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Aug 2024 • Proceedings of the National Academy of Sciences

Electron transport through two interacting channels in Azurin-based solid-state junctions

Ping’an Li, Sudipta Bera, Shailendra Kumar-Saxena, Israel Pecht, Mordechai Sheves, David Cahen, Yoram Selzer

The fundamental question of “what is the transport path of electrons through proteins?” initially introduced while studying long-range electron transfer between localized redox centers in proteins in vivo is also highly relevant to the transport properties of solid-state, dry metal–protein–metal junctions. Here, we report conductance measurements of such junctions, Au-(Azurin monolayer ensemble)-Bismuth (Bi) ones, with well-defined nanopore geometry and ~103 proteins/pore. Our results can be understood as follows. (1) Transport is via two interacting conducting channels, characterized by different spatial and time scales. The slow and spatially localized channel is associated with the Cu center of Azurin and the fast delocalized one with the protein’s polypeptide matrix. Transport via the slow channel is by a sequential (noncoherent) process and in the second one by direct, off-resonant tunneling. (2) The two …

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Aug 2024 • ChemBioChem

The Dynamic Plasticity of P. aeruginosa CueR Copper Transcription Factor upon Cofactor and DNA Binding

Ameer Yasin, Alysia Mandato, Lukas Hofmann, Yasmin Igbaria‐Jaber, Yulia Shenberger, Lada Gevorkyan‐Airapetov, Sunil Saxena, Sharon Ruthstein

Bacteria use specialized proteins, like transcription factors, to rapidly control metal ion balance. CueR is a Gram‐negative bacterial copper regulator. The structure of E. coli CueR complexed with Cu(I) and DNA was published, since then many studies have shed light on its function. However, P. aeruginosa CueR, which shows high sequence similarity to E. coli CueR, has been less studied. Here, we applied room‐temperature electron paramagnetic resonance (EPR) measurements to explore changes in dynamics of P. aeruginosa CueR in dependency of copper concentrations and interaction with two different DNA promoter regions. We showed that P. aeruginosa CueR is less dynamic than the E. coli CueR protein and exhibits much higher sensitivity to DNA binding as compared to its E. coli CueR homolog. Moreover, a difference in dynamical behavior was observed when P. aeruginosa CueR binds to …

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Aug 2024 • Journal of Biomedical Optics

Dependency of crossover point on absorption changes in bilayer diffusion reflection measurements

Channa Shapira, Yuval Yedvav, Hamootal Duadi, Haim Taitelbaum, Dror Fixler

SignificanceA better understanding of diffusion reflection (DR) behavior may allow it to be used for more noninvasive applications, including the development of in vivo non-damaging techniques, especially for medical topical diagnosis and treatments.AimFor a bilayer opaque substance where the attenuation of the upper layer is larger than the attenuation of the lower layer, the DR crossover point () is location where the photons coming from the bottom layer start affecting the DR. We aim to study the dependency of the on absorption changes in different layers for constant scattering and top layer thickness.ApproachMonolayer and bilayer optical tissue-like phantoms were prepared and measured using a DR system. The results were compared with Monte Carlo simulations.ResultsThere is an agreement between the experiments and the simulations. correlates with the square root of the absorption coefficient ratio …

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Aug 2024 • Biomass Conversion and Biorefinery

Biomass-derived Carbon dots and their coated surface as a potential antimicrobial agent

R Blessy Pricilla, Moorthy Maruthapandi, Arulappan Durairaj, Ivo Kuritka, John HT Luong, Aharon Gedanken

Carbon dots (CDs) with an average diameter of 6.3 nm were synthesized from the medicinal seed extract of Syzygium cumini L. using one-pot hydrothermal synthesis. The prepared CDs exhibited excitation-dependent emission characteristics with photoluminescence (PL) emission maxima at an excitation of 340 nm. The CDs at 500 µg/mL displayed antimicrobial activities against four common pathogens. Both Staphylococcus aureus and S. epidermidis were completely eradicated by CDs within 12 h, compared to 24 h for Escherichia coli and Klebsiella pneumonia. The release of various oxygen species (ROS) was postulated to play a critical role in bacterial eradication. The CDs decorated on cotton fabric by ultrasonication also displayed good antibacterial activities against the above bacteria. The finding opens a plausible use of CDs in biomedical textiles with potent antimicrobial properties against both Gram …

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Aug 2024 • Physical Review Materials

Observation of a second Dirac point in a graphene/superconductor bilayer

Gopi Nath Daptary, Eyal Walach, Udit Khanna, Efrat Shimshoni, Aviad Frydman

Two-dimensional (2D) materials have attracted vast research interest since the breakthrough discovery of graphene. One major benefit of such systems is the ability to tune the Fermi level through the charge neutrality point between electron and hole doping. Here we show that single layer graphene coupled to the low-density superconductor indium oxide (InO) exhibits two charge neutrality points, each of them representing electronic regions in which the carrier density can be tuned from hole to electron dominated. This is not seen in clean graphene or in a bilayer where the carrier density is extremely low. We suggest that the second charge neutrality point results from regions in the graphene layer just below superconducting islands in InO, where pairing is induced via the proximity effect; gating of this hybrid system therefore allows the tuning from hole to electron superconductivity through an ultralow carrier …

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Aug 2024 • Heliyon

Analysis of Ca1-xSrxCO3 phases generated by competitive Sr2+ replacement in pre-formed aragonite

Saja Nasser, Gili Cohen-Taguri, Tali Mass, Iddo Pinkas, Gil Goobes

The ratio of Sr/Ca ions in marine biogenic minerals is considered advantageous for tracking geochemical and biomineralization processes that occur in the oceans. It is debatable, though, whether the ratio in biominerals such as coral skeleton is simply related to values in the seawater environment or controlled by the organism. Recent data show that coral larvae produce partially disordered immature aragonite in Mg-containing Sr-poor calcifying fluids, which transforms into well-ordered aragonite in Mg-depleted Sr-enriched environments, upon animal metamorphosis into the sessile polyp state.Inspired by the process in young coral, we explored in vitro substitution of Ca by Sr in aragonite by exposing aragonite crystals precipitated a priori to Sr solutions with variable concentrations. The resulting biphasic material, comprised of Sr-doped aragonite and Ca-doped strontianite, was carefully analyzed for foreign …

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Aug 2024 • Electrochemical Society Meeting Abstracts 245

A Direct Dry Synthesis Route for High Purity Catalytic Nanoporous Metallic Films

Hannah Barad, Hyunah Kwon, Alex Ricardo Silva Olaya, Mariana Alárcon-Correa, Gunther Wittstock, Peer Fischer, Johannes D Bartl

Control of catalyst morphology is important because it affects many catalytic related properties such as, active sites, surface energy, and surface area, which can lead to tunable catalytic activity. Nanoporous metallic networks (NPMs), a morphology of interest for catalysis, contain many uncoordinated atoms at the surface and highly curved ligaments that can have a large effect on catalytic performance. Nanoporous self-supported metal structures have been synthesized in the past by dealloying of a master alloy,[1] which is a wet chemical method. This technique uses an Au-Ag alloy, from which Ag is etched away and which always results in NPMs containing residual amounts of the sacrificial metal (Ag) preventing the formation of high-purity structures. It follows that the catalytic properties of pure NPMs formed by dealloying can not be studied due to metal 'impurities' remaining in the structure. Although these …

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Aug 2024 • ACS Omega

Surface Plasmon Resonance Modulation by Complexation of Platinum on the Surface of Silver Nanocubes

Avi Huri, Yaakov Mandelbaum, Mike Rozenberg, Anya Muzikansky, Melina Zysler, David Zitoun

The use of plasmonic particles, specifically, localized surface plasmonic resonance (LSPR), may lead to a significant improvement in the electrical, electrochemical, and optical properties of materials. Chemical modification of the dielectric constant near the plasmonic surface should lead to a shift of the optical resonance and, therefore, the basis for color tuning and sensing. In this research, we investigated the variation of the LSPR by modifying the chemical environment of Ag nanoparticles (NPs) through the complexation of Pt(IV) metal cations near the plasmonic surface. This study is carried out by measuring the shift of the plasmon dipole resonance of Ag nanocubes (NCs) and nanowires (NWs) of differing sizes upon coating the Ag surface with a layer of polydopamine (PDA) as a coordinating matrix for Pt(IV) complexes. The red shift of up to 45 nm depends linearly on the thickness of the PDA/Pt(IV) layer and the …

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Aug 2024 • Batteries & Supercaps

Silicon Anodes for Lithium‐Ion Batteries Based on a New Polyimide Binder

David Lusztig, Shalom Luski, Netanel Shpigel, Naresh Vangapally, Doron Aurbach

Silicon is a promising candidate for replacing graphite in anodes for advanced Li‐ion batteries due to its high theoretical gravimetric energy density. However, silicon as an active anode material suffers from significant volume changes upon lithiation/delithiation, causing fast capacity fading. The performance of silicon anodes depends on the polymeric binders used, which form well‐bound Si particles matrices that accommodate the strains developed during their repeated lithiation, thus maintaining their integrity.

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Aug 2024 • The Journal of Physical Chemistry Letters 15 (32), 8177-8186, 2024

Predicting Conformational Ensembles of Intrinsically Disordered Proteins: From Molecular Dynamics to Machine Learning

Jana Aupič, Pavlína Pokorná, Sharon Ruthstein, Alessandra Magistrato

Intrinsically disordered proteins and regions (IDP/IDRs) are ubiquitous across all domains of life. Characterized by a lack of a stable tertiary structure, IDP/IDRs populate a diverse set of transiently formed structural states that can promiscuously adapt upon binding with specific interaction partners and/or certain alterations in environmental conditions. This malleability is foundational for their role as tunable interaction hubs in core cellular processes such as signaling, transcription, and translation. Tracing the conformational ensemble of an IDP/IDR and its perturbation in response to regulatory cues is thus paramount for illuminating its function. However, the conformational heterogeneity of IDP/IDRs poses several challenges. Here, we review experimental and computational methods devised to disentangle the conformational landscape of IDP/IDRs, highlighting recent computational advances that permit proteome …

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Aug 2024 • Advanced Energy Materials

Inclusion of Anion Additives in the Inner Solvation Shell to Regulate the Composition of Solid Electrolyte Interphase

Harshita Lohani, Ajit Kumar, Amreen Bano, Arpita Ghosh, Pratima Kumari, Aakash Ahuja, Abhinanda Sengupta, Dhruv Kumar, Dan Thomas Major, Sagar Mitra

An innovative approach to electrolyte engineering in carbonate electrolytes is introduced by incorporating high donor number dual anion additives into the conventional electrolyte system (1 M NaPF6 EC:PC). The active engagement of anions in the primary solvation shell effectively hinders the reduction of solvent molecules by reducing the Lowest Unoccupied Molecular Orbital (LUMO) of Na+‐solvent‐anion complex as compared to the LUMO of pure solvents or Na+‐solvent complex. The participation of anions leads to the formation of a thinner and an inorganic‐rich Solid Electrolyte Interphase on the hard carbon anode enhancing Initial Coulombic Efficiency and significantly improving its kinetics. Moreover, the system with dual anion additives exhibits oxidative stability up to 4.5 V, effectively mitigating the undesired side reactions at high voltage operation of the layered sodium nickel manganese oxide cathode …

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Aug 2024 • Nature Communications

Acoustically shaped DNA-programmable materials

ZA Arnon, S Piperno, DC Redeker, E Randall, AV Tkachenko, H Shpaisman, O Gang

Recent advances in DNA nanotechnology allow for the assembly of nanocomponents with nanoscale precision, leading to the emergence of DNA-based material fabrication approaches. Yet, transferring these nano- and micron-scale structural arrangements to the macroscale morphologies remains a challenge, which limits the development of materials and devices based on DNA nanotechnology. Here, we demonstrate a materials fabrication approach that combines DNA-programmable assembly with actively driven processes controlled by acoustic fields. This combination provides a prescribed nanoscale order, as dictated by equilibrium assembly through DNA-encoded interactions, and field-shaped macroscale morphology, as regulated by out-of-equilibrium materials formation through specific acoustic stimulation. Using optical and electron microscopy imaging and x-ray scattering, we further revealed the …

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Aug 2024 • Small

Multifunctional Liposomes Targeting Amyloid‐β Oligomers for Early Diagnosis and Therapy of Alzheimer's Disease

Sudipta Senapati, Kuldeep Tripathi, Khadeja Awad, Shai Rahimipour

Early detection and treatment are crucial for Alzheimer's disease (AD) management. Current diagnostic and therapeutic methods focus on late‐stage amyloid fibrils and plaques, overlooking toxic soluble amyloid β oligomers (AβOs) accumulating early in AD. A multifunctional liposome‐based platform is designed for early diagnosis and therapy of AD, leveraging a novel self‐assembled cyclic d,l‐α‐peptide (CP‐2) that selectively targets AβOs. Biocompatible CP‐2 conjugated liposomes (CP‐2‐LPs) effectively disrupt Aβ aggregation and mitigate Aβ‐mediated toxicity in human neuroblastoma cells. In transgenic Caenorhabditis elegans AD models, CP‐2‐LPs significantly outperformed free CP‐2 by improving cognitive and behavioral functions, extending lifespan, and reducing toxic AβO levels. Intravenous injection of fluorescently labeled CP‐2‐LPs reveals effective blood‐brain barrier penetration, with significantly …

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Aug 2024 • CRC Press, 2024

Magnetic Polymer Composites and Their Emerging Applications

Sayan Ganguly, Shlomo Margel, Poushali Das

Magnetic composite particles offer much potential for use in a variety of applications, including manufacturing, environmental protection, microfluidics, microelectronics, and biomedicine. Magnetic Polymer Composites and Their Emerging Applications explores leading research on the fabrication, characterization, properties, and all reported applications of magnetic polymer composites. Features: Discusses synthesis, properties, and modern fabrication technologies of magnetic polymer composites Describes the biocompatibility, suitability, and toxic effects of these materials Covers a variety of applications including those in biomedicine, wastewater treatment, soft robotics, 3D/4D printing, and agriculture Details opportunities and future directions in magnetic polymer composites and their surface decorations This unique book serves as a road map for materials engineers, as well as researchers, academics, technologists, and students working in sensor technology.

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Aug 2024 • arXiv preprint arXiv:2308.09336

Diffraction limit of light in curved space

Jingxuan Zhang, Chenni Xu, Patrick Sebbah, Li-Gang Wang

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.

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Aug 2024 • arXiv preprint arXiv:2408.09289

Mono‐Exponential Current Attenuation with Distance Across 16 nm Thick Bacteriorhodopsin Multilayers

Domenikos Chryssikos, Jerry A Fereiro, Jonathan Rojas, Sudipta Bera, Defne Tüzün, Evanthia Kounoupioti, Rui N Pereira, Christian Pfeiffer, Ali Khoshouei, Hendrik Dietz, Mordechai Sheves, David Cahen, Marc Tornow

The remarkable ability of natural proteins to conduct electricity in the dry state over long distances remains largely inexplicable despite intensive research. In some cases, a (weakly) exponential length-attenuation, as in off-resonant tunneling transport, extends to thicknesses even beyond 10 nm. This report deals with such charge transport characteristics observed in self-assembled multilayers of the protein bacteriorhodopsin (bR). About 7.5 nm to 15.5 nm thick bR layers were prepared on conductive titanium nitride (TiN) substrates using aminohexylphosphonic acid and poly-diallyl-dimethylammonium electrostatic linkers. Using conical EGaIn top contacts, an intriguing, mono-exponential conductance attenuation as a function of the bR layer thickness with a small attenuation coefficient is measured at zero bias. Variable-temperature measurements using evaporated Ti/Au top contacts yield effective energy barriers of about 100 meV from fitting the data to tunneling, hopping, and carrier cascade transport models. The observed temperature-dependence is assigned to the protein-electrode interfaces. The transport length and temperature dependence of the current densities are consistent with tunneling through the protein-protein and protein-electrode interfaces, respectively. Importantly, our results call for new theoretical approaches to find the microscopic mechanism behind the remarkably efficient, long-range electron transport within bR.

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Aug 2024 • Physical Review Materials

Observation of a second Dirac point in a graphene/superconductor bilayer

Gopi Nath Daptary, Eyal Walach, Udit Khanna, Efrat Shimshoni, Aviad Frydman

Two-dimensional (2D) materials have attracted vast research interest since the breakthrough discovery of graphene. One major benefit of such systems is the ability to tune the Fermi level through the charge neutrality point between electron and hole doping. Here we show that single layer graphene coupled to the low-density superconductor indium oxide (InO) exhibits two charge neutrality points, each of them representing electronic regions in which the carrier density can be tuned from hole to electron dominated. This is not seen in clean graphene or in a bilayer where the carrier density is extremely low. We suggest that the second charge neutrality point results from regions in the graphene layer just below superconducting islands in InO, where pairing is induced via the proximity effect; gating of this hybrid system therefore allows the tuning from hole to electron superconductivity through an ultralow carrier …

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Aug 2024 • Proceedings of the National Academy of Sciences

Electron transport through two interacting channels in Azurin-based solid-state junctions

Ping’an Li, Sudipta Bera, Shailendra Kumar-Saxena, Israel Pecht, Mordechai Sheves, David Cahen, Yoram Selzer

The fundamental question of “what is the transport path of electrons through proteins?” initially introduced while studying long-range electron transfer between localized redox centers in proteins in vivo is also highly relevant to the transport properties of solid-state, dry metal–protein–metal junctions. Here, we report conductance measurements of such junctions, Au-(Azurin monolayer ensemble)-Bismuth (Bi) ones, with well-defined nanopore geometry and ~103 proteins/pore. Our results can be understood as follows. (1) Transport is via two interacting conducting channels, characterized by different spatial and time scales. The slow and spatially localized channel is associated with the Cu center of Azurin and the fast delocalized one with the protein’s polypeptide matrix. Transport via the slow channel is by a sequential (noncoherent) process and in the second one by direct, off-resonant tunneling. (2) The two …

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Aug 2024 • Journal of Solution Chemistry

Heat of Dilution and Racemization of Chiral Amino Acid Solutions

Matan Oliel, Yitzhak Mastai

Chiral interactions play a crucial role in both chemistry and biology. Understanding the behavior of chiral molecules and their interactions with other molecules is essential, and chiral interactions in solutions are particularly important for studying chiral compounds. Chirality influences the physical and chemical properties of molecules, including solubility, reactivity, and biological activity. In this work, we used isothermal titration calorimetry (ITC), a powerful technique for studying molecular interactions, including chiral interactions in solutions. We conducted a series of ITC measurements to investigate the heat of dilution and the heat of racemization of several amino acids (Asparagine, Histidine, Serine, Alanine, Methionine, and Phenylalanine). We also performed ITC measurements under different solute concentrations and temperatures to examine the effects of these parameters on chiral interactions, as well as the …

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Aug 2024 • Optics Communications

A colour-encoded nanometric ruler for axial super-resolution microscopies

Ilya Olevsko, Omer Shavit, Moshe Feldberg, Yossi Abulafia, Adi Salomon, Martin Oheim

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. Also, comparison between techniques remains a major challenge due to the absence of suitable calibration tools that would permit a metrology along the microscope's optical axis. Likewise, such test samples would be useful as well for quantifying nanometric drift, or axial fluorophore mobility, or again for quantifying the sub-wavelength light confinement in near-field microscopies. In the present work, we propose a colour-encoded nanoscopic axial ruler. We provide a multi-layered single-excitation, dual-emission test slide, which translates the axial-distance problem into a spectral measurement. Our test slide combines, on a standard …

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Aug 2024 • arXiv preprint arXiv:2408.09276

Current rectification via Photosystem I monolayers induced by their orientation on hydrophilic self-assembled monolayers on titanium nitride

Jonathan Rojas, Zhe Wang, Feng Liu, Jerry A Fereiro, Domenikos Chryssikos, Thomas Dittrich, Dario Leister, David Cahen, Marc Tornow

Photosystem I (PSI) is a photosynthetic protein which evolved to efficiently transfer electrons through the thylakoid membrane. This remarkable process attracted the attention of the biomolecular electronics community, which aims to study and understand the underlying electronic transport through these proteins by contacting ensembles of PSI with solid-state metallic contacts. This paper extends published work of immobilizing monolayers of PSI with a specific orientation, by using organophosphonate self-assembled molecules with hydrophilic heads on ultra-flat titanium nitride. Electrical measurements carried out with eutectic GaIn top contacts showed current rectification ratios of up to ~200. The previously proposed rectification mechanism, relying on the protein's internal electric dipole, was inquired by measuring shifts in the work function. Our straightforward bottom-up fabrication method may allow for further experimental studies on PSI molecules, such as embedding them in solid-state, transparent top contact schemes for optoelectronic measurements.

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