arXiv subjects

Alberto Carta

Publications and source records attributed to Alberto Carta.

10 recordsLinked to original sources

arXiv2026

Strong correlations and local self-energies from on-site ensembles

Addressing the many-body electronic-structure problem is a central goal of modern condensed-matter physics. Paramagnetic Mott insulators, in particular, have long represented a challenge for standard approaches, such as density-functional theory. Historically, these systems have been tackled either by considering many-body dynamics, as in the case of dynamical mean-field theory (DMFT), or, more recently, by invoking a polymorphous description consisting of large supercells populated with static symmetry-broken motifs whose spatial average restores the paramagnetic state. Inspired by these viewpoints, we introduce the on-site dephased ensemble (DE) approximation, in which the local electronic-structure problem is described by a thermal ensemble of all accessible local static solutions; this gives rise to a strong frequency dependence of the local electronic self-energy, as seen in DMFT or in the coherent-potential approximation of disordered alloys. We show that the DE successfully recovers defining hallmarks of strongly correlated Mott systems, both in terms of the self-energy as well as the persistence of local moments in time, in quantitative agreement with DMFT. By bypassing expensive quantum Monte Carlo solvers or large supercell calculations, this approach offers efficient routes to treating paramagnetic Mott systems in a first-principles setting, and highlights a deeper connection between the physics of strong correlations and that of disorder.

cond-mat.str-el↗

arXiv2026

DFT+U+V is equivalent to DFT+U with density-dependent hybridized projectors

Hubbard-corrected density-functional theory (DFT+$U$) is a popular tool for first-principles modeling of materials with localized $d$ or $f$ electrons, but its on-site corrections tend to over-localize charge and break covalent bonds. Inter-site $+V$ corrections were introduced to counter this and are now widely used, but a formal justification has been lacking. Here we show that -- to first order in $V/U$ -- inter-site corrections are exactly equivalent to on-site DFT+$U$ evaluated on a density-matrix-dependent redefinition of the Hubbard projectors, hybridized with those of neighboring sites, providing insight into the explicit mechanism by which $V$ affects covalency. If the projectors are held frozen, as is common practice, the equivalence partially breaks down. Beyond reinterpreting the formalism, these results sharpen the questions of how $V$ should be computed and what the Hubbard subspaces fundamentally are.

cond-mat.mtrl-sci↗

arXiv2026

Probing the real-space density of spin-entangled electrons

On the textbook example of an isolated antiferromagnetic Heisenberg dimer, we demonstrate that the magnetic form factor and the magnetic electron density distribution can be extracted from the momentum-dependence of the inelastic neutron scattering (INS) intensity of a magnetic excitation. We measure the three-dimensional (3D) magnetic structure factor of the singlet-to-triplet excitation in Cu(II) acetate monohydrate with INS. Using a minimal parametrization of the magnetic electron density, we deduce the real-space density of the spin-entangled electrons and the transfer of magnetic electron density between metal and ligand atoms from the experimental data. Density functional theory (DFT) calculations reproduce the measured structure factor quantitatively, providing a direct validation of DFT broken-symmetry spin densities against full 3D INS data. The quantitative agreement between experiment, parametrization, and theory establishes a robust framework for determining magnetic form factors and the magnetic electron density in a broad range of magnetic materials and demonstrates INS as a probe of the envelope of spatial electronic wavefunctions.

cond-mat.str-el↗

arXiv2025

Hubbard dimer physics and the magnetostructural transition in the correlated cluster material Nb$_3$Cl$_8$

We present a combined computational and experimental study of Nb$_3$Cl$_8$, a correlated layered material containing Nb trimers, through the lens of competing intra- and intercluster interactions. Different proposed explanations for its magnetostructural transition such as charge disproportionation, antiferromagnetic quenching, and interlayer singlet formation are investigated in light of the various reported low-temperature structures. Our findings rule out the previously proposed charge-disproportionation, suggest an intricate interplay between Mott physics and the formation of interlayer singlets, and also hint at a possible explanation of the observed intratrimer scissoring distortion. We suggest that the physics of Nb$_3$Cl$_8$ should be understood in the context of weakly coupled Hubbard dimers.

cond-mat.str-el↗

arXiv2025

Bridging constrained random-phase approximation and linear response theory for computing Hubbard parameters

The predictive accuracy of popular extensions to density-functional theory (DFT) such as DFT+U and DFT plus dynamical mean-field theory (DFT+DMFT) hinges on using realistic values for the screened Coulomb interaction U. Here, we present a systematic comparison of the two most widely used approaches to compute this parameter, i.e. linear response theory (LRT) and the constrained random-phase approximation (cRPA), using a unified framework based on the use of maximally localized Wannier functions. We show that the U in LRT and cRPA can differ as much as 30%. We demonstrate that this discrepancy arises from two main differences: neglecting the response of the exchange-correlation potential in cRPA and additional excitation channels in LRT. By taking these differences into account, we can achieve near perfect agreement between the two techniques. Moreover, we show that in cases with strong hybridization between interacting and screening subspaces, the application of cRPA becomes ambiguous and can lead to unrealistically small U values, while LRT remains well-behaved. Our work formally connects both methods, sheds light on their strengths and limitations, and emphasizes the importance of using a consistent set of Wannier orbitals to ensure transferability of U values between different implementations.

cond-mat.str-el↗

arXiv2025

(Anti-)Altermagnetism from Orbital Ordering in the Ruddlesden-Popper Chromates Sr$_{n+1}$Cr$_n$O$_{3n+1}$

Altermagnets are collinear antiferromagnets with spin-split electronic states. We introduce Ruddlesden-Popper chromates Sr$_{n+1}$Cr$_n$O$_{3n+1}$ (including SrCrO$_3$) as candidate materials in which altermagnetism can emerge from spontaneous orbital ordering rather than crystal symmetry. First-principles calculations reveal a layer-dependent spin splitting: if the spin and orbital orders align in adjacent layers, the system exhibits non-relativistic spin splitting, and thus altermagnetism. In contrast, if either the spin or the orbital order is reversed in adjacent layers, we observe a layerwise uncompensated spin splitting, that is compensated in the adjacent layer, giving rise to the concept of anti-altermagnetism. In the RP series, odd $n$ members support coexistence of altermagnetism and anti-altermagnetism, whereas even $n$ and the perovskite limit are strictly anti-altermagnetic. In both cases, larger $n$ favors metallicity, and in odd $n$ compounds strain can further stabilize altermagnetism.

cond-mat.mtrl-sci↗

arXiv2024

Explicit demonstration of the equivalence between DFT+U and the Hartree-Fock limit of DFT+DMFT

Several methods have been developed to improve the predictions of density functional theory (DFT) in the case of strongly correlated electron systems. Out of these approaches, DFT+$U$, which corresponds to a static treatment of the local interaction, and DFT combined with dynamical mean field theory (DFT+DMFT), which considers local fluctuations, have both proven incredibly valuable in tackling the description of materials with strong local electron-electron interactions. While it is in principle known that the Hartree-Fock (HF) limit of the DFT+DMFT approach should recover DFT+$U$, demonstrating this equivalence in practice is challenging, due to the very different ways in which the two approaches are generally implemented. In this work, we introduce a way to perform DFT+$U$ calculations in Quantum ESPRESSO using Wannier functions as calculated by Wannier90, which allows us to use the same Hubbard projector functions both in DFT+$U$ and in DFT+DMFT. We benchmark these DFT+$U$ calculations against DFT+DMFT calculations where the DMFT impurity problem is solved within the HF approximation. Considering a number of prototypical materials including NiO, MnO, LaMnO$_3$, and LuNiO$_3$, we establish the sameness of the two approaches. Finally, we showcase the versatility of our approach by going beyond the commonly used atomic orbital-like projectors by performing DFT+$U$ calculations for VO$_2$ using a special set of bond-centered Wannier functions.

cond-mat.str-el↗

arXiv2024

Electronic Structure and Transport in the Potential Luttinger Liquids CsNb$_3$Br$_7$S and RbNb$_3$Br$_7$S

The crystal structures of ANb$_3$Br$_7$S (A = Rb and Cs) have been refined by single crystal X-ray diffraction, and are found to form highly anisotropic materials based on chains of the triangular Nb$_3$ cluster core. The Nb$_3$ cluster core contains seven valence electrons, six of them being assigned to Nb-Nb bonds within the Nb$_3$ triangle and one unpaired d electron. The presence of this surplus electron gives rise to the formation of correlated electronic states. The connectivity in the structures is represented by one-dimensional [Nb$_3$Br$_7$S]$^-$ chains, containing a sulphur atom capping one face ($\mu_3$) of the triangular niobium cluster, which is believed to induce an important electronic feature. Several types of studies are undertaken to obtain deeper insight into the understanding of this unusual type of material: the crystal structure, morphology and elastic properties are analysed, as well the (photo-) electrical properties and NMR relaxation. Electronic structure (DFT) calculations are performed in order to understand the electronic structure and transport in these compounds, and, based on the experimental and theoretical results, we propose that the electronic interactions along the Nb chains are sufficiently one-dimensional to give rise to Luttinger liquid (rather than Fermi liquid) behaviour of the metallic electrons.

cond-mat.str-el↗

arXiv2023

Emergence of a potential charge disproportionated insulating state in SrCrO$_{3}$

We use a combination of density functional theory (DFT) and dynamical mean-field theory (DMFT) to investigate the potential emergence of a charge-disproportionated insulating phase in SrCrO$_{3}$, whereby the Cr cations disproportionate according to $3\text{Cr}^{4+} \rightarrow 2\text{Cr}^{3+} + \text{Cr}^{6+}$ and arrange in ordered planes perpendicular to the cubic [111] direction. We show that the charge disproportionation couples to a structural distortion where the oxygen octahedra around the nominal Cr$^{6+}$ sites contract, while the octahedra surrounding the Cr$^{3+}$ sites expand and distort. Our results indicate that the charge-disproportionated phase can be stabilized for realistic values of the Hubbard $U$ and Hund's $J$ parameters, but this requires a scaling of the DFT+DMFT double counting correction by at least 35%. The disproportionated state can also be stabilized in DFT+U calculations for a specific magnetic configuration with antiparallel magnetic moments on adjacent Cr$^{3+}$ sites and no magnetic moment on the Cr$^{6+}$ sites. While this phase is higher in energy than other magnetic states that can arise in SrCrO$_{3}$, the presence of an energy minimum suggests that the charge disproportionated state represents a metastable state of SrCrO$_{3}$.

cond-mat.str-el↗

arXiv2022

Evidence for Jahn-Teller-driven metal-insulator transition in strained SrCrO3 from first principles calculations

Using density-functional theory (DFT) and its extension to DFT+$U$, we propose a possible scenario for a strain-induced metal-insulator transition which has been reported recently in thin films of SrCrO$_3$. The metal-insulator transition involves the emergence of a Jahn-Teller (JT) distortion similar to the case of the related rare-earth vanadates, which also exhibit a nominal $d^2$ occupation of the transition metal cation. Our calculations indicate that, for realistic values of the Hubbard $U$ parameter, the unstrained system exhibts a C-type antiferromagnetically ordered ground state, that is already rather close to a JT instability. However, the emergence of the JT distortion is disfavored by the large energetic overlap of the $d_{xz}$/$d_{yz}$ band with the lower lying $d_{xy}$ band. Tensile epitaxial strain lowers the energy of the $d_{xy}$ band relative to $d_{xz}$/$d_{yz}$ and thus brings the system closer to the nominal filling of $d_{xy}^1(d_{xz}d_{yz})^1$. The JT distortion then lifts the degeneracy between the $d_{xz}$ and $d_{yz}$ orbitals and thus allows to open up a gap in the electronic band structure.

cond-mat.str-el↗