arXiv subjects

Salvador Barraza-Lopez

Publications and source records attributed to Salvador Barraza-Lopez.

At least 19 recordsLinked to original sources

arXiv2026

Sliding and stacking thin homo-monolayers from energy landscapes and combinatorics

Structure leads to function: Knowing all possible ways to stack and slide identical monolayers enables the design of functionalities such as nonlinear optical responses and ferroelectricity in layered materials. Besides, mounting experimental evidence points to differing stacking configurations in few-monolayer and bulk samples. To exemplify the core concepts for stacking arbitrary monolayers, ground-state and metastable non-moiré SnSe stacks were first identified using density functional theory and employed to validate a ``divide and conquer'' combinatoral approach for determining the most probable stacking configurations in materials with an arbitrary number of identical monolayers. A small number of point groups accounts for all possible stacks, which explains experimental second-harmonic optical responses. Finite-temperature effects are also studied despite the granularity of available data. This comprehensive framework readily generalizes to provide a predictive description of arbitrary metastable few-homomonolayer stacks.

cond-mat.mtrl-sci↗

arXiv2026

Tuning Terahertz Optomechanics of MoS2 Bilayers with Homogeneous In-plane Strain

Homogeneous in-plane biaxial tensile strain strengthens the out-of-plane van der Waals (vdW) interaction in \MoS\ bilayers (BLs) and can be used to fine-tune their terahertz (THz) oscillations. Using ultralow-frequency Raman spectroscopy on hexagonal (2H) and rhombohedral (2R) stacked BLs, we observe a hardening of the interlayer breathing modes originating from a strain-induced Poisson contraction of the vdW separation between the layers characterized by an effective out-of-plane Poisson's ratio of $ν_\mathrm{eff} \approx 0.19\text{--}0.24$. Strikingly, this geometric contraction drives the system into a highly repulsive regime of the intermolecular potential, corresponding to a Grüneisen parameter of $γ\approx 14\text{--}20$. This value surpasses even the `giant' one reported for phosphorene, establishing these van der Waals BLs as highly tunable nonlinear mechanical platforms that can be addressed at the THz regime without external pressure knobs.

cond-mat.mtrl-sci↗

arXiv2025

Perturbative second-order optical susceptibility of bulk materials: a symmetry-enforced return to non-orthogonal localized basis sets

The second-order optical susceptibility of semiconductors $χ_{ijk}^{(2)}(-2ω;ω,ω)$ finds application in metrology, spectroscopy, telecommunications, material characterization, and quantum information. Pioneering calculations of $χ_{ijk}^{(2)}(-2ω;ω,ω)$ utilized non-orthogonal Gaussian orbitals centered at atoms. That formulation transitioned into plane-wave-based algorithms as time went by. As of late, nevertheless, multiple tools for calculating optical susceptibilities have recast the problem using Wannier ({\em i.e.}, {\em localized}) orbitals, making a comeback onto frameworks based on localized basis sets. Here, we present an approach for calculating $χ_{ijk}^{(2)}(-2ω;ω,ω)$ reliant on numerical pseudoatomic orbitals (PAOs) within perturbation theory in the velocity gauge. Its salient feature is a calculation of `Slater-Koster-like' two-center integrals of the momentum operator in between PAOs identified by symmetry. The approach was successfully tested on paradigmatic cubic silicon carbide (3C-SiC) and gallium arsenide, for which linear responses are contributed as well.

cond-mat.mtrl-sci↗

arXiv2025

Sliding multiferroicity in hexagonal stacked CrI3

Developing new multiferroics at the two-dimensional (2D) limit with energy-efficient magnetoelectric coupling can inform the interplay physics of novel orders and advance on-chip high-performance computing applications. Here we apply stacking order engineering to create a new type of 2D multiferroics, namely sliding multiferroics, based on polar hexagonal stacked (H-stacked) CrI3. This new stacking order removes structural inversion symmetry and gives rise to room temperature sliding ferroelectricity, as confirmed by Raman spectroscopy, second harmonic generation spectroscopy and electrical transport measurements. Building upon the gate-dependent reflective magnetic circular dichroism, first-principles calculations, and modeling, sliding ferroelectricity is shown to interplay with an emergent interfacial ferromagnetism via interlayer spin-polarized charge transfer. This coupling mechanism results in non-volatile magnetic switching by as low as 0.4V across the H-stacked CrI3. Our demonstration introduces polar stacking order engineering of 2D magnets as a general approach to create non-volatile 2D multiferroics with efficient magnetoelectric coupling, paving the way for low-power electronics and spintronics at the atomically thin limit.

cond-mat.mtrl-sci↗

arXiv2025

Reference lattice, sound, stiffness, and magnetic transitions of Ising monolayers

A reference lattice, away from which elastic distortions induced by the spin texturing of 2D magnets take hold, is motivated from a picture of pairwise Biot-Savart interactions among identical solenoids that either elongate or compress a (``zero-current'') spring lattice. Applied to a paradigmatic CrSiTe$_3$ monolayer (ML), the reference is given by the average between the atomic positions of FM and Néel AFM lattices; such an atomic disposition permits understanding structural distortions and elastic energies due to magnetism readily. Furthermore, the anisotropic speed of sound in the magnetic ground state explains an observed anisotropy of vibrational frequencies on similar magnets. Elastic stiffness constants are reported, too. Magnetic energies in four Ising structural configurations were calculated, and the strain needed for those 2D magnets to undergo an AFM to FM quantum phase transition was determined as well.

cond-mat.mtrl-sci↗

arXiv2024

Winding Berry dipole on uniaxially strained graphene/hBN/hBN moiré trilayers

Nonlinear Hall-like currents can be generated by a time-periodic alternating bias on two-dimensional (2D) materials lacking inversion symmetry. To hint that the moiré between graphene and its supporting substrate contributes to the homogeneity of nonlinear currents, the change in the local potential $ΔV(r)$ around horizontally strained graphene due to a homobilayer of hexagonal boron nitride (hBN) was obtained from ab initio calculations, and corrections to on-site energies and hopping matrix elements on graphene's tight-binding electronic dispersion of $π-$electrons were calculated. Relying on a semiclassical approximation, Berry dipoles $D$ are seen to change orientation and wind throughout the moiré lattice.

cond-mat.mes-hall↗

arXiv2024

Insulating moiré homobilayers lack a threefold symmetric second harmonic generation

Atoms within moiré bilayers relax in-plane to minimize elastic energy [e.g., Cazeaux et al., J. Elast. 154, 443 (2023)]; such relaxation brings their space group symmetries down to P1. Here, the ab initio second harmonic generation (SHG) of twisted and atomistically optimized hBN bilayers was determined at four twist angles ($θ=38.21^{\circ}$, $60.00^{\circ}$, $73.17^{\circ}$, and $98.21^{\circ}$) and for three displacements $\boldsymbolτ$ measured away from the ground state $AA^{\prime}$ configuration. All moiré bilayers have a P1 space symmetry after structural optimization. This situation is quite different to monolayers with hexagonal lattices, which retain a three-fold symmetry. We point out that the actual symmetries of the SHG reported for hBN bilayers on two experimental works do not coincide with the sixfold symmetric theoretical profiles they provide [either $\sin^2(3ϕ)$ or $\cos^2(3ϕ)$], and show that the intrinsic low structural symmetry of (atomically optimized) hBN bilayer moirés can in fact be read out from experimental SHG intensity profiles--which are tunable by $θ$ and by the frequency of light $ω$: The SHG is most definitely not sixfold-symmetric because moirés do not retain a three-fold symmetry. Furthermore, an extrinsic twofold symmetry of the SHG emission is realized by tilting the pump by an angle $α$ away from the 2D material's normal, regardless of $θ$ and $ω$. The design of in-plane and ultrathin sources of SHG with low symmetry could be useful for the eventual creation of entanglement sources from 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Tight-binding model with sublattice-asymmetric spin-orbit coupling for square-net nodal line Dirac semimetals

We study a 4-orbital tight-binding (TB) model for ZrSiS from the square sublattice generated by the Si atoms. After studying three other alternatives, we endow such model with a new effective spin-orbit coupling (SOC) consistent with {\em ab initio} dispersions around the Fermi energy ($E_F$) in four systematic steps: (1) We calculate the electronic dispersion of bulk ZrSiS using an implementation of density-functional theory (DFT) based on numeric atomic orbitals [{\em J. Phys.: Condens. Matter} {\bf 14}, 2745 (2002)] in which on-site and off-site SOC can be told apart. As a result, we determine that local SOC-induced band gaps around $E_F$ are predominantly created by the on-site contribution. (2) Gradually reducing the atomic basis set size, we then create an electronic band structure with 16 orbitals per unit cell (u.c.) which retains the qualitative features of the dispersion around $E_F$, including SOC-induced band gaps. (3) Zr is the heaviest element on this compound and it has a non-negligible contribution to the electronic dispersion around $E_F$; we show that it provides the strongest contribution to the SOC-induced band gap. (4) Using Löwdin partitioning approach, we project the effect of SOC onto the 4-orbital Hamiltonian. This way, we facilitate an effective SOC interaction that was explicitly informed by {\em ab initio} input.

cond-mat.mtrl-sci↗

arXiv2023

Creating a three dimensional intrinsic electric dipole on rotated CrI$_3$ bilayers

Two-dimensional (2D) materials are being explored as a novel multiferroic platform. One of the most studied magnetoelectric multiferroic 2D materials are antiferromagnetically-coupled (AFM) CrI$_3$ bilayers. Neglecting magnetism, those bilayers possess a crystalline point of inversion, which is only removed by the antiparallel spin configuration among its two constituent monolayers. The resultant intrinsic electric dipole on those bilayers has a magnitude no larger than 0.04 pC/m, it points out-of-plane, and it reverts direction when the--Ising-like--cromium spins are flipped (toward opposite layers {\em versus} away from opposite layers). The combined presence of antiferromagnetism and a weak intrinsic electric dipole makes this material a two-dimensional magnetoelectric multiferroic. Here, we remove the crystalline center of inversion of the bilayer by a relative $60^{\circ}$ rotation of its constituent monolayers. This process {\em enhances} the out-of-plane intrinsic electric dipole tenfold with respect to its magnitude in the non-rotated AFM bilayer and also creates an even stronger and switchable in-plane intrinsic electric dipole. The ability to create a three-dimensional electric dipole is important, because it enhances the magnetoelectric coupling on this experimentally accessible 2D material, which is explicitly calculated here as well.

cond-mat.mes-hall↗

arXiv2023

Thermally-driven phase transitions in freestanding low-buckled silicene, germanene, and stanene

Low-buckled silicene, germanene, and stanene are group$-IV$ graphene allotropes. They form a honeycomb lattice out of two interpenetrating ($A$ and $B$) triangular sublattices that are vertically separated by a small distance $Δ_z$. The atomic numbers $Z$ of silicon, germanium, and tin are larger to carbon's ($Z_C=6$), making them the first experimentally viable two-dimensional topological insulators. Those materials have a twice-energy-degenerate atomistic structure characterized by the buckling direction of the $B$ sublattice with respect to the $A$ sublattice [whereby the $B-$atom either protrudes {\em above} ($Δ_z>0$) or {\em below} ($Δ_z<0$) the $A-$atoms], and the consequences of that energy degeneracy on their elastic and electronic properties have not been reported thus far. Here, we uncover {\em ferroelastic, bistable} behavior on silicene, which turns into an {\em average} planar structure at about 600 K. Further, the creation of electron and hole puddles obfuscates the zero-temperature SOC induced band gaps at temperatures as low as 200 K, which may discard silicene as a viable two-dimensional topological insulator for room temperature applications. Germanene, on the other hand, never undergoes a low-buckled to planar 2D transformation, becoming amorphous at around 675 K instead, and preserving its SOC-induced bandgap despite of band broadening. Stanene undergoes a transition onto a crystalline 3D structure at about 300 K, preserving its SOC-induced electronic band gap up to that temperature. Unlike what is observed in silicene and germanene, stanene readily develops a higher-coordinated structure with a high degree of structural order. The structural phenomena is shown to have deep-reaching consequences for the electronic and vibrational properties of those two dimensional topological insulators.

cond-mat.mtrl-sci↗

arXiv2022

Two-atom-thin topological crystalline insulators lacking out of plane inversion symmetry

A two-dimensional topological crystalline insulator (TCI) with a single unit cell (u.c.) thickness is demonstrated here. To that end, one first shows that tetragonal ($C_4$ in-plane) symmetry is not a necessary condition for the creation of zero-energy metallic surface states on TCI slabs of finite-thicknesses, because zero-energy states persist even as all the in-plane rotational symmetries--furnishing topological protection--are completely removed. In other words, zero-energy levels on the model are not due to (nor are they protected by) topology. Furthermore, effective twofold energy degeneracies taking place at few discrete $k-$points away from zero energy in the bulk Hamiltonian--that are topologically protected--persist at the u.c.~thickness limit. The chiral nature of the bulk TCI Hamiltonian permits creating a $2\times 2$ square Hamiltonian, whose topological properties remarkably hold invariant at both the bulk and at the single u.c.~thickness limits. The identical topological characterization for bulk and u.c.-thick phases is further guaranteed by a calculation involving Pfaffians. This way, a two-atom-thick TCI is deployed hereby, in a demonstration of a topological phase that holds both in the bulk, and in two dimensions.

cond-mat.mes-hall↗

arXiv2022

Slippery paraelectric transition metal dichalcogenide bilayers

Traditional ferroelectrics undergo thermally-induced phase transitions whereby their structural symmetry increases. The associated higher-symmetry structure is dubbed {\em paraelectric}. Ferroelectric transition metal dichalcogenide bilayers have been recently shown to become paraelectric, but not much has been said of the atomistic configuration of such a phase. As discovered through numerical calculations that include molecular dynamics here, their paraelectricity can only be ascribed to a time average of ferroelectric phases with opposing intrinsic polarizations, whose switching requires macroscopically large areas to slip in unison.

cond-mat.mtrl-sci↗

arXiv2022

Elasticity of 2D ferroelectrics across their paraelectric phase transformation

The mechanical behavior of two-dimensional (2D) materials across 2D phase changes is unknown, and the finite temperature ($T$) elasticity of paradigmatic SnSe monolayers -- ferroelectric 2D materials turning paraelectric as their unit cell (u.c.) turns from a rectangle onto a square -- is described here in a progressive manner. To begin with, their zero$-T$ {\em elastic energy landscape} gives way to (Boltzmann-like) averages from which the elastic behavior is determined. These estimates are complemented with results from the strain-fluctuation method, which employs the energy landscape or {\em ab initio} molecular dynamics (MD) data. Both approaches capture the coalescence of elastic moduli $\langle C_{11}(T)\rangle=\langle C_{22}(T)\rangle$ due to the structural transformation. The broad evolution and sudden changes of elastic parameters $\langle C_{11}(T)\rangle$, $\langle C_{22}(T)\rangle$, and $\langle C_{12}(T)\rangle$ of these atomically-thin phase-change membranes establishes a heretofore overlooked connection among 2D materials and soft matter.

cond-mat.mtrl-sci↗

arXiv2021

Magnetic Topological Semimetal Phase with Electronic Correlation Enhancement in SmSbTe

The ZrSiS family of compounds hosts various exotic quantum phenomena due to the presence of both topological nonsymmorphic Dirac fermions and nodal-line fermions. In this material family, the LnSbTe (Ln= lanthanide) compounds are particularly interesting owing to the intrinsic magnetism from magnetic Ln which leads to new properties and quantum states. In this work, the authors focus on the previously unexplored compound SmSbTe. The studies reveal a rare combination of a few functional properties in this material, including antiferromagnetism with possible magnetic frustration, electron correlation enhancement, and Dirac nodal-line fermions. These properties enable SmSbTe as a unique platform to explore exotic quantum phenomena and advanced functionalities arising from the interplay between magnetism, topology, and electronic correlations.

cond-mat.mtrl-sci↗

arXiv2021

Metastable piezoelectric group IV monochalcogenide monolayers with a buckled honeycomb structure

Twelve two-dimensional group-IV monochalcogenide monolayers (SiS, SiSe, SiTe, GeS, GeSe, GeTe, SnS, SnSe, SnTe, PbS, PbSe, and PbTe) with a buckled honeycomb atomistic structure--belonging to symmetry group P3m1--and an out-of-plane intrinsic electric polarization are shown to be metastable by three independendent methods. First, we uncover a coordination-preserving structural transformation from the low-buckled honeycomb structure onto the lower-energy Pnm2$_1$ (or Pmmn for PbS, PbSe, and PbTe) phase to estimate {\em energy barriers} $E_B$ that must be overcome during such structural transformation. Using the curvature of the local minima and $E_B$ as inputs to Kramers escape formula, large escape times are found, implying the structural metastability of the buckled honeycomb phase (nevertheless, and with the exception of PbS and PbSe, these phases display escape times ranging from 700 years to multiple times the age of the universe, and can be considered "stable" for practical purposes only in that relative sense). The second demonstration is provided by phonon dispersion relations that include the effect of long-range Coulomb forces and display no negative vibrational modes. The third and final demonstration of structural metastability is furnished by room-temperature {\em ab initio} molecular dynamics for selected compounds. The magnitude of the electronic band gap evolves with chemical composition. Different from other binary two-dimensional compounds such as transition metal dichalcogenide monolayers and hexagonal boron nitride monolayers which only develop an in-plane piezoelectric response, the twelve group-IV monochalcogenide monolayers with a buckled honeycomb structure also display out-of-plane piezoelectric properties.

cond-mat.mtrl-sci↗

arXiv2020

Thermoelectricity of Tin Selenide Monolayers Across a Structural Phase Transition

SnSe monolayers experience a temperature induced two-dimensional Pnm2$_1 \to$ P4/nmm structural transformation precipitated by the softening of vibrational modes. The standard theoretical treatment of thermoelectricity---which relies on a zero temperature phonon dispersion and on a zero temperature electronic structure---is incapable of describing thermoelectric phenomena induced by structural transformations. Relying on structural data obtained from {\em ab initio} molecular dynamics calculations that is utilized in a non-standard way to inform of electronic and vibrational transport coefficients, the present work establishes a general route to understand thermoelectricity across phase transitions. Similar to recent experimental observations pointing to an overestimated thermoelectric figure of merit $ZT$ past the transition temperature, our work indicates a smaller $ZT$ when compared to its value predicted by the standard paradigm. Its decrease is related to the dramatic changes in the electrical conductivity and lattice thermal conductivity as the structural transformation ensues. Though exemplified on a SnSe monolayer, the method does not have any built-in assumptions concerning dimensionality, and thus applicable to arbitrary thermoelectric materials in one, two, and three dimensions.

cond-mat.mtrl-sci↗

arXiv2020

Beyond Graphene: Low-Symmetry and Anisotropic 2D Materials

Low-symmetry 2D materials---such as ReS$_2$ and ReSe$_2$ monolayers, black phosphorus monolayers, group-IV monochalcogenide monolayers, borophene, among others---have more complex atomistic structures than the honeycomb lattices of graphene, hexagonal boron nitride, and transition metal dichalcogenides. The reduced symmetries of these emerging materials give rise to inhomogeneous electron, optical, valley, and spin responses, as well as entirely new properties such as ferroelasticity, ferroelectricity, magnetism, spin-wave phenomena, large nonlinear optical properties, photogalvanic effects, and superconductivity. Novel electronic topological properties, nonlinear elastic properties, and structural phase transformations can also take place due to low symmetry. The "Beyond Graphene: Low-Symmetry and Anisotropic 2D Materials" Special Topic was assembled to highlight recent experimental and theoretical research on these emerging materials.

cond-mat.mes-hall↗

arXiv2020

Colloquium: Physical properties of group-IV monochalcogenide monolayers

We survey the state-of-the-art knowledge of ferroelectric and ferroelastic group-IV monochalcogenide monolayers. These semiconductors feature remarkable structural and mechanical properties, such as a switchable in-plane spontaneous polarization, soft elastic constants, structural degeneracies, and thermally-driven two-dimensional structural transformations. Additionally, these 2D materials also display selective valley excitations, valley Hall effects, and persistent spin helix behavior. After a description of their Raman spectra, a discussion of optical properties arising from their lack of centrosymmetry---such as an unusually strong second-harmonic intensity, large bulk photovoltaic effects, photostriction, and tunable exciton binding energies---is provided as well. The physical properties observed in these materials originate from (correlate with) their intrinsic and switchable electric polarization, and the physical behavior hereby reviewed could be of use in non-volatile memory, valleytronic, spintronic, and optoelectronic devices: these 2D multiferroics enrich and diversify the 2D materials toolbox.

cond-mat.mes-hall↗