Local symmetry-driven interfacial magnetization and electronic states in (ZnO)n/(w-FeO)n superlattices.

Superlattices constructed with the wide-band-gap semiconductor ZnO and magnetic oxide FeO, both in the wurtzite structure, have been investigated using spin-polarized first-principles calculations. The structural, electronic and magnetic properties of the (ZnO)n/(w-FeO)n superlattices were studied in great detail. Two different interfaces in the (ZnO)n/(w-FeO)n superlattices were identified and they showed very different magnetic and electronic properties. Local symmetry-driven interfacial magnetization and electronic states can arise from different Fe/Zn distributions at different interfaces or spin ordering of Fe in the superlattice. The local symmetry-driven interfacial magnetization and electronic states, originating either from different Fe/Zn distribution across interfaces I and II, or by spin ordering of Fe in the superlattice, can be identified. It was also found that, in the case of the ferromagnetic phase, the electrons are more delocalized for the majority spin but strongly localized for the minority spin, which resulted in interesting spin-dependent transport properties. Our results will pave the way for designing novel spin-dependent electronic devices through the construction of superlattices from semiconductors and multiferroics.

Influence of Zr aggregation on Li-ion conductivity of amorphous solid-state electrolyte Li-La-Zr-O.

In our study, we investigated the influence of the local structure of amorphous Li-La-Zr-O (a-LLZO) on Li-ion conductivity using ab initio molecular dynamics (AIMD). A-LLZO has shown promising properties in inhibiting the growth of lithium dendrites, making it a potential candidate for solid electrolytes in all-solid-state lithium batteries. The low Li-ion conductivity of a-LLZO is currently limiting its practical applications. Our findings revealed that the homogeneous distribution of Zr-O polyhedra within the pristine structure of a-LLZO contributes to enhanced Li-ion conductivity. By reducing the interconnections among Zr-O polyhedra, the AIMD-simulated a-LLZO sample achieved a Li-ion conductivity of 5.78 × 10-4 S/cm at room temperature, which is slightly lower than that of cubic LLZO (c-LLZO) with a Li-ion conductivity of 1.63 × 10-3 S/cm. Furthermore, we discovered that Li-ion conductivity can be influenced by adjusting the elemental ratios within a-LLZO. This suggests that fine-tuning the composition of a-LLZO can potentially further enhance its Li-ion conductivity and optimize its performance as a solid electrolyte in lithium batteries.

Variant Plateau's law in atomically thin transition metal dichalcogenide dome networks.

Since its fundamental inception from soap bubbles, Plateau's law has sparked extensive research in equilibrated states. However, most studies primarily relied on liquids, foams or cellular structures, whereas its applicability has yet to be explored in nano-scale solid films. Here, we observed a variant Plateau's law in networks of atomically thin domes made of solid two-dimensional (2D) transition metal dichalcogenides (TMDs). Discrete layer-dependent van der Waals (vdWs) interaction energies were experimentally and theoretically obtained for domes protruding in different TMD layers. Significant surface tension differences from layer-dependent vdWs interaction energies manifest in a variant of this fundamental law. The equivalent surface tension ranges from 2.4 to 3.6 N/m, around two orders of magnitude greater than conventional liquid films, enabling domes to sustain high gas pressure and exist in a fundamentally variant nature for several years. Our findings pave the way towards exploring variant discretised states with applications in opto-electro-mechanical devices.

Enhanced interactions of interlayer excitons in free-standing heterobilayers.

Strong, long-range dipole-dipole interactions between interlayer excitons (IXs) can lead to new multiparticle correlation regimes1,2, which drive the system into distinct quantum and classical phases2-5, including dipolar liquids, crystals and superfluids. Both repulsive and attractive dipole-dipole interactions have been theoretically predicted between IXs in a semiconductor bilayer2,6-8, but only repulsive interactions have been reported experimentally so far3,9-16. This study investigated free-standing, twisted (51°, 53°, 45°) tungsten diselenide/tungsten disulfide (WSe2/WS2) heterobilayers, in which we observed a transition in the nature of dipolar interactions among IXs, from repulsive to attractive. This was caused by quantum-exchange-correlation effects, leading to the appearance of a robust interlayer biexciton phase (formed by two IXs), which has been theoretically predicted6-8 but never observed before in experiments. The reduced dielectric screening in a free-standing heterobilayer not only resulted in a much higher formation efficiency of IXs, but also led to strongly enhanced dipole-dipole interactions, which enabled us to observe the many-body correlations of pristine IXs at the two-dimensional quantum limit. In addition, we firstly observed several emission peaks from moiré-trapped IXs at room temperature in a well-aligned, free-standing WSe2/WS2 heterobilayer. Our findings open avenues for exploring new quantum phases with potential for applications in non-linear optics.

Quantum spin Hall effect in tilted penta silicene and its isoelectronic substitutions.

Silicene, a competitive two-dimensional (2D) material for future electronic devices, has attracted intensive attention in condensed matter physics. Utilizing an adaptive genetic algorithm (AGA), we identify a topological allotrope of silicene, named tilted penta (tPenta) silicene. Based on first-principles calculations, the geometric and electronic properties of tPenta silicene and its isoelectronic substitutions (Ge, Sn) are investigated. Our results indicate that tPenta silicene exhibits a semimetallic state with distorted Dirac cones in the absence of spin-orbit coupling (SOC). When SOC is considered, it shows semiconducting behavior with a gap opening of 2.4 meV at the Dirac point. Based on the results of invariant ( = 1) and the helical edge states, we demonstrate that tPenta silicene is a topological insulator. Furthermore, the effect of isoelectronic substitutions on tPenta silicene is studied. Two stoichiometric phases, i.e., tPenta Si0.333Ge0.667 and tPenta Si0.333Sn0.667 are found to retain the geometric framework of tPenta silicene and exhibit high stabilities. Our calculations show that both tPenta Si0.333Ge0.667 and tPenta Si0.333Sn0.667 are QSH insulators with enlarged band gaps of 32.5 meV and 94.3 meV, respectively, at the HSE06 level, offering great potential for practical applications at room temperature.

Inorganic Lead-Free B-γ-CsSnI3 Perovskite Solar Cells Using Diverse Electron-Transporting Materials: A Simulation Study.

B-γ-CsSnI3 perovskite solar cells (PSCs) are simulated employing diverse electron-transporting layers (ETLs, including TiO2, ZnO, SnO2, GaN, C60, and PCBM), and a comparative study has been made. Both regular and inverted planar structures are simulated. Effects of the thickness of absorbers and ETLs, doping of ETLs, and interface trap states on the photovoltaic performance are studied to optimize the device structures. The regular structures have larger short-circuit current density (J sc) than the inverted structures, but the inverted structures have larger fill factor (FF). All of the simulated optimal PSCs have similar open-circuit voltages (V oc) of ∼0.96 V. The PSCs with TiO2 ETLs have the best photovoltaic performance, and the optimum structure exhibits the highest efficiency of 20.2% with a V oc of 0.97 V, J sc of 29.67 mA/cm2, and FF of 0.70. The optimal PSCs with ZnO, GaN, C60, and PCBM ETLs exhibit efficiencies of 17.88, 18.09, 16.71, and 16.59%, respectively. The optimal PSC with SnO2 ETL exhibits the lowest efficiency of 15.5% in all of the simulated PSCs due to its cliff-like band offset at the SnO2/CsSnI3 interface. Furthermore, the increase of interface trap density and capture cross section is found to reduce the photovoltaic performance of PSCs. This work contributes to designing and fabricating CsSnI3 PSCs.

Direct Measurement of Folding Angle and Strain Vector in Atomically Thin WS2 Using Second-Harmonic Generation.

Structural engineering techniques such as local strain engineering and folding provide functional control over critical optoelectronic properties of 2D materials. Local strain engineering at the nanoscale level is practically achieved via permanently deformed wrinkled nanostructures, which are reported to show photoluminescence enhancement, bandgap modulation, and funneling effect. Folding in 2D materials is reported to tune optoelecronic properties via folding angle dependent interlayer coupling and symmetry variation. The accurate and efficient monitoring of local strain vector and folding angle is important to optimize the performance of optoelectronic devices. Conventionally, the accurate measurement of both strain amplitude and strain direction in wrinkled nanostructures requires the combined usage of multiple tools resulting in manufacturing lead time and cost. Here, we demonstrate the usage of a single tool, polarization-dependent second-harmonic generation (SHG), to determine the folding angle and strain vector accurately and efficiently in ultrathin WS2. The folding angle in trilayer WS2 folds exhibiting 1-9 times SHG enhancement is probed through variable approaches such as SHG enhancement factor, maxima and minima SHG phase difference, and linear dichroism. In compressive strain induced wrinkled nanostructures, strain-dependent SHG quenching and enhancement is observed parallel and perpendicular, respectively, to the direction of the compressive strain vector, allowing us to determine the local strain vector accurately using a photoelastic approach. We further demonstrate that SHG is highly sensitive to band-nesting-induced transition (C-peak), which can be significantly modulated by strain. Our results show SHG as a powerful probe to folding angle and strain vector.

A super-stretchable boron nanoribbon network.

We have studied the mechanical properties of a two-dimensional (2D) boron nanoribbon network (BNRN) subjected to a uniaxial or a biaxial tensile strain using first principles calculations. The results show that the 2D BNRN is super-stretchable. The critical tensile strains of the BNRN in the χ-h1 phase along the a- and b-directions are 0.51 and 0.41, respectively, and that for the biaxial strain reaches an ultrahigh value of 0.84. By analyzing the B-B interatomic distance, coordination number and charge distribution, it is found that with increasing biaxial tensile strain, the χ-h1 BNRN undergoes two structural phase transitions, which are characterized by breaking of the B-B bonds and the partial transformation of the nanoribbon-like structures into chain-like structures. The strain-induced phase transitions significantly reduce the strain energy. We also discuss the elastic constants, Young's modulus, shear modulus, and Poisson's ratios. The super-stretchable and flexible mechanical properties of the BNRNs, together with their superior transport properties, make BNRNs useful in a wide range of applications in nanoscale electronic devices.

Excited State Biexcitons in Atomically Thin MoSe2.

The tightly bound biexcitons found in atomically thin semiconductors have very promising applications for optoelectronic and quantum devices. However, there is a discrepancy between theory and experiment regarding the fundamental structure of these biexcitons. Therefore, the exploration of a biexciton formation mechanism by further experiments is of great importance. Here, we successfully triggered the emission of biexcitons in atomically thin MoSe2, via the engineering of three critical parameters: dielectric screening, density of trions, and excitation power. The observed binding energy and formation dynamics of these biexcitons strongly support the model that the biexciton consists of a charge attached to a trion (excited state biexciton) instead of four spatially symmetric particles (ground state biexciton). More importantly, we found that the excited state biexcitons not only can exist at cryogenic temperatures but also can be triggered at room temperature in a freestanding bilayer MoSe2. The demonstrated capability of biexciton engineering in atomically thin MoSe2 provides a route for exploring fundamental many-body interactions and enabling device applications, such as bright entangled photon sources operating at room temperature.

New crystal structure prediction of fully hydrogenated borophene by first principles calculations.

New crystal structures of fully hydrogenated borophene (borophane) have been predicted by first principles calculation. Comparing with the chair-like borophane (C-boropane) that has been reported in literature, we obtained four new borophane conformers with much lower total-energy. The most stable one, washboard-like borophane (W-borophane), has energy about 113.41 meV/atom lower than C-borophane. In order to explain the relative stability of different borophane conformers, the atom configuration, density of states, charge transfer, charge density distribution and defect formation energy of B-H dimer have been calculated. The results show that the charge transfer from B atoms to H atoms is crucial for the stability of borophane. In different borophane conformers, the bonding characteristics between B and H atoms are similar, but the B-B bonds in W-borophane are much stronger than that in C-borophane or other structures. In addition, we examined the dynamical stability of borophane conformers by phonon dispersions and found that the four new conformers are all dynamically stable. Finally the mechanical properties of borophane conformers along an arbitrary direction have been discussed. W-borophane possesses unique electronic structure (Dirac cone), good stability and superior mechanical properties. W-borophane has broad perspective for nano electronic device.

High anisotropy of fully hydrogenated borophene.

We have studied the mechanical properties and phonon dispersions of fully hydrogenated borophene (borophane) under strains by first principles calculations. Uniaxial tensile strains along the a- and b-direction, respectively, and biaxial tensile strain have been considered. Our results show that the mechanical properties and phonon stability of borophane are both highly anisotropic. The ultimate tensile strain along the a-direction is only 0.12, but it can be as large as 0.30 along the b-direction. Compared to borophene and other 2D materials (graphene, graphane, silicene, silicane, h-BN, phosphorene and MoS2), borophane presents the most remarkable anisotropy in in-plane ultimate strain, which is very important for strain engineering. Furthermore, the phonon dispersions under the three applied strains indicate that borophane can withstand up to 5% and 15% uniaxial tensile strain along the a- and b-direction, respectively, and 9% biaxial tensile strain, indicating that mechanical failure in borophane is likely to originate from phonon instability.

Degenerate Effect on the Mobility of Holes in Graphane: A Study Based on Density Functional Theory Coupled with Deformation Potential Theory.

The traditional deformation potential method is not able to calculate the charge mobility of heavily doped degenerate semiconductors, in which inter-band scattering is not negligible. To theoretically predict the charge mobility of such semiconductors, an improved deformation potential method is required, in which the deformation potential constant is decomposed into two parts (hydrostatic and uniaxial terms) based on k⋅p theory to incorporate the inter-band scattering between degenerate valence bands. We propose a new method to calculate the heavy- and light-hole mobilities of graphane. The proposed method produces more appropriate values than the traditional methods. Hence, the new method can be applied to other 2D materials with degenerate bands.

Robust Excitons and Trions in Monolayer MoTe2.

Molybdenum telluride (MoTe2) has emerged as a special member in the family of two-dimensional transition metal dichalcogenide semiconductors, owing to the strong spin-orbit coupling and relatively small energy gap, which offers new applications in valleytronic and excitonic devices. Here we successfully demonstrated the electrical modulation of negatively charged (X(-)), neutral (X(0)), and positively charged (X(+)) excitons in monolayer MoTe2 via photoluminescence spectroscopy. The binding energies of X(+) and X(-) were measured to be ∼24 and ∼27 meV, respectively.The exciton binding energy of monolayer MoTe2 was measured to be 0.58 ± 0.08 eV via photoluminescence excitation spectroscopy, which matches well with our calculated value of 0.64 eV.