铱衬底上异质外延单晶金刚石: 过程与机理

doi:10.15541/jim20180587

摘要/Abstract

摘要：

金刚石因其独特的物理化学性质, 在探测器、光电子器件等领域得到了广泛的应用, 单晶金刚石更是因为具有大幅度提高这些器件功能的潜力而引起了众多学者的关注。目前在铱(Ir)衬底上异质外延生长的单晶金刚石具有最大尺寸和较为优异的生长质量。本文介绍了可用于外延金刚石的不同结构的衬底以及金刚石在铱(Ir)衬底上的形核和生长过程, 重点阐述了金刚石偏压辅助形核(BEN)和外延横向生长(ELO)的机理, 以及衬底图形化形核生长技术, 指出了目前研究存在的不足, 并对金刚石异质外延理论和实验研究方向进行了展望。

关键词: 单晶金刚石, 异质外延, 偏压辅助形核, 外延横向生长, 综述

Abstract:

Due to its unique physical and chemical property, diamond is widely used in many fields such as detectors and optoelectronic devices. Many scholars’ attention is drew into single crystal diamond because of its potential to significantly increase the functionality of these devices. Presently, single crystal diamonds grown heteroepitaxially on iridium (Ir) substrates reach the largest size and an excellent growth quality. In this paper, substrates with different structures for nucleation and growth processes of epitaxial diamond are introduced. The mechanisms of diamond nucleation by Bias Enhanced Nucleation (BEN) method and growth undergoing an Epitaxial Lateral Overgrowth (ELO) process are described, including technique of Patterned Nucleation and Growth(PNG). Limitations of current study are pointed out, and the future development of heteroepitaxial theory and experiment are also forecasted in this paper.

Key words: single crystal diamond, heteroepitaxial growth, bias enhanced nucleation, epitaxial lateral overgrowth, review

中图分类号:

O782

王杨, 朱嘉琦, 扈忠波, 代兵. 铱衬底上异质外延单晶金刚石: 过程与机理[J]. 无机材料学报, 2019, 34(9): 909-917.

WANG Yang, ZHU Jia-Qi, HU Zhong-Bo, DAI Bing. Heteroepitaxial Growth of Single Crystal Diamond Films on Iridium: Procedure and Mechanism[J]. Journal of Inorganic Materials, 2019, 34(9): 909-917.

图/表 8

图1 不同衬底上异质外延生长的金刚石的表面形貌[32,33,34]

Fig. 1 Heteroepitaxial diamond growth on different substrate materials[32,33,34] (a) c-BN(001); (b) c-BN(111); (c) Al2O3(0001); (d) Ni(001); (e) Ni(111); (f) Pt(111); (g) Si(001); (h) 4H-SiC(001); (i) Ir(001)

表1 基于Ir(100)衬底的不同膜系结构上金刚石的外延质量

Table 1 Quality of diamond grown on different layer structures based on Ir(100) substrate

Bottom substrate	Structure	Thickness	Quality	Ref.
Metal oxide (MO)	MgO(100)/Ir(100)/diamond(100)	50 μm	tilt0.16°	[42, 47]
	SrTiO₃(100)/Ir(100)/diamond(100)	34 μm	tilt0.17° twist0.38°	[48]
	Al₂O₃(11ˉ20)/Ir(100)/diamond(100)	38 μm	tilt~0.30°	[49]
Si	Si(100)/MgO(100)/Ir(100)/diamond(100)	8 μm	tilt0.88° twist4.13°	[50]
	Si(100)/YSZ(100)/Ir(100)/diamond(100)	1.60 mm	tilt0.18° twist0.29°	[16, 51]
	Si(100)/SrTiO₃(100)/Ir(100)/diamond(100)	350 μm	tilt0.38° twist0.98°	[52]
	Si(100)/CaF₂(100)/Ir(100)/diamond(100)	-	tilt0.61°	[53]

表2 金刚石在Ir上形核及生长过程的实验参数[59]

Table 2 Experimental conditions for Bias Enhanced Nucleation (BEN) and growth of diamond on iridium[59]

	Nucleation process			Primary growth	Rapid growth
	H₂ cleaning	H₂/CH₄ stabilization	BEN	Primary growth	Rapid growth
CH₄/%	0(Pure H₂)	4	4	0.6	5
Pressure/(×10³, Pa)	2	2	2	2	20
Power/W	400	400	400	400	3000
Bias voltage/V	0	0	-307	0	0
Substrate temperature/℃	(600±50)	(650±50)	(700±50)	(600±50)	(880±30)
Duration/min	10	10	40-45	30	Up to 48 h

图2 施加偏压时等离子体球的形状变化[57]

Fig. 2 Changes in the shape of plasma ball after application of bias voltage[57] (a) Photograph; (b) Schematic

图3 单晶金刚石在铱(Ir)衬底上异质外延的过程示意图[16, 60-64]

Fig. 3 Procedure of single diamond eptaxial growth on Ir substrate[16, 60-64] (a) Preparation of substrate; (b) Bias Enhanced Nucleation (BEN) process; (c) Oriented growth; (d) Patterned growth; (e) Heteroepitaxial diamond MS: Megnetron Sputtering; PLD: Pulsed Laser Deposition; MBE: Molecular Beam Epitaxy

图4 利用二次电子探测器观测到的SEM照片[72] (a) BEN过程后铱衬底表面形貌; (b) BEN过程后铱衬底局部表面形貌; (c)生长过程后同一位置形貌

Fig. 4 SEM images[72] of the iridium surface after BEN treatment (a), local spots after BEN (b) and after a subsequent growth step (c)

图5 (a~g)晶粒附着生长动态过程透射电镜照片, 在最终形成相同取向并附着生长前, 颗粒I和颗粒II之间多次短暂变换取向; (h)为图(g)中界面处高分辨率透射电镜照片[77]

Fig. 5 (a-g) Sequence of TEM images showing typical dynamics of the attachment process, with surfaces of particles I and II enabling transient contact at many points and orientations before finally attaching and growing together; (h) High-resolution image of interface in (g)[77]

图6 Ir/SrTiO3(100)上外延的不同厚度金刚石薄膜[48]

Fig. 6 Heteroepitaxial diamond films on Ir/SrTiO3(100)[48] (a-c) TEM images; (d) Reduction in mosaic spreaded with increasing thickness

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