Simulating the nanomechanical response of cyclooctatetraene molecules on a graphene device

We investigate the atomic and electronic structures of cyclooctatetraene (COT) molecules on graphene and analyze their dependence on external gate voltage using first-principles calculations. The external gate voltage is simulated by adding or removing electrons using density functional theory (DFT) calculations. This allows us to investigate how changes in carrier density modify the molecular shape, orientation, adsorption site, diffusion barrier, and diffusion path. For increased hole doping COT molecules gradually change their shape to a more flattened conformation and the distance between the molecules and graphene increases while the diffusion barrier drastically decreases. For increased electron doping an abrupt transition to a planar conformation at a carrier density of -8$\times$10$^{13}$ e/cm$^2$ is observed. These calculations imply that the shape and mobility of adsorbed COT molecules can be controlled by externally gating graphene devices

Strongly reshaped organic-metal interfaces: Tetracyanoethylene on Cu(100)

The interaction of the strong electron-acceptor tetracyanoethylene (TCNE) with the Cu(100) surface has been studied with scanning tunneling microscopy experiments and first-principles density functional theory calculations. We compare two different adsorption models with the experimental results and show that the molecular self-assembly is caused by a strong structural modification of the Cu(100) surface rather than the formation of a coordination network by diffusing Cu adatoms. Surface atoms become highly buckled and the chemisorption of TCNE is accompanied by a partial charge-transfer.Comment: 4 pages, 3 figures, to appear in Physical Review Letter

Visualizing and manipulating chiral interface states in a moir\'e quantum anomalous Hall insulator

Moir\'e systems made from stacked two-dimensional materials host novel correlated and topological states that can be electrically controlled via applied gate voltages. We have used this technique to manipulate Chern domains in an interaction-driven quantum anomalous Hall insulator made from twisted monolayer-bilayer graphene (tMBLG). This has allowed the wavefunction of chiral interface states to be directly imaged using a scanning tunneling microscope (STM). To accomplish this tMBLG carrier concentration was tuned to stabilize neighboring domains of opposite Chern number, thus providing topological interfaces completely devoid of any structural boundaries. STM tip pulse-induced quantum dots were utilized to induce new Chern domains and thereby create new chiral interface states with tunable chirality at predetermined locations. Theoretical analysis confirms the chiral nature of observed interface states and enables the determination of the characteristic length scale of valley polarization reversal across neighboring tMBLG Chern domains. tMBLG is shown to be a useful platform for imaging the exotic topological properties of correlated moir\'e systems.Comment: 30 pages, 13 figures, 1 tabl