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Register a new userOn the ab initio calculation of CVV Auger spectra in closed-shell systems
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We propose an ab initio method to evaluate the core-valence-valence (CVV) Auger spectrum of systems with filled valence bands. The method is based on the Cini-Sawatzky theory, and aims at estimating the parameters by first-principles calculations in the framework of density-functional theory (DFT). Photoemission energies and the interaction energy for the two holes in the final state are evaluated by performing DFT simulations for the system with varied population of electronic levels. Transition matrix elements are taken from atomic results. The approach takes into account the non-sphericity of the density of states of the emitting atom, spin-orbit interaction in core and valence, and non quadratic terms in the total energy expansion with respect to fractional occupation numbers. It is tested on two benchmark systems, Zn and Cu metals, leading in both cases to L23M45M45 Auger peaks within 2 eV from the experimental ones. Detailed analysis is presented on the relative weight of the various contributions considered in our method, providing the basis for future development. Especially problematic is the evaluation of the hole-hole interaction for systems with broad valence bands: our method underestimates its value in Cu, while we obtain excellent results for this quantity in Zn.
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An textit{ab initio} electronic structure calculation based on the generalized gradient approximation in the density functional theory is carried out to study the basic electronic states of hollandite vanadate K$_2$V$_8$O$_{16}$. We find that the states near the Fermi energy consist predominantly of the three $t_{2g}$-orbital components and the hybridization with oxygen $2p$ orbitals is small. The $d_{yz}$ and $d_{zx}$ orbitals are exactly degenerate and are lifted from the $d_{xy}$ orbital. The calculated band dispersion and Fermi surface indicate that the system is not purely one-dimensional but the coupling between the VO double chains is important. Comparison with available experimental data suggests the importance of electron correlations in this system.
The first part of this article centers on the fact that key features of the dynamical response of weakly-correlated materials (the alkalis, Al), have been found experimentally to differ qualitatively from simple-model behavior. In the absence of ab initio theory, the surprises embodied in the experimental data were imputed to effects of dynamical correlations. We summarize results of ab initio investigations of linear response, performed within time-dependent density-functional theory (TDDFT), in which the unexpected features of the observed spectra are shown to be due to band-structure effects. Contrary to conventional wisdom, the response cannot be understood universally, in terms of a simple scaling with the density, on going from metal to metal (e.g., through the alkali series) --even the shape of the dispersion curve for the plasmon energy is system-specific. The second part of this article starts out with the observation that a similar ab initio study of systems with more complex electronic structures would require the availability of a realistic approximation for the dynamical many-body kernel entering the density-response function in TDDFT. Thus, we outline a diagrammatic alternative, framed within the conserving-approximation method of Baym and Kadanoff. Using as a benchmark the band gap of Si obtained in the GW approximation, together with a diagrammatic (and conserving) solution of the ensuing Bethe-Salpeter equation, we discuss issues involving conservation laws, self-consistency, and sum rules. These conceptual issues are particularly important for the development of ab initio methods for the study of dynamical response and quasiparticle band structure of strongly-correlated materials. We argue that inclusion of short-range correlations absent in the GW approximation is a must, even in Si.
BaBiO3 is a well-known example of a 3D charge density wavecompound, in which the CDW behavior is induced by charge disproportionation at the Bi site. At ambient pressure, this compound is a charge-ordered insulator, but little is known about its high-pressure behavior. In this work, we study from first-principles the high-pressure phase diagram of BaBiO3 using phonon modes analysis and evolutionary crystal structure prediction. We show that charge disproportionation is very robust in this compound and persists up to 100 GPa. This causes the system to remain insulating up to the highest pressure we studied.
This lecture note reviews recently proposed sparse-modeling approaches for efficient ab initio many-body calculations based on the data compression of Greens functions. The sparse-modeling techniques are based on a compact orthogonal basis representation, intermediate representation (IR) basis functions, for imaginary-time and Matsubara Greens functions. A sparse sampling method based on the IR basis enables solving diagrammatic equations efficiently. We describe the basic properties of the IR basis, the sparse sampling method and its applications to ab initio calculations based on the GW approximation and the Migdal-Eliashberg theory. We also describe a numerical library for the IR basis and the sparse sampling method, irbasis, and provide its sample codes. This lecture note follows the Japanese review article [H. Shinaoka et al., Solid State Physics 56(6), 301 (2021)].
The present paper proposes the direct calculation of the microscopic contributions to the magneto-electric coupling, using ab initio methods. The electrostrictive and the Dzyaloshinskii-Moriya contributions were evaluated individually. For this purpose a specific method was designed, combining DFT calculations and embedded fragments, explicitely correlated, quantum chemical calculations. This method allowed us to calculate the evolution of the magnetic couplings as a function of an applied electric field. We found that in $rm YMnO_3$ the Dzyaloshinskii-Moriya contribution to the magneto-electric effect is three orders of magnitude weaker than the electrostrictive contribution. Strictive effects are thus dominant in the magnetic exchange evolution under an applied electric field, and by extension on the magneto-electric effect. These effects remain however quite small and the modifications of the magnetic excitations under an applied electric field will be difficult to observe experimentally. Another important conclusion is that the amplitude of the magneto-electric effect is very small. Indeed, it can be shown that the linear magneto-electric tensor is null due to the inter-layer symmetry operations.
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