Search results for "ELECTRONIC STRUCTURE"
showing 10 items of 722 documents
Basic Concepts and Methodology
2016
In this chapter, the main concepts relevant for the theoretical study of elementary photochemical processes are briefly reviewed. The notions of vibronic coupling and conical intersection are first introduced. The main basic tools from the molecular electronic structure theory and their use for the exploration of potential energy surfaces are then presented.
Spin Crossover, Liesst, and Niesst-Fascinating Electronic Games in Iron Complexes
1997
Abstract Coordination compounds of transition metal ions with open-shell electron configurations may exhibit dynamic electronic structure phenomena depending on the nature of the coordinating ligand sphere. The change of spin state with temperature (thermal spin crossover”) and light-induced electron transfer processes leading to long-lived metastable states are among the most fascinating electronic games encountered in transition metal compounds and are presently under intensive study by chemists and physicists. The first part of this lecture will survey briefly some highlights of previous work and present recent results on thermal spin crossover in iron(II) compounds. The second part of t…
Néel Vector Induced Manipulation of Valence States in the Collinear Antiferromagnet Mn 2 Au
2020
The coupling of real and momentum space is utilized to tailor electronic properties of the collinear metallic antiferromagnet Mn2Au by aligning the real space Neel vector indicating the direction o...
Quantum chemical simulations of hole self-trapping in semi-ionic crystals
1994
A novel formalism is presented for reliable calculations of the energetics of hole self-trapping in semi-ionic solids with mixed valence bands. Unlike previous model-Hamiltonian-type approaches, it is based on self-consistent quantum chemical INDO simulations of the atomistic and electronic structure of a self-trapped hole, making no a priori assumptions about a particular form of its localization (if any). This formalism is applied to the problem of hole self-trapping in corundum crystals (a -A1203). The hole self-trapping is found to be energetically favorable in the form of a diatomic 02 molecule with strong covalent bonding quite similar to the self-trapped hole (VK-center) in alkali ha…
Mixed-valence molecular four-dot unit for quantum cellular automata: Vibronic self-trapping and cell-cell response
2015
Our interest in this article is prompted by the vibronic problem of charge polarized states in the four-dot molecular quantum cellular automata (mQCA), a paradigm for nanoelectronics, in which binary information is encoded in charge configuration of the mQCA cell. Here, we report the evaluation of the electronic levels and adiabatic potentials of mixed-valence (MV) tetra-ruthenium (2Ru(ii) + 2Ru(iii)) derivatives (assembled as two coupled Creutz-Taube complexes) for which molecular implementations of quantum cellular automata (QCA) was proposed. The cell based on this molecule includes two holes shared among four spinless sites and correspondingly we employ the model which takes into accoun…
Electronic structure of the spin-12quantum magnet TiOCl
2005
We have studied the electronic structure of the spin-$1∕2$ quantum magnet TiOCl by polarization-dependent momentum-resolved photoelectron spectroscopy. From that, we confirm the quasi-one-dimensional nature of the electronic structure along the crystallographic $b$ axis and find no evidence for sizable phonon-induced orbital fluctuations as the origin for the noncanonical phenomenology of the spin-Peierls transition in this compound. A comparison of the experimental data to our own $\mathrm{LDA}+\mathrm{U}$ and Hubbard model calculations reveals a striking lack of understanding regarding the quasi-one-dimensional electron dispersions in the normal state of this compound.
Theoretical analysis of hole self-trapping in ionic solids: Application to the KCl crystal.
1993
A method for the calculation of the hole self-trapping (ST) energy in ionic crystals is proposed. It combines model-Hamiltonian and quantum-chemical approaches. An artificial path for the ST process has been suggested containing (a) a free hole not interacting with the lattice vibrations; (b) a free-hole wave packet localized in a small crystal volume in the form of the real ST state, all crystal ions being in their perfect lattice positions; (c) the final ST state of the hole, accompanied with a corresponding lattice relaxation, including strong displacements of ions belonging to the hole region. Some intermediate states might be adopted between (a) and (b) in order to simplify the calcula…
Effects of the Surface and Finite Temperature on the Electronic Structure of Metal Clusters
1996
The most fascinating feature of simple metal clusters is the existence of the electronic shell structure. This was observed first in alkali[1] and noble metals[2] and later also in some other nontransition metals[3,4,5]. The shell structure is a consequence of nearly free valence electrons confined to a finite volume. A spherical potential will always lead to a shell structure, the origin of which is the orbital angular momentum l and the large degeneracy (2l+1) associated with it. However, this primitive shell structure is strengthened by ’accidental’ degeneracies between states having different principal quantum numbers. Thus the shell structure of a hydrogen atom is different from that o…
Accurate Nonlinear Optical Properties for Small Molecules
2006
During the last decade it became possible to calculate by quantum chemical ab initio methods not only static but also frequency-dependent properties with high accuracy. Today, the most important tools for such calculations are coupled cluster response methods in combination with systematic hierarchies of correlation consistent basis sets. Coupled cluster response methods combine a computationally efficient treatment of electron correlation with a qualitatively correct pole structure and frequency dispersion of the response functions. Both are improved systematically within a hierarchy of coupled cluster models. The present contribution reviews recent advances in the highly accurate calculat…
Electronic structure of a quantum ring in a lateral electric field
2001
The electronic states of novel semiconductor quantum rings (QR's) under applied lateral electric fields are theoretically investigated for different values of the ratio ${r}_{2}{/r}_{1},$ where ${r}_{2}$ ${(r}_{1})$ is the outer (inner) radius of the ring. The eigenstates and eigenvalues of the Hamiltonian are obtained from a direct matrix diagonalization scheme. Numerical calculations are performed for a hard-wall confinement potential and the electronic states are obtained as a function of the electric field and the ratio ${r}_{2}{/r}_{1}.$ An anomalous behavior in the energy vs. electric-field fan plot due to the break of symmetry is predicted. Analytical expressions for the energy level…