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Clean transfer of chemical vapor deposition graphene film

Zhang Xiao-Bo Qing Fang-Zhu Li Xue-Song

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Clean transfer of chemical vapor deposition graphene film

Zhang Xiao-Bo, Qing Fang-Zhu, Li Xue-Song
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  • Graphene is believed to have promising applications in many fields because of its unique properties. At present, graphene films are mainly prepared on Cu substrates by chemical vapor deposition. The graphene films prepared in this way need to be transferred to the target substrates for further applications, while the transfer process inevitably induces contamination on graphene, which affects the properties of graphene and the performance of devices. Therefore, how to reduce or avoid contamination and realize the clean transfer of graphene is an important topic for the development of graphene transfer technology, which is the major topic of this review. Here, firstly, the transfer techniques of graphene are briefly reviewed, which can be classified according to different rules. For example, it can be classified as direct transfer, with which graphene is directly stuck to the target substrate, and indirect transfer, with which graphene is indirectly transferred to the target substrate with a carrier film. According to the way of separating graphene and the growth substrate, it can also be classified as dissolving transfer, with which the substrate is dissolved by chemical etchant, and delaminating transfer, with which graphene is delaminated from the substrate. Then the origins of contamination are discussed followed with how contamination affects graphene properties. The main contaminations induced by transfer are ions from the etchant and electrolyte, undissolved metal or metal oxide particles, and organic residues from carrier films. Contaminations have a great influence on the electrical, thermal and optical properties of graphene. Then the up-to-date progress of techniques for clean transfer is reviewed, including modifying the cleaning process or using alternative etchant/electrolyte to remove or suppress metal contamination and annealing graphene or using alternative carrier films (e.g., more dissoluble materials) to remove or suppress organic residues. Finally, the challenges of clean transfer of graphene are summarized, and future research directions and opportunities are prospected. This review not only contributes to the research of graphene film transfer technology, but also has great reference value for the clean fabrication of the whole two-dimensional materials and devices.
      Corresponding author: Qing Fang-Zhu, qingfz@uestc.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51802036, 51772043), the China Scholarship Council (Grant No. 201708515008), the Key Research and Development Program of Sichuan Province, China (Grant No. 2018GZ0434), and the Applied Basic Research Program of Sichuan Province, China (Grant No. 2019YJ0168).
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  • 图 1  石墨烯直接转移与间接转移示意图

    Figure 1.  Schematic of direct and indirect transfer of graphene

    图 2  各种转移方法示意图 (a) “卷对卷”转移[19]; (b)电化学分离转移[20]; (c)机械剥离转移[22]; (d)溶解基底的直接转移[25]

    Figure 2.  Schematics of various transfer methods: (a) “R2R” transfer[19]; (b) electrochemical delamination transfer[20]; (c) mechanical delamination transfer[22]; (d) direct transfer by dissolving the substrate[25].

    图 3  不同平均分子量PMMA转移的石墨烯的AFM图和归一化高度分布图[35], 其中对应PMMA的平均分子量为: (a), (e) 996000; (b), (f) 350000; (c), (g) 35000; (d), (h) 15000; AFM图像上方的曲线是AFM图像中白色斜线的线扫描, AFM图像尺寸为5 μm × 5 μm

    Figure 3.  AFM images and normalized height distribution profiles of transferred graphene using PMMA with different average molecular weight: (a), (e) 996000; (b), (f) 350000; (c), (g) 35000; (d), (h) 15000[35]. The curves above each AFM image represent the line profile of the white slanting line in the images. The size of AFM surface image is 5 μm × 5 μm.

    图 4  石墨烯与聚合物的相互作用力示意图[40] (a) 范德瓦耳斯力; (b) $ {\text{π}}$$ {\text{π}}$键; (c)静电力; (d)化学键

    Figure 4.  The interactions between polymers and graphene[40]: (a) van der Waals force; (b) $ {\text{π}}$$ {\text{π}}$ interactions; (c) electrostatic interactions; (d) chemical bonding.

    图 5  结合硅晶圆清洗技术的间接转移[29] (a)采用改进的石墨烯清洗方法的转移流程; (b), (c)传统转移和(d), (e)改进的石墨烯清洗转移的光学图像和扫描电子显微镜图像; (b)和(c)中金属微粒残留用蓝色圆圈标记, 小破洞用黄色圆圈标记, 多层石墨烯区域(对比度较暗)用箭头标记; (e)中箭头标记的窄的黑色线条为褶皱

    Figure 5.  Indirect graphene transfer with “modified RCA clean”[29]: (a) Transfer process flow; optical microscopy images and scanning electron microscopy images of (b), (c) traditional transferred graphene film and (d), (e) modified RCA cleaning transferred graphene film. In (b) and (c) the metal residues and the small holes are marked with blue circles and yellow circles, respectively, and the graphene adlayers (with darker contrast) are marked with arrows. The arrow in (e) points to the wrinkles (the dark lines).

    图 6  使用NH4OH+H2O2转移石墨烯流程图[49]

    Figure 6.  Schematic of graphene transfer with NH4OH and H2O2[49]

    图 7  热去离子水浸湿-剥离石墨烯转移流程图[50]

    Figure 7.  Schematic showing the steps of graphene transfer with hot deionized (DI) water[50].

    图 8  石墨烯在空气和H2/Ar 200 ℃退火2 h后的TEM图像[57] (a), (b)显示表面清洁度的细节, 下面对应面板中复制的着色的图像用以区分分解温度不同的PMMA残留物, 没有PMMA的区域在彩色图像中显示为灰色; 左下角的图解释了相应的颜色, 其中蓝色、红色和黄色分别代表PMMA-G, PMMA-A和Cu纳米颗粒; (c)图(b)中所示区域的TEM高分辨图, 显示仍有PMMA残留物

    Figure 8.  TEM images of graphene after air and H2/Ar two-step annealing at 250 ℃ for 2 h[57]. Panels (a) and (b) show the details of surface cleanliness. The same images are duplicated and colored in the lower panels to distinguish the PMMA residues that decomposed differently. The areas free of PMMA are shown in gray in the colored images. The bottom-left image interprets the meaning of different colors, in which blue, red, and yellow stand for PMMA-G, PMMA-A, and Cu nanoparticles, respectively. (c) Atomic resolution of graphene clean surface with PMMA residue shown piecewise at the bottom corner after annealing.

    图 9  用于石墨烯间接转移的中介层材料

    Figure 9.  Carrier layer materials for indirect transfer of graphene.

    图 10  TRT, PMMA, PET/Silicone作为中介层转移结果的对比[68] (a)−(c)光学显微图像; (d)−(f)三维AFM图像

    Figure 10.  (a)−(c) Optical and (d)−(f) three-dimensional AFM images showing the surface morphologies of the monolayer graphene films transferred onto SiO2/Si substrates by TRT, PMMA and PET/silicone, respectively[68].

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Metrics
  • Abstract views:  17746
  • PDF Downloads:  321
  • Cited By: 0
Publishing process
  • Received Date:  01 March 2019
  • Accepted Date:  27 March 2019
  • Available Online:  01 May 2019
  • Published Online:  05 May 2019

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