arXiv subjects

Motoharu Kitatani

Publications and source records attributed to Motoharu Kitatani.

At least 19 recordsLinked to original sources

arXiv2026

Heterostructuring as Gateway to Electron Doping of Nickelate Superconductors

Despite enormous expenditures in the research field, the electron-doped side of nickelate superconductors remains uncharted territory. Substituting the trivalent rare-earth cations by a tetravalent one hitherto failed. Here, we demonstrate by first-principles calculations a disorder-free route to electron dope Ruddlesden-Popper nickelates. When intercalating wide-band-gap insulating layers such as La$X$O$_3$ ($X$=Al, Ga, Sc) into La$_2$NiO$_4$, the extra (LaO)$^+$ layers act as electron donors, releasing carriers into the Ni-3$d$ orbitals. This electron doping puts La$_2$NiO$_4$:La$_2$AlO$_4$ naturally in the optimal region for $d_{x^2-y^2}$-wave superconductivity with T$_c$ exceeding 50 K. The same concept also allows us to electron dope La$_3$Ni$_2$O$_7$, the superconductor in the limelight.

cond-mat.supr-con↗

arXiv2025

Luttinger surface and exchange splitting induced by ferromagnetic fluctuations

Ferromagnetism in the single-orbital Hubbard model, which contains only local Coulomb repulsion and no explicit ferromagnetic exchange interactions, has been extensively studied. However, how the associated fluctuations influence the electronic properties near the transition remains a fundamental issue. Here, by applying the dynamical vertex approximation (D$\Gamma$A) to single-orbital systems with a partially flat band dispersion, we demonstrate that finite-correlation-length ferromagnetic fluctuations generate an emergent Luttinger surface and drive a Fermi surface expansion reminiscent of exchange splitting, even without magnetic order. We further derive an analytical expression that reproduces these effects, clarifying the microscopic origin for fluctuation-driven exchange splitting in correlated electron systems.

cond-mat.str-el↗

arXiv2025

Modulated Dirac bands and integer hopping ratios in a honeycomb lattice of phenalenyl-tessellation molecules

A family of nanographene molecules called phenalenyl-tessellation molecules (PTMs) exhibits two types of zero modes: a $\sqrt{3} \times \sqrt{3}$ type that spreads over the entire molecule and a vacancy-localized type. A periodic system of PTMs is expected to have low-energy bands that strongly reflect the properties of the zero modes of PTMs as effective atoms. In this study, we show that the low-energy Dirac bands in a class of honeycomb PTMs (H-PTM) can be represented by an effective honeycomb model which is determined only by the connections between neighboring effective atoms.The hopping parameters of H-PTM in each direction take positive integer ratios according to the connection order between two PTMs.By structurally designing each PTM, we can change the connection order of the PTMs and hence modulate the energy gap and the Fermi velocity of the Dirac band of the H-PTM. Moreover, we confirm that Dirac bands coexist with vacancy-localized zero modes in the H-PTM with vacancies.The result indicates that the nanographene structure arranging PTMs as effective atoms extends material design freedom that effectively generates a modulated Dirac electron system with coexisting localized electron spins for graphene-based electronic and quantum devices.

cond-mat.mes-hall↗

arXiv2025

Exploration of the potential energy surface for the conformational interconversion of the amyloid $\beta$ peptide at the fibril end

The formation of amyloid fibrils comprising amyloid $\beta$ (A$\beta$) peptides is associated with the pathology of Alzheimer's disease. In this study, we theoretically investigated the A$\beta$ structure at the fibril end using the density functional theory calculation. Several twisted conformations were identified as local minima in which a part of the peptide chain bends upward while the rest remains bound to the lower A$\beta$ monomer. Fibril-to-twisted conformational transition exhibited endothermic behavior, with endothermic energy increasing as more backbone hydrogen bonds were broken. In addition, the loss of van der Waals interaction from the hydrophobic sidechain contributed to endothermicity. The nudged elastic band method was applied to analyze the potential energy surface connecting the fibril and twisted conformations. Comparison of the activation barriers between different twisted conformations revealed that certain twisted conformations returned relatively easily to the fibril conformation, whereas others encountered a higher activation barrier and reverted less readily. Detailed structural analysis revealed that the twisted conformation's propensity to return originates from the local steric hindrance imposed by the sidechain near the torsional axis.

physics.bio-ph↗

arXiv2025

Entanglement in the pseudogap regime of cuprate superconductors

We find a strongly enhanced entanglement within the pseudogap regime of the Hubbard model. This entanglement is estimated from the quantum Fisher information and, avoiding the ill-conditioned analytical continuation, the quantum variance. Both are lower bounds for the actual entanglement that can be calculated from the (antiferromagnetic) susceptibility, obtained here with the dynamical vertex approximation. Our results qualitatively agree with experimental neutron scattering experiments for various cuprates. Theory predicts a $\ln(1/T)$ divergence of the entanglement for low temperatures $T$, which is however cut-off by the onset of superconductivity.

cond-mat.str-el↗

arXiv2025

Strong-coupling high-$T_{\rm c}$ superconductivity in doped correlated band insulators

We explore the superconducting properties of the bilayer Hubbard model, which exhibits a high transition temperature ($T_{\rm c}$) for an $s_{\pm}$ pairing, using a cluster extension of the dynamical mean-field theory. Unlike the single-layer Hubbard model, where the $d$-wave superconductivity emerges by doping the Mott insulator, the parent state of the bilayer system is a correlated band insulator. Above $T_{\rm c}$, slight hole (electron) doping introduces a striking dichotomy between electron and hole pockets: the electron (hole) pocket develops a pseudogap while the other becomes a nearly incipient band. We reveal that the superconductivity is driven by kinetic (potential) energy gain in the underdoped (overdoped) region. We also find a very short coherence length, for which we argue the relevance to multi-orbital physics. Our study offers crucial insights into the superconductivity in the bilayer Hubbard model potentially relevant to La$_3$Ni$_2$O$_7$.

cond-mat.supr-con↗

arXiv2025

Superconducting phase diagram of finite-layer nickelates Nd$_{n+1}$Ni$_n$O$_{2n+2}$

Following the successful prediction of the superconducting phase diagram for infinite-layer nickelates, here we calculate the superconducting $T_{\mathrm{c}}$ vs. the number of layers $n$ for finite-layer nickelates using the dynamical vertex approximation. To this end, we start with density functional theory, and include local correlations non-perturbatively by dynamical mean-field theory for $n=2$ to 7. For all $n$, the Ni $d_{x^2-y^2}$ orbital crosses the Fermi level, but for $n>4$ there are additional $(\pi, \pi)$ pockets or tubes that slightly enhance the layer-averaged hole doping of the $d_{x^2-y^2}$ orbitals beyond the leading $1/n$ contribution stemming from the valence electron count. We finally calculate $T_{\mathrm{c}}$ for the single-orbital $d_{x^2-y^2}$ Hubbard model by dynamical vertex approximation.

cond-mat.str-el↗

arXiv2024

Natural orbital impurity solver for real-frequency properties at finite temperature

We extend the natural orbital impurity solver [PRB 90, 085102 (2014)] to finite temperatures and apply it to calculate spectral and transport properties of correlated electrons within the dynamical mean-field theory. First, we benchmark our method against the exact diagonalization result for small clusters, finding that the natural orbital scheme works well not only for zero temperature but for low finite temperatures. The method yields smooth and sufficiently accurate spectra, which agree well with the results of the numerical renormalization group. Using the smooth spectra, we calculate the electric conductivity and Seebeck coefficient for the two-dimensional Hubbard model at low temperatures which are in the scope of many experiments and practical applications. These results demonstrate the usefulness of the natural orbital framework for obtaining the real frequency information of correlated electron systems.

cond-mat.str-el↗

arXiv2024

Designing a polymerized phenalenyl tessellation molecule to realize a super-honeycomb antiferromagnetic S = 3/2 spin system

In a multiply hydrogenated polymer of phenalenyl tessellation molecules (PTMs), spatially overlapping zero modes appear, and three spin-aligned electron spins per PTM are generated through direct exchange interactions in the strongly correlated electron system. This interaction was used to design a two-dimensional (2D) $S = 3/2$ Heisenberg spin system on a honeycomb lattice. Simulations of the electronic structure using density functional theory with the Wannierization method revealed an array of nonbonding molecular orbitals (zero modes) in the hydrogenated nanographene structure. Our analysis of the onsite interaction strength indicated that each zero mode was half-filled with a spin-active electron owing to electron correlation effects. The low-energy subspace of the resulting zero mode-tight-binding model suggests the formation of a 2D antiferromagnetic $S = 3/2$ Heisenberg system with an entangled quantum spin ground state.

cond-mat.mtrl-sci↗

arXiv2023

Possible bi-stable structures of pyrene-butanoic-acid-linked protein molecules adsorbed on graphene: Theoretical study

We theoretically analyze possible multiple conformations of protein molecules immobilized by 1-pyrenebutanoic-acid-succinimidyl-ester (PASE) linkers on graphene. The activation barrier between two bi-stable conformations exhibited by PASE is confirmed to be based on the steric hindrance effect between a hydrogen on the pyrene group and a hydrogen on the alkyl group of this molecule. Even after the protein is supplemented, this steric hindrance effect remains if the local structure of the linker consisting of an alkyl group and a pyrene group is maintained. Therefore, it is likely that the kinetic behavior of a protein immobilized with a single PASE linker exhibits an activation barrier-type energy surface between the bi-stable conformations on graphene. We discuss the expected protein sensors when this type of energy surface appears and provide a guideline for improving the sensitivity, especially as an oscillator-type biosensor.

physics.chem-ph↗

arXiv2023

Spin fluctuations sufficient to mediate superconductivity in nickelates

Infinite-layer nickelates show high-temperature superconductivity, and the experimental phase diagram agrees well with the one simulated within the dynamical vertex approximation (D$Γ$A). Here, we compare the spin-fluctuation spectrum behind these calculations to resonant inelastic X-ray scattering experiments. The overall agreement is good. This independent cross-validation of the strength of spin fluctuations strongly supports the scenario, advanced by D$Γ$A, that spin-fluctuations are the mediator of the superconductivity observed in nickelates.

cond-mat.supr-con↗

arXiv2023

Optimizing superconductivity: from cuprates via nickelates to palladates

Motivated by cuprate and nickelate superconductors, we perform a comprehensive study of the superconducting instability in the single-band Hubbard model. We calculate the spectrum and superconducting transition temperature $T_{\rm c}$ as a function of filling and Coulomb interaction for a range of hopping parameters, using the dynamical vertex approximation. We find the sweet spot for high $T_{\rm c}$ to be at intermediate coupling, moderate Fermi surface warping, and low hole doping. Combining these results with first principles calculations, neither nickelates nor cuprates are close to this optimum within the single-band description. Instead, we identify some palladates, notably RbSr$_2$PdO$_3$ and $A^{\prime}_2$PdO$_2$Cl$_2$ ($A^{\prime}$=Ba$_{0.5}$La$_{0.5}$), to be virtually optimal, while others, such as NdPdO$_2$, are too weakly correlated.

cond-mat.supr-con↗

arXiv2023

Nematicity-enhanced superconductivity in systems with a non-Fermi liquid behavior

We explore the interplay between nematicity~(spontaneous breaking of the sixfold rotational symmetry), superconductivity, and non-Fermi liquid behavior in partially flat-band models on the triangular lattice. A key result is that the nematicity (Pomeranchuk instability), which is driven by many-body effect and stronger in flat-band systems, enhances superconducting transition temperature in a systematic manner on the $T_{\rm c}$ dome. There, a $s_{x^2+y^2} - d_{x^2-y^2} - d_{xy}$-wave symmetry, in place of the conventional $d_{x^2-y^2}$-wave, governs the nematicity-enhanced pairing with a sharp rise in the $T_{\rm c}$ dome on the filling axis. When the sixfold symmetry is spontaneously broken, the pairing becomes more compact in real space than in the case when the symmetry is enforced. These are accompanied by a non-Fermi character of electrons in the partially flat bands with many-body interactions.

cond-mat.supr-con↗

arXiv2022

$\textit{Ab initio}$ Materials Design of Superconductivity in $d^9$ Nickelates

Motivated by the recent theoretical materials design of superconducting $d^9$ nickelates for which the charge transfer from the NiO$_2$ to the block layer is completely suppressed [M. Hirayama $\textit{et al.}$, Phys. Rev. B $\textbf{101}$, 075107 (2020)], we perform a calculation based on the dynamical vertex approximation and obtain the phase diagram of RbCa$_2$NiO$_3$ and $A_2$NiO$_2$Br$_2$ where $A$ is a cation with a valence of 2.5+. We show that the phase diagram of these nickelates exhibits the same essential features as those found in cuprates. Namely, superconductivity appears upon hole-doping into an antiferromagnetic Mott insulator, and the superconducting transition temperature shows a dome-like shape. This demonstrates that the electron correlations play an essential role in nickelate superconductors and we can control them by changing block layers.

cond-mat.supr-con↗

arXiv2022

Strongly correlated superconductivity with long-range spatial fluctuations

We review recent studies for superconductivity using diagrammatic extensions of dynamical mean field theory. These approaches take into account simultaneously both, the local correlation effect and spatial long-range fluctuations, which are essential to describe unconventional superconductivity in a quasi-two-dimensional plane. The results reproduce and predict the experimental phase diagrams of strongly correlated system such as cuprates and nickelates. Further studies reveal that the dynamical screening effect of the pairing interaction vertex has dramatic consequences for the transition temperature and may even support exotic mechanisms like odd-frequency pairing. We also discuss the dimensionality of layered materials and how to interpret the numerical results in two dimensions.

cond-mat.supr-con↗

arXiv2022

Interplay between magnetic and superconducting fluctuations in the doped 2d Hubbard model

We study the Hubbard model on a square lattice, using the dynamical vertex approximation and the parquet approximation. These methods allow us to describe the mutual interference of spin-fluctuations in the particle-hole channel and superconducting fluctuations in the cooperon channel in an unbiased way. For small dopings we find predominant commensurable antiferromagnetic spin- and d-wave superconducting fluctuations; for larger doping incommensurate antiferromagnetic spin fluctuations are concomitant to triplet s-wave superconducting fluctuations.

cond-mat.str-el↗

arXiv2022

Phase diagram of nickelate superconductors calculated by dynamical vertex approximation

We review the electronic structure of nickelate superconductors with and without effects of electronic correlations. As a minimal model we identify the one-band Hubbard model for the Ni 3$d_{x^2-y^2}$ orbital plus a pocket around the $A$-momentum. The latter however merely acts as a decoupled electron reservoir. This reservoir makes a careful translation from {nominal} Sr-doping to the doping of the one-band Hubbard model mandatory. Our dynamical mean-field theory calculations, in part already supported by experiment, indicate that the $Γ$ pocket, Nd 4$f$ orbitals, oxygen 2$p$ and {the} other Ni 3$d$ orbitals are not relevant in the superconducting doping regime. The physics is completely different if topotactic hydrogen is present or the oxygen reduction is incomplete. Then, a two-band physics hosted by the Ni 3$d_{x^2-y^2}$ and 3$d_{3z^2-r^2}$ orbitals emerges. Based on our minimal modeling we calculated the superconducting $T_c$ vs. Sr-doping $x$ phase diagram prior to experiment using the dynamical vertex approximation. For such a notoriously difficult to determine quantity as $T_c$, the agreement with experiment is astonishingly good. The prediction that $T_c$ is enhanced with pressure or compressive strain, has been confirmed experimentally as well. This supports that the one-band Hubbard model plus an electron reservoir is the appropriate minimal model.

cond-mat.supr-con↗

arXiv2021

Correlations turn electronic structure of finite-layer nickelates upside down

Motivated by the recent discovery of superconductivity in the pentalayer nickelate Nd$_6$Ni$_5$O$_{12}$ [Nature Materials 10.1038], we calculate its electronic structure and superconducting critical temperature. We find that electronic correlations are essential for pushing Nd$_6$Ni$_5$O$_{12}$ into the superconducting doping range as they shift the electron pockets above the Fermi energy. As a consequence, Nd$_6$Ni$_5$O$_{12}$ can be described with a single $d_{x^2-y^2}$ orbital per Ni. Instead, for the bilayer nickelate Nd$_3$Ni$_2$O$_6$ we find correlations to drive the system into a three-orbital regime also involving the Ni $d_{xz,yz}$ states. We suggest, however, that single-orbital physics with optimal doping can be restored by substituting 60% of the trivalent Nd or La by tetravalent Zr.

cond-mat.supr-con↗