气相沉积技术在原子制造领域的发展与应用

郭秦敏; 秦志辉

doi:10.7498/aps.70.20201436

摘要

随着未来信息器件朝着更小尺寸、更低功耗和更高性能方向的发展, 构建器件的材料尺寸将进一步缩小. 传统的“自上而下”技术在信息器件发展到纳米量级时遇到瓶颈, 而气相沉积技术由于其能在原子尺度构筑纳米结构引起极大关注, 被认为是最有潜力突破现有制造极限进而在原子尺度构造、搭建物质形态的“自下而上”方法. 本文重点讨论适用于低维材料的原子尺度制造的分子束外延技术和原子层沉积/刻蚀技术. 简要介绍相关技术中蕴含的科学原理及其在纳米信息器件加工和制造领域的应用, 并探讨如何在原子尺度实现对低维功能材料厚度和微观形貌的精密控制.

关键词:

Abstract

With the development of future information devices towards smaller size, lower power consumption and higher performance, the size of materials used to build devices will be further reduced. Traditional “top-down” technology has encountered a bottleneck in the development of information devices on a nanoscale, while the vapor deposition technology has attracted great attention due to its ability to construct nanostructures on an atomic scale, and is considered to have the most potential to break through the existing manufacturing limits and build nano-structures directly with atoms as a “bottom-up” method. During molecular beam epitaxy, atoms and molecules of materials are deposited on the surface in an “atomic spray painting” way. By such a method, some graphene-like two-dimensional materials (e.g., silicene, germanene, stanene, borophene) have been fabricated with high quality and show many novel electronic properties, and the ultrathin films (several atomic layers) of other materials have been grown to achieve certain purposes, such as NaCl ultrathin layers for decoupling the interaction of metal substrate with the adsorbate. In an atomic layer deposition process, which can be regarded as a special modification of chemical vapor deposition, the film growth takes place in a cyclic manner. The self- limited chemical reactions are employed to insure that only one monolayer of precursor (A) molecules is adsorbed on the surface, and the subsequent self- limited reaction with the other precursor (B) allows only one monolayer of AB materials to be built. And the self- assembled monolayers composed of usually long- chain molecules can be introduced as the active or inactive layer for area- selective atomic layer deposition growth, which is very useful in fabricating nano- patterned structures. As the reverse process of atomic layer deposition, atomic-layer etching processes can remove certain materials in atomic precision. In this paper we briefly introduce the principles of the related technologies and their applications in the field of nano- electronic device processing and manufacturing, and find how to realize the precise control of the thickness and microstructure of functional materials on an atomic scale.

Keywords:

作者及机构信息

郭秦敏¹,
秦志辉²

1.
武汉科技大学, 省部共建耐火材料与冶金国家重点实验室, 武汉　430081

2.
湖南大学物理与微电子科学学院, 微纳光电器件及应用教育部重点实验室, 长沙　410082

通信作者: 秦志辉, zhqin@hnu.edu.cn

基金项目: 国家自然科学基金(批准号: 51772087)和中国科学院战略性先导科技专项(B类)(批准号: XDB30000000)资助的课题

Authors and contacts

Guo Qin-Min¹,
Qin Zhi-Hui²

1.
State Key Laboratory of Refractories and Metallurgy, Wuhan University of Science and Technology, Wuhan 430081, China

2.
Key Laboratory for Micro/Nano Optoelectronic Devices of Ministry of Education, School of Physics and Electronics, Hunan University, Changsha 410082, China

Corresponding author: Qin Zhi-Hui, zhqin@hnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51772087) and the Strategic Priority Research Program (B) of Chinese Academy of Sciences (Grant No. XDB30000000)

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施引文献

图 1 MBE系统结构示意图

Fig. 1. Schematic diagram of MBE system.

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图 2 RHEED系统示意图和漫反射现象随着薄膜生长的关系示意图

Fig. 2. Schematic diagram of RHEED, and the relationship between diffuse reflection and film coverage during growth.

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图 3 (a) Pt(111)表面锗烯的理论计算结构; (b)−(g) 不同位置的Ge原子对以及Ge单原子与最近邻基底Pt原子间电子局域函数的计算模拟; (h)−(j) 锗烯的实验结果(LEED, STM图像及表观高度)^[37]

Fig. 3. (a) Theoretical model of germanene on Pt (111) surface, and the electron localization functions of the cross-sections between the germanium pairs (b)−(f) and between one germanium atom and its nearest Pt neighbor (g). (h)−(j) The experimental results of LEED pattern, STM image and the apparent height along the indicated line in the STM image, respectively^[37].

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图 4 (a) Cu(111)表面制备的锗烯; (b), (c) Cu(111)基底和锗烯的原子分辨图像; (d) 双层锗烯的吸附结构模型; (e) 相应的STM图像模拟, 与实验结果(c)吻合; (f) 单层(红色)和双层(黑色)锗烯的电子结构(STS谱), 插图为Cu(111)基底STS谱用于标定针尖状态^[38]

Fig. 4. (a) STM image of germanene on Cu(111); (b), (c) the atomic-resolved STM images of Cu (111) substrate and germanene, respectively; (d) the adsorption model of bilayer germanene; (e) the simulated STM image with the features fitting very well with the experimental observations; (f) the STS of monolayer (red) and bilayer (black) germanene, and inset is STS taken on the bare Cu(111) to verify the condition of the tip^[38].

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图 5 (a)−(c) 在Cu(111)表面MBE生长的不同取向的硒化铜蜂窝状结构的STM图像; (d) 用于标定针尖状态的Cu(111)表面标准STS谱; (e) CuSe结构的STS谱^[52]

Fig. 5. (a)−(c) The STM images of honeycomb structures with equivalent orientations on Cu(111) by means of MBE growth; (d) the standard STS of Cu(111) for checking tip status; (e) electronic structure (STS) of CuSe structures^[52].

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图 6 (a) 在Cu(100)上外延生长的NaCl薄膜^[36], 以及在其上的CoPc分子轨道的实验(b)和理论(c)图像^[53]

Fig. 6. (a) MBE growth of NaCl layers on Cu(100)^[36], on top of which the quasi-free molecular orbital of adsorbed CoPc can be observed. (b) and (c) are the STM image and theoretical simulation of molecular orbital, respectively^[53].

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图 7 两种主要的石墨烯的CVD生长机制^[75]　(a) 偏析机制; (b) 表面化学反应机制

Fig. 7. Two main mechanisms of CVD growth of graphene^[75] (a) Segregation mechanism; (b) surface reaction mechanism.

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图 8 原子层沉积系统示意图

Fig. 8. Schematic diagram of atomic layer deposition system.

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图 9 Al₂O₃层的ALD制备过程^[76]

Fig. 9. The ALD process of Al₂O₃^[76].

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图 10 (a) ALD与其他方式镀膜效果比较; (b) 在深高宽比Si结构上原子沉积Cu₂S薄膜的SEM照片^[120]

Fig. 10. (a) The coating effects of ALD and other methods; (b) cross-sectional SEM images of ALD Cu₂S film on silicon trench structure^[120].

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图 11 气体前驱体暴露量和沉积温度对原子层沉积镀膜速率的影响

Fig. 11. Effects of gaseous precursor exposure and deposition temperature on deposition rate of atomic layers.

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图 12 在SiO₂/H-Si表面选区ALD沉积High-k氧化铪制作MOSFET原型^[121]

Fig. 12. The area-selective ALD of high-k hafnium oxide on SiO₂/H-Si surface to fabricate MOSFET prototype.^[121]

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图 13 (a) 左边选区ALD的原理示意图, 右边为自组装钝化层的单体分子结构; (b) 自组装薄膜的缺陷(pinhole)影响ALD沉积过程的选择性; (c) 自组装分子的光聚合官能团(二炔基)在光诱导下聚合有效抑制缺陷产生; (d) 通过选区ALD沉积ZnO掩膜刻蚀后的微结构, 结构最窄宽度约为15 nm^[101]

Fig. 13. (a) Schematic diagram of area-selective ALD growth (left), and the monomer molecular structures forming inactive SAMs (right); (b) the pinhole defect affects the selectivity of ALD deposition; (c) photopolymeric functional groups (diacetylenyl) of SAMs can effectively inhibit defect formation in terms of photo-induced polymerization; (d) SEM micrograph of the microstructure obtained by etching with ZnO mask of area-selective ALD, and the width of narrowest structure reaches 15 nm^[101].

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图 14 ALE和ALD过程对比示意图^[132]

Fig. 14. Schematic diagram of ALE process compared with ALD^[132].

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图 15 双层石墨烯ALE刻蚀前后的光学显微图像(a), (b)以及相应的AFM图像(c), (d)和在各位点的拉曼谱(e)^[136]

Fig. 15. Optical microscopic images (a), (b) and AFM images (c), (d) of bilayer graphene before and after one cycle of ALE etching. (e) Raman spectrum of graphene taken at twelve points indicated in (a), (b) before and after etching^[136].

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图 16 单层石墨烯经过一个循环的ALE刻蚀前后的拉曼光谱^[136]

Fig. 16. Raman spectrum of monolayer graphene before and after one cycle of ALE^[136].

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图 17 (a)−(f) 经过PS纳米球掩膜的石墨烯加工过程; (g) 铜箔表面具有纳米模板的石墨烯^[142]

Fig. 17. (a)−(f) The growth and etching processes of graphene via PS nanoparticle mask; (g) the nano-patterned template graphene on Cu foil^[142].

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气相沉积技术在原子制造领域的发展与应用