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Damage-Free Transfer Mechanics of 2-Dimensional Materials

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Damage-Free Transfer Mechanics of 2-Dimensional Materials Kim et al. NPG Asia Materials (2021) 13:44 https://doi.org/10.1038/s41427-021-00311-1 NPG Asia Materials ARTICLE Open Access Damage-free transfer mechanics of 2-dimensional materials: competition between adhesion instability and tensile strain Chan Kim1,2,Min-AhYoon1,2,BongkyunJang1,2,Hyeon-DonKim2,Jae-HyunKim1,2,AnhTuanHoang 3, Jong-Hyun Ahn 3, Hyun-June Jung4, Hak-Joo Lee4 and Kwang-Seop Kim 1,2 Abstract The transfer of two-dimensional (2D) materials is crucial to the realization of 2D material-based devices for practical applications. The thinness of 2D materials renders them prone to mechanical damage during the transfer process and to degradation of their superior electrical and mechanical properties. Herein, the mechanisms involved in the damage of chemical vapor deposition-grown graphene (Gr) and MoS2 are investigated during a roll-based transfer process. We identify two different damage mechanisms, i.e., instability-induced damage and tensile strain-induced damage. The two mechanisms compete, depending on the thickness of the transfer medium, and induce dissimilar damage. By minimizing these two mechanisms, we realize and demonstrate the damage-free transfer of 2D materials. The sheet resistance and mobility of transferred Gr are 235 ± 29 Ω sq–1 and 2250 cm2 V–1 s–1, respectively, with no microscopic cracks or tear-out damage. We observe instability-induced damage to be ubiquitous in monolayer MoS2, thin metals, and thin oxide films. By understanding the instability-induced damage mechanism, a broad range of 2D materials and thin films can be transferred without mechanical damage. Damage-free transfer will contribute to the high-yield 1234567890():,; 1234567890():,; 1234567890():,; 1234567890():,; fabrication of 2D material-based electronic devices. Introduction The dry transfer method using a transfer film (TF) is The transfer of two-dimensional (2D) materials from preferred for the large-area transfer of 2D materials their growth substrates onto a target substrate is one of because it is readily scalable and compatible with a roll- the most important step for fabricating 2D hetero- based continuous transfer process. In 2010, large-area structures1,2 and 2D material-based devices for practical (30-inch) Gr was transferred onto a flexible target sub- – – applications3 5. 2D materials such as graphene (Gr)6 8, strate using thermal release tape (TRT) as the TF16. The 9,10 11–13 MoS2 , and h-BN can be synthesized with high first practical application of large-area Gr transfer was for quality on a large scale but are prone to damage when a touch panel, but TRT residues and cracks in the transferred. Transferring large-area 2D materials without transferred Gr were problematic. To overcome these any damage is essential for preserving their superior drawbacks, a two-layer TF consisting of a hard supporting electrical and mechanical properties on a target film and a thin compliant layer in contact with Gr via substrate14,15. dispersive adhesion was suggested17,18. The compliant layer provided conformal contact with the 2D materials, and the supporting layer helped the compliant layer Correspondence: Kwang-Seop Kim ([email protected]) 1University of Science & Technology (UST), Nanomechatronics, 217 Gajeong-ro, endure the significant deformation that was applied via Yuseong-gu, Daejeon 34113, Republic of Korea contact pressure during the roll-based transfer process. 2 Nano-Convergence Mechanical Systems Research Division, Korea Institute of The TF was further improved by applying a pressure- Machinery & Materials (KIMM), 156 Gajeongbuk-ro, Yuseong-gu, Daejeon 19 34103, Republic of Korea sensitive adhesive film (PSAF) as the compliant layer . Full list of author information is available at the end of the article © The Author(s) 2021 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a linktotheCreativeCommons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Kim et al. NPG Asia Materials (2021) 13:44 Page 2 of 11 44 The liquid-like PSAF improved the wetting of Gr on the broad range of 2D materials and provide guidance con- target substrate and had the lowest surface energy, leading cerning the damage-free transfer of large-area, high- to the decreased formation of ripples and cracks. Some quality 2D materials. roll-based transfer techniques have also been proposed for the reutilization of metal catalysts; these approaches Materials and methods – – include electrochemical20 23 and direct24 28 transfer. In Sample preparations these transfer methods, various polymer films that are a Monolayer Gr was synthesized on a 35-μm-thick Cu foil few tens of microns thick, such as silicone, ethylene-vinyl (JX Nippon Mining and Metals Corp., Japan) using the 33 acetate (EVA) copolymer, and polyvinyl alcohol (PVA), thermal CVD process . Monolayer MoS2 was grown on a are used as the compliant layer. However, the Gr trans- 4-inch-diameter wafer with a 300-nm-thick surface- ferred by these methods is still structurally damaged and functionalized SiO2/Si substrate in a 4.3 inch (inner dia- shows degraded electrical properties. meter) hot-wall quartz tube MOCVD system34. For the The compliant layer of a TF can significantly mitigate fabrication of the TF, PDMS (Sylgard 184; Dow Corning) damage to 2D materials when the layer is sufficiently soft and a PET film were used as the compliant layer and for conformal contact29. Notably, the contact and adhe- supporting film, respectively. Before coating with PDMS, sion forces that occur during the transfer process can lead a plasma surface treatment (CUTE plasma system; Femto to the deformation of the compliant layer by a strain that Science, South Korea) was performed on the PET film to is much larger than the failure strain of the 2D material30. enhance the adhesion between the PDMS and PET film. Additionally, the compliant layer should have sufficient PDMS was prepared by mixing liquid prepolymer (Sylgard adhesion to the 2D material to reduce damage during 184 A; Dow Corning, USA) and curing agent (Sylgard metal catalyst etching and TF lamination. When a 2D 184B; Dow Corning, USA). The mixture was coated as material is transferred onto a target substrate, the adhe- 25-, 50-, 100-, 200-, and 400-μm-thick layers onto the sion should be weaker than that between the 2D material PET film. To prepare the Gr/transfer film (Gr/TF), TF and the target substrate. Most studies to date have was laminated onto Gr grown on a Cu foil using a home- focused on increasing compliance to mitigate damage29 built roll-to-plate (R2P) transfer machine35,36. The Cu foil and on reducing the surface energy18,19 or interfacial was etched with 0.1 M ammonium persulfate (APS) energy23,31,32 of the compliant layer. However, there are solution or a 0.1 M APS solution containing 5 mM imi- few reports concerning the deformation of the compliant dazole and 50 mM sulfuric acid (IM-APS)33. After etch- layer that leads to mechanical damage of the 2D material. ing, the TF/Gr film was laminated on the SiO2/Si Here, we investigate the damage generation mechan- substrate under a contact load of 2 N/mm and a lamina- isms of 2D materials, such as chemical vapor deposition tion speed of 0.5 mm/s using the R2P transfer machine. (CVD)-grown monolayer Gr and monolayer MoS2, during Prior to the lamination process, various surface treat- a roll-based dry transfer process. Contrary to the common ments were performed on the SiO2/Si substrate. A plasma belief that damage derives mainly from the interfacial surface treatment (CUTE plasma system; Femto Science, energy difference between Gr and the contacting sub- South Korea) was used to increase the surface energy of strate, we find that the damage is significantly affected by the SiO2/Si substrate. An amorphous fluoropolymer the thickness-dependent deformation behavior of the (Teflon AF 1601; Chemours, USA) was diluted with compliant layer contacting the 2D material. Depending on Fluorinert FC-770 (Sigma–Aldrich, USA) to 0.006 wt%, the thickness of the compliant layer, two different damage and the Teflon mixture was coated on the SiO2/Si sub- mechanisms are found to be involved in damage genera- strate to reduce its surface energy. Then, the substrate was tion: instability-induced damage and tensile strain- baked in an oven at 160 °C for 10 min to remove residual induced damage. In the case of Gr transfer, when the solvent. optimal 100-μm-thick polydimethylsiloxane (PDMS) layer is used as the compliant layer, the transferred Gr has the Transfer process – lowest average sheet resistance of 235 ± 29 Ω sq 1 for an The TF was peeled off in two ways. Crack propagation area of 6 × 5 cm2 and the highest mobility of 2250 cm2 between the Gr and PDMS layer in real time was observed – – V 1 s 1. We confirm that the instability-induced damage using optical microscopy (OM), in which the TF was mechanism is also applicable to the transfer of monolayer slowly peeled off by slightly lifting one end of the TF. MoS2 and various thin metal and oxide films.
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