bluuebunny/crossref_metadata_2025_split huggingface dataset:
Plasmonic Nanoprobes for Multiplexed Fluorescence‐Free Super‐Resolution Imaging
Authors: Xu Jian , Zhang Tianyue , Yang Shenyu , Feng Ziwei , Li Haoying , Hu Dejiao , Qin Fei , Ouyang Xueying , Cao Yaoyu , Jiang Lingxiang , Li Xiangping 
Published: August 2018

AbstractNoble metal nanoparticles (NPs), owing to their unique optical and physicochemical properties, are routinely used for optical imaging and labeling of biological specimens. Even though they can provide vital information for studying multiple cellular events and their interplays at the same time, optically multiplexing and resolving specific NPs within a diffraction‐limited region labeled in complex biological specimens remains a fundamental challenge. By introducing and manipulating plasmonic resonance assisted saturable scattering effects, multiplexed fluorescence‐free super‐resolution imaging of gold NPs in tumor cells with remarkable subdiffraction resolution is demonstrated. The saturable scattering allows fluorescence‐free resolving single plasmonic nanoprobes with significantly improved resolution down to ≈100 nm. The revealed plasmonic resonance assisted saturation effect as well as the associated spectral flexibility to variant sizes provides access to multiplexing capability in complex bioenvironments. The demonstrated feasibility of two‐color super‐resolution cellular imaging is achieved at ultralow suppression powers ≈0.28 MW cm−2, corresponding to a two‐order of magnitude improvement compared to the state‐of‐the‐art of stimulated emission depletion (STED) nanoscopy.
Optical Nanoparticles for Cardiovascular Imaging
Authors: Hu Jie , Ortgies Dirk H. , Martín Rodríguez Emma , Rivero Fernando , Aguilar Torres Rio , Alfonso Fernando , Fernández Nuria , Carreño‐Tarragona Gonzalo , Monge Luis , Sanz‐Rodriguez Francisco , Iglesias Maria del Carmen , Granado Miriam , García‐Villalon Angel Luis , García Solé José , Jaque Daniel 
Published: August 2018

AbstractThe current status of the use of optical nanoparticles for imaging of the cardiovascular system is reviewed in detail. The different types of optical (luminescent, photoacoustic, and scattering) nanoparticles capable of vessel imaging and diagnosis are described, paying special attention to the use of optical nanoparticles for atherosclerosis detection and diagnosis, for advanced imaging of blood perfusion and, finally, for the detection and diagnosis of ischemic tissues. The advantages and disadvantages of different optical nanoparticles and related techniques for cardiovascular imaging are discussed in detail.
Cytokine‐Functionalized Synthetic Dendritic Cells for T Cell Targeted Immunotherapies
Authors: Eggermont Loek J. , Hammink Roel , Blank Kerstin G. , Rowan Alan E. , Tel Jurjen , Figdor Carl G. 
Published: August 2018

AbstractWidespread application of cytokine‐based therapies is hampered by severe toxic side effects, resulting from off‐target (immune) cell stimulation. This emphasizes the need for more precise targeting of cytokines to immune cells. While cytokines are generally active as soluble proteins, it is demonstrated here that synthetic mimics of immune cells based on polyisocyanopeptides (PICs), called synthetic dendritic cells (sDCs) can efficiently present immobilized cytokines to T cells, when targeted by anti‐CD3 antibodies. Anti‐CD3/IL‐2‐functionalized PICs induce strong T cell activation and proliferation, when compared to PICs functionalized with interleukin‐2 (IL‐2) alone. In contrast to the semi‐flexible PICs, immobilization of IL‐2 on a rigid micro‐sized scaffold results in significant loss of IL‐2 activity, signifying the importance of molecular flexibility on the PIC polymers to maintain function. Similarly, anti‐CD3/IFNα‐functionalized PICs support long‐term proliferation of T cells. Interferon‐α containing sDCs additionally promote the development of cytotoxic effector functions of T cells with limited upregulation of the inhibitory immune checkpoint PD‐1. This high cytolytic activity and low PD‐1 expression are essential to maintain effective anti‐cancer activity. Together, these results demonstrate that PICs form unique nano‐sized scaffolds that efficiently present immobilized cytokines to T cells, thus creating a powerful tool to improve cytokine‐based immunotherapies without concomitant off‐target toxicity.
Realistic Large‐Scale Modeling of Rashba and Induced Spin–Orbit Effects in Graphene/High‐Z‐Metal Systems
Authors: Voloshina Elena , Dedkov Yuriy 
Published: August 2018

AbstractGraphene, as a material with a small intrinsic spin–orbit interaction of approximately 1 µeV, has a limited application in spintronics. Adsorption of graphene on the surfaces of heavy metals was proposed to induce the strong spin splitting of the graphene π bands either via Rashba effect or due to the induced spin–orbit effects via hybridization of the valence band states of graphene and metal. Spin‐resolved photoelectron spectroscopy experiments performed on graphene adsorbed on the substrates containing heavy elements demonstrate the “giant” spin splitting of the π states of the order of 100 meV in the vicinity of the Fermi level (EF) and the K point. However, recent scanning tunneling spectroscopy experiments did not confirm these findings, leaving the fact of the observation of the “giant” Rashba effect or induced spin–orbit interaction in graphene still open. Thus, a detailed understanding of the physics in such systems is indispensable. From the theory side, this requires, first of all, correct modeling of the graphene/metal interfaces under study. Here, realistic super‐cell density‐functional theory calculations are presented, including dispersion interaction and spin–orbit interaction, for several graphene/high‐Z‐metal interfaces. While correctly reproducing the spin‐splitting features of the metallic surfaces, their modifications under graphene adsorption and doping level of graphene, it is revealed that neither “giant” Rashba‐ nor spin–orbit‐induced splitting of the graphene π states around EF take place.
Database‐Driven Materials Selection for Semiconductor Heterojunction Design
Authors: Shapera Ethan P. , Schleife André 
Published: August 2018

AbstractHeterojunctions are at the heart of many modern semiconductor devices with tremendous societal impact: Light‐emitting diodes shape the future of energy‐efficient lighting, solar cells are promising for renewable energy, and photoelectrochemistry seeks to optimize efficiency of the water‐splitting reaction. Design of heterojunctions is difficult due to the limited number of materials for which band alignment is known, and the experimental and computational difficulties associated with obtaining this data. Band alignment based on branch‐point energies (EBP) is shown to be a good and efficient approximation that can be obtained using data from existing electronic‐structure databases. Errors associated with this approach are comparable to those of expensive first‐principles computational techniques and experiments. EBP alignment is then incorporated into a framework capable of rapidly screening existing online databases to design semiconductor heterojunctions. The method is showcased for five different prototype cases: Transport layers are successfully predicted for CdSe‐ and InP‐based LEDs, and for CH3NH3PbI3‐ and nanoparticle PbS‐based solar absorbers. In addition, Cu2O as a possible hole‐transport layer for solar cells is examined. The framework addresses the challenge of accomplishing fast materials selection for heterostructure design by tying together first‐principles calculations and existing online materials databases.
Independent Band Modulation in 2D van der Waals Heterostructures via a Novel Device Architecture
Authors: Guo Zhongxun , Chen Yan , Zhang Heng , Wang Jianlu , Hu Weida , Ding Shijin , Zhang David Wei , Zhou Peng , Bao Wenzhong 
Published: August 2018

AbstractBenefiting from the technique of vertically stacking 2D layered materials (2DLMs), an advanced novel device architecture based on a top‐gated MoS2/WSe2 van der Waals (vdWs) heterostructure is designed. By adopting a self‐aligned metal screening layer (Pd) to the WSe2 channel, a fixed p‐doped state of the WSe2 as well as an independent doping control of the MoS2 channel can be achieved, thus guaranteeing an effective energy‐band offset modulation and large through current. In such a device, under specific top‐gate voltages, a sharp PN junction forms at the edge of the Pd layer and can be effectively manipulated. By varying top‐gate voltages, the device can be operated under both quasi‐Esaki diode and unipolar‐Zener diode modes with tunable current modulations. A maximum gate‐coupling efficiency as high as ≈90% and a subthreshold swing smaller than 60 mV dec−1 can be achieved under the band‐to‐band tunneling regime. The superiority of the proposed device architecture is also confirmed by comparison with a traditional heterostructure device. This work demonstrates the feasibility of a new device structure based on vdWs heterostructures and its potential in future low‐power electronic and optoelectronic device applications.
Highly Multiplexed Single‐Cell Protein Profiling with Large‐Scale Convertible DNA‐Antibody Barcoded Arrays
Authors: Zhao Peng , Bhowmick Sirsendu , Yu Jianchao , Wang Jun 
Published: August 2018

AbstractHighly multiplexed detection of proteins secreted by single cells is always challenging. Herein, a multiplexed in situ tagging technique based on single‐stranded DNA encoded microbead arrays and multicolor successive imaging for assaying single‐cell secreted proteins with high throughput and high sensitivity is presented. This technology is demonstrated to be capable of increasing the multiplexity exponentially. Upon integration with polydimethylsiloxane microwells, this platform is applied to detect ten immune effector proteins from differentiated single macrophages stimulated with lipopolysaccharide. Significant heterogeneity is observed when the derived human primary macrophages are analyzed. This versatile technology is expected to open new opportunities in systems biology, immune regulation studies, signaling analysis, and molecular diagnostics.
Simultaneous Monitoring of Sweat and Interstitial Fluid Using a Single Wearable Biosensor Platform
Authors: Kim Jayoung , Sempionatto Juliane R. , Imani Somayeh , Hartel Martin C. , Barfidokht Abbas , Tang Guangda , Campbell Alan S. , Mercier Patrick P. , Wang Joseph 
Published: August 2018

AbstractThe development of wearable biosensors for continuous noninvasive monitoring of target biomarkers is limited to assays of a single sampled biofluid. An example of simultaneous noninvasive sampling and analysis of two different biofluids using a single wearable epidermal platform is demonstrated here. The concept is successfully realized through sweat stimulation (via transdermal pilocarpine delivery) at an anode, alongside extraction of interstitial fluid (ISF) at a cathode. The system thus allows on‐demand, controlled sampling of the two epidermal biofluids at the same time, at two physically separate locations (on the same flexible platform) containing different electrochemical biosensors for monitoring the corresponding biomarkers. Such a dual biofluid sampling and analysis concept is implemented using a cost‐effective screen‐printing technique with body‐compliant temporary tattoo materials and conformal wireless readout circuits to enable real‐time measurement of biomarkers in the sampled epidermal biofluids. The performance of the developed wearable device is demonstrated by measuring sweat‐alcohol and ISF‐glucose in human subjects consuming food and alcoholic drinks. The different compositions of sweat and ISF with good correlations of their chemical constituents to their blood levels make the developed platform extremely attractive for enhancing the power and scope of next‐generation noninvasive epidermal biosensing systems.
Fully Functional Logic‐In‐Memory Operations Based on a Reconfigurable Finite‐State Machine Using a Single Memristor
Authors: Xu Nuo , Yoon Kyung Jean , Kim Kyung Min , Fang Liang , Hwang Cheol Seong 
Published: August 2018

AbstractMemristor offers a promising logic‐in‐memory (LIM) functionality to achieve the futuristic in‐memory computing machine, which may solve the problem of the “von Neumann bottleneck” in the conventional computer architecture. A sequential logic concept is capable of achieving LIM based on the finite‐state machine (FSM) using a single bipolar (BRS) or complementary resistive switching (CRS) memristor, where 14 of the 16 two‐input Boolean logic functions (XOR and XNOR are missing) are mapped between the resistance state and the terminal voltages. In this paper, a new FSM‐LIM concept based on a reconfigurable finite‐state machine (RFSM logic) is proposed, which is experimentally confirmed by a diode‐integrated single unipolar memristor. The scope of application of the proposed concept is further extended to three other asymmetric resistive switching devices, demonstrating the universality of the RFSM logic. With the use of different voltage conditions to denote logic input “1,” the function of FSM is reconfigured between the two state‐transition equations. Through the triggering of the two state‐transition equations alternatively, all the 16 Boolean logic functions can be achieved in three steps at most, without the assistance of reading operation. These correspond to the logical completeness and nonvolatility.
A Facile Strategy to Construct Amorphous Spinel‐Based Electrocatalysts with Massive Oxygen Vacancies Using Ionic Liquid Dopant
Authors: Sun Jing , Guo Niankun , Shao Zhiyu , Huang Keke , Li Yaowen , He Feng , Wang Qin 
Published: August 2018

AbstractOxygen vacancies are demonstrated to be beneficial to various electrocatalytic reactions. However, integrating oxygen vacancies into an amorphous catalyst with a large specific surface area, and investigating its effect on the oxygen evolution reaction remains a great challenge. Herein, oxygen vacancies are introduced into an amorphous N, P, and F tri‐doped CoFe2O4 using ionic liquid as a dopant. Simultaneously, ultrafine MoS2 nanoclusters are anchored onto its surface to increase the specific surface area. The vacancy‐rich MoS2/NPF‐CoFe2O4 exhibits an overpotential of 250 mV and a small Tafel slope of 41 mV dec−1, which is the best spinel‐based oxygen evolution reaction (OER) electrocatalysts so far. The excellent performance is attributed to massive oxygen vacancies, amorphous structure, large surface area, and synergistic coupling effects among active species. Density‐functional theory calculations reveal that the electronic structure of the catalyst can be modulated in the presence of heteroatoms and MoS2 nanoclusters, and then the energy barriers of intermediates are decreased as well, which enhances the OER performance. This design not only provides a simple strategy to construct amorphous structures with abundant oxygen vacancies using ionic liquid‐dopants, but also presents an in‐depth insight into the OER mechanism in alkaline solution.
Extended Conjugation Length of Nonfullerene Acceptors with Improved Planarity via Noncovalent Interactions for High‐Performance Organic Solar Cells
Authors: Liu Dongxue , Kan Bin , Ke Xin , Zheng Nan , Xie Zengqi , Lu Di , Liu Yongsheng 
Published: August 2018

AbstractThree low‐bandgap nonfullerene acceptors (NFAs) IDTO‐T‐4F, IDTO‐Se‐4F, and IDTO‐TT‐4F with extended conjugation length are designed and synthesized. Various π‐spacers, thiophene, selenophene, and thieno[3,2‐b]thiophene are incorporated to extend the conjugated length and enhance the backbone planarity via noncovalent O···S or O···Se interactions. These NFAs exhibit strong light absorption in the range of 600–900 nm with narrow bandgaps between 1.38 and 1.45 eV. By blending with a wide‐bandgap donor material PBDB‐T, organic solar cells (OSCs) based on these NFAs all yield high efficiency over 10% with low energy losses ranging from 0.52 to 0.59 eV. Importantly, as a result of relatively high lowest unoccupied molecular orbital level, large hole and electron mobility in blend film, and low charge carrier recombination loss, optimized devices based on IDTO‐T‐4F exhibit a large open‐circuit voltage of 0.864 V, a high short‐circuit current density of 20.12 mA cm−2, and a notable fill factor of 72.7%, leading to an impressive efficiency of 12.62%, which represents the best performance for NFA OSCs using noncovalent interactions in acceptor molecule design. The results indicate that optimizing the conjugation length and backbone planarity via intramolecular noncovalent O···S or O···Se interactions is a useful strategy for NFA materials invention toward high‐performance solar cells.
Surveillance of cancer risks for firefighters, police, and armed forces among men in a Canadian census cohort
Authors: Harris M. Anne , Kirkham Tracy L. , MacLeod Jill S. , Tjepkema Michael , Peters Paul A. , Demers Paul A. 
Published: August 2018

BackgroundFirefighters, police, and armed services may be exposed to hazards such as combustion by‐products and shift work.MethodsThe CanCHEC cohort linked 1991 census data to the Canadian cancer registry for follow up. Cox proportional hazards modeling was used to estimate hazard ratios (HRs) and 95% confidence intervals (CIs) to estimate risks for firefighter, police, or armed forces compared to workers in other occupations.ResultsThe cohort of 1 108 410 men included 4535 firefighters, 10 055 police, and 9165 armed forces. For firefighters, elevated risks were noted for Hodgkin's lymphoma (HR: 2.89, 95%CI: 1.29‐6.46), melanoma (HR: 1.67, 95%CI: 1.17‐2.37), and prostate cancer (HR: 1.18, 95%CI: 1.01‐1.37). Police had elevated risks for melanoma (HR:1.69, 95%CI: 1.32‐2.16) and prostate cancer (HR:1.28, 95%CI: 1.14‐1.42). No significant associations were found for armed forces workers.ConclusionsCanadian firefighters, police, and armed services, may be at an increased risk of developing certain cancers. Results suggested that a healthy worker effect may influence risk estimates.
Direkter Zugang zu Azulenen über eine Gold‐katalysierte Dimerisierung von Diarylalkinen
Authors: Claus Vanessa , Schukin Michael , Harrer Siegfried , Rudolph Matthias , Rominger Frank , Asiri Abdullah M. , Xie Jin , Hashmi A. Stephen K. 
Published: August 2018

AbstractEine einfache Gold‐katalysierte Methode für die Synthese von substituierten und modifizierbaren Azulenen wurde entwickelt. Die Azulene werden entweder über die Dimerisierung von Push‐Pull‐Diarylalkinen mit Fluor‐Substituenten in ortho‐ oder para‐Position, oder über die Dimerisierung eines symmetrischen elektronenreichen Diarylalkins gebildet. In Anwesenheit eines kationischen Gold‐Katalysators bilden die zwei Alkine ein hoch reaktives Vinyl‐Kation. Diese energiereiche Zwischenstufe wird durch eine passende Aryl‐Einheit abgefangen, sodass liefert in einem einzigen, perfekt atomökonomischen Schritt substituierte Azulene erhalten werden.
Applications of Selenonium Cations as Lewis Acids in Organocatalytic Reactions
Authors: He Xinxin , Wang Xinyan , Tse Ying‐Lung (Steve) , Ke Zhihai , Yeung Ying‐Yeung 
Published: August 2018

AbstractThe use of trisubstituted selenonium salts as organic Lewis acids in electrophilic halogenation and aldol‐type reactions has been developed. The substrate scope is broad. The reaction conditions are mild and compatible with various functionalities. This study opens a new avenue for the development of nonmetallic Lewis acid catalysis.
Nitrogen‐Doped Graphene Quantum Dots Enhance the Activity of Bi2O3 Nanosheets for Electrochemical Reduction of CO2 in a Wide Negative Potential Region
Authors: Chen Zhipeng , Mou Kaiwen , Wang Xiaohan , Liu Licheng 
Published: August 2018

AbstractLarge numbers of catalysts have been developed for the electrochemical reduction of CO2 to value‐added liquid fuels. However, it remains a challenge to maintain a high current efficiency in a wide negative potential range for achieving a high production rate of the target products. Herein, we report a 2D/0D composite catalyst composed of bismuth oxide nanosheets and nitrogen‐doped graphene quantum dots (Bi2O3‐NGQDs) for highly efficient electrochemical reduction of CO2 to formate. Bi2O3‐NGQDs demonstrates a nearly 100 % formate Faraday efficiency (FE) at a moderate overpotential of 0.7 V with a good stability. Strikingly, Bi2O3‐NGQDs exhibit a high activity (average formate FE of 95.6 %) from −0.9 V to −1.2 V vs. RHE. Additionally, DFT calculations reveal that the origin of enhanced activity in this wide negative potential range can be attributed to the increased adsorption energy of CO2(ads) and OCHO* intermediate after combination with NGQDs.
A Polyimide Nanolayer as a Metal‐Free and Durable Organic Electrode Toward Highly Efficient Oxygen Evolution
Authors: Lin Yun‐Xiao , Feng Wei‐Jie , Zhang Jun‐Jun , Xue Zhong‐Hua , Zhao Tian‐Jian , Su Hui , Hirano Shin‐Ichi , Li Xin‐Hao , Chen Jie‐Sheng 
Published: August 2018

AbstractThe exploitation of metal‐free organic polymers as electrodes for water splitting reactions is limited by their presumably low activity and poor stability, especially for the oxygen evolution reaction (OER) under more critical conditions. Now, the thickness of a cheap and robust polymer, poly(p‐phenylene pyromellitimide) (PPPI) was rationally engineered by an in situ polymerization method to make the metal‐free polymer available for the first time as flexible, tailorable, efficient, and ultra‐stable electrodes for water oxidation over a wide pH range. The PPPI electrode with an optimized thickness of about 200 nm provided a current density of 32.8 mA cm−2 at an overpotential of 510 mV in 0.1 mol L−1 KOH, which is even higher than that (31.5 mA cm−2) of commercial IrO2 OER catalyst. The PPPI electrodes are scalable and stable, maintaining 92 % of its activity after a 48‐h chronoamperometric stability test.
The Chemical Sciences and Equality, Diversity, and Inclusion
Authors: Mehta Goverdhan , Yam Vivian W. W. , Krief Alain , Hopf Henning , Matlin Stephen A. 
Published: August 2018

AbstractThere has been mounting concern over the absence of gender equality in the sciences in recent years. This has been accompanied by a broadening of the perspective, in order to address issues of equality, diversity and inclusion, relating to a wide range of circumstances in which individuals suffer discrimination. While some progress has been made in some countries, nationally or at the level of institutions, much more needs to be done. The chemical sciences can play a leading role in addressing biases, through 1) becoming a model of good systemic practice in policies, processes, and actions; 2) developing practical skills through training in cultural competence; and 3) promoting a stronger evidence base to uncover both the extent of problems and the degree to which approaches to improve equality, diversity, and inclusion are working.
Gold‐Catalyzed Dimerization of Diarylalkynes: Direct Access to Azulenes
Authors: Claus Vanessa , Schukin Michael , Harrer Siegfried , Rudolph Matthias , Rominger Frank , Asiri Abdullah M. , Xie Jin , Hashmi A. Stephen K. 
Published: August 2018

AbstractWe have developed a simple gold‐catalyzed procedure for the synthesis of substituted and modifiable azulenes. The azulenes are formed either by the dimerization of push–pull diarylalkynes bearing a fluorine atom in ortho or para position or by the dimerization of a symmetric electron‐rich diarylalkyne. In the presence of a cationic gold catalyst, the two alkynes can form a highly reactive vinyl cation. Trapping of this high‐energy intermediate by an appropriate aryl unit then delivers substituted azulenes in a single step and in a perfect atom economy.