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The combined feature of high thermal conductivity and high carrier mobility makes cubic boron arsenide (c-BAs) promising for high power and high frequency applications. In BAs-based electronics, the interaction between metals and BAs is crucial, as it significantly affects the electronic properties. One particular parameter is the Schottky barrier height (SBH), which plays a critical role in determining the transmission properties. The interfacial contact effects of BAs (110), (111), and (100) surfaces with a variety of metals have been carefully explored using first-principles calculations in order to characterize their electrical characteristics. For p-type SBHs, over different terminations, there is a strong linear trend with increasing metal work function, with a relatively steeper pinning coefficient of ∼0.2. The results show that the SBHs follow a relation of ϕ n (110) > ϕ n (111) > ϕ n (100). Clear metal induced gap states can be observed at the interfacial BAs, resulting in an enhanced Fermi level pinning effect. The Sc is excellent at generating Schottky contacts with relatively higher SBHs (∼0.9 eV). Pt has the smallest barrier height of ∼0.3 eV, making it ideal for ohmic electrodes with low contact resistance. This work provides insight into the properties at metal–BAs contact interfaces and provides a theoretical basis for the selection of suitable electrodes for high power BAs devices. [ABSTRACT FROM AUTHOR]

The mechanism of gate threshold voltage (VT) shifts observed in high κ/metal gate stacks is investigated by a density functional theory. This finds that VT depends on the band alignments and the chemical trends between the component oxide layers, such as HfO2, SrO, La2O3, Al2O3, and SiO2. Based on the electron counting rule, we have built three insulating SiO2/SrO, SiO2/La2O3, and SiO2/Al2O3 interfaces, all of which feature a clean bandgap. Two methods have been adopted to derive the band alignments between these four oxides, which are consistent with each other. The results show staggered, "staircase" band alignments and enable La2O3 and Al2O3 layers to shift the metal electrode Fermi level in opposite directions and to approach the Si conduction band and valence band edge positions, respectively. This analysis updates previous empirical models of this effect based on metal oxide ion densities or electronegativity scales and confirms that the oxide layer scheme is suitable for controlling the effective metal work functions in metal–oxide–semiconductor field-effect transistors. [ABSTRACT FROM AUTHOR]

Exploring the gas-solid compatibility between insulating gas and solids materials used in electrical equipment is of great significance for determining the long-term behavior of insulating gas trifluoromethanesulonyl fluoride (CF3SO2F). The gas-solid compatibility of CF3SO2F and its decomposition products with Ag, Zn, and ZnO common surfaces has been assessed based on first-principles calculations, with SF6 as the control group. CF3SO2F has excellent gas-solid compatibility with the solid surfaces by analyzing the adsorption configurations, adsorption energies, charge transfer, adsorption height, density of states, and ab initio molecular dynamics (AIMD) results. The external electric fields do not affect the excellent compatibility between CF3SO2F and the solid surfaces. Besides, the Ag(111) surface exhibits fine gas-solid compatibility with all decomposition products benefitting from its low surface energy. Originating in the existence of the three-center-four-electron (3c4e) π bond and F atoms with strong electronegativity in SO2F2, SO2F2 has poor compatibility with the Ag(110), (100), and Zn(001) surface. SO2, COF2, and HF gases may accelerate equipment failure due to the strong adsorption strength and poor compatibility with ZnO(100) and (110) surfaces. The results provide the theoretical guidance for the engineering application and long-term performance evaluation of CF3SO2F. [ABSTRACT FROM AUTHOR]

With ultra-wide bandgap and outstanding thermal properties, diamond-based high-power devices have excellent application prospects. The crystal structure and electronic property of the metal/hydrogen-terminated diamond (H-diamond) interfaces have been extensively studied experimentally, but the Schottky barrier height (SBH) theory at the metal/H-diamond interface has not been systematically investigated yet. In this work, SBHs of interfaces formed by H-diamond (111) surfaces with 12 metals (Y, Sc, Mg, Ag, Al, Ti, Cu, Co, Pd, Ni, Au and Pt) are investigated using ab-initio calculations. The fitted curve of the SBH with respect to the metal work function is obtained with a Fermi pinning factor of 0.30, which is close to the empirical value of 0.36. Due to the negative electron affinity of H-diamond, Schottky contacts can be formed with low work function metals, which is useful in device design to regulate the SBH and it is relatively easier to form ohmic contacts with high work function metals, leading to low contact resistances. Our work sheds light on the rational design of diamond-based semiconductor devices with low contact resistances. [ABSTRACT FROM AUTHOR]

The metal–insulator transition (MIT) in polycrystalline vanadium dioxide (VO2) is less sharp than in single-crystal VO2 due to the presence of grain boundaries (GBs). The MIT causes a resistivity change (Ron/Roff) across the MIT to decline from the single-crystal value of ∼104 and also causes a larger hysteresis across the transition. The properties of GBs in VO2 are studied as a function of GB tilt angle. We find that V–V site pairing, which causes a monoclinic phase VO2 to be semiconducting in bulk, also controls bandgap opening at GBs, thus influencing the overall metal–insulator behavior. The almost linear relationship between the ratio of adhesion energy divided by two times the surface energy and the GB energy indicates that the GB energy of twin GBs is primarily determined by re-binding across the GB rather than by the corresponding surface energy. Moreover, a steeper linear fit, characterized by a slope of 0.62, observed in the monoclinic phase VO2 suggests that the GB energy and stability have a higher tolerance to interfacial distortion at the boundary, compared to the rutile phase VO2 and TiO2. [ABSTRACT FROM AUTHOR]

Integration of transition metal dichalcogenides (TMDs) into next-generation semiconductor platforms has been limited due to a lack of effective passivation techniques for defects in TMDs. The formation of an organic-inorganic van der Waals interface between a monolayer (ML) of titanyl phthalocyanine (TiOPc) and a ML of MoS2 is investigated as a defect passivation method. A strong negative charge transfer from MoS2 to TiOPc molecules is observed in scanning tunneling microscopy. As a result of the formation of a van der Waals interface, the ION/IOFF in back-gated MoS2 transistors increases by more than two orders of magnitude, whereas the degradation in the photoluminescence signal is suppressed. Density functional theory modeling reveals a van der Waals interaction that allows sufficient charge transfer to remove defect states in MoS2. The present organic-TMD interface is a model system to control the surface/interface states in TMDs by using charge transfer to a van der Waals bonded complex.

Halide perovskites ABX3 are valuable photovoltaic and light-emitting materials due to their favorable optical properties of a direct bandgap and strong optical absorption just above the bandgap. Here, we show that these properties arise mainly from multi-centered X-B-X bonding and B-p X-p coupling. A bonding analysis finds that B–X bonds have shared electrons intermediate between that of ionic and covalent bonding. The B cation site p orbital interacts with left and right lobes of X-p orbitals, forming a special three-centered, two-electron X–B–X bond. This bonding mechanism is shown to give rise to unusually large optical matrix elements, especially in the visible spectrum, with the normalized matrix elements twice that of typical two-center bonds and transition probabilities four times larger. These cause a very sharp increase in optical absorption just above the gap. Experimental values of Urbach energies are found to be small, even if perovskites have disordered structures. The broad valence and conduction bands of the linearly aligned p orbitals cause dispersive band extrema, with small effective masses of both carriers at the R point, indicating a high carrier mobility. [ABSTRACT FROM AUTHOR]

Electrochemical CO2 reduction reaction (CO2RR) offers a sustainable strategy for producing fuels and chemicals. However, it suffers from sluggish CO2 activation and slow water dissociation. In this work, we construct a (P−O)δ− modified In catalyst that exhibits high activity and selectivity in electrochemical CO2 reduction to formate. A combination of in situ characterizations and kinetic analyses indicate that (P−O)δ− has a strong interaction with K+(H2O)n, which effectively accelerates water dissociation to provide protons. In situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) measurements together with density functional theory (DFT) calculations disclose that (P−O)δ− modification leads to a higher valence state of In active site, thus promoting CO2 activation and HCOO* formation, while inhibiting competitive hydrogen evolution reaction (HER). As a result, the (P−O)δ− modified oxide‐derived In catalyst exhibits excellent formate selectivity across a broad potential window with a formate Faradaic efficiency as high as 92.1 % at a partial current density of ~200 mA cm−2 and a cathodic potential of −1.2 V vs. RHE in an alkaline electrolyte. [ABSTRACT FROM AUTHOR]