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Register a new userCharacterization of Hydrogen Plasma Defined Graphene Edges
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Added by
Dominik Zumb\\\"uhl
Publication date
2019
fields
Physics
and research's language is
English
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We investigate the quality of hydrogen plasma defined graphene edges by Raman spectroscopy, atomic resolution AFM and low temperature electronic transport measurements. The exposure of graphite samples to a remote hydrogen plasma leads to the formation of hexagonal shaped etch pits, reflecting the anisotropy of the etch. Atomic resolution AFM reveals that the sides of these hexagons are oriented along the zigzag direction of the graphite crystal lattice and the absence of the D-peak in the Raman spectrum indicates that the edges are high quality zigzag edges. In a second step of the experiment, we investigate hexagon edges created in single layer graphene on hexagonal boron nitride and find a substantial D-peak intensity. Polarization dependent Raman measurements reveal that hydrogen plasma defined edges consist of a mixture of zigzag and armchair segments. Furthermore, electronic transport measurements were performed on hydrogen plasma defined graphene nanoribbons which indicate a high quality of the bulk but a relatively low edge quality, in agreement with the Raman data. These findings are supported by tight-binding transport simulations. Hence, further optimization of the hydrogen plasma etching technique is required to obtain pure crystalline graphene edges.
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We investigate the etching of a pure hydrogen plasma on graphite samples and graphene flakes on SiO$_2$ and hexagonal Boron-Nitride (hBN) substrates. The pressure and distance dependence of the graphite exposure experiments reveals the existence of two distinct plasma regimes: the direct and the remote plasma regime. Graphite surfaces exposed directly to the hydrogen plasma exhibit numerous etch pits of various size and depth, indicating continuous defect creation throughout the etching process. In contrast, anisotropic etching forming regular and symmetric hexagons starting only from preexisting defects and edges is seen in the remote plasma regime, where the sample is located downstream, outside of the glowing plasma. This regime is possible in a narrow window of parameters where essentially all ions have already recombined, yet a flux of H-radicals performing anisotropic etching is still present. At the required process pressures, the radicals can recombine only on surfaces, not in the gas itself. Thus, the tube material needs to exhibit a sufficiently low H radical recombination coefficient, such a found for quartz or pyrex. In the remote regime, we investigate the etching of single layer and bilayer graphene on SiO$_2$ and hBN substrates. We find isotropic etching for single layer graphene on SiO$_2$, whereas we observe highly anisotropic etching for graphene on a hBN substrate. For bilayer graphene, anisotropic etching is observed on both substrates. Finally, we demonstrate the use of artificial defects to create well defined graphene nanostructures with clean crystallographic edges.
Monatomic metal (e.g. silver) structures could form preferably at graphene edges. We explore their structural and electronic properties by performing density functional theory based first-principles calculations. The results show that cohesion between metal atoms, as well as electronic coupling between metal atoms and graphene edges offer remarkable structural stability of the hybrid. We find that the outstanding mechanical properties of graphene allow tunable properties of the metal monatomic structures by straining the structure. The concept is extended to metal rings and helices that form at open ends of carbon nanotubes and edges of twisted graphene ribbons. These findings demostrate the role of graphene edges as an efficient one-dimensional template for low-dimensional metal structures that are mechanotunable.
The influence of plasma etched sample edges on electrical transport and doping is studied. Through electrical transport measurements the overall doping and mobility are analyzed for mono- and bilayer graphene samples. As a result the edge contributes strongly to the overall doping of the samples. Furthermore the edge disorder can be found as the main limiting source of the mobility for narrow samples.
We have used scanning tunneling microscopy (STM) to investigate two types of hydrogen defect structures on monolayer graphene supported by hexagonal boron nitride (h-BN) in a gated field-effect transistor configuration. The first H-defect type is created by bombarding graphene with 1-keV ionized hydrogen and is identified as two hydrogen atoms bonded to a graphene vacancy via comparison of experimental data to first-principles calculations. The second type of H defect is identified as dimerized hydrogen and is created by depositing atomic hydrogen having only thermal energy onto a graphene surface. Scanning tunneling spectroscopy (STS) measurements reveal that hydrogen dimers formed in this way open a new elastic channel in the tunneling conductance between an STM tip and graphene.
A four-terminal donor quantum dot (QD) is used to characterize potential barriers between degenerately doped nanoscale contacts. The QD is fabricated by hydrogen-resist lithography on Si(001) in combination with $n$-type doping by phosphine. The four contacts have different separations ($d$ = 9, 12, 16 and 29 nm) to the central 6 nm $times$ 6 nm QD island, leading to different tunnel and capacitive coupling. Cryogenic transport measurements in the Coulomb-blockade (CB) regime are used to characterize these tunnel barriers. We find that field enhancement near the apex of narrow dopant leads is an important effect that influences both barrier breakdown and the magnitude of the tunnel current in the CB transport regime. From CB-spectroscopy measurements, we extract the mutual capacitances between the QD and the four contacts, which scale inversely with the contact separation $d$. The capacitances are in excellent agreement with numerical values calculated from the pattern geometry in the hydrogen resist. We show that by engineering the source-drain tunnel barriers to be asymmetric, we obtain a much simpler excited-state spectrum of the QD, which can be directly linked to the orbital single-particle spectrum.
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