separately prepared, and the crystalline raw material can be easily extracted from the crucible 1.

【００２３】このため、るつぼ１内の結晶状の材料を非
接触で抜き出すことができるため、結晶状の材料が汚染
される心配はない。For this reason, since the crystalline material in the crucible 1 can be extracted without contact, there is no fear that the crystalline material is contaminated.

【００２４】したがって、たとえば引上法での酸化物単
結晶育成において用いられる嵩密度の高い結晶状の原料
を容易にかつ高純度で作成することができ、大量の原料
を一回で注入できるので、炉内の耐火物部材５の変形を
防止したり、引上機の稼働率の低下を防止できる。Therefore, for example, a crystalline raw material having a high bulk density used for growing an oxide single crystal by the pulling method can be easily and highly purified, and a large amount of the raw material can be injected at one time. In addition, it is possible to prevent the refractory member 5 in the furnace from being deformed and to prevent the operating rate of the pulling machine from being lowered.

【００２５】次に、実験結果に基づいて上述の作用、効
果などについて説明する。Next, the operation, effects, and the like described above will be described based on experimental results.

【００２６】まず、るつぼ１の材質としては、イリジウ
ム（Ｉｒ）の他に、白金（Ｐｔ）あるいは白金−ロジウ
ム（Ｐｔ−Ｒｈ）が一般的であるが、タンタル酸リチウ
ム（Ｌｉ2 ＴａＯ3 ）がるつぼ１内で固化するとき、イ
リジウムのるつぼ１を用いると、軽い衝撃をるつぼ１に
加えただけで、この多結晶の部分がるつぼ１の内面より
容易に剥離した。これは、るつぼ１の内面に接する部分
の結晶は非常に細かい多結晶となっているためと考えら
れ、るつぼ１の材質が白金や白金−ロジウムの場合には
見られない現象である。First, as a material of the crucible 1, platinum (Pt) or platinum-rhodium (Pt-Rh) is generally used in addition to iridium (Ir), and lithium tantalate (Li 2 TaO 3 ) is used. When the iridium crucible 1 was used for solidification in the crucible 1, the polycrystalline portion was easily separated from the inner surface of the crucible 1 by applying only a light impact to the crucible 1. This is considered to be due to the fact that the crystals in contact with the inner surface of the crucible 1 are very fine polycrystals, and this phenomenon is not seen when the material of the crucible 1 is platinum or platinum-rhodium.

【００２７】したがって、この性質を利用して、イリジ
ウムのるつぼ１にるつぼ１の内面より剥離している大量
の結晶状の酸化物多結晶であるタンタル酸リチウムを容
易に作成できた。Therefore, utilizing this property, a large amount of polycrystalline lithium tantalate, which is a large amount of crystalline oxide polycrystal, which is peeled from the inner surface of the crucible 1 in the iridium crucible 1 can be easily formed.

【００２８】次に、るつぼ１としては、図５に示すよう
に、直径１８０ｍｍφ、高さ１８０ｍｍのイリジウム製
のものを用いて実験した。Next, as shown in FIG. 5, an experiment was conducted using a crucible 1 made of iridium having a diameter of 180 mm and a height of 180 mm.

【００２９】そして、このるつぼ１内にモル比の組成比
がＬｉ／Ｔａ＝０．９４３なるように、Ｌｉ2 ＣＯ3 と
Ｔａ2 Ｏ5 との粉を秤量して焼成した焼結原料を、２０
００ｇ、３０００ｇ、４０００ｇ、５０００ｇおよび６
０００ｇのように５通りの重量分を入れて、昇温、溶融
した後、降温、固化させて、るつぼ１内にタンタル酸リ
チウムの多結晶の結晶状の原料を作成した。Then, powder of Li 2 CO 3 and Ta 2 O 5 was weighed and calcined so that the composition ratio of Li / Ta = 0.943 in the crucible 1, 20
00g, 3000g, 4000g, 5000g and 6g
Five kinds of weights such as 000 g were added, and the temperature was raised and melted, then, the temperature was lowered and solidified to prepare a polycrystalline lithium tantalate raw material in the crucible 1.

【００３０】その後、作成した結晶状の原料の入ったる
つぼ１を逆さまにして、るつぼ１の底および側面を木槌
で叩き、るつぼ１内の多結晶の結晶状の原料の脱着状態
を調べると、表１に示す結果となった。Thereafter, the crucible 1 containing the formed crystalline material is turned upside down, and the bottom and sides of the crucible 1 are hit with a wooden mallet to check the desorption state of the polycrystalline crystalline material in the crucible 1. Table 1 shows the results.

【００３１】[0031]

【表１】 また、るつぼ１内の原料が少量の場合は、るつぼ１内の
結晶状の原料13が容易に完全に取り除ける。すなわち、
るつぼ１内に形成された結晶状の原料の状態であるが、
結晶状の原料13が少量、たとえば２０００ｇの場合は、
図６に示すように、結晶状の原料13は中央が盛り上がる
台地状の形状でるつぼ１の内面との接触部分はるつぼ１
の底面のみであった。また、原料が中量、たとえば３０
００ｇの場合は、図７に示すように、結晶状の原料13は
るつぼ１の側面にも一部で接触部分が生じていた。さら
に、原料が大量、たとえば４０００ｇの場合は、図８に
示すように、るつぼ１内の結晶状の材料13は水をるつぼ
１に入れたような形状で、るつぼ１の側面に結晶状の原
料13が接触していた。このように、るつぼ１内の結晶状
の材料の脱着のし易さは、るつぼ１の側面と結晶状の材
料13の接触部分の多さと関係していると考えられる。[Table 1] When the amount of the raw material in the crucible 1 is small, the crystalline raw material 13 in the crucible 1 can be easily and completely removed. That is,
It is the state of the crystalline raw material formed in the crucible 1,
When the amount of the crystalline raw material 13 is small, for example, 2000 g,
As shown in FIG. 6, the crystal raw material 13 has a plateau-like shape in which the center rises, and the portion in contact with the inner surface of the crucible 1 is the crucible 1.
It was only the bottom. Also, if the raw material is in a medium amount, for example 30
In the case of 00 g, as shown in FIG. 7, the crystalline raw material 13 had a contact portion on a part of the side surface of the crucible 1. Further, when the raw material is a large amount, for example, 4000 g, as shown in FIG. 8, the crystalline material 13 in the crucible 1 is shaped like water is put in the crucible 1, and the crystalline raw material is placed on the side of the crucible 1. 13 were in contact. As described above, it is considered that the ease of desorption of the crystalline material in the crucible 1 is related to the number of contact portions between the side surface of the crucible 1 and the crystalline material 13.

【００３２】さらに、上方に向けて広がる角度と抜き取
りやすさについて実験した。Further, an experiment was conducted on the angle spreading upward and the ease of removal.

【００３３】この実験では、上方に向けて広がる角度が
０°のストレート、２．５°、５°および１０°の４種
のるつぼを用い、それぞれのるつぼ内には、表１に示す
実験と同様のモル比の組成比がＬｉ／Ｔａ＝０．９４３
の焼結粉を８ｋｇ入れて、昇温、溶融した後、降温、固
化させて、るつぼ１内にタンタル酸リチウムの多結晶の
結晶状の原料を作成した。In this experiment, four types of crucibles having a straight angle extending upward of 0 °, 2.5 °, 5 ° and 10 ° were used. In each crucible, the experiment shown in Table 1 was performed. A composition ratio of the same molar ratio is Li / Ta = 0.943.
Then, 8 kg of the sintered powder was added, and the temperature was raised and melted, then the temperature was lowered and solidified, so that a polycrystalline lithium tantalate raw material was formed in the crucible 1.

【００３４】そして、作成した結晶状の原料の入ったる
つぼ１を逆さまにして、るつぼ１の底および側面を木槌
で叩き、るつぼ１内の多結晶の結晶状の原料の脱着状態
を調べると、表２に示す結果となった。Then, the crucible 1 containing the prepared crystalline material is turned upside down, and the bottom and side surfaces of the crucible 1 are hit with a wooden mallet to check the desorption state of the polycrystalline crystalline material in the crucible 1. Table 2 shows the results.

【００３５】[0035]

【表２】 したがって、たとえばるつぼ１の冷却の仕方によって
は、るつぼ１内に形成された結晶状の材料13に比較的大
きな単結晶部分が含まれていたり、クラックの少ないほ
ぼるつぼ１の形のままの固い多結晶となることがあり、
るつぼ１内の結晶状の材料13がるつぼ１内で引っ掛かっ
た状態となり、固化した結晶状の材料13を容易に抜き取
ることができない場合が生じることがあるが、るつぼ１
の上方の開口部に向かって直径が大きくなる形状のもの
を用いれば、るつぼ１内の結晶状の材料13をるつぼ１よ
り容易に取り出すことができる。特に、るつぼ１の上方
の開口部に向かったテーパ角が５°以上であれば、るつ
ぼ１内に固化させた多結晶の結晶状の材料13が大量であ
っても、容易に取り出せる。[Table 2] Therefore, for example, depending on how the crucible 1 is cooled, the crystalline material 13 formed in the crucible 1 may include a relatively large single crystal portion, or may have a hard multi-crystal structure with almost no cracks in the shape of the crucible 1. May become crystals,
In some cases, the crystalline material 13 in the crucible 1 is stuck in the crucible 1 and the solidified crystalline material 13 cannot be easily removed.
If a material having a shape whose diameter increases toward the opening above is used, the crystalline material 13 in the crucible 1 can be easily taken out from the crucible 1. In particular, if the taper angle toward the opening above the crucible 1 is 5 ° or more, even if a large amount of the polycrystalline crystalline material 13 solidified in the crucible 1 can be easily taken out.

【００３６】さらに、多数回使用した場合についても、
多結晶の結晶状の材料13のるつぼ１からの脱着のし易さ
について実験した。Further, even when used many times,
An experiment was conducted on the ease of desorption of the polycrystalline material 13 from the crucible 1.

【００３７】この実験では、上方に向けて広がる角度が
５°および１０°の２種のるつぼを用い、それぞれのる
つぼ内には、表２に示す実験と同様のモル比の組成比が
Ｌｉ／Ｔａ＝０．９４３の焼結粉を８ｋｇ入れて、昇
温、溶融した後、降温、固化させて、るつぼ１内にタン
タル酸リチウムの多結晶の結晶状の原料を１００回作成
した。この実験について、５０回目と１００回目につい
ては表３に示す結果となった。In this experiment, two types of crucibles whose upwardly diverging angles were 5 ° and 10 ° were used. In each crucible, the same compositional ratio of Li / Li as in the experiment shown in Table 2 was used. 8 kg of a sintered powder of Ta = 0.943 was added, the temperature was raised and melted, then the temperature was lowered and solidified, and a polycrystalline lithium tantalate raw material was formed 100 times in the crucible 1. In this experiment, the results shown in Table 3 were obtained for the 50th test and the 100th test.

【００３８】[0038]

【表３】 このように、るつぼ１の多数回使用に対しては、テーパ
角が５°以上であればかなりの効果を得ることができ、
１０°以上であれば十分な効果があることがわかった。
すなわち、イリジウムなどの貴金属製のるつぼ１を多数
回使用することにより、るつぼ１の内表面が荒れてくる
こと、るつぼ１自体の形状に変形が見られるなどの経時
が変化があり、いずれもるつぼ１からの多結晶の結晶状
の材料の抜き取りを困難にする要因と考えられる。な
お、テーパ角を大きく設定することにより、るつぼ１に
変形が生じても、るつぼ１の上方に向かって直径が増大
する状態を保持することを可能にしていると考えられ
る。[Table 3] As described above, for a large number of uses of the crucible 1, a considerable effect can be obtained if the taper angle is 5 ° or more.
It was found that a sufficient effect was obtained when the angle was 10 ° or more.
That is, by using the crucible 1 made of a noble metal such as iridium many times, the inner surface of the crucible 1 becomes rough, and the shape of the crucible 1 itself is deformed. This is considered to be a factor that makes it difficult to extract the polycrystalline material from Step 1. It is considered that setting a large taper angle makes it possible to maintain a state in which the diameter increases toward the top of the crucible 1 even if the crucible 1 is deformed.

【００３９】また、上記実施の形態ではタンタル酸リチ
ウムを用いたが、ニオブ酸リチウム（ＬｉＮｂＯ3 ）を
用いても同様な効果が得られる。すなわち、イリジウム
製のるつぼ１の内部に接する結晶が細かい多結晶の結晶
状の材料となる現象は、イリジウムの表面と酸化物融液
の濡れ性によるものと考えられるので、タンタル酸リチ
ウムやニオブ酸リチウムに限定されるものではなく、ラ
ンガサイト型結晶のような広義の酸化物結晶のいずれで
も対応できると考えられる。Although lithium tantalate is used in the above embodiment, similar effects can be obtained by using lithium niobate (LiNbO 3 ). That is, the phenomenon that the crystal in contact with the inside of the crucible 1 made of iridium becomes a fine polycrystalline material is considered to be due to the wettability between the surface of the iridium and the oxide melt, so that lithium tantalate or niobate is used. It is considered that the present invention is not limited to lithium, and any broadly defined oxide crystal such as a langasite type crystal can be used.

【００４０】また、上記実施の形態では、上方に向けて
直線状に直径が広がるテーパ状のるつぼ１を用いたが、
たとえば図９に示すような形状の下部の一部のみがテー
パ状で上方に向かって直径が広がり所定位置から上はス
トレート状の円筒状のるつぼ21でも、生成されたた結晶
がストレート状の円筒部分にまでかかっていなければ、
図１ないし図８に示すようにストレートのテーパ状に形
成されたるつぼ１と同様の効果を得ることができる。In the above-described embodiment, the tapered crucible 1 whose diameter is increased linearly upward is used.
For example, only a part of the lower part of the shape as shown in FIG. 9 is tapered, the diameter increases upward, and even from a predetermined position, even in a straight cylindrical crucible 21, the generated crystal is a straight cylindrical crucible. If it does n’t cover the part,
As shown in FIGS. 1 to 8, the same effect as the crucible 1 formed in a straight tapered shape can be obtained.

【００４１】さらに、図１０に示すように、上方での直
径の増加の割合が下方での直径の増加の割合に比べて小
さいような断面が湾曲した曲面のるつぼ22でもよい。こ
のような形状であれば、るつぼ22自体は使用による変形
が少なく、るつぼ22内に形成された多結晶の結晶状の材
料の抜き取りが多数回使用でも損なわれない効果を有す
る。Further, as shown in FIG. 10, the crucible 22 may have a curved cross section such that the rate of increase in the diameter at the top is smaller than the rate of increase in the diameter at the bottom. With such a shape, the crucible 22 itself has little deformation due to use, and has an effect that the extraction of the polycrystalline material formed in the crucible 22 is not impaired even if it is used many times.

【００４２】[0042]

【発明の効果】本発明によれば、嵩密度の高い酸化物多
結晶を容易にかつ高純度で製造できる。According to the present invention, an oxide polycrystal having a high bulk density can be easily produced with high purity.

【図面の簡単な説明】[Brief description of the drawings]

【図１】本発明の一実施の形態の酸化物多結晶の製造装
置を示す断面図である。FIG. 1 is a cross-sectional view showing an apparatus for producing an oxide polycrystal according to an embodiment of the present invention.

【図２】同上るつぼ内に焼結原料を収容した状態を示す
説明図である。FIG. 2 is an explanatory view showing a state in which a sintering raw material is accommodated in the crucible.

【図３】同上るつぼ内に焼結原料が溶けた融液を収容し
た状態を示す説明図である。FIG. 3 is an explanatory view showing a state where a melt in which a sintering raw material is melted is accommodated in the crucible.

【図４】同上るつぼ内の融液が固化して多結晶が形成さ
れた状態を示す説明図である。FIG. 4 is an explanatory diagram showing a state in which a melt in the crucible is solidified to form a polycrystal.

【図５】同上実験に用いたるつぼを示す説明図である。FIG. 5 is an explanatory view showing a crucible used in the experiment.

【図６】同上るつぼ内に少量の焼結原料を収容した状態
を示す説明図である。FIG. 6 is an explanatory view showing a state in which a small amount of sintering material is accommodated in the crucible.

【図７】同上るつぼ内に中量の焼結原料を収容した状態
を示す説明図である。FIG. 7 is an explanatory view showing a state in which a medium amount of sintering material is accommodated in the crucible.

【図８】同上るつぼ内に多量の焼結原料を収容した状態
を示す説明図である。FIG. 8 is an explanatory view showing a state in which a large amount of sintering raw materials are accommodated in the crucible.

【図９】同上他の実施の形態のるつぼを示す説明図であ
る。FIG. 9 is an explanatory diagram showing a crucible according to another embodiment of the present invention.

【図１０】同上また他の実施の形態のるつぼを示す説明
図である。FIG. 10 is an explanatory view showing a crucible according to another embodiment of the present invention.

【符号の説明】[Explanation of symbols]

１ 容器としてのるつぼ ８ 誘導加熱手段としての誘導加熱コイル 1 Crucible as container 8 Induction heating coil as induction heating means

Claims (8)

【特許請求の範囲】[Claims] 【請求項１】 貴金属製で上部の開口方向に向けて径が
増大する形状の容器に材料を入れ、 この材料を昇温させて溶融し、 この溶融した材料を降温して固化して酸化物多結晶を生
成し、 前記容器からこの酸化物多結晶を取り出すことを特徴と
する酸化物多結晶の製造方法。1. A material is placed in a container made of a noble metal and having a shape whose diameter increases toward an upper opening direction, the material is heated and melted, and the melted material is cooled and solidified by cooling. A method for producing an oxide polycrystal, comprising: generating a polycrystal and extracting the oxide polycrystal from the container. 【請求項２】 貴金属は、イリジウムであることを特徴
とする請求項１記載の酸化物多結晶の製造方法。2. The method for producing an oxide polycrystal according to claim 1, wherein the noble metal is iridium. 【請求項３】 酸化物多結晶を取り出す前に容器に衝撃
を与え酸化物多結晶を容器から剥離することを特徴とす
る請求項２記載の酸化物多結晶の製造方法。3. The method for producing an oxide polycrystal according to claim 2, wherein an impact is applied to the container before removing the oxide polycrystal, and the oxide polycrystal is separated from the container. 【請求項４】 容器は、５°以上の角度で径が増大する
ことを特徴とする請求項１ないし３いずれか記載の酸化
物多結晶の製造方法。4. The method for producing an oxide polycrystal according to claim 1, wherein the diameter of the container increases at an angle of 5 ° or more. 【請求項５】 貴金属製で上部の開口方向に向けて径が
増大する形状の容器と、 この容器を加熱する加熱手段とを具備したことを特徴と
する酸化物多結晶の製造装置。5. An apparatus for producing an oxide polycrystal, comprising: a precious metal container having a shape whose diameter increases toward an upper opening direction; and heating means for heating the container. 【請求項６】 貴金属は、イリジウムであることを特徴
とする請求項５記載の酸化物多結晶の製造装置。6. The apparatus for producing an oxide polycrystal according to claim 5, wherein the noble metal is iridium. 【請求項７】 容器は、５°以上の角度で径が増大する
ことを特徴とする請求項５または６記載の酸化物多結晶
の製造装置。7. The apparatus according to claim 5, wherein the diameter of the container increases at an angle of 5 ° or more. 【請求項８】 加熱手段は、容器の外周に設けられた誘
導加熱手段であることを特徴とする請求項５ないし７い
ずれか記載の酸化物多結晶の製造装置。8. The apparatus for producing an oxide polycrystal according to claim 5, wherein the heating means is an induction heating means provided on an outer periphery of the vessel.
JP10368125A 1998-12-24 1998-12-24 Production of oxide polycrystal and apparatus therefor Pending JP2000185920A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP10368125A JP2000185920A (en) 1998-12-24 1998-12-24 Production of oxide polycrystal and apparatus therefor

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP10368125A JP2000185920A (en) 1998-12-24 1998-12-24 Production of oxide polycrystal and apparatus therefor

Publications (1)

Publication Number Publication Date
JP2000185920A true JP2000185920A (en) 2000-07-04

Family

ID=18491032

Family Applications (1)

Application Number Title Priority Date Filing Date
JP10368125A Pending JP2000185920A (en) 1998-12-24 1998-12-24 Production of oxide polycrystal and apparatus therefor

Country Status (1)

Country Link
JP (1) JP2000185920A (en)

Similar Documents

Publication Publication Date Title
CN108531990A (en) Single-crystal manufacturing apparatus
JP5446241B2 (en) Melt composition controlled unidirectionally solidified crystal growth apparatus and crystal growth method
JPS59213697A (en) Pulling device for single crystal semiconductor
JP2000185920A (en) Production of oxide polycrystal and apparatus therefor
JPWO2005113436A1 (en) Cooled lump of molten silicon and method for producing the same
JPH1192284A (en) Production of silicon ingot having polycrystal structure solidified in one direction
JP6702249B2 (en) Oxide single crystal manufacturing method and oxide single crystal pulling apparatus
JP2995912B2 (en) Method for removing residual raw material in crucible
JP2018100202A (en) METHOD FOR GROWING LiNbO3 SINGLE CRYSTAL
JP2019043787A (en) Crystal growth apparatus and method of manufacturing single crystal
JPH11189487A (en) Production apparatus for oxide single crystal
US6497762B1 (en) Method of fabricating crystal thin plate under micro-gravity environment
JP2005239442A (en) Manufacturing method of oxide single crystal
JPH0477708B2 (en)
JP2022146327A (en) MANUFACTURING METHOD OF FeGa ALLOY SINGLE CRYSTAL
JPH0377159B2 (en)
JP2535773B2 (en) Method and apparatus for producing oxide single crystal
JP2002167295A (en) Method of removing raw material remained in crucible
JPH08133884A (en) Production of single crystal
JPS58151391A (en) Ampoule for producing semiconductor crystal
JP2023132269A (en) Apparatus and method for growing oxide single crystal
JP2022146328A (en) MANUFACTURING METHOD OF FeGa ALLOY SINGLE CRYSTAL
JPH08133883A (en) Single crystal growth apparatus
JPS60151296A (en) Manufacture of single crystal
JPH10338593A (en) Noble metal crucible for signal crystal growth by pulling up method