KR101213133B1 - ZnMgAlO thin films of UV ragne single crystalline Lattice matched to ZnO and Method for manufacturing the same - Google Patents
ZnMgAlO thin films of UV ragne single crystalline Lattice matched to ZnO and Method for manufacturing the same Download PDFInfo
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Abstract
The present invention provides a single crystal ZnMgAlO thin film for ultraviolet lattice matched with zinc oxide (ZnO), and a method for manufacturing the same, wherein a ZnO substrate is prepared, and a mixing ratio of magnesium oxide (MgO) and alumina (Al 2 O 3 ) is 5.5 to 5.7: 1. By growing a ZnMgAlO thin film on the ZnO substrate through a sputtering technique, it is possible to obtain a ZnMgAlO thin film having a high energy band gap and a lattice constant (atomic interplanar distance) that can be used in the ultraviolet region.
Description
The present invention relates to a single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO and a method for manufacturing the same, and more specifically, by adding magnesium oxide (MgO) and alumina (Al 2 O 3 ) to zinc oxide (ZnO), The present invention relates to a ZnMgAlO thin film having a matching lattice constant (atomic plane-to-atomic distance) and having a high energy band gap, that is, a single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO.
In recent years, research on optical devices has shifted to ultraviolet light emitting devices (UV LEDs), which are importantly applied to light sources, sterilization, energy-saving lighting, and the like of high density optical recording devices.
ZnO and ternary ZnMgO alloys have been studied very much for the UV light emitting device, and the energy band gap is modulated to about 4.05 eV by adding MgO to about 49 mol%.
However, ZnMgO thin film has a problem that the degree of lattice mismatch increases with increasing Mg content, which causes defects such as cracks and dislocations in the thin film, thereby adversely affecting the performance of the optoelectronic device.
That is, even in the case of ZnMgO thin film, the energy band gap can be increased, but as the Mg content increases, there is a problem in that the difference between the ZnO material and the lattice constant increases, which causes defects in the fabrication of optoelectronic devices. Cause adverse effects.
In addition, in the case of GaN-based nitride semiconductors, similar problems as described above are generated, which is the most important research in ultraviolet (UV) light emitting devices.
That is, during the growth of AlGaN thin films having a high AlN content on the GaN substrate, tensile stress due to lattice mismatch between the thin films is applied, and cracks are generated in the process of alleviating such stresses.
In addition, since Al dislocations have a high dislocation density due to lattice mismatch in AlGaN / GaN thin films, and these dislocations act as non-radiative recombination centers in the device, AlGaN thin films which are very sensitive to dislocations are used. Therefore, it is difficult to manufacture an efficient ultraviolet (UV) device having a short wavelength of 360 nm (Eg ~ 3.4) or less.
Therefore, it is important not only to develop a new material which can be used in the ultraviolet region and whose lattice constant matches ZnO or GaN material, but also to manufacture a single crystal thin film to manufacture a high efficiency ultraviolet (UV) photoelectric device.
The present invention is to solve the above problems, the object is to grow by adding magnesium oxide (MgO) and alumina (Al 2 O 3 ) to zinc oxide (ZnO), the lattice constant (atomic interplanar distance) is the same However, the present invention provides a ZnMgAlO thin film that can be used in the ultraviolet region and has a large energy band gap, that is, a single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO and a method of manufacturing the same.
In the single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO according to an aspect of the present invention for achieving the above object, the mixing ratio of the powder of magnesium oxide (MgO) and alumina (Al 2 O 3 ) on the ZnO substrate is 5.5 ~ It is characterized in that it is a thin film grown by sputtering technique using a mixed powder mixed in a ratio of 5.7: 1 as a target material.
Preferably, the component ratio of magnesium (Mg) and aluminum (Al) in the single crystal ZnMgAlO thin film is in the ratio of 2.7 to 2.9: 1.
On the other hand, according to another aspect of the present invention, the ZnO lattice matched UV single crystal ZnMgAlO thin film manufacturing method, a ZnO substrate is prepared, the mixing ratio of magnesium oxide (MgO) and alumina (Al 2 O 3 ) is 5.5 ~ 5.7: The ZnMgAlO thin film is grown on the ZnO substrate by sputtering using a mixed powder of 1 as a target material.
Preferably, the ZnMgAlO thin film is manufactured with a process pressure of 9 mTorr to 11 mTorr, a growth temperature of 580 ° C. to 620 ° C., and an RF applied power of 90 W to 110 W.
More preferably, in the single crystal ZnMgAlO thin film, the component ratio of magnesium (Mg) and aluminum (Al) is in a ratio of 2.7 to 2.9: 1.
According to the single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO according to the present invention and a method for manufacturing the same, a lattice constant (atomic) is added by growing magnesium oxide (MgO) and alumina (Al 2 O 3 ) to zinc oxide (ZnO). The ZnMgAlO thin film can be used in the ultraviolet region with the same distance between planes and has a large energy band gap.
Other objects and advantages of the present invention in addition to the above object will be apparent from the detailed description of the embodiments with reference to the accompanying drawings.
BRIEF DESCRIPTION OF THE DRAWINGS Fig. 1 shows the lattice constants and energy band gaps of Zn 1 -x- y Mg x Al y O thin films calculated by Vega's law.
Figure 2 is a view of the (a) XRD 2- theta (θ) and (b) CL spectrum of a Zn 1 -x- y Mg x Al y O thin film having a composition of Mg and Al.
FIG. 3 is a graph showing CL UV peak positions and lattice constants of ZnMgAlO and ZnMgO thin films measured in FIG. 2. FIG.
4 shows (a) CL spectrum and (b) XRD (002) locking curve of ZnMgAlO and ZnMgO thin films.
Figure 5 is a view of the (a) cross-sectional SEM image and (b) XRD 2- theta (θ) spectra of Zn 0 .78 Mg 0 .16 Al 0 .06 O / ZnO thin film.
Hereinafter, a single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO according to the present invention and a manufacturing method thereof will be described in detail with reference to the accompanying drawings.
FIG. 1 is a diagram illustrating lattice constants and energy band gap states of Zn 1 -x- y Mg x Al y O thin films calculated by Vega's law, and FIG. 2 is Zn 1 -x- y having Mg and Al compositions. (A) XRD 2-theta (theta) and (b) CL spectrum of Mg x Al y O film thin film.
3 is a diagram illustrating CL UV peak positions and lattice constants of the ZnMgAlO and ZnMgO thin films measured in FIG. 2, and FIG. 4 is (a) CL spectrum and (b) XRD (002) locking curve of ZnMgAlO and ZnMgO thin films. a view showing the Fig. 5 is a diagram illustrating the (a) cross-sectional SEM image and (b) XRD 2- theta (θ) spectra of Zn 0 .78 Mg 0 .16 Al 0 .06 O / ZnO thin film.
First, ZnMgAlO, which is a single crystal thin film for ultraviolet lattice matched to ZnO according to an aspect of the present invention, has a mixing ratio (%) of magnesium oxide (MgO) and alumina (Al 2 O 3 ) on a zinc oxide (ZnO) substrate of 5.5 to 5.7. It was prepared by growing by sputtering techniques using a mixed powder mixed so as to be in a ratio of 1: 1, preferably 5.6: 1 as a target material. Further, in magnesium oxide (MgO) and alumina (Al 2 O 3 ), the component ratio (%) of magnesium oxide (Mg) and aluminum (Al) is in a ratio of 2.7 to 2.9: 1, preferably 2.8: 1. It was prepared to be.
In this case, ZnMgAlO, which is a single crystal thin film for ultraviolet lattice matched to ZnO, may replace alumina (Al 2 O 3 ) with strontium oxide (SrO) or barium monoxide (BaO) to make the same lattice constant as ZnO.
On the other hand, according to another aspect of the present invention, a method for producing a single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO, preparing a ZnO substrate, the mixing ratio of magnesium oxide (MgO) and alumina (Al 2 O 3 ) is 5.5 ~ 5.7 It was prepared by growing (depositing) on the ZnO substrate by sputtering technique using a mixed powder having a mixing ratio of 1: 1, preferably 5.6: 1 as a target material.
At this time, when the ZnMgAlO thin film growth, the process pressure is set to 9mTorr ~ 11mTorr, the growth temperature is 580 ℃ ~ 620 ℃, RF applied power was set to 90W ~ 110W, prepared in a pure oxygen atmosphere.
Specifically, the lattice matched UV-crystalline single crystal ZnMgAlO thin film prepared according to the manufacturing method of the present invention was calculated through X-diffraction analysis (XRD) and confirmed whether the lattice constant coincided with the ZnO thin film.
In addition, the spectrum was obtained through cathodoluminescence analysis to determine the UV peak position emitted from the ZnMgAlO thin film according to the present invention.
In addition, scanning electron microscope (SEM) and atomic force microscope (AFM) were used to observe the microstructure of the ZnMgAlO thin film prepared according to the present invention, and quantitative chemical analysis was performed by electron probe micro -analyzer; EPMA).
FIG. 1 is a diagram showing the lattice constant and the state of the energy band gap of a theoretically designed Zn 1 -x- y Mg x Al y O thin film.
Lattice constant and energy band gap is law chopping guard (Vegard's rule) a was calculated using, Zn Mg 0 .81 0 .14 0 .05 O Al of Figure 1, Zn Mg 0 .62 0 .28 0 .10 Al O and Zn 0 .34 Mg 0 .56 Al 0 .20 as can be seen from O, Mg and Al is about 2.8 mixing ratio: 1 (MgO and Al 2 O 3 in a mixing ratio is also of Mg 0 .85 Al 0 1 As can be seen from .15 O, it coincides with the lattice constant of ZnO in 5.6: 1).
In this case, ZnO has a 0.3-nm interplanar spacing of the dense hexagonal structure (hcp), and a-axis interplanar spacing of Al 2 O 3 (hcp) is large at 0.476 nm. MgO is a cubic structure, and the distance between d (110) planes corresponding to the a-axis of the hcp structure is 0.298 nm.
In addition, the dotted line shown in FIG. 1 indicates a condition that the lattice match between ZnO and 5.6: 1 is the mixing ratio of MgO and Al 2 O 3 , Al 2 O 3 has an energy band gap of 7.0 eV, and MgO of 7.8 eV to be.
Therefore, it is theoretically possible to increase the energy band gap to 7.64 eV while lattice matching to ZnO (E g = 3.3 eV).
On the other hand, Figure 2 (a) shows the high-resolution X-ray diffraction (XRD) spectrum results of the ZnMgAlO thin film in which the mixing ratio of Mg and Al grown at a lattice matching ratio of approximately 2.8: 1.
For all samples, the peak corresponding to the (002) plane is observed at the same 34.42 °, which corresponds to the XRD peak position obtained in the pure ZnO thin film, which means that the lattice match with ZnO is obtained.
In addition, (b) of FIG. 2 shows cathode light emission (CL) spectra of ZnMgAlO thin films lattice matched to ZnO, and CL ultraviolet rays in a short wavelength (high energy) direction from 376 nm to 300 nm by adding MgO and Al 2 O 3. The (UV) peak was observed to shift.
On the other hand, Figure 3 summarizes the CL and XRD results of the ZnMgAlO thin film having a variety of compositions but the mixing ratio of Mg and Al is approximately 2.8: 1.
The ZnMgO thin films of FIG. 3 are shown together to compare with the lattice matched ZnMgAlO thin films.
As can be seen from FIG. 3, the quaternary ZnMgAlO thin film lattice matched to the ZnO substrate was calculated to be 0.521 nm which is very consistent with the c-axis lattice constant of the ZnO thin film, and was within ± 0.03%.
3, the position of the CL UV emission peak of the quaternary ZnMgAlO thin film is converted into energy. In FIG. 3, as the contents of MgO and Al 2 O 3 increased, the energy of the ZnMgAlO thin film increased from 376 nm (3.3 eV) to 300 nm (4.13 eV).
In addition, the energy of the CL UV peak of the ZnMgAlO thin film shown in FIG. 3 was very close to the theoretical value calculated in FIG. 1.
For example, in the case of Zn 0 .78 Mg 0 .16 Al 0 .06 O thin film, chopping the value calculated by the guard law eotneunde shows the 4.24eV, the position of the CL UV peak of 4.13eV in the case of actual thin film Had
In fact, since the position of the CL UV peak is observed slightly lower than the inherent band gap energy of the thin film, it can be said that the energy value of 4.13 eV is closer to the theoretical value of 4.24 eV. On the other hand, in the case of a ternary Zn 0 .84 Mg 0 .16 O thin film exhibited a remarkably low-3.53eV peak position than the theoretical value of 4.02eV.
In fact, it can be observed that the energy value of the ZnMgO thin film in FIG. 3 increases along the dotted line by the addition of Al 2 O 3 . In the case of the ternary ZnMgO, the reason that the energy band gap is significantly lower than the theoretical value is considered to be due to the difference in the crystal structure of ZnO (hexagonal dense structure) and MgO (square structure) and the presence of residual stress due to lattice mismatch. On the other hand. In the case of the lattice matched ZnMgAlO thin film, the energy band gap was close to the theoretical value by solving the problem occurring in the ternary system.
On the other hand, Figure 4 (a) shows the CL spectrum of the ZnMgO and ZnMgAlO thin film, the quaternary ZnMgAlO thin film has a significantly lower peak intensity in the visible region compared to the ternary ZnMgO. Peaks in the visible region are generally due to various point defects, and it can be seen that the defects are reduced in the quaternary ZnMgAlO.
Further, in Fig. 4 (b) to FIG ternary Zn 0 .84 Mg 0 .16 shows a comparison of the XRD full width at half maximum value in the locking curve O (173 arcsec) thin film than quaternary Zn 0 .78 Mg 0 .16 Al 0 . The half width value of the 06 O (97 arcsec) thin film is remarkably small. This means that the crystallinity of the ZnMgAlO thin film is very excellent, because the degree of lattice mismatch is very small and the defect density is very low.
On the other hand, Fig. 5 shows (a) cross-sectional SEM image and (b) XRD spectra of Zn 0 .78 Mg 0 .16 Al 0 .06 O / ZnO thin film.
5 shows a very flat surface shape from the SEM image of (a), which means that a high quality thin film is grown.
In addition, the surface roughness value measured by the atomic force microscope (AFM) was 0.88 nm, which was very small. In the XRD spectrum of FIG. 5B, only peaks corresponding to the (002) plane and the (004) plane were observed at 34.42 ° and the (004) plane at 72.56 °, and no peaks of other crystallographic planes were observed. This means that the single crystal thin film was grown while the ZnMgAlO thin film had the same lattice constant as the ZnO substrate. In FIG. 5 (b), no pattern other than the hexagonal dot pattern was observed in the XRD pole figure pattern, thereby demonstrating that the excellent single crystal ZnMgAlO thin film was grown.
Through the above-described experiments, a quaternary ZnMgAlO thin film lattice matched to a ZnO substrate was designed, grown, and evaluated for its properties. The XRD and CL spectra of ZnMgAlO thin films grown by sputtering show that the lattice constant and energy band gap (E g ) are very close to those calculated by Vegaard's law.
That is, the mixing ratio of MgO and Al 2 O 3 5.6: 1 (substantially the ratio of Mg and Al 2.8: 1) was from the lattice constant of the thin film matching the ZnMgAlO ZnO substrate, Zn 0 0 .78 Mg .16 Al 0. The energy band gap in the 06 O / ZnO thin film had a value of 4.2 eV.
While the present invention has been described in connection with what is presently considered to be practical exemplary embodiments, it is to be understood that the invention is not limited to the disclosed embodiments, but, on the contrary, Of course.
Claims (5)
A thin film grown on a ZnO substrate by sputtering, using a mixed powder mixed with a powder of magnesium oxide (MgO) and alumina (Al 2 O 3 ) in a ratio of 5.5 to 5.7: 1 as a target material. A single crystal ZnMgAlO thin film for UV lattice matched to ZnO.
The monocrystalline ZnMgAlO thin film for UV lattice matched to ZnO, characterized in that the ratio of magnesium (Mg) and aluminum (Al) in the single crystal ZnMgAlO thin film is a ratio of 2.7 ~ 2.9: 1.
Preparing a ZnO substrate and growing a ZnMgAlO thin film on the ZnO substrate by sputtering using a mixed powder having a mixture ratio of magnesium oxide (MgO) and alumina (Al 2 O 3 ) of 5.5 to 5.7: 1 as a target material. A method for producing a single crystal ZnMgAlO thin film for ultraviolet lattice matched to ZnO.
When the ZnMgAlO thin film is grown, the process pressure is 9mTorr ~ 11mTorr, the growth temperature is 580 ℃ ~ 620 ℃, RF applied power of 90W ~ 110W, characterized in that the lattice matched UV-crystalline single crystal ZnMgAlO thin film Manufacturing method.
The method of manufacturing a single crystal ZnMgAlO thin film for lattice matched to ZnO, characterized in that the ratio of magnesium (Mg) and aluminum (Al) in the single crystal ZnMgAlO thin film is a ratio of 2.7 ~ 2.9: 1.
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| Application Number | Priority Date | Filing Date | Title |
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| KR1020100015418A KR101213133B1 (en) | 2010-02-19 | 2010-02-19 | ZnMgAlO thin films of UV ragne single crystalline Lattice matched to ZnO and Method for manufacturing the same |
| PCT/KR2011/000981 WO2011102627A2 (en) | 2010-02-19 | 2011-02-15 | SINGLE CRYSTAL ZnMgAlO THIN FILM FOR ULTRAVIOLET RAYS, WHICH IS LATTICE MATCHED TO ZnO, AND PREPARATION METHOD THEREOF |
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| KR1020100015418A KR101213133B1 (en) | 2010-02-19 | 2010-02-19 | ZnMgAlO thin films of UV ragne single crystalline Lattice matched to ZnO and Method for manufacturing the same |
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| KR101213133B1 true KR101213133B1 (en) | 2012-12-18 |
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| JP2009263709A (en) | 2008-04-24 | 2009-11-12 | Hitachi Ltd | Sputtering target for depositing zinc oxide thin film, and display device and solar cell having zinc oxide thin film obtained by using the target, |
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| WO2008050479A1 (en) * | 2006-10-25 | 2008-05-02 | Stanley Electric Co., Ltd. | ZnO LAYER AND SEMICONDUCTOR LIGHT-EMITTING DEVICE |
| KR20080008306A (en) * | 2007-10-31 | 2008-01-23 | 주식회사 퀀텀디바이스 | The uv led with manufacturing method thereof |
| JP5019326B2 (en) * | 2008-02-23 | 2012-09-05 | シチズンホールディングス株式会社 | Method for producing MgaZn1-aO single crystal thin film |
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| JP2009263709A (en) | 2008-04-24 | 2009-11-12 | Hitachi Ltd | Sputtering target for depositing zinc oxide thin film, and display device and solar cell having zinc oxide thin film obtained by using the target, |
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| WO2011102627A3 (en) | 2011-11-24 |
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