bluuebunny/crossref_metadata_2025_split huggingface dataset:
Phase‐Dependent Band Gap Engineering in Alloys of Metal‐Semiconductor Transition Metal Dichalcogenides
Authors: Wang Shuxi , Cavin John , Hemmat Zahra , Kumar Khagesh , Ruckel Alexander , Majidi Leily , Gholivand Hamed , Dawood Radwa , Cabana Jordi , Guisinger Nathan , Klie Robert F. , Khalili‐Araghi Fatemeh , Mishra Rohan , Salehi‐Khojin Amin 
Published: September 2020

AbstractBandgap engineering plays a critical role in optimizing the electrical, optical and (photo)‐electrochemical applications of semiconductors. Alloying has been a historically successful way of tuning bandgaps by making solid solutions of two isovalent semiconductors. In this work, a novel form of bandgap engineering involving alloying non‐isovalent cations in a 2D transition metal dichalcogenide (TMDC) is presented. By alloying semiconducting MoSe2 with metallic NbSe2, two structural phases of Mo0.5Nb0.5Se2, the 1T and 2H phases, are produced each with emergent electronic structure. At room temperature, it is observed that the 1T and 2H phases are semiconducting and metallic, respectively. For the 1T structure, scanning tunneling microscopy/spectroscopy (STM/STS) is used to measure band gaps in the range of 0.42–0.58 at 77 K. Electron diffraction patterns of the 1T structure obtained at room temperature show the presence of a nearly commensurate charge density wave (NCCDW) phase with periodic lattice distortions that result in an uncommon 4 × 4 supercell, rotated approximately 4° from the lattice. Density‐functional‐theory calculations confirm that local distortions, such as those in a NCCDW, can open up a band gap in 1T‐Mo0.5Nb0.5Se2, but not in the 2H phase. This work expands the boundaries of alloy‐based bandgap engineering by introducing a novel technique that facilitates CDW phases through alloying.
Thermally Activated Delayed Fluorescence Sensitization for Highly Efficient Blue Fluorescent Emitters
Authors: Abroshan Hadi , Zhang Yadong , Zhang Xiaoqing , Fuentes‐Hernandez Canek , Barlow Stephen , Coropceanu Veaceslav , Marder Seth R. , Kippelen Bernard , Brédas Jean‐Luc 
Published: September 2020

AbstractHyperfluorescence is emerging as a powerful strategy to develop optoelectronic devices with high‐color purity and enhanced stability. It requires appropriate integration of a sensitizer displaying efficient thermally activated delayed fluorescence (TADF) and an emitter displaying strong, narrow‐band fluorescence. Here, through a joint computational and experimental approach, an unprecedented, end‐to‐end systems level description of the electronic and optical processes that take place in a hyperfluorescent emissive layer composed of a TADF sensitizer, 2,5‐bis(2,6‐di(9H‐carbazol‐9‐yl)phenyl)‐1,3,4‐oxadiazole (4CzDPO), and a fluorescent emitter, 2,5,8,11‐tetra‐tert‐butylperylene (TBPe) is provided. The photophysical properties measurement of the emissive layer is combined with the computational determination of the electronic properties, film morphology, and excitation transfer phenomena. The Förster resonance energy transfer rates from 4CzDPO to TBPe are on the order of 1011 s−1, considerably higher than the radiative and nonradiative recombination rates for 4CzDPO. These features ensure nearly complete energy transfer to TBPe, leading to a five‐fold increase in the photoluminescence quantum yields in the 4CzDPO:TBPe system in comparison to neat films of 4CzDPO. This approach highlights the factors that can provide efficient energy transfer from TADF molecules to fluorescent emitters, suppress energy transfer among TADF molecules, and avoid the need for a host material within the emissive layer.
High Fidelity Bidirectional Neural Interfacing with Carbon Fiber Microelectrodes Coated with Boron‐Doped Carbon Nanowalls: An Acute Study
Authors: Hejazi Maryam A. , Tong Wei , Stacey Alastair , Sun Shi H. , Yunzab Molis , Almasi Ali , Jung Young Jun , Meffin Hamish , Fox Kate , Edalati Khatereh , Nadarajah Athavan , Prawer Steven , Ibbotson Michael R. , Garrett David. J 
Published: September 2020

AbstractImplantable electrodes that can communicate with a small, selective group of neurons via both neural stimulation and recording are critical for the development of advanced neuroprosthetic devices. Microfiber electrodes with neuron‐scale cross‐sections have the potential to improve the spatial resolution for both stimulation and recording, while minimizing the chronic inflammation response after implantation. In this work, glass insulated microfiber electrodes are fabricated by coating carbon fibers with boron‐doped carbon nanowalls. The coating significantly improves the electrochemical properties of carbon fibers, leading to a charge injection capacity of 7.82 ± 0.35 mC cm−2, while retaining good flexibility, stability and biocompatibility. When used for neural interfacing, the coated microelectrodes successfully elicit localized stimulation responses in explanted retina, and are also able to detect signals from single neurons, in vivo with a signal‐to‐noise ratio as high as 6.7 in an acute study. This is the first report of using carbon nanowall coated carbon fibers for neural interfacing.
Flexible Supercapacitor Based on Organohydrogel Electrolyte with Long‐Term Anti‐Freezing and Anti‐Drying Property
Authors: Li Xilong , Lou Dongyang , Wang Hongyang , Sun Xiaoyi , Li Juan , Liu You‐Nian 
Published: September 2020

AbstractHydrogel electrolytes have spurred the development of flexible energy storage devices by endowing them with liquid‐like ion transport and solid‐like mechanical elasticity. However, traditional hydrogel electrolytes always lose these functions in climate change because the internal water undergoes freezing and/or dehydration. In this work, a flexible supercapacitor (OHEC) is assembled based on the organohydrogel electrolyte (OHE) and activated carbon electrode material. The OHE is composed of PAMPS/PAAm double‐network hydrogel soaked from 4 m LiCl/ethylene glycol and exhibits good conductivities (1.9 and 22.9 mS cm−1 at −20 and 25 °C, respectively). The OHEC exhibits broad temperature adaptability (from −20 to 80 °C) and extraordinary resistance to mechanical damage (above 100 kg crushing). The OHEC avoids the polarization at low temperatures and retains 77.8% capacitance retention after storage at −20 °C for 30 days. Without extra sealed packaging, the OHEC maintains remarkable cycling stability (only 8.7% capacitance decay after 10 000 cycles) and retains 77.3% capacitance at 80 °C after 56 h. The outstanding anti‐drying performance and improved interfacial compatibility of OHEC account for the good durability in the high‐temperature environments. Additionally, other salts (such as LiClO4, NaCl, and KCl) with favorable solubility in ethylene glycol can also serve in OHEs for wide temperature range supercapacitors.
Fighting against Drug‐Resistant Tumors using a Dual‐Responsive Pt(IV)/Ru(II) Bimetallic Polymer
Authors: Zeng Xiaolong , Wang Yufei , Han Jianxiong , Sun Wen , Butt Hans‐Jürgen , Liang Xing‐Jie , Wu Si 
Published: September 2020

AbstractDrug resistance is a major problem in cancer treatment. Herein, the design of a dual‐responsive Pt(IV)/Ru(II) bimetallic polymer (PolyPt/Ru) to treat cisplatin‐resistant tumors in a patient‐derived xenograft (PDX) model is reported. PolyPt/Ru is an amphiphilic ABA‐type triblock copolymer. The hydrophilic A blocks consist of biocompatible poly(ethylene glycol) (PEG). The hydrophobic B block contains reduction‐responsive Pt(IV) and red‐light‐responsive Ru(II) moieties. PolyPt/Ru self‐assembles into nanoparticles that are efficiently taken up by cisplatin‐resistant cancer cells. Irradiation of cancer cells containing PolyPt/Ru nanoparticles with red light generates 1O2, induces polymer degradation, and triggers the release of the Ru(II) anticancer agent. Meanwhile, the anticancer drug, cisplatin, is released in the intracellular environment via reduction of the Pt(IV) moieties. The released Ru(II) anticancer agent, cisplatin, and the generated 1O2 have different anticancer mechanisms; their synergistic effects inhibit the growth of drug‐resistant cancer cells. Furthermore, PolyPt/Ru nanoparticles inhibit tumor growth in a PDX mouse model because they circulate in the bloodstream, accumulate at tumor sites, exhibit good biocompatibility, and do not cause side effects. The results demonstrate that the development of stimuli‐responsive multi‐metallic polymers provides a new strategy to overcome drug resistance.
Recent Technological Advances in Fabrication and Application of Organic Electrochemical Transistors
Authors: Chen Shuai , Surendran Abhijith , Wu Xihu , Lee Sang Yeon , Stephen Meera , Leong Wei Lin 
Published: September 2020

AbstractOrganic electrochemical transistors (OECTs), where conjugated polymers undergo doping/dedoping from an electrolyte, are widely studied for applications ranging from switching elements, artificial synapses to transducers for biological sensing. The concurrent transport of electronic and ionic charges within the channel provide OECTs with excellent amplification capability and efficient ion‐to‐electron transduction at low operating voltages (<1 V). Herein, the latest research advances in the fabrication techniques and applications of OECTs are summarized. Particular focus is given on the emerging applications including sensors, neuromorphic devices, and electrophysiological monitoring. Finally, the future challenges and opportunities of conventional OECTs and novel all‐solid‐state OECTs are discussed.
Tunable Infrared Plasmon Response of Lithographic Sn‐doped Indium Oxide Nanostructures
Authors: Kapetanovic Viktor , Bicket Isobel Claire , Lazar Sorin , Lagos Maureen Joel , Botton Gianluigi Andrea 
Published: September 2020

AbstractTransparent conductive oxides (TCOs) have strong potential for plasmonic applications. Given their easily tunable properties and low energy response, significant challenges in the controlled fabrication and precise characterization of TCOs must be better understood before this potential can be realized. Here, the mid‐ to near‐infrared plasmonic response of Sn‐doped In2O3 (ITO) nanostructures is presented, fabricated top‐down using electron beam lithography and radio‐frequency sputtering. These equilateral ITO triangles of different side lengths are imaged at high spatial and energy resolution with monochromated electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope. Applying the Richardson–Lucy (RL) deconvolution algorithm to experimental EELS spectra reveals localized surface plasmon (LSP) excitations between 150 and 550 meV and a 730 meV bulk plasmon. This very‐low‐energy response to an electron beam is compared with boundary element method simulations of nanostructures. These simulations use the dielectric functions of continuous thin films of the same materials, characterized by ellipsometry, 4‐point probe, and Hall effect tests. Additionally, upon rapid thermal annealing of ITO, blue‐shifts in LSP energy, and longer LSP lifetimes are examined as a consequence of an amorphous‐to‐polycrystalline transformation and an increase in the free carrier density.
Photolithographic Fabrication of Upconversion Barcodes for Multiplexed Molecular Detection
Authors: Zeng Xiao , Vanga Sudheer Kumar , Poh Eng Tuan , Shi Yi , Sow Chorng Haur , Bettiol Andrew Anthony , Liu Xiaogang 
Published: September 2020

AbstractThe demands of clinical diagnostics and genetic analysis for high‐performance multiplex detection systems have driven substantial advancement from planar microarrays to suspension arrays for accurate encoding, inventorying, and detecting extensive databases of biomolecules. Despite the multitude of related works and the commercial availability of nanostructured arrays for biodetection, it remains challenging to develop biodetection modules of massive coding permutation with high production rates and fast reaction kinetics . Herein, the concurrent improvement in both production and coding capacities without compromising detection kinetics is reported using lithography‐based upconversion barcodes as the basis for bioassay detection modules. This method exploits microstructural forms of dense graphical encoding, with barcode production up to 109 per run at extensive color permutations. The upconversion barcoding technique requires a million times lower analyte consumption compared to currently available technologies. Moreover, the use of upconversion barcodes is demonstrated in a DNA hybridization test with high target specificity, low detection limit, and ease of flexible surface bioconjugation, enabling potential development of biomarkers in the analysis of massive proteomics, genomics, and metabolomics data.
Co(III)salen Catalyzed Enantioselective C3‐Indolylation of Spiro‐Epoxyoxindoles and Its Mechanistic Studies
Authors: Hajra Saumen , Roy Sayan , Mondal Ananda Shankar 
Published: September 2020

AbstractCatalytic asymmetric C3‐indolylation of N‐protected spiro‐epoxyoxindoles has been developed for the access of 3‐(3‐indolyl)‐oxindole methanols with excellent enantioselectivity (ee up to >99%). The widespread substrate scope and easily accessible Co(III)‐salen over 1,1′‐Spirobiindane‐7,7′‐diol phosphoric acid prove our condition to be more beneficial than the chiral Brønsted acid‐catalyzed reaction. Further, kinetic resolution of spiro‐epoxides is achieved in high enantiomeric excess under certain conditions. The detailed mechanistic study endorses that the feedback inhibition played a key role which restricts the dynamic kinetic resolution process. Besides it also revealed the SN2′ mechanism for the Co(III)‐salen catalysed C3‐indolylation of spiro‐epoxyoxindoles.magnified image
Catalytic Enantioselective Bromoaminocyclization and Bromocycloetherification
Authors: Wang Haitao , Zhong Haijing , Xu Xi , Xu Wei , Jiang Xiaojian 
Published: September 2020

AbstractWe apply a chiral anionic phase‐transfer system for the catalytic asymmetric bromoaminocyclization and bromocycloetherification of momo‐functional benzo‐cyclic alkenes. Various brominated tricyclic benzo‐heterocycles were produced with up to 99% yields and 99% enantiomeric excess. The resulting enantioenriched hexahydro‐benzoindoles are key building blocks of bioactive molecules.magnified image
Recent Advances in Catalytic Enantioselective Synthesis of Fluorinated α‐ and β‐Amino Acids
Authors: Zhang Xue‐Xin , Gao Yang , Hu Xiao‐Si , Ji Cong‐Bin , Liu Yun‐Lin , Yu Jin‐Sheng 
Published: September 2020

AbstractEnantioenriched fluorinated α‐ and β‐amino acids are often encountered in numerous pharmaceuticals and bioactive molecules, and also of great importance as probes in PET and NMR for studying the behavior of enzymes and for incorporation into peptides and drug candidates. Among various synthetic strategies developed, catalytic enantioselective synthesis proves to be one of the most facile and powerful protocols to construct such privileged structures. The past decade has witnessed considerable progress in the catalytic enantioselective construction of chiral fluorinated α‐ and β‐amino acid derivatives with structural diversity. In this review, we summarize these impressive achievements according to the bond‐forming way of fluorinated α‐ or β‐amino acids, respectively, and underline the remaining challenges. This information would provide important guidance and some inspiration for the researchers engaged in organic fluorine and medicinal chemistry.magnified image
EGF Relays Signals to COP1 and Facilitates FOXO4 Degradation to Promote Tumorigenesis
Authors: Choi Hyun Ho , Zou Shaomin , Wu Jian‐lin , Wang Huashe , Phan Liem , Li Kai , Zhang Peng , Chen Daici , Liu Qingxin , Qin Baifu , Nguyen Thu Anh Thai , Yeung Sai‐Ching J. , Fang Lekun , Lee Mong‐Hong 
Published: September 2020

AbstractForkhead‐Box Class O 4 (FOXO4) is involved in critical biological functions, but its response to EGF‐PKB/Akt signal regulation is not well characterized. Here, it is reported that FOXO4 levels are downregulated in response to EGF treatment, with concurrent elevation of COP9 Signalosome subunit 6 (CSN6) and E3 ubiquitin ligase constitutive photomorphogenic 1 (COP1) levels. Mechanistic studies show that CSN6 binds and regulates FOXO4 stability through enhancing the E3 ligase activity of COP1, and that COP1 directly interacts with FOXO4 through a VP motif on FOXO4 and accelerates the ubiquitin‐mediated degradation of FOXO4. Metabolomic studies demonstrate that CSN6 expression leads to serine and glycine production. It is shown that FOXO4 directly binds and suppresses the promoters of serine‐glycine‐one‐carbon (SGOC) pathway genes, thereby diminishing SGOC metabolism. Evidence shows that CSN6 can regulate FOXO4‐mediated SGOC gene expression. Thus, these data suggest a link of CSN6‐FOXO4 axis and ser/gly metabolism. Further, it is shown that CSN6‐COP1‐FOXO4 axis is deregulated in cancer and that the protein expression levels of CSN6 and FOXO4 can serve as prognostic markers for cancers. The results illustrate a pathway regulation of FOXO4‐mediated serine/glycine metabolism through the function of CSN6‐COP1 axis. Insights into this pathway may be strategically designed for therapeutic intervention in cancers.
The Downs and Ups of the SNAP Caseload: What Matters?
Authors: Dickert‐Conlin Stacy , Fitzpatrick Katie , Stacy Brian , Tiehen Laura 
Published: September 2020

AbstractBeginning in the 1990s, states have received unprecedented flexibility to determine Supplemental Nutrition Assistance Program (SNAP) eligibility and program administration. We find state SNAP policies accounted for nearly half of the 2000–2016 caseload increase. State economic conditions also play an important role in caseload changes, accounting for almost half of the 2007 through 2013 increase. Within distinct periods of our 1990–2016 data, policy and the economy make different contributions to caseload changes. Policy simulations indicate that mandating states to maintain their 2000 SNAP policies, prior to the greatest expansion in latitude, would have lowered 2000–2016 caseload growth by 38%.
A multicenter study evaluating the effectiveness and safety of single‐dose low molecular weight iron dextran vs single‐dose ferumoxytol for the treatment of iron deficiency
Authors: Cohen Jonathan , Khudanyan Arpine , Lu Jessica , Wing Jason , Olson Sven , Deloughery Thomas , Shatzel Joseph J. 
Published: September 2020

AbstractThere are multiple intravenous (IV) iron formulations available, of which several may be administered as single‐dose infusions such as low‐molecular weight iron dextran (LMWID), ferumoxytol, ferric carboxymaltose, and ferric derisomaltose. However, administration of ferumoxytol as a single‐dose infusion is off‐label as it is approved as a two‐dose series. Previous studies of ferumoxytol alone support the effectiveness and safety of the single‐dose regimen, but there is a paucity of data directly comparing single‐dose ferumoxytol to other single‐dose IV iron formulations. This multicenter cohort study sought to affirm the safety and effectiveness of single‐dose ferumoxytol compared to single‐dose LMWID. Overall, 906 patients who received single‐dose LMWID (n = 439) or ferumoxytol (n = 467) were identified, of whom 351 met criteria for the primary effectiveness endpoint defined as median change in hemoglobin (Hb), hematocrit (Hct), and ferritin 8 to 12 weeks from baseline. All 906 patients were included for the secondary analysis evaluating the incidence of adverse events (AE) and requirement of additional IV iron infusions. Median change in Hb (LMWID 0.5 g/dL; ferumoxytol 0.8 g/dL; P = .24), Hct (LMWID 1.1%; ferumoxytol 1.25%; P = .89), and ferritin (LMWID 87 ng/dL; ferumoxytol 71 ng/dL; P = .47) was not significantly different between groups. Both groups experienced similar rates of AEs (LMWID 2.3%; ferumoxytol 2.8%; P = .63). The LMWID patients more frequently required additional IV iron infusions (LMWID 28.5%; ferumoxtyol 16.1%; P < .001). These findings support that single‐dose ferumoxytol is effective and safe, and that patients may require fewer additional infusions compared to patients who received LMWID.
The Active Site of a Prototypical “Rigid” Drug Target is Marked by Extensive Conformational Dynamics
Authors: Singh Himanshu , Das Chandan K. , Vasa Suresh K. , Grohe Kristof , Schäfer Lars V. , Linser Rasmus 
Published: September 2020

AbstractDrug discovery, in particular optimization of candidates using medicinal chemistry, is generally guided by structural biology. However, for optimizing binding kinetics, relevant for efficacy and off‐target effects, information on protein motion is important. Herein, we demonstrate for the prototypical textbook example of an allegedly “rigid protein” that substantial active‐site dynamics have generally remained unrecognized, despite thousands of medicinal‐chemistry studies on this model over decades. Comparing cryogenic X‐ray structures, solid‐state NMR on micro‐crystalline protein at room temperature, and solution NMR structure and dynamics, supported by MD simulations, we show that under physiologically relevant conditions the pocket is in fact shaped by pronounced open/close conformational‐exchange dynamics. The study, which is of general significance for pharmacological research, evinces a generic pitfall in drug discovery routines.
Carbid‐Dihydride: kohlenstoffhaltige Spezies identifiziert in der Ta4+‐vermittelten Methandehydrierung
Authors: Lengyel Jozef , Levin Nikita , Wensink Frank J. , Lushchikova Olga V. , Barnett Robert N. , Landman Uzi , Heiz Ueli , Bakker Joost M. , Tschurl Martin 
Published: September 2020

AbstractDie Produkte der Methandehydrierung von Ta4+ Clustern in der Gasphase werden mittels Infrarot Multipler‐Photonendissoziationsspektroskopie (IRMPD) in Verbindung mit quantenchemischen Rechnungen strukturell charakterisiert. Die erhaltenen Spektren von [4Ta,C,2H]+ offenbaren eine Dominanz von Schwingungsbanden einer H2Ta4C+ Carbid‐Dihydridstruktur gegenüber deren eines HTa4CH+ Carbin‐Hydrids, wie Untersuchungen verschiedener Isotopologe zweifelsfrei zeigen. Da die Dehydrierung von Methan durch Kationen M+ typischerweise über eine Bildung von MCH2+ Carbenen oder HMCH+ Carbin‐Hydridstrukturen erfolgt, legt die Beobachtung einer H2MC+ Carbid‐Dihydridstruktur nahe, dass es notwendig ist, dieser oft vernachlässigten Klasse kohlenstoffhaltiger Intermediate in Reaktionen von Metallen mit Kohlenwasserstoffen Beachtung zu schenken.
Antioxidative Stannous Oxalate Derived Lead‐Free Stable CsSnX3 (X=Cl, Br, and I) Perovskite Nanocrystals
Authors: Kang Cuiting , Rao Huashang , Fang Yueping , Zeng Jiejun , Pan Zhenxiao , Zhong Xinhua 
Published: September 2020

AbstractLead‐free CsSnX3 perovskite NCs are becoming a promising alternative to CsPbX3 (X=Cl, Br, I), but suffer from extremely poor stability. Herein, we highlight the significant effect of SnII precursors used in the synthesis on the stability of the resultant CsSnX3 NCs. A method is proposed for synthesizing CsSnX3 NCs using Cs2CO3, SnC2O4, and NH4X as corresponding constituent precursors, wherein the ratio of reactants can be easily adjusted. Stable CsSnX3 NCs can be obtained with the use of antioxidative SnC2O4 as the SnII precursor. Experimental results show that the improvement of NCs stability is mainly ascribed to the role of oxalate in the SnC2O4 precursor. Oxalate ion has a strong antioxidative ability and can effectively inhibit the oxidation of SnII during the synthesis. Besides, oxalate as a bidentate capping ligand is shown to be coordinated on the surface of formed NCs. This can not only passivate the uncoordinated Sn on the surface but also prevent the oxidation of the NCs.