锂氮共掺杂ρ型氧化锌基薄膜制备及其发光器件研究
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摘要
ZnO是直接带隙II-VI族化合物，具有宽的禁带宽度，高的激子结合能，环境友好，原料丰富等优势，作为一种新型的光电半导体材料而备受关注。自从ZnO的室温光泵浦紫外受激发射被发现后，ZnO在紫外发光器件、低阈值激光器件、紫外探测器件等方面展现出巨大的应用潜力。然而p型掺杂是制约ZnO在光电领域应用面临的瓶颈问题，也是一个国际性难题。本论文针对制约ZnO发展的瓶颈性问题展开研究，取得的主要成果如下：
1.利用等离子体辅助分子束外延技术，在蓝宝石衬底上采用高温缓冲层的方法，制备了背景电子浓度约为1.5×10~(16)cm~(-3)的高质量的非故意掺杂ZnO薄膜，其比直接生长在蓝宝石上的ZnO薄膜降低了两个量级以上，与国际上报道的最好的结果（1×10~(16)cm~(-3)）相差无几。
2.在获得高质量非故意掺杂ZnO薄膜的基础上，通过光刻工艺构建了MSM插指结构的紫外探测器件，在8V偏压下此器件的响应度达到26000A/W，增益达到9×10~4，这是ZnO基紫外探测器目前已报道的最大的响应度和增益之一。
3.通过Li-N双受主共掺杂的方法，制备了p-MgZnO:(Li,N)薄膜，并构建了p-MgZnO:(Li,N)/n-ZnO单异质结结构的发光器件，实现了可持续工作的ZnO基发光器件，目前器件的连续工作时间已达97小时，这是ZnO基发光器件连续工作的首次报道，说明获得的p型ZnO具有良好的稳定性。
4.为了获得更短波长的发光器件，制备了p-Mg_(0.35)Zn_(0.65)O:(Li,N)/n-Mg_(0.20)Zn_(0.80)的MgZnO基异质结发光器件，实现了室温下的位于355nm的电致发光，据知这是首次报道MgZnO异质结发光器件及ZnO基发光器件的最短波长之一。
Zinc oxide (ZnO) has recently been considered as a potential candidate forshort-wavelength optoelectronic devices such as light-emitting devices (LEDs) andlaser diodes (LDs) for its large band gap of3.37eV and large exciton binding energyof60meV. However, the ZnO-based optoelectronic devices applications aredrastically hindered by the difficulties in realizing reliable and reproducible p-typeZnO. This work foucs on the aforementioned problems, the main results wereobtained as follows:
1. Obtaining high quality ZnO films with relatively low residual electronconcentration is a fundamental step towards efficient p-type doping and futureapplications in optoelectronic devices of ZnO. A route to high quality ZnO filmswith low electron concentration has been obtained by introducing a thin hightemperature ZnO buffer layer in a plasma-assissted molecular beam epitaxy(MBE). The residual electron concentration in the films is about1.5×10~(16)cm~(-3),which is comparable with the best value reported (1×10~(16)cm~(-3)).
2. High responsivity ultraviolet photodetector has been demonstrated based onZnO film. A responsivity of26000A/W has been achieved at8V bias, which isthe highest responsivity ever reported in a semiconductor based UV photodetector. The high responsivity has been attributed to the carrier-trappingprocess at the metal/semiconductor interface, which has been confirmed by theasymmetric barrier height at the two sides of the Au/ZnO interdigital electrodes.
3. Based on realization of high quality ZnO films with low electron concetration,Li-N condoping has been employed as the dual-acceptor dopant for the p-typedoping of MgZnO, and p-MgZnO:(Li,N)/n-ZnO single heterostructures have beenconstructed. Obvious near-band-edge (NBE) excitonic emissions coming fromZnO have been observed from the structures at room temperature, and the devicescan work continuously for about6.8h in air ambient under the injection of acontinuous current of20mA. By optimizing the structure, the LEDs can workcontinuously for about97hours, revealing the good reliability of the p-typeZnO-based films obtained by using the Li-N codoping method.
4. MgZnO-based heterostructured LEDs have been realized fromp-Mg_(0.35)Zn_(0.65)O:(Li,N)/n-Mg_(0.20)Zn_(0.80)O structure. Obvious emission peaked ataround355nm has been observed from the heterostructure, which can beattributed to the near-band-edge emission of the n-type Mg_(0.20)Zn_(0.80)O layer. Theresults reported in this paper may promise short UV or even deep ultravioletLEDs from MgZnO-based materials.
1.利用等离子体辅助分子束外延技术，在蓝宝石衬底上采用高温缓冲层的方法，制备了背景电子浓度约为1.5×10~(16)cm~(-3)的高质量的非故意掺杂ZnO薄膜，其比直接生长在蓝宝石上的ZnO薄膜降低了两个量级以上，与国际上报道的最好的结果（1×10~(16)cm~(-3)）相差无几。
2.在获得高质量非故意掺杂ZnO薄膜的基础上，通过光刻工艺构建了MSM插指结构的紫外探测器件，在8V偏压下此器件的响应度达到26000A/W，增益达到9×10~4，这是ZnO基紫外探测器目前已报道的最大的响应度和增益之一。
3.通过Li-N双受主共掺杂的方法，制备了p-MgZnO:(Li,N)薄膜，并构建了p-MgZnO:(Li,N)/n-ZnO单异质结结构的发光器件，实现了可持续工作的ZnO基发光器件，目前器件的连续工作时间已达97小时，这是ZnO基发光器件连续工作的首次报道，说明获得的p型ZnO具有良好的稳定性。
4.为了获得更短波长的发光器件，制备了p-Mg_(0.35)Zn_(0.65)O:(Li,N)/n-Mg_(0.20)Zn_(0.80)的MgZnO基异质结发光器件，实现了室温下的位于355nm的电致发光，据知这是首次报道MgZnO异质结发光器件及ZnO基发光器件的最短波长之一。
Zinc oxide (ZnO) has recently been considered as a potential candidate forshort-wavelength optoelectronic devices such as light-emitting devices (LEDs) andlaser diodes (LDs) for its large band gap of3.37eV and large exciton binding energyof60meV. However, the ZnO-based optoelectronic devices applications aredrastically hindered by the difficulties in realizing reliable and reproducible p-typeZnO. This work foucs on the aforementioned problems, the main results wereobtained as follows:
1. Obtaining high quality ZnO films with relatively low residual electronconcentration is a fundamental step towards efficient p-type doping and futureapplications in optoelectronic devices of ZnO. A route to high quality ZnO filmswith low electron concentration has been obtained by introducing a thin hightemperature ZnO buffer layer in a plasma-assissted molecular beam epitaxy(MBE). The residual electron concentration in the films is about1.5×10~(16)cm~(-3),which is comparable with the best value reported (1×10~(16)cm~(-3)).
2. High responsivity ultraviolet photodetector has been demonstrated based onZnO film. A responsivity of26000A/W has been achieved at8V bias, which isthe highest responsivity ever reported in a semiconductor based UV photodetector. The high responsivity has been attributed to the carrier-trappingprocess at the metal/semiconductor interface, which has been confirmed by theasymmetric barrier height at the two sides of the Au/ZnO interdigital electrodes.
3. Based on realization of high quality ZnO films with low electron concetration,Li-N condoping has been employed as the dual-acceptor dopant for the p-typedoping of MgZnO, and p-MgZnO:(Li,N)/n-ZnO single heterostructures have beenconstructed. Obvious near-band-edge (NBE) excitonic emissions coming fromZnO have been observed from the structures at room temperature, and the devicescan work continuously for about6.8h in air ambient under the injection of acontinuous current of20mA. By optimizing the structure, the LEDs can workcontinuously for about97hours, revealing the good reliability of the p-typeZnO-based films obtained by using the Li-N codoping method.
4. MgZnO-based heterostructured LEDs have been realized fromp-Mg_(0.35)Zn_(0.65)O:(Li,N)/n-Mg_(0.20)Zn_(0.80)O structure. Obvious emission peaked ataround355nm has been observed from the heterostructure, which can beattributed to the near-band-edge emission of the n-type Mg_(0.20)Zn_(0.80)O layer. Theresults reported in this paper may promise short UV or even deep ultravioletLEDs from MgZnO-based materials.
引文
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