高温退火Cu (111)衬底上生长高质量厘米尺寸单晶石墨烯

人工晶体学报 ›› 2023, Vol. 52 ›› Issue (11): 1980-1988.

高温退火Cu (111)衬底上生长高质量厘米尺寸单晶石墨烯

祁建海^1,2, 陈洋^1,2, 岳圆圆³, 吕炳辰^1,2, 程宇昂^1,2, 朱凤前^1,2, 贾玉萍^1,2, 李绍娟^1,2, 孙晓娟^1,2, 黎大兵^1,2

1.中国科学院长春光学精密机械与物理研究所,发光及应用国家重点实验室,长春 130033;
2.中国科学院大学,材料科学与光电工程中心,北京 100049;
3.吉林财经大学管理科学与信息工程学院,长春 130117

收稿日期:2023-04-13 出版日期:2023-11-15 发布日期:2023-11-17

Growth of High-Quality Centimeter-Size Single-Crystal Graphene on High-Temperature Annealed Cu (111) Substrate

QI Jianhai^1,2, CHEN Yang^1,2, YUE Yuanyuan³, LYU Bingchen^1,2, CHENG Yuang^1,2, ZHU Fengqian^1,2, JIA Yuping^1,2, LI Shaojuan^1,2, SUN Xiaojuan^1,2, LI Dabing^1,2

1. State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, China;
2. Center of Materials Science and Optoelectronics Engineering, University of the Chinese Academy of Sciences, Beijing 100049, China;
3. School of Management Science and Information Engineering, Jilin University of Finance and Economics, Changchun 130117, China

Received:2023-04-13 Online:2023-11-15 Published:2023-11-17
Contact: CHEN Yang, associate researcher. E-mail: cheny@ciomp.ac.cn;SUN Xiaojuan, researcher. E-mail: sunxj@ciomp.ac.cn
About author:QI Jianhai (1995—), male, from Jiangsu Province, master. E-mail: 2603591798@qq.com
Supported by:
National Key R&D Program of China (2021YFB3601600); National Natural Science Foundation of China (61827813, 52002368, 62121005, 62074147, 62022081, 61974099); Natural Science Foundation of Jilin Province (20230101345JC, 20230101107JC, 20230508132RC); Youth Innovation Promotion Association of the Chinese Academy of Sciences (Y201945, 2019222)

摘要/Abstract

摘要： 二维(2D)石墨烯具有原子层厚度,在电子器件中展示出突破摩尔定律限制的巨大潜力。目前,化学气相沉积(CVD)是一种广泛应用于石墨烯生长的方法,满足低成本、大面积生产和易于控制层数的需求。然而,由于催化金属(例如Cu)衬底一般为多晶特性,导致CVD法生长的石墨烯晶体质量相对较差。为此,通过高温退火工艺制备了Cu (111)单晶衬底,使石墨烯的初始成核过程得到了很好的控制,从而实现了厘米尺寸的高质量单晶石墨烯的制备。根据二者的晶格匹配关系,Cu (111)衬底为石墨烯生长提供了唯一的成核取向,相邻石墨烯成核岛的边界能够缝合到一起。单晶石墨烯具有高电导率,相较于原始多晶Cu上生长的石墨烯(1 415.7 Ω·sq^-1),其平均薄层电阻低至607.5 Ω·sq^-1。高温退火能够清洁铜箔,从而获得表面粗糙度较低的洁净石墨烯。将石墨烯用于场效应晶体管(FET),器件的最大开关比为145.5,载流子迁移率为2.31×10³ cm²·V^-1·s^-1。基于以上结果,相信本工作中的单晶石墨烯还满足其他高性能电子器件的制备。

关键词: Cu (111), 石墨烯, 高温退火, 化学气相沉积, 场效应晶体管

Abstract: Two-dimensional (2D) graphene has shown great potential of breakthrough of Moore's law limitation due to its atomic thickness in electronic devices. Up to now, chemical vapor deposition (CVD) is a widely applied method for graphene growth due to its low-cost, large-area production, and easy control in layer number. However, the CVD-grown graphene usually suffers from relatively low quality derived from the polycrystalline nature of catalytic metal (e.g., Cu) substrates. Herein, single-crystal Cu (111) substrates were fabricated by a high-temperature annealing process, initial nucleation of graphene on it has been well controlled, and high-quality and centimeter-size single-crystal graphene was achieved. The Cu (111) substrate provides onefold orientation for the graphene growth according to their lattice matching relation, and domain boundaries of neighboring graphene nuclei could stitch together. The as-grown single-crystal graphene has an average sheet resistance of 607.5 Ω · sq^-1. Compared to that of grown on the pristine polycrystalline Cu (1 415.7 Ω · sq^-1), it shows high electrical conductivity. High-temperature annealing purified the Cu foils, and induced a clean graphene surface with lower roughness. The quality of graphene is further verified by using it in a field-effect transistor (FET), resulting in a maximum switch ratio of 145.5 and carrier mobility of 2.31×10³ cm² · V^-1 · s^-1. Based on these results, we believe that the single-crystal graphene in present work is also feasible for fabricating other high-performance electronic devices.

Key words: Cu (111), graphene, high-temperature annealing, chemical vapor deposition, field-effect transistor

中图分类号:

O782⁺.7

祁建海, 陈洋, 岳圆圆, 吕炳辰, 程宇昂, 朱凤前, 贾玉萍, 李绍娟, 孙晓娟, 黎大兵. 高温退火Cu (111)衬底上生长高质量厘米尺寸单晶石墨烯[J]. 人工晶体学报, 2023, 52(11): 1980-1988.

QI Jianhai, CHEN Yang, YUE Yuanyuan, LYU Bingchen, CHENG Yuang, ZHU Fengqian, JIA Yuping, LI Shaojuan, SUN Xiaojuan, LI Dabing. Growth of High-Quality Centimeter-Size Single-Crystal Graphene on High-Temperature Annealed Cu (111) Substrate[J]. JOURNAL OF SYNTHETIC CRYSTALS, 2023, 52(11): 1980-1988.

参考文献

[1] NOVOSELOV K S, GEIM A K, MOROZOV S V, et al. Electric field effect in atomically thin carbon films[J]. Science, 2004, 306(5696): 666-669.
[2] LIU F, MING P B, LI J. Ab initio calculation of ideal strength and phonon instability of graphene under tension[J]. Physical Review B, 2007, 76(6): 064120.
[3] MOROZOV S V, NOVOSELOV K S, KATSNELSON M I, et al. Giant intrinsic carrier mobilities in graphene and its bilayer[J]. Physical Review Letters, 2008, 100(1): 016602.
[4] NOVOSELOV K S, FAL'KO V I, COLOMBO L, et al. A roadmap for graphene[J]. Nature, 2012, 490(7419): 192-200.
[5] GEIM A K. Nobel lecture: random walk to graphene[J]. Reviews of Modern Physics, 2011, 83(3): 851-862.
[6] NOVOSELOV K S. Graphene: materials in the Flatland (Nobel lecture)[J]. Angewandte Chemie, 2011, 50(31): 6986-7002.
[7] NOVOSELOV K S, JIANG D, SCHEDIN F, et al. Two-dimensional atomic crystals[J]. Proceedings of the National Academy of Sciences of the United States of America, 2005, 102(30): 10451-10453.
[8] BLAKE P, BRIMICOMBE P D, NAIR R R, et al. Graphene-based liquid crystal device[J]. Nano Letters, 2008, 8(6): 1704-1708.
[9] HERNANDEZ Y, NICOLOSI V, LOTYA M, et al. High-yield production of graphene by liquid-phase exfoliation of graphite[J]. Nature Nanotechnology, 2008, 3(9): 563-568.
[10] COLEMAN J N, LOTYA M, O'NEILL A, et al. Two-dimensional nanosheets produced by liquid exfoliation of layered materials[J]. Science, 2011, 331(6017): 568-571.
[11] LI M, ZHOU S S, WANG R Y, et al. In situ formed nanoparticle-assisted growth of large-size single crystalline h-BN on copper[J]. Nanoscale, 2018, 10(37): 17865-17872.
[12] LI X S, CAI W W, AN J, et al. Large-area synthesis of high-quality and uniform graphene films on copper foils[J]. Science, 2009, 324(5932): 1312-1314.
[13] BAE S, KIM H, LEE Y, et al. Roll-to-roll production of 30-inch graphene films for transparent electrodes[J]. Nature Nanotechnology, 2010, 5(8): 574-578.
[14] WU Y P, CHOU H, JI H X, et al. Growth mechanism and controlled synthesis of AB-stacked bilayer graphene on Cu-Ni alloy foils[J]. ACS Nano, 2012, 6(9): 7731-7738.
[15] RUT'KOV E V, AFANAS'EVA E Y, PETROV V N, et al. Fabrication of graphene and graphite films on the Ni(111) surface[J]. Technical Physics, 2016, 61(11): 1724-1728.
[16] SUN J, NAM Y, LINDVALL N, et al. Growth mechanism of graphene on platinum: surface catalysis and carbon segregation[J]. Applied Physics Letters, 2014, 104(15): 152107.
[17] WANG Q, WEI L, SULLIVAN M, et al. Graphene layers on Cu and Ni (111) surfaces in layer controlled graphene growth[J]. RSC Advances, 2013, 3(9): 3046-3053.
[18] YANG S Y, ZHANG J X, CHI M Y, et al. Excellent superelasticity of Cu-Al-Mn-Cr shape memory single crystal obtained only through annealing cast polycrystalline alloy[J]. Scripta Materialia, 2019, 165: 20-24.
[19] JIN S, HUANG M, KWON Y, et al. Colossal grain growth yields single-crystal metal foils by contact-free annealing[J]. Science, 2018, 362(6418): 1021-1025.
[20] WU M H, ZHANG Z B, XU X Z, et al. Seeded growth of large single-crystal copper foils with high-index facets[J]. Nature, 2020, 581(7809): 406-410.
[21] LI L, MA T, YU W, et al. Fast growth of centimeter-scale single-crystal copper foils with high-index planes by the edge-incision effect[J]. 2D Materials, 2021, 8(3): 035019.
[22] XU X Z, ZHANG Z H, DONG J C, et al. Ultrafast epitaxial growth of metre-sized single-crystal graphene on industrial Cu foil[J]. Science Bulletin, 2017, 62(15): 1074-1080.
[23] CHEN Y, ZHANG N, LI Y F, et al. Microscale-patterned graphene electrodes for organic light-emitting devices by a simple patterning strategy[J]. Advanced Optical Materials, 2018, 6(13): 1701348.
[24] GROOVER M P. Fundamentals of modern manufacturing: materials, processes and systems[M]. Wiley: Hoboken, NJ, 2019.
[25] LUO D, CHOE M, BIZAO R A, et al. Folding and fracture of single-crystal graphene grown on a Cu(111) foil[J]. Advanced Materials, 2022, 34(15): 2110509.
[26] SRIDHARA K, FEIGELSON B N, WOLLMERSHAUSER J A, et al. Electrochemically prepared polycrystalline copper surface for the growth of hexagonal boron nitride[J]. Crystal Growth & Design, 2017, 17(4): 1669-1678.
[27] CHO J Y, MIRPURI K, LEE D N, et al. Texture investigation of copper interconnects with a different line width[J]. Journal of Electronic Materials, 2005, 34(1): 53-61.
[28] ROBINSON Z R, TYAGI P, MURRAY T M, et al. Substrate grain size and orientation of Cu and Cu-Ni foils used for the growth of graphene films[J]. Journal of Vacuum Science & Technology A, 2012, 30(1): 011401.
[29] SONG L, CI L J, LU H, et al. Large scale growth and characterization of atomic hexagonal boron nitride layers[J]. Nano Letters, 2010, 10(8): 3209-3215.
[30] XIA F N, FARMER D B, LIN Y M, et al. Graphene field-effect transistors with high on/off current ratio and large transport band gap at room temperature[J]. Nano Letters, 2010, 10(2): 715-718.
[31] DENG T, ZHANG Z H, LIU Y X, et al. Three-dimensional graphene field-effect transistors as high-performance photodetectors[J]. Nano Letters, 2019, 19(3): 1494-1503.
[32] JMAI B, SILVA V, MENDES P M. 2D electronics based on graphene field effect transistors: tutorial for modelling and simulation[J]. Micromachines, 2021, 12(8): 979.