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WO2012093601A1 - SUBSTRAT DE CROISSANCE ÉPITAXIQUE ET DISPOSITIF À DEL AU GaN - Google Patents

SUBSTRAT DE CROISSANCE ÉPITAXIQUE ET DISPOSITIF À DEL AU GaN Download PDF

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Publication number
WO2012093601A1
WO2012093601A1 PCT/JP2011/079880 JP2011079880W WO2012093601A1 WO 2012093601 A1 WO2012093601 A1 WO 2012093601A1 JP 2011079880 W JP2011079880 W JP 2011079880W WO 2012093601 A1 WO2012093601 A1 WO 2012093601A1
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Prior art keywords
substrate
mask layer
hole
gan
growth mask
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English (en)
Japanese (ja)
Inventor
晋 平岡
覚成 勝本
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Mitsubishi Chemical Corp
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Mitsubishi Chemical Corp
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Priority to JP2012551834A priority Critical patent/JPWO2012093601A1/ja
Publication of WO2012093601A1 publication Critical patent/WO2012093601A1/fr
Anticipated expiration legal-status Critical
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10H—INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS
    • H10H20/00—Individual inorganic light-emitting semiconductor devices having potential barriers, e.g. light-emitting diodes [LED]
    • H10H20/01—Manufacture or treatment
    • H10H20/011—Manufacture or treatment of bodies, e.g. forming semiconductor layers
    • H10H20/013—Manufacture or treatment of bodies, e.g. forming semiconductor layers having light-emitting regions comprising only Group III-V materials
    • H10H20/0133—Manufacture or treatment of bodies, e.g. forming semiconductor layers having light-emitting regions comprising only Group III-V materials with a substrate not being Group III-V materials
    • H10H20/01335—Manufacture or treatment of bodies, e.g. forming semiconductor layers having light-emitting regions comprising only Group III-V materials with a substrate not being Group III-V materials the light-emitting regions comprising nitride materials
    • 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
    • C30B25/00—Single-crystal growth by chemical reaction of reactive gases, e.g. chemical vapour-deposition growth
    • C30B25/02—Epitaxial-layer growth
    • C30B25/18—Epitaxial-layer growth characterised by the substrate
    • 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
    • C30B29/10—Inorganic compounds or compositions
    • C30B29/40—AIIIBV compounds wherein A is B, Al, Ga, In or Tl and B is N, P, As, Sb or Bi
    • C30B29/403—AIII-nitrides
    • C30B29/406—Gallium nitride
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02367—Substrates
    • H01L21/0237—Materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02436—Intermediate layers between substrates and deposited layers
    • H01L21/02439—Materials
    • H01L21/02455—Group 13/15 materials
    • H01L21/02458—Nitrides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02518—Deposited layers
    • H01L21/02521—Materials
    • H01L21/02538—Group 13/15 materials
    • H01L21/0254—Nitrides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02612—Formation types
    • H01L21/02617—Deposition types
    • H01L21/02636—Selective deposition, e.g. simultaneous growth of mono- and non-monocrystalline semiconductor materials
    • H01L21/02639—Preparation of substrate for selective deposition
    • H01L21/02642—Mask materials other than SiO2 or SiN
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02612—Formation types
    • H01L21/02617—Deposition types
    • H01L21/02636—Selective deposition, e.g. simultaneous growth of mono- and non-monocrystalline semiconductor materials
    • H01L21/02647—Lateral overgrowth

Definitions

  • the present invention relates to an epitaxial growth substrate and a GaN-based LED (light emitting diode) device.
  • a GaN-based semiconductor is a compound semiconductor represented by the general formula Al a In b Ga 1-ab N (0 ⁇ a ⁇ 1, 0 ⁇ b ⁇ 1, 0 ⁇ a + b ⁇ 1), and is a group III nitride It is also called a semiconductor or a nitride-based III-V compound semiconductor.
  • An LED device structure composed of an n-type layer (n-type conductive layer), a p-type layer (p-type conductive layer), and a light emitting layer sandwiched between these layers is formed using a GaN-based semiconductor.
  • the resulting GaN-based LED device can generate light having a wavelength of near ultraviolet to green.
  • a white light emitting diode configured by combining a GaN-based LED device and a phosphor is put into practical use as a light source for a backlight unit of a liquid crystal display or a light source for white illumination.
  • a GaN-based LED device is manufactured through a process of epitaxially growing a GaN-based semiconductor on a sapphire substrate by vapor phase growth method such as MOVPE method. Therefore, a GaN-based LED device usually includes a sapphire substrate in its structure, and an LED device structure made of a GaN-based semiconductor is formed on the substrate. Recently, as the sapphire substrate, a patterned sapphire substrate (patterned sapphire substrate; hereinafter also referred to as PSS) is often used which has a non-flat surface processed by etching.
  • PSS patterned sapphire substrate
  • Non-Patent Document 1 reports a production example of a GaN-based LED device using a PSS having a triangular pyramid etched in a hot phosphoric acid-based solution. It has been reported that the output of the GaN-based LED device increases as the inclination of the pyramid side wall is made gentle (inclination angle 57.4 degrees to 31.6 degrees). Furthermore, a simulation result is obtained that the light extraction efficiency increases when the inclination angle of the pyramid sidewall is reduced from 80 degrees to 30 degrees.
  • Substantially the same as sapphire such as Al 2 O 3 , Eu 2 O 3 , La 2 O 3 , Sm 2 O 3 , WO 3 , Y 2 O 3, etc.
  • a substrate having a protrusion formed on the surface thereof made of a material having a refractive index closer to that of sapphire than a GaN-based semiconductor Patent Document 3
  • this substrate simulates PSS.
  • a GaN-based semiconductor is epitaxially grown on the PSS, which is useful for improving the light extraction efficiency, that is, a non-flat interface is formed between a GaN-based semiconductor and a sapphire having different refractive indexes. This is where the resulting structure can be introduced into LED devices.
  • the fact that the material for forming the non-flat interface with the GaN-based semiconductor is sapphire is not an essential element for the effect of improving the light extraction efficiency. That is, even if the material that forms the non-flat interface with the GaN-based semiconductor includes a non-sapphire material, if the non-sapphire material has a lower refractive index than the GaN-based semiconductor, it is comparable to PSS.
  • the interface formed between the non-sapphire material and the GaN-based semiconductor includes an inclined portion, the light extraction efficiency can be further improved.
  • the inclined portion refers to a portion inclined with respect to a plane parallel to a semiconductor layer such as a light emitting layer constituting the LED device structure.
  • one of the objects of the present invention is to provide a novel substrate for epitaxial growth for a GaN-based LED device, which gives an effect of improving the light extraction efficiency comparable to that of PSS.
  • the object of the present invention includes providing a GaN-based LED device using such a substrate for epitaxial growth.
  • an object of the present invention includes providing a method for manufacturing a GaN-based LED device using such an epitaxial growth substrate.
  • Embodiments of the present invention include the following epitaxial growth substrate, GaN-based LED device, and GaN-based LED device manufacturing method.
  • the growth mask layer has a through-hole that penetrates the growth mask layer in the thickness direction and whose cross-sectional area increases as the distance from the single crystal substrate increases.
  • the plurality of through holes are arranged so that at least the other three are adjacent to each other, and two adjacent two of the plurality of through holes arranged in this way are arbitrarily selected, and one of them is selected.
  • An epitaxial growth substrate for a GaN-based LED device wherein the first through-hole and the other through-hole are in contact with the side wall of the first through-hole and the side wall of the second through-hole.
  • the single crystal substrate is a sapphire substrate, a SiC substrate, a GaN substrate, an AlN substrate, a spinel substrate, a gallium oxide substrate, or a zinc oxide substrate.
  • the growth mask layer has a thickness of 0.5 to 3 ⁇ m.
  • the inclination angle of the side wall is 50 to 75 degrees when the distance from the single crystal substrate is half the thickness of the growth mask layer.
  • the substrate for epitaxial growth described in 1.
  • the growth mask layer has a through-hole that penetrates the growth mask layer in the thickness direction and whose cross-sectional area increases as the distance from the sapphire substrate increases.
  • the opening of the through hole on the bottom side of the growth mask layer is circular,
  • the plurality of through holes are arranged so that the other six are adjacent to each other, and two adjacent ones are arbitrarily selected from the plurality of through holes, one of which is a first through hole and the other is An epitaxial growth substrate in which the side wall of the first through hole is in contact with the side wall of the second through hole when the second through hole is formed.
  • GaN-based semiconductor laminate including an epitaxial growth substrate, an epitaxial growth layer formed on the epitaxial growth substrate, and an n-type layer, a p-type layer, and a light emitting layer sandwiched between the n-type layer and the p-type layer
  • a GaN-based LED device having: The substrate for epitaxial growth has a single crystal substrate, and a growth mask layer formed on one main surface of the single crystal substrate and including a dielectric having a lower refractive index than the GaN-based semiconductor laminate, The growth mask layer has a through-hole that penetrates the growth mask layer in the thickness direction and whose cross-sectional area increases as the distance from the single crystal substrate increases.
  • the plurality of through-holes are arranged so that at least three of them are adjacent to each other, and two adjacent two of the plurality of through-holes arranged in this way are arbitrarily selected, and one of them is the first
  • a GaN-based LED device in which the side wall of the first through hole and the side wall of the second through hole are in contact with each other when the through hole is the second through hole.
  • the single crystal substrate is a sapphire substrate, a SiC substrate, a GaN substrate, an AlN substrate, a spinel substrate, a gallium oxide substrate, or a zinc oxide substrate.
  • the inclination angle of the side wall is 30 to 75 degrees at a position half the thickness of the growth mask layer from the single crystal substrate.
  • the inclination angle of the side wall is 50 to 75 degrees when the distance from the single crystal substrate is half the thickness of the growth mask layer.
  • the GaN-based LED device described in 1. [19] The GaN-based LED device according to any one of [12] to [18], wherein the growth mask layer includes a dielectric having a lower refractive index than the single crystal substrate. [20] The GaN-based LED device according to [19], wherein the growth mask layer includes silicon oxide.
  • GaN-based semiconductor laminate including an epitaxial growth substrate, an epitaxial growth layer formed on the epitaxial growth substrate, and an n-type layer, a p-type layer, and a light emitting layer sandwiched between the n-type layer and the p-type layer
  • a GaN-based LED device having:
  • the substrate for epitaxial growth has a sapphire substrate and a growth mask layer containing silicon oxide formed on one main surface of the sapphire substrate,
  • the growth mask layer has a through-hole that penetrates the growth mask layer in the thickness direction and whose cross-sectional area increases as the distance from the sapphire substrate increases.
  • the opening of the through hole on the bottom side of the growth mask layer is circular,
  • the plurality of through holes are arranged so that the other six are adjacent to each other, and two adjacent ones are arbitrarily selected from the plurality of through holes, one of which is a first through hole and the other is
  • the first through hole and the second through hole are close to each other so that the side wall of the first through hole and the side wall of the second through hole are in contact with each other.
  • LED device [22]
  • the GaN-based LED device according to [21] wherein the inclination angle of the side wall is 50 to 75 degrees at a position where the distance from the single crystal substrate is half the thickness of the growth mask layer.
  • a method for manufacturing a GaN-based LED device comprising a laminate forming step of forming a GaN-based semiconductor laminate including a layer.
  • the openings of the through holes on the bottom side and the top side of the growth mask layer are circular,
  • An epitaxial growth substrate for a GaN-based LED device wherein the plurality of through holes are arranged in a close-packed manner with a pitch of 1.25 times or less the diameter of the opening on the upper surface side of the growth mask layer.
  • the substrate for epitaxial growth according to [24] wherein the single crystal substrate is a sapphire substrate, a SiC substrate, a GaN substrate, an AlN substrate, a spinel substrate, a gallium oxide substrate, or a zinc oxide substrate.
  • the inclination angle of the side wall is 30 to 75 degrees when the distance from the single crystal substrate is half the thickness of the growth mask layer.
  • the substrate for epitaxial growth described in 1.
  • the substrate for epitaxial growth described in 1. [29] The epitaxial growth substrate according to any one of [24] to [28], wherein the growth mask layer includes a dielectric having a lower refractive index than the single crystal substrate.
  • a method for manufacturing a GaN-based LED device comprising a laminate forming step of forming a GaN-based semiconductor laminate including a layer.
  • a non-flat interface useful for improving the light extraction efficiency is provided between the GaN-based semiconductor and the epitaxial growth substrate, and the light emission efficiency is excellent.
  • the GaN-based LED device can be easily and efficiently manufactured.
  • FIG. 1A and 1B show an epitaxial growth substrate according to the embodiment.
  • FIG. 1A is a plan view
  • FIG. 1B is a line X 1 -X 1 in FIG. It is sectional drawing in the position.
  • FIG. 2 is a cross-sectional view of the epitaxial growth substrate shown in FIG. 1 taken along the line X 2 -X 2 in FIG. 3A and 3B are cross-sectional views of an epitaxial growth substrate in which the inclination angle of the side wall of the through hole is not constant.
  • FIG. 3A shows an example in which the inclination angle of the side wall of the through hole H decreases with the distance from the single crystal substrate 11.
  • FIG. 3B shows an example in which the inclination angle of the side wall of the through hole H increases with the distance from the single crystal substrate 11.
  • 4 (a) and 4 (b) show an epitaxial growth substrate having the same through hole arrangement as the epitaxial growth substrate shown in FIG. 1, FIG. 4 (a) is a plan view, and FIG. 4 (b) is FIG. It is sectional drawing in the position of the XX line of (a).
  • FIGS. 5A to 5E are cross-sectional views for explaining a manufacturing process of the epitaxial growth substrate shown in FIG.
  • FIGS. 6A and 6B show an epitaxial growth substrate according to the embodiment.
  • FIG. 6A is a plan view
  • FIG. 6B is a perspective view.
  • FIG. 6A is a plan view
  • FIG. 6B is a perspective view.
  • FIG. 7 is a plan view of the epitaxial growth substrate according to the embodiment.
  • FIG. 8 is a plan view of the epitaxial growth substrate according to the embodiment.
  • FIG. 9 is a plan view of the epitaxial growth substrate according to the embodiment.
  • FIG. 10 is a plan view of the epitaxial growth substrate according to the embodiment.
  • FIGS. 11A to 11C are cross-sectional views showing the state of epitaxial growth of a GaN crystal on the epitaxial growth substrate according to the embodiment.
  • FIG. 12 is a cross-sectional view of a GaN-based LED device according to the embodiment.
  • FIGS. 13A to 13E are plan views of the epitaxial growth substrate assumed in simulation 1.
  • FIG. FIG. 14 shows the result of the simulation 1.
  • FIG. 15A to 15E are perspective views of the epitaxial growth substrate assumed in simulation 2.
  • FIG. FIG. 16 shows the result of the simulation 2.
  • FIGS. 17A to 17E are perspective views of the epitaxial growth substrate assumed in simulation 3.
  • FIG. 18 shows the result of the simulation 3.
  • FIG. 19 shows the result of the simulation 4.
  • 20A and 20B are perspective views of the epitaxial growth substrate assumed in simulation 5,
  • FIG. 20A shows the case where the growth mask layer exhibits a stripe pattern
  • FIG. 20B shows the growth mask. Each case shows a layer exhibiting a dot pattern.
  • FIG. 21 shows the result of the simulation 5.
  • FIG. 22 is a plan view of the epitaxial growth substrate according to the embodiment.
  • FIGS. 1 and 2 show the structure of an epitaxial growth substrate according to an embodiment of the present invention.
  • 1A is a plan view
  • FIG. 1B is a cross-sectional view taken along line X 1 -X 1 in FIG. 1A
  • FIG. 2 is a position taken along line X 2 -X 2 in FIG. FIG.
  • the epitaxial growth substrate 10 includes a single crystal substrate 11 and a growth mask layer 12 formed on one main surface thereof.
  • a plurality of through holes H are formed in the growth mask layer 12 so as to penetrate the growth mask layer 12 in the thickness direction, and the surface of the single crystal substrate 11 is exposed at the positions of the through holes H.
  • the single crystal substrate 11 a substrate usually used for epitaxial growth of a GaN-based semiconductor can be used.
  • the single crystal substrate 11 is preferably a sapphire substrate (c-plane, a-plane, r-plane), SiC substrate (4H, 6H), GaN substrate (c-plane, m-plane, s-plane), AlN substrate, spinel substrate, oxidation A substrate that hardly absorbs light in the visible wavelength range (380 to 780 nm) and has a refractive index equal to or lower than that of a GaN-based semiconductor, such as a gallium substrate and a zinc oxide substrate.
  • the single crystal substrate 11 is particularly preferably a c-plane sapphire substrate, a SiC substrate (4H, 6H), or a c-plane GaN substrate because a highly efficient GaN-based LED structure can be manufactured by c-axis growth.
  • the single crystal substrate 11 may be a substrate provided with an off angle.
  • the growth mask layer 12 is formed using, for example, silicon oxide, silicon oxynitride, silicon nitride, tantalum oxide, zirconium oxide, or the like. By forming the growth mask layer 12 using these dielectrics, a GaN-based semiconductor crystal is grown on the surface of the growth mask layer 12 when epitaxially growing a GaN-based semiconductor from the surface of the single crystal substrate 11 exposed through the through hole H. Is prevented from growing.
  • the material of the growth mask layer 12 is not limited to those exemplified above, and can be selected from various materials used for growth masks in GaN-based semiconductor ELO (Epitaxial Lateral Overgrowth).
  • ELO Epi Lateral Overgrowth
  • the growth mask layer 12 formed using silicon oxide, silicon oxynitride, silicon nitride, tantalum oxide, zirconium oxide or the like is formed of GaN, InGaN, Al x Ga 1-x N (0 ⁇ x ⁇ 0.2) or the like. It has a refractive index lower than that of a GaN-based semiconductor usually used in the main part of the LED system. Therefore, in the GaN-based LED device using the epitaxial growth substrate 10, the interface formed between the growth mask layer 12 and the GaN-based semiconductor has a property of reflecting light and a property of refracting light. Among the exemplified dielectrics, when the growth mask layer 12 is formed of silicon oxide having the lowest refractive index, the interface has the strongest effect of reflecting light and refracting light.
  • the thickness of the growth mask layer 12 is preferably 0.5 ⁇ m or more, more preferably 1 ⁇ m or more so that the area of the side wall of the through hole H is sufficiently large.
  • the thickness of the growth mask layer 12 is preferably 3 ⁇ m or less. If it is thicker than this, it takes a long time to grow a GaN-based semiconductor in order to embed the growth mask layer 12 during manufacture of the LED device, which may reduce the manufacturing efficiency of the LED device.
  • the thickness of the growth mask layer 12 may be 2 ⁇ m or less, and approximately 1.5 ⁇ m (1.25 to 1.75 ⁇ m) is appropriate.
  • the through-hole H provided in the growth mask layer 12 increases as the cross-sectional area increases from the single crystal substrate 11.
  • the cross-sectional area referred to here is an area of a cross section formed by cutting the through hole H along a plane parallel to the main surface of the single crystal substrate 11. Since the cross-sectional area of the through hole H changes in this way, as shown in FIGS. 1B and 2, the side wall of the through hole H has an inclined surface with an inclination angle ⁇ of less than 90 degrees.
  • the inclination angle ⁇ can be 15 to 80 degrees, preferably 30 to 75 degrees, and more preferably 50 to 75 degrees.
  • the inclination angle here is an inclination angle when the main surface of the single crystal substrate 11 is a reference plane (the same applies hereinafter).
  • the side wall does not need to have a constant inclination angle from the lower end (end on the single crystal substrate side) to the upper end (end on the side away from the single crystal substrate).
  • the inclination angle of the side wall of the through hole H may decrease as the distance from the single crystal substrate 11 increases.
  • the inclination angle of the side wall of the through hole H may increase as the distance from the single crystal substrate 11 increases.
  • the central portion inclination angle ⁇ 1/2 which is the inclination angle of the side wall of the through hole, at a position half the thickness t of the growth mask layer from the single crystal substrate 11 is set to 30 to 75 degrees, particularly 50 °. It is preferable that the angle be ⁇ 75 degrees.
  • a plurality of through holes H are arranged so that every other one is adjacent to the other six. Furthermore, when two adjacent ones of the plurality of through holes are arbitrarily selected, the two are close enough that one side wall and the other side wall touch each other. In other words, the plurality of through holes H are densely arranged so that a boundary where the side walls intersect between any two adjacent ones is formed. This will be described with reference to FIG. 4. As shown in FIG. 4A, six other through holes H 1 to H 6 are adjacent to the arbitrarily selected through hole H 0 .
  • the cross section of the growth mask layer 12 at the position of the XX line is horizontal at the top as shown in FIG. It has a shape with no part (in this example, a triangle).
  • a part of the side wall of the through hole H 0 is in contact with the side wall of the through hole H 2 , and the other part is in contact with the side wall of the through hole H 5 .
  • the upper end of the side wall of the through hole H 0 is partially in contact with the side wall of the through hole H 3 , and the other part is in contact with the side wall of the through hole H 6. Yes.
  • the GaN-based LED device structure is formed on the epitaxial growth substrate by providing the through-holes so densely that the side walls of the adjacent through-holes touch each other, the interface between the growth mask layer and the GaN-based semiconductor is occupied.
  • the ratio of the inclined portion can be increased.
  • 3 (a) and 3 (b) described above also show a cross section at a position where the side walls of two adjacent through holes are in contact with each other.
  • the cross section has a shape that does not have a horizontal portion at the top.
  • the size of the opening of the through hole H on the bottom surface (surface in contact with the single crystal substrate 11) side of the growth mask layer 12 should be such that the GaN-based semiconductor can be epitaxially grown from the surface of the single crystal substrate 11 exposed in the opening. That's fine.
  • Area of the opening is, for example, be a 0.5 ⁇ m 2 ⁇ 30 ⁇ m 2. The smaller the area, the higher the proportion of the inclined portion in the interface between the epitaxial growth substrate and the GaN semiconductor when the GaN-based LED device structure is formed on the epitaxial growth substrate 10, and the higher the light extraction efficiency. Become.
  • a single crystal substrate 11, for example, a normal c-plane sapphire substrate is prepared as a starting material.
  • a growth mask layer 12 is formed so as to uniformly cover the main surface of the single crystal substrate 11.
  • the method for forming the growth mask layer it may be appropriately selected from known thin film forming methods depending on the material forming the layer.
  • a plasma CVD method, a vacuum evaporation method, or a sputtering method can be preferably used.
  • a photoresist film P is formed on the surface thereof as shown in FIG.
  • the photoresist film P is patterned using a normal technique to form an opening h as shown in FIG.
  • the pattern of the opening h formed in the photoresist film P is the same as the pattern of the opening on the single crystal substrate 11 side of the through hole to be provided in the growth mask layer 12 in the target epitaxial growth substrate 10.
  • through holes H are formed in the growth mask layer 12 by dry etching methods such as reactive ion etching and plasma etching using the photoresist film P as an etching mask.
  • the etching rate of the growth mask layer is such that the photoresist film P disappears from the peripheral portion and the area is reduced. And the ratio of the etching rate of the photoresist film.
  • the side wall of the hole formed in the growth mask layer 12 can be inclined.
  • the photoresist film P is hard baked after patterning, its end face becomes tapered, that is, the film thickness in the peripheral portion is reduced, and therefore the disappearance of the peripheral portion of the photoresist film P in the etching process can be promoted.
  • the etching process may be continued until the photoresist film completely disappears.
  • the growth mask layer 22 is epitaxially grown without a horizontal plane on the upper surface side (the side opposite to the bottom surface side).
  • the substrate 20 for use is obtained.
  • the shape and arrangement of the through holes provided in the growth mask layer can be changed variously by changing the pattern of the openings formed in the photoresist film.
  • a plurality of through holes H provided in the growth mask layer 32 formed on the single crystal substrate 31 are arranged so that every other one is adjacent to the other three. Has been. When any two adjacent through holes are seen, one side wall and the other side wall of the two through holes are in contact with each other.
  • two types of through holes H A and H B growth mask layer 32' epitaxial growth substrate 30 showing a plan view shown in FIG. 22 can also be provided.
  • the arrangement of the through-holes HA is the same as the arrangement of the through-holes H shown in FIG.
  • the other type of through hole H B is disposed in a region not occupied by the through hole HA . A side wall and the side wall of the through hole H A of the through hole H B does not abut.
  • two kinds of the through-hole H A and H B the distance between both ends is the same (equal to the thickness of the growth mask layer 32 '), the bottom surface of the opening size growth mask layer It differs on the side and on the top side.
  • Such an epitaxial growth substrate having a plurality of types of through-holes with different side wall inclinations in the growth mask layer can be manufactured by a method of forming the through-holes in different processes for each type.
  • the side wall of the one type of through hole H A and the side wall of the other type of through hole H B may be in contact with each other.
  • each of the plurality of through holes H provided in the growth mask layer 42 formed on the single crystal substrate 41 has an equilateral triangular cross section (the main surface of the single crystal substrate 41). And a cross section formed by cutting along a plane parallel to the surface.
  • the growth mask layer 42 does not have a horizontal plane on the upper surface side. Twelve other through holes are adjacent to any through hole H provided in the growth mask layer 42. Of the twelve, three are arranged on the upper surface side of the growth mask layer 42 so that the opening and the opening of the through hole are in contact with each other by a line. The remaining nine are arranged on the upper surface side of the growth mask layer 42 so that the opening and the opening of the through hole are in contact with each other at a point.
  • each of the plurality of through holes H provided in the growth mask layer 52 formed on the single crystal substrate 51 has a rhombic cross section (on the main surface of the single crystal substrate 51). And a cross section obtained by cutting along a parallel plane.
  • the growth mask layer 52 does not have a horizontal plane on the upper surface side.
  • Eight other through holes are adjacent to any through hole H provided in the growth mask layer 52.
  • Four of the eight are arranged on the upper surface side of the growth mask layer 52 so that the opening and the opening of the through hole are in contact with each other by a line.
  • the remaining four are arranged on the upper surface side of the growth mask layer 52 so that the opening and the opening of the through hole are in contact with each other at a point.
  • each of the plurality of through holes H provided in the growth mask layer 62 formed on the single crystal substrate 61 has a regular hexagonal cross section (the main surface of the single crystal substrate 61). And a cross section formed by cutting along a plane parallel to the surface.
  • the growth mask layer 62 does not have a horizontal plane on the upper surface side.
  • Six other through holes are adjacent to any through hole H provided in the growth mask layer 62. All six of them are arranged so that the side wall forms a linear boundary with the side wall of the through hole.
  • Epitaxial growth of GaN-based semiconductor The method for epitaxially growing a GaN-based semiconductor on the epitaxial growth substrate of each of the above-described embodiments is not particularly limited. These methods can be used as appropriate. The most preferred method is the MOVPE method.
  • the single crystal substrate included in the epitaxial growth substrate is a substrate having a lattice constant difference with a GaN-based semiconductor such as a sapphire substrate
  • a known buffer layer technique can be preferably used.
  • a low-temperature buffer that forms a buffer layer made of a GaN-based semiconductor such as GaN, AlGaN, or AlN at a temperature lower than the temperature for growing a single crystal, for example, 400 to 600 ° C. Layer technology is useful.
  • FIG. 11A shows the above-described epitaxial growth substrate 10.
  • the single crystal substrate 11 exposed at the position of the through hole H provided in the growth mask layer 12 as shown in FIG.
  • the growth of the GaN crystal S1 is started from the surface.
  • the GaN crystal S1 grows in the thickness direction and grows laterally on the inclined sidewall of the through hole H. This is because the growth of the GaN crystal starting from the surface of the growth mask layer 12 hardly occurs.
  • the GaN crystal S1 grown from each through hole H becomes coreless when the film thickness exceeds the film thickness of the growth mask layer 12, and as shown in FIG. 11C, a layered body in which the growth mask layer 12 is embedded and integrated. To present. Since the crystal orientations of the GaN crystals S1 grown from the plurality of through holes H are aligned, coreless defects are unlikely to occur. Since the surface of the single crystal substrate 11 is subjected to batch finishing such as polishing before the growth mask layer 12 is formed, the quality of the exposed surface of the single crystal substrate 11 that becomes the crystal growth start surface is improved. This is because there is little variation. Here, when compared with PSS, coreless defects are likely to occur in the process of epitaxially growing a GaN-based semiconductor on PSS.
  • the entire non-flat surface used for epitaxial growth is a sapphire surface that can serve as a place to start the growth of a GaN-based semiconductor crystal, and the GaN-based semiconductor crystal can grow in different modes for each part on the non-flat surface ( This is because, for example, crystals can grow in different modes from the top surface and the side wall surface of the protrusion.
  • the epitaxial growth substrate according to each of the above-described embodiments even if the in-plane uniformity of the pattern of the growth mask layer is reduced, the surface of the single crystal substrate that is the growth start surface of the GaN-based semiconductor crystal Therefore, the in-plane uniformity of the quality of the GaN-based semiconductor crystal is not deteriorated.
  • FIG. 12 is a sectional view of a GaN-based LED device according to the embodiment.
  • the GaN-based LED device 100 includes a GaN-based semiconductor stacked body S2 formed by epitaxial growth on the epitaxial growth substrate 10 (consisting of the single crystal substrate 11 and the growth mask layer 12) according to the above-described embodiment. Yes.
  • the GaN-based semiconductor stacked body S2 includes an undoped layer S21, an n-type layer S22, a light emitting layer S23, and a p-type layer S24 in this order from the epitaxial growth substrate 10 side.
  • a negative electrode E1 is formed on the partially exposed surface of the n-type layer S22.
  • a translucent electrode E2 is formed on the upper surface of the p-type layer S24, and a positive electrode E3 is formed on a part thereof.
  • the undoped layer S21 is a layer made of, for example, GaN that is not doped with impurities.
  • the undoped layer S21 is epitaxially grown from the surface of the single crystal substrate 11 exposed through the through hole H formed in the growth mask layer 12, and covers the growth mask layer 12 in layers. ing.
  • the n-type layer S22 can be formed directly on the epitaxial growth substrate 10 without forming the undoped layer S21.
  • the n-type layer S22 is made of GaN doped with Si at a concentration of 1 ⁇ 10 18 cm ⁇ 3 to 1 ⁇ 10 19 cm ⁇ 3 , for example, and has a thickness of 2 to 6 ⁇ m.
  • the light emitting layer S23 preferably includes a quantum well layer made of undoped InGaN.
  • the light emitting layer S23 has an MQW structure in which such quantum well layers and barrier layers made of GaN or InGaN are alternately stacked.
  • the barrier layer is doped with Si.
  • the p-type layer S24 is made of, for example, GaN doped with Mg at a concentration of 5 ⁇ 10 19 cm ⁇ 3 to 1 ⁇ 10 21 cm ⁇ 3 , and has a thickness of 50 to 500 nm.
  • a contact layer can be provided as a layer for forming the negative electrode E1, a hole blocking layer made of n-type AlGaN, and an n-type strain relaxation made of InGaN or GaN / InGaN superlattice. Layers and the like can be provided. Inside the p-type layer S24, an electron block layer made of p-type AlGaN or the like can be provided under the contact layer provided as the uppermost layer.
  • the negative electrode E1 serves both as an ohmic electrode and an electrode pad, has an ohmic contact layer in a portion in contact with the n-type GaN layer S22, and a surface layer is an Au layer.
  • the ohmic contact layer can be formed of Al, Ti, Cr alone or an alloy, or can be formed of TCO (transparent conductive oxide).
  • the translucent electrode E2 is made of TCO.
  • an indium oxide-based TCO such as ITO and a zinc oxide-based TCO such as IZO can be preferably used.
  • the positive electrode E3 has a layer made of a metal having good adhesion to the TCO, for example, a layer made of Cr, Ni, Ti, Pt, Rh, etc., at the portion in contact with the translucent electrode E2, and the outermost layer is Au layer.
  • the inside of the GaN-based semiconductor laminate S2 is assumed to be optically uniform, and its refractive index is 2.43, which is the refractive index of GaN. Further, the GaN-based semiconductor laminate has an extinction coefficient of 10 ⁇ 7 .
  • the refractive index was set to 2.0 and the extinction coefficient was set to 0.02.
  • Both the negative electrode E1 and the positive electrode E3 had a diameter of 100 ⁇ m, a refractive index of 1.5, and an extinction coefficient of 1.88.
  • the refractive index and extinction coefficient refer to the value of Au.
  • the surface of the model LED device was a flat optical surface.
  • the simulation was performed by the ray tracing method using LightTools (registered trademark), which is illumination design analysis software of ORA (currently Synopsis).
  • the light extraction efficiency was defined as the ratio of the amount of light emitted from any surface of the model LED device to the outside of the device relative to the amount of light emitted from the light emitting layer S23.
  • the refractive index outside the device was 1.
  • FIG. 13 is a plan view of the epitaxial growth substrate assumed in this simulation.
  • FIGS. 13A to 13E show the pitch of the arrangement pattern of the through holes of 1.5 ⁇ m, 1.7 ⁇ m, and 2. The cases of 0 ⁇ m, 2.5 ⁇ m, and 4.0 ⁇ m are shown.
  • the growth mask layer has a circular mesh pattern, and has a plurality of through-holes having a circular opening on the bottom surface side and a constant inclination angle of the side wall.
  • each through hole In each through hole, the diameter of the opening on the bottom side of the growth mask layer was 1.1 ⁇ m, and the inclination angle of the side wall was 45 degrees.
  • the plurality of through holes are arranged closest to each other, and six other through holes are adjacent to each through hole. In other words, each through hole occupies the lattice position of the triangular lattice.
  • the thickness of the growth mask layer when the pitch of the arrangement pattern (period of the triangular lattice) was 1.7 ⁇ m or more was set to 0.45 ⁇ m. Therefore, when the pitch is larger than 2.0 ⁇ m, the side walls of the adjacent through holes do not touch each other. On the other hand, when the pitch is 1.7 ⁇ m or less, the growth mask layer does not have a horizontal surface on the upper surface side.
  • the refractive index of the growth mask layer was 1.45 (the refractive index of SiO 2 ).
  • the result of simulation 1 is shown in FIG.
  • the light extraction efficiency of the model LED device was the best when the pitch of the through hole arrangement pattern was 1.5 to 2.0 ⁇ m, that is, when the side walls of adjacent through holes touched each other. It was.
  • the light extraction efficiency when the pitch is 1.5 ⁇ m is lower than that when the pitch is 1.7 ⁇ m because the pitch is 1.5 ⁇ m than when the pitch is 1.7 ⁇ m. This is also because the thickness of the growth mask layer is small.
  • the diameter of the opening of the through hole on the upper surface side of the growth mask layer is 1.25 times.
  • the through holes are arranged in a close-packed manner with a pitch of preferably 1.1 times or less, more preferably 1.05 times or less.
  • FIG. 15 is a perspective view of the substrate for epitaxial growth assumed in this simulation.
  • FIGS. 15A to 15E show that the inclination angle of the side wall of the through hole is 15 degrees, 30 degrees, 45 degrees, 60 degrees, respectively. The case of 75 degrees is shown.
  • the growth mask layer has a circular mesh pattern, and has a plurality of through-holes having a circular opening on the bottom surface side and a constant inclination angle of the side wall. In any through hole, the diameter of the opening on the bottom surface side was 1.1 ⁇ m.
  • the plurality of through holes are arranged closest to each other, and six other through holes are adjacent to each through hole.
  • the pitch of the arrangement pattern of the through holes was 1.7 ⁇ m regardless of the inclination angle of the side wall. Therefore, even if the inclination angle of the side wall is different, the total area of the surface of the single crystal substrate exposed through the through hole of the growth mask layer is constant.
  • the thickness of the growth mask layer was set so that the growth mask layer did not have a horizontal plane on the upper surface side. Therefore, the greater the inclination angle of the side wall of the through hole, the greater the thickness of the growth mask layer.
  • the refractive index of the growth mask layer was 1.45 (the refractive index of SiO 2 ).
  • Results of simulation 2 are shown in FIG.
  • the light extraction efficiency of the model LED device was highest when the inclination angle of the side wall of the through hole was 60 to 75 degrees, and the value reached 59%.
  • the tilt angle is less than 60 degrees, the light extraction efficiency decreases as the tilt angle decreases, and the light extraction efficiency when the tilt angle is 15 degrees is 48%.
  • this tendency may be related not only to the inclination angle of the side wall of the through hole but also to the thickness of the growth mask layer. This is because the thickness of the growth mask layer when the inclination angle is 60 degrees and 75 degrees is about 6.5 times and about 14 times that when the inclination angle is 15 degrees, respectively.
  • FIG. 17 is a perspective view of the epitaxial growth substrate assumed in this simulation 3.
  • FIGS. 17A to 17E show the inclination angles of the side walls of the through holes of 15 degrees, 30 degrees, 45 degrees, and 60 degrees, respectively. , 75 degrees are shown.
  • the growth mask layer has a circular mesh pattern, and has a plurality of through-holes having a circular opening on the bottom surface side and a constant inclination angle of the side wall. In any case, the thickness of the growth mask layer was 0.45 ⁇ m, and the diameter of the opening on the bottom side of each through hole was 1.1 ⁇ m.
  • the plurality of through holes are arranged in a close-packed manner, and the pitch of the arrangement pattern is set so that the openings of adjacent through holes are in contact with each other on the upper surface side of the growth mask layer. Therefore, the gentler the inclination angle of the side wall of the through hole, the larger the pitch of the arrangement pattern, and the smaller the total area of the surface of the single crystal substrate exposed through the through hole.
  • the refractive index of the growth mask layer was 1.45 (the refractive index of SiO 2 ).
  • the result of the simulation 3 is shown in FIG.
  • the light extraction efficiency of the model LED device was good when the inclination angle of the side wall of the through hole was 30 to 75 degrees, particularly when it was larger than 45 degrees.
  • the light extraction efficiency when the tilt angle was 60 degrees reached 58%.
  • the tilt angle was less than 60 degrees, the light extraction efficiency tended to decrease as the tilt angle decreased.
  • the tilt angle was 15 degrees, the light extraction efficiency decreased to 46%.
  • the simulation value of the light extraction efficiency when the growth mask layer is not provided is about 25%, the light extraction by the growth mask layer is possible even when the inclination angle of the side wall of the through hole is 15 degrees. It can be said that the efficiency improvement effect is not small.
  • the light extraction efficiency was clearly higher when the inclination of the side wall of the cone was 45 degrees than when the inclination of the cone side wall was 64 degrees, whereas the latter In the LED device including the PSS having the pattern, the light extraction efficiency is slightly higher when the inclination of the side wall of the depression is 64 degrees than when it is 45 degrees.
  • the refractive index of the growth mask layer is 2.3, which is close to the refractive index of GaN, the light extraction efficiency is reduced to 45%.
  • the simulation value of the light extraction efficiency when the growth mask layer is not provided is still about 25%. Therefore, the effect of improving the light extraction efficiency by the growth mask layer is not small.
  • the growth mask layer pattern was a circular mesh pattern, a stripe pattern, and a dot pattern.
  • a pattern FIG. 13B
  • simulation 1 a pattern (FIG. 13B) when the pitch was 1.7 ⁇ m in simulation 1 was used. In this case, 38% of the area of the surface of the single crystal substrate is exposed through the through hole provided in the growth mask layer.
  • each of the linear growth mask layers has a bottom surface (a surface in contact with the single crystal substrate) and two inclined wall surfaces.
  • the cross section (cross section orthogonal to the longitudinal direction) is an isosceles triangle.
  • the width of the bottom surface of the growth mask layer in the direction perpendicular to the stripe direction was 2 ⁇ m
  • the inclination angle of the two wall surfaces was 45 degrees
  • the stripe pitch was 3.23 ⁇ m. In this case, 38% of the area of the surface of the single crystal substrate is exposed without being covered with the growth mask layer.
  • each of the dot-shaped growth mask layers has a cone shape as shown in FIG.
  • Each cone had a bottom diameter of 2 ⁇ m, a height of 1 ⁇ m, and a sidewall inclination angle of 45 degrees.
  • the cones were arranged in a close-packed manner, and the pitch of the arrangement pattern was 4 ⁇ m, which is twice the diameter of the bottom surface of the cone. In this case, 78% of the area of the surface of the single crystal substrate is exposed without being covered with the growth mask layer.
  • the result of simulation 5 is shown in FIG. Although the refractive index of the growth mask layer was changed in five ways between 1.45 and 2.30, in any case, the light extraction efficiency of the model LED device is the highest when the growth mask layer has a circular mesh pattern. It became high and became the lowest in the stripe pattern.
  • the GaN-based LED device obtained by epitaxially growing a GaN-based semiconductor on the epitaxial growth substrate according to the present invention has excellent luminous efficiency
  • the light source for a backlight unit of a liquid crystal display or for white illumination It can be preferably used for various light sources such as a light source.

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Abstract

Le principal objet de la présente invention est de produire un substrat de croissance épitaxique innovant à utiliser dans un dispositif à DEL au GaN, le substrat ayant un effet d'amélioration sur le rendement d'extraction de lumière par rapport à celui d'un PSS. Un mode de réalisation de la présente invention comprend un substrat de croissance épitaxique à utiliser dans un dispositif à DEL au GaN. Dans un exemple, le substrat de croissance épitaxique a une couche de masque de croissance qui comprend un substrat monocristallin et une substance diélectrique dont l'indice de réfraction est inférieur à celui du GaN; la couche de masque de croissance a un trou traversant qui traverse la couche de masque de croissance dans la direction de l'épaisseur et dont l'aire de section transversale augmente en s'éloignant du substrat monocristallin; et une pluralité de trous traversants sont agencés de manière à ce que l'un quelconque des trous traversants est adjacent à au moins trois autres. Quand deux trous adjacents sont arbitrairement sélectionnés parmi la pluralité de trous traversants ainsi agencés, et qu'un est défini comme premier trou traversant et que l'autre est défini comme second trou traversant, la paroi latérale du premier trou traversant et la paroi latérale du second trou traversant sont en butée.
PCT/JP2011/079880 2011-01-07 2011-12-22 SUBSTRAT DE CROISSANCE ÉPITAXIQUE ET DISPOSITIF À DEL AU GaN Ceased WO2012093601A1 (fr)

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JP2023092803A (ja) * 2021-12-22 2023-07-04 大日本印刷株式会社 結晶成長用基板、窒化ガリウム基板、半導体基板、および窒化ガリウム基板の製造方法
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