bluuebunny/crossref_metadata_2025_split huggingface dataset:
Assessment of Glial Fibrillary Acidic Protein Binding to the Surface of Leukocytes with Dark‐Field Imaging and Computational Analysis
Authors: Peng Fei , Jeong Sinyoung , Gonzalez German , Marks Haley , Ho Alexander , Roussakis Emmanuel , Krauledat Petra B. , Hansen Peter , Evans Conor L. 
Published: January 2021

AbstractThe glial fibrillary acidic protein (GFAP) is widely established as a traumatic brain injury (TBI) biomarker and can be used in early diagnosis. As essential primary human immune cells, leukocytes are recruited to injured cerebral sites during TBI response, where they can interact with and potentially bind to TBI biomarkers. To date, no studies have demonstrated ultra‐low GFAP binding enumeration on leukocytes. Herein, a dark‐field imaging technique coupled with computational analysis is introduced to quantify GFAP bound to peripheral blood mononuclear cells (PBMCs). Dark‐field microscopy (DFM) with a custom‐written image acquisition software is developed for rapid 3D PBMC imaging by utilizing specific antiGFAP monoclonal antibody functionalized gold nanoparticles (antiGFAP‐AuNPs) as contrast‐generating probes. Subsequently, the developed algorithm is utilized in processing thousands of acquired images for rapid visualization and enumeration of bound antiGFAP‐AuNP on each leukocyte. The proposed method is demonstrates the specific binding of GFAP to the surface of PBMCs on a healthy donor blood. Thereafter, subpopulations of PBMCs with antiGFAP‐AuNP binding are identified with the assistance of fluorescence imaging and DFM imaging, paving a new way to understanding the relationship between TBI and leukocyte classes. Hence, this study offers a rapid and ultra‐sensitive strategy for biomarker assessment following TBI.
Radiolabeling of Gold Nanocages for Potential Applications in Tracking, Diagnosis, and Image‐Guided Therapy
Authors: Qiu Jichuan , Liu Yongjian , Xia Younan 
Published: January 2021

AbstractGold nanocages (AuNCs) have emerged as a novel class of multifunctional nanomaterials with an array of applications in nanomedicine, including drug delivery, controlled release, as well as disease diagnosis and treatment. Labeling AuNCs with radionuclides not only offers additional therapeutic capabilities but also makes it easy to analyze their biodistribution, monitor their uptake by the tissue or organ of interest, and optimize their performance in both diagnosis and treatment. Here, an introduction to the chemical synthesis and optical properties of AuNCs is provided in the beginning. The methods developed for their radiolabeling are then showcased, followed by the use of radiolabeled AuNCs in tracking and quantifying their pharmacokinetics, including biodistribution, tumor uptake, and intratumoral distribution. Finally, their potential applications in targeted imaging and image‐guided therapy are discussed.
Synthetic Kramers Pair in Phononic Elastic Plates and Helical Edge States on a Dislocation Interface
Authors: Liu Ting‐Wei , Semperlotti Fabio 
Published: January 2021

AbstractIn conventional theories, topological band properties are intrinsic characteristics of the bulk material and do not depend on the choice of the reference frame. In this scenario, the principle of bulk‐edge correspondence can be used to predict the existence of edge states between topologically distinct materials. In this study, a 2D elastic phononic plate is proposed with a Kekulé‐distorted honeycomb pattern engraved on it. It is found that the pseudospin and the pseudospin‐dependent Chern numbers are not invariant properties, and the number is no longer a sufficient indicator to examine the existence of the edge state. The distinctive pseudospin texture and the pseudomagnetic field are also revealed. Finally, the synthetic helical edge states are successfully devised and experimentally implemented on a dislocation interface connecting two subdomains with bulk pattern identical up to a relative translation. The edge state is also imaged via laser vibrometry.
Ultrasmall, Bright, and Photostable Fluorescent Core–Shell Aluminosilicate Nanoparticles for Live‐Cell Optical Super‐Resolution Microscopy
Authors: Erstling Jacob A. , Hinckley Joshua A. , Bag Nirmalya , Hersh Jessica , Feuer Grant B. , Lee Rachel , Malarkey Henry F. , Yu Fei , Ma Kai , Baird Barbara A. , Wiesner Ulrich B. 
Published: January 2021

AbstractStochastic optical reconstruction microscopy (STORM) is an optical super‐resolution microscopy (SRM) technique that traditionally requires toxic and non‐physiological imaging buffers and setups that are not conducive to live‐cell studies. It is observed that ultrasmall (<10 nm) fluorescent core–shell aluminosilicate nanoparticles (aC’ dots) covalently encapsulating organic fluorophores enable STORM with a single excitation source and in a regular (non‐toxic) imaging buffer. It is shown that fourfold coordinated aluminum is responsible for dye blinking, likely via photoinduced redox processes. It is demonstrated that this phenomenon is observed across different dye families leading to probes brighter and more photostable than the parent free dyes. Functionalization of aC’ dots with antibodies allows targeted fixed cell STORM imaging. Finally, aC’ dots enable live‐cell STORM imaging providing quantitative measures of the size of intracellular vesicles and the number of particles per vesicle. The results suggest the emergence of a powerful ultrasmall, bright, and photostable optical SRM particle platform with characteristics relevant to clinical translation for the quantitative assessment of cellular structures and processes from live‐cell imaging.
Van der Waals PdSe2/WS2 Heterostructures for Robust High‐Performance Broadband Photodetection from Visible to Infrared Optical Communication Band
Authors: Kang Xiaolin , Lan Changyong , Li Fangzhou , Wang Wei , Yip SenPo , Meng You , Wang Fei , Lai Zhengxun , Liu Chuntai , Ho Johnny C 
Published: January 2021

AbstractDue to excellent electrical and optoelectronic properties, 2D transition metal dichalcogenides and their van der Waals (vdW) heterostructures have attracted great attention for broadband optoelectronics. Here, an unreported vdW PdSe2/WS2 heterostructure is developed for robust high‐performance broadband photodetection from visible to infrared optical communication band. These heterostructure devices are simply formed by direct selenization of Pd films pre‐deposited on the chemical vapor deposited monolayer WS2, followed by wet‐transfer onto device substrates with pre‐patterned electrodes. Importantly, the obtained heterostructure device exhibits an impressive broadband spectral photoresponse with response times less than 100 ms for different wavelength regions (532 to 1550 nm), where this performance is significantly better than that of pristine monolayer WS2 devices. This performance enhancement is attributed to the type I band alignment of the heterostructure. Under illumination, both intralayer and interlayer excitations are involved to generate carriers in the relevant layer, enabling the broadband photoresponse. Photocarriers would then undergo charge separation in the depletion region with electrons transferred into the charge transport layer of WS2 through the built‐in electric field, followed by the relaxation to valance band via interlayer or intralayer transition. All these findings can indicate the promising potential of vdW PdSe2/WS2 heterostructures for next‐generation high‐performance optoelectronics.
Recent Trends in the Synthesis and Mechanistic Implications of Phenanthridines
Authors: Talukdar Vishal , Vijayan Ajesh , Kumar Katari Naresh , Radhakrishnan K. V. , Das Parthasarathi 
Published: January 2021

AbstractPhenanthridine derivatives are one of the most intensively studied families of biologically active compounds. There has been considerable scientific interest in the turn of this century in the synthesis of these N‐containing heterocycles as they are prevalent in many alkaloids and also possess striking biological activities including antibacterial, antifungal, antitumor activities. In this regard, a number of synthetic approaches toward the construction of phenanthridine moieties with various substituents, and to increase their yield have been developed by the synthetic organic community. Even though many researchers have developed various innovative methods for the synthesis of phenanthridine derivatives for the past few years, still there is substantial scope for the discovery of novel synthetic methods. In this review, the latest developments in the diverse synthetic strategies of phenanthridine derivatives in the presence and absence of metals were described. The present review also enlightens the use of different reagents, the diversity of the substrates identified, and the plausible mechanisms unravelled towards the construction of these biologically relevant scaffolds.magnified image
Palladium‐Catalyzed Hydroarylation of Homopropargyl Iodoindoles with Concurrent Alkyl and Iodonium Migrations
Authors: Martín Irene , Aragoncillo Cristina , Almendros Pedro 
Published: January 2021

AbstractA selective palladium‐catalyzed C(sp) arylation/carbocyclization/iodonium migration reaction sequence has been accomplished. Novel 2‐iodo‐1‐aryl‐9H‐carbazoles are now easily available. As this result is contrary to the selectivity observed using gold catalysis, the formation of 2‐iodocarbazoles is noticeable, suggesting a metal‐controlled cyclization through chemo‐ and regioselective 1,2‐alkyl migration and 1,4‐iodonium migration.magnified image
Polarization Energies from Efficient Representation of the Linear Density–Density Response Function
Authors: Dreßler Christian , Sebastiani Daniel 
Published: January 2021

AbstractThe authors present a proof‐of‐concept study for the calculation of atomic forces on a solvated molecule by means of the linear density–density response function in its moment expanded representation. The density–density response function represents an efficient way to compute molecular forces for arbitrary external potentials via an ab initio scheme, without the need to perform an explicit self‐consistent quantum chemical calculation for each configuration of the chemical environment. Here, the authors show that it is indeed possible to determine the atomic forces of interacting bulk‐like molecular complexes due to polarization effects of the surrounding molecules with good accuracy. This study represents a significant step the practical applicability of the approach, which is still in a development phase. The potential application of the computational scheme in terms of molecular dynamics simulations is illustrated by considering a variety of cluster conformations, as they would be found within a molecular dynamics trajectory.
Critical Coupling and Perfect Absorption Using α‐MoO3 Multilayers in the Mid‐Infrared
Authors: Dong Daxing , Liu Youwen , Fu Yangyang 
Published: January 2021

Abstractα‐Phase molybdenum trioxide(α‐MoO3) is a biaxial van der Waals semiconductor that can naturally support anisotropic phonon polaritons with elliptic and hyperbolic in‐plane dispersion. α‐MoO3 can meet critical coupling (CC) condition for both transverse magnetic (TM) and transverse electric (TE) polarizations along the x and y directions and exhibit high absorption in the mid‐infrared region due to strong phonon polaritons. In this study, an absorber composed of few‐layer α‐MoO3 and one‐dimensional photonic crystal separated by a cavity is proposed. Perfect absorption for TE and TM polarized light is achieved at the longitudinal and transverse optical phonon frequencies, respectively. The underlying mechanism of perfect absorption is investigated by using coupled mode theory and simulating electric field and power dissipation profiles. The results prove that CC is responsible for the perfect absorption. Moreover, the influence of the thickness of α‐MoO3 layer, width of cavity between α‐MoO3 and photonic crystal, and angle of incident light on the CC and absorption performance are examined. Accordingly, the rules for realizing perfect absorption at different operation frequencies are established. Overall, this study provides useful insights on designing a perfect absorber based on α‐MoO3 for detection and sensing applications in the mid‐infrared region.
Elektrooxidative Rhodium‐katalysierte [5+2]‐Anellierung durch C‐H/O‐H‐Aktivierung
Authors: Wang Yulei , Oliveira João C. A. , Lin Zhipeng , Ackermann Lutz 
Published: January 2021

AbstractElektrooxidative Anellierungen mittels übergangsmetallkatalysierter C‐H‐Aktivierung haben sich als eine transformative Strategie für den schnellen Aufbau von fünf‐ und sechsgliedrigen Heterocyclen erwiesen. Im Gegensatz dazu berichten wir hier über die ersten elektrochemischen metallkatalysierten [5+2]‐Cycloadditionen für die Synthese von wertvollen Benzoxepinstrukturen durch C‐H/O‐H‐Aktivierung. Die effiziente Alkinanellierung zeichnet sich durch eine große Anwendungsbreite mit Elektrizität als einzigem Oxidationsmittel aus. Mechanistische Studien deuten auf einen Rhodium(III/I)‐Mechanismus hin, welcher über einen Benzoxepin‐koordinierten Rhodium(I)‐Sandwichkomplex als Katalysatorruhezustand und eine anodische Reoxidation zu Rhodium(III) verläuft.
Zum Mechanismus der elektrochemischen Dimerisierung von CO2 zu Oxalsäure
Authors: Kaiser U. , Heitz E. 
Published: January 2021

AbstractBei der elektrochemischen Reduktion von CO2 in wäßrigen Elektrolyten entsteht Ameisensäure,

während Versuche, mehrgliedrige Carbonsäuren herzustellen, bisher mißlangen. In aprotischen Lösungsmitteln ist die Reduktion von CO2 zu Oxalsäure möglich, da die zur Bildung von Ameisensäure notwendigen Protonen fehlen. Zwei Reaktionen sind zu diskutieren:

Die Art der Reduktion wird durch das Elektrodenmaterial und das Lösungsmittel beeinflußt. Elektrodenmaterialien, die CO2 stark chemisorbieren, begünstigen Reaktion (3). Schwach nukleophile aprotische Lösungsmittel (Propylencarbonat, Acetonitril) begünstigen (2). Bei teilaprotischen Bedingungen entstehen neben Ameisensäure und Oxalsäure die Reduktionsprodukte der Oxalsäure: Glykoll‐, Glyoxyl‐, Wein‐, Äpfel‐ und Bernsteinsäure.Die Versuche wurden in zwei‐ oder dreigeteilten Zellen durchgeführt. Als Trennwände dienten Anionen‐ und Kationenaustauschermembranen, um die Migration und Diffusion der an der Kathode gebildeten Carbonsäureanionen in den Anodenraum und umgekehrt von anodisch gebildeten Produkten in den Kathodenraum zu verhindern. Die Stromausbeute ist abhängig von den Reaktionsbedingungen; bisher wurden etwa 60% erreicht.Das erhaltene Carbonsäure‐Produktgemisch wurde mittels der Hochdruckflüssigkeitschromatographie analysiert.
Mixing and oxygen transfer characteristics of a microplate bioreactor with surface‐attached microposts
Authors: Fisher Justin T. , Gurney Travis O. , Mason Brittany M. , Fisher Jay K. , Kelly William J. 
Published: January 2021

AbstractBioprocess optimization for cell‐based therapies is a resource heavy activity. To reduce the associated cost and time, process development may be carried out in small volume systems, with the caveat that such systems be predictive for process scale‐up. The transport of oxygen from the gas phase into the culture medium, characterized using the volumetric mass transfer coefficient, kLa, has been identified as a critical parameter for predictive process scale‐up. Here, we describe the development of a 96‐well microplate with integrated Redbud Posts to provide mixing and enhanced kLa. Mixing in the microplate is characterized by observation of dyes and analyzed using the relative mixing index (RMI). The kLa is measured via dynamic gassing out method. Actuating Redbud Posts are shown to increase rate of planar homogeneity (2 min) verse diffusion alone (120 min) and increase oxygenation, with increasing stirrer speed (3500‐9000 rpm) and decreasing fill volume (150‐350 μL) leading to an increase in kLa (4‐88 h−1). Significant increase in Chinese Hamster Ovary growth in Redbud Labs vessel (580,000 cells mL‐1) versus the control (420,000 cells mL‐1); t(12.814) = 8.3678, p ≤ .001), and CD4+ Naïve cell growth in the microbioreactor indicates the potential for this technology in early stage bioprocess development and optimization.
Shoulder pad and macroglossia: “two signs of AL amyloidosis”
Authors: Suganthan Navaneethakrishnan , Navaradnam Piratheepan , Sujanitha Vathulan 
Published: January 2021

Abstract“Shoulder pad” sign resulting from deposition of amyloid in the periarticular soft tissue is rare but it is pathognomonic for immunoglobulin amyloidosis (AL). Although the detection remains a challenge, it gives a strong clue leading to prompt diagnosis.
Successful detection of covert paroxysmal atrial fibrillation due to insertable cardiac monitor in embolic stroke of undetermined source in a patient with situs inversus totalis
Authors: Kasai Yuhei , Shakya Sandeep , Miyaji Kotaro , Kanda Junji 
Published: January 2021

AbstractInsertable cardiac monitors in patients with situs inversus totalis can detect atrial arrhythmia as a cause of embolic stroke. It is important to premap the position of ICM in order to clearly visualize the P wave.
Concomitant Polymorphism and Nucleation Control of DL‐Methionine Through Antisolvent Crystallization
Authors: Suresh Manivel , Srinivasan Karuppannan 
Published: January 2021

AbstractThe concomitant polymorphism of the sulfur‐containing essential amino acid DL‐methionine was revealed, and α‐ and β‐polymorphic forms were separated from aqueous solution through antisolvent crystallization with ethanol as antisolvent. The addition of different volume fractions of ethanol into the mother solution reduces the solubility of DL‐methionine in double‐distilled water and in turn proportionately generates a range of supersaturation levels. This induces the nucleation of a stable β‐polymorph at low supersaturation levels, a mixture of α‐ and β‐ polymorphs at intermediate supersaturation levels, and a metastable α‐form at high supersaturation levels. Needle‐shaped α‐polymorphs and platy‐shaped β‐polymorphs were well distinguished through in‐situ optical microscopic analysis and their structural confirmation was done by X‐ray diffraction analysis.
Hybrid Transition‐Metal Oxide and Nitride@N‐Doped Reduced Graphene Oxide Electrodes for High‐Performance, Flexible, and All‐Solid‐State Supercapacitors
Authors: Jiang Lili , Mei Xiaotong , Gan Donglin , Song Shaowei , Lei Xiaobo , Cai Fanggong , Wang Yaqin , Zhang Qinyong , Lu Xiong , Ren Zhifeng 
Published: January 2021

AbstractNanoscale composites for high‐performance electrodes employed in flexible, all‐solid‐state supercapacitors are being developed. A series of binder‐free composites, each consisting of a transition bimetal oxide, a metal oxide, and a metal nitride grown on N‐doped reduced graphene oxide (rGO)‐wrapped nickel foam are obtained by using a universal strategy. Three different transition metals, Co, Mo, and Fe, are separately compounded with nickel ions, which originate from the nickel foam, to form three composites, NiCoO2@Co3O4@Co2N, NiMoO4@MoO3@Mo2N, and NiFe2O4@Fe3O4@Fe2N, respectively. These as‐prepared active materials have similar regular variation patterns in their properties, including better conductivity and battery‐mimicking pseudocapacitance, which result in their high whole‐electrode capacitance performance [2598.3 F g−1 (39.85 F cm−2), 3472.6 F g−1 (41.43 F cm−2) and 1907.5 F g−1 (3.41 F cm−2) for the composites incorporating Co, Mo, and Fe, respectively]. The as‐assembled flexible, all‐solid‐state NiCoO2@Co3O4@Co2N//KOH/PVA//NiCoO2@Co3O4@Co2N device can be easily bent and exhibits high energy density and power density of 92.8 Wh kg−1 and 1670.4 W kg−1, respectively. The universality of this design strategy could allow it to be employed in producing hybrid materials for high‐performance energy‐storage devices.
Fluorides of Silver Under Large Compression**
Authors: Kurzydłowski Dominik , Derzsi Mariana , Zurek Eva , Grochala Wojciech 
Published: January 2021

AbstractThe silver‐fluorine phase diagram has been scrutinized as a function of external pressure using theoretical methods. Our results indicate that two novel stoichiometries containing Ag+ and Ag2+ cations (Ag3F4 and Ag2F3) are thermodynamically stable at ambient and low pressure. Both are computed to be magnetic semiconductors under ambient pressure conditions. For Ag2F5, containing both Ag2+ and Ag3+, we find that strong 1D antiferromagnetic coupling is retained throughout the pressure‐induced phase transition sequence up to 65 GPa. Our calculations show that throughout the entire pressure range of their stability the mixed‐valence fluorides preserve a finite band gap at the Fermi level. We also confirm the possibility of synthesizing AgF4 as a paramagnetic compound at high pressure. Our results indicate that this compound is metallic in its thermodynamic stability region. Finally, we present general considerations on the thermodynamic stability of mixed‐valence compounds of silver at high pressure.
Metalloradical Cations and Dications Based on Divinyldiphosphene and Divinyldiarsene Ligands
Authors: Sharma Mahendra K. , Rottschäfer Dennis , Neumann Beate , Stammler Hans‐Georg , Danés Sergi , Andrada Diego M. , van Gastel Maurice , Hinz Alexander , Ghadwal Rajendra S. 
Published: January 2021

AbstractMetalloradicals are key species in synthesis, catalysis, and bioinorganic chemistry. Herein, two iron radical cation complexes (3‐E)GaCl4 [(3‐E).+ = [{(IPr)C(Ph)E}2Fe(CO)3].+, E = P or As; IPr = C{(NDipp)CH}2, Dipp = 2,6‐iPr2C6H3] are reported as crystalline solids. Treatment of the divinyldipnictenes {(IPr)C(Ph)E}2 (1‐E) with Fe2(CO)9 affords [{(IPr)C(Ph)E}2Fe(CO)3] (2‐E), in which 1‐E binds to the Fe atom in an allylic (η3‐EECvinyl) fashion and functions as a 4e donor ligand. Complexes 2‐E undergo 1e oxidation with GaCl3 to yield (3‐E)GaCl4. Spin density analysis revealed that the unpaired electron in (3‐E).+ is mainly located on the Fe (52–64 %) and vinylic C (30–36 %) atoms. Further 1e oxidation of (3‐E)GaCl4 leads to unprecedented η3‐EECvinyl to η3‐ECvinylCPh coordination shuttling to form the dications (4‐E)(GaCl4)2.