CN102394263A - Method for enhancing electroluminescent property of n-ZnO/AlN/p-GaN light-emitting diode - Google Patents
Method for enhancing electroluminescent property of n-ZnO/AlN/p-GaN light-emitting diode Download PDFInfo
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- CN102394263A CN102394263A CN2011103735472A CN201110373547A CN102394263A CN 102394263 A CN102394263 A CN 102394263A CN 2011103735472 A CN2011103735472 A CN 2011103735472A CN 201110373547 A CN201110373547 A CN 201110373547A CN 102394263 A CN102394263 A CN 102394263A
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Abstract
The invention discloses a method for enhancing the electroluminescent property of an n-ZnO/AlN/p-GaN light-emitting diode. Through the method, a layer of Ag nano particles is inserted in the n-ZnO film of the n-ZnO/AlN/p-GaN light-emitting diode, and the electroluminescent property of the n-ZnO/AlN/p-GaN heterojunction light-emitting diode is improved by utilizing the intercoupling action of an Ag localized state surface plasmon and ZnO near band edge light-emitting intensity. An experiment demonstrates that the localized state surface plasmon resonance peak of the Ag nano particles is close to a ZnO near band edge light-emitting peak so as to meet the resonance coupling condition, and the rough surface of the Ag nano particle is in favor of effectively coupling the plasmon into light and obviously improving the extraction efficiency of light. By utilizing the method disclosed by the invention, the electroluminescent property of the n-ZnO/AlN/p-GaN heterojunction light-emitting diode is obviously improved.
Description
Technical field
The present invention relates to the semiconductor photoelectronic device technical field, particularly a kind of method that strengthens the electroluminescent properties of n-ZnO/AlN/p-GaN light-emitting diode through the metal surface phasmon.
Background technology
Why ZnO can become the active material in semiconductor material with wide forbidden band and the field of optoelectronic devices; Reason be ZnO have bigger energy gap (～3.37eV) with high exciton bind energy (～60meV); Wet chemical etching technique is easy; Can the large tracts of land epitaxial growth, with and have crystal structure and an electrical properties close with GaN.Because the self compensation effect of ZnO, it is very difficult to obtain high-quality p type ZnO material stable, good reproducibility at present, thereby has restricted the development of zno-based device greatly.In recent years, carried out number of research projects about preparation of the device of zno-based light-emitting diode (LED) and performance raising aspect people, but the electroluminescent properties of device is undesirable always.
The metal surface phasmon promptly is to be positioned near the free electron in metal surface, the collective oscillation behavior of a kind of surface electronic that under electromagnetic field effect, produces.The collective oscillation quantization that is similar to the solid lattice atoms forms phonon, and the quantization of the collective motion of metal surface free electron is known as the metal surface phasmon.The luminescence generated by light aspect people that strengthen ZnO film about the metal surface phasmon have carried out number of research projects, have also obtained a series of significant achievements.
In this article; We insert one deck Ag nano particle through the inside of ZnO in n-ZnO/AlN/p-GaN LEDs device; Utilize the luminous strong effect of intercoupling of Ag local attitude surface phasmon and the nearly band edge of ZnO, significantly improved the electroluminescence intensity of n-ZnO/AlN/p-GaN heterojunction light-emitting diode.
Summary of the invention
The technical problem that (one) will solve
High to current zno-based p-i-n light-emitting diode cut-in voltage; Luminous efficiency is low; The tangible present situation of defect luminescence, main purpose of the present invention are to provide a kind of method of utilizing the metal surface phasmon to strengthen the electroluminescent properties of n-ZnO/AlN/p-GaN light-emitting diode.
(2) technical scheme
For achieving the above object; The invention provides a kind of method of electroluminescent properties of the n-ZnO/AlN/p-GaN of enhancing light-emitting diode; This method is in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, to insert one deck Ag nano particle; Utilize the luminous strong effect of intercoupling of Ag local attitude surface phasmon and the nearly band edge of ZnO, improve n-ZnO/AlN/p-GaN heterojunction light-emitting diode electroluminescent properties.
In the such scheme, said one deck Ag nano particle that in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, inserts is realized through the dewetting method.The said dewetting method of passing through is inserted one deck Ag nano particle in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film; Comprise: at first utilize rf magnetron sputtering device high growth temperature AlN film on the p-GaN substrate; Then utilize the rf magnetron sputtering system n-ZnO film of on the AlN film, growing; Send into again and on the n-ZnO film, deposit one deck Ag film in the ion beam assisted depositing system, send into then and carry out vacuum annealing in the rf magnetron sputtering system, form the Ag nano particle.
In the such scheme, saidly on the n-ZnO film, in the step of deposition one deck Ag film, use the main ion source, adopt Ar
+Ion bombardment Ag target; Ion beam assisted depositing system plate voltage is 500-1500V; Ion beam current is 5-50mA, and the underlayer temperature during deposition Ag film is a room temperature, and the Ar gas flow is 3-10sccm (a mark condition milliliter per minute); The Ag thin film deposition time is 50-500s, and Ag film original depth is 5-50nm.
In the such scheme, said p-GaN substrate, its hole concentration is 10
17-10
18/ cm
3, hole mobility is 10-50cm
2/ Vs.Said on the p-GaN substrate high growth temperature AlN film, AlN growth for Thin Film temperature is 400-1000 ℃, working gas is that volume ratio is 1: 1 Ar and N
2Mist, pressure is 1.0Pa in the growth room, growth power is 80W, sedimentation time is 5-12min, the thickness of AlN film is 5～50nm.
In the such scheme, the said n-ZnO film of on the AlN film, growing, n-ZnO depositing of thin film temperature is 400-700 ℃, and working gas is Ar, and pressure is 1.0Pa, and growth power is 80W, and sedimentation time is 30-120min, and the thickness of n-ZnO film is 150-700nm.
In the such scheme, in the said step of carrying out vacuum annealing, the background vacuum is 1.0 * 10 before the annealing
-5Pa, annealing temperature is 100-900 ℃, annealing time is 10-60min.
In the such scheme, after the said formation Ag nano particle, also comprise: utilize rf magnetron sputtering device continued growth n-ZnO film on the Ag nano particle that forms, to cover the Ag nano particle that generates; Adopt wet etching, an AlN film on the p-GaN substrate and a side that is inserted with the n-ZnO film of one deck Ag nano particle are eroded, expose the p-GaN substrate, form table top; On remaining n-ZnO film, make electrode TiAu alloy, on the table top that forms, make electrode NiAu alloy.
(3) beneficial effect
Can find out that from technique scheme the present invention has following beneficial effect:
1, the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode provided by the invention, after inserting one deck Ag nano particle in the n-ZnO film in device, device still can keep good electric property.
2, find through experiment; The method of the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode provided by the invention; Through inserting in the n-ZnO film in device behind one deck Ag nano particle through the luminous strong effect of intercoupling of the nearly band edge of Ag local attitude surface phasmon ZnO; The electroluminescent properties of device obviously improves, and defect luminescence obviously weakens simultaneously.
3, find through experiment; The local attitude surface plasmon resonance peak position of Ag nano particle is in～410nm; Close with the position of the nearly band-edge luminescence peaks of ZnO; Satisfy the resonance coupling condition, and the surface of coarse Ag nano particle helps the extraction efficiency that phasmon effectively is coupled into light and can obviously improves light.Utilize the present invention, greatly improved the electroluminescent properties of n-ZnO/AlN/p-GaN heterojunction light-emitting diode.Device electroluminescence intensity has nearly three times raising when injection current is 6mA, and defect luminescence is obviously suppressed simultaneously.Our result provides a feasible way that solves ZnO and the low luminous efficiency of other semi-conducting material, for the development of efficient zno-based light-emitting diode is had laid a good foundation.
Description of drawings
Fig. 1 is a n-ZnO/AlN/p-GaN heterojunction light-emitting diode structure sketch map provided by the invention;
Fig. 2 is the absorption spectrum of the Ag nano particle of on quartz substrate, growing;
Fig. 3 is inserting the room temperature electroluminescent spectrum of Ag nano particle front and back when injection current is 6mA for the n-ZnO/AlN/p-GaN heterojunction light-emitting diode according to embodiment of the invention preparation.
Embodiment
For making the object of the invention, technical scheme and advantage clearer, below in conjunction with specific embodiment, and with reference to accompanying drawing, to further explain of the present invention.
As shown in Figure 1; The present invention provides the method that strengthens the electroluminescent properties of n-ZnO/AlN/p-GaN light-emitting diode through the metal surface phasmon; Be in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, to insert one deck Ag nano particle; Utilize the luminous strong effect of intercoupling of Ag local attitude surface phasmon and the nearly band edge of ZnO, improve n-ZnO/AlN/p-GaN heterojunction light-emitting diode electroluminescent properties.
Wherein, said one deck Ag nano particle that in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, inserts is realized through the dewetting method.The said dewetting method of passing through is inserted one deck Ag nano particle in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film; Comprise: at first utilize rf magnetron sputtering device high growth temperature AlN film on the p-GaN substrate; Then utilize the rf magnetron sputtering system n-ZnO film of on the AlN film, growing; Send into again and on the n-ZnO film, deposit one deck Ag film in the ion beam assisted depositing system, send into then and carry out vacuum annealing in the rf magnetron sputtering system, form the Ag nano particle.
Saidly on the n-ZnO film, in the step of deposition one deck Ag film, use the main ion source, adopt Ar
+Ion bombardment Ag target; Ion beam assisted depositing system plate voltage is 500-1500V; Ion beam current is 5-50mA, and the underlayer temperature during deposition Ag film is a room temperature, and the Ar gas flow is 3-10sccm (a mark condition milliliter per minute); The Ag thin film deposition time is 50-500s, and Ag film original depth is 5-50nm.
In order to describe the method for the present invention in further detail, describe the present invention below in conjunction with the method for preparing the n-ZnO/AlN/p-GaN light-emitting diode through the electroluminescent properties of metal surface phasmon enhancing n-ZnO/AlN/p-GaN light-emitting diode.
The present invention prepares the method for n-ZnO/AlN/p-GaN light-emitting diode, specifically comprises the steps:
Step 1, at Al
2O
3Deposition p-GaN film 20 on the substrate 10, used growth apparatus is the MOCVD system, the hole concentration of p-GaN film 20 is 10
17-10
18Cm
-3, hole mobility is 10-80cm
2/ Vs;
Step 2, on p-GaN film 20 growing AIN film 30, used growth apparatus is the rf magnetron sputtering system, comprises Sample Room, settling chamber, vacuum system, radio-frequency power supply and matching system, substrate heating and temperature-controlling system, sample rotary system etc.;
Step 3, growing AIN film 30 used working gass are that volume ratio is 1: 1 Ar and N
2Mist, the gas mixture ratio example is 1: 1, gas pressure intensity is 1.0Pa in the AlN thin film growth process, radio frequency sputtering power is 80W, underlayer temperature is 700 ℃, sputtering time is 7min, growing period sample holder rotation makes film forming even;
Step 4, on AlN film 30 deposition n-ZnO film 40, used growth apparatus is the rf magnetron sputtering system, the depositing temperature of n-ZnO film 40 is 600 ℃; Working gas is Ar; Pressure is 1.0Pa, and growth power is 80W, and sedimentation time is 10min; The thickness of ZnO film is 40nm, and electron concentration is 10
17-10
18Cm
-3, electron mobility is 5-20cm
2/ Vs;
Step 5, on n-ZnO film 40 deposition Ag film 31, used growth apparatus is the ion beam assisted depositing system, the ion beam assisted depositing system plate voltage during deposition Ag film 31 is 1000V, ion beam current is 10mA;
Underlayer temperature when step 6, deposition Ag film 31 is a room temperature, and the Ar gas flow is 3sccm (a mark condition milliliter per minute), and sedimentation time is 140s, and the original depth of Ag film 31 is 10nm;
The background vacuum of rf magnetron sputtering system is 1.0 * 10 before step 8, deposition Ag film 31 after annealings
-5Pa.Annealing temperature during deposition Ag film 31 after annealings is 600 ℃, and annealing time is 30min;
Step 9, on Ag nano particle 32 continued growth n-ZnO film 40, used growth apparatus is the rf magnetron sputtering system, the depositing temperature of n-ZnO film 40 is 600 ℃; Working gas is Ar; Pressure is 1.0Pa, and growth power is 80W, and sedimentation time is 50min; The thickness of n-ZnO film 40 is 300nm, and electron concentration is 10
17-10
18Cm
-3, electron mobility is 5-20cm
2/ Vs;
Step 11, on the table top 21 of p-GaN film 20, make p type electrode 60, the material of p type electrode 60 is the NiAu alloy, manufacturing n type electrode 50 on n-ZnO film 40, and n type electrode 50 material therefors are the TiAu alloy.
Test result and analysis
According to the process conditions that provide in the foregoing description, utilize the rf magnetron sputtering system on GaN (0001) substrate, to prepare n-ZnO/AlN/p-GaN heterojunction light-emitting diode.The sketch map of device is as shown in Figure 1, through inserting one deck Ag nano particle in the n-ZnO film in device, utilizes luminous strong the intercoupling of Ag local attitude surface phasmon and n-ZnO band edge to be used for improving the electroluminescent properties of device.
Fig. 2 is the absorption spectrum of the Ag nano particle of on quartz substrate, growing, and we can find that the position of the absworption peak of Ag is positioned near the 419nm, corresponding to the absworption peak of the local attitude phasmon of Ag nano particle.
Fig. 3 is inserting the room temperature electroluminescent spectrum of Ag nano particle front and back when injection current is 6mA for n-ZnO/AlN/p-GaN heterojunction light-emitting diode.As can be seen from the figure, the electroluminescence peak position of reference device derives from the nearly band edge recombination luminescence among the ZnO near 387nm.After in device, inserting one deck Ag nano particle in the ZnO film, the electroluminescence of device obviously strengthens, and the electroluminescence intensity of device has three times enhancing when the forward injection current is 6mA, and the defect luminescence of broad is obviously suppressed between the 500-700nm simultaneously.In addition, the obvious red shift of electroluminescence peak position (387-400nm) of device behind insertion one deck Ag nano particle in ZnO.The raising of the device internal quantum efficiency that we cause the raising of device performance owing to Ag local attitude surface phasmon and luminous strong the intercoupling of the nearly band edge of n-ZnO.
Above-described specific embodiment; The object of the invention, technical scheme and beneficial effect have been carried out further explain, and institute it should be understood that the above is merely specific embodiment of the present invention; Be not limited to the present invention; All within spirit of the present invention and principle, any modification of being made, be equal to replacement, improvement etc., all should be included within protection scope of the present invention.
Claims (9)
1. method that strengthens the electroluminescent properties of n-ZnO/AlN/p-GaN light-emitting diode; It is characterized in that; This method is in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, to insert one deck Ag nano particle; Utilize the luminous strong effect of intercoupling of Ag local attitude surface phasmon and the nearly band edge of ZnO, improve n-ZnO/AlN/p-GaN heterojunction light-emitting diode electroluminescent properties.
2. the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode according to claim 1; It is characterized in that said one deck Ag nano particle that in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, inserts is realized through the dewetting method.
3. the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode according to claim 2; It is characterized in that; The said dewetting method of passing through is inserted one deck Ag nano particle in the n-ZnO of n-ZnO/AlN/p-GaN light-emitting diode film, comprising:
At first utilize rf magnetron sputtering device high growth temperature AlN film on the p-GaN substrate; Then utilize the rf magnetron sputtering system n-ZnO film of on the AlN film, growing; Send into again and on the n-ZnO film, deposit one deck Ag film in the ion beam assisted depositing system; Send into then and carry out vacuum annealing in the rf magnetron sputtering system, form the Ag nano particle.
4. the method for the electroluminescent properties of enhancing according to claim 3 n-ZnO/AlN/p-GaN light-emitting diode is characterized in that, saidly on the n-ZnO film, in the step of deposition one deck Ag film, uses the main ion source, adopts Ar
+Ion bombardment Ag target; Ion beam assisted depositing system plate voltage is 500-1500V; Ion beam current is 5-50mA, and the underlayer temperature during deposition Ag film is a room temperature, and the Ar gas flow is 3-10sccm (a mark condition milliliter per minute); The Ag thin film deposition time is 50-500s, and Ag film original depth is 5-50nm.
5. the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode according to claim 3 is characterized in that, said p-GaN substrate, and its hole concentration is 10
17-10
18/ cm
3, hole mobility is 10-50cm
2/ Vs.
6. the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode according to claim 3; It is characterized in that; Said on the p-GaN substrate high growth temperature AlN film, AlN growth for Thin Film temperature is 400-1000 ℃, working gas is that volume ratio is 1: 1 Ar and N
2Mist, pressure is 1.0Pa in the growth room, growth power is 80W, sedimentation time is 5-12min, the thickness of AlN film is 5～50nm.
7. the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode according to claim 3 is characterized in that, the said n-ZnO film of on the AlN film, growing; N-ZnO depositing of thin film temperature is 400-700 ℃; Working gas is Ar, and pressure is 1.0Pa, and growth power is 80W; Sedimentation time is 30-120min, and the thickness of n-ZnO film is 150-700nm.
8. the method for the electroluminescent properties of enhancing according to claim 3 n-ZnO/AlN/p-GaN light-emitting diode is characterized in that, in the said step of carrying out vacuum annealing, the background vacuum is 1.0 * 10 before the annealing
-5Pa, annealing temperature is 100-900 ℃, annealing time is 10-60min.
9. the method for the electroluminescent properties of enhancing n-ZnO/AlN/p-GaN light-emitting diode according to claim 3 is characterized in that, after the said formation Ag nano particle, also comprises:
Utilize rf magnetron sputtering device continued growth n-ZnO film on the Ag nano particle that forms, to cover the Ag nano particle that generates;
Adopt wet etching, an AlN film on the p-GaN substrate and a side that is inserted with the n-ZnO film of one deck Ag nano particle are eroded, expose the p-GaN substrate, form table top;
On remaining n-ZnO film, make electrode TiAu alloy, on the table top that forms, make electrode NiAu alloy.
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| CN102623588A (en) * | 2012-03-31 | 2012-08-01 | 中国科学院半导体研究所 | Method for manufacturing epitaxial structure of gallium nitride green light-emitting diode |
| CN103866246A (en) * | 2014-01-24 | 2014-06-18 | 中国科学院长春光学精密机械与物理研究所 | Ag nano-material having ultraviolet band with hybrid quadrupole and preparation method thereof |
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| CN107425098A (en) * | 2017-07-19 | 2017-12-01 | 东南大学 | The zno-based heterojunction light-emitting diode and preparation method of pure ultra-violet light-emitting can be achieved |
| GB2580827B (en) * | 2017-10-16 | 2022-02-23 | Ibm | Heterojunction Diode having a narrow bandgap semiconductor |
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Application publication date: 20120328 |