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Register a new userFirst principles vs second principles: Role of charge self-consistency in strongly correlated systems
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First principles approaches have been successful in solving many-body Hamiltonians for real materials to an extent when correlations are weak or moderate. As the electronic correlations become stronger often embedding methods based on first principles approaches are used to better treat the correlations by solving a suitably chosen many-body Hamiltonian with a higher level theory. Such combined methods are often referred to as second principles approaches. At such level of the theory the self energy, i.e. the functional that embodies the stronger electronic correlations, is either a function of energy or momentum or both. The success of such theories is commonly measured by the quality of the self energy functional. However, self-consistency in the self-energy should, in principle, also change the real space charge distribution in a correlated material and be able to modify the electronic eigenfunctions, which is often undermined in second principles approaches. Here we study the impact of charge self-consistency within two example cases: TiSe$_{2}$, a three-dimensional charge-density-wave candidate material, and CrBr$_{3}$, a two-dimensional ferromagnet, and show how real space charge re-distribution due to correlation effects taken into account within a first principles Greens function based many-body perturbative approach is key in driving qualitative changes to the final electronic structure of these materials.
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The fluctuations of the magnetic order parameter, or longitudinal spin excitations, are investigated theoretically in the ferromagnetic Fe and Ni as well as in the antiferromagnetic phase of the pnictide superconductor FeSe. The charge and spin dynamics of these systems is described by evaluating the generalized charge and spin density response function calculated from first-principles linear response time dependent density functional theory within adiabatic local spin density approximation. We observe that the formally non-interacting Kohn-Sham system features strong coupling between the magnetization and charge dynamics in the longitudinal channel and that the coupling is effectively removed upon the inclusion of the Coulomb interaction in the charge channel and the resulting appearance of plasmons. The longitudinal spin fluctuations acquire a collective character without the emergence of the Goldstone boson, similar to the case of paramagnon excitations in non-magnetic metals like Pd. In ferromagnetic Fe and Ni the longitudinal spin dynamics is governed by interactions between low-energy intraband electron-hole pairs while in quasi two dimensional antiferromagnet FeSe it is dominated by the interband transitions with energies of the order of exchange splitting. In the later material, the collective longitudinal magnetization fluctuations feature well defined energies and long life times for small momenta and appear below the particle-hole continuum. The modes become strongly Landau-damped for growing wave-vectors. We relate our theoretical findings to existing experimental spin-polarized electron energy loss spectroscopy results. In bulk bcc Fe, the longitudinal magnetic modes appear above the typical energies of transverse spin-waves, have energies comparable with the Stoner spin-flip excitation continuum, and are order of magnitude less energetic than the charge dynamics.
We present results of an ab-initio study of the electronic structure of 140 rare earth compounds. Specifically we predict an electronic phase diagram of the entire range of rare earth monopnictides and monochalcogenides, composed of metallic, semiconducting and heavy fermion-like regions, and exhibiting valency transitions brought about by a complex interplay between ligand chemistry and lanthanide contraction. The calculations exploit the combined effect of a first-principles methodology, which can adequately describe the dual character of electrons, itinerant vs. localized, and high throughput computing made possible by the increasing available computational power. Our findings, including the predicted intermediate valent compounds SmO and TmSe, are in overall excellent agreement with the available experimental data. The accuracy of the approach, proven e.g. through the lattice parameters calculated to within 1.5% of the experimental values, and its ability to describe localization phenomena in solids, makes it a competitive atomistic simulation approach in the search for and design of new materials with specific physical properties and possible technological applications.
The interplay between multiple bands, sizable multi-band electronic correlations and strong spin-orbit coupling may conspire in selecting a rather unusual unconventional pairing symmetry in layered Sr$_{2}$RuO$_{4}$. This mandates a detailed revisit of the normal state and, in particular, the $T$-dependent incoherence-coherence crossover. Using a modern first-principles correlated view, we study this issue in the actual structure of Sr$_{2}$RuO$_{4}$ and present a unified and quantitative description of a range of unusual physical responses in the normal state. Armed with these, we propose that a new and important element, that of dominant multi-orbital charge fluctuations in a Hunds metal, may be a primary pair glue for unconventional superconductivity. Thereby we establish a connection between the normal state responses and superconductivity in this system.
Vanadium dioxide(VO$_2$) is a paradigmatic example of a strongly correlated system that undergoes a metal-insulator transition at a structural phase transition. To date, this transition has necessitated significant post-hoc adjustments to theory in order to be described properly. Here we report standard state-of-the-art first principles quantum Monte Carlo (QMC) calculations of the structural dependence of the properties of VO$_2$. Using this technique, we simulate the interactions between electrons explicitly, which allows for the metal-insulator transition to naturally emerge, importantly without ad-hoc adjustments. The QMC calculations show that the structural transition directly causes the metal-insulator transition and a change in the coupling of vanadium spins. This change in the spin coupling results in a prediction of a momentum-independent magnetic excitation in the insulating state. While two-body correlations are important to set the stage for this transition, they do not change significantly when VO$_2$ becomes an insulator. These results show that it is now possible to account for electron correlations in a quantitatively accurate way that is also specific to materials.
Many inorganic pigments contain heavy metals hazardous to health and environment. Much attention has been devoted to the quest for non-toxic alternatives based on rare-earth elements. The computation of colors from first principles is a challenge to electronic structure methods however, especially for materials with localized f-orbitals. Here, starting from atomic positions only, we compute the color of the red pigment cerium fluorosulfide CeSF, as well as of mercury sulfide HgS (classic vermilion). Our methodology employs many-body theories to compute the optical absorption, combined with an intermediate length-scale modelization to assess how coloration depends on film thickness, pigment concentration and granularity. We introduce a quantitative criterion for the performance of a pigment. While for HgS this criterion is satisfied due to large transition matrix elements between wide bands, CeSF presents an alternative paradigm: the bright red color is shown to stem from the combined effect of the quasi two-dimensionality and the localized nature of 4f-states. Our work demonstrates the power of modern computational methods, with implications for the theoretical design of materials with specific optical properties.
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