Heteroepitaxial Diamond Nucleation and Growth on Iridium: First-principle Calculation

Weihua WANG, Leining ZHANG, Feng DING, Bing DAI, Jiecai HAN, Jiaqi ZHU, Yi JIA, Yu Yang

J Inorg Mat ›› 2024, Vol. 39 ›› Issue (4) : 416-422.

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Journal of Inorganic Materials

Abbreviation (ISO4): J Inorg Mat      Editor in chief: Lidong CHEN

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J Inorg Mat ›› 2024, Vol. 39 ›› Issue (4) : 416-422. DOI: 10.15541/jim20230392
RESEARCH ARTICLE

Heteroepitaxial Diamond Nucleation and Growth on Iridium: First-principle Calculation

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Abstract

Heteroepitaxy provides an effective path for the synthesis of diamond wafers. After more than 20 years of development, the diamond nucleation and growth technology on iridium substrates has enabled to prepare crystals with a maximum diameter of 3.5 inches, which opens a door to application diamond as ultimate semiconductor in the future chip industry. However, a series of problems that occur on heterogeneous substrates, such as surface nucleation, bias process window, and diamond epitaxial growth, need to overcome from the perspective of growth thermodynamics. In this study, aiming at the key issue how diamond can achieve epitaxial nucleation and growth in chemical vapor deposition atmosphere, a simulation study was carried out on the nucleation and growth process of diamond at the atomic scale based on the first-principle calculation. The results show that the adsorption of C atoms on the surface of the Ir substrate is more stable than that on the bulk phase, which indicates that diamond nucleation can only occur on the substrate surface. The number of C atoms of sp3 hybridization in the amorphous hydrogenated carbon layer increases firstly and then decreases with the increase of ion kinetic energy under ion bombardment, confirming the existence of the ion kinetic energy or bias voltage window in the high-density nucleation of diamond. The interfacial binding energy is the lowest (about -0.58 eV/C) when diamond is epitaxially grown along the Ir substrate, meaning that the interface binding energy is the decisive thermodynamic factor for the epitaxial growth. In conclusion, this study clarifies the thermodynamic mechanism of single crystal diamond epitaxial growth under the bias-assisted ion bombardment, and points out a great significant guidance for the growth of diamond and other carbon based semiconductors.

Key words

diamond / heteroepitaxy / nucleation and growth / first-principle / binding energy

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Weihua WANG , Leining ZHANG , Feng DING , et al . Heteroepitaxial Diamond Nucleation and Growth on Iridium: First-principle Calculation[J]. Journal of Inorganic Materials. 2024, 39(4): 416-422 https://doi.org/10.15541/jim20230392

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LIFSHITZ Y, KÖHLER T H, FRAUENHEIM T H, et al. The mechanism of diamond nucleation from energetic species. Science, 2002, 297(5586): 1531.
A model for diamond nucleation by energetic species (for example, bias-enhanced nucleation) is proposed. It involves spontaneous bulk nucleation of a diamond embryo cluster in a dense, amorphous carbon hydrogenated matrix; stabilization of the cluster by favorable boundary conditions of nucleation sites and hydrogen termination; and ion bombardment-induced growth through a preferential displacement mechanism. The model is substantiated by density functional tight-binding molecular dynamics simulations and an experimental study of the structure of bias-enhanced and ion beam-nucleated films. The model is also applicable to the nucleation of other materials by energetic species, such as cubic boron nitride.

Funding

National Key R&D Program of China(2020YFA0709700)
National Key R&D Program of China(2016YFE0201600)
National Natural Science Foundation of China(52072087)
Guangdong Key Research and Development Program(2020B010169002)
Heilongjiang Natural Science Foundation(YQ2020E008)
The Fundamental Research Funds for the Central Universities(HIT.OCEF.2022048)
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