The control of graphene double-layer formation in copper-catalyzed chemical vapor deposition

The growth of graphene during Cu-catalyzed chemical vapor deposition was studied using 12CH4 and 13CH4 precursor gasses. We suggest that the growth begins by the formation of a multilayer cluster. This seed increases its size but the growth speed of a particular layer depends on its proximity to the copper surface. The layer closest to the substrate grows fastest and thus further limits the growth rate of the upper layers. Nevertheless, the growth of the upper layers continues until the copper surface is completely blocked. It is shown that the upper layers can be removed by modification of the conditions of the growth by hydrogen etching.Comment: 17 pages, 4 figure

Superlattice in collapsed graphene wrinkles

Topographic corrugations, such as wrinkles, are known to introduce diverse physical phenomena that can significantly modify the electrical, optical and chemical properties of two-dimensional materials. This range of assets can be expanded even further when the crystal lattices of the walls of the wrinkle are aligned and form a superlattice, thereby creating a high aspect ratio analogue of a twisted bilayer or multilayer – the so-called twisted wrinkle. Here we present an experimental proof that such twisted wrinkles exist in graphene monolayers on the scale of several micrometres. Combining atomic force microscopy and Raman spectral mapping using a wide range of visible excitation energies, we show that the wrinkles are extremely narrow and their Raman spectra exhibit all the characteristic features of twisted bilayer or multilayer graphene. In light of a recent breakthrough – the superconductivity of a magic-angle graphene bilayer, the collapsed wrinkles represent naturally occurring systems with tuneable collective regimes

Mass-related inversion symmetry breaking and phonon self-energy renormalization in isotopically labeled AB-stacked bilayer graphene

A mass-related symmetry breaking in isotopically labeled bilayer graphene (2LG) was investigated during in-situ electrochemical charging of AB stacked (AB-2LG) and turbostratic (t-2LG) layers. The overlap of the two approaches, isotopic labeling and electronic doping, is powerful tool and allows to tailor, independently and distinctly, the thermal-related and transport-related phenomena in materials, since one can impose different symmetries for electrons and phonons in these systems. Variations in the system's phonon self-energy renormalizations due to the charge distribution and doping changes could be analyzed separately for each individual layer. Symmetry arguments together with first-order Raman spectra show that the single layer graphene (1LG), which is directly contacted to the electrode, has a higher concentration of charge carriers than the second graphene layer, which is not contacted by the electrode. These different charge distributions are reflected and demonstrated by different phonon self-energy renormalizations of the G modes for AB-2LG and for t-2LG.Czech Republic. Ministry of Education, Youth, and Sports (LH-13022)Czech Science Foundation (P208-12-1062)Conselho Nacional de Pesquisas (Brazil)National Science Foundation (U.S.) (NFS-DMR 10-04147