BINA

The closed topology of spherical crystals renders the presence of topological defects inevitable. These defects can organize in a plethora of different structures, such as “clouds” or grain boundary “scars”, challenging for theoretical modeling and experimental visualization. Visualizing the defects by fluorescent dye adsorption, we reveal ion concentration control of a clouds-to-scars transition, which we attribute to commonly neglected defects' core energy. The consequent line tension energy probes the defects' molecular scale energetics, enabling pattern tuning for future applications.

Plasmonic nanostructure arrays, designed for performance as pixels in an advanced SERS imaging device, were fabricated by gallium focused ion beam (FIB). Though the FIB is best suited for etching holes and negative structures, our previously reported simulations favor protrusions. Herein, we report on the FIB methodology to “sculpt” positive structures by “ion-blasting” away the surrounding material. Nanoprotrusions and nanoholes with different aspect ratios are compared experimentally with depth and height controlled by the dwell time. The amplitude and spectra of optical absorption and scattering from the two species are compared as a function of structure height. Measurements were performed using ASI’s model Rainbow hyperspectral camera, demonstrating the utility of hyperspectral microscopy for plasmonic imaging applications. Both the scattered and absorbed radiation display the broad peak …

Self-healing materials can become game changers for developing sustainable (opto)electronics. APbX3 halide (=X–) perovskites, HaPs, have shown a remarkable ability to self-heal damage. While we demonstrated self-healing in pure HaP compounds, in single crystals, and in polycrystalline thin films (as used in most devices), HaP compositions with multiple A+ (and X–) constituents are preferred for solar cells. We now show self-healing in mixed A+ HaPs. Specifically, if at least 15 atom % of the methylammonium (MA+) A cation is substituted for by guanidinium (Gua+) or acetamidinium (AA+), then the self-healing rate after damage is enhanced. In contrast, replacing MA+ with dimethylammonium (DMA+), comparable in size to Gua+ or AA+, does not alter this rate. Based on the times for self-healing, we infer that the rate-determining step involves short-range diffusion of A+ and/or Pb2+ cations and that the self …

The invention of X-ray interferometers has led to advanced phase-sensing devices that are invaluable in various applications. These include the precise measurement of universal constants, e.g. the Avogadro number, of lattice parameters of perfect crystals, and phase-contrast imaging, which resolves details that standard absorption imaging cannot capture. However, the sensitivity and robustness of conventional X-ray interferometers are constrained by factors, such as fabrication precision, beam quality, and, importantly, noise originating from external sources or the sample itself. In this work, we demonstrate a novel X-ray interferometric method of phase measurement with enhanced immunity to various types of noise, by extending, for the first time, the concept of the SU(1,1) interferometer into the X-ray regime. We use a monolithic silicon perfect crystal device with two thin lamellae to generate correlated photon pairs via spontaneous parametric down-conversion (SPDC). Arrival time coincidence and sum-energy filtration allow a high-precision separation of the correlated photon pairs, which carry the phase information from orders-of-magnitude larger uncorrelated photonic noise. The novel SPDC-based interferometric method presented here is anticipated to exhibit enhanced immunity to vibrations as well as to mechanical and photonic noise, compared to conventional X-ray interferometers. Therefore, this SU(1,1) X-ray interferometer should pave the way to unprecedented precision in phase measurements, with transformative implications for a wide range of applications.

Topological superconductivity is a promising concept for generating fault-tolerant qubits. Early experimental studies looked at hybrid systems and doped intrinsic topological or superconducting materials at very low temperatures. However, higher critical temperatures are indispensable for technological exploitation. Recent angle-resolved photoemission spectroscopy results have revealed that superconductivity in the type-I Weyl semimetal—trigonal PtBi2 (t-PtBi2)—is located at the Fermi-arc surface states, which renders the material a potential candidate for intrinsic topological superconductivity. Here we show, using scanning tunnelling microscopy and spectroscopy, that t-PtBi2 presents surface superconductivity at elevated temperatures (5 K). The gap magnitude is elusive: it is spatially inhomogeneous and spans from 0 to 20 meV. In particular, the large gap value and the shape of the quasiparticle excitation …

Developing polymer electrolytes as an alternative to aprotic liquid electrolytes for lithium and sodium-ion batteries aims to enhance their safety, durability, and cost. Among these, polyethylene oxide (PEO) is a favorite choice due to its wide availability, excellent versatility, and mechanical properties. PEO:NaTFSI and PEO:NaFSI are stable and efficient ion-conducting solid polymer electrolytes compared to other PEO:NaX matrices (for instance, X=[PF6]-, [ClO4]-). We tested Na/PEO:NaTFSI/NVP cells at low temperatures (40C) and carried out a series of electrochemical measurements to extract vital performance metrics such as diffusion coefficient, transference number, conductivity, and activation energy. Our findings emphasize the important role of the anions’ nature in the properties of polymeric electrolytes like those based on PEO, in which there are strong interactions between the ions and the oxygen atoms …

The invention of X-ray interferometers has led to advanced phase-sensing devices that are invaluable in various applications. These include the precise measurement of universal constants, e.g. the Avogadro number, of lattice parameters of perfect crystals, and phase-contrast imaging, which resolves details that standard absorption imaging cannot capture. However, the sensitivity and robustness of conventional X-ray interferometers are constrained by factors, such as fabrication precision, beam quality, and, importantly, noise originating from external sources or the sample itself. In this work, we demonstrate a novel X-ray interferometric method of phase measurement with enhanced immunity to various types of noise, by extending, for the first time, the concept of the SU(1,1) interferometer into the X-ray regime. We use a monolithic silicon perfect crystal device with two thin lamellae to generate correlated photon pairs via spontaneous parametric down-conversion (SPDC). Arrival time coincidence and sum-energy filtration allow a high-precision separation of the correlated photon pairs, which carry the phase information from orders-of-magnitude larger uncorrelated photonic noise. The novel SPDC-based interferometric method presented here is anticipated to exhibit enhanced immunity to vibrations as well as to mechanical and photonic noise, compared to conventional X-ray interferometers. Therefore, this SU(1,1) X-ray interferometer should pave the way to unprecedented precision in phase measurements, with transformative implications for a wide range of applications.

Recent progress has boosted the resolving power of optical microscopies to spatial dimensions well below the diffraction limit. Yet, axial super-resolution and axial single-molecule localisation typically require more complicated implementations than their lateral counterparts. In the present work, we propose a simple solution for axial metrology by providing a multi-layered single-excitation, dual-emission test slide, in which axial distance is colour-encoded. Our test slide combines on a standard microscope coverslip substrate two flat, thin, uniform and brightly emitting fluorophore layers, separated by a nanometric transparent spacer layer having a refractive index close to a biological cell. The ensemble is sealed in an index-matched protective polymer. As a proof-of-principle, we estimate the light confinement resulting from evanescent-wave excitation in total internal reflection fluorescence (TIRF) microscopy. Our test sample permits, even for the non-expert user, a facile axial metrology at the sub-100-nm scale, a critical requirement for axial super-resolution, as well as near-surface imaging, spectroscopy and sensing.

Lytic replication is essential for persistent infection of Kaposi’s sarcoma-associated herpesvirus (KSHV) and the pathogenesis of related diseases, and many cellular pathways are hijacked by KSHV proteins to initiate and control the lytic replication of this virus. However, the mechanism involved in KSHV lytic replication from the early to the late phases remains largely undetermined. We previously revealed that KSHV open reading frame 45 (ORF45) plays important roles in late transcription and translation. In the present study, we revealed that the Forkhead box proteins FoxK1 and FoxK2 are ORF45-binding proteins and are essential for KSHV lytic gene expression and virion production, and that depletion of FoxK1 or FoxK2 significantly suppresses the expression of many late viral genes. FoxK1 and FoxK2 directly bind to the promoters of several late viral genes, ORF45 augments the promoter binding and …

The invention of X-ray interferometers has led to advanced phase-sensing devices that are invaluable in various applications. These include the precise measurement of universal constants, e.g. the Avogadro number, of lattice parameters of perfect crystals, and phase-contrast imaging, which resolves details that standard absorption imaging cannot capture. However, the sensitivity and robustness of conventional X-ray interferometers are constrained by factors, such as fabrication precision, beam quality, and, importantly, noise originating from external sources or the sample itself. In this work, we demonstrate a novel X-ray interferometric method of phase measurement with enhanced immunity to various types of noise, by extending, for the first time, the concept of the SU(1,1) interferometer into the X-ray regime. We use a monolithic silicon perfect crystal device with two thin lamellae to generate correlated photon pairs via spontaneous parametric down-conversion (SPDC). Arrival time coincidence and sum-energy filtration allow a high-precision separation of the correlated photon pairs, which carry the phase information from orders-of-magnitude larger uncorrelated photonic noise. The novel SPDC-based interferometric method presented here is anticipated to exhibit enhanced immunity to vibrations as well as to mechanical and photonic noise, compared to conventional X-ray interferometers. Therefore, this SU(1,1) X-ray interferometer should pave the way to unprecedented precision in phase measurements, with transformative implications for a wide range of applications.

Optical spectroscopy the measurement of electromagnetic spectra is fundamental to various scientific domains and serves as the building block of numerous technologies. Computational spectrometry is an emerging field that employs an array of photodetectors with different spectral responses or a single photodetector device with tunable spectral response, in conjunction with numerical algorithms, for spectroscopic measurements. Compact single photodetectors made from layered materials are particularly attractive, since they eliminate the need for bulky mechanical and optical components used in traditional spectrometers and can easily be engineered as heterostructures to optimize device performance. However, compact tunable photodetectors are typically nonlinear devices and this adds complexity to extracting optical spectra from the device response. Here, we report on the training of an artificial neural network (ANN) to recover the full nonlinear spectral photoresponse of a nonlinear problem of high dimensionality of a single GeSe-InSe p-n heterojunction device. We demonstrate the functionality of a calibrated spectrometer in the spectral range of 400-1100 nm, with a small device footprint of ~25X25 micrometers, and we achieve a mean reconstruction error of 0.0002 for the power-spectrum at a spectral resolution of 0.35 nm. Using our device, we demonstrate a solution to metamerism, an apparent matching of colors with different power spectral distributions, which is a fundamental problem in optical imaging.

The significant heterogeneity of Wilms’ tumors between different patients is thought to arise from genetic and epigenetic distortions that occur during various stages of fetal kidney development in a way that is poorly understood. To address this, we characterized the heterogeneity of alternative mRNA splicing in Wilms’ tumors using a publicly available RNAseq dataset of high-risk Wilms’ tumors and normal kidney samples. Through Pareto task inference and cell deconvolution, we found that the tumors and normal kidney samples are organized according to progressive stages of kidney development within a triangle-shaped region in latent space, whose vertices, or “archetypes,” resemble the cap mesenchyme, the nephrogenic stroma, and epithelial tubular structures of the fetal kidney. We identified a set of genes that are alternatively spliced between tumors located in different regions of latent space and found that many of these genes are associated with the Epithelial to Mesenchymal Transition (EMT) and muscle development. Using motif enrichment analysis, we identified putative splicing regulators, some of which are associated with kidney development. Our findings provide new insights into the etiology of Wilms’ tumors and suggest that specific splicing mechanisms in early stages of development may contribute to tumor development in different patients.

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The formation of stable interphases on the electrodes is crucial for rechargeable lithium (Li) batteries. However, next-generation high-energy batteries face challenges in controlling interphase formation due to the high reactivity and structural changes of electrodes, leading to reduced stability and slow ion transport, which accelerate battery degradation. Here, we report an approach to address these issues by introducing multicomponent grain-boundary-rich interphase that boosts the rapid transport of ions and enhances passivation toward prolonged lifespan. This is guided by fundamental principles of solid-state ionics and geological crystallization differentiation theory, achieved through improved solvation chemistry. Demonstrations showcase how the introduction of the interphase substantially impacts the Li-ion transport across the interphase and the electrode–electrolyte compatibility in cost-effective electrolyte …

Natural and anomalous diffusion are widely observed and used to explore causes and consequences of movement across organisms, resulting in extensive use of the mean and mean-squared displacement (MSD). Using high-resolution data from over 70 million localizations of young and adult free-ranging Barn Owls (\textit{Tyto alba}), we demonstrate the necessity of a broad spectrum of displacement moments to characterize bird movement across scales. The mean and MSD -- interchangeable with moments and 2 -- are insufficient special cases. We reveal empirical strong anomalous diffusion as a nonlinear growth of displacement moments according to . The moment spectrum function displays piecewise linearity with a critical moment marking the crossover point between two scaling regimes, linked to a combination of age-specific behavioral modes. A critical timescale of five minutes marks an unexpected transition from a convex to a concave , related to environmental and behavioral constraints. Using two stochastic models of varying ecological complexity, we demonstrate that strong anomalous diffusion may be widespread in animal movement, underscoring the importance of expanding analysis beyond the average and MSD.

Methods: A total of 103 wild-type (WT) mice were injected with cobalt chloride by two routes in different concentrations: single intravenous (IV) high or low doses (total, n= 43); or daily repeated intraperitoneal (IP) high (three days) or low (28 days, 56 days) dose, and low-dose cobalt with added minocycline (56 days)(total, n= 60); 10 WT mice served as a control group. An additional group of 17 immunodeficient NOD scid gamma (NSG) mice were injected IV or IP with cobalt, and 10 NSG mice served as control. Cobalt levels were measured in blood, urine, and tears by particle-induced X-ray emission (PIXE). Macroscopic, immunohistochemical, electroretinography (ERG), and molecular studies were done. Results: PIXE revealed cobalt elimination from the blood by two hours, with increased levels in urine but under the detection limit in tears. In the retina, ERG recordings showed decreased b-wave amplitude. Apoptosis mainly involved the inner retina, with inner retinal inflammatory reaction in both WT and less in the NSG mice. In the optic nerves, an increased microglial and astrocytic activation was noted. Conclusions: This study demonstrated functional visual impairment with extensive inflammatory reaction secondary to cobalt toxicity in mice.

The development of efficient electrolytes is crucial for advancing magnesium (Mg) batteries, which hold promise for next-generation energy storage systems. Previously, electrolytes such as [Mg2(µ-Cl)3•6THF]+ [Ph4Al]-, A, and [Mg2(µ-Cl)3•6THF]+ [Ph3AlCl]-, B, have been studied, but their performance has been limited by issues related to ion dissociation and electrochemical stability. In this study, we report the synthesis of novel electrolytes by introducing polydentate ligands to these known systems, leading to the formation of [DME•MgCl•3THF]+ [Ph4Al]- 1 and [DG•MgCl•2THF]+ [Ph4Al]- 2, [Mg•3DME]2+ [Ph3AlCl-]2 3 and [Mg•2DG]2+ [Ph3AlCl-]2 4. These firstly discovered compounds were thoroughly characterized using X-ray crystallography and NMR spectroscopy. Our findings reveal that the choice of counter anion plays a pivotal role in the products and mechanism of the dissociation of the bridged [Mg2(µ-Cl)3•6THF]+ cation upon the addition of polydentate ligands. Specifically, with the [Ph4Al]- counter anion (precursor A), the dissociation results in a [MgCl]+ mono-cation, while with the [Ph3AlCl]- counter anion (precursor B), a [Mg]2+ divalent cation is formed. The resultant MgCl2 byproduct enhances solubility, expands electrochemical windows, and improves cyclic stability, leading to superior electrochemical performance of the new electrolytes (1, 2, 3, and 4) compared to the original precursors. These insights offer valuable guidelines for the design and synthesis of advanced electrolytes for rechargeable magnesium batteries, potentially paving the way for more efficient and stable energy storage solutions.

The development of efficient electrolytes is crucial for advancing magnesium (Mg) batteries, which hold promise for next-generation energy storage systems. Previously, electrolytes such as [Mg2(µ-Cl)3•6THF]+ [Ph4Al]-, A, and [Mg2(µ-Cl)3•6THF]+ [Ph3AlCl]-, B, have been studied, but their performance has been limited by issues related to ion dissociation and electrochemical stability. In this study, we report the synthesis of novel electrolytes by introducing polydentate ligands to these known systems, leading to the formation of [DME•MgCl•3THF]+ [Ph4Al]- 1 and [DG•MgCl•2THF]+ [Ph4Al]- 2, [Mg•3DME]2+ [Ph3AlCl-]2 3 and [Mg•2DG]2+ [Ph3AlCl-]2 4. These firstly discovered compounds were thoroughly characterized using X-ray crystallography and NMR spectroscopy. Our findings reveal that the choice of counter anion plays a pivotal role in the products and mechanism of the dissociation of the bridged [Mg2(µ-Cl)3•6THF]+ cation upon the addition of polydentate ligands. Specifically, with the [Ph4Al]- counter anion (precursor A), the dissociation results in a [MgCl]+ mono-cation, while with the [Ph3AlCl]- counter anion (precursor B), a [Mg]2+ divalent cation is formed. The resultant MgCl2 byproduct enhances solubility, expands electrochemical windows, and improves cyclic stability, leading to superior electrochemical performance of the new electrolytes (1, 2, 3, and 4) compared to the original precursors. These insights offer valuable guidelines for the design and synthesis of advanced electrolytes for rechargeable magnesium batteries, potentially paving the way for more efficient and stable energy storage solutions.

Mathematical models of voltammetric experiments commonly contain a singular point value for the reversible potential, whereas experimental data for surface-confined redox-active species is often interpreted to contain thermodynamic dispersion, meaning the population of molecules on the electrode possess a distribution of reversible potential values. Large amplitude ramped Fourier Transformed Alternating Current Voltammetry (FTacV), a technique in which a sinusoidal potential-time oscillation is overlaid onto a linear potential-time ramp, is known to provide access to higher order harmonic components that are largely devoid of non-Faradaic current. Initially, a theoretical study reveals that the use of very large amplitude sinusoidal oscillations reduces the apparent effects of thermodynamic dispersion; conversely, frequency can be varied to change the sensitivity of the measurement to kinetic dispersion. Subsequently, FTacV measurements are used to probe a highly thermodynamically dispersed surface-confined ferrocene derivative attached to a glassy carbon electrode, with amplitudes ranging from 25 to 300 mV and low frequency, which minimises the impact of kinetic dispersion. The results from the experimental study validate the theoretical predictions, demonstrating that we can vary the amplitude in FTacV experiments to tune in and out of thermodynamic dispersion.

Digital holographic microscopy (DHM) is a very popular interferometric technique for quantitative phase imaging (QPI). In DHM, an interferometer is combined with a microscope to create interference between an imaging beam containing information about the analysed sample and a clear reference beam carrying no sample information. To exploit the capability of reference beam in terms of useful sample information, we have recently proposed Cepstrum-based Interferometric Microscopy (CIM) [Opt. Las. Tech. 174, 110,626 (2024)] as a novel methodology involving the interference of two imaging beams carrying different sample information and to accurately retrieve quantitative phase data of both beams. In the earlier implementation, proof-of-concept of CIM was demonstrated for a Michelson-based layout requiring manual adjustments during the CIM methodology and validated only for low numerical aperture (NA …