Conduction Band Control of Oxyhalides with a Triple-Fluorite Layer for Visible Light Photocatalysis

The discovery of building blocks offers new opportunities to develop and control properties of extended solids. Compounds with fluorite-type Bi2O2 blocks host various properties including lead-free ferroelectrics and photocatalysts. In this study, we show that triple-layered Bi2MO4 blocks (M = Bi, La, Y) in Bi2MO4Cl allow, unlike double-layered Bi2O2 blocks, to extensively control the conduction band.

Modulation of the Electronic Properties of MXene (Ti3C2Tx) via Surface-Covalent Functionalization with Diazonium

The physical and chemical properties of MXenes are strongly dependent on surface terminations; thus, the tailoring of surface functional groups in two-dimensional transition-metal carbides (MXenes) may extend the applicability of these compelling materials to a wider set of fields. In this work, we demonstrate the chemical modification of Ti3C2Tx MXene via diazonium covalent chemistry and the subsequent effects on the electrical properties of MXene.

Ab initio perspective of ultra-scaled CMOS from 2D-material fundamentals to dynamically doped transistors

Using accurate dissipative DFT-NEGF atomistic-simulation techniques within the Wannier-Function formalism, we give a fresh look at the possibility of sub-10-nm scaling for high-performance complementary metal oxide semiconductor (CMOS) applications. We show that a combination of good electrostatic control together with high mobility is paramount to meet the stringent roadmap targets.

Morphology and Band Structure of Orthorhombic PbS Nanoplatelets: An Indirect Band Gap Material

PbS quantum dots and nanoplatelets (NPLs) are of enormous interest in the development of optoelectronic devices. However, some important aspects of their nature remain unclear. Recent studies have revealed that colloidal PbS NPLs may depart from the rock-salt crystal structure of bulk and form an orthorhombic (Pnma) modification instead.

Time-dependent screening explains the ultrafast excitonic signal rise in 2D semiconductors

We calculate the time evolution of the transient reflection signal in an MoS2 monolayer on a SiO2/Si substrate using first-principles out-of-equilibrium real-time methods. Our simulations provide a simple and intuitive physical picture for the delayed, yet ultrafast, evolution of the signal whose rise time depends on the excess energy of the pump laser: at laser energies above the A- and B-exciton, the pump pulse excites electrons and holes far away from the K valleys in the first Brillouin zone.

Real-space multiple scattering theory for superconductors with impurities

We implement the Bogoliubov-de Gennes (BdG) equation in real-space using the screened Korringa-Kohn-Rostoker (KKR) method. This allows us to solve, self-consistently, the superconducting state for 3D crystals including substitutional impurities with a full normal-state DFT band structure. We apply the theoretical framework to bulk Nb with impurities. Without impurities, Nb has an anisotropic gap structure with two distinct peaks around the Fermi level.

Kerker mixing scheme for self-consistent muffin-tin based all-electron electronic structure calculations

We propose a computationally efficient Kerker mixing scheme for robust and rapidly converging self-consistent-field calculations using all-electron first-principles electronic structure methods based on the muffin-tin partitioning of space. The mixing scheme is composed of the Kerker preconditioner in combination with quasi-Newton methods.

Oxidation States, Thouless’ Pumps, and Nontrivial Ionic Transport in Nonstoichiometric Electrolytes

Thouless’ quantization of adiabatic particle transport permits one to associate an integer topological charge with each atom of an electronically gapped material. If these charges are additive and independent of atomic positions, they provide a rigorous definition of atomic oxidation states and atoms can be identified as integer-charge carriers in ionic conductors. Whenever these conditions are met, charge transport is necessarily convective; i.e., it cannot occur without substantial ionic flow, a transport regime that we dub trivial.

Surface chemistry effects on work function, ionization potential and electronic affinity of Si(100), Ge(100) surfaces and SiGe heterostructures

We combine density functional theory and many body perturbation theory to investigate the electronic properties of Si(100) and Ge(100) surfaces terminated with halogen atoms (–I, –Br, –Cl, –F) and other chemical functionalizations (–H, –OH, –CH3) addressing the absolute values of their work function, electronic affinity and ionization potential. Our results point out that electronic properties of functionalized surfaces strongly depend on the chemisorbed species and much less on the surface crystal orientation.

Long-range ordered and atomic-scale control of graphene hybridization by photocycloaddition

Chemical reactions that convert sp2 to sp3 hybridization have been demonstrated to be a fascinating yet challenging route to functionalize graphene. So far it has not been possible to precisely control the reaction sites nor their lateral order at the atomic/molecular scale. The application prospects have been limited for reactions that require long soaking, heating, electric pulses or probe-tip press.