arXiv subjects

Ion Errea

Publications and source records attributed to Ion Errea.

At least 37 records · Page 2Linked to original sources

arXiv2025

A Comprehensive Study on A$_2$PdH$_2$: From Ambient to High Pressure

We present a comprehensive first--principles study of the structural stability and superconducting behavior of Li$_2$PdH$_2$ under high pressure. Using random structure searching and phonon calculations, we identify a pressure--induced phase transition from a tetragonal I4/mmm structure, stable up to 5 GPa, to a monoclinic C2/m phase that remains thermodynamically stable up to 50 GPa. Superconductivity is absent in the tetragonal phase, even when anharmonic effects are considered, due to weak electron--phonon coupling and limited hydrogen involvement near the Fermi level. In contrast, the monoclinic phase exhibits a weak but pressure-enhanced superconducting transition, with Tc increasing from 0.6 K at 10 GPa to 4.7 K at 50 GPa, mainly driven by low--frequency Li and Pd-derived phonon modes. We further explore the isostructural A$_2$PdH$_2$ (A = Na, K, Rb, Cs) series to evaluate the impact of alkali-metal substitution on stability and superconductivity. Na, K, and Rb analogs retain dynamic stability at ambient pressure, with weak superconducting critical temperatures of 3.2 K, 2.1 K, and negligible Tc, respectively. Cs$_2$PdH$_2$, however, exhibits phonon instabilities, suggesting a need for external stabilization. These findings highlight the delicate balance between lattice dynamics, electronic structure, and atomic mass in tuning superconductivity in palladium-based hydrides.

cond-mat.supr-con↗

arXiv2025

Simphony: A full tight-binding package for lattice vibrations and topological phonon analysis

Simphony is an open-source software package designed for the topological analysis of lattice vibrations based on Wannier tight-binding models. Its primary function is to classify the topology of novel materials by computing bulk and slab phonon band structures, extracting phonon surface spectra, and providing analysis tools such as Wilson loop calculations and Weyl node detection. The workflow is analogous to that of established electronic topology codes like Wannier90 and WannierTools. It also incorporates long-range polar interactions during the wannierization process, making Simphony one of the first tools capable of diagnosing topology in polar insulators.

cond-mat.mtrl-sci↗

arXiv2025

Long-range electron coherence in Kagome metals

The wave-like nature of electrons lies at the core of quantum mechanics, distinguishing them from classical particles. Landmark experiments have revealed phase coherence of mobile electrons within solids, such as Aharonov-Bohm interference in mesoscopic rings. However, this coherence is typically limited by numerous environmental interactions. Controlling and ideally mitigating such decoherence remains a central challenge in condensed matter physics. Here, we report magnetoresistance oscillations in mesoscopic pillars of the Kagome metal CsV$_3$Sb$_5$ for fields applied parallel to the Kagome planes. Their periodicity is independent of materials parameters, simply given by the number of flux quanta $h/e$ threading between adjacent Kagome layers akin to an atomic-scale Aharonov-Bohm interferometer. Intriguingly they occur under conditions not favorable for typical interference in solids, at temperatures above 20 K and in micrometer-scale devices well exceeding the single-particle mean free path. Further, the oscillations exhibit non-analytic field-angle dependence and scale consistently with a broad range of key electronic responses in CsV$_3$Sb$_5$, pointing to a cooperative mechanism that establishes intrinsic coherence. Our findings provide new insights into the debated origin of correlated order in CsV$_3$Sb$_5$ and establish Kagome metals as a promising platform for interaction-stabilized long-range electron coherence - crucial for both fundamental studies and technological advancements in quantum interference in metallic systems.

cond-mat.str-el↗

arXiv2025

Lattice thermal conductivity in the anharmonic overdamped regime

In crystalline materials, low lattice thermal conductivity is often associated with strong anharmonicity, which can cause significant deviations from the expected Lorentzian lineshape of phonon spectral functions. These deviations, occurring in an overdamped regime, raise questions about the applicability of the Boltzmann transport equation. Furthermore, strong anharmonicity can trigger structural phase transitions with temperature, which cannot be adequately described by the standard harmonic approximation. To address these challenges, we propose a novel approach for computing the lattice thermal conductivity. Our method combines the Green-Kubo linear response theory with the stochastic self-consistent harmonic approximation. The latter allows us to describe the temperature-dependent evolution of the crystal structure, including first- and second-order phase transitions, as well as the vibrational properties in highly anharmonic materials. The Green-Kubo method considers the entire lineshapes of phonon spectral functions in the calculation of the lattice thermal conductivity, thus eliminating the questionable use of phonon lifetimes in the overdamped regime, as well as naturally including coherent transport effects. Additionally, we extend our theory to model complex dynamical lattice thermal conductivity, enhancing our understanding of time-dependent thermoreflectance experiments. As a practical application, we employ this approach to calculate the lattice thermal conductivity of CsPbBr$_3$, a complex crystal known for its anomalous thermal transport behavior with a complex phase diagram. Our method is able to determine the thermal conductivity across different phases in good agreement with experiments.

cond-mat.mtrl-sci↗

arXiv2025

The Maximum $T_c$ of Conventional Superconductors at Ambient Pressure

The theoretical maximum critical temperature ($T_c$) for conventional superconductors at ambient pressure remains a fundamental question in condensed matter physics. Through analysis of electron-phonon calculations for over 20,000 metals, we critically examine this question. We find that while hydride metals can exhibit maximum phonon frequencies of more than 5000 K, the crucial logarithmic average frequency $ω_\text{log}$ rarely exceeds 1800 K. Our data reveals an inherent trade-off between $ω_\text{log}$ and the electron-phonon coupling constant $λ$, suggesting that the optimal Eliashberg function that maximizes $T_c$ is unphysical. Based on our calculations, we identify Li$_2$AgH$_6$ and its sibling Li$_2$AuH$_6$ as theoretical materials that likely approach the practical limit for conventional superconductivity at ambient pressure. Analysis of thermodynamic stability indicates that compounds with higher predicted $T_c$ values are increasingly unstable, making their synthesis challenging. While fundamental physical laws do not strictly limit $T_c$ to low-temperatures, our analysis suggests that achieving room-temperature conventional superconductivity at ambient pressure is extremely unlikely.

cond-mat.supr-con↗

arXiv2025

From superconductivity to non-superconductivity in LiPdH: a first principle approach

The layered structure of LiPdH was theoretically suggested to be a superconductor as a result of its larger electron-phonon coupling constant compared to that of PdH. However, the experimental results reported contrary findings, with no trace of superconductivity. We study the electronic, vibrational, and superconducting properties of the ambient pressure tetragonal phase of LiPdH ($P4/mmm$) within first principles density functional theory methods, both in the harmonic and anharmonic approximations for the lattice dynamics, and conclude that it does not show any superconducting behavior. High-pressure crystal structure prediction calculations indicate that no structural transition is expected to occur under pressure up to 100 GPa in LiPdH. Our theoretical calculations demonstrate that increasing pressure reduces the density of states at the Fermi surface and consequently weakens electron-phonon interactions, leading to a further suppression of the superconducting critical temperature.

cond-mat.supr-con↗

arXiv2025

A chemical bonding based descriptor for predicting the impact of quantum nuclear and anharmonic effects on hydrogen-based superconductors

Quantum nuclear effects (QNEs) can significantly alter a material's crystal structure and phonon spectra, impacting properties such as thermal conductivity and superconductivity. However, predicting a priori whether these effects will enhance or suppress superconductivity, or destabilize a structure, remains a grand challenge. Herein, we address this unresolved problem by introducing a descriptor, based upon the integrated crystal orbital bonding index (iCOBI), to predict the influence of QNEs on a crystal lattice's dynamic stability, phonon spectra and superconducting properties. We find that structures with atoms in symmetric chemical bonding environments exhibit greater resilience to structural perturbations induced by QNEs, while those with atoms in asymmetric bonding environments are more susceptible to structural alterations, resulting in enhanced superconducting critical temperatures.

cond-mat.supr-con↗

arXiv2025

Broad Spectral Tuning of Ultra-Low Loss Polaritons in a van der Waals Crystal by Intercalation

Phonon polaritons (PhPs) -- light coupled to lattice vibrations -- in polar van der Waals (vdW) crystals are promising candidates for controlling the flow of energy at the nanoscale due to their strong field confinement, anisotropic propagation, and ultra-long lifetime in the picosecond range \cite{ref1,ref2,ref3,ref4,ref5}. However, the lack of tunability in their narrow and material-specific spectral range -- the Reststrahlen Band (RB) -- severely limits their technological implementation. Here, we demonstrate that the intercalation of Na atoms in the vdW semiconductor $α$-V$_2$O$_5$ enables a broad spectral shift of RBs, and that the PhPs excited exhibit ultra-low losses (lifetime of $4 \pm 1$~ps), similar to PhPs in the non-intercalated crystal (lifetime of $6 \pm 1$ ps). We expect our intercalation method to be applicable to other vdW crystals, opening the door for the use of PhPs in broad spectral bands in the mid-infrared domain.

physics.optics↗

arXiv2024

Quantum Anharmonic Effects on the Superconductivity of I-43m CH4-H3S at High Pressures: a First-Principles Study

Making use of first-principles calculations we analyze the effect of quantum ionic fluctuations and lattice anharmonicity on the crystal structure and superconductivity of I-43m CH4-H3S, one of the lowest enthalpy structures in the C-S-H system, in the 150-300 GPa pressure range within the stochastic self-consistent harmonic approximation. We predict a correction to the crystal structure, which is formed by an H3S lattice and CH4 molecules, the phonon spectra, and the pressure-dependent superconducting critical temperatures, which have been estimated in previous calculations without considering ionic fluctuations on the crystal structure and assuming the harmonic approximation for the lattice dynamics. Our results show that quantum ionic fluctuations have an impact on the distance between H atoms and S atoms in the H3S host lattice, pushing it towards more symmetric bonds, while the methane molecules are barely affected. According to our anharmonic phonon spectra, this structure is dynamically stable above 150 GPa, which is 30 GPa lower than the pressure at which the harmonic approximation predicts the emergence of an instability. As a consequence of the strong anharmonic enhancement of the phonon frequencies, the electron-phonon coupling constant is suppressed by 46% at 200 GPa, and even more at lower pressures. As a result, the superconducting critical temperature is overestimated by around 50 K at 200 GPa, such that it falls below 150 K in the whole pressure range studied. Our results underline that ternary hydrides are subject to strong anharmonic effects on their structural, vibrational, and superconducting properties.

cond-mat.mtrl-sci↗

arXiv2024

Ambient pressure high temperature superconductivity in RbPH$_3$ facilitated by ionic anharmonicity

Recent predictions of metastable high-temperature hydride superconductors give hope that superconductivity at ambient conditions is within reach. In this work, we predict RbPH$_3$ as a new compound with a superconducting critical temperature around 100 K at ambient pressure, dynamically stabilized thanks to ionic quantum anharmonic effects. RbPH$_3$ is thermodynamically stable at 30 GPa in a perovskite $Pm\bar{3}m$ phase, allowing its experimental synthesis at moderate pressures far from the megabar regime. With lowering pressure it is expected to transform to a $R3m$ phase that should stay dynamically stable thanks to quantum fluctuations down to ambient pressures. Both phases are metallic, with the $R3m$ phase having three distinct Fermi surfaces, composed mostly of states with phosphorus and hydrogen character. The structures are held together by strong P-H covalent bonds, resembling the pattern observed in the high-temperature superconducting H$_3$S, with extra electrons donated by rubidium. These results demonstrate that quantum ionic fluctuations, neglected thus far in high-throughput calculations, can stabilize at ambient pressure hydride superconductors with a high critical temperature.

cond-mat.supr-con↗

arXiv2024

Unveiling the Mechanism of Phonon-Polariton Damping in α-MoO_3

Phonon polaritons (PhPs) (light coupled to lattice vibrations) in the highly anisotropic polar layered material molybdenum trioxide (α-MoO_3) are currently the focus of intense research efforts due to their extreme subwavelength field confinement, directional propagation and unprecedented low losses. Nevertheless, prior research has primarily concentrated on exploiting the squeezing and steering capabilities of α-MoO_3 PhPs, without inquiring much into the dominant microscopic mechanism that determines their long lifetimes, key for their implementation in nanophotonic applications. This study delves into the fundamental processes that govern PhP damping in α-MoO_3 by combining ab initio calculations with scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier-transform infrared (FTIR) spectroscopy measurements across a broad temperature range (from 8 to 300 K). The remarkable agreement between our theoretical predictions and experimental observations allows us to identify third-order anharmonic phonon-phonon scattering as the main damping mechanism of α-MoO_3 PhPs. These findings shed light on the fundamental limits of low-loss PhPs, a crucial factor for assessing their implementation into nanophotonic devices.

cond-mat.mtrl-sci↗

arXiv2024

Nontrivial Quantum Geometry and the Strength of Electron-Phonon Coupling

The coupling of electrons to phonons (electron-phonon coupling) is crucial for the existence of various phases of matter, in particular superconductivity and density waves. Here, we devise a theory that incorporates the quantum geometry of the electron bands into the electron-phonon coupling, demonstrating the crucial contributions of the Fubini-Study metric or its orbital selective version to the dimensionless electron-phonon coupling constant. We apply the theory to two materials, graphene and MgB$_2$ where the geometric contributions account for approximately 50\% and 90\% of the total electron-phonon coupling constant, respectively. The quantum geometric contributions in the two systems are further bounded from below by topological contributions. Our results suggest that the nontrivial electron band geometry/topology might favor superconductivity with relatively high critical temperature.

cond-mat.supr-con↗

arXiv2024

Observation of Chiral Surface State in Superconducting NbGe$_2$

The interplay between topology and superconductivity in quantum materials harbors rich physics ripe for discovery. In this study, we investigate the topological properties and superconductivity of the nonsymmorphic chiral superconductor NbGe$_2$ using high-resolution angle-resolved pho-toemission spectroscopy (ARPES), transport measurements, and ab initio calculations. The ARPES data revealed exotic chiral surface states on the (100) surface originating from the inherent chiral crystal structure. Supporting calculations indicate that NbGe$_2$ likely hosts elusive Weyl fermions in its bulk electronic structure. Furthermore, we uncovered the signatures of van Hove singularities that can enhance many-body interactions. Additionally, transport measurements demonstrated that NbGe$_2$ exhibits superconductivity below 2K. Overall, our comprehensive results provide the first concrete evidence that NbGe$_2$ is a promising platform for investigating the interplay between non-trivial band topology, possible Weyl fermions, van Hove singularities, and superconductivity in chiral quantum materials.

cond-mat.mes-hall↗

arXiv2024

Large impact of phonon lineshapes on the superconductivity of solid hydrogen

Phonon anharmonicity plays a crucial role in determining the stability and vibrational properties of high-pressure hydrides. Furthermore, strong anharmonicity can render phonon quasiparticle picture obsolete questioning standard approaches for modeling superconductivity in these material systems. In this work, we show the effects of non-Lorentzian phonon lineshapes on the superconductivity of high-pressure solid hydrogen. We calculate the superconducting critical temperature T$_\mathrm{C}$ \emph{ab initio} considering the full phonon spectral function and show that it overall enhances the T$_\mathrm{C}$ estimate. The anharmonicity-induced phonon softening exhibited in spectral functions increases the estimate of the critical temperature, while the broadening of phonon lines due to phonon-phonon interaction decreases it. Our calculations also reveal that superconductivity emerges in hydrogen in the $Cmca-12$ molecular phase VI at pressures between 450 and 500 GPa and explain the disagreement between the previous theoretical results and experiments.

cond-mat.supr-con↗

arXiv2024

Searching Materials Space for Hydride Superconductors at Ambient Pressure

We employed a machine-learning assisted approach to search for superconducting hydrides under ambient pressure within an extensive dataset comprising over 150 000 compounds. Our investigation yielded around 50 systems with transition temperatures surpassing 20 K, and some even reaching above 70 K. These compounds have very different crystal structures, with different dimensionality, chemical composition, stoichiometry, and arrangement of the hydrogens. Interestingly, most of these systems displayed slight thermodynamic instability, implying that their synthesis would require conditions beyond ambient equilibrium. Moreover, we found a consistent chemical composition in the majority of these systems, which combines alkali or alkali-earth elements with noble metals. This observation suggests a promising avenue for future experimental investigations into high-temperature superconductivity within hydrides at ambient pressure.

cond-mat.supr-con↗

arXiv2024

Molecularity: a fast and efficient criterion for probing superconductivity

We present an efficient criterion for probing the critical temperature of hydrogen based superconductors. We start by expanding the applicability of 3D descriptors of electron localization to superconducting states within the framework of superconducting DFT. We first apply this descriptor to a model system, the hydrogen chain, which allows to prove two main concepts: i) that the electron localization changes very little when the transition from the normal to the superconducting state takes place, i.e. that it can be described at the DFT level from the normal state; and ii) that the formation of molecules can be characterized within this theoretical framework, enabling to filter out systems with marked molecular character and hence with low potential to be good superconductors. These two ideas, are then exploited in real binary and ternary systems, showing i) that the bonding type can be characterized automatically; and ii) that this provides a new index which enables to feed machine learning algorithms for a better prediction of critical temperatures. Overall, this sets a grounded theoretical scenario for an automatic and efficient high-throughput of potential hydrogen based superconductors.

cond-mat.supr-con↗

arXiv2024

On the dynamical stability of copper-doped lead apatite

The recent claim of room temperature superconductivity in a copper-doped lead apatite compound, called LK-99, has sparked remarkable interest and controversy. Subsequent experiments have largely failed to reproduce the claimed superconductivity, while theoretical works have identified multiple key features including strong electronic correlation, structural instabilities, and dopability constraints. A puzzling claim of several recent theoretical studies is that both parent and copper-doped lead apatite structures are dynamically unstable at the harmonic level, questioning decades of experimental reports of the parent compound structures and the recently proposed copper-doped structures. In this work, we demonstrate that both parent and copper-doped lead apatite structures are dynamically stable at room temperature. Anharmonic phonon-phonon interactions play a key role in stabilizing some copper-doped phases, while most phases are largely stable even at the harmonic level. We also show that dynamical stability depends on both volume and correlation strength, suggesting controllable ways of exploring the copper-doped lead apatite structural phase diagram. Our results fully reconcile the theoretical description of the structures of both parent and copper-doped lead apatite with experiment.

cond-mat.supr-con↗

arXiv2023

Evidence for ground state coherence in a two-dimensional Kondo lattice

Kondo lattices are ideal testbeds for the exploration of heavy-fermion quantum phases of matter. While our understanding of Kondo lattices has traditionally relied on complex bulk f-electron systems, transition metal dichalcogenide heterobilayers have recently emerged as simple, accessible and tunable 2D Kondo lattice platforms where, however, their ground state remains to be established. Here we present evidence of a coherent ground state in the 1T/1H-TaSe2 heterobilayer by means of scanning tunneling microscopy/spectroscopy at 340 mK. Our measurements reveal the existence of two symmetric electronic resonances around the Fermi energy, a hallmark of coherence in the spin lattice. Spectroscopic imaging locates both resonances at the central Ta atom of the charge density wave of the 1T phase, where the localized magnetic moment is held. Furthermore, the evolution of the electronic structure with the magnetic field reveals a non-linear increase of the energy separation between the electronic resonances. Aided by ab initio and auxiliary-fermion mean-field calculations, we demonstrate that this behavior is inconsistent with a fully screened Kondo lattice, and suggests a ground state with magnetic order mediated by conduction electrons. The manifestation of magnetic coherence in TMD-based 2D Kondo lattices enables the exploration of magnetic quantum criticality, Kondo breakdown transitions and unconventional superconductivity in the strict two-dimensional limit.

cond-mat.str-el↗