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Effect of excess electron on structure, bonding, and spectral properties of sulfur/selenium based dichalcogen systems
摘要： First principle based quantum chemical methods are employed to characterize structure, bonding, and spectral properties of sulfur and selenium based dichalcogen systems in presence of an excess electron. Inter molecular two-center three-electron (2c-3e) bonding between two chalcogen (X) atoms is described in the systems of the type (R-X)2?- (R = Ph, PhCH2 X = S, Se). In addition, effect of electron withdrawing (-NO2) and electron donating (-CH3) groups in phenyl ring on the stability of these 2c-3e bonded systems is also studied in water medium applying a macroscopic hydration model. Molecular parameters and binding energy of the neutral, (R-X)2 and reduced, (R-X)2?- dichalcogen systems are compared. Search for minimum energy structures of these open shell doublet systems are carried out applying various density functionals with dispersion corrections and MP2 method considering 6-311++G (d,p) set of basis functions for all atoms. Effect of water medium is introduced through a macroscopic solvation model based on density (SMD). Frontier molecular orbitals based analysis is carried out for showing the definite presence of 2c-3e bond between two chalcogen atoms in these radical anions of sulfur and selenium based aromatic dichalcogen systems. Excited state calculations are performed on all these systems using Time Dependent Density Functional Theory (TDDFT). UV-Vis spectra are simulated and effect of solvent water on the absorption maximum of these radical anions is discussed. This study illustrates that the combination of electronic effect and geometrical flexibility decides the strength of two-center three-electron bond in these systems.
关键词： sulfur,hemi bond,radical anion,density functional theory,chalcogen,excess electron,2c-3e bond,antioxidant,selenium
更新于2025-09-04 15:30:14
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Formation mechanism of twin domain boundary in 2D materials: The case for WTe2
摘要： Our scanning tunneling microscopy (STM) study observes, for the first time, twin domain boundary (TDB) formations on the surface of WTe2 single crystal, which is glued by solidifying indium to Si substrate. In these TDB regions, a large inhomogeneous strain field, especially a critical shear strain of about 7%, is observed by geometric phase analysis. This observation does not obey the old believe that a small mechanical stress is sufficient to drive thermally-induced TDB formations in two-dimensional materials. To resolve the contradiction, we perform density functional theory calculations combined with elasticity theory analysis, which show that TDBs on WTe2 are entirely displacement-induced, for which a critical strain is necessary to overcome the onset barrier.
关键词： WTe2,twin domain boundary,density functional theory,strain,scanning tunneling microscopy (STM)
更新于2025-09-04 15:30:14
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Adsorption properties of O2 on the unequal amounts of binary co-doped graphene by B/N and P/N: A density functional theory study
摘要： Graphene acts as an advanced substrate material, and it has been used as an electrode in fuel cells because it can efficiently adsorb oxygen molecules. In this study, density functional theory (DFT) calculation has been performed to exactly simulate the adsorption and dissociation of oxygen molecules on the XY3-co-doped graphene. The results show that the positively charged P and B atoms act as active sites for oxygen adsorption on the surface of graphene. In addition, PN3-G and NP3-G exhibit higher catalytic activity than the other samples because of the facile transfer of electrons from the highest occupied molecular orbital (HOMO) of O2 to the orbital above the Fermi level in the samples. More interestingly, excessive adsorption leads to the direct dissociation of oxygen molecules and making further dissociation difficult. In conclusion, the adsorption of oxygen molecules at the hollow sites on the PN3-G and NP3-G occurs via the formation of a triangular ring or trans-formation into O2? is proposed as the optimal strategy because these routes are thermodynamically favorable and the associated energy barrier is low. Furthermore, after dissociation, it was found that the oxygen atoms preferably approach the P atom. This work may be useful as a reference for future experimental studies to develop effective metal-free catalysts for fuel-cell cathodes.
关键词： Density functional theory (DFT),XY3 co-doping,Graphene,Electron transfer,Adsorption
更新于2025-09-04 15:30:14
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Effective doublon and hole temperatures in the photo-doped dynamic Hubbard model
摘要： Hirsch’s dynamic Hubbard model describes the effect of orbital expansion with occupancy by coupling the doublon operator to an auxiliary boson. In the Mott insulating phase, empty sites (holes) and doubly occupied orbitals (doublons) become charge carriers on top of the half-filled background. We use the nonequilibrium dynamical mean field method to study the properties of photo-doped doublons and holes in this model in the strongly correlated regime. In particular, we discuss how photodoping leads to doublon and hole populations with different effective temperatures, and we analyze the relaxation behavior as a function of the boson coupling and boson energy. In the polaronic regime, the nontrivial energy exchange between doublons, holes, and bosons can result in a negative temperature distribution for the holes.
关键词： effective temperatures,doublons,holes,photo-doping,dynamic Hubbard model,nonequilibrium dynamical mean field theory
更新于2025-09-04 15:30:14
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LATTICE MAXWELL'S EQUATIONS (Invited Paper)
摘要： We discuss the ab initio rendering of four-dimensional (4-d) spacetime of Maxwell’s equations on random (irregular) lattices. This rendering is based on casting Maxwell’s equations in the framework of the exterior calculus of di?erential forms, and a translation thereof to a simplicial complex whereby ?elds and causative sources are represented as di?erential p-forms and paired with the oriented p-dimensional geometrical objects that comprise the set of spacetime lattice cells (simplices). We pay particular attention to the case of simplicial spacetime lattices because these can serve as building blocks of lattices made of more generic cells (polygons). The generalized Stokes’ theorem is used to construct discrete calculus operations on the lattice based upon combinatorial relations depending solely on the connectivity and relative orientation among simplices. This rendering provides a natural factorization of (lattice) 4-d spacetime Maxwell’s equations into a metric-free part and a metric-dependent part. The latter is encoded by discrete Hodge star operators which are built using Whitney forms, i.e., canonical interpolants for discrete di?erential forms. The derivation of Whitney forms is illustrated here using a geometrical construction based on the concept of barycentric coordinates to represent a point on a simplex, and the generalization thereof to represent higher-dimensional objects (lines, areas, volumes, and hypervolumes) in 4-d. We stress the role of the primal lattice, the barycentric dual lattice, and the barycentric decomposition lattice in achieving a complete description of the lattice theory. Lattice Maxwell’s equations based on the exterior calculus of di?erential forms and on the use of Whitney forms as ?eld interpolants inherits the symplectic structure and discrete analogues of conservation laws present in the continuum theory, such as energy and charge conservation. It also provides precise localization rules for the degrees of freedom associated with the di?erent ?elds and sources on the lattice, and design principles for constructing consistent numerical solution methods that are free from spurious modes, spectral pollution, and (unconditional) numerical instabilities. We also brie?y consider the relationship between lattice 4-d Maxwell’s equations and some incarnations of discretization schemes for Maxwell’s equations in (3 + 1)-d, such as ?nite-di?erences and ?nite-elements.
关键词： exterior calculus,Maxwell’s equations,lattice theory,differential forms,Hodge star operators,Whitney forms
更新于2025-09-04 15:30:14
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Tuning the Electronic Structure of Hydrogen-Decorated Silicene
摘要： The effects of strain, charge doping, and external electric field on the electronic structure of a free-standing silicene layer decorated by hydrogen atoms are studied by first-principles density functional theory. Various phases, including insulating, metallic, spin-polarized, and half-metallic have been found, depending on these external factors. The most efficient way of switching the system between these phases is charge doping. The character of the energy gap of the H/silicene system can also be modified, and for charged or for strained systems, the originally indirect gap can be tuned to become direct. The obtained results are very promising in view of the silicene functionalization and potential applications of silicene in the fields of spintronics and optoelectronics.
关键词： density functional theory (DFT),silicene,functionalization
更新于2025-09-04 15:30:14
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First-Principles Study of Point Defects in GaAs/AlAs Superlattice: the Phase Stability and the Effects on the Band Structure and Carrier Mobility
摘要： Advanced semiconductor superlattices play important roles in critical future high-tech applications such as aerospace, high-energy physics, gravitational wave detection, astronomy, and nuclear related areas. Under such extreme conditions like high irradiative environments, these semiconductor superlattices tend to generate various defects that ultimately may result in the failure of the devices. However, in the superlattice like GaAs/AlAs, the phase stability and impact on the device performance of point defects are still not clear up to date. The present calculations show that in GaAs/AlAs superlattice, the antisite defects are energetically more favorable than vacancy and interstitial defects. The AsX (X = Al or Ga) and XAs defects always induce metallicity of GaAs/AlAs superlattice, and GaAl and AlGa antisite defects have slight effects on the electronic structure. For GaAs/AlAs superlattice with the interstitial or vacancy defects, significant reduction of band gap or induced metallicity is found. Further calculations show that the interstitial and vacancy defects reduce the electron mobility significantly, while the antisite defects have relatively smaller influences. The results advance the understanding of the radiation damage effects of the GaAs/AlAs superlattice, which thus provide guidance for designing highly stable and durable semiconductor superlattice based electronic and optoelectronics for extreme environment applications.
关键词： Point defect,Electrical properties,GaAs/AlAs superlattice,Hybrid density functional theory
更新于2025-09-04 15:30:14
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Matching Multi-Sensor Remote Sensing Images via an Affinity Tensor
摘要： Matching multi-sensor remote sensing images is still a challenging task due to textural changes and non-linear intensity differences. In this paper, a novel matching method is proposed for multi-sensor remote sensing images. To establish feature correspondences, an affinity tensor is used to integrate geometric and radiometric information. The matching process consists of three steps. First, features from an accelerated segment test are extracted from both source and target images, and two complete graphs are constructed with their nodes representing these features. Then, the geometric and radiometric similarities of the feature points are represented by the three-order affinity tensor, and the initial feature correspondences are established by tensor power iteration. Finally, a tensor-based mismatch detection process is conducted to purify the initial matched points. The robustness and capability of the proposed method are tested with a variety of remote sensing images such as Ziyuan-3 backward, Ziyuan-3 nadir, Gaofen-1, Gaofen-2, unmanned aerial vehicle platform, and Jilin-1. The experiments show that the average matching recall is greater than 0.5, which outperforms state-of-the-art multi-sensor image-matching algorithms such as SIFT, SURF, NG-SIFT, OR-SIFT and GOM-SIFT.
关键词： matching blunder detection,affinity tensor,multi-sensor remote sensing image,graph theory,image matching
更新于2025-09-04 15:30:14
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Intrinsic correlation between electronic structure and degradation: from few layers to bulk black phosphorus
摘要： Black phosphorus (BP) has received much attention due to its fascinating properties, such as a high mobility and tunable band gap which covers the band gap lacuna between graphene and transition metal dichalcogenides. However, these advantages have been overshadowed due to the fast degradation of BP in ambient conditions. To overcome this obstacle, the degradation mechanisms should be unveiled with direct observation followed by a thorough analysis. Here, we reveal two sequential degradation processes and layer-dependent degradation rates of BP under dark conditions by scanning Kelvin probe microscopy (SKPM) measurements and theoretical modeling. The layer-dependent degradation is successfully interpreted with the oxidation model based on the Marcus-Gerischer theory (MGT). Under dark conditions, the electron transfer rate from BP to oxygen molecule depends on the number of layers that give different carrier concentrations. The oxidation rate is strongly dependent on the number of layers, and thus carrier concentrations. This suggests the possibility of stability improvement by carrier modulation. This work not only provides a deeper understanding of the degradation mechanism itself but also suggest new strategies for stable BP-based electronics design.
关键词： oxidation model,degradation,work function,Marcus-Gerischer theory,black phosphorus
更新于2025-09-04 15:30:14
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Insight of surface treatments for CMOS compatibility of InAs nanowires
摘要： A CMOS compatible process is presented in order to grow self-catalyzed InAs nanowires on silicon by molecular beam epitaxy. The crucial step of this process is a new in-situ surface preparation under hydrogen (gas or plasma) during the substrate degassing combined with an in-situ arsenic annealing prior to growth. Morphological and structural characterizations of the InAs nanowires are presented and growth mechanisms are discussed in detail. The major influence of surface termination is exposed both experimentally and theoretically using statistics on ensemble of nanowires and density functional theory (DFT) calculations. The differences observed between Molecular Beam Epitaxy (MBE) and Metal Organic Vapor Phase Epitaxy (MOVPE) growth of InAs nanowires can be explained by these different surfaces terminations. The transition between a vapor solid (VS) and a vapor liquid solid (VLS) growth mechanism is presented. Optimized growth conditions lead to very high aspect ratio nanowires (up to 50 nm in diameter and 3 micron in length) without passing the 410 °C thermal limit, which makes the whole process CMOS compatible. Overall, our results suggest a new method for surface preparation and a possible tuning of the growth mechanism using different surface terminations.
关键词： nanowires,growth modeling,self-catalyzed growth,hydrogen preparation,density functional theory (DFT) modeling,III-V semiconductors on silicon,InAs
更新于2025-09-04 15:30:14