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Mar 2022 • ACS Energy Letters

Stabilizing High-Voltage Lithium-Ion Battery Cathodes Using Functional Coatings of 2D Tungsten Diselenide

Sandipan Maiti, Rajashree Konar, Hadar Sclar, Judith Grinblat, Michael Talianker, Maria Tkachev, Xiaohan Wu, Aleksandr Kondrakov, Gilbert Daniel Nessim, Doron Aurbach

Functional surface coatings were applied on high voltage spinel (LiNi0.5Mn1.5O4; LNMO) and Ni-rich (LiNi0.85Co0.1Mn0.05O2; NCM851005) NCM cathode materials using few-layered 2H tungsten diselenide (WSe2). Simple liquid-phase mixing with WSe2 in 2-propanol and low-temperature (130 °C) heat treatment in nitrogen flow dramatically improved electrochemical performance, including stable cycling, high-rate performance, and lower voltage hysteresis in Li coin cells at 30 and 55 °C. Significantly improved capacity retention at 30 °C [Q401/Q9 of 99% vs 38% for LNMO and Q322/Q23 of 64% vs 46% for NCM851005] indicated efficient functionality. TEM and XPS clarified the coating distribution and coordination with the cathode surface, while postcycling studies revealed its sustainability, enabling lower transition metal dissolution and minor morphological deformation/microcrack formation. A modified and …

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Mar 2022 • Bulletin of the American Physical Society

Ultrafast carrier dynamics in Cu9S5 flakes

Andrea Villa, Madina Telkhozhayeva, Fabio Marangi, Eti Teblum, Aaron Ross, Mirko Prato, Luca Andena, Roberto Frassine, Francesco Scotognella, Gilbert Nessim

Copper chalcogenides have attracted attention due to their intrinsic doping properties. These materials display high carrier concentrations due to their defect-heavy structures, thus by varying their stoichiometry tunable plasmonic resonances can be observed, as it was shown previously for Cu 2-x S/Se/Te, with 09S 5 were studied by means of ultrafast transient absorption (TA) spectroscopy. The samples were pumped at 50 kHz with 50 fs pulses centered a 1.65 μm, in the region of the near-infrared (NIR) plasmonic resonance, and probed in the 1.1-1.6 μm range. The measurement was performed with a high sensitivity TA spectrometer utilizing a birefringent delay line interferometer and lock-in detection, avoiding the need for expensive IR multi-pixel detectors. We were able to measure the relaxation dynamics of the excited electrons, which are dominated by a fast decay (τ 1~ 400 fs) associated to electron-phonon …

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Mar 2022 • ChemSusChem 15 (8), e202200027, 2022

What is Next in Anion‐Exchange Membrane Water Electrolyzers? Bottlenecks, Benefits, and Future

Carlo Santoro, Alessandro Lavacchi, Piercarlo Mustarelli, Vito Di Noto, Lior Elbaz, Dario Dekel, Frederic Jaouen

As highlighted by the recent roadmaps from the European Union and the United States, water electrolysis is the most valuable high‐intensity technology for producing green hydrogen. Currently, two commercial low‐temperature water electrolyzer technologies exist ‐ alkaline water electrolyzer (A‐WE) and proton exchange membrane water electrolyzer (PEM‐WE). However, both have major drawbacks. A‐WE shows low productivity and efficiency, while PEM‐WE uses a significant amount of critical raw materials. Lately, the use of anion‐exchange membrane electrolyzers (AEM‐WE) has been proposed to overcome the limitations of the current commercial systems. AEM‐WE could become the cornerstone to achieve an intense, safe and resilient green hydrogen production to fulfill the hydrogen targets to achieve the 2050 decarbonization goals. Here we discuss the status of AEM‐WE development, with a focus on …

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Mar 2022 • ACS Applied Nano Materials

Synergy between Cobalt–Chromium-Layered Double Hydroxide Nanosheets and Oxidized Carbon Nanotubes for Electrocatalytic Oxygen Evolution

Bibhudatta Malik, Hari Krishna Sadhanala, SK Tarik Aziz, Sumit Majumder, Rajashree Konar, Aharon Gedanken, Gilbert Daniel Nessim

Enormous potential loss and sluggish kinetics of the oxygen evolution reaction (OER) limit the practical implementation of water electrolyser systems. We attempt to address these technical challenges through the synthesis of cobalt–chromium-layered double hydroxide nanosheets (CoCr LDH) on oxidized-carbon nanotube (O-CNT) backbones as efficient OER electrocatalysts. Microscopic and elemental distribution analysis suggests that interconnected sheets of CoCr LDH masks over O-CNTs. We tested various compositions of the CoCr LDH_O-CNT hybrid (by varying the molar ratios of Co and Cr) along with the weight adjustment between CoCr LDH and O-CNTs to obtain an optimal OER activity. Due to the synergistic effect, the CoCr-LDH(3:1)_O-CNT (2:1) exhibits the lowest overpotential of 290 mV at 10 mA cm–2 with a corresponding smaller Tafel slope of 42 mV dec–1, which outperforms the other tested …

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Mar 2022 • arXiv preprint arXiv:2203.04669

Enhancement of superconductivity upon reduction of carrier density in proximitized graphene

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

The superconducting transition temperature (Tc) of a single layer graphene coupled to an Indium oxide (InO) film, a low carrier-density superconductor, is found to increase with decreasing carrier density and is largest close to the average charge neutrality point in graphene. Such an effect is very surprising in conventional BCS superconductors. We study this phenomenon both experimentally and theoretically. Our analysis suggests that the InO film induces random electron and hole-doped puddles in the graphene. The Josephson effect across these regions of opposite polarity enhances the Josephson coupling between the superconducting clusters in InO, along with the overall Tc of the bilayer heterostructure. This enhancement is most effective when the chemical potential of the system is tuned between the charge neutrality points of the electron and hole-doped regions.

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Mar 2022 • Sciences

NIR fluorescence lifetime macroscopic imaging with a time-gated SPAD camera

X Michalet, A Ulku, J Smith, C Bruschini, S Weiss

The performance of SwissSPAD2 (SS2), a large scale, widefield time-gated CMOS SPAD imager developed for fluorescence lifetime imaging, has recently been described in the context of visible range and fluorescence lifetime imaging microscopy (FLIM) of dyes with lifetimes in the 2.5–4 ns range. Here, we explore its capabilities in the NIR regime relevant for small animal imaging, where its sensitivity is lower and typical NIR fluorescent dye lifetimes are much shorter (1 ns or less). We carry out this study in a simple macroscopic imaging setup based on a compact NIR picosecond pulsed laser, an engineered diffuser-based illumination optics, and NIR optimized imaging lens suitable for well-plate or small animal imaging. Because laser repetition rates can vary between models, but the synchronization signal frequency accepted by SS2 is fixed to 20 MHz, we first checked that a simple frequency-division scheme …

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Mar 2022 • ACS Applied Energy Materials

Combinatorial Synthesis and Screening of a Ternary NiFeCoOx Library for the Oxygen Evolution Reaction

A Usha Vijayakumar, N Aloni, V Thazhe Veettil, G Rahamim, SS Hardisty, M Zysler, S Tirosh, D Zitoun

The development of an efficient catalyst for the oxygen evolution reaction (OER) is critical to fulfilling the mission of hydrogen generation by water splitting. Various multicomponent systems have been investigated so far for the OER, although a systematic investigation is lacking and there are discrepancies as to which formulations make the best catalyst. Here, we perform a systematic investigation of a ternary Ni-Fe-Co oxide gradient library for the OER, using a combinatorial approach. This approach allows a much faster investigation of a vast compositional space compared to the traditional step by step approach. Also, it enables a more reliable comparison of the various catalysts as they all experience the same process and measurement conditions. We used the spray pyrolysis technique in combinatorial electrocatalyst screening for the first time for the generation of a gradient library of Ni-Fe-Co oxides …

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Mar 2022

System and method for use in remote sensing

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Mar 2022 • Nature Communications

Landscape of adenosine-to-inosine RNA recoding across human tissues

Orshay Gabay, Yoav Shoshan, Eli Kopel, Udi Ben-Zvi, Tomer D Mann, Noam Bressler, Roni Cohen‐Fultheim, Amos A Schaffer, Shalom Hillel Roth, Ziv Tzur, Erez Y Levanon, Eli Eisenberg

RNA editing by adenosine deaminases changes the information encoded in the mRNA from its genomic blueprint. Editing of protein-coding sequences can introduce novel, functionally distinct, protein isoforms and diversify the proteome. The functional importance of a few recoding sites has been appreciated for decades. However, systematic methods to uncover these sites perform poorly, and the full repertoire of recoding in human and other mammals is unknown. Here we present a new detection approach, and analyze 9125 GTEx RNA-seq samples, to produce a highly-accurate atlas of 1517 editing sites within the coding region and their editing levels across human tissues. Single-cell RNA-seq data shows protein recoding contributes to the variability across cell subpopulations. Most highly edited sites are evolutionary conserved in non-primate mammals, attesting for adaptation. This comprehensive set can …

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Mar 2022 • Proc. of SPIE Vol

Nano logic gates based on gold nanoparticles-carbon dots hybrid and its FLIM imaging

Shweta Pawar, Hamootal Duadi, Yafit Fleger, Dror Fixler

In today’s research area it is extremely important to assemble nanomaterials into electric devices at the nanoscale level due to the rapid expansion of nanotechnology in various fields. Designing a nanohybrid composed of gold nanoparticles (AuNPs) and red-emitting carbon dots (CDs) can be used to develop a fluorescence lifetime imaging (FLIM) based logic gate that can respond to multiple input parameters. The AuNPs are conjugated to CDs surfaces through a strong covalent linkage between them. These fluorescence lifetimes-based logic gates could be the new way to overcome the limitation of fluorescence intensity-based logic gates. The Au-CDs nanohybrid shows significant fluorescence quenching of pristine CDs after conjugation of gold nanoparticles. This quenched fluorescence can be recovered back by using a proper recovering agent giving us a reversible logic output. This nanohybrid can be used …

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Mar 2022 • Diagnostics

Simultaneous Noninvasive Detection and Therapy of Atherosclerosis Using HDL Coated Gold Nanorods

Rinat Ankri, Dorit Leshem-Lev, Hamootal Duadi, Emanuel Harari, Menachem Motiei, Edith Hochhauser, Eli I Lev, Dror Fixler

Cardiovascular disease (CVD) is a major cause of death and disability worldwide. A real need exists in the development of new, improved therapeutic methods for treating CVD, while major advances in nanotechnology have opened new avenues in this field. In this paper, we report the use of gold nanoparticles (GNPs) coated with high-density lipoprotein (HDL) (GNP-HDL) for the simultaneous detection and therapy of unstable plaques. Based on the well-known HDL cardiovascular protection, by promoting the reverse cholesterol transport (RCT), injured rat carotids, as a model for unstable plaques, were injected with the GNP-HDL. Noninvasive detection of the plaques 24 h post the GNP injection was enabled using the diffusion reflection (DR) method, indicating that the GNP-HDL particles had accumulated in the injured site. Pathology and noninvasive CT measurements proved the recovery of the injured artery treated with the GNP-HDL. The DR of the GNP-HDL presented a simple and highly sensitive method at a low cost, resulting in simultaneous specific unstable plaque diagnosis and recovery.

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Mar 2022 • Bulletin of the American Physical Society

Hidden magnetic memory and spontaneous superconducting vortices in alternating stacking compound 4Hb-TaS2

Eylon Persky, Anders Bjørlig, Irena Feldman, Avior Almoalem, Ehud Altman, Erez Berg, Itamar Kimchi, Jonathan Ruhman, Beena Kalisky

W61. 00009: Hidden magnetic memory and spontaneous superconducting vortices in alternating stacking compound 4Hb-TaS 2

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Mar 2022 • Imaging, Manipulation, and Analysis of Biomolecules, Cells, and Tissues XX …, 2022

Characterization of a large gated SPAD array for in vivo fluorescence lifetime imaging of drug target engagement

Jason T Smith, Alena Rudkouskaya, Shan Gao, Arin Ulku, Claudio Bruschini, Edoardo Charbon, Shimon Weiss, Margarida Barroso, Xavier Intes, Xavier Michalet

Near-Infrared wide-field Fluorescence Lifetime Imaging (FLI) has become an increasingly popular method due to its unique specificity in sensing the cellular micro-environment and/or protein-protein interactions via FRET, but the approach is still challenging due to inefficient detection modules. Here, we report on the characterization of a large gated SPAD array, SwissSPAD2, towards in vivo preclinical imaging of FLI-FRET. Fluorescence decay fitting as well as phasor analysis are used to demonstrate the ability of SwissSPAD2 to accurately quantify short lifetimes and associated lifetime parameters in both in vitro and in vivo experiments, in full agreement with gated ICCD measurements.

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Mar 2022 • arXiv preprint arXiv:2203.04669

Enhancement of superconductivity upon reduction of carrier density in proximitized graphene

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

The superconducting transition temperature (Tc) of a single layer graphene coupled to an Indium oxide (InO) film, a low carrier-density superconductor, is found to increase with decreasing carrier density and is largest close to the average charge neutrality point in graphene. Such an effect is very surprising in conventional BCS superconductors. We study this phenomenon both experimentally and theoretically. Our analysis suggests that the InO film induces random electron and hole-doped puddles in the graphene. The Josephson effect across these regions of opposite polarity enhances the Josephson coupling between the superconducting clusters in InO, along with the overall Tc of the bilayer heterostructure. This enhancement is most effective when the chemical potential of the system is tuned between the charge neutrality points of the electron and hole-doped regions.

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Mar 2022 • ACS Energy Letters

Anion–Diluent Pairing for Stable High-Energy Li Metal Batteries

Chunnan Zhu, Chuangchao Sun, Ruhong Li, Suting Weng, Liwu Fan, Xuefeng Wang, Lixin Chen, Malachi Noked, Xiulin Fan

Rechargeable Li metal batteries (LMBs) have attracted wide attention as promising candidates for the next generation of energy-storage systems. However, limited Coulombic efficiency and unregulated dendrite growth restrict its application. Here, we report a kind of electrolyte by introducing fluorinated aromatic diluents into high-concentration electrolytes (HCEs). Unlike other localized HCEs, the fluorinated aromatic diluents pairing with anions promote the formation of a homogeneous and robust solid–electrolyte interphase (SEI), which endows Li metal with an ultrahigh Coulombic efficiency of ∼99.8%. The Li||LiNi0.8Co0.1Mn0.1O2 battery holds a capacity retention of >80% over 260 cycles even with a thin Li anode (20 μm) and a high cathode loading (3.5 mAh cm–2). A 1.8 Ah Li||NMC811 pouch cell with a lean electrolyte delivers an energy density of 340 Wh kg–1 and a stable cycling life over 200 cycles. The …

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Mar 2022 • Bulletin of the American Physical Society

One dimensional quantum Wigner crystals and SU (4) magnetism

Gergely Zarand, Shahal Ilani, Assaf Hamo, Catalin Pascu Moca, Örs Legeza, Ilanit Shapir, Sharon Pecker

The quantum crystal of electrons, predicted by Jenő Wigner almost 90 years ago, is one of the most elusive states of matter. In the very dilute limit, where the crystal forms, disorder effects and inhomogeneity very easily destroy this fragile state of matter, which is therefore very hard to be observed in its pristine form. It is also a major challenge for theorists to produce quantitative results in this strongly interacting, dilute limit, where the melting of the crystal occurs. We present corroborated experimental and theoretical results, which lead to a recent, direct observation of the spatial crystal structure of one dimensional Wigner quantum crystals in carbon nanotubes [1]. In the experiments, we a non-invasive single electron (hole) probe is employed, and we compare the experimental results with self-consistent DMRG simulations. We also investigate the tunneling of the crystal in a double well potential, and demonstrate by …

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Mar 2022 • arXiv preprint arXiv:2203.00688

High-resolution absorption measurements with free-electron lasers using ghost spectroscopy

Yishai Klein, Edward Strizhevsky, Flavio Capotondi, Dario De Angelis, Luca Giannessi, Matteo Pancaldi, Emanuele Pedersoli, Giuseppe Penco, Kevin C Prince, Or Sefi, Young Yong Kim, Ivan A Vartanyants, Sharon Shwartz

We demonstrate a simple and robust high-resolution ghost spectroscopy approach for x-ray and extreme ultraviolet absorption spectroscopy at free-electron laser sources. Our approach requires an on-line spectrometer before the sample and a downstream bucket detector. We use this method to measure the absorption spectrum of silicon, silicon carbide and silicon nitride membranes in the vicinity of the silicon L2,3-edge. We show that ghost spectroscopy allows the high-resolution reconstruction of the sample spectral response using a coarse energy scan with self-amplified spontaneous emission radiation. For the conditions of our experiment the energy resolution of the ghost-spectroscopy reconstruction is higher than the energy resolution reached by scanning the energy range by narrow spectral bandwidth radiation produced by the seeded free-electron laser. When we set the photon energy resolution of the ghost spectroscopy to be equal to the resolution of the measurement with the seeded radiation, the measurement time with the ghost spectroscopy method is shorter than scanning the photon energy with seeded radiation. The exact conditions for which ghost spectroscopy can provide higher resolution at shorter times than measurement with narrow band scans depend on the details of the measurements and on the properties of the samples and should be addressed in future studies.

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Mar 2022 • Optical and Quantum Sensing and Precision Metrology II, PC120160Z, 2022

Nonlinear quantum interferometer in the time and frequency domains

Moti Fridman, Eliahu Cohen

Interferometers are highly sensitive to phase differences and are utilized in numerous schemes. Quantum interferometers are able to improve the sensitivity of classical interferometers beyond the shot-noise limit. This is done by employing squeezed states of light and destructive interference of the noise in the system. We developed a quantum SU(1,1) interferometer in the time domain. Our nonlinear quantum interferometer creates interference of the input signals at different times and frequencies. We can control the time and frequency differences for investigating the full temporal and spectral structure of the signal. This quantum interferometer can be utilized for sensing ultrafast phase changes, quantum imaging, temporal mode encoding, and studying the temporal structure of entangled photons.

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Mar 2022 • Inorganics

Improved Electrochemical Behavior and Thermal Stability of Li and Mn-Rich Cathode Materials Modified by Lithium Sulfate Surface Treatment

Hadar Sclar, Sandipan Maiti, Rosy Sharma, Evan M Erickson, Judith Grinblat, Ravikumar Raman, Michael Talianker, Malachi Noked, Aleksandr Kondrakov, Boris Markovsky, Doron Aurbach

High-energy cathode materials that are Li- and Mn-rich lithiated oxides—for instance, 0.35Li2MnO3.0.65LiNi0.35Mn0.45Co0.20O2 (HE-NCM)—are promising for advanced lithium-ion batteries. However, HE-NCM cathodes suffer from severe degradation during cycling, causing gradual capacity loss, voltage fading, and low-rate capability performance. In this work, we applied an effective approach to creating a nano-sized surface layer of Li2SO4 on the above material, providing mitigation of the interfacial side reactions while retaining the structural integrity of the cathodes upon extended cycling. The Li2SO4 coating was formed on the surface of the material by mixing it with nanocrystalline Li2SO4 and annealing at 600 °C. We established enhanced electrochemical behavior with ~20% higher discharge capacity, improved charge-transfer kinetics, and higher rate capability of HE-NCM cathodes due to the presence of the Li2SO4 coating. Online electrochemical mass spectrometry studies revealed lower CO2 and H2 evolution in the treated samples, implying that the Li2SO4 layer partially suppresses the electrolyte degradation during the initial cycle. In addition, a ~28% improvement in the thermal stability of the Li2SO4-treated samples in reactions with battery solution was also shown by DSC studies. The post-cycling analysis allowed us to conclude that the Li2SO4 phase remained on the surface and retained its structure after 100 cycles.

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Mar 2022 • Nanoscale Imaging, Sensing, and Actuation for Biomedical Applications XIX …, 2022

Extraction of absorption coefficients from two-layer phantoms based on crossover point in diffuse reflectance

Pavitra Sokke Rudraiah, Hamootal Duadi, Dror Fixler

We performed a Monte Carlo simulation to detect the tattoo ink location in the dermis layer of the human skin. Tattoo ink (thickness of 0.2mm) was located between the upper dermis layer (thickness of 2mm) and the lower dermis layer (thickness of 8mm). An appreciable difference in the spatially resolved diffuse reflectance (DR) intensity was found between the skin without tattoo and the tattooed skin. The point at which the skin without tattoo and the tattooed skin DR intensity profile intersect is called the crossover point (Cp). The slopes were extracted from the DR intensity profile before and after the Cp for a wavelength range from 400-1,000nm. The slopes are extracted from each wavelength, and we plotted the calculated square slopes versus wavelength. In the shorter wavelengths region (400-500nm), two-layer (2L) behavior was observed, and in the longer wavelengths region (600-1,000nm), a single layer …

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Mar 2022 • Nanoscale Imaging, Sensing, and Actuation for Biomedical Applications XIX …, 2022

Golden exosomes: a new platform for cancer theranostics

Adi Anaki, Oshra Betzer, Menachem Motiei, Tamar Sadan, Dror Fixler, Rachela Popovtzer

Delivery of therapeutics to tumors is a major challenge, due to the sequence of formidable biological barriers in the body and tumor, which limit the penetration of various nano-carriers and drugs into the tumor. Exosomes are promising vectors for delivery of anti-tumor therapies, due to their biocompatibility, ability to evade clearance, and innate ability to home to, and interact with, target cells. However, promoting clinical application of exosome-based therapeutics requires elucidation of key issues, including exosome bio-distribution, tumor targeting, and the ability to overcome tumor barriers. Here, we examined these parameters using mesenchymal stem cell (MSCs)-derived exosomes loaded with gold nanoparticles (GNPs), aiming to delineate design principles for therapy loading and delivery. This novel technology provides essential and fundamental knowledge on exosomes for enhanced targeted drug …

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