Yue-Yu Zhang

Two-Dimensional SiS Layers with Promising Electronic and Optoelectronic Properties: Theoretical Prediction.

Two-dimensional (2D) semiconductors can be very useful for novel electronic and optoelectronic applications because of their good material properties. However, all current 2D materials have shortcomings that limit their performance. As a result, new 2D materials are highly desirable. Using atomic transmutation and differential evolution global optimization methods, we identified two group IV-VI 2D materials, Pma2-SiS and silicene sulfide. Pma2-SiS is found to be both chemically, energetically, and thermally stable. Most importantly, Pma2-SiS has shown good electronic and optoelectronic properties, including direct bandgaps suitable for solar cells, good mobility for nanoelectronics, good flexibility of property tuning by layer control and applied strain, and good air stability as well. Therefore, Pma2-SiS is expected to be a promising 2D material in the field of 2D electronics and optoelectronics. The designing principles demonstrated in identifying these two tantalizing examples have great potential to accelerate the finding of new functional 2D materials.

Intrinsic Instability of the Hybrid Halide Perovskite Semiconductor CH3NH3PbI3

The organic-inorganic hybrid perovskite CH3NH3PbI3 has attracted significant interest for its high performance in converting solar light into electrical power with an efficiency exceeding 20%. Unfortunately, chemical stability is one major challenge in the development of the CH3NH3PbI3 solar cells. It was commonly assumed that moisture or oxygen in the environment causes the poor stability of hybrid halide perovskites, however, here we show from the first-principles calculations that the room-temperature tetragonal phase of CH3NH3PbI3 is thermodynamically unstable with respect to the phase separation into CH3NH3I + PbI2, i.e., the disproportionation is exothermic, independent of the humidity or oxygen in the atmosphere. When the structure is distorted to the low-temperature orthorhombic phase, the energetic cost of separation increases, but remains small. Contributions from vibrational and configurational entropy at room temperature have been considered, but the instability of CH3NH3PbI3 is unchanged. When I is replaced by Br or Cl, Pb by Sn, or the organic cation CH3NH3 by inorganic Cs, the perovskites become more stable and do not phase-separate spontaneously. Our study highlights that the poor chemical stability is intrinsic to CH3NH3PbI3 and suggests that element-substitution may solve the chemical stability problem in hybrid halide perovskite solar cells.

Direct Observation of the Bandwidth Control Mott Transition in the NiS

The bulk electronic structure of NiS

_{2-x}

_{2-x}

Se

Se

_x

_x

Multiband System

is studied across the bandwidth-control Mott transition (BCMT) by soft X-ray angle-resolved photoemission spectroscopy. The microscopic picture of the BCMT in this multiband non-half-filled system is revealed for the first time. We show that Se doping does not alter the Fermi surface volume. When approaching the insulating phase with decreasing Se concentration, we observed that the Fermi velocity continuously decreases. Meanwhile, the coherent quasiparticle weight continuously decreases and is transferred to higher binding energies, until it suddenly disappears across the Mott transition. In the insulating phase, there is still finite spectral weight at the Fermi energy, but it is incoherent and dispersionless due to strong correlations. Our results provide a direct observation of BCMT, and unveil its distinct characters in a multiband non-half-filled system.

Electronic structure of the BaTi 2 As 2 O parent compound of the titanium-based oxypnictide superconductor

The electronic structure of BaTi2As2O, a parent compound of the newly discovered titanium-based oxypnictide superconductors, is studied by angle-resolved photoemission spectroscopy. The electronic structure shows multi-orbital nature and possible three-dimensional character. An anomalous temperature-dependent spectral weight redistribution and broad lineshape indicate the incoherent nature of the spectral function. At the density-wave-like transition temperature around 200 K, a partial gap opens at the Fermi patches. These findings suggest that BaTi2As2O is likely a charge density wave material in the strong interaction regime.

Structural Evolution and Optoelectronic Applications of Multilayer Silicene

Despite the recent progress on two-dimensional multilayer materials (2DMM) with weak interlayer interactions, the investigation on 2DMM with strong interlayer interactions is far from its sufficiency. Here we report on first-principles calculations that clarify the structural evolution and optoelectronic properties of such a 2DMM, multilayer silicene. With our newly developed global optimization algorithm, we discover the existence of rich dynamically stable multilayer silicene phases, the stability of which is closely related to the extent of sp3 hybridization that can be evaluated by the average bonds and effective bond angles. The stable Si(111) surface structures are obtained when the silicene thickness gets up to four, showing the critical thickness for the structural evolution. We also find that the multilayer silicene with pi-bonded surfaces present outstanding optoelectronic properties for the solar cells and optical fiber communications due to the incorporation of sp2-type bonds in the sp3-type bonds dominated system. This study is helpful to complete the picture of structure and related property evolution of 2DMM with strong interlayer interactions.

Self-passivation rule and structure of CdTe Σ3 (112) grain boundaries

The theoretical study of grain boundaries (GBs) in polycrystalline semiconductors is currently stalemated by their complicated nature, which is difficult to extract from any direct experimental characterization. Usually, coincidence-site-lattice models are constructed simply by aligning two symmetric planes ignoring various possible reconstructions. Here, we propose a general self-passivation rule to determine the low-energy GB reconstruction and find new configurations for the CdTe \ensuremath{\Sigma}3 (112) GBs. First-principles calculations show that it has lower formation energies than the prototype GBs adopted widely in previous studies. Surprisingly, the reconstructed GBs show self-passivated electronic properties without deep-level states in the band gap. Based on the reconstructed configurations, we revisited the influence of