Publications

Developing new glass electrolytes with the necessary room-temperature ionic conductivity (similar to 10(-3) Scm(-1)) for solid-state batteries, especially sodium-ion (Na+) batteries, has been impeded by the lack of a clear relationship between composition, structure, and conductivity in glass materials. This study highlights the impact of the mixed glass formers on the structure, Na+-ion dynamics, and glass conductivity. To this end, we substituted SiO2 for P2O5 in sodium alumino-phosphate glass while maintaining a constant molar concentration of Al2O3 and Na2O. A detailed analysis combining molecular simulations and experiments revealed that the glass containing 15 mol% SiO2 exhibited the highest DC ionic conductivity of similar to 9 x 10(-6) Scm(-1) at 473 K, followed by a decrease for 20 mol% SiO2. To understand this behavior, microscopic characteristic length such as critical hopping distance and Na+ diffusion coefficients were correlated with structural changes using AC conductivity analysis. Altogether, we elucidate the composition-dependent Na+ ion dynamics in the alumino-phosphate glass system, with factors like mobile charge carrier concentration, ion mobility, and coulombic forces influenced by the structure of different glass compositions.

Chalcogenide glasses (ChGs) are a class of amorphous materials presenting remarkable mechanical, optical, and electrical properties, making them promising candidates for advanced photonic and optoelectronic applications. With the increasing integration of artificial intelligence in modern materials design, we are able to systematically select, prepare, and optimize appropriate compositions for desired applications in a manner that was unachievable before. This study employs various machine learning models to reliably predict the refractive index at 20 degrees C using a small dataset of 541 samples extracted from the SciGlass database. The input for the algorithms consists of a selected set of physico-chemical features computed for the chemical composition of each entry. Additionally, these algorithms served as inner models for an ensemble logistic regression estimator that achieved a superior R2 value of 0.8985. SHAP feature analysis of the second-best model, CatBoostRegressor (R2 = 0.8920), revealed the importance of elemental density, atomic weight, ground state atomic gap, and fraction of p valence electrons in tuning the value of the refractive index of a chalcogenide compound.

The catalytic hydrodeoxygenation (HDO) of lignocellulose-derived pyrolysis oil is a critical process for producing high-quality biofuels. This study investigates the effect of the Mg/Al molar ratio on the catalytic performance of CuMg(Al)O mixed oxide catalysts in the HDO reaction of benzyl alcohol as a model oxygenated compound. They were synthesized by coprecipitation with a fixed Cu content of 15 at. %, with respect to cations, and different Mg/Al molar ratios (0/1, 1/1, 3/1, 5/1, and 1/0). The catalysts were characterized using X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), UV-vis spectroscopy, nitrogen adsorption-desorption isotherms, temperature-programmed reduction with hydrogen (H2-TPR), and temperature-programmed desorption (TPD) of CO2 and NH3. It has been shown that the Mg/Al molar ratio strongly influences the physicochemical characteristics of the CuMg(Al)O mixed oxides and, hence, their catalytic performance. Catalytic tests were conducted in a stainless-steel autoclave reactor and the obtained results indicated that the systems with Mg/Al molar ratios of 3/1 and 5/1, issued from layered double hydroxide precursors, exhibited the highest activity, with yields to toluene higher than 85%. This superior performance is attributed to the well-dispersed copper species on the catalyst surface combined with appropriate acid-base properties. As the CuMg(Al)O system with Mg/Al molar ratio of 5/1 was the best in terms of benzyl alcohol conversion, i.e., ca. 98% at 230 degrees C, under 5 atm of H2, for 3 h of reaction time, with high selectivity to toluene of ca. 87%, the influence of the reaction time, temperature and reusability over multiple reaction cycles on its performance were investigated.

The search for advanced materials has been growing, and high entropy alloys (HEAs) are emerging as promising candidates for application in the fusion domain. This work investigates the effect of Cr on the FeTaTiW medium entropy alloy to form (CrFeTaTi)70W30 high entropy alloy, comparing the experimental production and characterization with the simulation (molecular dynamics and hybrid molecular dynamics-Monte Carlo) of the phases formed. The alloys were produced by mechanical alloying and sintered by spark plasma sintering. Both simulations have shown that a body-centered cubic structure is formed for both compositions. Monte Carlo simulation provides a more precise prediction of microstructural formation and element segregation. Microstructural examination of the consolidated material revealed the presence of a W-rich phase and a Ti-rich phase, consistent with the phase separation observed in the MC simulations. Moreover, X-ray diffraction analysis of the milled powder for FeTaTiW and (CrFeTaTi)70W30 confirmed the formation of a bcc (body-centered cubic)-type structure with a low fraction of intermetallic phases. Mechanical testing showed ductile behavior at 1000 degrees C where (CrFeTaTi)70W30 showed a stress magnitude almost double that of FeTaTiW. Additionally, the thermal diffusivity between 20 and 1000 degrees C of both alloys increases as the temperature rises. (CrFeTaTi)70W30 exhibits an increase from 3 to 5 mm2/s, while FeTaTiW increases from 4 to 9 mm2/s. Still, both system's thermal diffusivity values are lower than those of CuCrZr and pure tungsten. Despite this, the study underscores the promising attributes of HEAs and highlights areas for further optimization to enhance its suitability for extreme conditions.

The gas sensitivity of field-effect structures with 2D-MoS2 channels selectively grown between Mo electrodes using the Mo-CVD method was investigated by measuring the effect of molecular adsorption from air on the device source-drain current (Isd). The channels were composed of interconnected atomically thin MoS2 grains, with their density and average thickness varied by choosing two different distances (15 and 20 mu m) between the Mo contacts. A high response to the tested stimuli, including molecule adsorption, illumination and gate voltage changes, was observed. A significant, persistent photoconduction was induced by positive charge accumulation on traps, most likely at grain boundaries and associated defects. Isd increased under high vacuum, both in the dark and under illumination. The relative dark current response to the transition from air to high vacuum reached up to 1000% at the turn-on voltage. When monitored during the gradual change in air pressure, Isd exhibited a non-monotonic function, sharply peaking at about 10-2 mbar, suggesting molecular adsorption on different defect sites and orientations of adsorbed H2O molecules, which were capable of inducing electron accumulation or depletion. Despite the screening of disorder by extra electrons, the #20 mu m sample remained more sensitive to air molecules on its surface. The high vacuum state was also investigated by annealing devices at temperatures up to 340 K in high vacuum, followed by measurements down to 100 K. This revealed thermally stimulated currents and activation energies of trapping electronic states assigned to sulfur vacancies (230 meV) and other shallow levels (85-120 meV), possibly due to natural impurities, grain boundaries or disorder defects. The results demonstrate the high sensitivity of these devices to molecular adsorption, making the technology promising for the easy fabrication of chemical sensors.

The transition from planar to three-dimensional (3D) magnetic nanostructures represents a significant advancement in both fundamental research and practical applications, offering vast potential for next-generation technologies like ultrahigh-density storage, memory, logic, and neuromorphic computing. Despite being a relatively new field, the emergence of 3D nanomagnetism presents numerous opportunities for innovation, prompting the creation of a comprehensive roadmap by leading international researchers. This roadmap aims to facilitate collaboration and interdisciplinary dialogue to address challenges in materials science, physics, engineering, and computing. The roadmap comprises eighteen sections, roughly divided into three blocks. The first block explores the fundamentals of 3D nanomagnetism, focusing on recent trends in fabrication techniques and imaging methods crucial for understanding complex spin textures, curved surfaces, and small-scale interactions. Techniques such as two-photon lithography and focused electron beam-induced deposition enable the creation of intricate 3D architectures, while advanced imaging methods like electron holography and synchrotron x-ray tomography provide nanoscale spatial resolution for studying magnetization dynamics in three dimensions. Various 3D magnetic systems, including coupled multilayer systems, artificial spin-ice, magneto-plasmonic systems, topological spin textures, and molecular magnets are discussed. The second block introduces analytical and numerical methods for investigating 3D nanomagnetic structures and curvilinear systems, highlighting geometrically curved architectures, interconnected nanowire systems, and other complex geometries. Finite element methods are emphasized for capturing complex geometries, along with direct frequency domain solutions for addressing magnonic problems. The final block focuses on 3D magnonic crystals and networks, exploring their fundamental properties and potential applications in magnonic circuits, memory, and spintronics. Computational approaches using 3D nanomagnetic systems and complex topological textures in 3D spintronics are highlighted for their potential to enable faster and more energy-efficient computing.

Today, flexible and lightweight electronics are regarded as a viable alternative to conventional rigid and heavy devices in various application fields. In the optoelectronic area, organic semiconductors offer advantages such as high absorption coefficients, low processing temperatures, mechanical flexibility and compatibility with plastic substrates, while inorganic nanostructures provide good electronic properties and high thermal stability. Thus, composite films with enhanced properties can be achieved by inserting inorganic nanostructures within organic layers. In this research work, CuS nanoparticles were prepared by wet chemical precipitation and then added to an organic mixture containing poly(3-hexylthiophene) (P3HT) and N,N-bis-(1-dodecyl)perylene-3,4,9,10 tetracarboxylic diimide (AMC14), a chemically synthesized semiconductor, for fabricating hybrid composite films by matrix assisted pulsed laser evaporation (MAPLE) on indium tin oxide/poly(ethylene terephthalate) (ITO/PET) flexible substrates. A comparative assessment of the morphological, compositional, optical and electrical properties of the composite (P3HT:AMC14:CuS) and organic (P3HT:AMC14) layers was performed to evaluate their applicability in the photovoltaic cells. The transmission and emission spectra of the composite films are dominated by the optical features of AMC14, a perylene diimide derivative compound used as acceptor. In the case of devices based on MAPLE deposited composite layer fabricated on ITO/PET substrates, the electrical measurements carried under illumination revealed an improvement in the open circuit voltage parameter emphasizing their potential applications in the flexible device area.

Following the approach of inducing structural constrains for the creation of polar nanodomains/nanoregions in the perovskite thin films, the photoelectrochemical properties of complex heterostructures based on LaFeO3 and BiFeO3 materials have been studied in correlation with the imposed structural strain and polarization orientation anisotropy conditions. The LFO/BFO thin film heterostructures have been tested using photoelectrochemical (PEC) technique. The recorded photocurrent values for the heterostructure with the LFO layer on top- LFO/BFO/STON- in the potentiodinamic regime are considerably higher (similar to 1.64 mA/cm(2) at 2 V vs RHE) than those obtained for BFO/LFO/STON heterostructure where the BFO layer is acting as the surface layer (similar to 0.32 mA/cm(2) at 2 V vs RHE). Moreover, the LFO/BFO/STON heterostructure exhibits both photocathodic and photoanodic behavior. The atomic resolution STEM data demonstrate the polarization orientation anisotropy in LFO/BFO/STON heterostructure, due to the cooperative effects of competing surface chemistry and polarization of the LFO/BFO interface over the magnitude and orientation of the Fe3+ cations displacement within the La3+ cages. For the BFO/LFO/STON heterostructure however, robust single-oriented domains with large Fe3+ cations displacement characteristics for long-range ferroelectric order, has been revealed also. Taking into account the possibility to control the PEC features such as charge distribution/transport characteristics for both photocathodic/photoanodic reactions, as well as the control of the polarization direction without a pre-poling process, this work is of relevance for applications where the use of a top electrode is not possible.

We present herein the synthesis of novel [2 + 2] and [3 + 3] N-acylhydrazone-based macrocycles using a pool of dialdehydes and dihydrazides, under thermodynamic control. The resulting macrocycles, which were assigned triangular and rectangular shapes, were characterised in the solid state. The rectangular macrocycle was further investigated in solution by absorption and emission spectroscopy. Additionally, the rectangular macrocycle was used in various assays to investigate the hosting capacity towards various guests using NMR, HRMS, UV-visible and fluorescence spectroscopy. Theoretical calculations regarding structure and properties of the novel compounds were in agreement with the experimental details. The experimental data showed intriguing results toward tetra-n-butylammonium fluoride.

Synchrotron-based small- and wide-angle X-ray scattering is used to elucidate the structure of low-dimensional lepidocrocite-titanate-based nanofilaments. In the colloidal state, they consist of quantum-confined 1D NFs, loosely associated into nanoribbons, one lepidocrocite sheet thick (about 4 & Aring;), 30-40 & Aring; wide (5-8 NFs), and more than 300 & Aring; long. In the dry state, they reach a final state of extended sheets, stacked three to about twenty high, whose crystallinity increases with stack height, in parallel with a decrease in photocatalytic activity. These findings suggest a kinetic pathway for the self-assembly of initially 1D titanate nanoribbons into 2D and ultimately 3D structures, providing context for a recent body of work on these low-dimensional materials.