Search results for "Electronic Structure"
showing 10 items of 722 documents
On-Surfaces Synthesis on Insulating Substrates
2016
On-surface synthesis has attracted great attention in recent years due to its promising potential for creating functional structures on surfaces. An important aspect of on-surface synthesis is the capability to arrive at covalently linked thermally stable structures that offer the possibility for application even in harsh environments outside ultra-high vacuum conditions. Additionally, covalent linking allows for fabricating conjugated structures with superior electron transport properties. Especially, the latter is of tremendous interest when considering future applications in the field of molecular electronics. Having molecular electronics applications in mind explains the need for decoup…
Electronic structure of the ground and excited states of beta-carboline.
2008
Coupled-cluster calculations are used to compute the energy of conversion between the neutral and the zwitterionic forms of beta-carboline. The stability of the different species is discussed in terms of charge separation and aromatic character, which is related to magnetic criteria. By means of a linear response formalism the vertical excitation energies and oscillator strengths of the lowest singlet states of both structures as well as of the cationic species are determined. General agreement of the relative position and intensity of the different peaks with experimental data is achieved, but the overall spectra are slightly displaced because of solvent effects.
Elementary presentation of self‐consistent intermediate Hamiltonians and proposal of two totally dressed singles and doubles configuration interactio…
1994
Intermediate Hamiltonians are effective Hamiltonians which are defined on an N‐dimensional model space but which only provide n<N exact eigenvalues and the projections of the corresponding eigenvectors onto the model space. For a single root research, the intermediate Hamiltonian may be obtained from the restriction of the Hamiltonian to the model space by an appropriate, uniquely defined dressing of the diagonal energies or of the first column. Approximate self‐consistent dressings may be proposed. The simplest perturbative form gives the same result as the original 2nd order intermediate Hamiltonian or the ‘‘shifted Bk’’ technique but it is of easier implementation. Self‐consistent inclus…
First-principles comparative study of perfect and defective CsPbX3 (X = Br, I) crystals
2020
We thank R. Merkle for numerous fruitful discussions and G. Siegle for experimental assistance. This study was partly supported by the M-ERA-NET project SunToChem (EK). Calculations were performed using computational facilities of St. Petersburg State University and Max Planck Institute for Solid State Research. Open Access funding provided by the Max Planck Society.
Cubic aromaticity in ligand-stabilized doped Au superatoms
2021
The magnetic response of valence electrons in doped gold-based [M@Au8L8]q superatoms (M = Pd, Pt, Ag, Au, Cd, Hg, Ir, and Rh; L = PPh3; and q = 0, +1, +2) is studied by calculating the gauge including magnetically induced currents (GIMIC) in the framework of the auxiliary density functional theory. The studied systems include 24 different combinations of the dopant, total cluster charge, and cluster structure (cubic-like or oblate). The magnetically induced currents (both diatropic and paratropic) are shown to be sensitive to the atomic structure of clusters, the number of superatomic electrons, and the chemical nature of the dopant metal. Among the cubic-like structures, the strongest arom…
Atomic and Electronic Structure of the Corundum (0001) Surface
1996
AbstractThe electronic structure and geometry of the Al terminated corundum (0001) surface were studied using a slab model within the ab-initio Hartree-Fock technique. The distance between the top Al plane and the next O basal plane is found to be considerably reduced on relaxation (by 0.57 Å, i.e. by 68% of the corresponding interlayer distance in the bulk). An interpretation of experimental photoelectron spectra (UPS Hel) and metastable impact electron spectra (MIES) is given. Calculated projected densities of states exhibit a strong dependence on the relaxation of surface atoms.
Influence of the Nature of the Ligand on Dirhodium(II) Carbene Species: A Theoretical Analysis
2008
The influence of three prototypic families of bridging ligands (carboxylate, carboxamidate, and ortho-metalated arylphosphines) on the electronic structure of dirhodium(II) carbene complexes was theoretically analyzed. The calculations indicated that the electron donation of the ligand to the Rh atom, rather than the chelating ability or the metal−ligand orbital mixing, was responsible for tuning carbene charge via back-donation, which can influence the reactivity and selectivity of the dirhodium complexes in catalytic carbene transfer reactions.
Enhanced operational stability through interfacial modification by active encapsulation of perovskite solar cells
2020
Encapsulates are, in general, the passive components of any photovoltaic device that provides the required shielding from the externally stimulated degradation. Here we provide comprehensive physical insight depicting a rather non-trivial active nature, in contrast to the supposedly passive, atomic layer deposition (ALD) grown Al2O3 encapsulate layer on the hybrid perovskite [(FA0.83MA0.17)0.95Cs0.05PbI2.5Br0.5] photovoltaic device having the configuration: glass/FTO/SnO2/perovskite/spiro-OMeTAD/Au/(±) Al2O3. By combining various electrical characterization techniques, our experimental observations indicate that the ALD chemistry produces considerable enhancement of the electronic conductiv…
Spin state, electronic structure and bonding on C-scorpionate [Fe(II)Cl2(tpm)] catalyst: An experimental and computational study
2020
Abstract The Fe(II) spin state in the condensed phase of [Fe(II)Cl2(tpm)] (tpm = [tris(pyrazol-1-yl)methane]; 1) catalyst has been determined through a combined experimental and theoretical investigation of X-Ray Absorption Spectroscopy (XAS) at the FeL2,3-edges and NK-edge. Results indicated that in this phase a mixed singlet/triplet state is plausible. These results have been compared with the already know Fe singlet spin state of the same complex in water solution. A detailed analysis of the electronic structure and bonding mechanism of the catalyst showed that the preference for the low-spin diamagnetic ground state, strongly depends upon the ligands, the bulk solvent and the interactio…
Dielectric response of BaTiO electronic states under AC fields via microsecond time-resolved X-ray absorption spectroscopy
2021
This research was performed under the approval of the Photon Factory Program Advisory Committee (PF-PAC; Contract Numbers 2015G580, 2017G587, and 2019G614) and was financially supported by JSPS KAKENHI Grant Numbers 18H01153 , 19H02426 , and 18K19126 . The experiment for measuring spectra in Fig. 6 (b) was performed on beamline BM26A (proposal MA 2731) at the European Synchrotron Radiation Facility (ESRF), Grenoble, France. We are grateful to Local Contact at the ESRF for providing assistance in using beamline BM26A. Institute of Solid State Physics, University of Latvia as the Center of Excellence has received funding from the European Union’s Horizon 2020 Framework Programme H2020-WIDESPRE…