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CN203174223U - Composite baseplate and functional elements - Google Patents

Composite baseplate and functional elements Download PDF

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Publication number
CN203174223U
CN203174223U CN 201320072801 CN201320072801U CN203174223U CN 203174223 U CN203174223 U CN 203174223U CN 201320072801 CN201320072801 CN 201320072801 CN 201320072801 U CN201320072801 U CN 201320072801U CN 203174223 U CN203174223 U CN 203174223U
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China
Prior art keywords
inclusion
gallium nitride
layer
nitride film
base plate
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Chinese (zh)
Inventor
岩井真
今井克宏
坂井正宏
平尾崇行
吉野隆史
下平孝直
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NGK Insulators Ltd
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NGK Insulators Ltd
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Abstract

A composite baseplate (7) is provided with a seed crystal baseplate (1) and a gallium nitride film (3), wherein the seed crystal baseplate (1) is made of gallium nitride with a yellow glowing effect which can be observed through a fluorescence microscope; the gallium nitride film (3) is bred by a melted liquid under a nitrogenous atmosphere on the seed crystal baseplate (1) through the flux growth method, and the yellow glowing effect is not observed; the composite baseplate (7) comprises an occluded foreign substance distribution layer (3a) and an occluded foreign substance lacking layer (3b); the occluded foreign substance distribution layer (3a) is arranged on an area 50 micrometers lower than the boundary on the seed crystal baseplate (1) side on which the gallium nitride film (3) is arranged; the area is distributed with occluded foreign substances originating from components of the melted liquid; and the occluded foreign substance lacking layer (3b) is arranged on the occluded foreign substance distribution layer (3a) and lacks occluded foreign substances.

Description

Composite base plate and functional element
Technical field
The present invention relates to by the film formed composite base plate of gan and use the functional element of this composite base plate.Such composite base plate can be used for power parts that headlight that composite base plate is used for the White LED of high colour rendering and automobile uses with the umformer of ultra-high brightness LED laser diode, Hybrid Vehicle with the indicating meter of led light source, pure green etc. etc.
Background technology
In recent years, people use 13 family's element nitrides of gan etc. to make the semiconductor devices of blue leds and White LED, bluish voilet semiconductor laser etc. in active research, and its semiconductor devices is applied to various electronic machines.Gallium nitride based semiconductor devices is in the past mainly made by vapor phase process.Specifically, by organo-metallic vapour deposition process (MOVPE) etc. the thin film heterogeneity epitaxial growth of gan is made at sapphire substrate and silicon carbide substrate.At this moment, because thermal expansivity and lattice parameter between substrate and the gallium nitride film differ greatly, therefore can produce highdensity dislocation (lattice imperfection is a kind of in the crystallization) at gan.Therefore, be difficult to obtain the low high-quality gan of dislocation desity with vapor phase process.
Flux method is a kind of of liquid phase method, and under the situation of gan, by sodium Metal 99.5 is used as fusing assistant, the necessary temperature of the crystalline growth of gan can be relaxed be about 800 ℃, and pressure relaxes and is number MPa.Particularly, in the mixed molten liquid of sodium Metal 99.5 and gallium, dissolve nitrogen, make gan become hypersaturated state and be grown to crystallization.In this kind liquid phase method, compare to vapor phase process and be difficult to take place dislocation, therefore can obtain the low high-quality gan of dislocation desity.
Research and development about this kind flux method are very in vogue.For example, the Japanese Patent spy opens among the 2005-263622, since in the flux method in the past the crystal growth rate of the thickness direction (C direction of principal axis) of gan be about 10 μ m/h low speed, at liquid-gas interface uneven equal nucleus to take place easily generate, thereby proposed to overcome the making method of the gan of these problems.
The applicant opens among the 2010-168236 in the Japanese Patent spy and files an application with regard to the relevant of stirring intensity and inclusion generation.Disclose in this patent, in order to make the crystalline growth of no inclusion, made the speed of growth in suitable scope, adjusted speed of rotation and the turn around condition of crucible.
In addition, in the special table of Japanese Patent 2005-506271 the situation that forms the specific gallium nitride crystal of jaundice coloured light at crystal seed is disclosed.
Summary of the invention
The inventor is formed in the nitride single-crystal on the crystal seed with flux method putting down in writing in order to open 2010-168236 as the Japanese Patent spy, continues research by eliminating the quality that inclusion further promotes nitride single-crystal.Based on the quality perspective of nitride single-crystal, further reducing defect concentration is extremely important from aspects such as lifting luminous efficiencies.
Especially, breeding the composite base plate of the gallium nitride crystal of non-yellowing coloured light at the gan crystal seed of jaundice coloured light, tell both differences easily, is desirable substrate in the manufacturing of functional element.Aspect such composite base plate, thereby strong expectation provides high-quality functional element by further reduction defect concentration.
Problem of the present invention provides a kind of composite base plate, and this composite base plate is the composite base plate of breeding the gallium nitride film of non-yellowing coloured light at the gan crystal seed substrate of jaundice coloured light, and its surface defect density is further reduced.
Composite base plate of the present invention, it is characterized in that, it is a kind of composite base plate with crystal seed substrate and gallium nitride film, described crystal seed substrate is made of the gan of seeing Yellow luminous effect by fluorescence microscope, described gallium nitride film is bred by liquation under nitrogen containing atmosphere by flux method on described crystal seed substrate, do not see described Yellow luminous effect, the inclusion that described composite base plate comprises the inclusion distribution layer of the inclusion that is distributed with the composition that is derived from described liquation that is arranged at the zone below the interface 50 μ m of the described crystal seed substrate-side of described gallium nitride film and is arranged at the described inclusion of shortage on this inclusion distribution layer lacks layer.
In addition, the present invention relates to a kind of functional element, it is characterized in that, the functional layer that is constituted by 13 family's element nitride films that this functional element possesses described composite base plate and forms by vapor phase process on described gallium nitride film.
The inventor finds in the process with the gallium nitride crystal film forming on the crystal seed substrate of jaundice coloured light in research, not only to reduce inclusion, but the near interface of the crystal seed side by making it moderately to residue in gallium nitride crystal, even compare with the gallium nitride crystal that does not almost have inclusion, also can further reduce the defect concentration of crystallization, thereby finish the present invention.
That is, the crystallization that has the inclusion of several microns sizes by order is only grown in 50 microns zone of the early growth period of the gallium nitride single crystal that utilizes flux method, and the dislocation of crystallization significantly descends, and brings the superperformance as various device.This finds and engages in that to utilize flux method to carry out the those skilled in the art's that breed the general knowledge of gallium nitride crystal opposite.
Description of drawings
Fig. 1 (a) shows sectional view for the pattern of the gan crystal seed substrate 1 of jaundice coloured light, (b) for formed the pattern demonstration sectional view of the state of gallium nitride crystal 3 on the crystal seed substrate 1 by flux method.
Fig. 2 (a), Fig. 2 (b) are respectively the pattern demonstration figure of near zone of the crystal seed substrate 1 of gallium nitride film 3.
Fig. 3 (a) is for grinding composite base plate 7 in the pattern demonstration figure of the intact composite base plate 7A of grinding that obtains, Fig. 3 (b) is the pattern demonstration figure of the functional element 9 that forms functional layer 8 at composite base plate 7A and obtain, and Fig. 3 (c) is the pattern demonstration figure of the functional element 9A that forms functional layer 8A at composite base plate 7A and obtain.
Fig. 4 is the mode chart that shows the device of the manufacturing that can be used in nitride single-crystal of the present invention.
Fig. 5 is the figure that shows the container of the manufacturing that can be used in nitride single-crystal of the present invention.
Embodiment
(purposes)
Composite base plate of the present invention and functional element, the headlight that can be used for requiring high-quality technical field, for example is called as the White LED of high colour rendering of back luminescent lamp and automobile with the indicating meter of led light source, pure green etc. with the employed power parts of umformer of ultra-high brightness LED laser diode, Hybrid Vehicle etc.
(crystal seed substrate)
At first, show crystal seed substrate 1 in Fig. 1 (a).1b is the back side of substrate 1.Also can buffer layer etc. be set at substrate 1.
The material that constitutes the crystal seed substrate is to see the gan of Yellow luminous effect by fluorescence microscope.
When substrate arranges buffer layer, the preferred vapor growth method of its formation method, Metalorganic chemical vapor deposition method (MOCVD:Metal Organic Chemical Vapor Deposition) method, hydride gas-phase epitaxy (HVPE) method, pulsed laser deposition (PXD) method, MBE method, subliming method can have been exemplified.Preferred especially organometallic chemistry vapour deposition process.
Gan to the jaundice coloured light that uses in this patent is stated.
Wideer peak appears in this gallium nitride crystal scope at 2.2 ~ 2.5eV except the exciton transition (UV) from band (band) to band.This is called Yellow luminous (YL) or yellow band (YB).
By using fluorescent microscope, can only excite the Yellow luminous of this scope, detect have or not Yellow luminous.
Like this Yellow luminous results from the relevant radiation processing of natural flaw that originally just has with crystallization as nitrogen is damaged.Such defective becomes luminescence center.Think that the impurity of Ni, the Co that the chances are by deriving from reaction environment, transition metal such as Cr, Ti etc. enters in the gan, thereby forms Yellow luminous center.
The gallium nitride crystal of such jaundice coloured light is as being disclosed in the special table of Japanese Patent 2005-506271.
This gallium nitride crystal, the surface dislocation density of preferred+C face is 10 8/ cm 2Below.In addition, gallium nitride crystal contains transition metal such as Ti, Fe, Co, Cr or Ni.Moreover, preferably with 10 17/ cm 3To 10 21/ cm 3Concentration contain donor and/or receptor and/or magnetic-doped dose.In addition, the dislocation desity of preferred gallium nitride crystal is 10 4~ 10 8/ cm 2, the full width at half maximum that the X line of (0002) crystal face is measured is below the 150arcsec.
More than the preferred 200 μ m of the thickness of crystal seed substrate, more preferably more than the 400 μ m.
(gallium nitride film)
Then, shown in Fig. 1 (b), on crystal seed substrate 1, form gallium nitride film 3 by flux method on the 1a.Herein, among the present invention, from the interface 50 μ m of crystal seed substrate 1 with the interior inclusion distribution layer 3a that is formed with, be formed with inclusion thereon and lack a layer 3b.In addition, T is the thickness of gallium nitride film 3, and t is the thickness of inclusion distribution layer, in 50 μ m.
Among the present invention, be provided with inclusion distribution layer 3a in the zone below the interface 1a 50 μ m of crystal seed substrate 1 side of gallium nitride film 3.Among Fig. 2,5 is inclusion.
Herein, inclusion refers to, constituted and is included in out-phase in the nitride film by the material that is derived from the contained composition of liquation.The contained composition of liquation refers to, fusing assistant (basic metal of sodium etc.), gallium element and other additives.
This additive can be enumerated carbon, low melting point metal (tin, bismuth, silver, gold), refractory metal (transition metal of iron, manganese, titanium, chromium etc.).Low melting point metal has to prevent being oxidized to purpose of sodium and the situation of adding, and refractory metal has from the container of dress crucible and breeds the situation that the well heater etc. of stove is sneaked into.
Constitute the material of inclusion, be typically the alloy of fusing assistant and gallium and the mixture of metal simple-substance and alloy, or carbon, or the aggregate of the micro-crystallization of gallium or polycrystalline.For example, Ga 4Na, Ga 2Na 3Deciding than alloy or Ga like this 2O 3, Al 2O 3Mixture.
Inclusion distribution layer and the following mensuration of shortage layer.
That is, be dispersed with inclusion in the inclusion distribution layer, can be by the observation of transmitted light type opticmicroscope to this.Specifically, for from the visual field of the visual field, interface height 50 μ m * width 100 μ m,, can observe inclusion and disperse during with the optics microscopic with 200 times of multiplying powers.
In the inclusion distribution layer, inclusion exists towards the interface direction in principle.Herein, inclusion can be arranged and forms alignment layer towards the interface direction, but also random dispersion.
In addition, also can be this situation: the regional integration below interface thickness 50 μ m can become the inclusion distribution layer, but the part in also can the zone below interface thickness 50 μ m becomes the inclusion distribution layer, and there is not inclusion in all the other.That is, the whole zone that there is no need below interface thickness 50 μ m all is dispersed with inclusion.
That is, five layers when dividing towards the per 10 μ m of thickness direction from the interface are observed inclusion respectively.Then, observe whether being dispersed with inclusion in each layer.More preferably, in preferred one deck at least the area ratio of inclusion more than 1%, most preferably more than 2%.There is no special higher limit, but crystallinity worsens easily if inclusion is crossed at most, therefore, from this viewpoint, the area ratio of inclusion is preferably below 10%, more preferably below 7%, most preferably below 5%.
In addition, it is desirable to, for the regional integration below interface thickness 50 μ m, the area ratio of inclusion is preferably more than 1%, most preferably more than 2%.There is no special higher limit, but crystallinity worsens easily if inclusion is crossed at most, therefore, from this viewpoint, the area ratio of inclusion is preferably below 10%, more preferably below 7%, most preferably below 5%.
But, the following calculating of the area ratio in the inclusion distribution layer.That is, as Fig. 2, with crystal seed and on nitride film downcut along cross section, grind cross section with the diamond lap slurry of about 1 micron of particle diameter.Then, with the transmissive optical microscope photographing cross section of 200 times of multiplying powers, the image that obtains is implemented binary conversion treatment.Binary conversion treatment is implemented by the Image pro plus of U.S. Media Cybernetics company.
Specifically put down in writing the method for binary conversion treatment herein.At first, transmitted light type optical microphotograph mirror image is not had compression and upload to computer (TIFF form).Because it is not if compress (jpeg) then image difference, therefore preferred.In addition, image is preferably uploaded with the high pixel count more than the 1M pixel as far as possible.Be 8 gray scales (bit grayscale) with this image transitions.That is, each pixel of image is classified as 0 ~ 255 gray scale.According to the intensity distribution function (if above-mentioned software is then selected " indication range ") of software, read the gray scale of peak strength.As X PeakIn addition, read from intensity profile and be distributed as 99.9% gray-scale value.As X 99.9Then, determine the threshold value of binaryzation.Be divided into two kinds of situations, establish the following gray scale of this threshold value for all white, the above gray scale of threshold value is all black.This threshold value is with X Peak* 2-X 99.9Try to achieve.Then, the black part of bianry image is divided into inclusion.Then, for target zone, remove the area of inclusion with the entire area of inclusion distribution layer, thereby calculate the area ratio in the inclusion distribution layer.
For example, in the example of Fig. 2 (a), inclusion 5 is arranged near the 1a of interface, and in the example of Fig. 2 (b), inclusion 5 is arranged in the place away from interface 1a.What person no matter, each layer when per 10 μ m divide from the interface all is denominator with the area, is molecule with the area ratio of wherein contained inclusion.
Inclusion shortage layer is the visual field to visual field height 50 μ m * width 100 μ m, when 200 times of multiplying powers are observed down, can't observe the layer that inclusion disperses with opticmicroscope.But inclusion lacks in the layer, and a spot of inclusion is inevitably separated out and be there is no obstruction.Particularly, the preferred less than 1% of the area ratio of above-mentioned inclusion more preferably below 0.5%, most preferably be can't see inclusion in fact.In addition, preferably occupied by inclusion shortage layer till the film surface from interface thickness 50 μ m.
In addition, in the inclusion distribution layer, preferably the area of each inclusion is less, particularly, and preferred 60 μ m 2Below, more preferably 20 μ m 2Below.But the deviation during owing to manufacturing is separated out area and is surpassed 60 μ m 2Inclusion till there is no obstruction, but at this moment, area surpasses 60 μ m 2The number of inclusion in the visual field of per 50 μ m * 100 μ m, be below 2 preferably, more preferably below 1.
The thickness T of gallium nitride film and indefinite, but more than the preferred 50 μ m, more preferably more than the 100 μ m.T there is no the special upper limit, but based on the viewpoint on making, can be below 5mm.
Gallium nitride film is the film of non-yellowing coloured light when fluorescent microscope is measured.This gallium nitride film has the situation of the light of the Bluish white sent in fluorescent microscope is measured.It is unclear that for this luminous origin, but the peculiar phenomenon of this method for making.Knowing by the PL spectrometry, is that emission wavelength is 430 to 500nm very wide spectrum.
(processing of nitride film of the present invention)
Composite base plate 7 shown in Fig. 1 (b) can directly be used as equipment portion's material.But, according to purposes, can the composite base plate 7A shown in Fig. 3 (a) as, the surface of grinding gallium nitride film forms the gallium nitride film 3A that has ground.Ginding process is as there being following method for example: after the plane is made in the grinding of being undertaken by the emery wheel with bonded-abrasive (grinding), the free abrasive of use diamond lap slurry etc. grinds (lapping), uses acidity or alkaline CMP slurry to carry out precise finiss (polish) afterwards.In addition, from the viewpoint of the present invention, below the preferred 300 μ m of the thickness after the grinding of gallium nitride film, more preferably below the 150 μ m.
For example, the power parts of using with the umformer of ultra-high brightness LED laser diode, Hybrid Vehicle with the indicating meter of led light source, pure green etc. for the headlight of the White LED that composite base plate is used for high colour rendering and automobile etc. must carry out attrition process to the surface of the gallium nitride film of film forming.At this moment, if the set-back of gallium nitride film is less, then affixes to grinding plate and become easily, can reduce required amount of grinding.In addition, when forming functional layer by vapor phase process etc. on gallium nitride film, the quality of this functional layer can promote.
, by the present invention the inclusion distribution layer is set herein, effective to the set-back that reduces film.This effect the thickness with the inclusion distribution layer be thickness that 1 o'clock, inclusion lack layer be 20 ~ 0.1 o'clock the most remarkable.
That is, if during with the thickness 1 of inclusion distribution layer, inclusion lack layer thickness below 20, then the inhibition of set-back is remarkable.Based on this viewpoint, inclusion lacks the thickness of layer more preferably below 10.
In addition, if with the thickness of inclusion distribution layer be 1 o'clock, inclusion lack layer thickness more than 0.1, then the quality of the functional layer that forms on the gallium nitride film can promote.Based on this viewpoint, inclusion lacks the thickness of layer more preferably more than 0.5.
Set-back of the present invention after gallium nitride film is bred, the viewpoint of the difficulty of the platform when affixing to attrition process is preferably below 200 μ m, more preferably below the 150 μ m.
(functional layer and functional element)
On the composite base plate that so obtains, form functional layer with vapor phase process.
The functional layer of Xing Chenging can be simple layer like this, also can be multilayer.In addition, as function, can be used for power parts that the headlight of the White LED of the high colour rendering of high brightness and automobile uses with the umformer of ultra-high brightness LED laser diode, Hybrid Vehicle with the indicating meter of led light source, pure green etc. etc.
By vapor phase process, when preferably making semiconductor light-emitting-diode (LED) by Metalorganic chemical vapor deposition method (MOCVD) legal system, the dislocation desity of LED inside (luminescent layer) becomes and becomes equal with composite base plate at composite base plate.
From becoming the viewpoint of film quality (suppressing surface imperfection takes place), the film-forming temperature of functional layer is preferred more than 900 ℃, more preferably more than 1000 ℃.In addition, the viewpoint that the In from the control functional layer forms, the film-forming temperature of functional layer is preferred below 1200 ℃, more preferably below 1150 ℃.
The preferred 13 family's element nitrides of the material of functional layer.13 family's elements refer to the 13rd family's element in the periodic law of elements table that IUPAC formulates.13 family's elements specifically are gallium, aluminium, indium, thallium etc.In addition, as additive, can enumerate carbon, low melting point metal (tin, bismuth, silver, gold), refractory metal (transition metal of iron, manganese, titanium, chromium etc.).Low melting point metal has to prevent being oxidized to purpose of sodium and the situation of adding, and refractory metal has from the container of dress crucible and breeds the situation that the well heater etc. of stove is sneaked into.
For example, shown in Fig. 3 (b), form functional layer 8 at composite base plate 7A, as functional element 9.Here, functional layer 8 can form multilayer.For example, in the example of Fig. 3 (c), formed light emitting element structure 8A.Thus, obtain the few light emitting element structure of dislocation desity, so the internal quantum of luminous element 9A improves.
Light emitting element structure 8A is such as possessing the n type semiconductor layer, be arranged at the light-emitting zone on this n type semiconductor layer and be arranged at p-type semiconductor layer on this light-emitting zone.In the luminous element 9A of Fig. 3 (c), be formed with n type contact layer 8a, n type composite bed 8b, active coating 8c, p-type composite bed 8d, p-type contact layer 8e at gallium nitride film 3, constitute light emitting element structure 8A.
(manufacturing installation and condition)
Fig. 4, Fig. 5 show is the formation of device that can be used in the manufacturing of nitride film of the present invention.
Apparatus for crystal production 10 possesses the pressure vessel 12 that has vacuum-pumping maybe can supply with pressurized nitrogen, the universal stage 30 that can rotate and mounting in the outer container 42 of this universal stage 30 in this pressure vessel 12.
Pressure vessel 12 forms the drum that top and bottom are plectane, and inside has the heating space 16 that is surrounded by well heater cover 14.This heating space 16, except epimere well heater 18a, the stage casing well heater 18b and hypomere well heater 18c of the above-below direction of the side by being disposed at heater housing 14, the bottom heater 18d of bottom surface that also can be by being disposed at heater housing 14 regulates internal temperature.This heating space 16 has improved thermal insulation by the heater insulation material 20 on every side that covers heater housing 14.In addition, on the pressure vessel 12, be connected with the nitrogen pipe arrangement 24 of nitrogengas cylinder 22, what be connected with vacuum pump 26 simultaneously vacuumizes pipe arrangement 28.Nitrogen pipe arrangement 24 connects pressure vessel 12, heater insulation material 20 and heater housing 14, is opened on the inside of heating space 16.This nitrogen pipe arrangement 24 has branch halfway, and also there is opening in the gap between pressure vessel 12 and heater insulation material 20.Heater housing 14, though not airtight fully, in order not make the bigger pressure difference of inside and outside generation of heater housing 14, and with nitrogen be supplied to heater housing 14 inside and outside.On the take-off pipe of in the nitrogen pipe arrangement 24 and internal communication heating space 16, the mass flow controller 25 of adjustable throttle amount is installed.Vacuumize pipe arrangement 28 and connect pressure vessel 12, the clearance opening between pressure vessel 12 and heater insulation material 20.If the outside of heater housing 14 is vacuum state, then the heating space 16 that connects by nitrogen pipe arrangement 24 also becomes vacuum state.
Universal stage 30 forms discoid, is disposed at the below of heating space 16.Below this universal stage 30, the turning axle 34 with inner magnet 32 is installed.This turning axle 34 is inserted into the following all-in-one-piece tubular cover body 36 with pressure vessel 12 by heater housing 14 and heater insulation material 20.In the periphery of cover body 36, by not shown motor, can dispose the external magnet 38 of tubular rotatably.This external magnet 38, it is relative with the inner magnet 32 of turning axle 34 by cover body 36 to be situated between.Therefore, along with the rotation of external magnet 38, the turning axle 34 with inner magnet 32 can rotate, and then universal stage 30 can rotation.In addition, along with moving up and down of external magnet 38, the turning axle 34 with inner magnet 32 can move up and down, and then universal stage 30 can move up and down.
Outer container 42, the metal outer container that possesses the upper opening of the metal that bottom tube-like is arranged outer container main body 44 processed and this outer container main body 44 of sealing covers 46.Container cover 46 outside, from following center nitrogen ingress pipe 48 are installed obliquely upward.This nitrogen ingress pipe 48 is designed to, even outer container 42, can not conflict with nitrogen pipe arrangement 24 close to nitrogen pipe arrangement 24 along with the rotation of universal stage 30 yet.Both distance when particularly, nitrogen ingress pipe 48 is near nitrogen pipe arrangement 24 is set to several mm ~ tens of cm.The inside of outer container main body 44 is provided with the inner jar 16 of Fig. 5.
That is, in the example of Fig. 5, inner jar 16 is two-layer laminate.Each container 16 is made of main body 16a and lid 16b.In the inner space of container 16, take in, be laminated with regulation number, 2 crucibles 14 for example.Each crucible 14 is made of main body 14a and lid 14b, takes in the material of liquation 13 in main body 14a.
The use-case that makes to the crystallization plates manufacturing installation 10 of the present embodiment of formation like this describes.For example, prepare gallium, as the sodium Metal 99.5 of fusing assistant.In crucible 14, crystal seed substrate 1 be impregnated in the mixed molten liquid that contains gallium and sodium Metal 99.5, use heating space 16 heating of each well heater 18a ~ 18d when making universal stage 30 rotations on one side, supply with pressurized nitrogen to mixed molten liquid on one side, in mixed molten liquid, make the crystalline growth of gan thus on the crystal seed substrate.If add carbon in right amount to mixed molten liquid, then can suppress the generation of stray crystal, therefore comparatively desirable.Stray crystal refers to, the place crystallization beyond the crystal seed substrate gan.The gallium nitride crystal plate of growing in mixed molten liquid in the crucible can be after cooling, by adding organic solvent (for example lower alcohol of methyl alcohol or ethanol etc.) to container, and the unwanted material of dissolving fusing assistant etc. in this organic solvent, thus reclaim.
When making the gallium nitride crystal plate as described above, Heating temperature is set at below the boiling point of the mixed molten liquid under the pressurized nitrogen atmosphere.Particularly, be preferably set to 700 ~ 1000 ℃, more preferably be set at 800 ~ 900 ℃.For the temperature that makes heating space 16 even, preferably be set at temperature by the order of epimere well heater 18a, stage casing well heater 18b, hypomere well heater 18c, bottom heater 18d and uprise, or epimere well heater 18a and stage casing well heater 18b are set at uniform temp T1, hypomere well heater 18c and bottom heater 18d are set at the temperature T 2 that is higher than this temperature T 1.In addition, the pressure of pressurized nitrogen is preferably set to 1 ~ 7MPa, more preferably is set at 2 ~ 6MPa.In order to adjust the pressure of pressurized nitrogen, at first, drive vacuum pump 26, by vacuumizing pipe arrangement 28, make the internal pressure of pressure vessel 12 become high vacuum state (for example below the 1Pa or below the 0.1Pa), then, will vacuumize pipe arrangement 28 by not shown valve closure, undertaken by the inside and outside supply nitrogen of nitrogen pipe arrangement 24 to heater housing 14 from nitrogengas cylinder 22.Gallium nitride crystal is at growing period, owing to nitrogen gas dissolved in mixed molten liquid be consumed, the pressure of pressurized nitrogen descends, therefore, in crystalline growth, to the nitrogen of heating space 16 by mass flow controller 25 sustainable supplies regulation flow.During this period, the take-off pipe that communicates with the outside of heater housing 14 in the nitrogen pipe arrangement 24 is by not shown valve closure.
Preferably the pressure of described pressurization atmosphere is set in the scope of 1 ~ 7MPa.Like this, compare to the situation of the pressure that is set at several 100MPa, the resistance to pressure of manufacturing installation can be lower, therefore can expect its miniaturization and that becomes.
, when making described container rotate, can make described container counter-rotating herein, also can rotate in the same direction as.When making container to a direction rotation, speed of rotation is set at for example 10 ~ 30rpm.In addition, when making the container counter-rotating, speed of rotation is set at for example 10 ~ 30rpm.
In addition, preferably after inclusion distribution layer of the present invention is generated, make container stop the rotation.At this moment, preferred 100 seconds ~ 6000 seconds of rotation stand-by time, more preferably 600 seconds ~ 3600 seconds.In addition, preferred 10 seconds ~ 600 seconds of the rotational time before and after the rotation stand-by time, the preferred 10 ~ 30rpm of speed of rotation.
In addition, shoal by making the liquation in the crucible 14, can promote the comprising of inclusion at initial stage.For this reason, preferably as shown in Figure 5, use highly lower crucible 14, in liquation at the horizontal crystal seed substrate 11 of crucible bottom.In addition, crucible 14 that preferably will be highly lower is stacked a plurality of.In addition, by shortening the unsaturation time before crystallization is bred, can promote equally that the inclusion in the initial stage comprises.Meanwhile, by as the adjusted speed of rotation, the generation of the initial stage that can suppress to breed inclusion later.
In addition, the unsaturation time refers to, the timed interval that liquation no show state of saturation, crystalline growth do not begin.
In addition, the ratio (mol ratio) of the 13 family's element nitride/fusing assistants (for example sodium) in the liquation based on viewpoint of the present invention, preferably makes it higher, more than the preferred 18mol%, more preferably more than the 25mol%.By making it strengthen, can promote that the inclusion in the initial stage comprises.But if this ratio becomes excessive, then downtrending appears in crystalline quality, below the therefore preferred 40mol%.
Definition to the monocrystalline among the application is set forth.Though comprise the textbook monocrystalline that atom is arranged regularly in the crystallization integral body, have more than and be defined in this, refer to the monocrystalline that circulates on the general industry.That is, crystallization can contain defective to a certain degree, or can there be distortion the inherence, maybe can contain impurity, is to distinguish mutually, these are called monocrystalline and use identical meaning with polycrystalline (pottery).
Embodiment
(embodiment 1)
Use Fig. 4, apparatus for crystal production shown in Figure 5, make gallium nitride crystal.Below describe its order in detail.
At first, in the glove box of argon atmosphere, at the end of the crucible 14 of internal diameter φ 70mm with crystal seed substrate horizontal arrangement.
But the crystal seed substrate is made of gallium nitride single crystal, and the thickness of substrate is 300 ± 30 microns, and the size on plane is diameter 50.8 ± 0.2mm.With the defect concentration on the surface of crystal seed substrate by CL(cathodeluminescence) measure and estimate, be about 1 ~ 6 * 10 7/ cm 2In addition, the following operation of the material back of crystal seed substrate is measured with fluorescent microscope, obtained following result.
Fluorescent microscope uses the BX series of Olympus Corp's system, excites strainer to adopt BP330-385(only to see through the light of wavelength 330-385nm), suction strainer has adopted BA420(to absorb the light of the following wavelength of 420nm).Excitation light source is extra-high-pressure mercury vapour lamp.Excite the band (band) of gan to hold (364nm) with these formations, the impurity band of only taking the visible region with the CCD photographic camera is luminous, the visual observation.
Then, sodium Metal 99.5 15g, gallium 10g, carbon 39mg(Ga/Na ratio are 0.5mol% for 18mol%, C/Na ratio) be filled in the crucible 14.Crucible 14 is put into the inner jar 16 of stainless steel, again inner jar 16 is put into outer container 14, the opening of outer container main body is closed with the outer container lid that the nitrogen ingress pipe is installed.This outer container is arranged on the universal stage that has carried out vacuum bakeout in advance, pressure vessel 12 is closed loam cake, airtight.
Then, will be evacuated to below the 0.1Pa in the pressure vessel with vacuum pump.Then, epimere well heater, stage casing well heater, hypomere well heater and bottom heater are adjusted to 860 ℃, 860 ℃, 870 ℃, 870 ℃ respectively on one side, the temperature of heating space is heated to be 865 ℃ on one side, till on one side from nitrogengas cylinder importing nitrogen to 4.0MPa, make outer container turn clockwise all the time around the speed of central shaft with 30rpm.Pick-up period a=1 second, hold-time b=15 second, deceleration time c=1 second, stand-by time d=2000 second.Then, this state was kept 10 hours.Afterwards, naturally cool to room temperature after, open the lid of pressure vessel, therefrom take out crucible, drop into ethanol to crucible, sodium Metal 99.5 is dissolved in ethanol after, reclaim the gallium nitride crystal plate of having grown.The size of this gallium nitride crystal plate is 2 inches of φ, plants about 0.1mm that grown on the substrate.Therefore, average crystal growth rate can estimate to be about 10 μ m/h.
In addition, the degree of depth of liquation is about 4mm, and the unsaturation time is about 2 hours.
Observed the cross section of the crystallization of growth.As a result, in the zone of about 20 μ m at growth beginning initial stage, have size as can be known and be several microns inclusion.This inclusion is carried out sims analysis, detect sodium and gallium.In addition, the inclusion area ratio in each layer is shown in table 1.In addition, the inclusion area ratio in the 50 μ m of interface is about 5%, and the inclusion area ratio that inclusion thereon lacks in the layer is about 0%.
In addition, the area of the inclusion of display area maximum in the table 2.
Be thickness 70 μ m with this regional attrition process of having grown, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 5~ 10 6/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate.
The material of the gallium nitride film that obtains is measured with fluorescent microscope as described above, obtained following result.
Present blueness or water colour in visual.Measure luminescent spectrum with spectrum analyzer, centre wavelength is 460nm, and full width at half maximum (FWHM) (full width at half maximum) is about 60nm, luminous for wide spectrum.
(embodiment 2)
Form gallium nitride film similarly to Example 1.But sense of rotation is periodic inversion.In addition, counter-rotating is repeated in pick-up period=1 second, hold-time=15 second, deceleration time=1 second, stand-by time=3000 second.
Observed the cross section of the crystallization of growth.As a result, in the zone of 50 μ m at growth beginning initial stage, have size as can be known and be several microns inclusion.This inclusion is carried out sims analysis, detect sodium and gallium.Inclusion area ratio in each layer shows in table 1.In addition, the inclusion area ratio in the 20 μ m of interface is about 2%, and the inclusion area ratio that inclusion thereon lacks in the layer is about 0%.
The regional attrition process of this growth to becoming thickness 70 μ m, is adjusted into 0.4mm with the thickness of substrate integral body.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 5~ 10 6/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate.
(embodiment 3)
Form gallium nitride film similarly to Example 1.But sense of rotation is periodic inversion.In addition, counter-rotating is repeated in pick-up period=1 second, hold-time=15 second, deceleration time=1 second, stand-by time=3000 second.Speed of rotation is 10rpm.
Observed the cross section of the crystallization of growth.As a result, in the zone of 50 μ m at growth beginning initial stage, have size as can be known and be several microns inclusion.This inclusion is carried out sims analysis, detect sodium and gallium.Inclusion area ratio in each layer shows in table 1.In addition, the inclusion area ratio in the 20 μ m of interface is about 4%, and the inclusion area ratio that inclusion thereon lacks in the layer is about 0%.
Be thickness 70 μ m with the regional attrition process of this growth, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 5~ 10 6/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate.
(embodiment 4)
Form gallium nitride film similarly to Example 1.But sense of rotation only is that speed of rotation is 30rpm clockwise.In addition, sodium Metal 99.5 is 13.5g, gallium 18g, carbon 35mg, and Ga/Na is than being 30mol%.
Observed the cross section of the crystallization of growth.As a result, in the zone of 20 μ m at growth beginning initial stage, have size as can be known and be several microns inclusion.This inclusion is carried out sims analysis, detect sodium and gallium.Inclusion area ratio in each layer shows in table 1.In addition, the inclusion area ratio in the 50 μ m of interface is about 5%, and the inclusion area ratio that inclusion thereon lacks in the layer is about 0%.
Be thickness 70 μ m with the regional attrition process of this growth, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 5~ 10 6/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate.
(embodiment 5)
Form gallium nitride film similarly to Example 1.But sodium Metal 99.5 is 13.5g, gallium 18g, carbon 35mg, and Ga/Na is than being 30mol%.
Observed the cross section of the crystallization of growth.As a result, in the zone of 50 μ m at growth beginning initial stage, have size as can be known and be several microns inclusion.This space part is carried out sims analysis, detect sodium and gallium.Inclusion area ratio in each layer is shown in table 1.In addition, the inclusion area ratio in the 20 μ m of interface is about 5%, and the inclusion area ratio that inclusion thereon lacks in the layer is about 0%.
Be thickness 70 μ m with the regional attrition process of this growth, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 5~ 10 6/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate.
(comparative example 1)
Form gallium nitride film similarly to Example 1.But sodium Metal 99.5 is 10g, gallium 5g, carbon 39mg, and Ga/Na is than being 10mol%.In addition, under the situation of not stopping the rotation, Yi Bian bred with clockwise 30rpm rotation on one side all the time in 15 hours.The size of this gallium nitride crystal plate is 2 inches of φ, plants about 0.1mm that grown on the substrate.Therefore, average crystal growth rate can estimate to be about 6.7 μ m/h.
Observed the cross section of the crystallization of growth.As a result, in the zone of 50 μ m at growth beginning initial stage, there is not inclusion as can be known.
Be thickness 70 μ m with the regional attrition process of this growth, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 7/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate, but many than embodiment 1 defective.
(comparative example 2)
Form gallium nitride film similarly to Example 1.But, under the situation of not stopping the rotation, Yi Bian bred with clockwise 30rpm rotation on one side all the time in 15 hours.The size of this gallium nitride crystal plate is 2 inches of φ, plants about 0.1mm that grown on the substrate.
Observed the cross section of the crystallization of growth.As a result, in the zone of 50 μ m at growth beginning initial stage, there is not inclusion as can be known.
Be thickness 70 μ m with the regional attrition process of this growth, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 7/ cm 2About, compare significantly reduction with the defect concentration of kind of substrate, but many than embodiment 1 defective.
(comparative example 3)
Form gallium nitride film similarly to Example 1.But sodium Metal 99.5 is 13.5g, gallium 18g, carbon 35mg, and Ga/Na is than being 30mol%.In addition, though carry out periodic inversion, speed of rotation is 10rpm.The size of this gallium nitride crystal plate is 2 inches of φ, plants about 0.1mm that grown on the substrate.
Observed the cross section of the crystallization of growth.As a result, in the zone of 50 μ m at growth beginning initial stage, have bigger inclusion as can be known.This inclusion is carried out sims analysis, detect sodium and gallium.In addition, the inclusion area ratio in the 50 μ m of interface is about 10%, and the inclusion area ratio in the zone thereon is about 5%.
Be thickness 80 μ m with the regional attrition process of this growth, the thickness of substrate integral body is adjusted into 0.4mm.To the defect concentration on surface by CL(cathodeluminescence) measure and estimate, be 10 7/ cm 2About.
The relation of table 1 growth thickness and inclusion area occupation ratio
Figure BDA00002833096600131
The maximum inclusion area of table 2
Figure BDA00002833096600132
Figure BDA00002833096600133
(comparative example 7)
Form gallium nitride film similarly to Example 1.But, epimere well heater, stage casing well heater, hypomere well heater and bottom heater are adjusted to 840 ℃, 840 ℃, 850 ℃, 850 ℃ respectively, the temperature of heating space is heated to be 845 ℃, kept 10 hours with this state.The size of this gan is 2 inches of φ, plants about 0.20mm that grown on the substrate.
The result of the cross-section of the crystallization of growing as can be known not only in the zone of 50 μ m at growth beginning initial stage, and also has inclusion and contains layer in the zone of 50 ~ 200 μ m.Inclusion area ratio in the 50 μ m of interface is about 10%, and the inclusion area ratio in the zone of 50 ~ 60 μ m is about 8%.
In addition, when using this gallium nitride crystal plate with LED structure film forming, the part that contains inclusion becomes concavo-convex growth, can't make LED.
In addition, in each above-mentioned embodiment, comparative example, identical with embodiment 1 by the result of fluorescent microscope observation gallium nitride film.

Claims (6)

1. a composite base plate is characterized in that, is a kind of composite base plate with crystal seed substrate and gallium nitride film,
Described crystal seed substrate is made of the gan of seeing Yellow luminous effect by fluorescence microscope, and described gallium nitride film is the film of being bred, do not seen described Yellow luminous effect on described crystal seed substrate by flux method under nitrogen containing atmosphere by liquation,
The inclusion that described composite base plate comprises the inclusion distribution layer of the inclusion that is distributed with the composition that is derived from described liquation that is arranged at the zone below the interface 50 μ m of the described crystal seed substrate-side of described gallium nitride film and is arranged at the described inclusion of shortage on this inclusion distribution layer lacks layer.
2. composite base plate according to claim 1 is characterized in that, during along the cross-sectional view of described gallium nitride film, the maximum area of the described inclusion in the described inclusion distribution layer is at 60 μ m 2Below.
3. composite base plate according to claim 1 and 2 is characterized in that, contains at least 1 in germanium, silicon, the oxygen in the described gallium nitride film, is shown as the n type.
4. according to any described composite base plate of claim 1 ~ 3, it is characterized in that, is 1 o'clock with the thickness of described inclusion distribution layer, and the thickness that described inclusion lacks layer is 20 ~ 0.1.
5. a functional element is characterized in that, the functional layer that is made of 13 family's element nitride films that possesses any described composite base plate of claim 1 ~ 4 and form by vapor phase process on described gallium nitride film.
6. functional element according to claim 5 is characterized in that, described functional layer has lighting function.
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108291329A (en) * 2015-12-11 2018-07-17 日本碍子株式会社 13 race's element nitride crystal substrates and function element

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108291329A (en) * 2015-12-11 2018-07-17 日本碍子株式会社 13 race's element nitride crystal substrates and function element
CN108291329B (en) * 2015-12-11 2019-03-01 日本碍子株式会社 Group 13 element nitride crystal substrate and functional device

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