点缺陷调控: 宽禁带II族氧化物半导体的机遇与挑战

谢修华; 李炳辉; 张振中; 刘雷; 刘可为; 单崇新; 申德振

doi:10.7498/aps.68.20191043

摘要

宽禁带II族氧化物半导体材料体系, 包括氧化铍(BeO)、氧化镁(MgO)、氧化锌(ZnO)及合金, 拥有较大的激子结合能(ZnO 60 meV, MgO 80 meV), 较高的光学增益(ZnO 300 cm^–1)以及较宽的可调带隙(ZnO 3.37 eV, MgO 7.8 eV, BeO 10.6 eV), 具有实现紫外及深紫外波段低阈值激光器的独特优势, 同时也是取代传统气体放电灯(汞灯、氘灯、准分子灯、氙灯)成为深紫外乃至真空紫外光源的重要候选材料之一. 虽然经过20余年的研究历程, ZnO基pn同质结近紫外电致发光方向取得了长足进步, 但是, 随着带隙的展宽, 伴随而来的受主(施主)离化能变高(百毫电子伏特量级), 使得室温等效热能(26 meV)无法实现对杂质能级上的空穴(电子)有效离化; 此外, 掺杂过程中存在的自补偿效应也进一步弱化了载流子的产率, 以上因素已经成为了阻碍宽禁带II 族氧化物半导体实现紫外激光器件及向更短波长扩展的瓶颈性问题, 同时也是其他宽禁带半导体材料共同面对的难题. 对材料电学及发光性能的调控往往取决于对关键缺陷态的识别与控制, 丰富的点缺陷及其组合类型, 使宽禁带II族氧化物半导体成为研究缺陷物理的重要平台. 针对特定点缺陷的识别及表征将有望发现并进一步构建能级较浅的缺陷态, 为电学性能调控提供基础. 本文从高质量外延生长、杂质与点缺陷、p型掺杂及紫外电致发光三个方面阐述II族氧化物半导体近期研究结果, 通过对相关研究工作的概览, 阐明该体系作为深紫外光源材料的独特优势的同时, 指明未来针对电学性能调控的关键在于对点缺陷的调控.

关键词:

宽禁带 /
点缺陷 /
掺杂 /
离化能

Abstract

II-oxides wide-bandgap semiconductor, including the beryllium oxide (BeO), magnesium oxide (MgO), zinc oxide (ZnO), have large exciton binding energy (ZnO 60 meV, MgO 80 meV), high optical gain (ZnO 300 cm^–1) and wide tunable band gap (3.37 eV ZnO, MgO 7.8 eV, BeO 10.6 eV), which are the advantages of achieving low-threshold laser devices in the ultraviolet wavelength. It is also one of the important candidates to replace the traditional gas arc lamp (such as mercury lamp, deuterium lamp, excimer lamp, xenon lamp etc.) as the source of deep ultraviolet and even vacuum ultraviolet. Although, during the past decades, the ZnO-based pn homojunction devices have made great progress in the near-UV electroluminescence, but as the band gap broadens, the acceptor (or donor) ionization energy becomes higher (On the order of hundreds meV), which causing the room temperature equivalent thermal energy (26 meV) cannot make the impurities ionizing effectively. In addition, the self-compensation effect in the doping process further weakens the carrier yield. These above drawbacks have become the bottleneck that hinders II-oxides wide-bandgap semiconductor from achieving ultraviolet laser devices and expanding to shorter wavelengths, and are also a common problem faced by other wide-bandgap semiconductor materials. The regulation of the electrical and luminescent properties of materials often depends on the control of critical defect states. The rich point defects and their combination types make the II-oxides wide-bandgap semiconductors an important platform for studying defect physics. For the identification and characterization of specific point defects, it is expected to discover and further construct shallower defect states, which will provide a basis for the regulation of electrical performance. In this paper, recent research results of II-oxides wide-bandgap semiconductors will be described from three aspects: high-quality epitaxial growth, impurity and point defects, p-type doping and ultraviolet electroluminescence. Through the overview of related research works, II-oxides wide-bandgap semiconductors are clarified as deep ultraviolet light sources materials. Meanwhile, indicates that the key to the regulation of electrical performance in the future lies in the regulation of point defects.

Keywords:

作者及机构信息

1.
中国科学院长春光学精密机械与物理研究所, 发光学及应用国家重点实验室, 长春　130033

2.
郑州大学, 物理工程学院, 郑州　450001

通信作者: 申德振, shendz@ciomp.ac.cn

基金项目: 国家重大科研仪器设备研制专项(批准号: 11727902)和吉林省优秀青年人才基金项目(批准号: 20190103042JH)资助的课题.

Authors and contacts

1.
State Key Laboratory of Luinescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, China

2.
Zhengzhou University, School of Physics and Engineering, Zhengzhou 450001, China

Corresponding author: Shen De-Zhen, shendz@ciomp.ac.cn

Funds: Project supported by the National Key Scientific Instrument and Equipment Development Project of China (Grant No. 11727902) and the Excellent Young Scientists Fund of Jilin Province, China (Grant No. 20190103042JH).

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施引文献

图 1 ZnO外延生长过程中缓冲层的RHEED线条图像演变过程　(a)氧等离子体处理后的蓝宝石(0001)表面; (b) 二维成核阶段的MgO缓冲层表面; (c) MgO缓冲层开始三维成岛状生长; (d) 薄层低温ZnO缓冲层生长在MgO上; (e) 退火后的ZnO缓冲层表现出平整二维表面^[9]

Fig. 1. Evolution of RHEED line image of buffer layer during epitaxial growth of ZnO: (a) Oxygen plasma treated sapphire (0001) surface; (b) MgO buffer layer surface in two-dimensional nucleation stage; (c) the MgO buffer layer begins to grow into three-dimensional islands; (d) thin layer low temperature ZnO buffer layer grown on MgO; (e) annealed ZnO buffer layer exhibits a flat two-dimensional surface^[9]

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图 2 ZnO在c面蓝宝石上的原子排列示意图　(a)厚度为1 nm的MgO缓冲层; (b)厚度大于3 nm的MgO缓冲层^[14]

Fig. 2. Schematic diagram of atomic arrangement of ZnO on c-sapphire: (a) MgO buffer layer with a thickness of 1 nm; (b) MgO buffer layer with a thickness greater than 3 nm^[14]

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图 3 ZnO与GaN异质界面的STEM图像, 通过Zn束流保护, 获得了清晰陡峭的界面, 保证了外延层的Zn极性均一^[17]

Fig. 3. The STEM image of the hetero interface between ZnO and GaN, and it is protected by Zn beam, which obtains a clear and sharp interface and ensures uniformity of Zn polarity in the epitaxial layer^[17]

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图 4 N掺杂MgZnO薄膜原子力图像, 粗糙度为0.72 nm^[29]

Fig. 4. Atomic force image of N-doped MgZnO film with roughness of 0.72 nm^[29]

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图 5 II族氧化物半导体带隙与晶格常数关系

Fig. 5. Relationship between band gap and lattice constant of group II oxide semiconductors.

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图 6 (a), (b)二维电子气系统中应变层应力类型与压电极化方向; (c) BeMgZnO体系下应变类型随组分比例的变化情况^[56]

Fig. 6. (a), (b) Strain stress type and piezoelectric polarization direction in two-dimensional electron gas system; (c) variation of strain type with composition ratio in BeMgZnO system^[56]

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图 7 ZnO薄膜中杂质浓度的深度分布情况　(a)非故意掺杂层中Si, Mo, Ta, Al的分布情况; (b)氮掺杂层中C, B, N, Cl, F的分布情况; (c) 施主型杂质元素经抑制后的纵向分布情况^[79]

Fig. 7. Depth distribution of impurity concentration in ZnO thin films: (a) Distribution of Si, Mo, Ta and Al in unintentionally doped layers; (b) longitudinal distribution of donor-type impurity elements after suppression^[79]

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图 8 ZnO单晶衬底上外延层中杂质元素的SIMS数据^[80]

Fig. 8. SIMS data of impurity elements in epitaxial layers on ZnO single crystal substrates^[80]

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图 9 极性面ZnO单晶衬底在氧环境下经1150 ℃退火1h前后, 杂质种类及含量变化情况^[23]

Fig. 9. Changes in impurity types and contents of O-polar ZnO single crystal substrate after annealing at 1150 ℃ for 1 hour in an oxygen atmosphere^[23]

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图 10 (a)稀盐酸刻蚀后的ZnO单晶Zn极性表面; (b)稀盐酸刻蚀前后, Si元素的深度分布^[81,82]

Fig. 10. (a) Zn polar surface of ZnO single crystal after being etched by dilute hydrochloric acid; (b) depth distribution of Si element before and after being etched dilute hydrochloric acid^[81,82]

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图 11 沿极性表面外延时, Zn极性与O极性表面极化电荷分布情况以及利用光生非平衡载流子构建Zn极性表面层富电子环境^[17]

Fig. 11. Zn polar and O polar surface polarized charge distribution along epitaxial surface and Zn polar surface layer rich electronic environment using photogenerated unbalanced carriers^[17]

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图 12 Zn极性表面(2 × 2) + V_Zn重构的STM图像及结构示意图^[105]

Fig. 12. STM image and structure diagram of Zn polar surface (2 × 2) + V_Zn reconstruction^[105]

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map

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