Searcharxiv⌕ Search

arXiv subjects

Daniel Hernangómez-Pérez

Publications and source records attributed to Daniel Hernangómez-Pérez.

18 recordsLinked to original sources

Optical Response Beyond Magnetic Symmetries

The optical response of magnetic materials is conventionally classified through magnetic space groups (MSGs), where spin and lattice are locked by the relativistic spin-orbit interaction. However, most optical observables are governed primarily by nonrelativistic physics, and thus a purely MSG-based description can overlook important insights. Here we systematically show that spin-space groups (SSGs), which operate at the nonrelativistic level, provide a broader and more predictive framework for analyzing a variety of optical responses of magnets. Focusing on linear optical absorption, we derive the transformation rules imposed by SSGs and show that they generate effective real-space point groups, which can enforce relations among charge response coefficients that are absent from conventional MSG analysis. We illustrate the basic principle in a Lieb-lattice altermagnet model with tunable spin-orbit coupling, where SSG predictions on the linear dichroism remain remarkably accurate even when relativistic band splittings become sizable. We further establish the predictive power of this framework through first-principles calculations on two altermagnetic candidates: the actinide UCr2Si2C, where the optical absorption remains nearly isotropic despite its strong spin-orbit coupling and the pronounced anisotropy apparent from magnetic symmetries, and the transition-metal fluoride RbMnF4, where birefringence is confined to a single plane by symmetries emerging exclusively from SSGs. Finally, we extend the concept to the spin Hall response of the coplanar noncollinear antiferromagnet ScMnO3, where SSGs explain the hierarchy of calculated spin Hall coefficients, demonstrating their direct relevance to spintronics as well.

cond-mat.mtrl-sci↗

Many-body quantum chaos in excitonic spectra from first principles

We demonstrate that realistic excitonic many-body Hamiltonians obtained from first-principles GW-Bethe-Salpeter equation calculations can exhibit quantum chaos governed by random-matrix universality. Considering a prototypical van der Waals heterostructure (WS$_2$-graphene), with and without lattice disorder, we analyze their energy-resolved spectral correlations and identify a disorder-driven crossover from regular to complete chaotic dynamics. We show that while pristine samples exhibit incomplete chaos (non-ergodicity) due to an approximate valley symmetry that restricts excitonic mixing, the presence of disorder-induced electronic flat bands act as a catalyst for valley mixing to drive the system into a fully developed chaotic (ergodic) regime with reduced symmetry. Crucially, fluctuations in many-body oscillator strengths are shown to follow universal Porter-Thomas statistics, directly linking the underlying quantum chaos and experimentally accessible optical observables. Finally, by examining long-range spectral correlations, we estimate the Thouless time associated to excitonic mixing across the entire many-body bandwidth. Our results establish excitons as a highly tunable platform for probing many-body ergodicity and its spectroscopic signatures in realistic interacting 2D materials.

cond-mat.mes-hall↗

Efficient prediction of highly anisotropic excitonic properties in the layered antiferromagnet CrSBr via time-dependent density functional theory

CrSBr, a layered anisotropic van der Waals antiferromagnet, has recently emerged as a versatile platform where strong coupling between optical excitations and magnetic order enables magneto-optical control in low dimensions. While experiments have progressed rapidly, predictive and reliable ab initio descriptions remain limited to self-consistent, many-body perturbation theory that is computationally expensive and technically challenging. Here we present an alternative approach that accurately predicts the electronic and optical properties of CrSBr at substantially lower computational cost, while retaining quantitative accuracy in the coupling between excitons and magnetic order. Using a tuned hybrid density functional with on-site corrections, we reproduce fundamental and optical gaps and quantitatively capture the interaction between excitonic transitions and magnetic order. We then employ this functional to investigate excitonic shifts induced by spin canting, that would result from applying an external magnetic field. Our results establish an efficient framework for modeling excitonic and magneto-optical phenomena in layered magnetic semiconductors.

cond-mat.mtrl-sci↗

Roadmap on Advancements of the FHI-aims Software Package

Electronic-structure theory is the foundation of the description of materials including multiscale modeling of their properties and functions. Obviously, without sufficient accuracy at the base, reliable predictions are unlikely at any level that follows. The software package FHI-aims has proven to be a game changer for accurate free-energy calculations because of its scalability, numerical precision, and its efficient handling of density functional theory (DFT) with hybrid functionals and van der Waals interactions. It treats molecules, clusters, and extended systems (solids and liquids) on an equal footing. Besides DFT, FHI-aims also includes quantum-chemistry methods, descriptions for excited states and vibrations, and calculations of various types of transport. Recent advancements address the integration of FHI-aims into an increasing number of workflows and various artificial intelligence (AI) methods. This Roadmap describes the state-of-the-art of FHI-aims and advancements that are currently ongoing or planned.

cond-mat.mtrl-sci↗

Efficient $GW$ band structure calculations using Gaussian basis functions and application to atomically thin transition-metal dichalcogenides

We present a $GW$ space-time algorithm for periodic systems in a Gaussian basis including spin-orbit coupling. We employ lattice summation to compute the irreducible density response and the self-energy, while we employ $k$-point sampling for computing the screened Coulomb interaction. Our algorithm enables accurate and computationally efficient quasiparticle band structure calculations for atomically thin transition-metal dichalcogenides. For monolayer MoS$_\text{2}$, MoSe$_\text{2}$, WS$_\text{2}$, and WSe$_\text{2}$, computed $GW$ band gaps agree on average within 50 meV with plane-wave-based reference calculations. $G_0W_0$ band structures are obtained in less than two days on a laptop (Intel i5, 192 GB RAM) or in less than 30 minutes using 1024 cores. Overall, our work provides an efficient and scalable framework for $GW$ calculations on atomically thin materials.

cond-mat.mtrl-sci↗

Generalized many-body exciton g-factors: magnetic hybridization and non-monotonic Rydberg series in monolayer WSe$_2$

Magneto-optics of low dimensional semiconductors, such as monolayer transition metal dichalcogenides, offers a vast playground for exploring complex quantum phenomena. However, current ab initio approaches fail to capture important experimental observations related to brightening of excitonic levels and their g-factor dependence. Here, we develop a robust and general first principles framework for many-body exciton g-factors by incorporating off-diagonal terms for the spin and orbital angular momenta of single-particle bands and many-body states for magnetic fields pointing in arbitrary spatial directions. We implement our framework using many-body perturbation theory via the GW-Bethe-Salpeter equation (BSE) and supplement our analysis with robust symmetry-based models, establishing a fruitful synergy between many-body GW-BSE and group theory. Focusing on the archetypal monolayer WSe$_2$, we accurately reproduce the known results of the low-energy excitons including the Zeeman splitting and the dark/grey exciton brightening. Furthermore, our theory naturally reveals fundamental physical mechanisms of magnetic-field hybridization of higher-energy excitons (s- and p-like) and resolves the long-standing puzzle of the experimentally measured non-monotonic Rydberg series (1s-4s) of exciton g-factors. Our framework offers a comprehensive approach to investigate, rationalize, and predict the non-trivial interplay between magnetic fields, angular momenta, and many-body exciton physics in van der Waals systems.

cond-mat.mes-hall↗

Surface-state engineering for nonlinear charge and spin photocurrent generation

We systematically explore a pathway for generating nonlinear charge and spin photocurrents using spin-orbit-split surface states. This mechanism enables net charge and spin flow along the surface plane even in centrosymmetric bulk environments like the Rashba prototype Au(111), where we establish the key principles by combining model predictions with density functional calculations. We further identify the Tl/Si(111) surface, characterized by strong non-Rashba spin-orbit coupling, as a prime candidate for experimental validation; with slight doping, it develops metallic spin-orbit-split states featuring remarkable relativistic properties while the bulk remains semiconducting. Our non-linear simulations reveal distinct angular signatures and magnitudes comparable to bulk ferroelectrics, highlighting the potential of surface-state photocurrents for low-bias optoelectronic applications. Moreover, the intricate spin polarization of surface states opens new possibilities as a nonlinear spin filter, providing a far more versatile platform than the spin Hall effect.

cond-mat.mes-hall↗

Molecular Transport

Single-molecule junctions - nanoscale systems where a molecule is connected to metallic electrodes - offer a unique platform for studying charge, spin and energy transport in non-equilibrium many-body quantum systems, with few parallels in other areas of condensed matter physics. Over the past decades, these systems have revealed a wide range of remarkable quantum phenomena, including quantum interference, non-equilibrium spin-crossover, diode-like behavior, or chiral-induced spin selectivity, among many others. To develop a detailed understanding, it turned out essential to have available ab initio-based tools for accurately describing quantum transport in such systems. They need to be capable of capturing the intricate electronic structure of molecules, sometimes in the presence of electron-electron or electron-phonon interactions, in out-of-equilibrium environments. Such tools are indispensable also for experimentally observed phenomena explained in terms of parametrized tight-binding models for the quantum transport problem. While FHI-aims also offers specialized transport routines, e.g. for chemically functionalized nanotubes or nanotube networks, our focus in this section is on the AITRANSS package designed for simulations of single-molecule transport. AITRANSS is an independent post-processing tool that combined with FHI-aims enables the calculation of electronic transport properties, as well as atom-projected density of states, spin properties and the simulation of scanning tunneling microscope images in molecular junctions. Pilot versions of the code extend some of these capabilities to non-linear transport in the applied bias, with plans to include these features in future releases of the package.

cond-mat.mes-hall↗

Designable exciton mixing through layer alignment in WS$_2$-graphene heterostructures

Optical properties of heterostructures composed of layered 2D materials, such as transition metal dichalcogenides (TMDs) and graphene, are broadly explored. Of particular interest are light-induced energy transfer mechanisms in these materials and their structural roots. Here, we use state-of-the-art first-principles calculations to study the excitonic composition and the absorption properties of WS$_2$-graphene heterostructures as a function of interlayer alignment and the local strain resulting from it. We find that Brillouin zone mismatch and the associated energy level alignment between the graphene Dirac cone and the TMD bands dictate an interplay between interlayer and intralayer excitons, mixing together in the many-body representation upon the strain-induced symmetry breaking in the interacting layers. Examining the representative cases of the 0$^\circ$ and 30$^\circ$ interlayer twist angles, we find that this exciton mixing strongly varies as a function of the relative alignment. We quantify the effect of these structural modifications on exciton charge separation between the layers and the associated graphene-induced homogeneous broadening of the absorption resonances. Our findings provide guidelines for controllable optical excitations upon interface design and shed light on the importance of many-body effects in the understanding of optical phenomena in complex heterostructures.

cond-mat.mtrl-sci↗

Low-scaling GW algorithm applied to twisted transition-metal dichalcogenide heterobilayers

The $GW$ method is widely used for calculating the electronic band structure of materials. The high computational cost of $GW$ algorithms prohibits their application to many systems of interest. We present a periodic, low-scaling and highly efficient $GW$ algorithm that benefits from the locality of the Gaussian basis and the polarizability. The algorithm enables $G_0W_0$ calculations on a MoSe$_2$/WS$_2$ bilayer with 984 atoms per unit cell, in 42 hours using 1536 cores. This is four orders of magnitude faster than a plane-wave $G_0W_0$ algorithm, allowing for unprecedented computational studies of electronic excitations at the nanoscale.

physics.chem-ph↗

Reduced absorption due to defect-localized interlayer excitons in transition metal dichalcogenide-graphene heterostructures

Associating the presence of atomic vacancies to excited-state transport phenomena in two dimensional semiconductors is of emerging interest, and demands detailed understanding of the involved exciton transitions. Here we study the effect of such defects on the electronic and optical properties of WS$_2$-graphene and MoS$_2$-graphene van der Waals heterobilayers by employing many-body perturbation theory. We find that the combination of chalcogen defects and graphene adsorption onto the transition metal dichalcogenide layer can radically alter the optical properties of the heterobilayer, due to a combination of dielectric screening, the impact of the missing chalcogen atoms in the intralayer and interlayer optical transitions, and the different nature of each layer. By analyzing the intrinsic radiative rates of the most stable subgap excitonic features, we find that while the presence of defects introduces low-lying optical transitions, resulting in excitons with larger oscillator strength, it also decreases the optical response associated to the pristine-like transition-metal dichalcogenide intralayer excitons. Our findings relate excitonic features with interface design for defect engineering in photovoltaic and transport applications.

cond-mat.mes-hall↗

Spin-defect characteristics of single sulfur vacancies in monolayer $\text{MoS}_2$

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer $\text{MoS}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

cond-mat.mes-hall↗

Charge quenching at defect states in transition metal dichalcogenide-graphene van der Waals heterobilayers

We study the dynamical properties of point-like defects, represented by monoatomic chalcogen vacancies, in WS$_2$-graphene and MoS$_2$-graphene heterobilayers. Employing a multidisciplinary approach based on the combination of ab initio, model Hamiltonian and density matrix techniques, we propose a minimal interacting model that allows for the calculation of electronic transition times associated to population and depopulation of the vacancy by an additional electron. We obtain the "coarse-grained" semiclassical dynamics by means of a master equation approach and discuss the potential role of virtual charge fluctuations in the internal dynamics of impurity quasi-degenerate states. The interplay between the symmetry of the lattice and the spin degree of freedom through the spin-orbit interaction and its impact on charge quenching is studied in detail.

cond-mat.mes-hall↗

Tunable magneto-optical properties in MoS$_2$ via defect-induced exciton transitions

The presence of chalcogen vacancies in monolayer transition metal dichalcogenides (TMDs) leads to excitons with mixed localized-delocalized character and to reduced valley selectivity. Recent experimental advances in defect design in TMDs allow for a close examination of such mixed exciton states as a function of their degree of circular polarization under external magnetic fields, revealing strongly varying defect-induced magnetic properties. A theoretical understanding of these observations and their physical origins demands a predictive, structure-sensitive theory. In this work, we study the effect of chalcogen vacancies on the exciton magnetic properties in monolayer MoS$_2$. Using many-body perturbation theory, we show how the complex excitonic picture associated with the presence of defects -- with reduced valley and spin selectivity due to hybridized electron-hole transitions -- leads to structurally-controllable exciton magnetic response. We find a variety of g-factors with changing magnitudes and sign depending on the exciton energy and character. Our findings suggest a pathway to tune the nature of the excitons -- and by that their magneto-optical properties -- through defect architecture.

cond-mat.mtrl-sci↗

Mixed excitonic nature in water-oxidized BiVO$_4$ surfaces with defects

BiVO$_4$ is a promising photocatalyst for efficient water oxidation, with surface reactivity determined by the structure of active catalytic sites. Surface oxidation in the presence of oxygen vacancies induces electron localization, suggesting an atomistic route to improve the charge transfer efficiency within the catalytic cycle. In this work, we study the effect of oxygen vacancies on the electronic and optical properties at BiVO$_4$ surfaces upon water oxidation. We use density functional theory and many-body perturbation theory to explore the change in the electronic and quasiparticle energy levels and to evaluate the electron-hole coupling as a function of the underlying structure. We show that while the presence of defects alters the atomic structure and largely modifies the wavefunction nature, leading to defect-localized states at the quasipatricle gap region, the optical excitations remain largely unchanged due to substantial hybridization of defect and non-defect electron-hole transitions. Our findings suggest that defect-induced surface oxidation supports improved electron transport, both through bound and tunable electronic states and via a mixed nature of the optical transitions, expected to reduce electron-hole defect trapping.

cond-mat.mtrl-sci↗

Quartic multifractality and finite-size corrections at the spin quantum Hall transition

The spin quantum Hall (or class C) transition represents one of the few localization-delocalization transitions for which some of the critical exponents are known exactly. Not known, however, is the multifractal spectrum, $τ_q$, which describes the system-size scaling of inverse participation ratios $P_q$, i.e., the $q$-moments of critical wavefunction amplitudes. We here report simulations based on the class C Chalker-Coddington network and demonstrate that $τ_q$ is (essentially) a quartic polynomial in $q$. Analytical results fix all prefactors except the quartic curvature that we obtain as $γ=(2.22\pm{0.15})\cdot10^{-3}$. In order to achieve the necessary accuracy in the presence of sizable corrections to scaling, we have analyzed the evolution with system size of the entire $P_q$-distribution function. As it turns out, in a sizable window of $q$-values this distribution function exhibits a (single-parameter) scaling collapse already in the pre-asymptotic regime, where finite-size corrections are not negligible. This observation motivates us to propose a novel approach for extracting $τ_q$ based on concepts borrowed from the Kolmogorov-Smirnov test of mathematical statistics. We believe that our work provides the conceptual means for high-precision investigations of multifractal spectra also near other localization-delocalization transitions of current interest, especially the integer (class A) quantum Hall effect.

cond-mat.dis-nn↗

Photoinduced electronic and spin properties of two-dimensional electron gases with Rashba spin-orbit coupling under perpendicular magnetic fields

We theoretically investigate photoinduced phenomena induced by time-periodic driving fields in two-dimensional electron gases under perpendicular magnetic fields with Rashba spin-orbit coupling. Using perturbation theory, we provide analytical results for the Floquet-Landau energy spectrum appearing due to THz radiation. By employing the resulting photo-modulated states, we compute the dynamical evolution of the spin polarization function for an initially prepared coherent state. We find that the interplay of the magnetic field, Rashba spin-orbit interaction and THz radiation can lead to inversion of the spin polarization. The dynamics also induces fractional revivals and non-trivial beating patterns in the autocorrelation function due to interference of the photo-modulated quantum states. We also calculate the transverse photo-assisted conductivity in the linear response regime using Kubo formalism and analyze the impact of the radiation field and Rashba spin-orbit interaction. In the static limit, we find that our results reduce to well-known expressions of the conductivity in non-relativistic and quasi-relativistic (topological insulator surfaces) two-dimensional electron gas thoroughly described in the literature. We discuss the possible experimental detection of our theoretical prediction and their relevance for spin-orbit physics at high magnetic fields.

cond-mat.mes-hall↗

Reorganization energy and polaronic effects of pentacene on NaCl films

Due to recent advances in scanning-probe technology, the electronic structure of individual molecules can now also be investigated if they are immobilized by adsorption on non-conductive substrates. As a consequence, different molecular charge-states are now experimentally accessible. Thus motivated, we investigate as an experimentally relevant example the electronic and structural properties of a NaCl(001) surface with and without pentacene adsorbed (neutral and charged) by employing density functional theory. We estimate the polaronic reorganization energy to be $E_\text{reorg} \simeq 0.8-1.0$ eV, consistent with experimental results obtained for molecules of similar size. To account for environmental effects on this estimate, different models for charge screening are compared. Finally, we calculate the density profile of one of the frontier orbitals for different occupation and confirm the experimentally observed localization of the charge density upon relaxation of the substrate from ab-initio calculations.

cond-mat.mtrl-sci↗