RESUMEN
Graphene (Gr) has shown great potential in the field of oxidation protection for metals. However, numerous studies have shown that Gr will suffer structural degradation on metal surface during high-temperature oxidation, which significantly limited the effectiveness of their oxidation protection. Therefore, understanding the degradation mechanism of Gr is of great interest to enhance their structural stability. Here, the effect of copper (Cu) surface roughness on the high-temperature structural stability of single-layer graphene (SLG) was examined using Cu covered with SLG as a model material. SLG/Cu with different roughness values was obtained via high-temperature annealing of the model material. After high-temperature oxidation at 500 °C, Raman spectra analysis showed that the defect density of the oxidized SLG increased from 41% to 81% when the surface roughness varied from 37 nm to 81 nm. Combined with density functional theory calculations, it was found that the lower formation energy of the C-O bond on rough Cu surfaces (0.19 eV) promoted the formation of defects in SLG. This study may provide guidance for improving the effectiveness of SLG for the oxidation protection of metallic materials.
RESUMEN
Direct in situ growth of graphene on dielectric substrates is a reliable method for overcoming the challenges of complex physical transfer operations, graphene performance degradation, and compatibility with graphene-based semiconductor devices. A transfer-free graphene synthesis based on a controllable and low-cost polymeric carbon source is a promising approach for achieving this process. In this paper, we report a two-step thermal transformation method for the copper-assisted synthesis of transfer-free multilayer graphene. Firstly, we obtained high-quality polymethyl methacrylate (PMMA) film on a 300 nm SiO2/Si substrate using a well-established spin-coating process. The complete thermal decomposition loss of PMMA film was effectively avoided by introducing a copper clad layer. After the first thermal transformation process, flat, clean, and high-quality amorphous carbon films were obtained. Next, the in situ obtained amorphous carbon layer underwent a second copper sputtering and thermal transformation process, which resulted in the formation of a final, large-sized, and highly uniform transfer-free multilayer graphene film on the surface of the dielectric substrate. Multi-scale characterization results show that the specimens underwent different microstructural evolution processes based on different mechanisms during the two thermal transformations. The two-step thermal transformation method is compatible with the current semiconductor process and introduces a low-cost and structurally controllable polymeric carbon source into the production of transfer-free graphene. The catalytic protection of the copper layer provides a new direction for accelerating the application of graphene in the field of direct integration of semiconductor devices.
RESUMEN
As a typical two-dimensional material, graphene (Gr) has shown great potential to be used in thermal management applications due to its ultrahigh in-plane thermal conductivity (k). However, low interface thermal conductance (ITC) between Gr and metals to a large extent limits the effective heat dissipation in Gr-based devices. Therefore, having a deep understanding on heat transport at Gr-metal interfaces is essential. Because of the semimetallic nature of Gr, electrons would possibly play a role in the heat transport across Gr-metal interfaces as heat carriers, whereas, However, how much the electron can participate in this process and how to optimize the total ITC considering both electron and phonon transportations have not yet been revealed yet. Therefore, in this work, hydrogenation-treated Gr (H-Gr) was sandwiched by nickel (Ni) nanofilms to compare with the samples containing pure Gr for investigating the interfacial electron behaviors. Moreover, both Gr and H-Gr sets of the samples were prepared with different layer numbers (N) ranging from 1 to 7, and the corresponding ITC was systematically studied based on both time-domain thermoreflectance measurements and theoretical calculations. We found that a larger ITC can be obtained when N is low, and the ITC may reach a peak value when N is 2 in certain circumstances. The present findings not only provide a comprehensive understanding on heat transport across Gr-metal interfaces byconsidering a combined effect of the interfacial interaction strength, phonon mode mismatch, and electron contributions, but also shed new lights on interface strucure optimiazations of Gr-based devices.
