金刚石(111)/Al界面形成及性能的第一性原理研究

孙士阳; 迟中波; 徐平平; 安泽宇; 张俊皓; 谭心; 任元

doi:10.7498/aps.70.20210572

摘要

针对金刚石/Al界面的形成和性能, 采用第一性原理计算方法, 研究了Al原子在H终止金刚石表面的吸附及其迁移行为, 以及金刚石/Al界面的结构与黏附功. 结果表明: Al原子吸附对金刚石原子表面结构不敏感, 且表面迁移激活能非常小, 其原因是Al与H原子间没有形成化学键, 仅有少量电荷转移, 为物理吸附; 由吸附位置生长而形成的金刚石/Al界面为亚稳结构, 不具有能量稳定性. 本文结果为理解金属纳米掩膜的形成机理提供重要的理论参考.

关键词:

Abstract

The simple and convenient metallic mask method is a significant method of preparing diamond nanostructures. The metallic mask method has poor repeatability and can not give the ideal results, because it is supported by no theory about formation of surface mental nanoparticles and its technological parameters are optimized by no experimental techniques that are expensive either. Aiming at the formation and performance of the diamond/Al interface, this paper adopts the first-principles to study the adsorption and migration behavior of Al atoms on the H-terminated diamond surface and the structure of the diamond/Al interface. The results show that the highest adsorption energy is at the T4 position, which is only 0.181 eV, through comparing the adsorption energies of Al atoms at the highly symmetrical positions (Top, Br, H3 and T4) on the surface of the H-terminated diamond (111). The adsorption energies at these different positions are similar and the maximum difference is only 0.019 eV. There is formed no chemical bond, although Al has partial charge transfer on the H-terminated surface through the analysis of differential charge density and worse layout distribution. This phenomenon can be considered as electrostatic adsorption. That is to say, the adsorption of Al atoms are physical adsorption. The smooth potential energy surface also makes it easier for Al atoms to migrate on the diamond surface. The calculation results reveal that the migration activation energies of the two possible migration paths (from T4 position to Br position and from T4 to Top position) are 0.011 eV and 0.026 eV respectively. The above results imply that the metal Al and diamond are mainly connected by weak force, so the adhesion work of the three diamond/Al interface structures is compared based on the geometric stacking structure. The results show that the adhesion work of the three interfaces is around 0. These results indicate that the stability of the diamond/Al interface is not high and the stable structure of the interface is easily destroyed when the external environment changes. This speculation can be confirmed in molecular dynamics. When the simulated temperature is 300 ℃, the liquefied metal Al obviously accumulates into spheres. According to the above research results, we deduce that the metallic mask method does not require high requirements for the relationship between the metal and the substrate material, which depends mainly on the surface topography of the base material. This research provides an important theoretical reference for understanding the formation mechanism of metal nanomasks.

Keywords:

作者及机构信息

内蒙古科技大学机械工程学院, 包头　014010

通信作者: 孙士阳, sunshy@imust.edu.cn

基金项目: 国家自然科学基金(批准号: 61765012)、内蒙古自治区自然科学基金(批准号: 2020LH08009, 2019LH05009)和内蒙古自治区高等学校科学研究项目(批准号: NJZY20099)资助的课题

Authors and contacts

School of Mechanical Engineering, Inner Mongolia University of Science and Technology, Baotou 014010, China

Corresponding author: Sun Shi-Yang, sunshy@imust.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 61765012), the Natural Science Foundation of Inner Mongolia Autonomous Region, China (Grant Nos. 2020LH08009, 2019LH05009), and the Scientific Research Foundation of the Higher Education Institutions of Inner Mongolia Autonomous Region, China (Grant No. NJZY20099)

文章全文 : translate this paragraph

参考文献

[1]	Zhou Y, Zhi J, Zou Y 2008 Anal. Chem. 80 4141 Google Scholar
[2]	Gu H, Su X D 2006 J. Phys. Chem. B 109 3611 Google Scholar
[3]	Smirnov W, Kriele A, Yang N 2010 Diamond Relat. Mater. 19 186 Google Scholar
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施引文献

图 1 H终止金刚石(111)表面模型, 其中棕色球表示C原子, 白色小球表示表面H原子　(a)模型原子分布的立体结构示意图; (b)金刚石(111)表面格点位置示意图

Fig. 1. H-Ter diamond (111) surface model: (a) Three-dimensional structure diagram of model atom distribution; (b) location of diamond (111) surface grid points. Brown spheres represent C atoms, white spheres represent surface H atoms.

下载: 全尺寸图片幻灯片

图 2 单个Al原子在H-Ter表面吸附位置及迁移路径, 其中纵坐标为插入点的能量差值

Fig. 2. Adsorption positions and migration paths of single Al atom on H-Ter surface. The ordinate is the energy difference of the insertion point.

下载: 全尺寸图片幻灯片

图 3 Al原子在Br (a), H3 (b), Top (c), T4 (d)吸附位置的电荷密度分布图, 图中银白色球为Al原子, 颜色从蓝到红表示电荷密度从高到低

Fig. 3. Charge density distribution of single Al atom adsorbed on Br (a), H3 (b), Top (c), and T4 (d) sites, respectively. The big silver ball in the picture is Al atom. The color from blue to red indicates the charge density from high to low.

下载: 全尺寸图片幻灯片

图 4 金刚石/Al界面处Al液形成过程

Fig. 4. Formation process of molten aluminum at the diamond/Al interface.

下载: 全尺寸图片幻灯片

图 5 金刚石/Al界面的PDOS图, 图中的L表示距离界面远近的C原子层数

Fig. 5. PDOS diagram of metal aluminum-diamond interface. The L indicates the lay of C atom far from the interface.

下载: 全尺寸图片幻灯片

表 1 金刚石弹性常数及弹性模量

Table 1. Elastic constants and modulus of diamond.

a/Å C₁₁/GPa C₁₂/GPa C₄₄/GPa B/GPa E/GPa G/GPa

Text value 3.523 10.311 1.104 5.464 668.621 102.606 34.821
Experimental value ^[35] 3.567 10.764 1.252 5.961 708.082 99.324 33.601

下载: 导出CSV

表 2 单个Al原子的吸附能

Table 2. Adsorption energies of a single Al atom.

Top T4 H3 Br

E_tot /eV –892.761 –892.779 –892.776 –892.775
E_ad/eV 0.162 0.181 0.176 0.177
$ {E}_{\mathrm{a}\mathrm{d}}^{{*}} $/eV 0.145 0.162 0.159 0.157

下载: 导出CSV

表 3 不同吸附结构中Al原子及其周边原子电荷转移量

Table 3. Amount of charge transfer of Al atom and its surrounding atoms in different adsorption structures.

site Element
C1/e C2/e H1/e H2/e Al/e

Br –0.022 –0.029 0.045 0.045 –0.117
H3 –0.025 –0.020 0.047 0.046 –0.138
T4 –0.026 –0.028 0.047 0.046 –0.137
Top –0.027 –0.024 0.023 0.072 –0.130

下载: 导出CSV

表 4 由吸附位置形成界面的黏附功

Table 4. Adhesion work of the interface formed by the adsorption position.

Top T4 H3

W_ad/(J·m^–2) 0.019 0.023 0.034

下载: 导出CSV

map

[1]	Zhou Y, Zhi J, Zou Y 2008 Anal. Chem. 80 4141 Google Scholar
[2]	Gu H, Su X D 2006 J. Phys. Chem. B 109 3611 Google Scholar
[3]	Smirnov W, Kriele A, Yang N 2010 Diamond Relat. Mater. 19 186 Google Scholar
[4]	Loginov P A, Zhassay U A, Bychkova M Y 2020 Int. J. Refract. Met. Hard Mater. 92 105289 Google Scholar
[5]	陆延青, 肖敏, 彭茹雯 2020 中国基础科学 22 11 Google Scholar Lu Y Q, Xiao M, Peng R W 2020 China Basic. Sci. 22 11 Google Scholar
[6]	Yu Y, Wu L, Zhi J 2015 Angew. Chem. 46 14326 Google Scholar
[7]	Zhang J, Cao J X, Chen X 2015 Phys. Rev. B 91 045417 Google Scholar
[8]	Liao M, Hishita S, Watanabe E 2010 Adv. Mater. 22 47 Google Scholar
[9]	Masuda H, Yanagishita T, Yasui K 2001 Adv. Mater. 13 247 Google Scholar
[10]	Yang N, Uetsuka H, Williams O A 2009 Phys. Status Solidi R 206 9 Google Scholar
[11]	Okuyama S, Matsushita S I, Fujishima A 2002 Langmuir 18 8282 Google Scholar
[12]	Scholze A, Schmidt W G, Kgckell P 1996 Mater. Sci. Eng., C 37 158 Google Scholar
[13]	Stampfl C, Derry T E, Makau N W 2010 J. Phys. Condens. Matter 22 475005 Google Scholar
[14]	Larsson K, Lunell S 1997 J. Phys. Chem. A 101 76 Google Scholar
[15]	Nie J L, Xiao H Y, Zu X T 2006 Chem. Phys. 326 308 Google Scholar
[16]	Hong X Y, Xu L, Gu C 2007 Appl. Surf. Sci. 253 4260 Google Scholar
[17]	于洋 2004 硕士学位论文 (长春: 吉林大学) Yu Y 2004 M. S. Thesis (Changchun: Jilin University) (in Chinese)
[18]	徐力方, 顾长志, 于洋 2004 53 2710 Google Scholar Xu L F, Gu C Z, Yu Y 2004 Acta Phys. Sin. 53 2710 Google Scholar
[19]	刘峰斌, 金秀婷, 张畅 2020 有色金属工程 10 21 Google Scholar Liu F B, Jin X T, Zhang C 2020 Nonferrous Metal Engineering. 10 21 Google Scholar
[20]	Kresse G, Furthmüller J B 1996 Comput. Mater. Sci. 6 15 Google Scholar
[21]	Blöchl P E 1994 Phys. Rev. B 50 17953 Google Scholar
[22]	Perdew J P, Burke K 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[23]	Payne M C, Teter M P, Allan D C, Arias T A, Joannopoulos J D 1992 Rev. Mod. Phys. 64 1045 Google Scholar
[24]	Methfessel M, Paxton A T 1989 Phys. Rev. B 40 3616 Google Scholar
[25]	Hendrik J, Monkhorst H J, James D P 1976 Phys. Rev. B 13 5188 Google Scholar
[26]	Maniopoulou A, Davidson E 2012 Comput. Phys. Commun. 183 1696 Google Scholar
[27]	刘峰斌, 汪家道, 陈大融 2010 59 6556 Google Scholar Liu B F, Wang J D, Chen D R 2010 Acta Phys. Sin. 59 6556 Google Scholar
[28]	Kawarada H. 1996 Surf. Sci. Rep. 26 205 Google Scholar
[29]	Siegel D J, Hector L G, Adams J B 2002 Acta Mater. 50 619 Google Scholar
[30]	Taubin G 1991 IEEE. Trans. Pattern Anal. 13 1115 Google Scholar
[31]	Almtoft K P, Ejsing A M, Bøttiger J 2007 J. Mater. Res. 22 1018 Google Scholar
[32]	Voigt W 1966 Lehrbuch der Kristallphysik (Vol. 1) (Germany: Springer Fachmedien Wiesbaden Gmbh) p3
[33]	Reuss A 1929 Appl. Math. Mech. 9 49 Google Scholar
[34]	Hill R 1952 Proc. Phys. Soc. 65 349 Google Scholar
[35]	基泰尔 1979 固体物理导论(北京: 科学出版社) 第341页 Kittel C 1979 Introduction to Solid State Physics (Beijing: Science Press) p341 (in Chinese)

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金刚石(111)/Al界面形成及性能的第一性原理研究