CN102214749A - Light emitting diode having vertical structure, and method for peeling off thin film from substrate - Google Patents
Light emitting diode having vertical structure, and method for peeling off thin film from substrate Download PDFInfo
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- CN102214749A CN102214749A CN2011101650573A CN201110165057A CN102214749A CN 102214749 A CN102214749 A CN 102214749A CN 2011101650573 A CN2011101650573 A CN 2011101650573A CN 201110165057 A CN201110165057 A CN 201110165057A CN 102214749 A CN102214749 A CN 102214749A
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Abstract
The invention relates to a light emitting diode (LED) having a vertical structure, and a method for peeling off a thin film from a substrate. The technical scheme at least comprises the following steps of: 1) pre-burying and growing a zinc oxide buffer layer on an epitaxial growth substrate, preparing an LED epitaxial slice on the epitaxial growth substrate and performing table-board etching on the epitaxial slice by a dry etching process; 2) manufacturing a reflecting mirror, an ohm electrode layer and a metal bonding and adhering layer on the P-face of the surface of epitaxial slice; 3) inverting the epitaxial slice to another heat conducting substrate by a metal bonding process; 4) performing liquid chemical erosion on the bonded epitaxial slice in a chemical erosion slot; and 5) manufacturing an N-type electrode, texturing an N-type surface and etching the surface to finish manufacturing the LED having the vertical structure. The manufacturing process is simple and requirements on equipment are low; the peeling process of the epitaxial growth substrate is performed on a batch of epitaxial slices at the same time, and the yield is increased remarkably; and inner quantum efficiency cannot be negatively influenced.
Description
Technical field
The invention belongs to gallium nitride based light emitting diode with vertical structure technical field, be specifically related to a kind of method that relates to light emitting diode with vertical structure and film and substrate desquamation.
Background technology
The development of semiconductor light-emitting-diode (Light Emitting Diode is hereinafter to be referred as LED) has many decades history, and it has in signal demonstration, backlight and solid-state illumination field extremely widely uses.LED(based on III-V compounds of group gallium nitride (GaN) material comprises its Al, In alloy material at present) can cover the most of wave band from the deep ultraviolet to the visible light.The device architecture of LED is to form P-type and N-type layer film by epitaxial growth technology, general is luminous zone with N-type interlayer framework by the charge carrier recombination region that can form with different periodicity sandwich constructions in the P-type, and epitaxially grown substrate adopts sapphire (Al2O3) substrate.Device is finished steps such as the making of separation, electrode of chip and surface-texturing and is formed through semiconducter process, add forward bias and inject electronics after photon is compound and luminous after encapsulation.According to being with design, can realize that the light of different wave length produces and output.
Traditional LED device architecture places the same side of LED film with N type and P type electrode, i.e. the surface of film, and do not have electrode owing to the existence of the Sapphire Substrate of insulation at the bottom of film.In this design, P-type and N-type electrode adopt the local dry cavity etching process to be distributed in the both sides of chip surface, and injection current is flow through the luminous zone of LED by horizontal direction.Such LED device has limited the full-size of led chip monolithic and the luminous efficiency of integral device because uneven electronics laterally injects and side diffusion causes inhomogeneous luminous from P-type electrode district to N-type electrode district.Under the high current density injection condition, it is congested that electric current appears in the zone of close N type electrode easily, causes the too high even whole LED component failure of local temperature.Simultaneously, to be converted into heat energy owing to fail to be converted into the input electric energy of luminous energy in the LED device work of this planar structure, this heat energy can not effectively loose to encapsulation base plate by the Sapphire Substrate of thermal conductivity extreme difference, therefore limited the further lifting of device power, become the big obstacle of the therefrom low power display device of LED to the application of the illuminating device of high-power and super high power.Be electric current congestion problems and the heat radiation bottleneck problem that solves chip, need to change the structure of LED device, make N-type and P-type electrode become vertical stratification from horizontal structure, promptly injection current mainly evenly flows through the LED device architecture in the mode perpendicular to film surface.Vertical stratification device for the LED film realizing growing on the Sapphire Substrate, it is the way (US006071795) that Ultra-Violet Laser is peeled off that people such as the Nathan W. Cheung in California, USA university Berkeley branch school have proposed to adopt selectivity optics processing technology, utilize the strong light absorption of Ultra-Violet Laser to produce the GaN localized heat and decompose, realize separating of LED film and Sapphire Substrate at the interface of sapphire material and GaN material.The limitation of this method is the special equipment that needs complex and expensive, laser lift-off is a monolithic epitaxial wafer serial process, and each chip in every sheet epitaxy sheet is peeled off one by one by the laser step-scan, work efficiency is low, complex process produces stress mismatch to the LED luminous zone and causes degradation under the internal quantum efficiency.
Summary of the invention
The objective of the invention is to, the method of a kind of light emitting diode with vertical structure and film thereof and substrate desquamation is provided, to overcome the serial process that can only carry out the monolithic epitaxial wafer that existing gallium nitride based light emitting diode with vertical structure modular construction and manufacture method thereof exist, complex process, to the LED luminous zone produce that stress mismatch causes that internal quantum efficiency descends problem.
To achieve these goals, the technical solution used in the present invention is:
A kind of film of light emitting diode with vertical structure and the method for substrate desquamation is characterized in that: this method utilizes wet chemical to peel off, and may further comprise the steps at least:
1) on epitaxial growth substrate 11, buries developing zinc oxide resilient coating 12 in advance, on epitaxial growth substrate 11, prepare the LED epitaxial wafer again, by dry etch process epitaxial wafer is carried out mesa etch then, epitaxial wafer is carried out selectivity figure etching, finish led chip and separate with the chip-scale of carrying out at interval according to the size of design, etching depth sees through the epitaxial loayer film at least;
2) the P-on epitaxial wafer surface face according to the graphic making reflective mirror of chip design, ohmic electrode layer, metal bonding adhesion layer and crisscross reflector-free, do not have Ohmic electrode and do not have the white space of metal bonding adhesion layer;
3) epitaxial wafer is inverted on another heat-conducting substrate 203 by metal bonding technology;
4) bonding is good epitaxial wafer carries out the aqueous chemical corrosion in chemical corrosion groove, liquid chemical reagent is by the space of chip chamber and the white space of reservation, the ZnO resilient coating is corroded, when treating that the ZnO resilient coating is corroded fully, epitaxial growth substrate and LED film separate, and the LED film is stayed on the counter-rotating substrate, and epitaxial growth substrate comes off automatically, formation can be made the structure of vertical stratification LED device, and this moment, the N-N-type semiconductor N was exposed to the surface;
5) by making N-type electrode, N-type surface-texturing, surface etch, finish the making of vertical stratification LED.
The growth technique of described ZnO resilient coating (12) includes but not limited to the Organometallic Chemistry vapour phase epitaxy, molecular beam epitaxy, atomic layer epitaxy, pulsed laser deposition; ZnO resilient coating (12) finish in same growth apparatus with follow-up LED film or in advance on substrate deposit standby; The thickness of ZnO is between 0.1 micron to 100 microns.
Described heat-conducting substrate be moulding in advance and the substrate of the good bonding metal layer of evaporation, include but not limited to Si, AlSi, Cu, CuMo, CuW, or adopt the Heat Conduction Material heat-conducting substrate of thermal finalization again that applies indefinite form or liquid.
Described chemical reagent includes but not limited to the hydrochloric acid dilution, in room temperature or be higher than under the temperature that room temperature is lower than 100C, and down auxiliary in ultrasonic vibration, chemical reagent flows into epitaxial wafer from the led chip trench lateral.
A kind of light emitting diode with vertical structure is characterized in that: comprise
One epitaxial growth substrate 11,
One ZnO resilient coating 12 is positioned on this epitaxial growth substrate 11,
One GaN resilient coating 13 is positioned on this ZnO resilient coating 12,
One N type GaN layer 14 is positioned on the GaN resilient coating 13,
One-period property multilayer luminous zone-quantum well 15 is positioned on this N type GaN layer 14,
One electronic barrier layer 16 is positioned on this periodicity multilayer luminous zone-quantum well 15,
One P type GaN layer 17 is positioned on this electronic barrier layer 16.
Choosing of the epitaxial growth substrate of described LED includes but not limited to that sapphire, aluminium nitride, gallium nitride, silicon, carborundum, its crystal orientation include but not limited to 0001 polarization such as grade, semipolar and non-polarized direction; Selected substrate comprises patterned surface texture.
Described N type GaN layer is provided with N-face electrode metal layer, forms ohmic contact with N type layer semi-conducting material, for single or multi-layer metal structure, includes but not limited to titanium, aluminium, gold, vanadium and its alloy.
The present invention buries developing zinc oxide (ZnO) resilient coating in advance by adopting on substrate in outer layer growth, utilize the ZnO layer in chemical corrosion, can be easy to epitaxial growth substrate be separated with the LED film by the principle of liquid chemical reagent (for example hydrochloric acid) corrosion.
With respect to prior art, advantage of the present invention and beneficial effect are: (1) technology is made simple, and equipment requirements is low; (2) epitaxial wafer is in batches carried out simultaneously the stripping technology of epitaxial growth substrate, output capacity obviously improves; (3) the substrate desquamation technology that provides of this patent does not require the light absorption and the permeability of substrate, makes the substrates that much can't realize with laser lift-off (for example Si, GaN, SiC etc.) can implement stripping technology; (4) huge stress and the impulsive force of having avoided laser lift-off in transient high temperature that Sapphire Substrate and LED film interface produce and mechanical separation process, to produce, can not increase the fault of construction of LED epitaxial loayer, be a kind of chip technology technology of internal quantum efficiency not being had negative effect; (5) the method not only can be used for making the led chip of small size (some microns), also is applicable to the led chip of making large scale (millimeter or centimetre) simultaneously, opens up new chip dimension for realizing that semiconductor lighting is used.
Description of drawings
Below in conjunction with drawings and Examples this patent is further specified.
Fig. 1 is that the present invention contains the LED epitaxial structure schematic diagram on the Sapphire Substrate of ZnO resilient coating.
Fig. 2 is the schematic flow sheet of substrate desquamation technology of the present invention.
Fig. 3 is the cross sectional representation that the present invention carries out the Sapphire Substrate stripping technology.
Fig. 4 is the top plan view after the light emitting diode (LED) chip with vertical structure fluting etching of the present invention.
Fig. 5 be light emitting diode (LED) chip with vertical structure of the present invention fluting and transfer to heat-conducting substrate after cross sectional representation.
The primary clustering symbol description:
The 11-epitaxial growth substrate, 201-P-face reflective mirror and ohmic contact metal layer; The 12-ZnO resilient coating, 202-P-face metal diffusion barrier layer and bonded layer, the 13-GaN resilient coating, 203-heat-conducting substrate, 14-N-type GaN layer, 15-is multilayer luminous zone-quantum well periodically, the 16-electronic barrier layer, 17-P type GaN layer, the barrier layer of 18-quantum well, the potential well layer of 19-quantum well, the 20-LED film.
Embodiment
The present invention will be further described with preferred specific embodiment below in conjunction with accompanying drawing.In concrete designs with in making, the LED structure that the present invention proposes will modify its part-structure and size within the specific limits according to the needs of application and manufacturing process enforcement, and choosing of material carried out accommodation.
Referring to Fig. 2-Fig. 5, choosing of the epitaxial growth substrate 11 of LED of the present invention includes but not limited to sapphire (Al
2O
3), aluminium nitride (AlN), gallium nitride (GaN), silicon (Si), carborundum (SiC), its crystal orientation includes but not limited to polarization, semipolar and non-polarized directions such as (0001).Thereby selected substrate can comprise patterned surface texture to be improved light extraction efficiency and reduces dislocation density.
Is example with sapphire as substrate, utilizes wet chemical of the present invention to carry out separating process, and step comprises: (1) has in growth on the LED membrane structure of ZnO resilient coating 12 by litho pattern, adopts BCl
3Or Cl
2Deng the plasma etching industrial of reacting gas, the GaN in chip gap is carried out the step etching.Etching depth is decided according to the thickness of LED film, but will guarantee that etching penetrates all LED thin-film materials, comprises that ZnO resilient coating 12(vertical view sees Fig. 3); Then, continue etching epitaxial growth substrate 11, this process may comprise the replacing reacting gas, to reach at the be etched best etching effect of material of difference; The degree of depth of substrate etching will guarantee greater than 1 micron, can reach tens microns (the transversal Fig. 4 of meeting personally).(2) surface of P type GaN layer 17 is by the way of photoetching or mechanical mask evaporation, evaporation P type ohmic contact metal layer 201, and this layer while be as the reflective mirror material of high reflectance, and the light that vertical stratification LED is produced reflexes to the optical interface that goes out of LED effectively.This P type ohmic contact metal layer can be single metal or multi-layer metal structure.(3) on the ohmic contact metal layer 201 of chip, adopt sandwich construction by photoetching or mechanical mask evaporation metal diffusion barrier layer and bonded layer 202. metal diffusion barrier layers, effectively stop the counterdiffusion mutually of bonded layer and ohmic metal interlayer; The metal bonding layer can be a multilayer, is used for bonding heat-conducting substrate in bonding technology.The separated region of attention between chip do not have ohmic metal layer 201 and metal diffusion barrier layer and bonded layer 202.(4) can will have the LED film transfer of graphical P-face electrode to heat-conducting substrate thus.Heat-conducting substrate can be moulding in advance and the substrate of the good bonding metal layer of evaporation, include but not limited to materials such as Si, AlSi, Cu, CuMo, CuW, also can be adopt apply indefinite form or liquid Heat Conduction Material again the way of thermal finalization form heat-conducting substrate.(5) in the aqueous chemical reactive tank, inject chemical reagent, include but not limited to the hydrochloric acid dilution of specific concentrations, in room temperature or be higher than under the temperature that room temperature is lower than 100C, assisting down of ultrasonic vibration, chemical reagent flows into epitaxial wafer from the led chip trench lateral, contact (see figure 5) with the ZnO resilient coating, corrosion and displacement ZnO composition, after the ZnO layer for the treatment of all chips is corroded and finishes, epitaxial growth substrate automatically and the LED divided thin film from, substrate comes off, and the LED film is still stayed and shifted on the heat-conducting substrate.(6) the LED film surface after peeling off is included but not limited to processing such as chemical machinery polishing or plasma etching, make the graphical and evaporation of N-type electrode then, and carry out the texturing of N-type laminar surface, improve light extraction efficiency.
Growth ZnO resilient coating 12 on substrate 11 is used for the chemical corrosion sacrifice layer of vertical stratification LED film and substrate separation process.While owing to the lattice matched of ZnO and GaN material, can reduce the stress effect of LED film in growth course, improve the GaN resilient coating of subsequent growth and the crystal mass of N type GaN layer, luminous zone and P type layer.
The growth technique of ZnO resilient coating includes but not limited to Organometallic Chemistry vapour phase epitaxy (MOCVD), molecular beam epitaxy (MBE), atomic layer epitaxy (ALD), pulsed laser deposition (PLD); ZnO resilient coating and follow-up LED film in same growth apparatus, finish or in advance on substrate deposit standby; The thickness of ZnO is between 0.1 micron to 100 microns.
On the surface of ZnO resilient coating 12, form GaN resilient coating (non-impurity-doped) 13 and N type GaN layer 14 successively, the heterostructure of luminous zone 15(multilayer periodic performance band structure), electronic barrier layer 16 and P-type material layer 17.In the LED of some wavelength structure, can there be one deck AlGaN thin layer to be used for improving the antistatic property of device in the n type material layer; In luminescent layer, can insert one deck hole blocking layer.Luminescent layer is a quantum well structure, comprises barrier layer and the lower potential well layer of bandwidth that bandwidth is higher.Above-mentioned each material layer all can be made of the compound semiconductor of nitride, includes but not limited to InxAlyGa1-x-yN (0≤x≤1,0≤y≤1,0≤x+y≤1), and the ratio of x and y can be according to LED design goes out the optical wavelength design.The semiconductor band gap of N type layer and P type layer is higher than the semi-conducting material band gap of luminescent layer, guarantees that the light that sends can be transmitted into beyond the device.Above-mentioned layers of material all can mix or undope as required, for example doped silicon (Si) can form N-type layer, magnesium (Mg) and form P-type layer etc., its doping way comprise continuous doping and discontinuous doping (such as, pulsed is mixed (delta doping)) etc.In order to obtain higher electronics and hole concentration, also can utilize the built-in polarized electric field of nitride to mix, promptly introduce unadulterated higher bandwidth material and form superlattice structure (polarization doped superlattice) at doped region.Also can comprise similar superlattice structure in the N type layer and be used for reducing dislocation density.
Referring to Fig. 1, the structural representation for a kind of light emitting diode with vertical structure of the present invention comprises
One substrate,
One ZnO resilient coating is positioned on this substrate,
One GaN resilient coating is positioned on this ZnO resilient coating,
One N type layer is positioned on the GaN resilient coating,
One luminous zone is positioned on this N type layer,
One electronic barrier layer is positioned on this luminous zone,
One P layer is positioned on this electronic barrier layer.
The sidewall of led chip and the non-metallized section of light-emitting area are by for example insulating material film such as SiO2, Si3N4 covering of surface passivation layer.The generation type of insulating barrier includes but not limited to use plasma reinforced chemical vapour deposition (PECVD), and by photoetching process in methods such as insulating barrier formation rule patterns.The size of chip no longer depends on the beam spot size of laser lift-off, but can be selected according to design, and the groove by chip step etching defines, and has broken away from the restriction of large size chip.
N-face electrode metal layer and N type layer semi-conducting material form ohmic contact, can be single or multi-layer metal structures, include but not limited to titanium (Ti), aluminium (Al), gold (Au), vanadium (V) and its alloy.
Claims (7)
1. the method for the film of a light emitting diode with vertical structure and substrate desquamation, it is characterized in that: this method utilizes wet chemical to peel off, and may further comprise the steps at least:
1) on epitaxial growth substrate (11), buries developing zinc oxide resilient coating (12) in advance, go up preparation LED epitaxial wafer in epitaxial growth substrate (11) again, by dry etch process epitaxial wafer is carried out mesa etch then, epitaxial wafer is carried out selectivity figure etching, finish led chip and separate with the chip-scale of carrying out at interval according to the size of design, etching depth sees through the epitaxial loayer film at least;
2) the P-on epitaxial wafer surface face according to the graphic making reflective mirror of chip design, ohmic electrode layer, metal bonding adhesion layer and crisscross reflector-free, do not have Ohmic electrode and do not have the white space of metal bonding adhesion layer;
3) epitaxial wafer is inverted on another heat-conducting substrate (203) by metal bonding technology;
4) bonding is good epitaxial wafer carries out the aqueous chemical corrosion in chemical corrosion groove, liquid chemical reagent is by the space of chip chamber and the white space of reservation, the ZnO resilient coating is corroded, when treating that the ZnO resilient coating is corroded fully, epitaxial growth substrate and LED film separate, and the LED film is stayed on the counter-rotating substrate, and epitaxial growth substrate comes off automatically, formation can be made the structure of vertical stratification LED device, and this moment, the N-N-type semiconductor N was exposed to the surface;
5) by making N-type electrode, N-type surface-texturing, surface etch, finish the making of vertical stratification LED.
2. the method for the film of a kind of light emitting diode with vertical structure according to claim 1 and substrate desquamation, it is characterized in that: the growth technique of described ZnO resilient coating (12) includes but not limited to the Organometallic Chemistry vapour phase epitaxy, molecular beam epitaxy, atomic layer epitaxy, pulsed laser deposition; ZnO resilient coating (12) finish in same growth apparatus with follow-up LED film or in advance on substrate deposit standby; The thickness of ZnO is between 0.1 micron to 100 microns.
3. the method for the film of a kind of light emitting diode with vertical structure according to claim 1 and 2 and substrate desquamation, it is characterized in that: described heat-conducting substrate is substrate moulding in advance and the good bonding metal layer of evaporation, include but not limited to Si, AlSi, Cu, CuMo, CuW, or the Heat Conduction Material that adopt to apply indefinite form or the liquid heat-conducting substrate of thermal finalization again.
4. the method for the film of a kind of light emitting diode with vertical structure according to claim 3 and substrate desquamation, it is characterized in that: described chemical reagent, include but not limited to the hydrochloric acid dilution, in room temperature or be higher than under the temperature that room temperature is lower than 100C, assisting down of ultrasonic vibration, chemical reagent flows into epitaxial wafer from the led chip trench lateral.
5. a light emitting diode with vertical structure is characterized in that: comprise
One epitaxial growth substrate (11),
One ZnO resilient coating (12) is positioned on this epitaxial growth substrate (11),
One GaN resilient coating (13) is positioned on this ZnO resilient coating (12),
One N type GaN layer (14) is positioned on the GaN resilient coating (13),
One-period property multilayer luminous zone-quantum well (15) is positioned on this N type GaN layer (14),
One electronic barrier layer (16) is positioned on this periodicity multilayer luminous zone-quantum well (15),
One P type GaN layer (17) is positioned on this electronic barrier layer (16).
6. a kind of light emitting diode with vertical structure according to claim 5, it is characterized in that: choosing of the epitaxial growth substrate of described LED includes but not limited to that sapphire, aluminium nitride, gallium nitride, silicon, carborundum, its crystal orientation include but not limited to 0001 polarization such as grade, semipolar and non-polarized direction; Selected substrate comprises patterned surface texture.
7. according to claim 5 or 6 described a kind of light emitting diode with vertical structure, it is characterized in that: described N type GaN layer is provided with N-face electrode metal layer, forms ohmic contact with N type layer semi-conducting material, for single or multi-layer metal structure, include but not limited to titanium, aluminium, gold, vanadium and its alloy.
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