arXiv subjects

Harrison LaBollita

Publications and source records attributed to Harrison LaBollita.

At least 19 recordsLinked to original sources

arXiv2026

Unraveling Fermi liquid charge and heat transport in RuO$_{2}$

RuO$_2$ is a multi-orbital Fermi liquid for which an array of complementary experimental measurements has recently become available, making it a stringent testbed for quantitative many-body electronic structure theory. Using realistic dynamical mean-field calculations, we compute the spectroscopic and transport properties of RuO$_2$ in the paramagnetic state. We identify RuO$_2$ as a moderately correlated Fermi liquid and obtain (semi-)quantitative agreement with experiment for its optical conductivity, electrical resistivity, and thermopower. This broad agreement across complementary observables establishes a ``precision'' many-body description of RuO$_2$ and allows remaining discrepancies to be identified as meaningful tests of the theory. In particular, the calculated electronic thermal resistivity significantly undershoots the experimentally inferred low-temperature thermal resistivity, raising an important puzzle concerning the relative relaxation of charge and heat currents in the Fermi liquid regime. We explore low-temperature electron-phonon scattering as a possible mechanism for resolving this discrepancy, while a fully quantitative description remains an open problem. More broadly, our results demonstrate the power of combining precision DFT+DMFT calculations with complementary experimental probes to build and critically test quantitative descriptions of correlated quantum materials.

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arXiv2026

GEM: An implementation of the ghost-Gutzwiller approximation for simulating interacting quantum systems

We present GEM (Ghost Embedding Method), an open-source software package written in Python for computing equilibrium properties of strongly correlated electronic systems within the ghost-Gutzwiller approximation method. GEM provides a computationally efficient framework for studying multi-orbital lattice models. It supports zero- and finite-temperature calculations and symmetry broken phases. It is integrated with the TRIQS ecosystem, providing tools for model construction, self-consistent solution, and evaluation of physical observables. We first detail the method's theoretical formulation, then we present the software architecture, and finally we introduce some practical workflow, which also validates the implementation against established results. In particular, we illustrate the capabilities of GEM through multiorbital and finite-temperature applications and discuss its computational cost relative to more demanding quantum embedding approaches.

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arXiv2026

Bobkingite, a new coupled sawtooth chain platform

We investigate the mineral bobkingite, \ce{Cu5(OH)8Cl2(H2O)2}, as a potential realization of the sawtooth chain. Using \textit{ab initio} methods, we estimate the magnetic exchange couplings and find that bobkingite hosts quasi-one-dimensional sawtooth chains, with residual three-dimensional interactions strongly suppressed by the crystal geometry. Examining the full exchange network, we find that the classical model exhibits an extensive manifold of nearly degenerate states with emergent two-dimensional character, which spin-wave theory shows to persist to leading order in quantum fluctuations as Ising degrees of freedom. Unlike other sawtooth candidates, bobkingite has negligible vertical interchain coupling, preserving a one-dimensional degeneracy even in the presence of ordering, suggesting that any long-range order is weak. Thermal fluctuations may thus stabilize a finite-temperature classical spin liquid regime, with a cascade of transitions upon cooling into successively lower-dimensional degenerate states, making bobkingite a compelling platform for exploring sawtooth chain physics.

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arXiv2026

Electron-phonon origins of unconventional resistivity in moderately correlated perovskite oxides

Transition-metal perovskite oxides exhibit moderately correlated metallic phases, several of which exhibit a $T^2$ resistivity scaling up to temperatures far exceeding the regime where Fermi-liquid electron-electron scattering is expected to dominate. Some of these materials, such as SrMoO$_3$, also exhibit unexplained ultra-low room-temperature resistivity. We demonstrate that in SrMoO$_3$, SrWO$_3$, SrTaO$_3$, SrNbO$_3$, and SrVO$_3$ electron-phonon scattering results in quadratic-scaling resistivity due to the shape of the Fermi surface and the thermal activation of optical phonons. We also reveal that the origin of the low resistivity of SrMoO$_3$ is an overall low electron-phonon coupling strength, and identify SrWO$_3$ and SrTaO$_3$ as other possible low-resistivity oxides. Additionally, we find that the strength of electron-phonon coupling is sensitive to structural distortions, energies of optical phonons, and the treatment of electronic correlations. This suggests design principles for finding other ultra-high conductivity transition-metal oxides, and has significant implications for theoretical interpretation of direct-current resistivity in transition-metal oxides and beyond.

cond-mat.mtrl-sci↗

arXiv2026

Squeezing dynamical singlets in bilayer nickelates

We present realistic calculations within the density functional plus cluster dynamical mean-field formalism indicating that the physics of the the bilayer Ruddlesden-Popper nickelates is to a significant extent controlled by interlayer "dynamical singlets'' which are formed from the $3z^{2}-r^{2}$ orbitals singly occupied by electrons and are hybridized with itinerant planar $x^{2}-y^{2}$ orbitals. The hybridization is found to respond differently to hydrostatic pressure and to epitaxial strain, capturing the experimentally observed dichotomy between bulk single crystals and epitaxial thin films and reproducing several experimental results including angle-resolved photoemission and transport measurements.

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arXiv2026

Electron vs. hole doping in infinite-layer nickelates: electronic structure, magnetism and correlations

The observation of superconductivity in undoped infinite-layer nickelates $R$NiO$_2$ ($R$ = rare earth) challenges our current understanding and calls for a re-examination of the underlying electronic structure of this family of materials. In this context, it is particularly important to extend the investigation of $R$NiO$_2$ compounds from the intensively studied hole-doped regime to the almost unexplored electron-doped one. Here, we use a combination of density-functional theory and dynamical mean-field theory to study the evolution of the electronic structure of infinite-layer nickelates in these two doping regimes. We find a striking asymmetry in the self-doping of the Ni-$d_{x^2-y^2}$ band due to the $R(5d)$ states: while this effect is strongly suppressed upon hole doping, electron doping instead leads to an increase in the size of the $R(5d)$ electron pockets, but without effectively hole-doping the Ni-$d_{x^2-y^2}$ band. This asymmetry has an important impact on the magnetic response as antiferromagnetism is rapidly suppressed upon hole doping, whereas it remains the ground state upon electron doping. Despite these differences, electronic correlations on both sides of the phase diagram are dominated by the Ni $d_{x^2-y^2}$ orbital, suggesting that a single-band description may be appropriate for infinite-layer nickelates in both the electron- and hole-doped regimes.

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arXiv2026

Correlated electronic structure of the alternating monolayer-bilayer nickelate La$_{5}$Ni$_{3}$O$_{11}$

The recent discovery of superconductivity under pressure in Ruddlesden-Popper (RP) nickelates has attracted a great deal of attention. Here, using charge-self consistent density-functional theory plus dynamical mean-field theory, we study the correlated electronic structure of the latest superconducting member of the family: the alternating single-layer bilayer nickelate La$_{5}$Ni$_{3}$O$_{11}$. Due to its alternating single-layer and bilayer structural motif, this hybrid RP nickelate exhibits layer-selective physics with the single-layer neighboring a Mott instability, rendering the bilayer the dominant contributor to its low-energy physics, both at ambient and high pressure. The electronic structure of La$_{5}$Ni$_{3}$O$_{11}$ ultimately resembles that of the bilayer compound La$_{3}$Ni$_{2}$O$_{7}$, pointing to the presence of universal features in the family of superconducting RP nickelates. Thus, La$_{5}$Ni$_{3}$O$_{11}$ provides a new platform to disentangle the key degrees of freedom underlying superconductivity in pressurized RP nickelates, underscoring the central role of the bilayer structural motif.

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arXiv2026

Superconducting phase diagram of multi-layer square-planar nickelates

The discovery of superconductivity in square-planar nickelates has offered a rich materials platform to explore the origins of cuprate-like superconductivity. Experimental investigations however have largely been limited to the infinite-layer $R$NiO$_2$ ($R$=rare-earth) nickelates. Here, we construct a phase diagram of multi-layer square-planar Nd$_{n+1}$Ni$_n$O$_{2n+2}$ compounds and discover signatures of superconductivity for $n$ = 4 - 8. Upon decreasing the dimensionality $n$, the superconducting anisotropy evolves due to 4$f$ electron effects, and electronic structure characteristics approach cuprate-like behavior. Magnetic fluctuations persist from within the superconducting regime and into the over-doped, non-superconducting regime. Remarkably, the superconducting regime overlaps with that of chemically-doped infinite-layer nickelates, demonstrating underlying commonalities and distinct differences across varying structural realizations of square-planar nickelates. Our work establishes this layered template for creating new nickel-based superconductors.

cond-mat.supr-con↗

arXiv2026

Low-temperature transport in high-conductivity correlated metals: a density-functional plus dynamical mean-field study of cubic perovskites

While methods based on density-functional perturbation theory have dramatically improved our understanding of electron-phonon contributions to transport in materials, methods for accurately capturing electron-electron scattering relevant to low temperatures have seen significantly less development. The case of high-conductivity, moderately correlated materials characterized by low scattering rates is particularly challenging, since exquisite numerical precision of the low-energy electronic structure is required. Recent methodological advancements to density-functional theory combined with dynamical mean-field theory (DFT+DMFT), including adaptive Brillouin-zone integration and numerically precise self-energies, enable a rigorous investigation of electron-electron scattering in such materials. In particular, these tools may be leveraged to perform a robust scattering-rate analysis on both real- and imaginary-frequency axes. Applying this methodology to a subset of ABO$_3$ perovskite oxides -- SrVO$_3$, SrMoO$_3$, PbMoO$_3$, and SrRuO$_3$ -- we demonstrate its ability to qualitatively and quantitatively describe electron-electron contributions to the temperature-dependent direct-current resistivity. This combination of numerical techniques offers fundamental insight into the role of electronic correlations in transport phenomena and provides a predictive tool for identifying materials with potential for technological applications.

cond-mat.mtrl-sci↗

arXiv2026

Fermi-Liquid $T^2$ Resistivity: Dynamical Mean-Field Theory Meets Experiment

Direct-current resistivity is a key probe for the physical properties of materials. In metals, Fermi-liquid (FL) theory serves as the basis for understanding transport. A $T^2$ behavior of the resistivity is often taken as a signature of FL electron-electron scattering. However, the presence of impurity and phonon scattering as well as material-specific aspects such as Fermi surface geometry can complicate this interpretation. We demonstrate how density-functional theory combined with dynamical mean-field theory can be used to elucidate the FL regime. We take as examples SrVO$_{3}$ and SrMoO$_{3}$, two moderately correlated perovskite oxides, and establish a precise framework to analyze the FL behavior of the self-energy at low energy and temperature. Reviewing published low-temperature resistivity measurements, we find agreement between our calculations and experiments performed on samples with exceptionally low residual resistivity. This comparison emphasizes the need for further theoretical, synthesis, and characterization developments in these and other FL materials.

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arXiv2026

Electronic layer decoupling driven by density-wave order in La$_4$Ni$_3$O$_{10}$

We probe the density-wave transition of the trilayer nickelate La$_4$Ni$_3$O$_{10}$ with polarization-resolved infrared spectroscopy. The low-energy electrodynamics is strongly anisotropic, with metallic in-plane and insulating out-of-plane character. In the ordered phase, the anisotropy grows more than an order of magnitude as the out-of-plane conductivity is sharply suppressed. We interpret this enhancement as an effective electronic decoupling of the Ni-O layers, driven by a spin-density-wave-induced redistribution of Ni-$d_{z^2}$ occupation within the trilayers. This electronic response is accompanied by clear shifts and splittings of the out-of-plane phonons, compatible with a density-wave instability of electronic origin.

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arXiv2025

Role of correlations in Ruddlesden-Popper bilayer nickelates under compressive strain

The recent discovery of superconductivity in thin films of the bilayer Ruddlesden-Popper (RP) nickelate La$_3$Ni$_2$O$_7$ (La327) under compressive strain has generated enormous interest, opening up further opportunities to stabilize superconductivity in this class of materials at ambient pressure. To better understand the many-body normal state from which superconductivity arises, it is important to ascertain the nature and role of correlations in its electronic structure. To provide insights into this question, we use a fully charge self-consistent DFT+e-DMFT (eDMFT) approach to study La327 at several compressive strain levels. At the strain level where superconductivity has been observed experimentally (-2\%), in contrast with DFT and DFT+$U$ results, the so-called $γ$ pocket emerges and the associated band, of mostly $d_{z^2}$ character, crosses the Fermi level exhibiting `flat band''-like features when dynamical correlations are included. Larger strain levels suppress the $γ$ pocket, which may have implications for superconductivity or its pairing symmetry.

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arXiv2025

Lattice-charge coupling in a trilayer nickelate with intertwined density wave order

Intertwined charge and spin correlations are ubiquitous in a wide range of transition metal oxides and are often perceived as intimately related to unconventional superconductivity. Theoretically envisioned as driven by strong electronic correlations, the intertwined order is usually found to be strongly coupled to the lattice as signaled by pronounced phonon softening. Recently, both charge/spin density waves (CDW/SDW) and superconductivity have been discovered in several Ruddlesden-Popper (RP) nickelates, in particular trilayer nickelates RE4Ni3O10 (RE=Pr, La). The nature of the intertwined order and the role of lattice-charge coupling are at the heart of the debate about these materials. Using inelastic X-ray scattering, we mapped the phonon dispersions in RE4Ni3O10 and found no evidence of phonon softening near the CDW wavevector over a wide temperature range. Calculations of the electronic susceptibility revealed a peak at the observed SDW ordering vector but not at the CDW wavevector. The absence of phonon softening is in sharp contrast to that in canonical oxide materials, notably cuprates. Our experimental and theoretical findings highlight the crucial role of the spin degree of freedom and establish a foundation for understanding the interplay between superconductivity and density-wave transitions in RP nickelate superconductors and beyond.

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arXiv2025

Topotactic oxidation of Ruddlesden-Popper nickelates reveals new structural family: oxygen-intercalated layered perovskites

Layered perovskites such as the Dion-Jacobson, Ruddlesden-Popper, and Aurivillius families host a wide range of correlated electron phenomena, from high-temperature superconductivity to multiferroicity. Here we report a new family of layered perovskites, realized through topotactic oxygen intercalation of La_{n+1}Ni_{n}O_{3n+1} (n=1-4) Ruddlesden-Popper nickelate thin films grown by ozone-assisted molecular-beam epitaxy. Post-growth ozone annealing induces a large c-axis expansion - 17.8% for La_{2}NiO_{4} (n=1) - that monotonically decreases with increasing n. Surface X-ray diffraction coupled with Coherent Bragg Rod Analysis reveals that this structural expansion arises from the intercalation of approximately 0.7 oxygen atoms per formula unit into interstitial sites within the rock salt spacer layers. The resulting structures exhibit a spacer layer composition intermediate between that of the Ruddlesden-Popper and Aurivillius phases, defining a new class of layered perovskites. Oxygen-intercalated nickelates exhibit metallicity and significantly enhanced nickel-oxygen hybridization, a feature linked to high-temperature superconductivity. Our work establishes topotactic oxidation as a powerful synthetic approach to accessing highly oxidized, metastable phases across a broad range of layered oxide systems, offering new platforms to tune properties via spacer-layer chemistry.

cond-mat.mtrl-sci↗

arXiv2025

Unconventional polaronic ground state in superconducting LiTi$_2$O$_4$

Geometrically frustrated lattices can display a range of correlated phenomena, ranging from spin frustration and charge order to dispersionless flat bands due to quantum interference. One particularly compelling family of such materials is the half-valence spinel Li$B_2$O$_4$ materials. On the $B$-site frustrated pyrochlore sublattice, the interplay of correlated metallic behavior and charge frustration leads to a superconducting state in LiTi$_2$O$_4$ and heavy fermion behavior in LiV$_2$O$_4$. To date, however, LiTi$_2$O$_4$ has primarily been understood as a conventional BCS superconductor despite a lattice structure that could host more exotic groundstates. Here, we present a multimodal investigation of LiTi$_2$O$_4$, combining ARPES, RIXS, proximate magnetic probes, and ab-initio many-body theoretical calculations. Our data reveals a novel mobile polaronic ground state with spectroscopic signatures that underlie co-dominant electron-phonon coupling and electron-electron correlations also found in the lightly doped cuprates. The cooperation between the two interaction scales distinguishes LiTi$_2$O$_4$ from other superconducting titanates, suggesting an unconventional origin to superconductivity in LiTi$_2$O$_4$. Our work deepens our understanding of the rare interplay of electron-electron correlations and electron-phonon coupling in unconventional superconducting systems. In particular, our work identifies the geometrically frustrated, mixed-valence spinel family as an under-explored platform for discovering unconventional, correlated ground states.

cond-mat.supr-con↗

arXiv2025

Pressure effects on the electronic structure and magnetic properties of infinite-layer nickelates

Motivated by the discovery of superconductivity in infinite-layer nickelates RNiO$_2$ (R= rare-earth), and the subsequent enhancement of their T$_c$ with pressure, we investigate the evolution of the electronic structure and magnetic properties of this family of materials via first-principles calculations employing hydrostatic and chemical pressure as tuning knobs. Overall, our analysis shows that pressure tends to increase the R-$5d$ self-doping effect, as well as the Ni-$d _{x^{2}-y^{2}}$ bandwidth, the $e_g$ energy splitting, the charge transfer energy, and the superexchange ($J$). Using the energy scale of $J$ as a predictor of superconducting tendencies, we anticipate that pressure can indeed be a feasible means to further increase the T$_c$ in this family of materials.

cond-mat.supr-con↗

arXiv2025

Stabilizing the calculation of the self-energy in dynamical mean-field theory using constrained residual minimization

We propose a simple and efficient method to calculate the electronic self-energy in dynamical mean-field theory (DMFT), addressing a numerical instability often encountered when solving the Dyson equation. Our approach formulates the Dyson equation as a constrained optimization problem with a simple quadratic objective. The constraints on the self-energy are obtained via direct measurement of the leading order terms of its asymptotic expansion within a continuous time quantum Monte Carlo framework, and the use of the compact discrete Lehmann representation of the self-energy yields an optimization problem in a modest number of unknowns. We benchmark our method for the non-interacting Bethe lattice, as well as DMFT calculations for both model systems and ab-initio applications.

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arXiv2024

Electronic correlations, layer distinction, and electron doping in the alternating single-layer trilayer La$_{3}$Ni$_{2}$O$_{7}$ polymorph

We employ a density-functional theory plus dynamical mean-field theory framework to investigate the correlated electronic structure of the alternating single-layer trilayer (1313) polymorph of La$_3$Ni$_2$O$_7$ under pressure. At ambient pressure, the single-layer is in a Mott insulating regime and the low-energy physics is dominated by the trilayer block. Under pressure, the gap in the single-layer block closes due to orbital-selective physics, enabling charge transfer into the trilayer block. This change in effective doping of the trilayer block is likely linked to the higher T$_c$ obtained in La$_3$Ni$_2$O$_7$-1313 ($\sim$ 80 K) when compared to the nominal trilayer La$_4$Ni$_3$O$_{10}$ ($\sim$ 30 K). We conclude that correlation-driven layer differentiation is crucial in the La$_3$Ni$_2$O$_7$-1313 polymorph and that its low-energy physics aligns closely with the trilayer La$_4$Ni$_3$O$_{10}$ compound (in spite of the apparent differences in nominal filling) rather than with the conventional bilayer La$_3$Ni$_2$O$_7$.

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