arXiv subjects

Gustavo Martini Dalpian

Publications and source records attributed to Gustavo Martini Dalpian.

4 recordsLinked to original sources

arXiv2026

Alloy engineering of Magnetic phases in two-dimensional Chromium Trihalides

Two-dimensional magnetic materials offer unique opportunities for exploring low-dimensional spin phenomena and next-generation spintronic devices. Chromium trihalides CrX3 (X = Cl, Br, I) belong to an important family of these materials, where alloying opens pathways for tailoring their electronic, magnetic, optical properties, and thermodynamic stability. In this work, we present a density functional theory study of CrX3 compounds and their ternary alloys. Our results show that for the pure compounds, the ground state is ferromagnetic (FM), with the antiferromagnetic-zigzag (AFM-Z) and paramagnetic (PM) phases being close in energy. For these pure systems, the band gap variation among different magnetic phases does not exceed 0.16 eV, and the average magnetic moments on Cr atoms increase from Cl to Br to I. For the alloys, the FM state remains the lowest-energy configuration, but the energy difference towards the AFM-Z phase decreases for compounds with lower iodine concentration. The calculated band gaps reveal a pronounced bowing along the compositional edge connecting CrCl3 and CrI3. The Curie temperatures show a smooth variation across compositions, consistent with the nearly linear behavior of the magnetic exchange parameters. Based on the calculated mixing enthalpy and configurational entropy, the approximate Gibbs free energy indicates that alloy formation becomes thermodynamically favorable at finite temperatures, which is important to overcome the intrinsic experimental instability of these compounds.

cond-mat.mtrl-sci↗

arXiv2025

Stability and Dynamics of Sn-based Halide Perovskites: Insights from MACE-MP-0 and Molecular Dynamics Simulations

Tin-based halide perovskites have emerged as promising lead-free alternatives for optoelectronic applications, yet their structural stability and phase behavior at finite temperatures remain challenging to predict. Here, we assess the predictive capabilities of the foundational machine learning model MACE-MP-0 - trained on a broad chemical space and applied without system-specific fine-tuning - for the temperature-dependent behavior of CsSnBr3 and Cs2SnBr6. Molecular Dynamics simulations in the NpT ensemble were performed from 100 K to 500 K, and thermodynamic and structural descriptors including enthalpy, specific heat, radial distribution functions, translational order, bond angle distributions, and vibrational spectra were analyzed. Our results show that CsSnBr3 undergoes a low-temperature orthorhombic-to-cubic phase transition, evidenced by both the evolution of lattice parameters and subtle anomalies in enthalpy and specific heat, although the experimentally observed intermediate tetragonal phase is not captured. In contrast, Cs2SnBr6 remains cubic and maintains a more rigid octahedral framework across the entire temperature range. Overall, MACE-MP-0 qualitatively reproduces key thermal and structural features of these materials, highlighting its usefulness as a first step for studying new materials. For cases where capturing more subtle phase behavior is required, system-specific fine-tuning with Density Functional Theory data should be considered.

cond-mat.mtrl-sci↗

arXiv2018

Bond disproportionation, charge self-regulation and ligand holes in s-p and in d electron ABX3 perovskites by density functional theory

Some ABX3 perovskites exhibit different local environments (DLE) for the same B atoms in the lattice, an effect referred to as disproportionation, distinguishing such compounds from perovskites that have single local environments (SLE). The basic phenomenology of disproportionation involves the absence of B-atom charge ordering, the creation of different B-X bond length for different local environments, the appearance of metal (in SLE) to insulator (in DLE) transition, and the formation of ligand holes. We point out that this phenomenology is common to a broad range of chemical bonding patterns in ABX3 compounds, either with s-p electron B-metal cations (BaBiO3, CsTlF3), or noble metal cation (CsAuCl3), as well as d-electron cations (SmNiO3, CaFeO3). We show that underlying much of this phenomenology is the self-regulating response, whereby in strongly bonded metal-ligand systems with high lying ligand orbitals, the system protects itself from creating highly charged cations by transferring ligand electrons to the metal, thus preserving a nearly constant metal charge in DLE, while creating B-ligand bond alternation and ligand-like conduction band (ligand hole). We are asking what are the minimal theory ingredients needed to explain the main features of this SLE-to-DLE phenomenology, such as its energetic driving force, bond length changes, possible modifications in charge density and density of state changes. Using as a guide the lowering of the total energy in DLE relative to SLE, we show that density functional calculations describe this phenomenology across the whole chemical bonding range without resort to special strong correlation effects, beyond what DFT naturally contains. In particular, lower total energy configurations (DLE) naturally develop bond alternation, gaping of the metallic SLE state, and absence of charge ordering with ligand hole formation.

cond-mat.mtrl-sci↗

arXiv2018

Spins in Semiconductor Nanocrystals

Semiconductor nanocrystals are being used as hosts to trap and manipulate single spins. Spins in nanocrystals can have different properties than their bulk counterparts, owing both to quantum confinement and surface effects. We will show that spins can be generated in nanocrystals by the insertion of impurities, either magnetic or not, or by magnetic polarons present at dangling bonds at their surfaces. This chapter reports theoretical contributions to this field, where the Density Functional Theory is used to simulate these functionalized nanocrystals.

cond-mat.mes-hall↗