arXiv subjects

Sebastian E. Reyes-Lillo

Publications and source records attributed to Sebastian E. Reyes-Lillo.

15 recordsLinked to original sources

arXiv2026

Systematic display of the spin splitting in band structures of representative altermagnetic crystals

In this work we demonstrate a novel approach to exhibit the unique spin splitting that is typical of collinear altermagnets. This approach is to plot band structures on Brillouin zone paths that sample general k-points to show a representative picture that corresponds to Brillouin zone averages. This is in contrast to conventional band structure plotting which plots band structures on the highest-symmetry points and lines, and thus in many cases can fail to show any altermagnetic spin splitting at all. Our investigation compares the new approach with the band structures of collinear altermagnets using conventional band structure plotting. We report the band structure and symmetry analysis for MnTe, CrSb, SmFeO3, ScCrO3, LaMnO3, TlCrO3, HoFeO3, InCrO3 and DyFeO3. This result clearly demonstrates the advantage of this novel method for displaying the spin splitting of collinear altermagnets.

cond-mat.mtrl-sci↗

arXiv2026

AlterSeeK-Path: Systematic construction of generalized band-structure paths for displaying altermagnetic spin splitting

Altermagnetic materials exhibit spin splitting in their electronic band structures while maintaining zero net magnetization. However, conventional high-symmetry k-paths generally hide this splitting because they follow symmetry lines that in most cases enforce spin degeneracy. We present AlterSeeK-Path, an open-source Python tool that systematically constructs generalized band-structure paths for collinear altermagnets. The method selects the centroid of the conventional irreducible wedge used in routine band-structure calculations as the representative general k-point, maps it to a spin-flip-related partner, and inserts paired segments through these points into the standard high-symmetry path; these segments systematically sample the interior of the irreducible wedge. We demonstrate the construction for all 54 three-dimensional combinations of extended Bravais lattice type and spin Laue group across the six crystal systems that support collinear altermagnetism, and for the 12 two-dimensional cases spanning the four compatible two-dimensional Bravais lattices. Representative band structures are shown for the distinct lattice/path cases. With AlterSeeK-Path, these band structures can be constructed with essentially the same effort as conventional band structures.

cond-mat.mtrl-sci↗

arXiv2026

First-principles finite-size correction schemes for point defects of Cu$_3$N

Point defects play a key role in determining semiconductor properties, such as electrical conductivity and photoluminescence, and often enable functional behavior. Accurate first-principles supercell simulations of point defects require reliable finite-size corrections. In this study, we combine PBE+U structural relaxations with HSE hybrid-functional calculations to determine defect formation energies and thermodynamic transition levels of Cu$_3$N. Finite-size trends are quantified using $Γ$-point calculations in supercells containing 256, 864, and 2048 atoms. We assess and extend the Makov-Payne and Lany-Zunger correction schemes by introducing additional $1/L^n$ terms, together with core-level potential alignment and defect-specific scaling models. Using Cu$_3$N as a case study, we show that charged vacancies with strongly localized defect states are accurately described by the Makov-Payne-type scaling ($1/L + 1/L^{3}$), whereas interstitial defects with shallow or weakly localized electronic character are better captured by a hydrogenic impurity model that accounts for defect-band dispersion. Residual trends for neutral or weakly localized defects are described by higher-order polynomial fits in $1/L^{3}$ and $1/L^{4}$. Hybrid-functional energetics corrected using PBE+U-based finite-size trends confirm the intrinsic $p$-type character of Cu$_3$N under the conditions considered and demonstrate that no single finite-size correction can be transferred across all defect types.

cond-mat.mtrl-sci↗

arXiv2025

Confinement-Driven Exciton Behavior in 2D Halide Perovskites from Dielectric-Dependent Hybrid Methods

Understanding how dielectric anisotropy governs excitonic behavior in two-dimensional (2D) halide perovskites is critical for predicting and engineering their optoelectronic properties. In this work, we investigate Cs(n+1)PbnBr3n+1 nanoplatelets (n = 2-5) experimentally and theoretically and show that the interplay between dielectric confinement and anisotropic screening critically determines both their electronic structure and excitonic landscape. To incorporate the dielectric screening effects, the Coulomb kernel in the Fock exchange term is refined using a model dielectric function together with a model Bethe-Salpeter Equation approach. The exciton binding energies show a monotonic decrease from 0.26 eV to 0.21 eV from n = 2 to 5, with 20 meV decrease per layer up to n = 4, and thereafter less change. The relatively small change per layer is a consequence of the strong spatial localization of excitons. By analyzing directionally resolved dielectric tensors, we demonstrate that the in-plane dielectric constant predominantly dictates optical transitions and is close to converging to the bulk value already at n = 5, while the out-of-plane dielectric response reflects the confined nature of excitonic wave functions as expected. Our calculated absorption spectra capture experimental results within 0.02 eV throughout the confinement regime (n = 2-5). The effects of lattice dynamics on the dimensionally dependent dielectric response and subsequent exciton screening occurring on longer time-scales than the optical response are also analyzed, important for analysis and interpretation of exciton lifetime, diffusion, and band alignments. The results establish a clear correlation between dielectric anisotropy, electronic structure, and exciton binding energy at different timescales in layered perovskites, providing essential insight for the design of 2D optoelectronic materials and devices.

cond-mat.mtrl-sci↗

arXiv2025

High-throughput screening of charge-order-induced ferroelectrics

Charge-order-induced ferroelectrics display important technological applications in spintronics devices due to the possibility of magnetoelectric coupling and fast electronic switching. However, the list of known charge-order-induced ferroelectrics remains limited, hindering the fundamental understanding of the phenomena and the optimization of materials for real applications. In this work, we develop a high-throughput workflow to screen for charge-order-induced ferroelectrics in The Materials Project database. We use the local symmetry and bond valence sum to determine 147 materials displaying a coexistence of charge order and ferroelectric polarization. Then, ab initio simulations are used to identify 21 charge-order-induced ferroelectric candidates in which the ferroelectric polarization originates from or is structurally coupled to the charge order. For the final 21 candidates, we use symmetry-adapted modes and first-principles calculations to determine the structural coupling term between charge order and polar distortions and compute electronic properties, respectively.

cond-mat.mtrl-sci↗

arXiv2025

G-type Antiferromagnetic BiFeO$_3$ is a Multiferroic $g$-wave Altermagnet

G-type antiferromagnetic BiFeO$_3$ is shown to be an altermagnet. We present the band structure using an unconventional scheme designed to highlight the distinctive spin splitting which is characteristic of altermagnets. We define and show plots of the spin-splitting function in reciprocal space. We show that the nodal surfaces of the spin-splitting function that follow from symmetry can be classified into two types, which we call symmetry-enforced and continuity-enforced. We describe the spin-splitting function with a simple parametrization in a basis of symmetry-adapted plane waves. Using group-theory analysis based on irreducible representations of the crystallographic Laue group, we confirm that the altermagnetism of G-type BiFeO$_3$ is $g$-wave and present a complete classification table for the general three-dimensional case. Finally, we discuss the effect of ferroelectric switching on the altermagnetic order, and identify three classes of ferroelectric altermagnets.

cond-mat.mtrl-sci↗

arXiv2025

Intrinsic inverse band gap versus polarization relation in ferroelectric materials

Ferroelectric materials have promising applications in solar-energy conversion and electro-optic devices. The internal gradient fields produced by the macroscopic polarization may improve electronic and transport semiconducting properties. However, ferroelectrics tend to display relatively large band gaps and hence low solar-energy conversion efficiencies. In this work, we explore materials with an intrinsic inverse relation between band gap and polarization in a single ferroelectric phase. Ferroelectrics with an inverse band gap versus polarization relation are characterized by low density of states contribution at the conduction states and negligible orbital hybridization at the valence states. We use high-throughput and first principles methods to find 15 ferroelectric materials with an inverse band gap versus polarization relation in the Materials Project database. Our work provides a new pathway to design small-band gap large-polarization ferroelectrics, by simultaneously tailoring the band gap and polarization of ferroelectrics with an inverse relation through an external tuning parameter.

cond-mat.mtrl-sci↗

arXiv2024

Interfacial proximity and interplay between Kondo and short-range magnetic correlations in heterostructures

In this work, we investigate the influence of interlayer distance in a heterostructure containing both Kondo effects and short-range magnetic correlations. Our proposed heterostructure comprises three coupled square lattice layers. The first layer is governed by the Kondo-Heisenberg lattice model involving $f$- and $d$-electrons, which interact via Kondo and Heisenberg couplings, $J_{K}$ and $J_{H}$, respectively. The other two layers consist of non-interacting itinerant electrons, where coupling with the first layer is determined by two perpendicular hopping parameters. We find that varying the interlayer couplings induces electronic dynamics at the interface, altering the behavior of mean-field parameters describing the Kondo effect and short-range magnetic correlations. The system's temperature - interlayer hopping parameter phase diagram exhibits a sequence of discontinuous and continuous transitions. In the cases, $|J_{K}|<|J_{H}|$ and $|J_{K}|>|J_{H}|$ rich phase diagrams are found which include Kondo, ferromagnetic and antiferromagnetic correlations. Our work provides insights into hosting Kondo correlations in heterostructures.

cond-mat.str-el↗

arXiv2022

"Double-path" ferroelectrics and the sign of the piezoelectric response

In this work, we propose a class of ferroelectrics (which we denote "double-path" ferroelectrics), characterized by two competing polarization switching paths for which the change in polarization is different and in fact of opposite sign. Depending on which path is favorable under given conditions, this leads to different identification of up- and down-polarized states. Since the sign of piezoelectric response depends on the assignment of up- or down-polarized state for a specific structure, this means that the material can exhibit different signs of the piezoelectric response under different conditions. We focus on HfO$_2$ as a key example. Our first-principles calculations show that there are two competing paths in HfO$_2$, resulting from different displacements of the atoms from the initial to the final structures, and the change in polarization along these two paths is of opposite sign. These results provide a natural explanation for the recently observed discrepancy in the signs of piezoelectric responses in HfO$_2$ between theoretical first-principles calculations and experimental observation. Further, this allows predictions of how to favor one path over another by changes in conditions and compositional tuning. This family of materials also includes other candidates, such as CuInP$_2$S$_6$ and theoretically proposed LaVO$_3$-SrVO$_3$ superlattice. We finally note that double-path ferroelectrics possess novel electromechanical properties since the signs of their piezoelectric responses can be switched.

cond-mat.mtrl-sci↗

arXiv2021

Antiferroelectric negative capacitance from a structural phase transition in zirconia

Crystalline materials with broken inversion symmetry can exhibit a spontaneous electric polarization, which originates from a microscopic electric dipole moment. Long-range polar or anti-polar order of such permanent dipoles gives rise to ferroelectricity or antiferroelectricity, respectively. However, the recently discovered antiferroelectrics of fluorite structure (HfO$_2$ and ZrO$_2$) are different: A non-polar phase transforms into a polar phase by spontaneous inversion symmetry breaking upon the application of an electric field. Here, we show that this structural transition in antiferroelectric ZrO$_2$ gives rise to a negative capacitance, which is promising for overcoming the fundamental limits of energy efficiency in electronics. Our findings provide insight into the thermodynamically 'forbidden' region of the antiferroelectric transition in ZrO$_2$ and extend the concept of negative capacitance beyond ferroelectricity. This shows that negative capacitance is a more general phenomenon than previously thought and can be expected in a much broader range of materials exhibiting structural phase transitions.

cond-mat.mtrl-sci↗

arXiv2019

Ferroelectricity in [111]-oriented epitaxially strained SrTiO$_3$ from first principles

We use first principles density functional theory calculations to investigate the effect of biaxial strain in the low-temperature structural and ferroelectric properties of [111]-oriented SrTiO$_3$. We find that [111] biaxial strain, achievable by coherent epitaxial growth along the [111] direction, induces structural distortions in SrTiO$_3$ that are not present in either bulk or [001]-oriented SrTiO$_3$. Under [111] biaxial strain, SrTiO$_3$ displays ferroelectricity at tensile strain, and paraelectricity at compressive strain. We compute the phonon spectrum and macroscopic polarization of SrTiO$_3$ as a function of [111] biaxial strain, and relate our results to the predictions of the free energy phenomenological model of Pertsev, Tagantsev and Setter [Phys. Rev. B 61, 825 (2000); Phys. Rev. B 65, 219901 (2002)].

cond-mat.mtrl-sci↗

arXiv2016

Electric field and strain induced Rashba effect in hybrid halide perovskites

Using first principles density functional theory calculations, we show how Rashba-type energy band splitting in the hybrid organic-inorganic halide perovskites APbX$_3$ (A=CH$_3$NH$_3^+$, CH(NH$_2$)$_2^+$, Cs$^+$ and X=I, Br) can be tuned and enhanced with electric fields and anisotropic strain. In particular, we demonstrate that the magnitude of the Rashba splitting of tetragonal (CH$_3$NH$_3$)PbI$_3$ grows with increasing macroscopic alignment of the organic cations and electric polarization, indicating appreciable tunability with experimentally-feasible applied fields, even at room temperature. Further, we quantify the degree to which this effect can be tuned via chemical substitution at the A and X sites, which alters amplitudes of different polar distortion patterns of the inorganic PbX$_3$ cage that directly impact Rashba splitting. In addition, we predict that polar phases of CsPbI$_3$ and (CH$_3$NH$_3$)PbI$_3$ with $R3c$ symmetry possessing considerable Rashba splitting might be accessible at room temperature via anisotropic strain induced by epitaxy, even in the absence of electric fields.

cond-mat.mtrl-sci↗

arXiv2016

Effects of quantum confinement on excited state properties of SrTiO$_3$ from ab initio many-body perturbation theory

The Ruddlesden-Popper (RP) homologous series Sr$_{n+1}$Ti$_{n}$O$_{3n+1}$ provides a useful template for the study and control of the effects of dimensionality and quantum confinement on the excited state properties of the complex oxide SrTiO$_3$. We use ab initio many-body perturbation theory within the $GW$ approximation and the Bethe-Salpeter equation approach to calculate quasiparticle energies and absorption spectrum of Sr$_{n+1}$Ti$_{n}$O$_{3n+1}$ for $n=1-5$ and $\infty$. Our computed direct and indirect optical gaps are in excellent agreement with spectroscopic measurements. The calculated optical spectra reproduce the main experimental features and reveal excitonic structure near the gap edge. We find that electron-hole interactions are important across the series, leading to significant exciton binding energies that increase for small $n$ and reach a value of 330~meV for $n=1$, a trend attributed to increased quantum confinement. We find that the lowest-energy singlet exciton of Sr$_2$TiO$_4$ ($n=1$) localizes in the 2D plane defined by the TiO$_2$ layer, and explain the origin of its localization.

cond-mat.mtrl-sci↗

arXiv2014

Antiferroelectricity in thin film ZrO2 from first principles

Density functional calculations are performed to investigate the experimentally-reported field-induced phase transition in thin-film ZrO2 (J. Muller et al., Nano. Lett. 12, 4318). We find a small energy difference of ~ 1 meV/f.u. between the nonpolar tetragonal and polar orthorhombic structures, characteristic of antiferroelectricity. The requisite first-order transition between the two phases, which atypically for antiferroelectrics have a group-subgroup relation, results from coupling to other zone-boundary modes, as we show with a Landau-Devonshire model. Tetragonal ZrO2 is thus established as a previously unrecognized lead-free antiferroelectric with excellent dielectric properties and compatibility with silicon. In addition, we demonstrate that a ferroelectric phase of ZrO2 can be stabilized through epitaxial strain, and suggest an alternative stabilization mechanism through continuous substitution of Zr by Hf.

cond-mat.mtrl-sci↗

arXiv2014

Antiferroelectricity and ferroelectricity in epitaxially strained PbZrO3 from first principles

Density functional calculations are performed to study the effect of epitaxial strain on PbZrO3. We find a remarkably small energy difference between the epitaxially strained polar R3c and nonpolar Pbam structures over the full range of experimentally accessible epitaxial strains -3% < η< 4%. While ferroelectricity is favored for all compressive strains, for tensile strains the small energy difference between the nonpolar ground state and the alternative polar phase yields a robust antiferroelectric ground state. The coexistence of ferroelectricity and antiferroelectricity observed in thin films is attributed to a combination of strain and depolarization field effects.

cond-mat.mtrl-sci↗