density functional theory calculations
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Materials ◽  
2022 ◽  
Vol 15 (2) ◽  
pp. 648
Han Yan ◽  
Xiong Xu ◽  
Peng Li ◽  
Peijie He ◽  
Qing Peng ◽  

Ultrathin silver films with low loss in the visible and near-infrared spectrum range have been widely used in the fields of metamaterials and optoelectronics. In this study, Al-doped silver films were prepared by the magnetron sputtering method and were characterized by surface morphology, electrical conductivity, and light transmittance analyses. Molecular dynamics simulations and first-principles density functional theory calculations were applied to study the surface morphologies and migration pathway for the formation mechanisms in Al-doped silver films. The results indicate that the migration barrier of silver on a pristine silver surface is commonly lower than that of an Al-doped surface, revealing that the aluminum atoms in the doping site decrease the surface mobility and are conducive to the formation of small islands of silver. When the islands are dense, they coalesce into a single layer, leading to a smoother surface. This might be the reason for the observably lower 3D growth mode of silver on an Al-doped silver surface. Our results with electronic structure insights on the mechanism of the Al dopants on surface morphologies might benefit the quality control of the silver thin films.

2022 ◽  
Vol 12 (1) ◽  
Yichen Jin ◽  
Mouhui Yan ◽  
Tomislav Kremer ◽  
Elena Voloshina ◽  
Yuriy Dedkov

AbstractA broad family of the nowadays studied low-dimensional systems, including 2D materials, demonstrate many fascinating properties, which however depend on the atomic composition as well as on the system dimensionality. Therefore, the studies of the electronic correlation effects in the new 2D materials is of paramount importance for the understanding of their transport, optical and catalytic properties. Here, by means of electron spectroscopy methods in combination with density functional theory calculations we investigate the electronic structure of a new layered van der Waals $$\hbox {FePX}_3$$ FePX 3 (X: S, Se) materials. Using systematic resonant photoelectron spectroscopy studies we observed strong resonant behavior for the peaks associated with the $$3d^{n-1}$$ 3 d n - 1 final state at low binding energies for these materials. Such observations clearly assign $$\hbox {FePX}_3$$ FePX 3 to the class of Mott–Hubbard type insulators for which the top of the valence band is formed by the hybrid Fe-S/Se electronic states. These observations are important for the deep understanding of this new class of materials and draw perspectives for their further applications in different application areas, like (opto)spintronics and catalysis.

2022 ◽  
Vol 7 (1) ◽  
M. Garnica ◽  
M. M. Otrokov ◽  
P. Casado Aguilar ◽  
I. I. Klimovskikh ◽  
D. Estyunin ◽  

AbstractWe study the surface crystalline and electronic structures of the antiferromagnetic topological insulator MnBi2Te4 using scanning tunneling microscopy/spectroscopy (STM/S), micro(μ)-laser angle-resolved photoemission spectroscopy (ARPES), and density functional theory calculations. Our STM images reveal native point defects at the surface that we identify as BiTe antisites and MnBi substitutions. Bulk X-ray diffraction further evidences the presence of the Mn-Bi intermixing. Overall, our characterizations suggest that the defects concentration is nonuniform within crystals and differs from sample to sample. Consistently, the ARPES and STS experiments reveal that the Dirac point gap of the topological surface state is different for different samples and sample cleavages, respectively. Our calculations show that the antiparallel alignment of the MnBi moments with respect to those of the Mn layer can indeed cause a strong reduction of the Dirac point gap size. The present study provides important insights into a highly debated issue of the MnBi2Te4 Dirac point gap.

Nanomaterials ◽  
2022 ◽  
Vol 12 (2) ◽  
pp. 236
Jinyun Liu ◽  
Yajun Zhu ◽  
Junfei Cai ◽  
Yan Zhong ◽  
Tianli Han ◽  

Long-term stable secondary batteries are highly required. Here, we report a unique microcapsule encapsulated with metal organic foams (MOFs)-derived Co3O4 nanocages for a Li-S battery, which displays good lithium-storage properties. ZIF-67 dodecahedra are prepared at room temperature then converted to porous Co3O4 nanocages, which are infilled into microcapsules through a microfluidic technique. After loading sulfur, the Co3O4/S-infilled microcapsules are obtained, which display a specific capacity of 935 mAh g−1 after 200 cycles at 0.5C in Li-S batteries. A Coulombic efficiency of about 100% is achieved. The constructed Li-S battery possesses a high rate-performance during three rounds of cycling. Moreover, stable performance is verified under both high and low temperatures of 50 °C and −10 °C. Density functional theory calculations show that the Co3O4 dodecahedra display large binding energies with polysulfides, which are able to suppress shuttle effect of polysulfides and enable a stable electrochemical performance.

2022 ◽  
Heigo Ers ◽  
Liis Siinor ◽  
Carolin Siimenson ◽  
Enn Lust ◽  
Piret Pikma

The interface between semi-metallic Sb(111) electrode and ionic liquid with 4,4’-bipyridine addition has been studied. Using in situ scanning tunnelling microscopy and electrochemical impedance spectroscopy, the desorption of 4,4’-bipyridine was demonstrated and a dense underlying structure, formed below a sparse self-assembled monolayer, was visualized. The first SAM layer in contact with the electrode consisted of tightly packed ordered rows, which fine structure has been identified with density functional theory calculations supported by machine learning. The second SAM layer, on top of the first, is characterised by low surface concentration and its unit cell was obtained experimentally. The detection of two separate adsorbed layers indicates that the ordering of organic molecules could extend well beyond the monolayer on the electrode’s surface. These insights are of fundamental and practical importance in the development of nanoelectronic devices.

2022 ◽  
Vol 13 (1) ◽  
Yan Shao ◽  
Wei Gao ◽  
Hejin Yan ◽  
Runlai Li ◽  
Ibrahim Abdelwahab ◽  

AbstractMolecularly soft organic-inorganic hybrid perovskites are susceptible to dynamic instabilities of the lattice called octahedral tilt, which directly impacts their carrier transport and exciton-phonon coupling. Although the structural phase transitions associated with octahedral tilt has been extensively studied in 3D hybrid halide perovskites, its impact in hybrid 2D perovskites is not well understood. Here, we used scanning tunneling microscopy (STM) to directly visualize surface octahedral tilt in freshly exfoliated 2D Ruddlesden-Popper perovskites (RPPs) across the homologous series, whereby the steric hindrance imposed by long organic cations is unlocked by exfoliation. The experimentally determined octahedral tilts from n = 1 to n = 4 RPPs from STM images are found to agree very well with out-of-plane surface octahedral tilts predicted by density functional theory calculations. The surface-enhanced octahedral tilt is correlated to excitonic redshift observed in photoluminescence (PL), and it enhances inversion asymmetry normal to the direction of quantum well and promotes Rashba spin splitting for n > 1.

2022 ◽  
Vol 5 (1) ◽  
Ole Bunjes ◽  
Lucas A. Paul ◽  
Xinyue Dai ◽  
Hongyan Jiang ◽  
Tobias Claus ◽  

AbstractAtomic scale studies of the anchoring of catalytically active complexes to surfaces may provide valuable insights for the design of new catalytically active hybrid systems. In this work, the self-assembly of 1D, 2D and 3D structures of the complex fac-Re(bpy)(CO)3Cl (bpy = 2,2′-bipyridine), a CO2 reduction catalyst, on the Ag(001) surface are studied by a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Infrared and sum frequency generation spectroscopy confirm that the complex remains chemically intact under sublimation. Deposition of the complexes onto the silver surface at 300 K leads to strong local variations in the resulting surface coverage on the nanometer scale, indicating that in the initial phase of deposition a large fraction of the molecules is desorbing from the surface. Low coverage regions show a decoration of step edges aligned along the crystal’s symmetry axes <110>. These crystallographic directions are found to be of major importance to the binding of the complexes to the surface. Moreover, the interaction between the molecules and the substrate promotes the restructuring of surface steps along these directions. Well-aligned and decorated steps are found to act as nucleation point for monolayer growth (2D) before 3D growth starts.

2022 ◽  
Vol 3 (1) ◽  
pp. 15-26
Argyris Tilemachou ◽  
Matthew Zervos ◽  
Andreas Othonos ◽  
Theodoros Pavloudis ◽  
Joseph Kioseoglou

Cu3N with a cubic crystal structure is obtained in this paper by the sputtering of Cu under N2 followed by annealing under NH3: H2 at 400 °C, after which it was doped with iodine at room temperature resulting into p-type Cu3N with hole densities between 1016 and 1017 cm−3. The Cu3N exhibited distinct maxima in differential transmission at ~2.01 eV and 1.87 eV as shown by ultrafast pump-probe spectroscopy, corresponding to the M and R direct energy band gaps in excellent agreement with density functional theory calculations, suggesting that the band gap is clean and free of mid-gap states. The Cu3N was gradually converted into optically transparent γ-CuI that had a hole density of 4 × 1017 cm−3, mobility of 12 cm2/Vs and room temperature photoluminescence at 3.1 eV corresponding to its direct energy band gap. We describe the fabrication and properties of γ-CuI/TiO2/Cu3N and γ-CuI/Cu3N p-n heterojunctions that exhibited rectifying current-voltage characteristics, but no photogenerated current attributed to indirect recombination via shallow states in Cu3N and/or deep states in the γ-CuI consistent with the short (ps) lifetimes of the photoexcited electrons-holes determined from transient absorption–transmission spectroscopy.

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