Methods and devices for growing oxide crystals in oxygen atmosphere

Patent metadata

Field	Value
Publication number	US-11319645-B2
Application number	US-202016903334-A
Country	US
Kind code	B2
Filing date	Jun 16, 2020
Priority date	Aug 21, 2019
Publication date	May 3, 2022
Grant date	May 3, 2022

Abstract

The present disclosure discloses a method for growing a crystal in oxygen atmosphere. The method may include compensating a weight of a reactant, introducing a flowing gas, improving a volume ratio of oxygen during a cooling process, providing a heater in a temperature field, and optimizing parameters. According to the method, problems may be solved, for example, cracking and component deviation of the crystal during a crystal growth process, and without oxygen-free vacancy. The method for growing the crystal may have excellent repeatability and crystal performance consistency.

First claim

We claim:

1. A method for growing a crystal, comprising:
weighting reactants based on a molar ratio of the reactants according to a reaction equation for generating the crystal after a first preprocessing operation is performed on the reactants, wherein the first preprocessing operation includes a roasting operation under 800° C.˜1400° C.;
placing the reactants, on which a second preprocessing operation has been performed, into a crystal growth device after an assembly preprocessing operation is performed on a crucible of the crystal growth device, wherein
the second preprocessing operation includes at least one of a reactants mixing operation or a pressing operation at room temperature; and
the assembly processing operation includes at least one of a coating operation, an acid soaking and cleaning operation, or an impurity cleaning operation;

introducing a flowing gas into the crystal growth device after sealing the crystal growth device, the flowing gas including a mixed gas of oxygen and one or more of nitrogen and inert gas;
operating the crystal growth device to execute a crystal growth operation based on Czochralski technique, wherein the crystal growth operation at least includes a process for melting the reactants, a growing process, and a cooling process, wherein during the cooling process:
when a temperature drops to 1400° C.˜800° C., increasing a volume ratio of oxygen in the flowing gas from an initial volume ratio of oxygen in the flowing gas to 20%˜30% and reducing an initial cooling rate of the cooling process; and
when the temperature drops below 800° C., decreasing the volume ratio of oxygen in the flowing gas to 1%-20%.

2. The method of claim 1 , wherein the crystal includes gadolinium aluminum gallium garnet (GAGG), yttrium aluminum garnet (YAG), lutetium orthosilicate (LSO), lutetium yttrium orthosilicate (LYSO), gadolinium yttrium oxy orthosilicate (GYSO), terbium gallium garnet (TGG), gadolinium gallium garnet (GGG), yttrium orthovanadate (YVO4), gadolinium orthosilicate (GSO), sapphire, or a doped crystal thereof.

3. The method of claim 1 , wherein the crystal includes cerium-doped LSO or cerium-doped LYSO, and the weighting the reactants based on the molar ratio of the reactants according to the reaction equation for generating the crystal after the first preprocessing operation is performed on the reactants includes:
weighting the reactants based on the molar ratio of the reactants according to a reaction equation (1) or a reaction equation (2) after the first preprocessing operation is performed on the reactants:
(1− x )Lu 2 O 3 +SiO 2 +2 x CeO 2 →Lu 2(1-x) Ce 2x SiO 5 +x/ 2O 2 ↑  (1)

(1− x−y )Lu 2 O 3 +y Y 2 O 3 +SiO 2 +2 x CeO 2 →Lu 2(1-x-y) Y 2y Ce 2x SiO 5 +x/ 2O 2 ↑  (2)

where x=[0.0001%, 6%], y=(0, 100%), and a weight range of SiO 2 being 0.01%˜10% in excess of a weight of SiO 2 calculated according to the reaction equation (1) or the reaction equation (2).

4. The method of claim 1 , wherein a purity of each of the reactants is greater than 99%.

5. The method of claim 1 , wherein a flow rate of the flowing gas is 10 L/min˜40 L/min.

6. The method of claim 1 , wherein the initial volume ratio of oxygen in the flowing gas is 0.001%˜20%.

7. The method of claim 1 , wherein a purity of each of the reactants is greater than 99.9%.

8. The method of claim 1 , wherein the initial cooling rate is within a range of 65° C./h˜95° C./h.

9. The method of claim 1 , wherein the initial cooling rate is within a range of 55° C./h˜65° C./h.

10. The method of claim 1 , wherein the initial cooling rate is within a range of 15° C./h˜19° C./h.

11. The method of claim 1 , wherein a cooling time of the cooling process is 20 hours˜100 hours.

12. The method of claim 1 , wherein a cooling time of the cooling process is 50 hours˜70 hours.

13. The method of claim 1 , wherein a cooling time of the cooling process is 55 hours˜65 hours.

Assignees

• Meishan Boya Advanced Mat Co Ltd

Inventors

• Wang Yu
• Guan Weiming
• Li Min

Classifications

• C01F17/00

  Compounds of rare earth metals · CPC title

• C01B33/10

  Compounds containing silicon, fluorine, and other elements · CPC title

• C01B33/08

  Compounds containing halogen · CPC title

• C30B29/22 Primary

  Complex oxides · CPC title

• C09K11/7774

  Aluminates · CPC title