BINA

This review focuses on the application of nuclear magnetic resonance (NMR) spectroscopy in the study of lithium and sodium battery electrolytes. Lithium-ion batteries are widely used in electronic devices, electric vehicles, and renewable energy systems due to their high energy density, long cycle life, and low self-discharge rate. The sodium analog is still in the research phase, but has significant potential for future development. In both cases, the electrolyte plays a critical role in the performance and safety of these batteries. NMR spectroscopy provides a non-invasive and non-destructive method for investigating the structure, dynamics, and interactions of the electrolyte components, including the salts, solvents, and additives, at the molecular level. This work attempts to give a nearly comprehensive overview of the ways that NMR spectroscopy, both liquid and solid state, has been used in past and present studies …

Rechargeable magnesium batteries (RMBs) have the potential to contribute towards alternative energy storage due to their low cost, high abundance, dendrites free deposition of Mg and high volumetric energy density. Organometallic complex-based electrolytes in ethereal solutions have been extensively studied in the context of RMBs due to their ability to facilitate highly reversible magnesium deposition in rechargeable magnesium batteries, while demonstrating wide enough electrochemical stability windows. However, these solutions containing unique mixture of organo-halo aluminate complexes have detrimental effect on the anodic stability of metallic current collectors for cathodes, like Ni and Al foils. In this work, we were able to synthesize and isolate Mg 2 Cl 3 (THF) 6 Ph 2 AlCl 2/THF electrolyte as the sole electroactive species using simple precursors: Ph 2 AlCl and MgCl 2 in THF, via atom efficient mono …

With an increasing demand for high-energy-density lithium-ion batteries (LIBs), nickel-rich cathodes such as LiNi0.9Mn0.05Co0.05O2 (NMC90) have gained significant interest due to their relatively low cobalt and high specific energy. However, cycling stability is compromised due to parasitic reactions at the electrode–electrolyte interfaces of NMC90. Herein, we demonstrate improved electrochemical properties of NMC90 using di-tert-butylmethyl adamantoyl silane (RSiCOAd: R is tBu(CH3)2 and Ad is 1-Ad) as an additive in a commercial electrolyte. Upon detailed electrochemical and spectroscopic analysis, we demonstrate that the RSiCOAd additive undergoes in situ decomposition to form a fluorinated organosiloxane passivation layer on the NMC90 surface and enhanced fluorination on the lithium anode surface. This phenomenon could significantly mitigate the parasitic reactions at the cathode–electrolyte …

We investigate a quantum walk on a ring represented by a directed triangle graph with complex edge weights and monitored at a constant rate until the quantum walker is detected. To this end, the first hitting time statistics is recorded using unitary dynamics interspersed stroboscopically by measurements, which is implemented on IBM quantum computers with a midcircuit readout option. Unlike classical hitting times, the statistical aspect of the problem depends on the way we construct the measured path, an effect that we quantify experimentally. First, we experimentally verify the theoretical prediction that the mean return time to a target state is quantized, with abrupt discontinuities found for specific sampling times and other control parameters, which has a well-known topological interpretation. Second, depending on the initial state, system parameters, and measurement protocol, the detection probability can be less than one or even zero, which is related to dark-state physics. Both, return-time quantization and the appearance of the dark states are related to degeneracies in the eigenvalues of the unitary time evolution operator. We conclude that, for the IBM quantum computer under study, the first hitting times of monitored quantum walks are resilient to noise. Yet, finite resolution effects lead to new topological, chirality, and broadening effects, which disappear in the asymptotic theory with an infinite number of measurements. Our results point the way for the development of novel quantum walk algorithms that exploit measurement-induced effects on quantum computers.

Hard x-ray imaging is indispensable across diverse fields owing to its high penetrability. However, the resolution of traditional x-ray imaging modalities, such as computed tomography (CT) systems, is constrained by factors including beam properties, the absence of optical components, and detection resolution. As a result, typical resolution in commercial imaging systems is limited to a few hundred microns. This study advances high-photon-energy imaging by extending the concept of computational ghost imaging to multipixel ghost imaging with x-rays. We demonstrate a remarkable enhancement in resolution from 500 microns to approximately 20 microns for an image spanning 0.9 by 1 cm^2, comprised of 400,000 pixels and involving only 1000 realizations. Furthermore, we present a high-resolution CT reconstruction using our method, revealing enhanced visibility and resolution. Our achievement is facilitated by an innovative x-ray lithography technique and the computed tiling of images captured by each detector pixel. Importantly, this method can be scaled up for larger images without sacrificing the short measurement time, thereby opening intriguing possibilities for noninvasive high-resolution imaging of small features that are invisible with the present modalities.

Biofilms comprising sessile microorganisms attached to surfaces are increasingly researched for their importance in medicine and industry. Current studies focus on development of antibiotics that unfortunately can lead to resistance and environmental pollution. Phosphonium cations are known to exhibit significant activity with less resistance. Here, silane-phosphonium thin coatings are applied by Stöber polymerization of new silane-phosphonium monomer onto oxidized polypropylene film to eliminate phosphonium leaching and reduce the risk of environmental pollution. The composition and morphology were investigated by infrared spectroscopy, X-ray photoelectron spectroscopy, atomic force microscopy and contact angle measurements. Coating durability was assessed by adhesion test. The significant anti-biofilm activity against S. aureus and E. coli suggests applications in medicine and agriculture.

Phase retardation is a cornerstone of modern optics, yet, at mid-infrared (mid-IR) frequencies, it remains a major challenge due to the scarcity of simultaneously transparent and birefringent crystals. Most materials resonantly absorb due to lattice vibrations occurring at mid-IR frequencies, and natural birefringence is weak, calling for hundreds of microns to millimeters-thick phase retarders for sufficient polarization rotation. Here, we demonstrate mid-IR phase retardation with flakes of α-MoO3 that are more than ten times thinner than the operational wavelength, achieving 90 degrees polarization rotation within one micrometer of material. We report conversion ratios above 50% in reflection or transmission mode, and wavelength tunability by several micrometers. Our results showcase that exfoliated flakes of low-dimensional crystals can serve as a platform for mid-IR miniaturized integrated low-loss polarization control.

Rechargeable magnesium batteries (RMBs) have the potential to contribute towards alternative energy storage due to their low cost, high abundance, dendrites free deposition of Mg and high volumetric energy density. Organometallic complex-based electrolytes in ethereal solutions have been extensively studied in the context of RMBs due to their ability to facilitate highly reversible magnesium deposition in rechargeable magnesium batteries, while demonstrating wide enough electrochemical stability windows. However, these solutions containing unique mixture of organo-halo aluminate complexes have detrimental effect on the anodic stability of metallic current collectors for cathodes, like Ni and Al foils. In this work, we were able to synthesize and isolate Mg2Cl3(THF)(6)Ph2AlCl2/THF electrolyte as the sole electroactive species using simple precursors: Ph2AlCl and MgCl2 in THF, via atom efficient mono …

The fogging of transparent surfaces—condensation of water vapor in the air to a small liquid surface at specific environmental conditions—scatters incident light, creating a blurry vision. Fogging presents a significant challenge in various industries, adversely affecting numerous applications including plastic packaging, agricultural films, and various optical devices. Superhydrophobic or superhydrophilic coatings are the main strategies used to induce antifogging to minimize light scattering. Here, an innovative approach is introduced to mitigate fogging by modifying the surface properties of polymeric films, focusing on corona-treated polyethylene as a model. Coatings were prepared in two successive steps: the addition of radical co-polymerization of methacryloxypropyltriethoxysilane and N-vinylpyrrolidone followed by the step-growth Stöber polymerization of the formed silane monomer. The polymeric dispersion was spread on oxidized films via a Mayer rod and dried. Scanning and force microscopy, FIB, XPS, and UV-vis spectroscopy revealed a thin coating composed of cross-linked siloxane (Si-O-Si) covalently bonded to surface hydroxyls exposing pyrrolidone groups. Contact angle measurements, hot-fog examination, and durability tests indicated a durable antifogging activity.

Extracellular vesicles (EVs), through their complex cargo, can reflect the state of their cell of origin and change the functions and phenotypes of other cells. These features indicate strong biomarker and therapeutic potential and have generated broad interest, as evidenced by the steady year‐on‐year increase in the numbers of scientific publications about EVs. Important advances have been made in EV metrology and in understanding and applying EV biology. However, hurdles remain to realising the potential of EVs in domains ranging from basic biology to clinical applications due to challenges in EV nomenclature, separation from non‐vesicular extracellular particles, characterisation and functional studies. To address the challenges and opportunities in this rapidly evolving field, the International Society for Extracellular Vesicles (ISEV) updates its ‘Minimal Information for Studies of Extracellular Vesicles’, which …

Water pollution caused by hazardous substances, particularly heavy metal (HM) ions, poses a threat to human health and the environment. Traditional methods for measuring HM in water are expensive and time-consuming and require extensive sample preparation. Therefore, developing robust, simple, and sensitive techniques for the detection and classification of HM is needed. We propose an optical approach that exploits the full scattering profile, meaning the angular intensity distribution, and utilizes the iso-pathlength (IPL) point. This point appears where the intensity is constant for different scattering coefficients, while the absorption coefficient is set. The absorption does not affect the IPL point position, it only reduces its intensity. In this paper, we explore the wavelength influence on the IPL point both in Monte Carlo simulations and experimentally. Next, we present the characterization of ferric chloride (FeCl2 …

Biofilms comprising sessile microorganisms attached to surfaces are increasingly researched for their importance in medicine and industry. Current studies focus on development of antibiotics that unfortunately can lead to resistance and environmental pollution. Phosphonium cations are known to exhibit significant activity with less resistance. Here, silane-phosphonium thin coatings are applied by Stöber polymerization of new silane-phosphonium monomer onto oxidized polypropylene film to eliminate phosphonium leaching and reduce the risk of environmental pollution. The composition and morphology were investigated by infrared spectroscopy, X-ray photoelectron spectroscopy, atomic force microscopy and contact angle measurements. Coating durability was assessed by adhesion test. The significant anti-biofilm activity against S. aureus and E. coli suggests applications in medicine and agriculture.

Gonadal sex determination in mice is a complex and dynamic process, which is crucial for the development of functional reproductive organs. The expression of genes involved in this process is regulated by a variety of genetic and epigenetic mechanisms. Recently, there has been increasing evidence that transposable elements (TEs), which are a class of mobile genetic elements, play a significant role in regulating gene expression during embryogenesis and organ development. In this study, we aimed to investigate the involvement of TEs in the regulation of gene expression during mouse embryonic gonadal development. Through bioinformatics analysis, we aimed to identify and characterize specific TEs that operate as regulatory elements for sex-specific genes, as well as their potential mechanisms of regulation. We identified TE loci expressed in a time- and sex-specific manner along fetal gonad development that correlate positively and negatively with nearby gene expression, suggesting that their expression is integrated to the gonadal regulatory network. Moreover, chromatin accessibility and histone post-transcriptional modification analyses in differentiating supporting cells revealed that TEs are acquiring a sex-specific signature for promoter-, enhancer-, and silencer-like elements, with some of them being proximal to critical sex-determining genes. Altogether, our study introduces TEs as the new potential players in the gene regulatory network that controls gonadal development in mammals.

We propose a method to extract the upper laser level’s (ULL’s) excess electronic temperature from the analysis of the maximum light output power (P max) and current dynamic range ΔJ d = (J max − J th) of terahertz quantum cascade lasers (THz QCLs). We validated this method, both through simulation and experiment, by applying it on THz QCLs supporting a clean three-level system. Detailed knowledge of electronic excess temperatures is of utmost importance in order to achieve high temperature performance of THz QCLs. Our method is simple and can be easily implemented, meaning an extraction of the excess electron temperature can be achieved without intensive experimental effort. This knowledge should pave the way toward improvement of the temperature performance of THz QCLs beyond the state-of-the-art.

The development of new nanoparticle-based antibiotics with biocompatible properties is an emerging advance in nanotechnology. This study advocated the development of carbon dots (CDs) doped with nitrogen, nitrogen with sulfur, and nitrogen with boron (N, NS, and NB-CDs). This led to changes in the properties of the CDs, both chemically and biologically. A facile hydrothermal technique was used to synthesize CDs and the formation of CDs was confirmed through various analytical techniques. The CDs had sizes ranging from 3.2 – 4.8 nm and ζ-potential values of +13 to 27 mV. The doped CDs exhibited moderate changes in fluorescence behaviors depending on the excitation wavelength (λex). The N- and NB-doped CDs were effective at eliminating gram-negative pathogens (E. coli and K. pneumoniae), with minimum inhibitory concentrations (MIC) of 300 µg/mL and 400 µg/mL, respectively. The …

We introduce a novel time-energy uncertainty relationship within the context of restarts in monitored quantum dynamics. Initially, we investigate the concept of ``first hitting time'' in quantum systems using an IBM quantum computer and a three-site ring graph as our starting point. Previous studies have established that the mean recurrence time, which represents the time taken to return to the initial state, is quantized as an integer multiple of the sampling time, displaying pointwise discontinuous transitions at resonances. Our findings demonstrate that, the natural utilization of the restart mechanism in laboratory experiments, driven by finite data collection time spans, leads to a broadening effect on the transitions of the mean recurrence time. Our newly proposed uncertainty relation captures the underlying essence of these phenomena, by connecting the broadening of the mean hitting time near resonances, to the intrinsic energies of the quantum system and to the fluctuations of recurrence time. This work not only contributes to our understanding of fundamental aspects related to quantum measurements and dynamics, but also offers practical insights for the design of efficient quantum algorithms with mid-circuit measurements.

Rechargeable Mg‐ion Batteries (RMB) containing a Mg metal anode offer the promise of higher specific volumetric capacity, energy density, safety, and economic viability than lithium‐ion battery technology, but their realization is challenging. The limited availability of suitable inorganic cathodes compatible with electrolytes relevant to Mg metal anode restricts the development of RMBs. Despite the promising capability of some oxides to reversibly intercalate Mg+2 ions at high potential, its lack of stability in chloride‐containing ethereal electrolytes, relevant to Mg metal anode hinders the realization of a full practical RMB. Here the successful in situ encapsulation of monodispersed spherical V2O5 (≈200 nm) is demonstrated by a thin layer of VS2 (≈12 nm) through a facile surface reduction route. The VS2 layer protects the surface of V2O5 particles in RMB electrolyte solution (MgCl2 + MgTFSI in DME). Both V2O5 …

MolOptimizer is a user-friendly computational toolkit designed to streamline the hit-to-lead optimization process in drug discovery. MolOptimizer extracts features and trains machine learning models using a user-provided, labeled, and small-molecule dataset to accurately predict the binding values of new small molecules that share similar scaffolds with the target in focus. Hosted on the Azure web-based server, MolOptimizer emerges as a vital resource, accelerating the discovery and development of novel drug candidates with improved binding properties.

The development of durable platinum-group-metal-free oxygen reduction reaction (ORR) catalysts is a key research direction for enabling the wide use of fuel cells. Here, we use a combination of experimental measurements and density functional theory calculations to study the activity and durability of seven iron-based metallophthalocyanine (MPc) ORR catalysts that differ only in the identity of the substituent groups on the MPcs. While the MPcs show similar ORR activity, their durabilities as measured by the current decay half-life differ greatly. We find that the energy difference between the hydrogenated intermediate structure and the final demetalated structure (ΔEdemetalation) of the MPcs is linearly related to the degradation reaction barrier energy. Comparison to the degradation data for the previously studied metallocorrole systems suggested that ΔEdemetalation also serves as a descriptor for the corrole …

Membrane protein biogenesis poses acute challenges to protein homeostasis, and how they are selectively escorted to the target membrane is not well understood. Here we address this question in the guided-entry-of-tail-anchored protein (GET) pathway, in which tail-anchored membrane proteins (TAs) are relayed through an Hsp70-Sgt2-Get3 chaperone triad for targeting to the endoplasmic reticulum. We show that the Hsp70 ATPase cycle and TA substrate drive dimeric Sgt2 from a wide-open conformation to a closed state, in which TAs are protected by both substrate binding domains of Sgt2. Get3 is privileged to receive TA from closed Sgt2, whereas off-pathway chaperones remove TAs from open Sgt2. Sgt2 closing is less favorable with suboptimal GET substrates, which are rejected during or after the Hsp70-to-Sgt2 handover. Our results demonstrate how fine-tuned conformational dynamics in Sgt2 enable …

A major hypothesis for the etiology of type 1 diabetes (T1D) postulates initiation by viral infection, leading to double-stranded RNA (dsRNA)-mediated interferon response and inflammation; however, a causal virus has not been identified. Here, we use a mouse model, corroborated with human islet data, to demonstrate that endogenous dsRNA in beta cells can lead to a diabetogenic immune response, thus identifying a virus-independent mechanism for T1D initiation. We found that disruption of the RNA editing enzyme adenosine deaminases acting on RNA (ADAR) in beta cells triggers a massive interferon response, islet inflammation, and beta cell failure and destruction, with features bearing striking similarity to early-stage human T1D. Glycolysis via calcium enhances the interferon response, suggesting an actionable vicious cycle of inflammation and increased beta cell workload.