This paper summarises the theory and functionality behind Questaal, an open-source suite of codes for calculating the electronic structure and related properties of materials from first principles. The formalism of the linearised muffin-tin orbital (LMTO) method is revisited in detail and developed further by the introduction of short-ranged tight-binding basis functions for full-potential calculations. The LMTO method is presented in both Green's function and wave function formulations for bulk and layered systems. The suite's full-potential LMTO code uses a sophisticated basis and augmentation method that allows an efficient and precise solution to the band problem at different levels of theory, most importantly density functional theory, LDA+U , quasi-particle self-consistent GW and combinations of these with dynamical mean field theory. This paper details the technical and theoretical bases of these methods, their implementation in Questaal, and provides an overview of the code's design and capabilities. framework of an extension to the linear muffin-tin orbital (LMTO) technique including a highly precise and efficient full-potential implementation. An advanced fully-relativistic, non-collinear implementation based on the atomic sphere approximation is used for calculating transport and magnetic properties.

We present a detailed study of local and nonlocal correlations in the electronic structure of elemental transition metals carried out by means of the quasiparticle self-consistent GW (QSGW) and dynamical mean field theory (DMFT). Recent high resolution ARPES and Haas-van Alphen data of two typical transition metal systems (Fe and Ni) are used as a case study. (i) We find that the properties of Fe are very well described by QSGW. Agreement with cyclotron and very clean ARPES measurements is excellent, provided that final-state scattering is taken into account. This establishes the exceptional reliability of QSGW also in metallic systems. (ii) Nonetheless QSGW alone is not able to provide an adequate description of the Ni ARPES data due to strong local spin fluctuations. We surmount this deficiency by combining nonlocal charge fluctuations in QSGW with local spin fluctuations in DMFT. (iii) Finally we show that the dynamics of the local fluctuations are actually not crucial. The addition of an external static field can lead to similarly good results if nonlocal correlations are included through QSGW.

Using mathematical formalism borrowed from dynamical systems theory, a complete analytical investigation of the critical behaviour of the stationary flow configuration for the low angular momentum axisymmetric black hole accretion provides valuable insights about the nature of the phase trajectories corresponding to the transonic accretion in the steady state, without taking recourse to the explicit numerical solution commonly performed in the literature to study the multi-transonic black hole accretion disc and related astrophysical phenomena. Investigation of the accretion flow around a non rotating black hole under the influence of various pseudo-Schwarzschild potentials and forming different geometric configurations of the flow structure manifests that the general profile of the parameter space divisions describing the multi-critical accretion is roughly equivalent for various flow geometries. However, a mere variation of the polytropic index of the flow cannot map a critical solution from one flow geometry to the another, since the numerical domain of the parameter space responsible to produce multi-critical accretion does not undergo a continuous transformation in multi-dimensional parameter space. The stationary configuration used to demonstrate the aforementioned findings is shown to be stable under linear perturbation for all kind of flow geometries, black hole potentials, and the corresponding equations of state used to obtain the critical transonic solutions. Finally, the structure of the acoustic metric corresponding to the propagation of the linear perturbation studied are discussed for various flow geometries used.

Unconventional superconductivity in Sr 2 RuO 4 has been intensively studied for decades. However, the nature of pairing continues to be widely debated. Here we develop a detailed ab initio theory, coupling quasiparticle self-consistent GW approximation with dynamical mean field theory (DMFT), including both local and non-local correlations to address the subtle interplay among spin, charge and orbital degrees of freedom. We report that the superconducting instability has multiple triplet and singlet components. In the unstrained case the triplet eigenvalues are larger than the singlets. Under uniaxial strain, the triplet eigenvalues drop and the singlet components increase. This is concomitant with our observation of spin and charge fluctuations shifting closer to wave-vectors favoring singlet pairing. We identify a complex mechanism where charge fluctuations and spin fluctuations cooperate in the evenparity channel under strain leading to increment in critical temperature (Tc), thus proposing a novel mechanism for pushing the frontier of critical temperature (Tc) in unconventional 'triplet' superconductors.

High temperature superconductivity has been found in many kinds of compounds built from planes of Cu and O, separated by spacer layers. Understanding why critical temperatures are so high has been the subject of numerous investigations and extensive controversy. To realize high temperature superconductivity, parent compounds are either hole-doped, such as La 2 CuO 4 (LCO) with Sr (LSCO), or electron doped, such as Nd 2 CuO 4 (NCO) with Ce (NCCO). In the electron doped cuprates, the antiferromagnetic phase is much more robust than the superconducting phase. However, it was recently found that the reduction of residual out-of-plane apical oxygens dramatically affects the phase diagram, driving those compounds to a superconducting phase. Here we use a recently developed first principles method to explore how displacement of the apical oxygen (A-O) in LCO affects the optical gap, spin and charge susceptibilities, and superconducting order parameter. By combining quasiparticle self-consistent GW (QSGW ) and dynamical mean field theory (DMFT), that LCO is a Mott insulator; but small displacements of the apical oxygens drive the compound to a metallic state through a localization/delocalization transition, with a concomitant maximum d-wave order parameter at the transition. We address the question whether NCO can be seen as the limit of LCO with large apical displacements, and elucidate the deep physical reasons why the behaviour of NCO is so different than the hole doped materials. We shed new light on the recent correlation observed between T c and the charge transfer gap, while also providing a guide towards the design of optimized high-Tc superconductors. Further our results suggest that strong correlation, enough to induce Mott gap, may not be a prerequisite for high-Tc superconductivity.

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Excitons with large binding energies ~2–3 eV in CrX3 have been characterized as being localized (Frenkel) excitons that emerge from the atomic d − d transitions between the Cr-3d-t2g and eg orbitals. The argument has gathered strength in recent years as the excitons in recently made monolayers are found at almost the same energies as the bulk. The Laporte rule, which restricts such parity forbidden atomic transitions, can relax if a symmetry-breaking mechanism is present. While what can be classified as a purely Frenkel exciton is a matter of definition, we show using an advanced first principles parameter-free approach that these excitons in CrX3, in both its bulk and monolayer variants, have band origin and it is the dp hybridization between Cr and X that primarily acts as the symmetry-breaking mechanism that relaxes the Laporte rule. We show that the character of these excitons is mostly determined by the Cr-d orbital manifold, nevertheless, the fractions of the spectral weight shared with the ligand halogen states increases as the dp hybridization enhances. The hybridization enhances as the halogen atom becomes heavier, bringing the X-p states closer to the Cr-d states in the sequence Cl → Br → I, with an attendant increase in exciton intensity and a decrease in binding energy. By applying a range of different kinds of perturbations that qualitatively mimics the effects originating from the missing vertex in self-energy, we show that moderate changes to the two-particle Hamiltonian that essentially modifies the Cr-d-X-p hybridization, can alter both the intensities and positions of the exciton peaks. A detailed analysis of several deep-lying excitons, with and without strain, elucidates the fact that the exciton is most Frenkel-like in CrCl3 and CrBr3 and acquires mixed Frenkel–Wannier character in CrI3, making the excitons in CrI3 most susceptible to environmental screening and spin–orbit coupling.

We explore the electronic band structure of freestanding monolayers of chromium trihalides CrX 3 , X = Cl, Br, I, within an advanced ab initio theoretical approach based on the use of Green's function functionals. We compare the local density approximation with the quasiparticle self-consistent GW (QSGW) approximation and its self-consistent extension (QSG W ) by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction W. We show that, at all levels of theory, the valence band consistently changes shape in the sequence Cl → Br → I, and the valence band maximum shifts from the M point to the point. By analyzing the dynamic and momentum-dependent self-energy, we show that QSG W adds to the localization of the systems in comparison with QSGW, thereby leading to a narrower band and reduced amount of halogens in the valence band manifold. Further analysis shows that X = Cl is most strongly correlated, and X = I is least correlated (most bandlike) as the hybridization between Cr d and X p enhances in the direction Cl → Br → I. For CrBr 3 and CrI 3 , we observe remarkable differences between the QSGW and QSG W valence band structures, while their eigenfunctions are very similar. We show that weak perturbations, like moderate strain, weak changes to the d-p hybridization, and adding small U , can flip the valence band structures between these two solutions in these materials.