Showing papers on "Electronic band structure published in 2021"

Observation of flat bands in twisted bilayer graphene

Abstract: Transport experiments in twisted bilayer graphene have revealed multiple superconducting domes separated by correlated insulating states1–5. These properties are generally associated with strongly correlated states in a flat mini-band of the hexagonal moire superlattice as was predicted by band structure calculations6–8. Evidence for the existence of a flat band comes from local tunnelling spectroscopy9–13 and electronic compressibility measurements14, which report two or more sharp peaks in the density of states that may be associated with closely spaced Van Hove singularities. However, direct momentum-resolved measurements have proved to be challenging15. Here, we combine different imaging techniques and angle-resolved photoemission with simultaneous real- and momentum-space resolution (nano-ARPES) to directly map the band dispersion in twisted bilayer graphene devices near charge neutrality. Our experiments reveal large areas with a homogeneous twist angle that support a flat band with a spectral weight that is highly localized in momentum space. The flat band is separated from the dispersive Dirac bands, which show multiple moire hybridization gaps. These data establish the salient features of the twisted bilayer graphene band structure. Spectroscopic measurements using nano-ARPES on twisted bilayer graphene directly highlight the presence of the flat bands.

Boosting triplet self-trapped exciton emission in Te(IV)-doped Cs 2 SnCl 6 perovskite variants

Abstract: Perovskite variants have attracted wide interest because of the lead-free nature and strong self-trapped exciton (STE) emission. Divalent Sn(II) in CsSnX3 perovskites is easily oxidized to tetravalent Sn(IV), and the resulted Cs2SnCl6 vacancy-ordered perovskite variant exhibits poor photoluminescence property although it has a direct band gap. Controllable doping is an effective strategy to regulate the optical properties of Cs2SnX6. Herein, combining the first principles calculation and spectral analysis, we attempted to understand the luminescence mechanism of Te4+-doped Cs2SnCl6 lead-free perovskite variants. The chemical potential and defect formation energy are calculated to confirm theoretically the feasible substitutability of tetravalent Te4+ ions in Cs2SnCl6 lattices for the Sn-site. Through analysis of the absorption, emission/excitation, and time-resolved photoluminescence (PL) spectroscopy, the intense green-yellow emission in Te4+:Cs2SnCl6 was considered to originate from the triplet Te(IV) ion 3P1→1S0 STE recombination. Temperature-dependent PL spectra demonstrated the strong electron-phonon coupling that inducing an evident lattice distortion to produce STEs. We further calculated the electronic band structure and molecular orbital levels to reveal the underlying photophysical process. These results will shed light on the doping modulated luminescence properties in stable lead-free Cs2MX6 vacancy-ordered perovskite variants and be helpful to understand the optical properties and physical processes of doped perovskite variants.

Self-Doping Surface Oxygen Vacancy-Induced Lattice Strains for Enhancing Visible Light-Driven Photocatalytic H2 Evolution over Black TiO2.

Abstract: The synergistic effect of surface oxygen vacancy with induced lattice strains on visible light-driven photocatalytic H2 evolution over black TiO2 was investigated. Experimental measurements and theoretical calculations on the lattice parameters of black TiO2 show that surface oxygen vacancies induce internal lattice strain during two-step aluminothermic reduction, which regulates the band structure and optimizes the photoinduced charge behavior of black TiO2. The hydrogen evolution rate of black TiO2 with strain modification shows a 12-fold increase to 1.882 mmol/g· h (equal to 4.705 μmol/cm2·h) under visible light illumination. The metastable state caused by the surface oxygen vacancies leads to the formation of a high-energy surface, which enhances visible light absorption and improves the photoinduced charge separation efficiency. Furthermore, the internal lattice strain provides the driving force and channel for the directional movement of photoinduced electrons from the bulk to the high-energy surface for photocatalytic H2 evolution. This strategy provides a new method for designing a high-performance photocatalyst for H2 production.

Dirac cone, flat band and saddle point in kagome magnet YMn 6 Sn 6 .

Abstract: Kagome-lattices of 3d-transition metals hosting Weyl/Dirac fermions and topological flat bands exhibit non-trivial topological characters and novel quantum phases, such as the anomalous Hall effect and fractional quantum Hall effect. With consideration of spin-orbit coupling and electron correlation, several instabilities could be induced. The typical characters of the electronic structure of a kagome lattice, i.e., the saddle point, Dirac-cone, and flat band, around the Fermi energy (EF) remain elusive in magnetic kagome materials. We present the experimental observation of the complete features in ferromagnetic kagome layers of YMn6Sn6 helically coupled along the c-axis, by using angle-resolved photoemission spectroscopy and band structure calculations. We demonstrate a Dirac dispersion near EF, which is predicted by spin-polarized theoretical calculations, carries an intrinsic Berry curvature and contributes to the anomalous Hall effect in transport measurements. In addition, a flat band and a saddle point with a high density of states near EF are observed. These multi-sets of kagome features are of orbital-selective origin and could cause multi-orbital magnetism. The Dirac fermion, flat band and saddle point in the vicinity of EF open an opportunity in manipulating the topological properties in magnetic materials.

High-Pressure Synthesis of Dirac Materials: Layered van der Waals Bonded BeN 4 Polymorph

Abstract: High-pressure chemistry is known to inspire the creation of unexpected new classes of compounds with exceptional properties. Here, we employ the laser-heated diamond anvil cell technique for synthesis of a Dirac material BeN_{4}. A triclinic phase of beryllium tetranitride tr-BeN_{4} was synthesized from elements at ∼85 GPa. Upon decompression to ambient conditions, it transforms into a compound with atomic-thick BeN_{4} layers interconnected via weak van der Waals bonds and consisting of polyacetylene-like nitrogen chains with conjugated π systems and Be atoms in square-planar coordination. Theoretical calculations for a single BeN_{4} layer show that its electronic lattice is described by a slightly distorted honeycomb structure reminiscent of the graphene lattice and the presence of Dirac points in the electronic band structure at the Fermi level. The BeN_{4} layer, i.e., beryllonitrene, represents a qualitatively new class of 2D materials that can be built of a metal atom and polymeric nitrogen chains and host anisotropic Dirac fermions.

Exotic Topological Bands and Quantum States in Metal-Organic and Covalent-Organic Frameworks

Abstract: ConspectusMetal-organic and covalent-organic frameworks (MOFs/COFs) have been extensively studied for fundamental interests and their promising applications, taking advantage of their unique structural properties, i.e., high porosity and large surface-to-volume ratio. However, their electronic and magnetic properties have been somewhat overlooked because of their relatively poor performance as conductive and/or magnetic materials. Recent experimental breakthroughs in synthesizing two-dimensional (2D) π-conjugated MOFs/COFs with high conductivity and robust magnetism through doping have generated renewed and increasing interest in their electronic properties. Meanwhile, comprehensive theoretical studies of the underlying physical principles have led to discovery of many exotic quantum states, such as topological insulating states, which were only observed in inorganic systems. Especially, the diversity and high tunability of MOFs/COFs have provided a playground to explore novel quantum physics and quantum chemistry as well as promising applications.The band theory has empowered us to understand the most fundamental electronic properties of inorganic crystalline materials, which can also be used to better understand MOFs/COFs. The first obvious difference between the two is that instead of atomic orbitals residing at lattice sites of inorganic crystals, molecular orbitals of organic ligands are predominant in MOFs/COFs. The second key difference is that usually all atomic orbitals in an inorganic crystal are subject to one common group of lattice symmetry, while atomic orbitals of metal ion and molecular orbitals of different organic ligands in MOFs/COFs belong to different subgroups of lattice symmetries. Both these differences will impact the band structure of MOFs/COFs, in particular making it more complex. Consequently, which subset of bands are of most importance depends strongly on the location of Fermi level, i.e., electron counting and charge doping. Furthermore, there are usually two types of characteristic electrons coupled in MOFs, i.e., strongly correlated localized d and f electrons and diffusive s and p electrons, which interplay with lattice, orbital, and spin degrees of freedom, leading to more exotic topological and magnetic band structures.In this Account, we present an up-to-date review of recent theoretical developments to better understand the exotic band structures of MOFs/COFs. Starting from three fundamental 2D lattice models, i.e., honeycomb, Kagome, and Lieb lattices, exotic Dirac and flat bands as well as the intriguing topological quantum states they host, e.g., quantum spin Hall and quantum anomalous Hall states, are outlined. In addition to the single-lattice models, we further elaborate on combined lattice model Hamiltonians, which give rise to overlapping bands hosting novel quantum states, such as nodal-line Dirac semimetal and unconventional superconducting states. Also, first-principles predictions of candidate MOFs/COFs that host these exotic bands and hence quantum phases are reviewed, which greatly extends the pool of materials beyond inorganic crystals for hosting exotic band structures.

Semiconductor-to-metal transition in bilayer MoSi$_2$N$_4$ and WSi$_2$N$_4$ with strain and electric field

Abstract: With exceptional electrical and mechanical properties and at the same time air-stability, layered MoSi2N4 has recently draw great attention. However, band structure engineering via strain and electric field, which is vital for practical applications, has not yet been explored. In this work, we show that the biaxial strain and external electric field are effective ways for the band gap engineering of bilayer MoSi$_2$N$_4$ and WSi$_2$N$_4$. It is found that strain can lead to indirect band gap to direct band gap transition. On the other hand, electric field can result in semiconductor to metal transition. Our study provides insights into the band structure engineering of bilayer MoSi$_2$N$_4$ and WSi$_2$N$_4$ and would pave the way for its future nanoelectronics and optoelectronics applications.

Nodeless kagome superconductivity in LaRu 3 Si 2

Abstract: We report muon spin rotation (μSR) experiments together with first-principles calculations on microscopic properties of superconductivity in the kagome superconductor LaRu3Si2 with Tc≃ 7K. Below Tc, μSR reveals type-II superconductivity with a single s-wave gap, which is robust against hydrostatic pressure up to 2 GPa. We find that the calculated normal state band structure features a kagome flat band, and Dirac as well as van Hove points formed by the Ru-dz2 orbitals near the Fermi level. We also find that electron-phonon coupling alone can only reproduce a small fraction of Tc from calculations, which suggests other factors in enhancing Tc such as the correlation effect from the kagome flat band, the van Hove point on the kagome lattice, and the high density of states from narrow kagome bands. Our experiments and calculations taken together point to nodeless moderate coupling kagome superconductivity in LaRu3Si2.

Moiré superlattice on the surface of a topological insulator

Abstract: Twisting van der Waals heterostructures to induce correlated many body states provides a novel tuning mechanism in solid state physics. In this work, we theoretically investigate the fate of the surface Dirac cone of a three-dimensional topological insulator subject to a superlattice potential. Using a combination of diagrammatic perturbation theory, lattice model simulations, and ab initio calculations we elucidate the unique aspects of twisting a single Dirac cone with an induced moir\'e potential and the role of the bulk topology on the reconstructed surface band structure. We report a dramatic renormalization of the surface Dirac cone velocity as well as demonstrate a topological obstruction to the formation of isolated minibands. Due to the topological nature of the bulk, surface band gaps cannot open; instead additional satellite Dirac cones emerge, which can be highly anisotropic and made quite flat. We discuss the implications of our findings for future experiments.

Pressure dependence of structural, elastic, electronic, thermodynamic, and optical properties of van der Waals-type NaSn2P2 pnictide superconductor: Insights from DFT study

Abstract: NaSn2P2 is a recently discovered superconducting system belonging to a particular class of materials with van der Waals (vdW) structure. There is enormous interest in vdW compounds because of their intriguing electrical, optical, chemical, thermal, and superconducting state properties. We have studied the pressure dependent structural, thermo-physical, electronic band structure, and superconducting state properties of this quasi-two dimensional system in details for the first time via ab initio technique. The optical properties are also investigated for different electric field polarizations for the first time. Structural, electronic, and optical properties were explored via density functional theory (DFT) calculations. Thermal properties were investigated using the quasi-harmonic Debye model. NaSn2P2 is found to be mechanically stable in the pressure range 0–3.0 GPa. The elastic anisotropy indices point towards high level of mechanical and bonding anisotropy in NaSn2P2 consistent with its highly layered structure. The elastic constants, moduli, and Debye temperature (θD) show non-monotonic variation with pressure, particularly close to 1.0 GPa. The pressure dependent superconducting transition temperature, Tc, of NaSn2P2 is predicted to vary strongly with the pressure dependent variation of θD. The electronic energy dispersion curves, E(k), reveal high level of direction dependence; the effective masses of charge carries are particularly high for the out-of-plane (c-axis) charge transport. The optical parameters compliment the underlying electronic energy density of states features and are weakly dependent on the polarization of the incident electric field. The reflectivity of NaSn2P2 is very high in the visible region and remains quite high and non-selective over an extended energy range in the ultraviolet region. The absorption coefficient is also high in the mid-ultraviolet band. All these optical features render NaSn2P2 suitable for optoelectronic device applications.

Layered Perovskite Oxyiodide with Narrow Band Gap and Long Lifetime Carriers for Water Splitting Photocatalysis.

Abstract: The development of semiconductors with narrow band gap and high stability is crucial for achieving solar to chemical energy conversion. Compounds with iodine, which has a high polarizability, have attracted attention because of their narrow band gap and long carrier lifetime, as typified by halide perovskite solar cells; however, they have been regarded as unsuitable for harsh photocatalytic water splitting because iodine is prone to self-oxidation. Here, we demonstrate that Ba2Bi3Nb2O11I, a layered Sillen-Aurivillius oxyiodide, not only has access to a wider range of visible light than its chloride and bromide counterparts, but also functions as a stable photocatalyst, efficiently oxidizing water. Density functional theory calculations reveal that the oxygen 2p orbitals in the perovskite block, rather than the fluorite Bi2O2 block as previously pointed out, anomalously push up the valence band maximum, which can be explained by a modified Madelung potential analysis that takes into account the high polarizability of iodine. In addition, the highly polarizable iodide contributes to longer carrier lifetime of Ba2Bi3Nb2O11I, allowing for a significantly higher quantum efficiency than its chloride and bromide counterparts. Visible-light-driven Z-scheme water splitting was achieved for the first time in an iodine-based system using Ba2Bi3Nb2O11I as an oxygen-evolution photocatalyst. The present study provides a novel approach for incorporating polarizable "soft" anions into building blocks of layered materials to manipulate the band structure and improve the carrier dynamics for visible-light responsive functions.

Transport and recombination properties of group-III doped SiCNTs

Abstract: Silicon carbide nanotubes (SiCNTs) have attracted extensive scientific and commercial interest due to their excellent properties. Based on the first principles, the lattice and energy band structure of group III element-doped SiCNTs are studied, it is found that when the electronegativity of the doped atoms is less than that of the surrounding atoms, except for an acceptor energy level near the top of the valence band, a deep impurity level is also produced near the conduction band. Numerical simulation results show that the substitution of silicon is beneficial to improve the transport performance of SiCNTs, while the substitution of C atoms is more beneficial to the improvement of recombination performance. Further analysis showed that the dominant role in the transport process of doped SiCNTs is the optical phonon scattering mechanism. The increase in non-equilibrium minority carrier lifetime when C is substituted is due to the large acceptor ionization energy, which reduces the trapping rate of holes. This will improve the photon excitation and radiation performance of doped SiCNTs.

Dynamic band structure measurement in the synthetic space

Abstract: Band structure theory plays an essential role in exploring physics in both solid-state systems and photonics. Here, we demonstrate a direct experimental measurement of the dynamic band structure in a synthetic space including the frequency axis of light, realized in a ring resonator under near-resonant dynamic modulation. This synthetic lattice exhibits the physical picture of the evolution of the wave vector reciprocal to the frequency axis in the band structure, analogous to a one-dimensional lattice under an external force. We experimentally measure the trajectories of the dynamic band structure by selectively exciting the band with a continuous wave source with its frequency scanning across the entire energy regime of the band. Our results not only provide a new perspective for exploring the dynamics in fundamental physics of solid-state and photonic systems with the concept of the synthetic dimension but also enable great capability in band structure engineering in photonics.

Interaction-Driven Filling-Induced Metal-Insulator Transitions in 2D Moiré Lattices.

Abstract: Using a realistic band structure for twisted ${\mathrm{WSe}}_{2}$ materials, we develop a theory for the interaction-driven correlated insulators to conducting metals transitions through the tuning of the filling factor around commensurate fractional fillings of the moir\'e unit cell in the 2D honeycomb lattice, focusing on the dominant half-filled Mott insulating state, which exists for both long- and short-range interactions. We find metallic states slightly away from half-filling, as have recently been observed experimentally. We discuss the stabilities and the magnetic properties of the resulting insulating and metallic phases, and comment on their experimental signatures. We also discuss the nature of the correlated insulator states at the rational fractional fillings.

Cubic AgMnSbTe3 Semiconductor with a High Thermoelectric Performance.

Abstract: The reaction of MnTe with AgSbTe2 in an equimolar ratio (ATMS) provides a new semiconductor, AgMnSbTe3. AgMnSbTe3 crystallizes in an average rock-salt NaCl structure with Ag, Mn, and Sb cations statistically occupying the Na sites. AgMnSbTe3 is a p-type semiconductor with a narrow optical band gap of ∼0.36 eV. A pair distribution function analysis indicates that local distortions are associated with the location of the Ag atoms in the lattice. Density functional theory calculations suggest a specific electronic band structure with multi-peak valence band maxima prone to energy convergence. In addition, Ag2Te nanograins precipitate at grain boundaries of AgMnSbTe3. The energy offset of the valence band edge between AgMnSbTe3 and Ag2Te is ∼0.05 eV, which implies that Ag2Te precipitates exhibit a negligible effect on the hole transmission. As a result, ATMS exhibits a high power factor of ∼12.2 μW cm-1 K-2 at 823 K, ultralow lattice thermal conductivity of ∼0.34 W m-1 K-1 (823 K), high peak ZT of ∼1.46 at 823 K, and high average ZT of ∼0.87 in the temperature range of 400-823 K.

Reconstruction of moiré lattices in twisted transition metal dichalcogenide bilayers

Abstract: An important step in understanding the exotic electronic, vibrational, and optical properties of the moir\'e lattices is the inclusion of the effects of structural relaxation of the unrelaxed moir\'e lattices. Here, we propose novel structures for twisted bilayer of transition metal dichalcogenides. For $\ensuremath{\theta}\ensuremath{\gtrsim}58.{4}^{\ensuremath{\circ}}$, we show a dramatic reconstruction of the moir\'e lattices, leading to a trimerization of the unfavorable stackings. We show that the development of curved domain walls due to the threefold symmetry of the stacking energy landscape is responsible for such lattice reconstruction. Furthermore, we show that the lattice reconstruction notably changes the electronic band structure. This includes the occurrence of flat bands near the edges of the conduction as well as valence bands, with the valence band maximum, in particular, corresponding to localized states enclosed by the trimer. We also find possibilities for other complicated, entropy stabilized, lattice reconstructed structures.

Direct extrapolation techniques on the energy band diagram of BiVO4 thin films

Abstract: Bismuth vanadate (BiVO4) is one of the n-type semiconductors which has attracted attention as one of the promising photoanodes semiconductor for photoelectrochemical water splitting due to its small optical band gap, low cost, negative conduction band edge and good stability. In this work, BiVO4 thin films is fabricated by using electrodeposition method and the XRD spectra reveal that the sample crystallizes in monoclinic scheelite type. The optical bands show the bandgap energy of BiVO4 thin films is 2.40 eV as determined by Tauc plot and exhibits an anodic photocurrent. Further study is focusing on determination of the conduction band (CB) and valence band (VB) of BiVO4 thin films which is derived experimentally by using XPS analysis, Mott–Schottky plot and Cyclic Voltammetry (CV) technique. Based on the results, it is found that different analysis techniques exhibit almost similar values of CB and VB of BiVO4 thin films. All techniques give VB maximum in the range of 2.02 eV–2.05 eV and CB minimum in the range of −0.35 eV to −0.39 eV. However, the flat-band potential determined from Mott–Schottky plot is nearly 0.1 eV from CB potential caused by the presence of Fermi level and the effect of Helmholtz capacitance for dielectric semiconductors. These findings clearly show that the experimental values of different analysis techniques give comprehensive approach to understanding the energy band structure of the BiVO4 thin films.

Creation of moiré bands in a monolayer semiconductor by spatially periodic dielectric screening.

Abstract: Moire superlattices of two-dimensional van der Waals materials have emerged as a powerful platform for designing electronic band structures and discovering emergent physical phenomena. A key concept involves the creation of long-wavelength periodic potential and moire bands in a crystal through interlayer electronic hybridization or atomic corrugation when two materials are overlaid. Here we demonstrate a new approach based on spatially periodic dielectric screening to create moire bands in a monolayer semiconductor. This approach relies on reduced dielectric screening of the Coulomb interactions in monolayer semiconductors and their environmental dielectric-dependent electronic band structure. We observe optical transitions between moire bands in monolayer WSe2 when it is placed close to small-angle-misaligned graphene on hexagonal boron nitride. The moire bands are a result of long-range Coulomb interactions, which are strongly gate tunable, and can have versatile superlattice symmetries independent of the crystal lattice of the host material. Our result also demonstrates that monolayer semiconductors are sensitive local dielectric sensors.

Band structure and superconductivity in twisted trilayer graphene

Abstract: We study the symmetries of twisted trilayer graphene's band structure under various extrinsic perturbations, and analyze the role of long-range electron-electron interactions near the first magic angle. The electronic structure is modified by these interactions in a similar way to twisted bilayer graphene. We analyze electron pairing due to long-wavelength charge fluctuations, which are coupled among themselves via the Coulomb interaction and additionally mediated by longitudinal acoustic phonons. We find superconducting phases with either spin-singlet/valley-triplet or spin-triplet/valley-singlet symmetry, with critical temperatures up to a few Kelvin for realistic choices of parameters.

Measurement of Conduction and Valence Bands g-Factors in a Transition Metal Dichalcogenide Monolayer.

Abstract: The electron valley and spin degree of freedom in monolayer transition-metal dichalcogenides can be manipulated in optical and transport measurements performed in magnetic fields. The key parameter for determining the Zeeman splitting, namely, the separate contribution of the electron and hole g factor, is inaccessible in most measurements. Here we present an original method that gives access to the respective contribution of the conduction and valence band to the measured Zeeman splitting. It exploits the optical selection rules of exciton complexes, in particular the ones involving intervalley phonons, avoiding strong renormalization effects that compromise single particle g-factor determination in transport experiments. These studies yield a direct determination of single band g factors. We measure g_{c1}=0.86±0.1, g_{c2}=3.84±0.1 for the bottom (top) conduction bands and g_{v}=6.1±0.1 for the valence band of monolayer WSe_{2}. These measurements are helpful for quantitative interpretation of optical and transport measurements performed in magnetic fields. In addition, the measured g factors are valuable input parameters for optimizing band structure calculations of these 2D materials.