We present direct experimental evidence of broken chirality in graphene by analyzing electron scattering processes at energies ranging from the linear (Dirac-like) to the strongly trigonally warped region. Furthermore, we are able to measure the energy of the van Hove singularity at the M point of the conduction band. Our data show a very good agreement with theoretical calculations for free-standing graphene. We identify a new intravalley scattering channel activated in case of a strongly trigonally warped constant energy contour, which is not suppressed by chirality. Finally, we compare our experimental findings with T-matrix simulations with and without the presence of a pseudomagnetic field and suggest that higher order electron hopping effects are a key factor in breaking the chirality near to the van Hove singularity.

The control of recently observed spintronic effects in topological-insulator/ferromagnetic-metal (TI/FM) heterostructures is thwarted by the lack of understanding of band structure and spin textures around their interfaces. Here we combine density functional theory with Green's function techniques to obtain the spectral function at any plane passing through atoms of Bi2Se3 and Co or Cu layers comprising the interface. Instead of naively assumed Dirac cone gapped by the proximity exchange field spectral function, we find that the Rashba ferromagnetic model describes the spectral function on the surface of Bi2Se3 in contact with Co near the Fermi level EF0, where circular and snowflake-like constant energy contours coexist around which spin locks to momentum. The remnant of the Dirac cone is hybridized with evanescent wave functions from metallic layers and pushed, due to charge transfer from Co or Cu layers, a few tenths of an electron-volt below EF0 for both Bi2Se3/Co and Bi2Se3/Cu interfaces while hosting distorted helical spin texture wounding around a single circle. These features explain recent observation of sensitivity of spin-to-charge conversion signal at TI/Cu interface to tuning of EF0. Crucially for spin-orbit torque in TI/FM heterostructures, few monolayers of Co adjacent to Bi2Se3 host spectral functions very different from the bulk metal, as well as in-plane spin textures (despite Co magnetization being out-of-plane) due to proximity spin-orbit coupling in Co induced by Bi2Se3. We predict that out-of-plane tunneling anisotropic magnetoresistance in Cu/Bi2Se3/Co vertical heterostructure can serve as a sensitive probe of the type of spin texture residing at EF0.

The control of recently observed spintronic effects at topological-insulator/ferromagnetic-metal (TI/FM) interfaces is thwarted by the lack of understanding of their band structure and spin texture. Here we combine density functional theory with Green's function techniques to obtain the spectral function at any plane passing through atoms of Bi$_2$Se$_3$ and Co or Cu layers comprising the interface. In contrast to naively expected Dirac cone gapped by the proximity exchange field, we find that the Rashba ferromagnetic model describes (for some range of momenta) the spectral function on the surface of Bi$_2$Se$_3$ in contact with Co near the Fermi energy $E_F^0$, where circular and snowflake-like constant energy contours coexist around which spin locks to momentum. Interestingly, similar in-plane spin textures are also injected into first three monolayers of Co adjacent to Bi$_2$Se$_3$ due to spin-orbit proximity effect. The remnant of the Dirac cone is hybridized with evanescent wave functions injected by metallic layers and pushed, due to charge transfer from Co or Cu layers, few tenths of eV below $E_F^0$ for both Bi$_2$Se$_3$/Co and Bi$_2$Se$_3$/Cu interfaces while hosting distorted helical spin texture wounding around a single circle. These features can explain recent observation [K. Kondou et al., Nat. Phys. 12, 1027 (2016)] of extreme sensitivity of spin-to-charge conversion signal at TI/Cu interface to tuning of $E_F^0$. We predict that tunneling anisotropic magnetoresistance in vertical heterostructure like Cu/Bi$_2$Se$_3$/Co, where current flowing perpendicular to its interfaces is modulated by rotating magnetization from out-of-plane to in-plane direction, can be employed to probe the type of spin texture residing at $E_F^0$ via purely charge transport measurement.

Using the X-ray standing wave method, scanning tunneling microscopy, low energy electron diffraction, and density functional theory, we precisely determine the lateral and vertical structure of hexagonal boron nitride on Ir(111). The moiré superstructure leads to a periodic arrangement of strongly chemisorbed valleys in an otherwise rather flat, weakly physisorbed plane. The best commensurate approximation of the moiré unit cell is (12 × 12) boron nitride cells resting on (11 × 11) substrate cells, which is at variance with several earlier studies. We uncover the existence of two fundamentally different mechanisms of layer formation for hexagonal boron nitride, namely, nucleation and growth as opposed to network formation without nucleation. The different pathways are linked to different distributions of rotational domains, and the latter enables selection of a single orientation only.

Based on a new family of NiII cubane-like clusters, this work addresses current challenges in synthesis, analysis and dynamics of single-molecule-magnet (SMM) systems. Investigation of various synthetic routes and desorption-sorption processes yielded series of isomorphous compounds: [Ni4L4(CH3OH)4]·xsolv, [Ni4L4(CH3OH)4] and [Ni4L4]. In order to analyze these deceivingly simple materials, several analytical and quantum mechanical methods had to be used. This revealed materials with mixed lattice solvents, statistical disorder of the solvent, and disordered [Ni4L4] cores, what offered an insight into risks of the self-assembly process and interconversion dynamics of the investigated NiII family. These findings also allowed structural-magnetic relationships to be established, and the outcomes were exploited in two turns: in first, effect of the coordinated and lattice solvent on the magnetic properties was examined, and in second, magnetic properties were used to facilitate crystal structure determination.

Electrostatic gating enables key functionality in modern electronic devices by altering the properties of materials. While classical electrostatics is usually sufficient to understand the effects of gating in extended systems, the inherent quantum properties of gating in nanostructures offer unexplored opportunities for materials and devices. Using first-principles calculations for Co/bilayer graphene, Co/BN/graphene, and Co/BN/benzene, as well as a simple physical model, we show that heterostructures with two-dimensional materials yield tunable magnetic proximity effects. van der Waals bonding is identified as a requirement for large electronic structure changes by gating, enabling both the magnitude and sign change of spin polarization in physisorbed graphene. The ability to electrically reverse the spin polarization of an electrode provides an alternative to using the applied magnetic field or spin transfer torque in spintronic devices, thus transforming a spin valve into a spin transistor.