arXiv subjects

Guilherme S. L. Fabris

Publications and source records attributed to Guilherme S. L. Fabris.

12 recordsLinked to original sources

arXiv2026

Interfacial Charge Transfer and Morphology Govern Magnetism in Ultrathin VOx/MoSe2 Heterostructures

Engineering magnetism in two-dimensional semiconductors through interfacial interactions offers an attractive alternative to substitutional doping and provides opportunities for integrating magnetic and optoelectronic functionality within the same heterostructure. Here, we investigate ultrathin VOx films deposited on monolayer MoSe2 and demonstrate a pronounced enhancement of the magnetic response upon formation of the VOx/MoSe2 interface. Combined structural, spectroscopic, magnetic, and first-principles analyses support a consistent picture in which finite VOx clusters possess intrinsic magnetic moments that are further enhanced by electron transfer from MoSe2 to the oxide. The predicted charge transfer is also consistent with the increased trion contribution observed in the photoluminescence response of the heterostructure. Beyond this interfacial enhancement, the magnetic behavior is strongly governed by the morphology of the ultrathin oxide. A crossover from discontinuous clusters to more continuous films produces qualitatively different temperature dependences: the continuous-film regime exhibits conventional thermal demagnetization and coercive softening, whereas the clustered regime displays an unusual increase in magnetization and nonmonotonic coercivity with increasing temperature. These contrasting responses are captured by a phenomenological model in which morphology determines the collective magnetic dynamics through a distribution of effective reversal barriers and their thermally activated accessibility. Together, the results establish a unified picture in which interfacial charge transfer enhances the local magnetic moments of VOx, while nanoscale morphology governs their collective magnetic dynamics, providing complementary routes for controlling magnetism in oxide/transition-metal dichalcogenide heterostructures.

cond-mat.mes-hall↗

arXiv2026

Metallic Organometallic and Semiconducting Covalent Phases of Free-Standing $γ$-Graphdiyne Molecular Wires

One-dimensional carbon allotropes combining sp and sp2 hybridizations provide a versatile platform for atomically precise quantum wires with tunable electronic, vibrational, and mechanical responses. Recent on-surface synthesis has realized the $γ$-graphdiyne molecular wire on Au(100) in two interconvertible phases sharing an identical aromatic backbone but distinct linkage chemistry: an organometallic intermediate with C-Au-C bridges and a fully covalent product with diacetylenic linkages. While experimental techniques characterize the on-surface periodicity and C$\equiv$C Raman signatures, the intrinsic properties of the free-standing wires remain inaccessible. Here, we address this gap using hybrid-functional first-principles calculations. The covalent phase is a semiconductor with a direct band gap of 2.02 eV, a polyynic bond-length alternation of 0.117 Å, and a chain periodicity reproducing experiment within -0.5%. Conversely, the organometallic phase exhibits partial cumulenization and 1D metallic behavior, with spin channels crossing the Fermi level. Both isolated polymers demonstrate dynamic stability with Young's moduli of 995 nN and 861 nN, respectively, where the C-Au-C bridge acts as a soft link absorbing 9.2% of axial deformation at +6% macroscopic strain. Species-resolved vibrational analysis identifies an effective-conjugation-coordinate band at 1408 cm$^{-1}$ for the covalent phase and Au-projected modes below 400 cm$^{-1}$ for the intermediate, offering diagnostic fingerprints for phase discrimination during thermal or chemical conversion.

cond-mat.mtrl-sci↗

arXiv2026

Ion-Engineered Insulator-to-Semiconductor Transition in Natural 2D Biotite

Naturally occurring layered silicates offer an abundant yet unexplored class of 2D materials, but their insulating nature limits their functional utility. Here, we demonstrate a chemical strategy that transforms liquid-phase-exfoliated biotite nanosheets into a tunable 2D semiconductor through controlled NaOH treatment. The resulting insulator-to-semiconductor transition originates from Na incorporation, defect generation, and local structural reconstruction while largely preserving the layered framework. Structural and chemical analyses reveal lattice distortion, interlayer reorganization, hydroxylation, and partial Na+-K+ exchange, establishing the origin of the electronic restructuring. This transformation broadens the optical response, shifting the approximately 221 nm absorption toward approximately 280 and 975 nm, reducing the optical bandgap from approximately 5.2 to 3.2-3.5 eV, and introducing low-energy transitions at approximately 1.12-1.17 eV. Electrical measurements reveal nonlinear transport with currents reaching close to 10 microA, demonstrating activated carrier conduction. Ultrafast transient absorption reveals pronounced excited-state absorption, with carrier cooling (0.16-0.38 ps) followed by fast (35-60 ps) and long-lived (336-491 ps) relaxation associated with trap-mediated recombination. Fluence-dependent dynamics reveal a hot-phonon bottleneck at elevated carrier densities. Together with density functional theory calculations, these results establish chemical defect and ion engineering as a powerful route for converting naturally abundant layered minerals into electronically tunable 2D materials for emerging optoelectronic and ultrafast photonic technologies.

cond-mat.mtrl-sci↗

arXiv2026

Plasmonic Mediated Atomically Engineered 2D Aluminium Quasicrystals for Dopamine Biosensing

Dopamine levels are linked to neurological illnesses like Parkinson's and Alzheimer's. Thus, reliable and sensitive detection of dopamine is crucial for early diagnosis and surveillance of neurodegenerative diseases. Non-noble-metal-based nanomaterials are ideal for light-mediated sensing of organic molecules. Among these, 2D quasicrystal structures consisting of five elements, namely Al70Co10Fe5Ni10Cu5, provide active sites due to their high surface-to-volume ratio, making them excellent for organic chemical sensing. Here, we propose a simple, label-free, spatial self-phase-modulation (SSPM)-based sensing method in liquid form. SSPM-based time evolution of the diffraction pattern for varied mixing levels of a 1100 ppb dopamine solution shows a shift in the active 2D Al QC solution. The 1100 ppb solution shows a distinct value, indicating a change in the nonlinear refractive index. Time-evolution analysis is used to calculate sensitivities to changes in the nonlinear refractive index and time constant. The SPR-activated 2D Al QC nanostructure is used to demonstrate dopamine sensing and to perform qualitative and quantitative evaluations. The SSPM-based sensing has been further compared with other optical-based sensing methods such as Raman spectroscopy, UV-Vis spectroscopy, and FTIR spectroscopy. The experimental observations are also explained using DFT-based simulations. The current SSPM method can be used for rapid, large-scale medical diagnostics.

cond-mat.mtrl-sci↗

arXiv2026

Stacking-Tunable Electronic Properties in Recently Synthesized Hydrogen-Substituted Graphdiyne

Recent progress in porous carbon materials has highlighted the importance of structural design in controlling emergent physicochemical properties. In this context, hydrogen-substituted graphdiyne (HsGDY), a three-dimensional framework derived from graphdiyne (GDY), has recently emerged as a promising architecture whose stacking-dependent behavior remains largely unexplored. Here, we present a comprehensive first-principles investigation of the structural, electronic, and optical properties of HsGDY across distinct stacking sequences. Our results identify the AA and ABC configurations as the most energetically favorable, with AA corresponding to the global minimum, consistent with recent experimental observations. Electronic-structure analysis reveals that HsGDY is an indirect semiconductor with an electronic band gap of 0.89 eV (optB88-vdW), primarily governed by interlayer coupling and van der Waals interactions. The optical response exhibits pronounced absorption features spanning the visible to ultraviolet regions, highlighting strong potential for optoelectronic applications. \textit{Ab initio} molecular dynamics (AIMD) simulations at 700 K confirm the thermal robustness of the framework, with negligible structural distortions. Collectively, these findings elucidate the stacking-dependent stability and semiconducting character of HsGDY, providing a solid theoretical foundation for its integration into next-generation nanoelectronic and energy-harvesting technologies.

cond-mat.mtrl-sci↗

arXiv2025

Ambient-Induced Selenium Segregation and Nanoparticle Formation in 2H-HfSe2: An Experimental and Theoretical Study

We investigate the air-induced degradation of few-layer hafnium diselenide (HfSe$_2$) through combined experimental and theoretical approaches. AFM and SEM reveal the formation of selenium-rich spherical features upon ambient exposure, while EDS confirms Se segregation. \textit{Ab initio} molecular dynamics simulations show that Se atoms migrate to flake edges and that O/O$_2$ exposure leads to selective Hf oxidation, breaking Se--Hf bonds and expelling Se atoms. No stable Se--O bonds are observed, indicating structural reorganization rather than oxidation. These findings emphasize the material's instability in air and the importance of encapsulation for preserving HfSe$_2$ in practical applications. Scanning tunneling spectroscopy confirms the semiconducting character of the nanoparticles, with an electronic bandgap compatible with that of elemental Se. These results highlight the critical role of lattice defects and oxidation dynamics in the degradation process and underscore the need for encapsulation strategies to preserve the integrity of HfSe$_2$-based devices.

cond-mat.mtrl-sci↗

arXiv2025

From Glaphene to Glaphynes: A Hybridization of 2D Silica Glass and Graphynes

Hybrid two-dimensional (2D) materials have attracted increasing interest as platforms for tailoring electronic properties through interfacial design. Very recently, a novel hybrid 2D material termed glaphene, which combines monolayers of 2D silica glass and graphene, was experimentally realized. Inspired by glaphenes, we proposed a new class of similar structures named glaphynes, which are formed by stacking SiO$_2$ monolayers onto $α$-, $β$-, and $γ$-graphynes. Graphynes are 2D carbon allotropes with the presence of acetylenic groups (triple bonds). The glaphynes' structural and electronic properties were investigated using the density functional tight-binding (DFTB) method, as implemented in the DFTB+ package. Our analysis confirms their energetic and structural stability. We have observed that in the case of glaphynes, the electronic proximity effect can indeed open the electronic band gap, but not for all cases, even with the formation of Si-O-C bonds between silica and graphynes.

cond-mat.mtrl-sci↗

arXiv2025

A Concise Review of Recently Synthesized 2D Carbon Allotropes: Amorphous Carbon, Graphynes, Biphenylene and Fullerene Networks

Two-dimensional (2D) carbon allotropes have received considerable attention due to their unique properties and potential applications in several fields, including electronics, catalysis, energy storage, and sensing. Following the experimental realization of graphene, numerous other 2D carbon structures have been proposed and, in some cases, successfully synthesized. This work presents a concise review of the recently experimentally realized 2D carbon allotropes, including graphynes, biphenylene-based networks, fullerene networks, and monolayer amorphous carbon. For each class, we discuss structural characteristics, theoretical predictions, and synthesis methods, with emphasis on the interplay between theory and experiment. We also highlight instances where experimental studies overlooked relevant theoretical contributions. Finally, we identify theoretically predicted structures that remain unexplored experimentally, suggesting opportunities for synthesis-driven investigations.

cond-mat.mtrl-sci↗

arXiv2025

Magnetism Induced by Azanide and Ammonia Adsorption in Defective Molybdenum Disulfide and Diselenide: A First-Principles Study

Two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted considerable attention due to their tunable structural, electronic, and spin-related properties, particularly in the presence of point defects and molecular adsorbates. Motivated by these aspects, we have investigated using first-principles methods the magnetic properties induced by azanide (NH$_2$) and ammonia (NH$_3$) adsorption on defective monolayers of Molybdenum Disulfide (MoS$_2$) and Diselenide(MoSe$_2$). Spin-polarized density functional theory (DFT) was employed to investigate the impact of mono- and di-vacancies on the local spin environment and the role of molecular adsorption in modifying magnetic behavior. The results show that pristine chalcogen vacancies do not generate magnetism, whereas the adsorption of NH$_2$ and NH$_3$ creates localized magnetic moments in Mo-based dichalcogenides. A notable case occurs for MoSe$_2$, where NH$_3$ dissociation into NH$_2$ and H fragments on the same side of the surface produces a net magnetic moment of 2.0 $μ_B$. Tests performed on W-based dichalcogenides under equivalent conditions showed no magnetic response, and are reported here only for comparison. These findings demonstrate that molecular adsorption combined with defect engineering can be a practical approach to tune magnetism in 2D materials, with potential relevance for spintronic and sensing applications.

cond-mat.mtrl-sci↗

arXiv2025

Visible-Light Photocatalytic Degradation of Cresols using Sustainable 3D-Printed Bi4O5I2-Hematite Scaffold

In photocatalysis, the reusability limit of catalysts can contribute to secondary pollution, posing ecological risks. Addressing this, the present study explores the integration of additive manufacturing with photocatalysis by decorating Bi$_4$O$_5$I$_2$ onto a 3D-printed hematite scaffold (Bi$_4$O$_5$I$_2$@3DH) for the degradation of cresols. The 3D-printed hematite grid, fabricated via direct ink writing, exhibited excellent rheological behavior ($τγ= 24$ Pa), allowing precise shape retention. The sintered Bi$_4$O$_5$I$_2$ was subsequently immobilized via a facile dip-coating method. Under optimized conditions, the composite achieved 99.78\% degradation of 20 mg/L p-cresol within 240 min of irradiation. Notably, hematite served as a porous substrate and contributed to photocatalytic activity. Density functional theory simulations with Hubbard correction (DFT+U) indicated an interfacial charge transfer of approximately -0.9 electrons from hematite to Bi$_4$O$_5$I$_2$, confirming a S-scheme heterojunction between hematite and Bi$_4$O$_5$I$_2$ semiconductors, validating experimental observations. The composite demonstrated strong performance across varied water matrices and in the presence of other cresol isomers. It also retained 84.28\% degradation efficiency after 10 cycles, with negligible catalyst leaching. Furthermore, in vitro and in silico ecotoxicity analyses revealed reduced toxicity of the degradation products. The current work presents a novel and scalable strategy, advancing the use of earth-abundant hematite minerals in sustainable environmental remediation.

physics.chem-ph↗

arXiv2025

Defect Engineered Layer Dependent Nonlinear Optical Response in Two Dimensional Muscovite for Efficient Optical Limiting

Light-matter interactions in two-dimensional (2D) materials have gained significant interest due to their distinctive optical and electronic properties. Recently, silicates have emerged as a promising new class of 2D materials, but their nonlinear optical properties remain largely unexplored. In this study, we demonstrate layer-dependent nonlinear absorption and optical limiting capabilities of 2D muscovite using femtosecond laser excitation at 450 nm. The two-photon absorption (TPA) coefficient is highly sensitive to both the number of layers and excitation intensity, increasing markedly from (3.91+/-0.06)x10^3 cm GW^-1 in multilayer structures to (6.94+/-0.17)x10^5 cm GW^-1 in the monolayer limit at a peak intensity of 68 GW cm^-2, highlighting a strong layer-dependent enhancement in nonlinear absorption. Additionally, monolayer muscovite exhibits an optical limiting threshold of 1.46 mJ cm^-2, outperforming graphene and other 2D dichalcogenides. This enhanced TPA arises from quantum confinement and intrinsic lattice defects that facilitate nonlinear optical transitions. Density functional theory reveals that liquid-phase exfoliation disrupts potassium interlayers and induces oxygen vacancies, generating mid-gap electronic states that significantly enhance TPA. These insights open new avenues for designing low-fluence, high-efficiency optical limiters using 2D silicates.

physics.optics↗

arXiv2023

Reversible Actuation of $α$-Borophene Nanoscrolls

In this work, we proposed and investigated the structural and electronic properties of boron-based nanoscrolls (armchair and zigzag) using the DFTB+ method. We also investigated the electroactuation process (injecting and removing charges). A giant electroactuation was observed, but the results show relevant differences between the borophene and carbon nanoscrolls. The molecular dynamics simulations showed that the scrolls are thermally and structurally stable for a large range of temperatures (up to 600K) and the electroactuation process can be easily tuned and can be entirely reversible for some configurations.

cond-mat.mes-hall↗