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Oct 2023 • Materials Today Energy

Aqueous proton batteries based on acetic acid solutions: mechanistic insights

Bar Gavriel, Gil Bergman, Meital Turgeman, Amey Nimkar, Yuval Elias, Mikhael D Levi, Daniel Sharon, Netanel Shpigel, Doron Aurbach

Large grid energy storage devices are critical for the success of the clean and sustainable energy revolution. As Li-ion batteries are earmarked for electric vehicles and portable devices such as laptops and cellphones, other electrochemical systems should be developed that enable cost-effective, safe, and durable large-scale energy storage. Due to the low cost and non-flammability of aqueous electrolyte solutions, much effort is being put into development of 'beyond-Li' batteries and supercapacitors that can work in these environments. Here, we propose new proton batteries comprising an acetic acid electrolyte solution, NiII[FeIII(CN)6]2/3·4H2O Prussian blue analog cathodes, and Ti3C2Tx MXene anodes. Both electrodes were investigated independently to discover ideal settings for electrochemical performance and stability. Significant attention was given to the cathodes' protons storage mechanism. In-situ …

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Oct 2023 • ACS Omega

Revealing the DNA Binding Modes of CsoR by EPR Spectroscopy

Yasmin Igbaria-Jaber, Lukas Hofmann, Lada Gevorkyan-Airapetov, Yulia Shenberger, Sharon Ruthstein

In pathogens, a unique class of metalloregulator proteins, called gene regulatory proteins, sense specific metal ions that initiate gene transcription of proteins that export metal ions from the cell, thereby preventing toxicity and cell death. CsoR is a metalloregulator protein found in various bacterial systems that “sense” Cu(I) ions with high affinity. Upon copper binding, CsoR dissociates from the DNA promoter region, resulting in initiation of gene transcription. Crystal structures of CsoR in the presence and absence of Cu(I) from various bacterial systems have been reported, suggesting either a dimeric or tetrameric structure of these helical proteins. However, structural information about the CsoR-DNA complex is missing. Here, we applied electron paramagnetic resonance (EPR) spectroscopy to follow the conformational and dynamical changes that Mycobacterium tuberculosis CsoR undergoes upon DNA binding in …

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Oct 2023

Roadmap on Label‐Free Super‐Resolution Imaging

Vasily N Astratov, Yair Ben Sahel, Yonina C Eldar, Luzhe Huang, Aydogan Ozcan, Nikolay Zheludev, Junxiang Zhao, Zachary Burns, Zhaowei Liu, Evgenii Narimanov, Neha Goswami, Gabriel Popescu, Emanuel Pfitzner, Philipp Kukura, Yi‐Teng Hsiao, Chia‐Lung Hsieh, Brian Abbey, Alberto Diaspro, Aymeric LeGratiet, Paolo Bianchini, Natan T Shaked, Bertrand Simon, Nicolas Verrier, Matthieu Debailleul, Olivier Haeberlé, Sheng Wang, Mengkun Liu, Yeran Bai, Ji‐Xin Cheng, Behjat S Kariman, Katsumasa Fujita, Moshe Sinvani, Zeev Zalevsky, Xiangping Li, Guan‐Jie Huang, Shi‐Wei Chu, Omer Tzang, Dror Hershkovitz, Ori Cheshnovsky, Mikko J Huttunen, Stefan G Stanciu, Vera N Smolyaninova, Igor I Smolyaninov, Ulf Leonhardt, Sahar Sahebdivan, Zengbo Wang, Boris Luk'yanchuk, Limin Wu, Alexey V Maslov, Boya Jin, Constantin R Simovski, Stephane Perrin, Paul Montgomery, Sylvain Lecler

Label‐free super‐resolution (LFSR) imaging relies on light‐scattering processes in nanoscale objects without a need for fluorescent (FL) staining required in super‐resolved FL microscopy. The objectives of this Roadmap are to present a comprehensive vision of the developments, the state‐of‐the‐art in this field, and to discuss the resolution boundaries and hurdles that need to be overcome to break the classical diffraction limit of the label‐free imaging. The scope of this Roadmap spans from the advanced interference detection techniques, where the diffraction‐limited lateral resolution is combined with unsurpassed axial and temporal resolution, to techniques with true lateral super‐resolution capability that are based on understanding resolution as an information science problem, on using novel structured illumination, near‐field scanning, and nonlinear optics approaches, and on designing superlenses based …

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Oct 2023 • Quantum

Kirkwood-Dirac quasiprobability approach to the statistics of incompatible observables

Matteo Lostaglio, Alessio Belenchia, Amikam Levy, Santiago Hernández-Gómez, Nicole Fabbri, Stefano Gherardini

Recent work has revealed the central role played by the Kirkwood-Dirac quasiprobability (KDQ) as a tool to properly account for non-classical features in the context of condensed matter physics (scrambling, dynamical phase transitions) metrology (standard and post-selected), thermodynamics (power output and fluctuation theorems), foundations (contextuality, anomalous weak values) and more. Given the growing relevance of the KDQ across the quantum sciences, our aim is two-fold: First, we highlight the role played by quasiprobabilities in characterizing the statistics of quantum observables and processes in the presence of measurement incompatibility. In this way, we show how the KDQ naturally underpins and unifies quantum correlators, quantum currents, Loschmidt echoes, and weak values. Second, we provide novel theoretical and experimental perspectives by discussing a wide variety of schemes to access the KDQ and its non-classicality features.

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Oct 2023 • Nature Nanotechnology

High-energy all-solid-state lithium batteries enabled by Co-free LiNiO2 cathodes with robust outside-in structures

Longlong Wang, Ayan Mukherjee, Chang-Yang Kuo, Sankalpita Chakrabarty, Reut Yemini, Arrelaine A Dameron, Jaime W DuMont, Sri Harsha Akella, Arka Saha, Sarah Taragin, Hagit Aviv, Doron Naveh, Daniel Sharon, Ting-Shan Chan, Hong-Ji Lin, Jyh-Fu Lee, Chien-Te Chen, Boyang Liu, Xiangwen Gao, Suddhasatwa Basu, Zhiwei Hu, Doron Aurbach, Peter G Bruce, Malachi Noked

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 …

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Oct 2023 • ACS Nano

Triggering Gaussian-to-Exponential Transition of Displacement Distribution in Polymer Nanocomposites via Adsorption-Induced Trapping

Ming Hu, Hongbo Chen, Hongru Wang, Stanislav Burov, Eli Barkai, Dapeng Wang

Triggering Gaussian-to-Exponential Transition of Displacement Distribution in Polymer Nanocomposites via Adsorption-Induced Trapping | ACS Nano ACS ACS Publications C&EN CAS Find my institution Log In ACS Nano ACS Publications. Most Trusted. Most Cited. Most Read Share Share on Facebook Twitter WeChat Linked In Reddit Email ACS Nano All Publications/Website OR SEARCH CITATIONS My Activity Recently Viewed New Polycyclic Diamine Scaffolds from Dimerization of 3-Alkyl-1,4-dihydropyridines in Acidic Medium. Clinical Translation of Aptamers for COVID-19 Synthesis of an Advanced Intermediate of the Jatrophane Diterpene Pl-4: A Dibromide Coupling Approach Photoelectron Spectroscopic and Theoretical Studies of MmC6F5 Anionic Complexes (M = Pb and Bi; m = 1−4) Thermodynamics and Its Applications, Second Edition (Modell, Michael; Reid, Robert C.) Publications publications my …

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Oct 2023 • Scientific Reports

Full-optical photoacoustic imaging using speckle analysis and resolution enhancement by orthogonal pump patterns projection

Viktor Vorobev, David Weidmann, Sergey Agdarov, Yafim Beiderman, Nadav Shabairou, Matan Benyamin, Florian Klämpfl, Michael Schmidt, Dmitry Gorin, Zeev Zalevsky

This paper presents an approach for achieving full optical photoacoustic imaging with enhanced resolution utilizing speckle pattern analysis. The proposed technique involves projecting patterns derived from binary masks corresponding to orthogonal functions onto the target to elicit a photoacoustic signal. The resulting signal is then recorded using a high-speed camera and analyzed using correlation analysis of the speckle motion. Our results demonstrate the feasibility of this optical approach to achieve imaging with enhanced resolution without the need for physical contact with the target, opening up new possibilities for non-invasive medical imaging and other applications.

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Oct 2023 • arXiv preprint arXiv:2210.02743

Tracking nanoscale perturbation in active disordered media

Renu Yadav, Patrick Sebbah, Maruthi M Brundavanam

The disorder induced feedback makes random lasers very susceptible to any changes in the scattering medium. The sensitivity of the lasing modes to perturbations in the disordered systems have been utilized to map the regions of perturbation. A tracking parameter, that takes into account the cumulative effect of changes in the spatial distribution of the lasing modes of the system has been defined to locate the region in which a scatterer is displaced by a few nanometers. We show numerically that the precision of the method increases with the number of modes. The proposed method opens up the possibility of application of random lasers as a tool for monitoring locations of nanoscale displacement which can be useful for single particle detection and monitoring.

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Oct 2023

Applying Nuclear Forward Scattering as in situ and operando Tool for the Characterization of FeN4 moieties in the hydrogen evolution reaction

Nils Heppe, Charlotte Gallenkamp, Rifael Snitkoff-Sol, Stephen Paul, Nicole Segura-Salas, Dominik Moritz, Bernd Kaiser, Wolfram Jaegermann, Vasily Potapkin, Atefeh Jafari, Volker Schünemann, Olaf Leupold, Lior Elbaz, Vera Krewald, Ulrike Kramm

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.

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Oct 2023 • 244th ECS Meeting (October 8-12, 2023)

Computational Studies of Structure, Composition, and Electrochemical Behavior of Li-Ion Battery Components

Dan Major, Amreen Bano


Sep 2023 • Angewandte Chemie (International ed. in English)

Is “Water in Salt” Electrolytes the Ultimate Solution? Achieving High Stability of Organic Anodes in Diluted Electrolyte Solutions Via a Wise Anions Selection

Amey Nimkar, Khorsed Alam, Gil Bergman, Mikhael D Levi, Dan Thomas Major, Netanel Shpigel, Doron Aurbach

The introduction of the water‐in‐salt (WIS) concept, using highly concentrated electrolyte solutions to prevent water splitting and widen the electrochemical stability window, has greatly influenced modern aqueous batteries. The successful implementation of these electrolyte solutions in many electrochemical systems shifts the focus from diluted to WIS electrolyte solutions. Considering the high costs and the tendency of these nearly saturated solutions to crystallize, this trend can be carefully re‐evaluated. Herein we show that the stability of organic electrodes comprising the active material perylene‐3,4,9,10‐tetracarboxylic dianhydride (PTCDA), is strongly influenced by the solvation character of the anions rather than the concentration of the electrolyte solution. Even though the charging process of PTCDA involves solely insertion of cations (i.e., principal counter‐ions), surprisingly, the dominant factor influencing its …

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Sep 2023 • Journal of Vacuum Science & Technology B

Measuring and understanding the nanomechanical properties of halide perovskites and their correlation to structure—A perspective

Irit Rosenhek-Goldian, David Cahen, Sidney R Cohen

The class of materials termed halide perovskites has experienced a meteoric rise in popularity due to their potential for photovoltaic and related applications, rivaling the well-established silicon devices within a few short years of development. These materials are characterized by several intriguing properties, among them their mechanical behavior. The study of their response to stress is essential for proper device development, while being of fundamental scientific interest in its own right. In this perspective, we highlight the key concerns surrounding this topic, critically analyzing the measurement techniques and considering the challenges in the current level of understanding.

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Sep 2023 • Journal of Raman Spectroscopy

Enhancement of the E12g and A1g Raman modes and layer identification of 2H‐WS2 nanosheets with metal coatings

Bharathi Rajeswaran, Rajashree Konar, Rena Yitzhari, Gilbert Daniel Nessim, Yaakov Raphael Tischler

Raman spectroscopy in transition metal dichalcogenides (TMDCs) helps determine their structural information and layer dependency. Because it is non‐destructive and fast, it is an archetypal spectroscopic technique to investigate the structure and defects in TMDCs. In our earlier study, we used a metal‐dielectric coating to enhance Raman signal of WS2 because the Raman Spectra measured from WS2 coated on the standard Si/SiO2 was significantly lower. This metal‐dielectric coating allowed access to the otherwise unavailable E12g and A1g modes of WS2. In this study, we compare the Raman spectra of WS2 on a Si/SiO2 to that of metal layers (Au [200 nm] and Al [200 nm]). A significant enhancement in the Raman signal of 2‐3L WS2 is observed for both the Au and Al coatings. Although 200 nm Au coating enhances the Raman Signal better than the 10 nm Au coating, it does not resolve the other …

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Sep 2023 • Journal of The Electrochemical Society

The Effect of Titania Additives on the Performance of PEO-Based Solid Sodium Batteries: Bulk and Interfacial Aspects

Gayathri peta, hadas Alon-Yehezkel, Nagaprasad Reddy Samala, Shaul Bublil, Yuval Elias, Ilya Grinberg, Miryam Fayena-Greenstein, Doron Aurbach

Nanometric fillers are known to affect the electrochemical performance of polymer electrolytes. Here, nanowires and nanotubes of TiO2 with the same crystal structure are compared as additives to poly(ethylene oxide) based electrolytes for solid state sodium batteries. Electrochemical studies of symmetric cells with blocking and non-blocking electrodes examined the effects of the additive shapes on the bulk electrolyte and Na-electrolyte interface. Impedance spectroscopy was used as a major electroanalytical tool. To obtain a full perspective, all-solid-state batteries were evaluated. In galvanostatic measurements the filler shape effect is most noticeable at a high current density. TiO2 nanotubes improve the solid electrolyte behavior considerably more than titania nanowires. This effect is related mainly to the interface of the polymeric matrix with the electrodes.

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Sep 2023 • Joule

Stabilized Li-S batteries with anti-solvent-tamed quasi-solid-state reaction

Yatao Liu, Linhan Xu, Yongquan Yu, MengXue He, Han Zhang, Yanqun Tang, Feng Xiong, Song Gao, Aijun Li, Jianhui Wang, Shenzhen Xu, Doron Aurbach, Ruqiang Zou, Quanquan Pang

The transition from dissolution-precipitation to quasi-solid-state sulfur reaction promises restricted polysulfide shuttle and lean electrolyte operation of Li-S batteries but incurs poor reaction kinetics. We here demonstrate that structural reorganization of sparingly solvating electrolytes (SSEs)—which is uniquely afforded by using low-density and low-cost aromatic anti-solvents—is vital for taming the quasi-solid-state sulfur reaction. Aromatic anti-solvents disrupt the interconnected structure of concentrated tetrahydrofuran (THF) electrolyte, uniquely creating subdomains that act to dissolve elemental sulfur, thus accelerating its consumption and re-formation while maintaining ultralow polysulfides solubility. The altered subdomains further result in robust solid electrolyte interphase (SEI) on lithium metal. As a result, the Li-S cell with a 3 mgsulfur cm−2 sulfur cathode can cycle steadily for ∼160 cycles with a lean …

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Sep 2023 • arXiv preprint arXiv:2309.13126

Stretched-exponential relaxation in weakly-confined Brownian systems through large deviation theory

Lucianno Defaveri, Eli Barkai, David A Kessler

Stretched-exponential relaxation is a widely observed phenomenon found in glassy systems. It was previously modeled with non-Markovian dynamics reflecting a memory effect. Here, we study a Brownian particle under the influence of a confining, albeit weak, potential field that grows with distance as a sub-linear power law. We find that for this memoryless model, observables display stretched-exponential relaxation. The probability density function of the system is studied using a rate function ansatz. We obtain analytically the stretched-exponential exponent along with an anomalous power-law scaling of length with time. The rate function exhibits a point of nonanalyticity, indicating a dynamical phase transition. In particular, the rate function is double-valued both to the left and right of this point, leading to four different rate functions, depending on the choice of initial conditions and symmetry.

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Sep 2023 • Physical Review E

Controls that expedite first-passage times in disordered systems

Marc Höll, Alon Nissan, Brian Berkowitz, Eli Barkai

First-passage time statistics in disordered systems exhibiting scale invariance are studied widely. In particular, long trapping times in energy or entropic traps are fat-tailed distributed, which slow the overall transport process. We study the statistical properties of the first-passage time of biased processes in different models, and we employ the big-jump principle that shows the dominance of the maximum trapping time on the first-passage time. We demonstrate that the removal of this maximum significantly expedites transport. As the disorder increases, the system enters a phase where the removal shows a dramatic effect. Our results show how we may speed up transport in strongly disordered systems exploiting scale invariance. In contrast to the disordered systems studied here, the removal principle has essentially no effect in homogeneous systems; this indicates that improving the conductance of a poorly …

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Sep 2023 • arXiv preprint arXiv:2309.13197

X-ray Parametric Down Conversion at the APS Synchrotron

NJ Hartley, D Hodge, T Buckway, R Camacho, P Chow, E Christie, A Gleason, S Glenzer, A Halavanau, AM Hardy, C Recker, S Sheehan, S Shwartz, H Tarvin, M Ware, J Wunschel, Y Xiao, RL Sandberg, G Walker

We present measurements of X-ray Parametric Down Conversion at the Advanced Photon Source synchrotron facility. We use an incoming pump beam at 22 keV to 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.

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Sep 2023 • arXiv preprint arXiv:2109.04237

Study of entanglement via a multi-agent dynamical quantum game

Bar Y Peled, Amit Te'eni, Eliahu Cohen, Avishy Carmi

At both conceptual and applied levels, quantum physics provides new opportunities as well as fundamental limitations. We hypothetically ask whether quantum games inspired by population dynamics can benefit from unique features of quantum mechanics such as entanglement and nonlocality. For doing so we extend quantum game theory and demonstrate that in certain models mimicking ecological systems where several predators feed on the same prey, the strength of quantum entanglement between the various species has a profound effect on the asymptotic behavior of the system. For example, if there are sufficiently many predator species who are all equally correlated with their prey, they are all driven to extinction. Our results are derived in two ways: by analyzing the asymptotic dynamics of the system, and also by modeling the system as a quantum correlation network. The latter approach enables us to …

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Sep 2023 • Journal of Power Sources 579, 233312, 2023

Lead-acid batteries and lead–carbon hybrid systems: A review

Naresh Vangapally, Tirupathi Rao Penki, Yuval Elias, Sadananda Muduli, Satyanarayana Maddukuri, Shalom Luski, Doron Aurbach, Surendra Kumar Martha

Lead-acid systems dominate the global market owing to simple technology, easy fabrication, availability, and mature recycling processes. However, the sulfation of negative lead electrodes in lead-acid batteries limits its performance to less than 1000 cycles in heavy-duty applications. Incorporating activated carbons, carbon nanotubes, graphite, and other allotropes of carbon and compositing carbon with metal oxides into the negative active material significantly improves the overall health of lead-acid batteries. Carbons play a vital role in advancing the properties of lead-acid batteries for various applications, including deep depth of discharge cycling, partial state-of-charge, and high-rate partial state-of-charge cycling. Therefore, lead-carbon hybrid batteries and supercapacitor systems have been developed to enhance energy-power density and cycle life. This review article provides an overview of lead-acid …

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Sep 2023 • Nucleic Acids Research

IGHV allele similarity clustering improves genotype inference from adaptive immune receptor repertoire sequencing data

Ayelet Peres, William D Lees, Oscar L Rodriguez, Noah Y Lee, Pazit Polak, Ronen Hope, Meirav Kedmi, Andrew M Collins, Mats Ohlin, Steven H Kleinstein, Corey T Watson, Gur Yaari

In adaptive immune receptor repertoire analysis, determining the germline variable (V) allele associated with each T- and B-cell receptor sequence is a crucial step. This process is highly impacted by allele annotations. Aligning sequences, assigning them to specific germline alleles, and inferring individual genotypes are challenging when the repertoire is highly mutated, or sequence reads do not cover the whole V region. Here, we propose an alternative naming scheme for the V alleles, as well as a novel method to infer individual genotypes. We demonstrate the strengths of the two by comparing their outcomes to other genotype inference methods. We validate the genotype approach with independent genomic long-read data. The naming scheme is compatible with current annotation tools and pipelines. Analysis results can be converted from the proposed naming scheme to the nomenclature determined …

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