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Dec 2022 • Cell Reports Physical Science

A cost-effective water-in-salt electrolyte enables highly stable operation of a 2.15-V aqueous lithium-ion battery

Meital Turgeman, Vered Wineman-Fisher, Fyodor Malchik, Arka Saha, Gil Bergman, Bar Gavriel, Tirupathi Rao Penki, Amey Nimkar, Valeriia Baranauskaite, Hagit Aviv, Mikhael D Levi, Malachi Noked, Dan Thomas Major, Netanel Shpigel, Doron Aurbach

Extensive efforts are currently underway to develop safe and cost-effective electrolytes for large-scale energy storage. In this regard, water-based electrolytes may be an attractive option, but their narrow electrochemical stability window hinders their realization. Although highly concentrated fluorinated electrolytes have been shown to be highly effective in suppression of water splitting, enabling significant widening of the applied potential range, they utilize expensive salts (e.g., lithium bis(trifluoromethane sulfonyl) imide [LiTFSI] or lithium trifluoromethane sulfonate [LiOTf]); hence, they cannot be considered for practical applications. Here, we demonstrate a cost-effective aqueous electrolyte solution combining 14 M LiCl and 4 M CsCl that allows stable operation of a 2.15-V battery comprising a TiO2 anode and LiMn2O4 cathode. Addition of CsCl to the electrolyte plays a double role in system stabilization: the added …

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Dec 2022 • arXiv preprint arXiv:2212.07502

Entanglement measures for two-particle quantum histories

Danko Georgiev, Eliahu Cohen

Quantum entanglement is a key resource, which grants quantum systems the ability to accomplish tasks that are classically impossible. Here, we apply Feynman's sum-over-histories formalism to interacting bipartite quantum systems and introduce entanglement measures for bipartite quantum histories. Based on the Schmidt decomposition of the matrix comprised of the Feynman propagator complex coefficients, we prove that bipartite quantum histories are entangled if and only if the Schmidt rank of this matrix is larger than 1. The proposed approach highlights the utility of using a separable basis for constructing the bipartite quantum histories and allows for quantification of their entanglement from the complete set of experimentally measured sequential weak values. We then illustrate the non-classical nature of entangled histories with the use of Hardy's overlapping interferometers and explain why local hidden variable theories are unable to correctly reproduce all observable quantum outcomes. Our theoretical results elucidate how the composite tensor product structure of multipartite quantum systems is naturally extended across time and clarify the difference between quantum histories viewed as projection operators in the history Hilbert space or viewed as chain operators and propagators in the standard Hilbert space.

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Dec 2022 • Scientific Reports

Current dependence of the negative magnetoresistance in superconducting NbN nanowires

Zoharchen Sofer, Avner Shaulov, Yosef Yeshurun

Magnetoresistance measurements in amorphous NbN nanowires show that transport current affects their negative magnetoresistance (nMR) in a manner qualitatively similar to temperature. In particular, the current suppresses the nMR and, beyond a certain level it eliminates the effect altogether. As the temperature dependence of the nMR effect is more pronounced at low currents, similarly the current dependence of the effect is more pronounced at low temperatures. These results are discussed in terms of the phenomenological model which attributes the nMR to the interplay between the resistance originating from the rate of phase slips via the Josephson relation and the Ohmic contribution from quasiparticles charge imbalance that accompany fluctuations of the order parameter in the nanowire.

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Dec 2022 • The Journal of Physical Chemistry B

Origin of Catalysis by Nitroalkane Oxidase

Dan Thomas Major, Prashant Kumar Gupta, Jiali Gao

The rate of proton abstraction of the carbon acid nitroethane by Asp402 is accelerated by a factor of 108 in the enzyme nitroalkane oxidase (NAO) relative to that by the organic base acetate ion in water. The Cα proton of nitroalkanes is known to exhibit an abnormal correlation between its acidity strength and the rate of deprotonation, with an unusually slow rate of deprotonation in water. This work examines the origin of NAO catalysis, revealing that the rate enhancement by the enzyme is due to transition-state stabilization, restoring the normal behavior of the linear free energy relationship of Bronsted acids. Interestingly, NAO employs the ubiquitous cofactor flavin adenosine diphosphate (FAD) to perform the subsequent oxidation. Does the FAD cofactor also affect the catalytic rate of the initial proton transfer process of the overall nitroalkane oxidation? Classical molecular dynamics and path-integral simulations …

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Nov 2022

Ultrasound stimulation of piezoelectric nanocomposite hydrogels boosts cartilage regeneration

Leonardo Ricotti, Andrea Cafarelli, Cristina Manferdini, Diego Trucco, Lorenzo Vannozzi, Elena Gabusi, Francesco Fontana, Paolo Dolzani, Yasmin Saleh, Enrico Lenzi, Marta Columbaro, Manuela Piazzi, Jessika Bertacchini, Andrea Aliperta, Markys Cain, Paola Parlanti, Carsten Jost, Yirij Fedutik, Gilbert Nessim, Madina Telkhozhayeva, Eti Teblum, Erik Dumont, Chiara Delbaldo, Giorgia Codispoti, Lucia Martini, Matilde Tschon, Milena Fini, Gina Lisignoli

Osteoarthritis implies a progressive degeneration of the whole joint. Cartilage is particularly affected, with in ammation playing a pivotal role1. In recent years, cartilage regeneration has been pursued through several bioengineering strategies and using different stem cell types2-6. Adipose-derived mesenchymal stromal cells (ASCs) constitute an intriguing and minimally invasive option. However, the use of ASCs for cartilage regeneration is hampered by a relatively ine cient expression of key chondrogenic markers7. Thus, new strategies to boost both in situ targeting and chondrogenesis of ASCs are highly desirable. Here we show that ASCs embedded in a nanocomposite hydrogel including piezoelectric nanomaterials and graphene oxide nano akes, and stimulated with ultrasound waves with precisely controlled parameters (1 MHz and 250 mW/cm2, for 5 min once every two days for a period of 10 days) dramatically boost cell chondrogenic commitment. Furthermore, this stimulation regimen also has a considerable anti-in ammatory effect. The proposed nanocomposite hydrogel also shows excellent biocompatibility in vivo. Our results show for the rst time the chondrogenic potential of the combined piezoelectric nanoparticle-ultrasound stimulus; the proposed paradigm has the potential to trigger cartilage regeneration in osteoarthritis, focal cartilage defects and other pathological conditions involving cartilage lesions and degeneration. Future efforts should expand preclinical data, and target clinical applications of this therapeutic strategy.

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Nov 2022 • Materials

Phosphate-Trapping Liposomes for Long-Term Management of Hyperphosphatemia

Chen Tzror-Azankot, Adi Anaki, Tamar Sadan, Menachem Motiei, Rachela Popovtzer

Hyperphosphatemia is a typical complication of end-stage renal disease, characterized by elevated and life-threatening serum phosphate levels. Hemodialysis does not enable sufficient clearance of phosphate, due to slow cell-to-plasma kinetics of phosphate ions; moreover, dietary restrictions and conventional treatment with oral phosphate binders have low success rates, together with adverse effects. Here, we developed a new concept of phosphate-trapping liposomes, to improve and prolong the control over serum phosphate levels. We designed liposomes modified with polyethylene glycol and encapsulated with the phosphate binder ferric citrate (FC liposomes). These liposomes were found to trap phosphate ions in their inner core, and thereby lower free phosphate ion concentrations in solution and in serum. The FC liposomes showed higher phosphate binding ability as phosphate concentrations increased. Moreover, these liposomes showed a time-dependent increase in uptake of phosphate, up to 25 h in serum. Thus, our findings demonstrate effective long-term phosphate trapping by FC liposomes, indicating their potential to reduce serum phosphate toxicity and improve current management of hyperphosphatemia.

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Nov 2022 • Materials

Phosphate-Trapping Liposomes for Long-Term Management of Hyperphosphatemia

Chen Tzror-Azankot, Adi Anaki, Tamar Sadan, Menachem Motiei, Rachela Popovtzer

Hyperphosphatemia is a typical complication of end-stage renal disease, characterized by elevated and life-threatening serum phosphate levels. Hemodialysis does not enable sufficient clearance of phosphate, due to slow cell-to-plasma kinetics of phosphate ions; moreover, dietary restrictions and conventional treatment with oral phosphate binders have low success rates, together with adverse effects. Here, we developed a new concept of phosphate-trapping liposomes, to improve and prolong the control over serum phosphate levels. We designed liposomes modified with polyethylene glycol and encapsulated with the phosphate binder ferric citrate (FC liposomes). These liposomes were found to trap phosphate ions in their inner core, and thereby lower free phosphate ion concentrations in solution and in serum. The FC liposomes showed higher phosphate binding ability as phosphate concentrations increased. Moreover, these liposomes showed a time-dependent increase in uptake of phosphate, up to 25 h in serum. Thus, our findings demonstrate effective long-term phosphate trapping by FC liposomes, indicating their potential to reduce serum phosphate toxicity and improve current management of hyperphosphatemia.

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Nov 2022 • Scientific Reports

Characterization of alternative mRNA splicing in cultured cell populations representing progressive stages of human fetal kidney development

Yishay Wineberg, Itamar Kanter, Nissim Ben-Haim, Naomi Pode-Shakked, Efrat Bucris, Tali Hana Bar-Lev, Sarit Oriel, Harel Reinus, Yishai Yehuda, Rotem Gershon, Rachel Shukrun, Dekel Dov Bar-Lev, Achia Urbach, Benjamin Dekel, Tomer Kalisky

Nephrons are the functional units of the kidney. During kidney development, cells from the cap mesenchyme—a transient kidney-specific progenitor state—undergo a mesenchymal to epithelial transition (MET) and subsequently differentiate into the various epithelial cell types that create the tubular structures of the nephron. Faults in this transition can lead to a pediatric malignancy of the kidney called Wilms’ tumor that mimics normal kidney development. While human kidney development has been characterized at the gene expression level, a comprehensive characterization of alternative splicing is lacking. Therefore, in this study, we performed RNA sequencing on cell populations representing early, intermediate, and late developmental stages of the human fetal kidney, as well as three blastemal-predominant Wilms’ tumor patient-derived xenografts. Using this newly generated RNAseq data, we identified a set …

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Nov 2022 • Journal of The Electrochemical Society

Improving Li Anode Reversibility in Li–S Batteries by ZnO Coated Separators Using Atomic Layer Deposition

Shalev Blanga, Reut Yemini, Eti Teblum, Merav Tsubery, Sarah Taragin, Malachi Noked

Lithium-sulfur batteries (LSB) are considered a very attractive alternative to lithium-ion batteries due to their high theoretical capacity and low cost of the active materials. However, the realization of LSB is hostage to many challenges associated with the cathode and anode response to the electrochemical conditions inside the battery cell. While working with LSB, elemental sulfur undergoes multielectron reduction reactions until it is reduced to Li 2 S. The intermediate long chain lithium-polysulfide (LiPS) species are soluble, hence diffuse through the electrolyte solution from the cathode side to the anode. This" shuttle" phenomenon considered to be one of the main issues of LSB. Most effort in investigating LSB focused on the cathode side while only few considered the importance of the lithium anode reversibility and the separator role in preventing the" shuttle" phenomenon. In the current work, we use Atomic Layer …

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Nov 2022 • The Journal of Physical Chemistry C

Nanostructure-free Metal–Dielectric Stacks for Raman Scattering Enhancement and Defect Identification in CVD-Grown Tungsten Disulfide (2H-WS2) Nanosheets

Bharathi Rajeswaran, Rajashree Konar, Sriram Guddala, Tali Sharabani, Eti Teblum, Yaakov Raphael Tischler, Gilbert Daniel Nessim

Low-wavenumber Raman (LWR) spectroscopy determines signatures in structural information and layer-to-layer dependency of transition metal dichalcogenides (TMDCs). It supports proper 2D TMDC analysis and subsequent layer verification. The nondestructive nature and ultrafast detection make LWR measurements imperative for layer variations and defect investigations. Interference-enhanced Raman scattering utilizes a metal–dielectric layer to enhance the Raman signal. This has been used to study graphene, C60, and Te. Here, we investigate using Al/Al2O3 coatings to enhance the LWR scattering of different 2H-WS2 layers and understand the structures of these large-area nanosheets. Phase-pure WS2 is synthesized by CVD, and the layers are exfoliated via ultrasonication at 80 kHz. Layers were drop-casted on Al/Al2O3 coatings of different thicknesses of Al2O3 to study differences in bilayers up to a …

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Nov 2022 • Beilstein Journal of Organic Chemistry

Synthetic study toward the diterpenoid aberrarone

Liang Shi, Zhiyu Gao, Yiqing Li, Yuanhao Dai, Yu Liu, Lili Shi, Hong-Dong Hao

An approach to aberrarone, an antimalarial diterpenoid natural product with tetracyclic skeleton is reported. Key to the stereoselective preparation of the 6-5-5 tricyclic skeleton includes the mediation of Nagata reagent for constructing the C1 all-carbon quaternary centers and gold-catalyzed cyclopentenone synthesis through C–H insertion.

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Nov 2022 • The Journal of Physical Chemistry C

Nanostructure-free Metal–Dielectric Stacks for Raman Scattering Enhancement and Defect Identification in CVD-Grown Tungsten Disulfide (2H-WS2) Nanosheets

Bharathi Rajeswaran, Rajashree Konar, Sriram Guddala, Tali Sharabani, Eti Teblum, Yaakov Raphael Tischler, Gilbert Daniel Nessim

Low-wavenumber Raman (LWR) spectroscopy determines signatures in structural information and layer-to-layer dependency of transition metal dichalcogenides (TMDCs). It supports proper 2D TMDC analysis and subsequent layer verification. The nondestructive nature and ultrafast detection make LWR measurements imperative for layer variations and defect investigations. Interference-enhanced Raman scattering utilizes a metal–dielectric layer to enhance the Raman signal. This has been used to study graphene, C60, and Te. Here, we investigate using Al/Al2O3 coatings to enhance the LWR scattering of different 2H-WS2 layers and understand the structures of these large-area nanosheets. Phase-pure WS2 is synthesized by CVD, and the layers are exfoliated via ultrasonication at 80 kHz. Layers were drop-casted on Al/Al2O3 coatings of different thicknesses of Al2O3 to study differences in bilayers up to a …

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Nov 2022 • Solid State Ionics

Multi-spray pyrolysis for combinatorial synthesis of materials libraries and their high-throughput screening: Application to Li-ion conducting electrolytes

Shay Tirosh, Niv Aloni, David Cahen, Diana Golodnitsky

We present a multi-head spray pyrolysis system and its application in high-throughput combinatorial synthesis for research of solid Li-ion conductors. Each spraying nozzle is fed with a separate precursor solution. The overlap of areas that are sprayed leads to unprecedented composition flexibility of the films obtained after pyrolysis. Thus, a library with a continuous composition spread of a Li-La-P-O model system is formed. The Li-ion conduction was determined on 169 cells of the library, using high throughput impedance measurements in a controlled environment. While the activation energies that were found were relatively small, Li-ion conduction was still low. This low mobility is hypothesized to originate from the sub-optimal occupation of Li sites in the non-stoichiometric materials' lattices, and/or porosity and tortuosity issues, which in turn, reduces their effective concentration and contribution to ion transport. In …

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Nov 2022 • Progress in Retinal and Eye Research 89, 101029, 2022

Inherited retinal diseases: linking genes, disease-causing variants, and relevant therapeutic modalities

Nina Schneider, Yogapriya Sundaresan, Prakadeeswari Gopalakrishnan, Avigail Beryozkin, Mor Hanany, Erez Y Levanon, Eyal Banin, Shay Ben-Aroya, Dror Sharon

Inherited retinal diseases (IRDs) are a clinically complex and heterogenous group of visual impairment phenotypes caused by pathogenic variants in at least 277 nuclear and mitochondrial genes, affecting different retinal regions, and depleting the vision of affected individuals. Genes that cause IRDs when mutated are unique by possessing differing genotype-phenotype correlations, varying inheritance patterns, hypomorphic alleles, and modifier genes thus complicating genetic interpretation. Next-generation sequencing has greatly advanced the identification of novel IRD-related genes and pathogenic variants in the last decade. For this review, we performed an in-depth literature search which allowed for compilation of the Global Retinal Inherited Disease (GRID) dataset containing 4,798 discrete variants and 17,299 alleles published in 31 papers, showing a wide range of frequencies and complexities among …

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Nov 2022 • Energy Storage Materials

Double gas treatment: A successful approach for stabilizing the Li and Mn-rich NCM cathode materials’ electrochemical behavior

Sandipan Maiti, Hadar Sclar, Judith Grinblat, Michael Talianker, Maria Tkachev, Merav Tsubery, Xiaohan Wu, Malachi Noked, Boris Markovsky, Doron Aurbach

Herein, a systematic surface modification approach via double gas (SO2 and NH3) treatment at elevated temperatures is described, aimed to achieve a stable electrochemical performance of Li and Mn-rich NCM cathode materials of a typical composition 0.33Li2MnO3•0.67LiNi0.4Co0.2Mn0.4O2 (HE-NCM). Partial surface reduction of Mn4+ and the formation of a modified interface comprising Li-ions conductive nano-sized Li2SO4/Li2SO3 phases are established. Li-coin cells’ prolonged cycling performance demonstrated significantly improved capacity retention (∼2.2 times higher than untreated cathode materials) for the double-gas-treated cathodes after 400 cycles at a 1.0 C rate. Stable discharge potential and lower voltage hysteresis during cycling were also achieved through the double gas treatment. Comparative electrochemical studies in full-pouch cells [vs. Graphite anodes] also demonstrated …

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Nov 2022 • Physical Review B

Universality and microstrain origin of the ramp reversal memory effect

Elihu Anouchi, Naor Vardi, Yoav Kalcheim, Ivan K Schuller, Amos Sharoni

The recently discovered ramp reversal memory (RRM) is a nonvolatile memory effect observed in correlated oxides with temperature-driven insulator–metal transitions (IMT). It appears as a resistance increase at predefined temperatures that are set or erased by simple heating–cooling (ie, ramp reversal) protocols. Until now RRM was measured for two materials: VO 2 and NdNiO 3. A heuristic model suggests that the RRM is caused by a local transition temperature increase at boundaries of spatially separated metallic and insulating domains during ramp reversal. However, there is no experimental measure of the magnitude of the effect, which is crucial for the development of a theoretical account of the RRM. Here we show that V 2 O 3 also shows RRM, including all related features, highlighting the generality of the effect. Moreover, an analysis of the RRM as an effective (average) increase of the critical …

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Nov 2022 • Advanced Energy Materials

Superstructure Variation and Improved Cycling of Anion Redox Active Sodium Manganese Oxides Due to Doping by Iron

Xiaodong Qi, Langyuan Wu, Zhiwei Li, Yuxuan Xiang, Yunan Liu, Kangsheng Huang, Elias Yuval, Doron Aurbach, Xiaogang Zhang

Anionic redox provides an effective way to overcome the capacity bottleneck of sodium‐ion batteries. A dominant role is played by the arrangement of alkali A and transition metal M in the NaxAyM1‐yO2 superstructure. Here, in situ X‐ray diffraction and ex situ 7Li nuclear magnetic resonance of P2 type Na0.6Li0.2Mn0.8O2 with ribbon‐ordered superstructure illustrate structural changes and explain the evolution of the electrochemical behavior of electrodes comprising this active mass, during cycling. Upon substitution of a small amount of manganese by iron, Na0.67Li0.2Mn0.73Fe0.07O2 is formed with a honeycomb‐ordered superstructure. Experimental characterizations and theoretical calculations elucidate the effect of iron on oxygen redox activity. The iron‐doped material considerably outperforms the undoped Na0.6Li0.2Mn0.8O2 as a cathode material for rechargeable Na‐ion batteries. This research reveals …

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Nov 2022 • ACS Applied Polymer Materials

Carbon Dot Biopolymer-Based Flexible Functional Films for Antioxidant and Food Monitoring Applications

Poushali Das, Sayan Ganguly, Syed Rahin Ahmed, Masoomeh Sherazee, Shlomo Margel, Aharon Gedanken, Seshasai Srinivasan, Amin Reza Rajabzadeh

Heteroatom-doped carbon dot (CD)-reinforced flexible, antioxidant, and UV-resistant polymeric thin films have been fabricated by a facile physical compounding strategy associated with the ‘cast and peel’ technique. The prepared CDs were found to be stable in aqueous media because of their zeta potential value (−5.85 mV). There was no significant change in the zeta potential values during 7 days of storage, indicating the long-term stability of CPCDs. CD-reinforced thermoplastic starch (TPS)/κ-carrageenan hybrid films have been developed as antioxidants to improve the shelf-life of agro-products. Besides this, they also qualified for mechanical strength (>40 MPa), transparency (∼77%), nondeteriorative dimensional integrity at a high relative humidity (∼97%), and UV-resistant properties. For assessing the food preservation behavior, the leaching of CDs also has been studied by time-dependent sustained …

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Nov 2022 • Crystal Growth & Design

Localized Heating Tailors Nucleation for Reproducible Growth of Thin Halide Perovskite Single Crystals

Sujit Kumar, Alexandra Rukban, Julia Sinisi, Vinayaka H Damle, David Cahen

Halide perovskites (HaPs) are functional semiconductors that can be prepared in a simple, near-room-temperature process. With thin polycrystalline HaP films, excellent solar cells, light-emitting diodes (LEDs), and (also as single crystals) high-energy radiation detectors have been demonstrated. The very low single-crystal defect densities make HaP thin single crystals (TSCs), instead of polycrystalline HaP films an attractive option, to boost device performances and for fundamental research. However, growing TSCs is challenging primarily because of random multiple nucleations, which, in the often-used space-confined geometry, is favored at the substrate boundaries, where loss of organo-amines and solvents occurs. We show that fewer and better-quality thin crystals nucleate and grow reproducibly away from the substrate edges in the substrate center, if we localize the heating (needed for inverse-temperature …

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Nov 2022 • arXiv preprint arXiv:2211.06278

Temperature-dependence of the CISS effect from measurements in Chiral molecular intercalation super-lattices

Subhajit Sarkar, Seif Alwan, Amos Sharoni, Yonatan Dubi

We detail here some matters arising from the recent paper by Qian et. al., Nature 606, pages 902-908 (2022). We demonstrate, based on data supplied by Qian et. al., and corroborated by theoretical modeling, that one of the central conclusions of the manuscript - namely the behavior of the chirality-induced spin-selectivity (CISS) effect at low temperatures - can actually be consistently interpreted in a different way, which is in fact opposite to the interpretation proposed by Qian et. al.

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Nov 2022 • Superconductor Science and Technology

Characterization of YBa2Cu3O7− δ coplanar resonator for microwave kinetic inductance detectors

Ariel Roitman, A Shaulov, Y Yeshurun

We demonstrate an improved YBa 2 Cu 3 O 7− δ-based microwave kinetic inductance detector with a quality factor and noise equivalent power, $\sim {10^{-12}}{\mkern 1mu}{\text {W}}{\mkern 1mu}{\sqrt {{\text {Hz}}}^{-1}} $ at 10 K. Zero field cooled (ZFC) and field cooled (FC) measurements of the magnetic field dependence of the resonance characteristics, show substantially different behavior, indicating that both the screening currents and vortices play a role. The ZFC measurements exhibit a sharp decrease of the resonance frequency, , and at low fields, up to the full penetration field, revealing the dominant role of the screening currents. In contrast, the FC measurements exhibit a moderate decrease of and with field, revealing the role of vortices and reflecting the field dependence of the penetration depth in a d-wave superconductor.

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