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利用可描述气-固转变的三模晶体相场模型，在原子尺度上研究了不同衬底条件下石墨烯结构的形核过程.结果表明：无论衬底存在与否，气态原子均是先聚集为无定形过渡态团簇，随着气态原子的不断堆积和固相团簇中原子位置的不断调整，过渡态团簇逐渐转变为有序的石墨烯晶核，在此过程中，五元环结构具有重要的过渡作用；石墨烯在结构匹配较好的衬底（如面心立方（face-centered cubic，FCC）结构（111）和（110））上生长时，可形成几乎没有结构缺陷单晶石墨烯岛；在无衬底或结构匹配性较差的衬底（如FCC结构（100）面）上生长时，形成的石墨烯岛结构缺陷和晶界较多，不利于高质量石墨烯的制备.Two-dimensional materials with unique and excellent physical and chemical properties have attracted much attention in recent years. Among the two-dimensional materials, graphene or grapheme-like materials with honeycomb structure can be mainly prepared by the chemical vapor deposition (CVD) method. The key of this method is to select the substrates and control the nucleation and growth process of honeycomb structures. Graphene prepared by CVD contains many structure defects and grain boundaries, which mainly arise from nucleation process. However, the nucleation mechanism of graphene prepared by CVD method is not very clear. In addition, more than ten kinds of metal substrates can be used as substrate materials in CVD methods, such as Cu and Ni, which have nearly always face-centered cubic (FCC) structures and similar functions in the preparation process. In order to better describe the nucleation of graphene and understand the influences of metal substrates, we introduce the structural order parameter into the three-mode phase-field crystal model to distinguish the low-density gas phase from condensed phases. Nucleation processes of graphene on substrates with different symmetries are studied at an atomic scale by using the three-mode phase-field crystal model, which can simulate transitions between highly correlated condensed phases and low-density vapor phases. Simulation results indicate that no matter whether there is a substrate in the nucleation process, firstly gaseous atoms gather to form amorphous transitional clusters, and then amorphous transitional clusters gradually transform into ordered graphene crystals, with continuous accumulation of new gaseous atoms and position adjustment of atoms. In the nucleation process, five membered ring structures act as a transitional function. When grown on the substrate with a good geometric match with the honeycomb lattice, such as (111) plane of FCC metals, the graphene island has small structural defects. However, when grown without a substrate or on the substrate with a bad geometric match, such as (100) plane of FCC metals, the graphene island contains many structural defects and grain boundaries, which are not conducive to the preparation of high quality graphene. Compared with the (100) crystal plane of the tetragonal cell, the (110) crystal plane of the rectangular cell is favorable for the preparation of graphene single crystals with less defects. Therefore, the appropriate metal substrate can promote the nucleation process of graphene and reduce the formation of distortions and defects during the nucleation and growth of graphene.
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Keywords:
- phase-field crystal model /
- nucleation /
- graphene /
- metal substrate
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[21] Luo Z, Kim S, Kawamoto N, Rappe A M, Johnson A T 2011 ACS Nano 5 9154
[22] Yu Q, Jauregui L A, Wu W, Colby R, Tian J, Su Z, Cao H, Liu Z, Pandey D, Wei D, Chung T F, Peng P, Guisinger N P, Stach E A, Bao J, Pei S S, Chen Y P 2011 Nat. Mater. 10 443
[23] Gao J, Yuan Q, Hu H, Zhao J, Ding F 2011 J. Phys. Chem. C 115 17695
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[25] Wang Y, Page A J, Nishimoto Y, Qian H J, Morokuma K, Irle S 2011 J. Am. Chem. Soc. 133 18837
[26] Rasool H I, Song E B, Mecklenburg M, Regan B C, Wang K L, Weiller B H, Gimzewski J K 2011 J. Am. Chem. Soc. 133 12536
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[1] Somani P R, Somani S P, Umeno M 2006 Chem. Phys. Lett. 430 56
[2] Li X, Cai W, An J, Kim S, Nah J, Yang D, Piner R, Velamakanni A, Jung I, Tutuc E, Banerjee S K, Colombo L, Ruoff R S 2009 Science 324 1312
[3] Chen H, Zhu W, Zhang Z 2010 Phys. Rev. Lett. 104 186101
[4] Wu P, Zhang W, Li Z, Yang J, Hou J G 2010 J. Chem. Phys. 133 183
[5] Loginova E, Bartelt N C, Feibelman P J, McCarty K F 2008 New J. Phys. 10 093026
[6] Loginova E, Bartelt N C, Feibelman P J, Mccarty K F 2009 New J. Phys. 11 063046
[7] Elder K R, Katakowski M, Haataja M, Grant M 2002 Phys. Rev. Lett. 88 245701
[8] Elder K R, Grant M 2004 Phys. Rev. E 70 051605
[9] Backofen R, Rtz A, Voigt A 2007 Philos. Mag. Lett. 87 813
[10] Tegze G, Tth G I, Grnsy L 2011 Phys. Rev. Lett. 106 195502
[11] Guo Y L, Wang J C, Wang Z J, Tang S, Zhou Y L 2012 Acta Phys. Sin. 61 146401 (in Chinese) [郭耀麟, 王锦程, 王志军, 唐赛, 周尧和 2012 物理学报 61 146401]
[12] Greenwood M, Provatas N, Rottler J 2010 Phys. Rev. Lett. 105 045702
[13] Greenwood M, Oforiopoku N, Rottler J, Provatas N 2011 Phys. Rev. B 84 064104
[14] Guo C, Wang J C, Li J J, Wang Z J, Tang S 2016 J. Phys. Chem. Lett. 7 5008
[15] Guo C, Wang J C, Wang Z J, Li J J, Guo Y L, Huang Y H 2016 Soft Matter 12 4666
[16] Schwalbach E J, Warren J A, Wu K A, Voorhees P W 2013 Phys. Rev. E 88 023306
[17] Mkhonta S K, Elder K R, Huang Z F 2013 Phys. Rev. Lett. 111 035501
[18] Tang S, Bakofen R, Voigt A https://tu-dresden de/mn/ math/wir/forschung/forschungsprojekte/cosima_ simulation_von_rt_cvd_text [2017-5-25]
[19] Steinhardt P J, Nelson D R, Ronchetti M 1983 Phys. Rev. B 28 784
[20] ten Wolde P R, Ruizmontero M J, Frenkel D 1995 Phys. Rev. Lett. 75 2714
[21] Luo Z, Kim S, Kawamoto N, Rappe A M, Johnson A T 2011 ACS Nano 5 9154
[22] Yu Q, Jauregui L A, Wu W, Colby R, Tian J, Su Z, Cao H, Liu Z, Pandey D, Wei D, Chung T F, Peng P, Guisinger N P, Stach E A, Bao J, Pei S S, Chen Y P 2011 Nat. Mater. 10 443
[23] Gao J, Yuan Q, Hu H, Zhao J, Ding F 2011 J. Phys. Chem. C 115 17695
[24] Gao J, Yip J, Zhao J, Yakobson B I, Ding F 2011 J. Am. Chem. Soc. 133 5009
[25] Wang Y, Page A J, Nishimoto Y, Qian H J, Morokuma K, Irle S 2011 J. Am. Chem. Soc. 133 18837
[26] Rasool H I, Song E B, Mecklenburg M, Regan B C, Wang K L, Weiller B H, Gimzewski J K 2011 J. Am. Chem. Soc. 133 12536
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