BINA

Surfaces of classical spherical liquid droplets are isotropic, promoting the random distribution of surface-adsorbed molecules. Here we demonstrate a counterintuitive temperature-controlled self-assembly of well-defined and highly ordered patterns of surface-adsorbed fluorescent molecules on the surfaces of water-suspended spherical oil droplets. These patterns are induced by precisely self-positioned, topology-dictated structural defects in a crystalline monolayer covering these droplets’ surfaces over a wide temperature range. We elucidate the pattern formation mechanism, visualize the defects’ positions and map the stress fields within the surface crystal. The observed phenomena provide insights into the interfacial freezing effect on curved surfaces, enable precise positioning of functional ligands on droplets for their self-assembly into higher-hierarchy structures– and may also play an important role in vital …

Bromine complexing agents (BCAs) are seen as a promising route to mitigate the potential health and environmental risks of the bromine-based redox-flow batteries, like the hydrogen bromine redox flow battery (H2–Br2 RFB). The most studied BCAs are based on the pyridinium anion, which may adsorb and inhibit the Pt catalyst required in the H2–Br2 RFB system for the hydrogen reactions. Herein the effect of two BCAs (ethyl-pyridinium bromide and hexyl-pyridinium bromide) on a Pt electrocatalyst are studied, along with a potential methodology to prevent adsorption of the BCA through a polydopamine (PDA) coating. The results show that the pyridinium anion is adsorbed on Pt throughout a large potential range (−0.02 to 1.0 V), reducing the availability of the surface for the adsorption of other species. The PDA coating prevented this adsorption, but itself experiences adsorption of the BCA leading to some …

Extreme value (EV) statistics of correlated systems are widely investigated in many fields, spanning the spectrum from weather forecasting to earthquake prediction. Does the unavoidable discrete sampling of a continuous correlated stochastic process change its EV distribution? We explore this question for correlated random variables modeled via Langevin dynamics for a particle in a potential field. For potentials growing at infinity faster than linearly and for long measurement times, we find that the EV distribution of the discretely sampled process diverges from that of the full continuous dataset and converges to that of independent and identically distributed random variables drawn from the process’s equilibrium measure. However, for processes with sublinear potentials, the long-time limit is the EV statistics of the continuously sampled data. We treat processes whose equilibrium measures belong to the three EV …

The goal of the experiment was to investigate higher-order X-ray-optical sum-frequency generation (XSFG) as a means to study the dynamics of linear and nonlinear optically-induced local polarization effects in solids with Angstrom resolution. XSFG can be used as time-resolved atomic-scale probe of the dynamics of optically induced charge densities. The ability to optically control carrier dynamics in samples at the microscopic scale has the potential to become the basis of ultrafast optical switching of currents and future petahertz optoelectronic devices.

We investigate a tight binding quantum walk on a graph. Repeated stroboscopic measurements of the position of the particle yield a measured "trajectory", and a combination of classical and quantum mechanical properties for the walk are observed. We explore the effects of the measurements on the spreading of the packet on a one dimensional line, showing that except for the Zeno limit, the system converges to Gaussian statistics similarly to a classical random walk. A large deviation analysis and an Edgeworth expansion yield quantum corrections to this normal behavior. We then explore the first passage time to a target state using a generating function method, yielding properties like the quantization of the mean first return time. In particular, we study the effects of certain sampling rates which cause remarkable change in the behavior in the system, like divergence of the mean detection time in finite systems and a decomposition of the phase space into mutually exclusive regions, an effect that mimics ergodicity breaking, whose origin here is the destructive interference in quantum mechanics. For a quantum walk on a line we show that in our system the first detection probability decays classically like , this is dramatically different compared to local measurements which yield a decay rate of , indicating that the exponents of the first passage time depends on the type of measurements used.

Surfaces of classical spherical liquid droplets are isotropic, promoting the random distribution of surface-adsorbed molecules. Here we demonstrate a counterintuitive temperature-controlled self-assembly of well-defined and highly ordered patterns of surface-adsorbed fluorescent molecules on the surfaces of water-suspended spherical oil droplets. These patterns are induced by precisely self-positioned, topology-dictated structural defects in a crystalline monolayer covering these droplets’ surfaces over a wide temperature range. We elucidate the pattern formation mechanism, visualize the defects’ positions and map the stress fields within the surface crystal. The observed phenomena provide insights into the interfacial freezing effect on curved surfaces, enable precise positioning of functional ligands on droplets for their self-assembly into higher-hierarchy structures– and may also play an important role in vital …

Single Nucleotide Polymorphism markers (SNPs) have great potential to identify individuals, family relations, biogeographical ancestry, and phenotypic traits. In many forensic situations DNA mixtures of a victim and an unknown suspect exist. Extracting from such samples the suspect's SNP profile can be used to assist investigation and gather intelligence. Computational tools to determine inclusion/exclusion of a known individual from a mixture exist, but no algorithm to extract an unknown SNP profile without a list of suspects is available. We present here AH-HA, a novel computational approach for extracting an unknown SNP profile from a whole genome sequencing (WGS) of a two person mixture. It utilizes techniques similar to the ones used in haplotype phasing. It constructs the inferred genotype as an imperfect mosaic of haplotypes from a reference panel of the target population. It is shown to outperform more simplistic approaches, maintaining high performance through a wide range of sequencing depths (500x-5x). AH-HA can be applied in cases of victim-suspect mixtures and improve the capabilities of the investigating forces. This approach can be extended to more complex mixtures, with more donors and less prior information, further motivating the development of SNP based forensics technologies.

Ni-rich LiNi1–x–yCoxMnyO2 (1 – x – y > 0.5) (NCMs) cathode materials have shown great promise in energy-intensive applications, such as electric vehicles. However, as many layered cathodes do, they suffer from structural and electrochemical degradation during cycling. In this study, we show that Nd- and Y-doped materials, Li(Ni0.85Co0.1Mn0.05)0.995Nd0.005O2 and Li(Ni0.85Co0.1Mn0.05)0.995Y0.005O2, have significantly better structural, electrochemical, and thermal properties compared to the reference LiNi0.85Co0.1Mn0.05O2 (NCM85) due to enhanced structural stability. The doped electrodes were found to have significantly higher specific discharge capacities, better capacity retention, and lower voltage hysteresis compared to the reference (undoped) electrodes. SEM images of the focused-ion beam (FIB) cut of the particles of the doped material showed that they have less cracks when compared …

Considering the global spread of bacterial infections, the development of anti-biofilm surfaces with high antimicrobial activities is highly desired. This work unraveled a simple, sonochemical method for coating Cu2O nanoparticles (NPs) on three different flexible substrates: polyester (PE), nylon 2 (N2), and polyethylene (PEL). The introduction of Cu2O NPs on these substrates enhanced their surface hydrophobicity, induced ROS generation, and completely inhibited the growth of sensitive (Escherichia coli and Staphyloccocus aureus) and drug-resistant (MDR E. coli and MRSA) planktonic and biofilm. The experimental results confirmed that Cu2O-PE exhibited complete biofilm mass reduction ability for all four strains, whereas Cu2O-N2 showed more than 99% biomass inhibition against both drug-resistant and sensitive pathogens in 6 h. Moreover, Cu2O-PEL also indicated a 99.95, 97.73, 98.00, and 99.20 …

Here, we report a simple route of synthesizing bulk layered TiS2 via chemical vapor transport (CVT) using non-toxic inorganic precursors, followed by successful isolation of few-layered TiS2 flakes using high-frequency-based liquid-phase exfoliation. Exfoliated TiS2 flakes exhibit significantly enhanced photocatalytic activity towards the degradation of tetracycline hydrochloride (TCH) under simulated solar light irradiation, achieving ~ 95% degradation efficiency with its reaction rate constants six times higher than that of the bulk counterpart. The underlying degradation mechanism can be attributed to the fully exposed reactive sites originating from the well-defined layered structure. Trapping experiments coupled with electron paramagnetic resonance (EPR) measurements confirm the generation of electrons and hydroxyl radicals as major active species. The photodegradation pathway and intermediates of TCH …

Ni-rich LiNi1–x–yCoxMnyO2 (1 – x – y > 0.5) (NCMs) cathode materials have shown great promise in energy-intensive applications, such as electric vehicles. However, as many layered cathodes do, they suffer from structural and electrochemical degradation during cycling. In this study, we show that Nd- and Y-doped materials, Li(Ni0.85Co0.1Mn0.05)0.995Nd0.005O2 and Li(Ni0.85Co0.1Mn0.05)0.995Y0.005O2, have significantly better structural, electrochemical, and thermal properties compared to the reference LiNi0.85Co0.1Mn0.05O2 (NCM85) due to enhanced structural stability. The doped electrodes were found to have significantly higher specific discharge capacities, better capacity retention, and lower voltage hysteresis compared to the reference (undoped) electrodes. SEM images of the focused-ion beam (FIB) cut of the particles of the doped material showed that they have less cracks when compared …

In this paper we explore the effects of nonadiabatic external driving on the dynamics of an electronic system coupled to two electronic leads and to a phonon mode, with and without damping. In the limit of slow driving, we establish nonadiabatic corrections to thermodynamic and transport quantities. In particular, we study the first-order correction to the work done by the driving, the charge current, and the vibrational excitation using a perturbative expansion. We then compare the results to the numerically exact hierarchical equations of motion (HEOM) approach. Furthermore, the HEOM analysis spans both the weak and strong system-bath coupling regime and the slow-and fast-driving limits. We show that the electronic friction and the nonadiabatic corrections to the charge current provide a clear indicator for the Franck-Condon effect and for nonresonant tunneling processes. We also discuss the validity of the …

In recent years, lignin has drawn increasing attention for different applications due to its intrinsic antibacterial and antioxidant properties, coupled with biodegradability and biocompatibility. However, chemical modification or combination with metals is usually required to increase its antimicrobial functionality and produce biobased added-value materials for applications wherein bacterial growth should be avoided, such as biomedical and food industries. In this work, a sonoenzymatic approach for the simultaneous functionalization and nanotransformation of lignin to prepare metal-free antibacterial phenolated lignin nanoparticles (PheLigNPs) is developed. The grafting of tannic acid, a natural phenolic compound, onto lignin was achieved by an environmentally friendly approach using laccase oxidation upon the application of high-intensity ultrasound to rearrange lignin into NPs. PheLigNPs presented higher …

The important phenomenon of electrical double layer (EDL) is often described by mathematical relations between surface charges, variation of electrostatic potentials with distance and distribution of ions across the interface between charged surfaces (or particles) and electrolyte solutions. A major advance was made in the last decade in understanding complex EDL relationships with an emphasis on nano-porous carbonaceous materials. These understandings were usually exploited for the interpretation of electro-sorption phenomena connected to capacitive deionization (CDI) processes. The aim of this short paper is to demonstrate, based on previous studies, how models of EDL in nano-porous carbons can be the basis for modification of carbonaceous materials for other applications, like sensors and energy extraction from salinity gradients.

Bromine complexing agents (BCAs) are seen as a promising route to mitigate the potential health and environmental risks of the bromine-based redox-flow batteries, like the hydrogen bromine redox flow battery (H2–Br2 RFB). The most studied BCAs are based on the pyridinium anion, which may adsorb and inhibit the Pt catalyst required in the H2–Br2 RFB system for the hydrogen reactions. Herein the effect of two BCAs (ethyl-pyridinium bromide and hexyl-pyridinium bromide) on a Pt electrocatalyst are studied, along with a potential methodology to prevent adsorption of the BCA through a polydopamine (PDA) coating. The results show that the pyridinium anion is adsorbed on Pt throughout a large potential range (−0.02 to 1.0 V), reducing the availability of the surface for the adsorption of other species. The PDA coating prevented this adsorption, but itself experiences adsorption of the BCA leading to some …

Levulinic acid (LA) is one of the top twelve chemicals listed by the US Department of Energy that can be derived from biomass. It serves as a building block and platform chemical for producing a variety of chemicals, fuels and materials which are currently produced in fossil based refineries. LA is a key strategic chemical, as fuel grade chemicals and plastic substitutes can be produced by its catalytic conversion. LA derivatisation to various product streams, such as alkyl levulinates via esterification, γ-valerolactone via hydrogenation and N-substituted pyrrolidones via reductive amination and many other transformations of commercial utility are possible owing to the two oxygen functionalities, namely, carbonyl and carboxyl groups, present within the same substrate. Various biomass feedstock, such as agricultural wastes, marine macroalgae, and fresh water microalgae were successfully converted to LA in high yields. Finding a substitute to mineral acid catalysts for the conversion of biomass to LA is a challenge. The use of an ultrasound technique facilitated the production of promising nano-solid acid catalysts including Ga salt of molybophosphoric acid and Ga deposited mordenite zeolite, with optimum amounts of Lewis and Bronsted acidities needed for the conversion of glucose to LA in high yields, being 56 and 59.9 wt.% respectively. Microwave irradiation technology was successfully utilized for the accelerated production of LA (53 wt.%) from glucose in a short duration of 6 min, making use of the unique synergistic catalytic activity of ZnBr2 and HCl.

Forward Brillouin point sensing is demonstrated in a multi-core fiber. Acoustic waves are stimulated by light in one core and monitored using a grating in another. Measurements distinguish between ethanol and water outside the cladding.

The environment humidity effects on performance of halide perovskites (HaPs), especially MAPbI3, are known. Nevertheless, it is hard to find direct experimental evidence of H2O in the bulk materials at the levels lower than that of Monohydrate (MAPbI3.H2O). Here, for the first time, direct experimental evidence of water being released from bulk (µm‐s deep) of MAPbI3 single crystal is reported. The thermogravimetric analysis coupled with mass spectrometry (TGA‐MS) of evolved gases is used to detect the MS signal of H2O from the penetrable depth and correlate it with the TGA mass loss due to H2O leaving the material. These measurements yield an estimate of the average H2O content of 1 H2O molecule per three MAPbI3 formula units (MAPbI3.0.33H2O). Under the relatively low temperature conditions no other evolved gases that can correspond to MAPbI3 decomposition products, are observed in the MS. In …

Ni-rich LiNi1–x–yCoxMnyO2 (1 – x – y > 0.5) (NCMs) cathode materials have shown great promise in energy-intensive applications, such as electric vehicles. However, as many layered cathodes do, they suffer from structural and electrochemical degradation during cycling. In this study, we show that Nd- and Y-doped materials, Li(Ni0.85Co0.1Mn0.05)0.995Nd0.005O2 and Li(Ni0.85Co0.1Mn0.05)0.995Y0.005O2, have significantly better structural, electrochemical, and thermal properties compared to the reference LiNi0.85Co0.1Mn0.05O2 (NCM85) due to enhanced structural stability. The doped electrodes were found to have significantly higher specific discharge capacities, better capacity retention, and lower voltage hysteresis compared to the reference (undoped) electrodes. SEM images of the focused-ion beam (FIB) cut of the particles of the doped material showed that they have less cracks when compared …

We show that a Bose–Einstein condensate consisting of dark excitons forms in GaAs coupled quantum wells at low temperatures. We find that the condensate extends over hundreds of micrometers, well beyond the optical excitation region, and is limited only by the boundaries of the mesa. We show that the condensate density is determined by spin-flipping collisions among the excitons, which convert dark excitons into bright ones. The suppression of this process at low temperature yields a density buildup, manifested as a temperature-dependent blueshift of the exciton emission line. Measurements under an in-plane magnetic field allow us to preferentially modify the bright exciton density and determine their role in the system dynamics. We find that their interaction with the condensate leads to its depletion. We present a simple rate-equations model, which well reproduces the observed temperature, power, and …

Various conditions cause dispersions of particulate matter to circulate inside the anterior chamber of a human eye. These dispersed particles might reduce visual acuity or promote elevation of intraocular pressure (IOP), causing secondary complications such as particle related glaucoma, which is a major cause of blindness. Medical and surgical treatment options are available to manage these complications, yet preventive measures are not currently available. Conceptually, manipulating these dispersed particles in a way that reduces their negative impact could prevent these complications. However, as the eye is a closed system, manipulating dispersed particles in it is challenging. Standing acoustic waves have been previously shown to be a versatile tool for manipulation of bioparticles from nano-sized extracellular vesicles up to millimeter-sized organisms. Here we introduce for the first time a novel method utilizing standing acoustic waves to noninvasively manipulate intraocular particles inside the anterior chamber. Using a cylindrical acoustic resonator, we show ex vivo manipulation of pigmentary particles inside porcine eyes. We study the effect of wave intensity over time and rule out temperature changes that could damage tissues. Optical coherence tomography and histologic evaluations show no signs of damage or any other side effect that could be attributed to acoustic manipulation. Finally, we lay out a clear pathway to how this technique can be used as a non-invasive tool for preventing secondary glaucoma. This concept has the potential to control and arrange intraocular particles in specific locations without causing any damage to …