arXiv subjects

Antia S. Botana

Publications and source records attributed to Antia S. Botana.

At least 19 recordsLinked to original sources

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.

cond-mat.str-el↗

arXiv2026

Electronic structure of higher-order layered palladates: La$_{n+1}$Pd$_{n}$O$_{2n+2}$ $(n = 4-7)$

The square-planar layered nickelates R$_{n+1}$Ni$_n$O$_{2n+2}$ (R= Nd, $n=4-7$) have been recently shown to be superconducting without the need for chemical doping or pressure. Here, we examine the electronic structure of the analog higher-order square-planar palladates -- that have not yet been synthesized -- via \textit{ab initio} calculations. These layered palladates exhibit larger bandwidths, an increased $p-d$ hybridization, and less interference from R-$d$ bands at the Fermi level. These characteristics make them closer cuprate analogs and promising candidates to pursue in the context of unconventional superconductivity.

cond-mat.str-el↗

arXiv2026

Persistent structural distortions and absent superconductivity in trilayer nickelate thin films

A new family of high-temperature superconductors was recently discovered in the $n=2,3$ Ruddlesden-Popper nickelates, where superconductivity emerges concomitant with suppression of parent density waves and structural octahedral rotations under hydrostatic pressure. Intriguingly, compressive strain mimics the structural effects of pressure in the $n=2$ phase, yielding ambient-pressure superconductivity. However, analogous strain-stabilized superconductivity has not been realized in the $n=3$. Here, we use atomically-precise synthesis, transport, picoscale electron microscopy, and synchrotron X-ray diffraction to probe $n=3$ La$_4$Ni$_3$O$_{10}$ thin films. Although compressive strain suppresses density wave order, we do not observe superconductivity even under the largest strain state. Importantly, we identify a structural distortion unique to strained $n=3$ thin films that may inhibit superconductivity: persistent, layer-inequivalent octahedral rotations around the $c$-axis. Our results highlight key differences between the $n=3$ and $n=2$ systems, suggesting that ambient-pressure superconductivity in the $n=3$ may require new methods beyond epitaxial strain engineering.

cond-mat.mtrl-sci↗

arXiv2026

Electronic structure trends in La$_{2}R$Ni$_2$O$_7$ ($R=$ Pr, Nd, Sm) from first-principles

The discovery of superconductivity in bilayer La$_3$Ni$_2$O$_7$ under pressure has sparked tremendous attention on Ruddlesden-Popper (RP) nickelates. Recently, a higher superconducting transition temperature of 96 K was reported in Sm-doped La$_3$Ni$_2$O$_7$ single crystals at $\sim$ 22 GPa. Motivated by this experimental observation, we systematically explore the crystal structure and electronic properties of La$_3$Ni$_2$O$_7$ doped with different rare-earth elements in comparison to the undoped counterpart. As expected due to the effect of chemical pressure, we find that the volume of La$_{2}$$R$Ni$_2$O$_7$ ($R=$ Pr, Nd, Sm) progressively decreases with doping from Pr to Sm. We further find a pressure-induced structural transition to tetragonal symmetry that approximately coincides with the emergence of superconductivity in all cases. This transition is characterized by the emergence of flat $d_{z^2}$ bands at the Fermi level in the electronic structure. Despite subtle distinctions in the electronic structure between undoped and $R$-doped La$_3$Ni$_2$O$_7$, an increase in the dominant planar hopping is obtained as the $R$ size decreases. In contrast, the out-of-plane hopping decreases (in spite of the $c$ lattice constant compression), due to the decrease in the apical Ni-O$_{\rm rocksalt}$ bond length. Our findings provide further microscopic insights into the effects of $R$-doping in the electronic structure of RP nickelate superconductors in connection to $T_c$.

cond-mat.supr-con↗

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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2026

Pressure and strain tuning of the alternating bilayer-trilayer Ruddlesden-Popper nickelate: crystal and electronic structure

We use first-principles calculations to investigate the crystal and electronic structure of the hybrid bilayer-trilayer Ruddlesden-Popper (RP) nickelate La$_7$Ni$_5$O$_{17}$ under hydrostatic pressure and biaxial compressive strain. By analyzing the irreducible representations of the dynamically unstable phonon modes in the high-symmetry $P4/mmm$ structure, we identify a dynamically stable lower-symmetry $C2/c$ structure containing octahedral tilts. The application of both pressure and compressive strain tends to suppress the octahedral tilts, effectively tetragonalizing the structure, in analogy with the conventional RPs. The electronic structure under hydrostatic pressure and strain has similarities, but it differs in the position of the $d_{z^2}$ bonding band from the trilayer block. This band crosses the Fermi level at a pressure of 30 GPa, but it remains below it for any level of compressive strain. This strain-induced modification mirrors the electronic structure changes observed in the conventional bilayer nickelate.

cond-mat.mtrl-sci↗

arXiv2026

Tuning the magnetic properties of Kitaev materials via the antiferromagnetic proximity effect: Novel phases and application to an $α$-RuCl$_3$/MnPS$_3$ bilayer

In recent years, the increasing level of control over van der Waals (vdW) heterostructures has opened new routes to tune the properties of quantum materials. Motivated by these developments, we examine the potential consequences of interfacing a Kitaev honeycomb magnet, such as $α$-RuCl$_3$, with a nearly lattice-matched vdW antiferromagnet. By combining perturbation theory, exact diagonalization, and a classical energy-minimization method, we show that an effective staggered magnetic field originating from the vdW antiferromagnet can drive a monolayer of a Kitaev material into various novel phases, including an antichiral Kitaev spin liquid, a nonmagnetic nematic phase, and different types of skyrmion crystals. We then apply first-principle simulations to assess the prospect of concretely realizing this setup in a heterobilayer of $α$-RuCl$_3$ and the easy-axis antiferromagnet MnPS$_3$.

cond-mat.str-el↗

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

Structural stability, electronic structure, and magnetic properties of the single-layer trilayer La3Ni2O7 polymorph

A polymorph of the bilayer nickelate La3Ni2O7 that displays an alternating single-layer (SL) and trilayer (TL; 1313) stacking pattern has recently been discovered. Signatures of superconductivity under pressure have been found in this phase. At ambient pressure, La3Ni2O7-1313 has been reported to crystallize in three different space-group symmetries Cmmm, Imma, and Fmmm. Unlike the commonly observed tilted NiO6 octahedra in perovskite nickelates, the Cmmm phase exhibits no NiO6 tilts, implying that this structural feature alone may be insufficient to give rise to superconductivity in Ruddlesden-Popper nickelates. Here, we employ first-principles calculations and group theory analysis to study the pressure dependence of the structural instabilities in this SL-TL La3Ni2O7 polymorph. At ambient pressure, we identify multiple unstable phonon branches in the highest symmetry (Cmmm) structure at various high-symmetry points of the Brillouin zone. Distortions associated with these instabilities lead to one of the other experimentally reported space groups (Imma) that does display octahedral tilts. The magnetic tendencies indicate that the electronic structure of La3Ni2O7-1313 at ambient pressure is dominated by the TL block, as the SL is in a Mott-insulating regime. Under pressure, a tetragonal P4/mmm structure becomes stable, in agreement with experiments.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2025

Preferential site ordering alters the magnetic structure of Sm$_3$Ru$_4$Sn$_{13-x}$Ge$_x$ ($x = 0$-2)

An important aspect of materials research is the ability to tune different physical properties through controlled alloying. The Ln$_3$M$_4$X$_{13}$ (Ln = Lanthanide, M = Transition Metal, X = Tetrel) filled skutterudite family is of interest due to the tunability of its constituent components and their effects on physical properties, such as superconductivity and complex magnetism. In this work, Sm$_3$Ru$_4$Sn$_{13-x}$Ge$_x$ (x = 0 -- 2) was synthesized via excess Sn-flux and characterized using powder and single-crystal X-ray diffraction, magnetometry, X-ray photoelectron spectroscopy, and heat capacity. Sm$_3$Ru$_4$Sn$_{13}$ and its Ge-solid-solution members crystallize in the Pm-3n space group, which has two unique Wyckoff positions for the tetrel (X) site. In the solid solution members, Ge shows preferential occupancy for one of the two Wyckoff sites, reaching $\sim$60$\%$ and 100$\%$ occupancy when x = 1 and 2, respectively. Magnetometry and heat capacity measurements of Sm$_3$Ru$_4$Sn$_{13}$ indicated antiferromagnetic ordering at $T_N$ = 7.3 K. However, Sm$_3$Ru$_4$Sn$_{12}$Ge and Sm$_3$Ru$_4$Sn$_{11}$Ge$_2$ showed notably lower-temperature antiferromagnetic phase transitions with substantial peak-broadening at $T_N$ = 5.5 K and 4.1 K, respectively. These data suggest that alloying Ge into Sm$_3$Ru$_4$Sn$_{13}$ causes magnetic frustration within the structure, likely attributable to a change in the density of states from additional Ge $p$ states at the Fermi level. This work demonstrates that preferentially alloying Ge in Sm$_3$Ru$_4$Sn$_{13-x}$Ge$_x$ allows for more precise tunability of its magnetic structure, elucidating design principles for different quantum phases in intermetallic materials.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

arXiv2025

Electronic structure of Ruddlesden-Popper nickelates: strain to mimic the effects pressure

Signatures of superconductivity under pressure have recently been reported in the bilayer La$_3$Ni$_2$O$_7$ and trilayer La$_4$Ni$_3$O$_{10}$ Ruddlesden-Popper (RP) nickelates with general chemical formula La$_{n+1}$Ni$_n$O$_{3n+1}$ ($n=$ number of perovskite layers along the $c$-axis). The emergence of superconductivity is always concomitant with a structural transition in which the octahedral tilts are suppressed, bringing the apical Ni-O-Ni angle to 180$^\circ$ and causing an increase in the out-of-plane $d_{z^2}$ orbital overlap. Due to this strong interlayer coupling, a flat band of pure $d_{z^2}$ character crosses the Fermi level. Here, using first-principles calculations, we explore biaxial strain (both compressive and tensile) as a means to mimic the electronic structure characteristics of RP nickelates (up to $n=5$) under hydrostatic pressure. Our findings highlight that strain allows to decouple the structural and electronic structure effects obtained under hydrostatic pressure: while compressive strain brings the apical Ni-O-Ni angle closer to 180$^\circ$, it shifts the $d_{z^2}$ flat bands away from the Fermi energy, giving rise to a more cuprate-like electronic structure. In contrast, tensile strain reduces the apical Ni-O-Ni angle (to values $\sim$ 160$^\circ$), but it recovers the flat $d_{z^2}$ band at the Fermi level appearing in the bilayer and trilayer RPs under pressure. Overall, strain represents a promising way to tune the electronic structure of RP nickelates and could be an alternative route to achieve superconductivity at ambient pressure in this family of materials.

cond-mat.supr-con↗

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↗