SearcharxivSearch

arXiv subjects

Gabriel R. Schleder

Publications and source records attributed to Gabriel R. Schleder.

At least 19 recordsLinked to original sources

Cross-Geometry Transferability Assessment of Universal Machine Learning Interatomic Potentials: From Bulk Materials to Atomic Nanowires

Foundation machine-learning interatomic potentials (MLIPs) enable atomistic simulations at substantially lower computational cost than first-principles methods, but their reliability across structural geometries remains insufficiently understood. Here, we construct a density-functional-theory dataset of ZrO2 configurations spanning bulk, slab, particle, neck, and atomically thin wire environments motivated by an experimentally observed ZrO2 desintering process involving neck thinning and atomic wire formation. We first benchmark 26 pretrained MLIPs and observe pronounced geometry-dependent degradation in zero-shot predictions. Without any training, after only reference-energy alignment, the best zero-shot model (ORB-V3) reaches energy and force root-mean-square errors of 6 meV/atom and 197.3 meV/Å, respectively, with the largest force errors in neck and wire configurations. We then compare zero-shot inference, fine-tuning, and training from scratch strategies. Fine-tuning yields lower energy and force errors than training from scratch, while both require comparable wall-clock time. Geometry-specific fine-tuning improves in-domain accuracy but frequently produces negative transfer to other structural classes, whereas mixed-geometry fine-tuning reduces cross-geometry errors. Evaluations of elastic and vibrational properties, surface energies, and neck dynamics further show that rankings based on average energy and force errors do not universally predict property-level behavior. These results demonstrate that geometry-diverse target data and independent physical validations are necessary when adapting foundation MLIPs to low-coordination (ionic) nanostructures.

cond-mat.mtrl-sci

Fuzzy Neural Network Performance and Interpretability of Quantum Wavefunction Probability Predictions

Predicting quantum wavefunction probability distributions is crucial for computational chemistry and materials science, yet machine learning (ML) models often face a trade-off between accuracy and interpretability. This study compares Artificial Neural Networks (ANNs) and Adaptive Neuro-Fuzzy Inference Systems (ANFIS) in modeling quantum probability distributions for the H$_{2}^+$ ion, leveraging data generated via Physics-Informed Neural Networks (PINNs). While ANN achieved superior accuracy (R$^2$ = 0.99 vs ANFIS's 0.95 with Gaussian membership functions), it required over 50x more parameters (2,305 vs 39-45). ANFIS, however, provided unique interpretability: its Gaussian membership functions encoded spatial electron localization near proton positions ($μ= 1.2 A$), mirroring Born probability densities, while fuzzy rules reflected quantum superposition principles. Rules prioritizing the internuclear direction revealed the system's 1D symmetry, aligning with Linear Combination of Atomic Orbitals theory--a novel data-driven perspective on orbital hybridization. Membership function variances ($σ$) further quantified electron delocalization trends, and peak prediction errors highlighted unresolved quantum cusps. The choice of functions critically impacted performance: Gaussian/Generalized Bell outperformed Sigmoid, with errors improving as training data increased, showing scalability. This study underscores the context-dependent value of ML: ANN for precision and ANFIS for interpretable, parameter-efficient approximations that link inputs to physical behavior. These findings advocate hybrid approaches in quantum simulations, balancing accuracy with explainability to accelerate discovery. Future work should extend ANFIS to multi-electron systems and integrate domain-specific constraints (e.g., kinetic energy terms), bridging data-driven models and fundamental physics.

physics.chem-ph

Performance Assessment of Universal Machine Learning Interatomic Potentials: Challenges and Directions for Materials' Surfaces

Machine learning interatomic potentials (MLIPs) are one of the main techniques in the materials science toolbox, able to bridge ab initio accuracy with the computational efficiency of classical force fields. This allows simulations ranging from atoms, molecules, and biosystems, to solid and bulk materials, surfaces, nanomaterials, and their interfaces and complex interactions. A recent class of advanced MLIPs, which use equivariant representations and deep graph neural networks, is known as universal models. These models are proposed as foundational models suitable for any system, covering most elements from the periodic table. Current universal MLIPs (UIPs) have been trained with the largest consistent dataset available nowadays. However, these are composed mostly of bulk materials' DFT calculations. In this article, we assess the universality of all openly available UIPs, namely MACE, CHGNet, and M3GNet, in a representative task of generalization: calculation of surface energies. We find that the out-of-the-box foundational models have significant shortcomings in this task, with errors correlated to the total energy of surface simulations, having an out-of-domain distance from the training dataset. Our results show that while UIPs are an efficient starting point for fine-tuning specialized models, we envision the potential of increasing the coverage of the materials space towards universal training datasets for MLIPs.

cond-mat.mtrl-sci

Magnetic control of Weyl nodes and wave packets in three-dimensional warped semimetals

We investigate the topological phase transitions driven by band warping and a transverse magnetic field, for three-dimensional Weyl semimetals. First, we use the Chern number as a mathematical tool to derive the topological phase diagram. Next, we associate each of the topological sectors to a given angular momentum state of a rotating wave packet. Then we show how the position of the Weyl nodes can be manipulated by a transverse external magnetic field that ultimately quenches the wave packet rotation, first partially and then completely, thus resulting in a sequence of field-induced topological phase transitions. Finally, we calculate the current-induced magnetization and the anomalous Hall conductivity of a prototypical warped Weyl material. Both observables reflect the topological transitions associated with the wave packet rotation and can help to identify the elusive 3D quantum anomalous Hall effect in three-dimensional, warped Weyl materials.

cond-mat.mes-hall

Phyllosilicates as earth-abundant layered materials for electronics and optoelectronics: Prospects and challenges in their ultrathin limit

Phyllosilicate minerals are an emerging class of naturally occurring layered insulators with large bandgap energy that have gained attention from the scientific community. This class of lamellar materials has been recently explored at the ultrathin two-dimensional level due to their specific mechanical, electrical, magnetic, and optoelectronic properties, which are crucial for engineering novel devices (including heterostructures). Due to these properties, phyllosilicates minerals can be considered promising low-cost nanomaterials for future applications. In this Perspective article, we will present relevant features of these materials for their use in potential 2D-based electronic and optoelectronic applications, also discussing some of the major challenges in working with them.

physics.app-ph

One-Dimensional Moiré Physics and Chemistry in Heterostrained Bilayer Graphene

Twisted bilayer graphene (tBLG) has emerged as a promising platform to explore exotic electronic phases. However, the formation of moiré patterns in tBLG has thus far been confined to the introduction of twist angles between the layers. Here, we propose heterostrained bilayer graphene (hBLG), as an alternative avenue to access twist-angle-free moiré physics via lattice mismatch. Using atomistic and first-principles calculations, we demonstrate that uniaxial heterostrain can promote isolated flat electronic bands around the Fermi level. Furthermore, the heterostrain-induced out-of-plane lattice relaxation may lead to a spatially modulated reactivity of the surface layer, paving the way for the moiré-driven chemistry and magnetism. We anticipate that our findings can be readily generalized to other layered materials.

cond-mat.mtrl-sci

Lattice reconstruction in MoSe$_2$-WSe$_2$ heterobilayers synthesized by chemical vapor deposition

Vertical van der Waals heterostructures of semiconducting transition metal dichalcogenides realize moiré systems with rich correlated electron phases and moiré exciton phenomena. For material combinations with small lattice mismatch and twist angles as in MoSe$_2$-WSe$_2$, however, lattice reconstruction eliminates the canonical moiré pattern and instead gives rise to arrays of periodically reconstructed nanoscale domains and mesoscopically extended areas of one atomic registry. Here, we elucidate the role of atomic reconstruction in MoSe$_2$-WSe$_2$ heterostructures synthesized by chemical vapor deposition. With complementary imaging down to the atomic scale, simulations, and optical spectroscopy methods we identify the coexistence of moiré-type cores and extended moiré-free regions in heterostacks with parallel and antiparallel alignment. Our work highlights the potential of chemical vapor deposition for applications requiring laterally extended heterosystems of one atomic registry or exciton-confining heterostack arrays.

cond-mat.mes-hall

Domain-dependent surface adhesion in twisted few-layer graphene: Platform for moiré-assisted chemistry

Twisted van der Waals multilayers are widely regarded as a rich platform to access novel electronic phases, thanks to the multiple degrees of freedom such as layer thickness and twist angle that allow control of their electronic and chemical properties. Here, we propose that the stacking domains that form naturally due to the relative twist between successive layers act as an additional "knob" for controlling the behavior of these systems, and report the emergence and engineering of stacking domain-dependent surface chemistry in twisted few-layer graphene. Using mid-infrared near-field optical microscopy and atomic force microscopy, we observe a selective adhesion of metallic nanoparticles and liquid water at the domains with rhombohedral stacking configurations of minimally twisted double bi- and tri-layer graphene. Furthermore, we demonstrate that the manipulation of nanoparticles located at certain stacking domains can locally reconfigure the moiré superlattice in their vicinity at the μm-scale. In addition, we report first-principles simulations of the energetics of adhesion of metal atoms and water molecules on the stacking domains in an attempt to elucidate the origin of the observed selective adhesion. Our findings establish a new approach to controlling moiré-assisted chemistry and nanoengineering.

cond-mat.mtrl-sci

Pressure--enhanced fractional Chern insulators in moiré transition metal dichalcogenides along a magic line

We show that pressure applied to twisted WSe$_2$ can enhance the many-body gap and region of stability of a fractional Chern insulator at filling $ν= 1/3$. Our results are based on exact diagonalization of a continuum model, whose pressure-dependence is obtained through {\it ab initio} methods. We interpret our results in terms of a {\it magic line} in the pressure-{\it vs}-twist angle phase diagram: along the magic line, the bandwidth of the topmost moiré valence band is minimized while simultaneously its quantum geometry nearly resembles that of an ideal Chern band. We expect our results to generalize to other twisted transition metal dichalcogenide homobilayers.

cond-mat.str-el

Connecting Higher-Order Topology with the Orbital Hall Effect in Monolayers of Transition Metal Dichalcogenides

Monolayers of transition metal dichalcogenides (TMDs) in the 2H structural phase have been recently classified as higher-order topological insulators (HOTI), protected by $C_3$ rotation symmetry. In addition, theoretical calculations show an orbital Hall plateau in the insulating gap of TMDs, characterized by an orbital Chern number. We explore the correlation between these two phenomena in TMD monolayers in two structural phases: the noncentrosymmetric 2H and the centrosymmetric 1T. Using density functional theory, we confirm the characteristics of 2H-TMDs and reveal that 1T-TMDs are identified by a $\mathbb{Z}_4$ topological invariant. As a result, when cut along appropriate directions, they host conducting edge-states, which cross their bulk energy-band gaps and can transport orbital angular momentum. Our linear response calculations thus indicate that the HOTI phase is accompanied by an orbital Hall effect. Using general symmetry arguments, we establish a connection between the two phenomena with potential implications for spin-orbitronics.

cond-mat.mes-hall

Twistronics of Janus transition metal dichalcogenide bilayers

Twisted multilayers of two-dimensional (2D) materials are an increasingly important platform for investigating quantum phases of matter, and in particular, strongly correlated electrons. The moiré pattern introduced by the relative twist between layers creates effective potentials of long-wavelength, leading to electron localization. However, in contrast to the abundance of 2D materials, few twisted heterostructures have been studied until now. Here we develop a first-principle continuum theory to study the electronic bands introduced by moire patterns of twisted Janus transition metal dichalcogenides (TMD) homo- and hetero-bilayers. The model includes lattice relaxation, stacking-dependent effective mass, and Rashba spin-orbit coupling. We then perform a high-throughput generation and characterization of DFT-extracted continuum models for more than a hundred possible combinations of materials and stackings. Our model predicts that the moiré physics and emergent symmetries depend on chemical composition, vertical layer orientation, and twist angle, so that the minibands wavefunctions can form triangular, honeycomb, and Kagome networks. Rashba spin-orbit effects, peculiar of these systems, can dominate the moiré bandwidth at small angles. Our work enables the detailed investigation of Janus twisted heterostructures, allowing the discovery and control of novel electronic phenomena.

cond-mat.mtrl-sci

First principles physics-informed neural network for quantum wavefunctions and eigenvalue surfaces

Physics-informed neural networks have been widely applied to learn general parametric solutions of differential equations. Here, we propose a neural network to discover parametric eigenvalue and eigenfunction surfaces of quantum systems. We apply our method to solve the hydrogen molecular ion. This is an ab-initio deep learning method that solves the Schrodinger equation with the Coulomb potential yielding realistic wavefunctions that include a cusp at the ion positions. The neural solutions are continuous and differentiable functions of the interatomic distance and their derivatives are analytically calculated by applying automatic differentiation. Such a parametric and analytical form of the solutions is useful for further calculations such as the determination of force fields.

cs.LG

Amorphous Bi$_2$Se$_3$ structural, electronic, and topological nature by first-principles

Crystalline $\rm Bi_2Se_3$ is one of the most explored three-dimensional topological insulator, with a $0.3\;\rm eV$ energy gap making it promising for applications. Its amorphous counterpart could bring to light new possibilities for large scale synthesis and applications. Using ab initio molecular dynamics simulations, we have studied realistic amorphous $\rm Bi_2Se_3$ phases generated by different processes of melting, quenching, and annealing. Extensive structural and electronic characterizations show that the melting process induces an energy gap decrease ruled by growth of the defective local environments. This behavior dictates a weak stability of the topological phase to disorder, characterized by the spin Bott index. Interestingly, we identify the occurrence of topologically trivial surface states in amorphous $\rm Bi_2Se_3$ that show a strong resemblance with standard helical topological states. Our results and methods advance the search of topological phases in three-dimensional amorphous solids.

cond-mat.mtrl-sci

Machine learning for materials discovery: two-dimensional topological insulators

One of the main goals and challenges of materials discovery is to find the best candidates for each interest property or application. Machine learning rises in this context to efficiently optimize this search, exploring the immense materials space, consisting of simultaneously the atomic, compositional, and structural spaces. Topological insulators, presenting symmetry-protected metallic edge states, are a promising class of materials for different applications. However, further, development is limited by the scarcity of viable candidates. Here we present and discuss machine learning-accelerated strategies for searching the materials space for two-dimensional topological materials. We show the importance of detailed investigations of each machine learning component, leading to different results. Using recently created databases containing thousands of ab initio calculations of 2D materials, we train machine learning models capable of determining the electronic topology of materials, with an accuracy of over 90%. We can then generate and screen thousands of novel materials, efficiently predicting their topological character without the need for a priori structural knowledge. We discover 56 non-trivial materials, of which 17 novel insulating candidates for further investigation, for which we corroborate their topological properties with density functional theory calculations. This strategy is 10$\times$ more efficient than the trial-and-error approach while few orders of magnitude faster and is a proof of concept for guiding improved materials discovery search strategies.

cond-mat.mtrl-sci

Conformational analysis of tannic acid: environment effects in electronic and reactivity properties

Polyphenols are natural molecules of crucial importance in many applications, of which tannic acid (TA) is one of the most abundant and established. Most high-value applications require precise control of TA interactions with the system of interest. However, the molecular structure of TA is still not comprehended at the atomic level, of which all electronic and reactivity properties depend. Here, we combine an enhanced sampling global optimization method with density functional theory (DFT)-based calculations to explore the conformational space of TA assisted by unsupervised machine learning visualization, and then investigate its lowest energy conformers. We study the external environment's effect on the TA structure and properties. We find that vacuum favors compact structures by stabilizing peripheral atoms' weak interactions, while in water, the molecule adopts more open conformations. The frontier molecular orbitals of the conformers with lowest harmonic vibrational free energy have a HOMO-LUMO energy gap of 2.21 (3.27) eV, increasing to 2.82 (3.88) eV in water, at the DFT generalized gradient approximation (and hybrid) level of theory. Structural differences also change the distribution of potential reactive sites. We establish the fundamental importance of accurate structural consideration in determining TA and related polyphenols interactions in relevant technological applications.

physics.chem-ph

Unveiling the dopant segregation effect at hematite interfaces

Understanding the effects of atomic structure modification in hematite photoanodes is essential for the rational design of high-efficiency functionalizations. Recently it was found that interface modification with Sn/Sb segregates considerably increases hematite photocatalytic efficiency. However, the understanding of the different electronic effects of these modifications at the atomic level is still lacking. This letter describes the segregation effects of two different dopants-Sn and Sb-on both the solid-solid (grain-boundaries) and solid-liquid interfaces (surfaces) of hematite. Within an ab-initio approach, we quantitatively extract the potential barrier reduction on polycrystalline interfaces due to the dopant, which causes an increase in the inter-grain electron transport. Concomitantly, the dopants' segregation on hematite surfaces results in a decrease of the oxygen vacancy formation energy. Such vacancies lead to the experimentally observed rise of the flat-band potential. The comprehension of the electronic effects of dopants on both types of interfaces explains the experimental peak efficiency of interface-modified hematite with dopant segregates, also enabling the control and design of interfaces for different higher-efficiency applications.

cond-mat.mtrl-sci

Computational Design of Moiré Assemblies Aided by Artificial Intelligence

Two-dimensional (2D) layered materials, demonstrating significantly different properties from their bulk counterparts, offer a materials platform with potential applications from energy to information processing devices. Although some single- and few-layer forms of materials such as graphene and transition metal dichalcogenides have been realized and thoroughly studied, the space of arbitrarily layered assemblies is still mostly unexplored. The main goal of this work is to demonstrate precise control of layered materials' electronic properties through careful choice of the constituent layers, their stacking, and relative orientation. Physics-based and AI-driven approaches for the automated planning, execution, and analysis of electronic structure calculations are applied to layered assemblies based on prototype one-dimensional (1D) materials and realistic 2D materials. We find it is possible to routinely generate moiré band structures in 1D with desired electronic characteristics such as a band gap of any value within a large range, even with few layers and materials (here, four and six, respectively). We argue that this tunability extends to 2D materials by showing the essential physical ingredients are already evident in calculations of two-layer MoS$_2$ and multi-layer graphene moiré assemblies.

cond-mat.mes-hall

Disorder effects of vacancies on the electronic transport properties of realistic topological insulators nanoribbons: the case of bismuthene

The robustness of topological materials against disorder and defects is presumed but has not been demonstrated explicitly in realistic systems. In this work, we use state-of-the-art density functional theory and recursive nonequilibrium Green's functions methods to study the effect of disorder in the electronic transport of long nanoribbons, up to 157 nm, as a function of vacancy concentration. In narrow nanoribbons, even for small vacancy concentrations, defect-like localized states give rise to hybridization between the edge states erasing topological protection and enabling backscattering events. We show that the topological protection is more robust for wide nanoribbons, but surprisingly it breaks down at moderate structural disorder. Our study helps to establish some bounds on defective bismuthene nanoribbons as promising candidates for spintronic applications.

cond-mat.mes-hall