Efficient First-Principles Methodology for the Calculation of the All-Phonon Inelastic Scattering in Solids.

Inelastic scattering experiments are key methods for mapping the full dispersion of fundamental excitations of solids in the ground as well as nonequilibrium states. A quantitative analysis of inelastic scattering in terms of phonon excitations requires identifying the role of multiphonon processes. Here, we develop an efficient first-principles methodology for calculating the all-phonon quantum mechanical structure factor of solids. We demonstrate our method by obtaining excellent agreement between measurements and calculations of the diffuse scattering patterns of black phosphorus, showing that multiphonon processes play a substantial role. The present approach constitutes a step towards the interpretation of static and time-resolved electron, x-ray, and neutron inelastic scattering data.

Quantum Confinement of Electron-Phonon Coupling in Graphene Quantum Dots.

On the basis of first-principles calculations and the special displacement method, we demonstrate the quantum confinement scaling law of the phonon-induced gap renormalization of graphene quantum dots (GQDs). We employ zigzag-edged GQDs with hydrogen passivation and embedded in hexagonal boron nitride. Our calculations for GQDs in the sub-10 nm region reveal strong quantum confinement of the zero-point renormalization ranging from 20 to 250 meV. To obtain these values we introduce a correction to the Allen-Heine theory of temperature-dependent energy levels that arises from the phonon-induced splitting of 2-fold degenerate edge states. This correction amounts to more than 50% of the gap renormalization. We also present momentum-resolved spectral functions of GQDs, which are not reported in previous contributions. Our results lay the foundation to systematically engineer temperature-dependent electronic structures of GQDs for applications in solar cells, electronic transport, and quantum computing devices.

Modelling of Three-Dimensional Nanographene.

Monte Carlo simulations and tight-binding calculations shed light on the properties of three-dimensional nanographene, a material composed of interlinked, covalently-bonded nanoplatelet graphene units. By constructing realistic model networks of nanographene, we study its structure, mechanical stability, and optoelectronic properties. We find that the material is nanoporous with high specific surface area, in agreement with experimental reports. Its structure is characterized by randomly oriented and curved nanoplatelet units which retain a high degree of graphene order. The material exhibits good mechanical stability with a formation energy of only ∼0.3 eV/atom compared to two-dimensional graphene. It has high electrical conductivity and optical absorption, with values approaching those of graphene.

Probing the structure and energetics of dislocation cores in SiGe alloys through Monte Carlo simulations.

We present a methodology for the investigation of dislocation energetics in segregated alloys based on Monte Carlo simulations which equilibrate the topology and composition of the dislocation core and its surroundings. An environment-dependent partitioning of the system total energy into atomic contributions allows us to link the atomistic picture to continuum elasticity theory. The method is applied to extract core energies and radii of 60 degrees glide dislocations in segregated SiGe alloys which are inaccessible by other methods.