Nanoelectronics – theory and simulation


N. Friedrich, P. Brandimarte, J. Li, S. Saito, S. Yamaguchi, I. Pozo, D. Peña, T. Frederiksen, A. Garcia-Lekue, D. Sánchez-Portal, and J. I. Pascual
Magnetism of topological boundary states induced by boron substitution in graphene nanoribbons
Phys. Rev. Lett. 125, 146801 (2020) [PRL Cover] [arXiv:2004.10280] [HTML5]

Graphene nanoribbons (GNRs), low-dimensional platforms for carbon-based electronics, show the promising perspective to also incorporate spin polarization in their conjugated electron system. However, magnetism in GNRs is generally associated to localized states around zigzag edges, difficult to fabricate and with high reactivity. Here we demonstrate that magnetism can also be induced away from physical GNR zigzag edges through atomically precise engineering topological defects in its interior. A pair of substitutional boron atoms inserted in the carbon backbone breaks the conjugation of their topological bands and builds two spin-polarized boundary states around. The spin state was detected in electrical transport measurements through boron-substituted GNRs suspended between tip and sample of a scanning tunneling microscope. First-principle simulations find that boron pairs induce a spin 1, which is modified by tuning the spacing between pairs. Our results demonstrate a route to embed spin chains in GNRs, turning them basic elements of spintronic devices.

S. Sanz, P. Brandimarte, G. Giedke, D. Sánchez-Portal, and T. Frederiksen
Crossed graphene nanoribbons as beam splitters and mirrors for electron quantum optics
Phys. Rev. B 102, 035436 (2020) [arXiv:2005.11391] [HTML5]

We analyze theoretically 4-terminal electronic devices composed of two crossed graphene nanoribbons (GNRs) and show that they can function as beam splitters or mirrors. These features are identified for electrons in the low-energy region where a single valence or conduction band is present. Our modeling is based on pz orbital tight-binding with Slater-Koster type matrix elements fitted to accurately reproduce the low-energy bands from density functional theory calculations. We analyze systematically all devices that can be constructed with either zigzag or armchair GNRs in AA and AB stackings. From Green's function theory the elastic electron transport properties are quantified as a function of the ribbon width. We find that devices composed of relatively narrow zigzag GNRs and AA-stacked armchair GNRs are the most interesting candidates to realize electron beam splitters with a close to 50-50 ratio in the two outgoing terminals. Structures with wider ribbons instead provide electron mirrors, where the electron wave is mostly transferred into the outgoing terminal of the other ribbon, or electron filters where the scattering depends sensitively on the wavelength of the propagating electron. We also test the robustness of these transport properties against variations in intersection angle, stacking pattern, lattice deformation (uniaxial strain), inter-GNR separation, and electrostatic potential differences between the layers. These generic features show that GNRs are interesting basic components to construct electronic quantum optical setups.

W. Schattke, T. Frederiksen, M.A. Van Hove, and R. Díez Muiño
Nanomechanics of a hydrogen molecule suspended between two equally charged tips
Phys. Rev. B 101, 195436 (2020) [arXiv:1910.11619] [HTML5]

The geometric configuration and energy of a hydrogen molecule centered between two point-shaped tips of equal charge are calculated with the variational quantum Monte Carlo (QMC) method without the restriction of the Born-Oppenheimer (BO) approximation. The ground-state nuclear distribution, stability, and low-vibrational excitations are found to deviate significantly from the BO treatment based on a potential energy surface obtained with the same QMC accuracy. The quantum-mechanical distribution of the molecular axis direction and the bond length at a subnanometer level is fundamental for understanding nanomechanical dynamics with embedded hydrogen. The cylindrical symmetry of the tip arrangement yields a uniform azimuthal distribution of the molecular axis vector relative to the tip-tip axis. For fixed tip separation, the QMC sampling shows that the polar angle distribution of the molecular axis is centered around the equatorial plane for positive tip charge (transverse alignment) and around the tip-tip direction for negative tip charge (bridge alignment). These deviations from spherical symmetry are magnified as the tip-tip distance decreases. Our results thus show that the molecular orientation in the junction can be controlled by the tip charge and separation, suggesting an application in the field of molecular machines.

J. Li, S. Sanz, J. Castro-Esteban, M. Vilas-Varela, N. Friedrich, T. Frederiksen, D. Peña, and J. I. Pascual
Uncovering the triplet ground state of triangular graphene nanoflakes engineered with atomic precision on a metal surface
Phys. Rev. Lett. 124, 177201 (2020) [DOI] [arXiv:1912.08298] [HTML5]

Graphene can develop large magnetic moments in custom-crafted open-shell nanostructures such as triangulene, a triangular piece of graphene with zigzag edges. Current methods of engineering graphene nanosystems on surfaces succeeded in producing atomically precise open-shell structures, but demonstration of their net spin remains elusive to date. Here, we fabricate triangulenelike graphene systems and demonstrate that they possess a spin S=1 ground state. Scanning tunneling spectroscopy identifies the fingerprint of an underscreened S=1 Kondo state on these flakes at low temperatures, signaling the dominant ferromagnetic interactions between two spins. Combined with simulations based on the meanfield Hubbard model, we show that this S=1 π paramagnetism is robust and can be turned into an S=1/2 state by additional H atoms attached to the radical sites. Our results demonstrate that π paramagnetism of high-spin graphene flakes can survive on surfaces, opening the door to study the quantum behavior of interacting π spins in graphene systems.

T. Jasper-Toennies, M. Gruber, S. Johannsen, T. Frederiksen, A. Garcia-Lekue, T. Jäkel, F Roehricht, R. Herges, and R. Berndt
Rotation of Ethoxy and Ethyl Moieties on a Molecular Platform on Au(111)
ACS Nano 14, 3907-3916 (2020) [DOI]

Molecular rotors have attracted considerable interest for their prospects in nanotechnology. However, their adsorption on supporting substrates, where they may be addressed individually, usually modifies their properties. Here, we investigate the switching of two closely-related three-states rotors mounted on platforms on Au(111) using low-temperature scanning tunneling microscopy and density functional theory calculations. Being physisorbed the platforms retain important gas-phase properties of the rotor. This simplifies a detailed analysis, and permits, for instance, the identification of the vibrational modes involved in the rotation process. The symmetry provided by the platform enables active control of the rotation direction through electrostatic interactions with the tip and charged neighboring adsorbates. The present investigation of two model systems may turn out useful for designing platforms that provide directional rotation and for transferring more sophisticated molecular machines from the gas-phase to surfaces.