BINA

Acoustic-directed assembly is a modular and flexible bottom-up technique with the potential to pattern a wide range of materials. Standing acoustic waves have been previously employed for patterning preformed metal particles, however, direct patterning of metallic structures from precursors remains unexplored. Here, we investigate utilization of standing waves to exert control over chemical reaction products, while also exploring their potential in the formation of multi-layered and composite micro-structures. Periodic metallic micro-structures were formed in a single step, simplifying microstructure fabrication. Concentric structures were obtained by introducing a metal precursor salt and a reducing agent into a cylindrical piezoelectric resonator that also served as a reservoir. In addition, we introduce an innovative approach to directly fabricate metallic multi-layer and composite structures by reducing different metal ions or adding nanoparticles during the reduction step. Fewer steps are needed, compared with other methods, and there is no need to stabilize the nanoparticles or to ensure chemical affinity between the metallic matrix and inorganic nanoparticles. This innovative approach is promising for production of complex microstructures with enhanced functionality and controlled properties.

The hexatic phase is an intermediate stage in the melting process of a 2D crystal due to topological defects. Recently, this exotic phase was experimentally identified in the vortex lattice of 2D weakly disordered superconducting MoGe by scanning tunneling microscopic measurements. Here we study this vortex state by the Nernst effect, which is an effective and sensitive tool to detect vortex motion, especially in the superconducting fluctuation regime. We find a surprising Nernst sign reversal at the melting transition of the hexatic phase. We propose that they are a consequence of vortex dislocations in the hexatic state which diffuse preferably from the cold to hot.

Weak values and Kirkwood--Dirac (KD) quasiprobability distributions have been independently associated with both foundational issues in quantum theory and advantages in quantum metrology. We propose simple quantum circuits to measure weak values, KD distributions, and spectra of density matrices without the need for post-selection. This is achieved by measuring unitary-invariant, relational properties of quantum states, which are functions of Bargmann invariants, the concept that underpins our unified perspective. Our circuits also enable experimental implementation of various functions of KD distributions, such as out-of-time-ordered correlators (OTOCs) and the quantum Fisher information in post-selected parameter estimation, among others. An upshot is a unified view of nonclassicality in all those tasks. In particular, we discuss how negativity and imaginarity of Bargmann invariants relate to set coherence.

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.

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.

Intraocular pressure (IOP) measurements comprise an essential tool in modern medicine for the early diagnosis of glaucoma, the second leading cause of human blindness. The world's highest prevalence of glaucoma is in low-income countries.Current diagnostic methods require experience in running expensive equipment as well as the use of anesthetic eye drops. We present herein a remote photonic IOP biomonitoring method based on deep learning of secondary speckle patterns, captured by a fast camera, that are reflected from eye sclera stimulated by an external sound wave. By combining speckle pattern analysis with deep learning, high precision measurements are possible.

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.

Immunoglobulins (IGs), critical components of the human immune system, are composed of heavy and light protein chains encoded at three genomic loci. The IG Kappa (IGK) chain locus consists of two large, inverted segmental duplications. The complexity of IG loci has hindered effective use of standard high-throughput methods for characterizing genetic variation within these regions. To overcome these limitations, we leverage long-read sequencing to create haplotype-resolved IGK assemblies in an ancestrally diverse cohort (n=36), representing the first comprehensive description of IGK haplotype variation at population-scale. We identify extensive locus polymorphism, including novel single nucleotide variants (SNVs) and a common novel ~24.7 Kbp structural variant harboring a functional IGKV gene. Among 47 functional IGKV genes, we identify 141 alleles, 64 (45.4%) of which were not previously curated. We report inter-population differences in allele frequencies for 14 of the IGKV genes, including alleles unique to specific populations within this dataset. Finally, we identify haplotypes carrying signatures of gene conversion that associate with enrichment of SNVs in the IGK distal region. These data provide a critical resource of curated genomic reference information from diverse ancestries, laying a foundation for advancing our understanding of population-level genetic variation in the IGK locus.

Nuclear forward scattering (NFS) is a synchrotron-based technique relying on the recoil-free nuclear resonance effect similar to Mössbauer spectroscopy. In this work, we introduce NFS for in situ and operando measurements during electrocatalytic reactions. The technique enables faster data acquisition and better discrimination of certain iron sites in comparison to Mössbauer spectroscopy. It is directly accessible at various synchrotrons to a broad community of researchers and applicable to multiple metal isotopes. We demonstrate the power of this technique with the hydrogen evolution mechanism of an immobilized iron porphyrin supported on carbon. Such catalysts are often considered as model systems for iron-nitrogen-carbon (FeNC) catalysts. Using in situ and operando NFS in combination with theoretical predictions of spectroscopic data enables the identification of the intermediate that is formed prior to the rate determining step. The conclusions on the reaction mechanism can be used for future optimization of immobilized molecular catalysts and metal-nitrogen-carbon (MNC) catalysts.

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 …

A critical current challenge in the development of all-solid-state lithium batteries (ASSLBs) is reducing the cost of fabrication without compromising the performance. Here we report a sulfide ASSLB based on a high-energy, Co-free LiNiO2 cathode with a robust outside-in structure. This promising cathode is enabled by the high-pressure O2 synthesis and subsequent atomic layer deposition of a unique ultrathin LixAlyZnzOδ protective layer comprising a LixAlyZnzOδ surface coating region and an Al and Zn near-surface doping region. This high-quality artificial interphase enhances the structural stability and interfacial dynamics of the cathode as it mitigates the contact loss and continuous side reactions at the cathode/solid electrolyte interface. As a result, our ASSLBs exhibit a high areal capacity (4.65 mAh cm−2), a high specific cathode capacity (203 mAh g−1), superior cycling stability (92% capacity retention …

Modulation of electronic properties of materials by electric fields is central to the operation of modern semiconductor devices, providing access to complex electronic behaviors and greater freedom in tuning the energy bands of materials. Here, we explore one-dimensional superlattices induced by a confining electrostatic potential in monolayer MoS, a prototypical two-dimensional semiconductor. Using first-principles calculations, we show that periodic potentials applied to monolayer MoS induce electrostatic superlattices in which the response is dominated by structural distortions relative to purely electronic effects. These structural distortions reduce the intrinsic band gap of the monolayer substantially while also polarizing the monolayer through piezoelectric coupling, resulting in spatial separation of charge carriers as well as Stark shifts that produce dispersive minibands. Importantly, these minibands inherit the valley-selective magnetic properties of monolayer MoS, enabling fine control over spin-valley coupling in MoS and similar transition-metal dichalcogenides.

Quantum tunneling (QT) is not an effect often considered in chemistry, and rightfully so. However, in many cases it is significant, and in some cases it is even considerable. In this chapter we will describe the basic tenets of QT with a focus on catalysis, followed by some of the most important tools to study and compute them. The chapter goes on to address the title of the chapter by discussing several clear cases of QT for hydrogen-based reactions in organometallic, enzymatic, astrochemical, and organic systems. The insights highlighted in the chapter showcase the importance of QT in specific catalyzed reactions and help uncover the instances that are worth of attention.

We present measurements of X-ray Parametric Down Conversion at the Advanced Photon Source synchrotron facility. Using an incoming pump beam at 22 keV, we observe the simultaneous, elastic emission of down-converted photon pairs generated in a diamond crystal. The pairs are detected using high count rate silicon drift detectors with low noise. Production by down-conversion is confirmed by measuring time-energy correlations in the detector signal, where photon pairs within an energy window ranging from 10 to 12 keV are only observed at short time differences. By systematically varying the crystal misalignment and detector positions, we obtain results that are consistent with the constant total of the down-converted signal. Our maximum rate of observed pairs was 130/hour, corresponding to a conversion efficiency for the down-conversion process of .

The non-Markovian continuous-time random walk model, featuring fat-tailed waiting times and narrow distributed displacements with a non-zero mean, is a well studied model for anomalous diffusion. Using an analytical approach, we recently demonstrated how a fractional space advection diffusion asymmetry equation, usually associated with Markovian L\'evy flights, describes the spreading of a packet of particles. Since we use Gaussian statistics for jump lengths though fat-tailed distribution of waiting times, the appearance of fractional space derivatives in the kinetic equation demands explanations provided in this manuscript. As applications we analyse the spreading of tracers in two dimensions, breakthrough curves investigated in the field of contamination spreading in hydrology and first passage time statistics. We present a subordination scheme valid for the case when the mean waiting time is finite and the variance diverges, which is related to L\'evy statistics for the number of renewals in the process.

Overcoming diffraction limit is crucial for obtaining high-resolution image and observing fine microstructure. With this conventional difficulty still puzzling us and the prosperous development of wave dynamics of light interacting with gravitational fields in recent years, how spatial curvature affect the diffraction limit is an attractive and important question. Here we investigate the issue of diffraction limit and optical resolution on two-dimensional curved spaces - surfaces of revolution (SORs) with constant or variable spatial curvature. We show that the diffraction limit decreases and resolution is improved on SORs with positive Gaussian curvature, opening a new avenue to super-resolution. The diffraction limit is also influenced by propagation direction, as well as the propagation distance in curved space with variable spatial curvature. These results provide a possible method to control optical resolution in curved space or equivalent waveguides with varying refractive index distribution and may allow one to detect the presence of non-uniform strong gravitational effect by probing locally the optical resolution.

In recent years, there has been a lot of interest in biodegradable surface-engineered iron oxide nanoparticles (IONPs) because they could be used in drug delivery and other biomedical fields. This chapter gives an overview of the current state of research on how to make biodegradable IONPs, how to engineer their surfaces, and how to make them work for drug delivery and other biomedical applications. Because these nanoparticles are biodegradable, they will break down and leave the body in a safe way, reducing worries about toxicity. Also, the surface of IONPs can be changed to make them more stable, biocompatible, and able to target specific cells or tissues. This makes it easier for drugs to get to where they need to go. The review talks about how natural polymers, peptides, and targeting ligands are used to change the surface, as well as how these changes affect the physicochemical properties and …

One of the most challenging tasks in analytical chemistry is the determination of the chirality (identi cation of an enantio-meric composition) in solids mainly because of the strict requirements of the pharmaceutical industry for enantiomerically pure drugs. Although there are a few methods available to accomplish enantio-differentiation in solids, for example: X-ray diffraction (XRD), differential scanning calorimetry (DSC), CD spectroscopy, and low-frequency (LF) Raman spectroscopy, this is still very challenging. In this work, we have developed a new method to measure the chirality of crystals, based on electron paramagnetic resonance (EPR) spectroscopy of chiral crystals doped with Cu2+ as the EPR active ion. Here, we demonstrate our approach using a model system of L-and DL-Histidine crystals doped with Cu2+. We show that EPR measurements of the Cu2+-doped Histidine crystals can accurately determine the chirality and enantiomeric composition of the crystals. We present a very preliminary example of this technique, and we hope that in the future it will be possible to re ne and develop this method for many other chiral organic crystal systems.

A universal methodology for coding-decoding the complex amplitude field of an imaged sample in coherent microscopy is presented, where no restrictions on any of the two interferometric beams are required. Thus, the imaging beam can be overlapped with, in general, any other complex amplitude distribution and, in particular, with a coherent and shifted version of itself considering two orthogonal directions. The complex field values are retrieved by a novel Cepstrum-based algorithm, named as Spatial-Shifting Cepstrum (SSC), based on a weighted subtraction of the Cepstrum transform in the cross-correlation term of the object field spectrum in addition with the generation of a complex pupil from the combination of the information retrieved from different holographic recordings (one in horizontal and one in vertical direction) where one of the interferometric beams is shifted 1 pixel. As a result, the field of view is …

We demonstrate an experimental technique to characterize genuinely nonclassical multi-time correlations using projective measurements with no ancillae. We implement the scheme in a nitrogen-vacancy center in diamond undergoing a unitary quantum work protocol. We reconstruct quantum-mechanical time correlations encoded in the Margenau-Hills quasiprobabilities. We observe work extraction peaks five times those of sequential projective energy measurement schemes and in violation of newly-derived stochastic bounds. We interpret the phenomenon via anomalous energy exchanges due to the underlying negativity of the quasiprobability distribution.

Quantum reference frames have attracted renewed interest recently, as their exploration is relevant and instructive in many areas of quantum theory. Among the different types, position and time reference frames have captivated special attention. Here, we introduce and analyze a non-relativistic framework in which each system contains an internal clock, in addition to its external (spatial) degree of freedom and, hence, can be used as a spatiotemporal quantum reference frame. Among other applications of this framework, we show that even in simple scenarios with no interactions, the relative uncertainty between clocks affects the relative spatial spread of the systems.