Search Results (97)

Prototype-Based Networks (PBNs) are inherently interpretable architectures that facilitate understanding of model outputs by analyzing the activation of specific neurons—referred to as prototypes—during the forward pass. The learned prototypes serve as transformations of the input space into a latent representation that more effectively encapsulates the main characteristics shared across data samples, thereby enhancing classification performance. Crucially, these prototypes can be decoded and projected back into the original input space, providing direct interpretability of the features learned by the network. While this characteristic marks a meaningful advancement toward the realization of fully interpretable artificial intelligence systems, our findings reveal that prototype representations can be deliberately or inadvertently manipulated without compromising the superficial appearance of explainability. In this study, we conduct a series of empirical investigations that demonstrate this phenomenon, framing it as a structural paradox potentially intrinsic to the architecture or its design, which may represent a significant robustness challenge for explainable AI methodologies. Full article

Halide perovskite-based memristors are promising neuromorphic devices due to their unique ion migration and interface tunability, yet their conduction mechanisms remain unclear, causing stability and performance issues. Here, we engineer interstitial Ag⁺ ions within a quasi-two-dimensional (quasi-2D) halide perovskite ((C₆H₅C₂H₄NH₃)₂Cs_n−1Pb_nI_3n+1) to enhance device stability and controllability. The introduced Ag⁺ ions occupy organic interlayers, forming thermodynamically stable structures and introducing deep-level energy states without structural distortion, which do not act as non-radiative recombination centers, but instead serve as efficient charge trapping centers that stabilize intermediate resistance states and facilitate controlled filament evolution during resistive switching. This modification also leads to enhanced electron transparency near the Fermi level, contributing to improved charge transport dynamics and device performance. Under external electric fields, these Ag⁺ ions act as mobile ionic species, facilitating controlled filament formation and stable resistive switching. The resulting devices demonstrate exceptional performance, featuring an ultrahigh on/off ratio (∼10⁸) and low operating voltages (∼0.31 V), surpassing existing benchmarks. Our findings highlight the dual role of Ag⁺ ions in structural stabilization and conduction modulation, providing a robust approach for high-performance perovskite memristor engineering. Full article

The two-dimensional (2D) Ruddlesden–Popper perovskite exhibits superior chemical stability but suffers from compromised photoelectric properties due to the van der Waals gap. This study presents a novel investigation of surface passivation effects on quasi-2D perovskite X₂Cs_n−1Pb_nI_3n+1 (n = 1–6; X = MA, FA, PEA) using DFT methods, revealing three key advances: First, we demonstrate that organic cation passivation (MA⁺, FA⁺, PEA⁺) enables exceptional stability improvements, with FA-passivated structures showing optimal stability—a crucial finding for materials design. Second, we identify a critical thickness effect (n > 3) where bandgaps converge to <1.6 eV (approaching bulk values) while maintaining strong absorption, establishing the minimum layer requirement for optimal performance. Third, we reveal that effective masses balance and absorption strengthens significantly when n > 3. These fundamental insights provide a transformative strategy to simultaneously enhance both stability and optoelectronic properties in quasi-2D perovskites. Full article

Covalent triazine frameworks (CTFs) have gained recognition as stable porous organic polymers, for example, for CO₂ separation. From the monomer 4,4′-(phenazine-5,10-diyl)dibenzonitrile (pBN), new pBN-CTFs were synthesized using the ionothermal method with a variation in temperature (400 and 550 °C) and the ZnCl₂-to-monomer ratio (10 and 20). N₂ adsorption yielded BET surface areas up to 1460 m²g ⁻¹. The pBN-CTFs are promising CO₂ adsorbents and are comparable to other benchmark CTFs such as CTF-1 with a CO₂ uptake of pBN-CTF-10-550 at 293 K of up to 54 cm³ g⁻¹ or 96 mg g⁻¹, with a CO₂/CH₄ IAST selectivity of 22 for a 50% mixture of CO₂/CH₄. pBN-CTF-10-400 has a very high heat of adsorption of 79 kJ mol⁻¹ for CO₂ near zero coverage in comparison to other CTFs, and it also stays well above the liquefaction heat of CO₂ due to its high microporosity of 50% of the total pore volume. Full article

Seven lager beers and seven non-alcoholic counterparts, marketed by the same producers, were analyzed for their total phenolic content (TPC), radical scavenging activity (RSA) towards the DPPH radical and ThioBarbituric Index (TBI). All beers were also subjected to spin trapping experiments at 60 °C in the presence of PBN. To our knowledge, this is the first time that non-alcoholic beers (NABs) have been subjected to spin trapping experiments coupled with Electron Spin Resonance (ESR) spectroscopy. The evolution of the intensity of the PBN radical adducts during the first 150 min was represented graphically and the intensity at 150 min (I₁₅₀) and the area under the curve (AUC), were measured. The I₁₅₀ and the AUC of lagers and NABs are significantly different, whereas the TPC, the EC₅₀ of the DPPH assay, and the TBI of the two groups are superimposed. A relationship, previously proposed by us, to correlate ESR spectroscopy parameters with others obtained from UV-Vis spectrophotometry, was also applied, demonstrating its practicability. Multivariate analysis shows that clustering in two separate groups occurs only if I₁₅₀ and AUC are included in the model. Based on these results, ESR spectroscopy can be applied to study the oxidative stability of NABs. Full article

First-principles calculations were conducted to examine the impact of three sulfonamide-containing molecules (H₄N₂O₂S, CH₈N₄O₃S, and C₂H₂N₆O₄S) adsorbed on the FAPbI₃(001) perovskite surface, aiming to establish a significant positive correlation between the molecular structures and their regulatory effects on the perovskite surface. A systematic comparison was conducted to evaluate the adsorption stability of the three molecules on the two distinct surface terminations. The results show that all three molecules exhibit strong adsorption on the FAPbI₃(001) surface, with C₂H₁₂N₆O₄S demonstrating the most favorable binding stability due to its extended frameworks and multiple electron-donating/withdrawing groups. Simpler molecules lacking carbon skeletons exhibit weaker adsorption and less dependence on surface termination. Ab initio molecular dynamics simulations (AIMD) further corroborated the thermal stability of the stable adsorption configurations at elevated temperatures. Electronic structure analysis reveals that molecular adsorption significantly reconstructs the density of states (DOS) on the PbI₂-terminated surface, inducing shifts in band-edge states and enhancing energy-level coupling between molecular orbitals and surface states. In contrast, the FAI-terminated surface shows weaker interactions. Charge density difference (CDD) analysis indicates that the molecules form multiple coordination bonds (e.g., Pb–O, Pb–S, and Pb–N) with uncoordinated Pb atoms, facilitated by –SO₂–NH₂ groups. Bader charge and work function analyses indicate that the PbI₂-terminated surface exhibits more pronounced electronic coupling and interfacial charge transfer. The C₂H₁₂N₆O₄S adsorption system demonstrates the most substantial reduction in work function. Optical property calculations show a distinct red-shift in the absorption edge along both the XX and YY directions for all adsorption systems, accompanied by enhanced absorption intensity and broadened spectral range. These findings suggest that sulfonamide-containing molecules, particularly C₂H₁₂N₆O₄S with extended carbon skeletons, can effectively stabilize the perovskite interface, optimize charge transport pathways, and enhance light-harvesting performance. Full article

Despite the rapid efficiency advancement of perovskite solar cells (PSCs), non-radiative recombination at the buried interface between self-assembled monolayers (SAMs) and perovskite remains a critical bottleneck, primarily due to interfacial defects and energy level mismatch. In this study, we demonstrate a bifunctional interlayer engineering strategy by introducing 4,5-diiodoimidazole (4,5-Di-I) at the Me-4PACz/perovskite interface. This approach uniquely addresses two fundamental limitations of SAM-based interfaces: the insufficient defect passivation capability of conventional Me-4PACz due to steric hindrance effects and the poor perovskite wettability on hydrophobic SAM surfaces that exacerbates interfacial voids. The imidazole derivatives not only form strong Pb–N coordination bonds with undercoordinated Pb²⁺ but also modulate the surface energy of Me-4PACz, enabling the growth of pinhole-free perovskite films with preferential crystal orientation. The champion device with 4,5-Di-I modification achieves a power conversion efficiency (PCE) of 24.10%, with a V_OC enhancement from 1.12 V to 1.14 V, while maintaining 91% of initial PCE after 1300 h in N₂ atmosphere (25 °C), demonstrating superior stability under ISOS-L-2 protocols. This work establishes a universal strategy for interfacial multifunctionality design, proving that simultaneous defect suppression and crystallization control can break the long-standing trade-off between efficiency and stability in solution-processed photovoltaics. Full article

Using reduced-dimensional halide perovskites is emerging as a promising strategy for enhancing the stability of optoelectronic devices such as solar cells, even if their performances remain a step below those of the 3D halide perovskites. Two-dimensional Ruddlesden–Popper (2D-RP) structures are characterized by the n parameter that represents the number of PbI₆ layers in the spacer-separated perovskite slabs. The present study focuses on formamidinium (FA)-based 2D-RP type perovskites denoted as PMA₂FA_n−1Pb_nI_3n+1 (PMA = Phenylmethylammonium or benzylammonium). We investigate the effect of n on the one step growth mechanism and the film morphology, microstructure, phase purity, and optoelectronic properties. Our findings demonstrate that the average n is not only determined by the initial spacer content in the precursor solution but also by the thermal annealing process that leads to a partial spacer loss. Depending on n, perovskite solar cells achieving a power conversion efficiency up to 21%, coupled with enhanced film stability compared to 3D perovskites have been prepared. By using MACl additive and an excess of PbI₂ in the perovskite precursor solution, we have been able to achieve high efficiency and to stabilize the n = 5 perovskite solar cells. This research represents a significant stride in comprehending the formation of FA-based layered perovskites through one-step sequential deposition, enabling control over their phase distribution, composition, and orientation. Full article

Probabilistic Boolean Networks (PBN) can model the dynamics of complex biological systems, as well as other non-biological systems like manufacturing systems and smart grids. In this proof-of-concept paper, we propose a PBN architecture with a learning process that significantly enhances fault and failure prediction in manufacturing systems. This concept was tested using a PBN model of an ultrasound welding process and its machines. Through various experiments, the model successfully learned to maintain a normal operating state. Leveraging the complex properties of PBNs, we utilize them as an adaptive learning tool with positive feedback, demonstrating that these networks may have broader applications than previously recognized. This multi-layered PBN architecture offers substantial improvements in fault detection performance within a positive feedback network structure that shows greater noise tolerance than other methods. Full article

Phosphorylated nitrones belong to an important class of compounds with several applications, such as their therapeutic potency to reduce oxidative stress or as spin-trapping agents. This review covers available synthetic methods for the preparation of both non-cyclic and cyclic phosphorylated nitrones, including the possibilities of the modification of structures with selected functional groups, as well as examples of their application. As reported, the incorporation of diethoxyphosphoryl function into the structure of PBN and DMPO resulted in obtaining their phosphorylated analogs, i.e., N-benzylidene-1-diethoxyphosphoryl-1-methylethylamine N-oxide (PPN) and 5-(diethoxyphosphoryl)-5-methyl-1-pyrroline-N-oxide (DEPMPO), respectively, both forming spin adducts of improved stability in comparison to the reference non-phosphorus nitrones. Moreover, antioxidant and neuroprotective activity observed in the group of phosphorylated nitrones makes them promising candidates for therapeutics. Full article

Probabilistic Boolean Networks can capture the dynamics of complex biological systems as well as other non-biological systems, such as manufacturing systems and smart grids. In this proof-of-concept manuscript, we propose a Probabilistic Boolean Network architecture with a learning process that significantly improves the prediction of the occurrence of faults and failures in smart-grid systems. This idea was tested in a Probabilistic Boolean Network model of the WSCC nine-bus system that incorporates Intelligent Power Routers on every bus. The model learned the equality and negation functions in the different experiments performed. We take advantage of the complex properties of Probabilistic Boolean Networks to use them as a positive feedback adaptive learning tool and to illustrate that these networks could have a more general use than previously thought. This multi-layered PBN architecture provides a significant improvement in terms of performance for fault detection, within a positive-feedback network structure that is more tolerant of noise than other techniques. Full article

This longitudinal study examined how active gastrointestinal (GI) cancer types affect immune responses to SARS-CoV-2, focusing on the ability to neutralize the Omicron variants. Patients with GI cancer (n = 168) were categorized into those with hepatocellular carcinoma, hepatic metastatic GI cancer, non-hepatic metastatic GI cancer, and two control groups of patients with and without underlying liver diseases. Humoral and cellular immune responses were evaluated before and after Omicron antigen exposures. In the pre-Omicron era, humoral SARS-CoV-2 immunity decreased after three antigen contacts without further antigen exposure. While Omicron neutralization was significantly lower than wildtype neutralization (p < 0.01), Omicron infections were yet mild to moderate. Additional Omicron exposures improved IgG levels (p < 0.01) and Omicron neutralization (p < 0.01). However, this effect was significantly less intense in patients with active GI cancer, particularly in patients with pancreaticobiliary neoplasms (PBN; p = 0.04), with underlying immunodeficiency (p = 0.05), and/or under conventional chemotherapy (p = 0.05). Pre-Omicron SARS-CoV-2 immunity prevented severe clinical courses of infections with Omicron variants in patients with GI cancer. However, in patients with PBN, with underlying immunodeficiency, and/or under conventional chemotherapy initial contacts with Omicron antigens triggered only reduced immune responses. Thus, subgroups could be identified for whom booster vaccinations are of special clinical significance. Full article

The insular cortex is an important hub for sensory and emotional integration. It is one of the areas consistently found activated during pain. While the insular’s connections to the limbic system might play a role in the aversive and emotional component of pain, its connections to the descending pain system might be involved in pain intensity coding. Here, we used anterograde tracing with viral expression of mCherry fluorescent protein, to examine the connectivity of insular axons to different brainstem nuclei involved in the descending modulation of pain in detail. We found extensive connections to the main areas of descending pain control, namely, the periaqueductal gray (PAG) and the raphe magnus (RMg). In addition, we also identified an extensive insular connection to the parabrachial nucleus (PBN). Although not as extensive, we found a consistent axonal input from the insula to different noradrenergic nuclei, the locus coeruleus (LC), the subcoereuleus (SubCD) and the A5 nucleus. These connections emphasize a prominent relation of the insula with the descending pain modulatory system, which reveals an important role of the insula in pain processing through descending pathways. Full article

Following Dirac’s notation in Quantum Mechanics (QM), we propose the Probability Bracket Notation (PBN), by defining a probability-bra (P-bra), P-ket, P-bracket, P-identity, etc. Using the PBN, many formulae, such as normalizations and expectations in systems of one or more random variables, can now be written in abstract basis-independent expressions, which are easy to expand by inserting a proper P-identity. The time evolution of homogeneous Markov processes can also be formatted in such a way. Our system P-kets are identified with probability vectors and our P-bra system is comparable with Doi’s state function or Peliti’s standard bra. In the Heisenberg picture of the PBN, a random variable becomes a stochastic process, and the Chapman–Kolmogorov equations are obtained by inserting a time-dependent P-identity. Also, some QM expressions in Dirac notation are naturally transformed to probability expressions in PBN by a special Wick rotation. Potential applications show the usefulness of the PBN beyond the constrained domain and range of Hermitian operators on Hilbert Spaces in QM all the way to IT. Full article

The present study is a theoretical investigation into the structural evolution, electronic properties, and photoelectron spectra of phosphorus-doped boron clusters PB_n^0/− (n = 3–17). The results of this study revealed that the lowest energy structures of PB_n⁻ (n = 3–17) clusters, except for PB₁₇⁻, exhibit planar or quasi-planar structures. The lowest energy structures of PB_n (n = 3–17), with the exceptions of PB₇, PB₉, and PB₁₅, are planar or quasi-planar. The ground state of PB₇ has an umbrella-shaped structure, with C_6V symmetry. Interestingly, the neutral cluster PB₁₅ has a half-sandwich-like structure, in which the P atom is attached to three B atoms at one end of the sandwich, exhibiting excellent relative and chemical stability due to its higher second-order energy difference and larger HOMO–LUMO energy gap of 4.31 eV. Subsequently, adaptive natural density partitioning (AdNDP) and electron localization function (ELF) analyses demonstrate the bonding characteristics of PB₇ and PB₁₅, providing support for the validity of their stability. The calculated photoelectron spectra show distinct characteristic peaks of PB_n⁻ (n = 3–17) clusters, thus providing theoretical evidence for the future identification of doped boron clusters. In summary, our work has significant implications for understanding the structural evolution of doped boron clusters PB_n^0/− (n = 3–17), motivating further experiments regarding doped boron clusters. Full article