Gallium nitride self-supported substrate, light-emitting device and manufacturing method therefor
Provided is a self-supporting gallium nitride substrate useful as an alternative material for a gallium nitride single crystal substrate, which is inexpensive and also suitable for having a large area. This substrate is composed of a plate composed of gallium nitride-based single crystal grains, wherein the plate has a single crystal structure in the approximately normal direction. This substrate can be manufactured by a method comprising providing an oriented polycrystalline sintered body; forming a seed crystal layer composed of gallium nitride on the sintered body so that the seed crystal layer has crystal orientation mostly in conformity with the crystal orientation of the sintered body; forming a layer with a thickness of 20 μm or greater composed of gallium nitride-based crystals on the seed crystal layer so that the layer has crystal orientation mostly in conformity with crystal orientation of the seed crystal layer; and removing the sintered body.
1. A self-supporting gallium nitride substrate composed of a plate composed of a plurality of gallium nitride-based single crystal grains, wherein the plate has a single crystal structure in an approximately normal direction, wherein the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate connect to a bottom surface of the self-supporting gallium nitride substrate without intervention of a grain boundary, and wherein a ratio D T /D B , which is a ratio of a cross-sectional average diameter D T at an outermost surface of the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate to a cross-sectional average diameter D B at an outermost surface of the gallium nitride-based single crystal grains exposed at a bottom surface of the self-supporting gallium nitride substrate, is greater than 1.0.
2. The self-supporting gallium nitride substrate according to claim 1 , wherein a cross-sectional average diameter of the gallium nitride-based single crystal grains at an outermost surface of the substrate is 0.3 μm or greater.
3. The self-supporting gallium nitride substrate according to claim 2 , wherein the cross-sectional average diameter is 3 μm or greater.
4. The self-supporting gallium nitride substrate according to claim 2 , wherein the cross-sectional average diameter is 20 μm or greater.
5. The self-supporting gallium nitride substrate according to claim 1 , having a thickness of 20 μm or greater.
6. The self-supporting gallium nitride substrate according to claim 1 , having a diameter of 100 μm or greater.
7. The self-supporting gallium nitride substrate according to claim 1 , wherein the gallium nitride-based single crystal grains have crystal orientation that is mostly aligned in the approximately normal direction.
8. The self-supporting gallium nitride substrate according to claim 1 , wherein the gallium nitride-based single crystal grains are doped with an n-type dopant or a p-type dopant.
9. The self-supporting gallium nitride substrate according to claim 1 , wherein the gallium nitride-based single crystal grains are free from a dopant.
10. The self-supporting gallium nitride substrate according to claim 1 , wherein the gallium nitride-based single crystal grains are made of a mixed crystal.
11. The self-supporting gallium nitride substrate according to claim 1 , wherein an aspect ratio T/D T , which is defined as a ratio of a thickness T of the self-supporting gallium nitride substrate to a cross-sectional average diameter D T at an outermost surface of the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate, is 0.7 or greater.
12. A light emitting device comprising:
the self-supporting gallium nitride substrate according to claim 1 ; and
a light emitting functional layer formed on the substrate, wherein the light emitting functional layer has at least one layer composed of a plurality of semiconductor single crystal grains, wherein the at least one layer has a single crystal structure in an approximately normal direction.
13. The self-supporting light emitting device according to claim 12 , wherein a cross-sectional average diameter of the semiconductor single crystal grains at an outermost surface of the light emitting functional layer is 0.3 μm or greater.
14. The light emitting device according to claim 13 , wherein the cross-sectional average diameter is 3 μm or greater.
15. The light emitting device according to claim 12 , wherein the semiconductor single crystal grains have a structure in which grains are grown mostly in conformity with crystal orientation of the self-supporting gallium nitride substrate.
16. The light emitting device according to claim 12 , wherein the light emitting functional layer is composed of a gallium nitride-based material.
17. A method for manufacturing a light emitting device, comprising the steps of:
providing the self-supporting gallium nitride substrate of claim 1 ; and
forming on the self-supporting gallium nitride substrate at least one layer composed of a plurality of semiconductor single crystal grains, wherein the at least one layer has a single crystal structure in an approximately normal direction, so that the at least one layer has crystal orientation mostly in conformity with crystal orientation of the gallium nitride substrate, thereby providing a light emitting functional layer.
18. The method according to claim 17 , wherein the light emitting functional layer is composed of a gallium nitride-based material.
19. The self-supporting gallium nitride substrate according to claim 1 , wherein the ratio D T /D B is 1.5 or greater.
20. A method for manufacturing a self-supporting gallium nitride substrate, comprising the steps of:
providing an oriented polycrystalline sintered body;
forming a seed crystal layer composed of gallium nitride on the oriented polycrystalline sintered body so that the seed crystal layer has crystal orientation mostly in conformity with crystal orientation of the oriented polycrystalline sintered body;
forming a layer with a thickness of 20 μm or greater composed of gallium nitride-based crystals on the seed crystal layer so that the layer has crystal orientation mostly in conformity with crystal orientation of the seed crystal layer; and
removing the oriented polycrystalline sintered body to obtain the self-supporting gallium nitride substrate, wherein gallium nitride-based single crystal grains exposed at a o surface of the self-supporting gallium nitride substrate connect to a bottom surface of the self-supporting gallium nitride substrate without intervention of a grain boundary, and wherein a ratio D T /D B , which is a ratio of a cross-sectional average diameter D T at an outermost surface of the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate to a cross-sectional average diameter D B at an outermost surface of the gallium nitride-based single crystal grains exposed at a bottom surface of the self-supporting gallium nitride substrate, is greater than 1.0.
21. The method according to claim 20 , wherein the oriented polycrystalline sintered body is an oriented polycrystalline alumina sintered body.
22. The method according to claim 20 , wherein an average grain diameter of grains constituting the oriented polycrystalline sintered body on a plate surface is 0.3 to 1000 μm.
23. The method according to claim 20 , wherein formation of the layer composed of the gallium nitride-based crystals is performed by Na flux method.
24. The method according to claim 20 , wherein the oriented polycrystalline sintered body is transparent or translucent.
25. A self-supporting gallium nitride substrate composed of a plate composed of a plurality of gallium nitride-based single crystal grains, wherein the plate has a single crystal structure in an approximately normal direction, wherein the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate connect to a bottom surface of the self-supporting gallium nitride substrate without intervention of a grain boundary, and wherein a cross-sectional average diameter of the gallium nitride-based single crystal grains at an outermost surface of the substrate is from 20 μm to 1000 μm.
26. The self-supporting gallium nitride substrate according to claim 25 , wherein the cross-sectional average diameter is from 50 μm to 500 μm.
27. The self-supporting gallium nitride substrate according to claim 25 , having a thickness of 20 μm or greater.
28. The self-supporting gallium nitride substrate according to claim 25 , having a diameter of 100 mm or greater.
29. The self-supporting gallium nitride substrate according to claim 25 , wherein the gallium nitride-based single crystal grains have crystal orientation that is mostly aligned in the approximately normal direction.
30. The self-supporting gallium nitride substrate according to claim 25 , wherein the gallium nitride-based single crystal grains are doped with an n-type dopant or a p-type dopant.
31. The self-supporting gallium nitride substrate according to claim 25 , wherein the gallium nitride-based single crystal grains are free from a dopant.
32. The self-supporting gallium nitride substrate according to claim 25 , wherein the gallium nitride-based single crystal grains are made of a mixed crystal.
33. The self-supporting gallium nitride substrate according to claim 25 , wherein a ratio D T /D B , which is a ratio of a cross-sectional average diameter D T at an outermost surface of the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate to a cross-sectional average diameter D B at an outermost surface of the gallium nitride-based single crystal grains exposed at a bottom surface of the self-supporting gallium nitride substrate, is greater than 1.0.
34. The self-supporting gallium nitride substrate according to claim 25 , wherein an aspect ratio T/D T , which is defined as a ratio of a thickness T of the self-supporting gallium nitride substrate to a cross-sectional average diameter D T at an outermost surface of the gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate, is 0.7 or greater.
35. A light emitting device comprising:
the self-supporting gallium nitride substrate according to claim 25 ; and
a light emitting functional layer formed on the substrate, wherein the light emitting functional layer has at least one layer composed of a plurality of semiconductor single crystal grains, wherein the at least one layer has a single crystal structure in an approximately normal direction.
36. The self-supporting light emitting device according to claim 35 , wherein a cross-sectional average diameter of the semiconductor single crystal grains at an outermost surface of the light emitting functional layer is 20 μm or greater.
37. The light emitting device according to claim 36 , wherein the cross-sectional average diameter is 50 μm or greater.
38. The light emitting device according to claim 35 , wherein the semiconductor single crystal grains have a structure in which grains are grown mostly in conformity with crystal orientation of the self-supporting gallium nitride substrate.
39. The light emitting device according to claim 35 , wherein the light emitting functional layer is composed of a gallium nitride-based material.
40. A method for manufacturing a self-supporting gallium nitride substrate, comprising the steps of:
providing an oriented polycrystalline sintered body;
forming a seed crystal layer composed of gallium nitride on the oriented polycrystalline sintered body so that the seed crystal layer has crystal orientation mostly in conformity with crystal orientation of the oriented polycrystalline sintered body;
forming a layer with a thickness of 20 μm or greater composed of gallium nitride-based crystals on the seed crystal layer so that the layer has crystal orientation mostly in conformity with crystal orientation of the seed crystal layer; and
removing the oriented polycrystalline sintered body to obtain the self-supporting gallium nitride substrate, wherein gallium nitride-based single crystal grains exposed at a top surface of the self-supporting gallium nitride substrate connect to a bottom surface of the self-supporting gallium nitride substrate without intervention of a grain boundary, and wherein a cross-sectional average diameter of the gallium nitride-based single crystal grains at an outermost surface of the substrate is from 20 μm to 1000 μm.
41. The method according to claim 40 , wherein the oriented polycrystalline sintered body is an oriented polycrystalline alumina sintered body.
42. The method according to claim 40 , wherein an average grain diameter of grains constituting the oriented polycrystalline sintered body on a plate surface is 0.3 to 1000 μm.
43. The method according to claim 40 , wherein formation of the layer composed of the gallium nitride-based crystals is performed by Na flux method.
44. The method according to claim 40 , wherein the oriented polycrystalline sintered body is transparent or translucent.
45. A method for manufacturing a light emitting device, comprising the steps of:
providing the self-supporting gallium nitride substrate of claim 25 ; and
forming on the self-supporting gallium nitride substrate at least one layer composed of a plurality of semiconductor single crystal grains, wherein the at least one layer has a single crystal structure in an approximately normal direction, so that the at least one layer has crystal orientation mostly in conformity with crystal orientation of the gallium nitride substrate, thereby providing a light emitting functional layer.
46. The method according to claim 45 , wherein the light emitting functional layer is composed of a gallium nitride-based material.