Catalase Detection via Membrane-Based Pressure Sensors.

Membrane-based sensors (MePSs) exhibit remarkable precision and sensitivity in detecting pressure changes. MePSs are commonly used to monitor catalytic reactions in solution, generating gas products crucial for signal amplification in bioassays. They also allow for catalyst quantification by indirectly measuring the pressure generated by the gaseous products. This is particularly interesting for detecting enzymes in biofluids associated with disease onset. To enhance the performance of a MePS, various structural factors influence membrane flexibility and response time, ultimately dictating the device's pressure sensitivity. In this study, we fabricated MePSs using polydimethylsiloxane (PDMS) and investigated how structural modifications affect the Young's modulus (E) and residual stress (σ0) of the membranes. These modifications have a direct impact on the sensors' sensitivity to pressure variations, observed as a function of the volume of the chamber (Σ) or of the mechanical properties of the membrane itself (S). MePSs exhibiting the highest sensitivities were then employed to detect catalyst quantities inducing the dismutation of hydrogen peroxide, producing dioxygen as a gaseous product. As a result, a catalase enzyme was successfully detected using these optimized MePSs, achieving a remarkable sensitivity of (22.7 ± 1.2) µm/nM and a limit of detection (LoD) of 396 pM.

The First Nucleic Acid Strands May Have Grown on Peptides via Primeval Reverse Translation.

The central dogma of molecular biology dictates that, with only a few exceptions, information proceeds from DNA to protein through an RNA intermediate. Examining the enigmatic steps from prebiotic to biological chemistry, we take another road suggesting that primordial peptides acted as template for the self-assembly of the first nucleic acids polymers. Arguing in favour of a sort of archaic "reverse translation" from proteins to RNA, our basic premise is a Hadean Earth where key biomolecules such as amino acids, polypeptides, purines, pyrimidines, nucleosides and nucleotides were available under different prebiotically plausible conditions, including meteorites delivery, shallow ponds and hydrothermal vents scenarios. Supporting a protein-first scenario alternative to the RNA world hypothesis, we propose the primeval occurrence of short two-dimensional peptides termed "selective amino acid- and nucleotide-matching oligopeptides" (henceforward SANMAOs) that noncovalently bind at the same time the polymerized amino acids and the single nucleotides dispersed in the prebiotic milieu. In this theoretical paper, we describe the chemical features of this hypothetical oligopeptide, its biological plausibility and its virtues from an evolutionary perspective. We provide a theoretical example of SANMAO's selective pairing between amino acids and nucleosides, simulating a poly-Glycine peptide that acts as a template to build a purinic chain corresponding to the glycine's extant triplet codon GGG. Further, we discuss how SANMAO might have endorsed the formation of low-fidelity RNA's polymerized strains, well before the appearance of the accurate genetic material's transmission ensured by the current translation apparatus.

Light Emission Properties of Thermally Evaporated CH3NH3PbBr3 Perovskite from Nano- to Macro-Scale: Role of Free and Localized Excitons.

Over the past decade, interest about metal halide perovskites has rapidly increased, as they can find wide application in optoelectronic devices. Nevertheless, although thermal evaporation is crucial for the development and engineering of such devices based on multilayer structures, the optical properties of thermally deposited perovskite layers (spontaneous and amplified spontaneous emission) have been poorly investigated. This paper is a study from a nano- to micro- and macro-scale about the role of light-emitting species (namely free carriers and excitons) and trap states in the spontaneous emission of thermally evaporated thin layers of CH3NH3PbBr3 perovskite after wet air UV light trap passivation. The map of light emission from grains, carried out by SNOM at the nanoscale and by micro-PL techniques, clearly indicates that free and localized excitons (EXs) are the dominant light-emitting species, the localized excitons being the dominant ones in the presence of crystallites. These species also have a key role in the amplified spontaneous emission (ASE) process: for higher excitation densities, the relative contribution of localized EXs basically remains constant, while a clear competition between ASE and free EXs spontaneous emission is present, which suggests that ASE is due to stimulated emission from the free EXs.

Potential of CO2-laser processing of quartz for fast prototyping of microfluidic reactors and templates for 3D cell assembly over large scale.

Carbon dioxide (CO2)-laser processing of glasses is a versatile maskless writing technique to engrave micro-structures with flexible control on shape and size. In this study, we present the fabrication of hundreds of microns quartz micro-channels and micro-holes by pulsed CO2-laser ablation with a focus on the great potential of the technique in microfluidics and biomedical applications. After discussing the impact of the laser processing parameters on the design process, we illustrate specific applications. First, we demonstrate the use of a serpentine microfluidic reactor prepared by combining CO2-laser ablation and post-ablation wet etching to remove surface features stemming from laser-texturing that are undesirable for channel sealing. Then, cyclic olefin copolymer micro-pillars are fabricated using laser-processed micro-holes as molds with high detail replication. The hundreds of microns conical and square pyramidal shaped pillars are used as templates to drive 3D cell assembly. Human Umbilical Vein Endothelial Cells are found to assemble in a compact and wrapping way around the micro-pillars forming a tight junction network. These applications are interesting for both Lab-on-a-Chip and Organ-on-a-Chip devices.

Pulsed Laser Deposition of CsPbBr3 Films: Impact of the Composition of the Target and Mass Distribution in the Plasma Plume.

All-inorganic cesium lead bromine (CsPbBr3) perovskites have gained a tremendous potential in optoelectronics due to interesting photophysical properties and much better stability than the hybrid counterparts. Although pulsed laser deposition (PLD) is a promising alternative to solvent-based and/or thermal deposition approaches due to its versatility in depositing multi-elemental materials, deep understanding of the implications of both target composition and PLD mechanisms on the properties of CsPbBr3 films is still missing. In this paper, we deal with thermally assisted preparation of mechano-chemically synthesized CsPbBr3 ablation targets to grow CsPbBr3 films by PLD at the fluence 2 J/cm2. We study both Cs rich- and stoichiometric PbBr2-CsBr mixture-based ablation targets and point out compositional deviations of the associated films resulting from the mass distribution of the PLD-generated plasma plume. Contrary to the conventional meaning that PLD guarantees congruent elemental transfer from the target to the substrate, our study demonstrates cation off-stoichiometry of PLD-grown CsPbBr3 films depending on composition and thermal treatment of the ablation target. The implications of the observed enrichment in the heavier element (Pb) and deficiency in the lighter element (Br) of the PLD-grown films are discussed in terms of optical response and with the perspective of providing operative guidelines and future PLD-deposition strategies of inorganic perovskites.

Efficient Flexible Inorganic Perovskite Light-Emitting Diodes Fabricated with CsPbBr3 Emitters Prepared via Low-Temperature in Situ Dynamic Thermal Crystallization.

The present study systematically investigates the morphology and crystallization process of inorganic CsPbBr3 perovskite layer films fabricated by thermal coevaporation in conjunction with continuous low-temperature thermal annealing to promote in situ dynamic thermal crystallization. The results confirm for the first time that both the crystal grain size and the compactness of the CsPbBr3 films can be tuned during the thermal coevaporation fabrication process via in situ dynamic thermal crystallization. The performance of the PeLEDs employing the CsPbBr3 films as the emitter layer is investigated in detail with respect to the substrate temperature and deposition rate employed during deposition of the CsPbBr3 film. This study provides guidelines for developing suitable film production processes and highlights future challenges that must be addressed to facilitate the commercial development of large-area, uniform, and flexible perovskite-based optoelectronic devices.

All-Inorganic CsPbBr3 Perovskite Films Prepared by Single Source Thermal Ablation.

Hybrid organo-lead halide perovskites are becoming the benchmark material for next generation photovoltaics and a very important player for other applications such as photodetectors and light emitting diodes. Nevertheless, the most important issue hindering the large-scale application of these materials remains their intrinsic instability due to the organic cation. Although the substitution with inorganic cesium (Cs) enhances stability, in most cases solution deposition methods of fully inorganic perovskites result in high surface roughness and poor surface coverage. This work reports on the evaporation of the CsPbBr3 precursor by Single Source Thermal Ablation, showing that just after deposition films consist of a mixture of CsPbBr3, CsPb2Br5, and Cs4PbBr6 due to a vertical composition gradient. We point out that mild post deposition treatments lead to the conversion of CsPb2Br5 and Cs4PbBr6 into CsPbBr3 due to its higher thermodynamic stability. Conversion results into smooth and pinhole-free CsPbBr3 films with good light absorption and emission properties. We demonstrate the suitability of obtained films for planar devices by preparing perovskite-based pure-green light emitting diodes, thus promoting Single Source Thermal Ablation as a promising alternative deposition technique for all-inorganic perovskite-based devices.

A flexible plasma-treated silver-nanowire electrode for organic light-emitting devices.

Silver nanowires (AgNWs) are a promising candidate to replace indium tin oxide (ITO) as transparent electrode material. However, the loose contact at the junction of the AgNWs and residual surfactant polyvinylpyrrolidone (PVP) increase the sheet resistance of the AgNWs. In this paper, an argon (Ar) plasma treatment method is applied to pristine AgNWs to remove the PVP layer and enhance the contact between AgNWs. By adjusting the processing time, we obtained AgNWs with a sheet resistance of 7.2Ω/□ and a transmittance of 78% at 550 nm. To reduce the surface roughness of the AgNWs, a peel-off process was used to transfer the AgNWs to a flexible NOA63 substrate. Then, an OLED was fabricated with the plasma-treated AgNWs electrode as anode. The highest brightness (27000 cd/m2) and current efficiency (11.8 cd/A) was achieved with a 30 nm thick light emitting layer of tris-(8-hydroxyquinoline) aluminum doped with 1% 10-(2-benzothiazolyl)-2,3,6,7-tetrahydro-1,1,7,7-tetramethyl-1H,5 H,11H-(1)-benzopyropyrano(6,7-8-I,j)quinolizin-11-one. Compared to thermal annealing, the plasma-treated AgNW film has a lower sheet resistance, a shorter processing time, and a better hole-injection. Our results indicate that plasma treatment is an effective and efficient method to enhance the conductivity of AgNW films, and the plasma-treated AgNW electrode is suitable to manufacture flexible organic optoelectronic devices.

The Bright Side of Perovskites.

Incubating in the rise of perovskite photovoltaic era, the advances in material design encourage further promising optoelectronic exploitations. Here, we evaluate halide perovskite envisioning light-emitting applications, with a particular focus to the role that this material can effectively play in the field, discussing advantages and limitations with respect to state of art competing players. Specific benefits derive from the use of low dimensional and nanostructured perovskites, marginally exploited in photovoltaic devices, allowing for a tuning of the excited states properties and for the obtainment of intrinsic resonating structures. Thanks to these unique properties, halide perovskite ensure a great potential for the development of high-power applications, such as lighting and lasing.

A colour tunable microcavity by weak-to-strong coupling regime transition through a light-switchable material.

An organic based microcavity showing fully reversible colour tunability has been achieved for the first time. The emission output changes according to the modulation from pure photonic to polaritonic resonant modes through UV irradiation of the light-switchable matrix.

Aryl 5-substitution of a phenyl-pyridine based ligand as a viable way to influence the opto-electronic properties of bis-cyclometalated Ir(III) heteroleptic complexes.

This manuscript reports on the synthesis, the photophysical study and the electroluminescent properties of a series of heteroleptic cyclometalated iridium(III) complexes based on 2,5-diaryl-pyridines as C^N cyclometalating ligands and acetylacetonate as ancillary ligand. The complexes were characterised by elemental analysis, ESI-MS, multinuclear NMR, TGA and electrochemistry. Their optical properties were investigated by UV-Vis and photoluminescence. DFT and TD-DFT calculations provided further insights into the effects of the 5-aryl substitution on the electronic and photophysical properties of the new complexes. The presence of suitable π-extended ligands exerts a beneficial effect on the performances of the corresponding solution-processed light-emitting diodes, leading to a maximum brightness of 10,620 cd m(-2) at a current efficiency of 10.0 cd A(-1).

A review of macroscopic thrombus modeling methods.

Hemodynamics applied to mechanobiology offers powerful means to predict thrombosis, and to understand the kinetics of thrombus formation on areas of vascular damage in blood flowing through the human circulatory system. Specifically, the advances in computational processing and the progress in modeling complex biological processes with spatio-temporal multi-scale methods have the potential to shift the way in which cardiovascular diseases are diagnosed and treated. This article systematically surveys the state of the art of macroscopic computational fluid dynamics (CFD) Computational fluid dynamics techniques for modeling thrombus formation, highlighting their strengths and weaknesses. In particular, a comprehensive and systematic revision of the hemodynamics models and methods is given, and the strengths and weaknesses of those employed for studying thrombus formation are highlighted.

Light absorption enhancement in heterostructure organic solar cells through the integration of 1-D plasmonic gratings.

The integration of a plasmonic lamellar grating in a heterostructure organic solar cell as a light trapping mechanism is investigated with numerical Finite Elements simulations. A global optimization of all the geometric parameters has been performed. The obtained wide-band enhancement in optical absorption is correlated with both the propagating and the localized plasmonic modes of the structure, which have been identified and characterized in detail.

AngioLab--a software tool for morphological analysis and endovascular treatment planning of intracranial aneurysms.

Determining whether and how an intracranial aneurysm should be treated is a tough decision that clinicians face everyday. Emerging computational tools could help clinicians analyze clinical data and make these decisions. AngioLab is a single graphical user interface, developed on top of the open source framework GIMIAS, that integrates some of the latest image analysis and computational modeling tools for intracranial aneurysms. Two workflows are available: Advanced Morphological Analysis (AMA) and Endovascular Treatment Planning (ETP). AngioLab has been evaluated by a total of 62 clinicians, who considered the information provided by AngioLab relevant and meaningful. They acknowledged the emerging need of these type of tools and the potential impact they might have on the clinical decision-making process.

Monodispersed molecular donors for bulk hetero-junction solar cells: from molecular properties to device performances.

The relations between the chemical-physical properties of novel designed monodispersed donors and their photovoltaic performances are discussed. The importance of intermolecular interactions is emphasized to figure out the achievement of high performing bulk hetero-junction solar cells which are solution processed.

Petascale lattice-Boltzmann studies of amphiphilic cubic liquid crystalline materials in a globally distributed high-performance computing and visualization environment.

We present very large-scale rheological studies of self-assembled cubic gyroid liquid crystalline phases in ternary mixtures of oil, water and amphiphilic species performed on petascale supercomputers using the lattice-Boltzmann method. These nanomaterials have found diverse applications in materials science and biotechnology, for example, in photovoltaic devices and protein crystallization. They are increasingly gaining importance as delivery vehicles for active agents in pharmaceuticals, personal care products and food technology. In many of these applications, the self-assembled structures are subject to flows of varying strengths and we endeavour to understand their rheological response with the objective of eventually predicting it under given flow conditions. Computationally, our lattice-Boltzmann simulations of ternary fluids are inherently memory- and data-intensive. Furthermore, our interest in dynamical processes necessitates remote visualization and analysis as well as the associated transfer and storage of terabytes of time-dependent data. These simulations are distributed on a high-performance grid infrastructure using the application hosting environment; we employ a novel parallel in situ visualization approach which is particularly suited for such computations on petascale resources. We present computational and I/O performance benchmarks of our application on three different petascale systems.

Pure white hybrid light-emitting device with color rendering index higher than 90.

The realization of white-light sources with a combination of high color rendering index (CRI), which is the average of the first eight rendering indices, and the deep-red color rendering R9 is an important challenge in the field of solid-state lighting. Herein, we report on a pure white hybrid light-emitting device combining a deep-blue emission from a polymer with blue, green, and red emissions from ternary CdSe/ZnS quantum dots. By carefully designing the device structure and tuning the ratio of QDs with different sizes, high CRI of 94 and R9 of 92 at 525 cd/m(2) were achieved.

A molecular level simulation of a twisted nematic cell.

We have performed a Monte Carlo simulation of a sub-micrometric twisted nematic cell with nearly 106 particles using an off-lattice molecular model of a liquid crystal. This computer experiment is a proof of principle that molecular models can be pushed to the limit of the system sizes addressable with finite element models thus bridging the mesoscopic gap for multiscale modelling while providing a direct molecular level view of the working of the display. This approach, that allows a direct prediction of molecular organisations, properties, and responses of device systems without the requirement of prior estimate or knowledge of material properties (e.g., elastic constants), is particularly important in view of simulating materials and devices for which these quantities are not known. Results for the molecular organisation are discussed, with particular regard to its helical nature in the field-off state.

Polarized light emitting diode by long-range nanorod self-assembling on a water surface.

We demonstrate a straightforward strategy to fabricate a multilayer inorganic/organic polarized light-emitting diode device based on highly ordered arrays of rod-shaped nanocrystals as the active species. We have developed a simple and effective method that allows colloidal CdSe/CdS core/shell nanorods to be laterally aligned in smectic or nematic phases on the surface of water. A floating film of such ordered nanorods has been collected by a poly(dimethylsiloxane) (PDMS) stamp pad and transferred by contact printing onto previously evaporated organic layers. Thanks to the lateral nanorod alignment the as-prepared film exhibited strong polarized photoluminescence and it has been used as emissive layer in the polarized electroluminescent device.