bluuebunny/crossref_metadata_2025_split huggingface dataset:
Strong Coupling of Exciton and High‐Q Mode in All‐Perovskite Metasurfaces
Authors: Al‐Ani Ibrahim A. M. , As'Ham Khalil , Huang Lujun , Miroshnichenko Andrey E. , Lei Wen , Hattori Haroldo T. 
Published: October 2021

AbstractRecently developed halide perovskite semiconductors are viewed as an excellent platform to realize exciton‐polariton at room temperature due to their large oscillation strength. Here, the optimized strong coupling between the exciton of perovskite and quasi‐bound state in the continuum (QBIC) with high‐quality factor (Q‐factor), supported by all‐perovskite metagrating, including magnetic dipole (MD)‐QBIC and toroidal dipole (TD)‐QBIC is demonstrated. By taking advantage of extreme electric field confinement enabled by a high‐Q mode, it is found that the maximum Rabi splitting can be enhanced up to a record high value of 400 meV, almost twice the Rabi splitting reported in the same perovskite‐based subwavelength metasurface. The simulation results reveal that both the Q‐factor of QBIC mode and the thickness of the perovskite metasurface play dominant roles in the enhanced strong coupling. It is also demonstrated that adding a protection layer of poly(methyl methacrylate) on the top of the perovskite metagrating has a negligible effect on the maximized Rabi‐splitting. These results suggest a new approach for studying exciton‐polaritons and may pave the way toward flexible, large‐scale, and low‐cost integrated polaritonic devices and the realization of polariton lasing at room temperature.
Broadband and High‐Sensitivity Time‐Resolved THz System Using Grating‐Assisted Tilted‐Pulse‐Front Phase Matching
Authors: Cui Wei , Awan Kashif Masud , Huber Rupert , Dolgaleva Ksenia , Ménard Jean‐Michel 
Published: October 2021

AbstractA broadband and sensitive time‐resolved terahertz (THz) configuration relying on noncollinear optical interactions is presented. This noncollinear scheme enables a higher THz generation and detection efficiency in nonlinear crystals. The concept relies on a pair of thick (2 mm) GaP crystals with a phase grating etched on their surface to achieve phase matching between a diffracted near‐infrared pulse and a THz wave propagating at normal incidence. This system is compared to a standard collinear scheme based on thin (0.2 mm) crystals and, while both systems provide access to a spectral bandwidth extending up to 6.5 THz, it is found that the noncollinear configuration improves the THz signal by more than a factor of 400 and the dynamic range of the system by 30 dB at a frequency of 3 THz.
Synthesis of Indole‐ and Pyrrole‐Fused Seven‐Membered Nitrogen Heterocycles via Acid‐Base Switchable Cyclization Involving Cleavage of Amide C−N Bonds
Authors: Hao Yanke , Zhou Pan , Niu Kaikai , Song Hongjian , Liu Yuxiu , Zhang Jingjing , Wang Qingmin 
Published: October 2021

AbstractWe report the method for synthesis of indole‐ and pyrrole‐fused seven‐membered nitrogen heterocycles by means of acid‐base switchable cyclization reactions. The reactions involved cleavage of amide C−N bonds, chemoselective N‐1 or C‐3 acylation, and 1,4‐Michael addition. This method could be used to construct two different kinds of seven‐membered rings in one step from the same starting material without the need for a transition‐metal catalyst.magnified image
Fabricating Ag/PW12/Zr‐mTiO2 Composite via Doping and Interface Engineering: An Efficient Catalyst with Bifunctionality in Photo‐ and Electro‐Driven Nitrogen Reduction Reactions
Authors: Feng Caiting , Liu Jiquan , Li Qinlong , Ji Lei , Wu Panfeng , Yuan Xiaoxiao , Hu Huaiming , Jiang Hai‐Ying , Xue Ganglin 
Published: October 2021

AbstractDriven by solar power and derived electricity, ambient photo‐ and electrochemical nitrogen fixations are considered promising strategies to produce low‐concentration NH3/NH4+. Under the principles of doping and interface engineering, a Ag/PW12/Zr‐mTiO2 composite is fabricated in a one‐pot synthesis, where zirconium‐doped mesoporous TiO2 is co‐decorated with silver nanoparticles (Ag NPs, optimal 1 wt%) and phosphotungstic acid (PW12, optimal 10 wt%). Enhanced nitrogen chemisorption is achieved owing to Zr‐doping, where the mesoporous structure of Zr‐mTiO2 favors nitrogen mass transfer. Ag NPs decoration leads to visible light absorption. At the interface, PW12 and Ag NPs decelerate the recombination of photo‐generated charge carriers. A Z‐scheme mechanism is suggested for the hetero‐junction, and the surface plasmon resonance effect of Ag NPs is considered in the composite. Consequently, a NH3/NH4+ production rate of 324.2 µmol gcat−1 h−1 is achieved in the photo‐driven process, together with the structure‐reactivity relationship between transient photocurrent intensity and catalytic efficiency. Moreover, constructing Ag/PW12/Zr‐mTiO2 heterojunction introduces a plentitude of active sites for the electrochemical process, together with enhanced charge transfer efficiency at the interface. Hence, an excellent NH3/NH4+ production rate of 55.0 µg mgcat−1 h−1 is accomplished at −0.6 V vs RHE. The robustness and superior activity of Ag/PW12/Zr‐mTiO2 in both photo‐ and electro‐driven processes may offer an opportunity for effectively utilizing sunlight.
Targeted Anti‐Tumor Immunotherapy Using Tumor Infiltrating Cells
Authors: Xie Yifan , Xie Feng , Zhang Lei , Zhou Xiaoxue , Huang Jun , Wang Fangwei , Jin Jin , Zhang Long , Zeng Linghui , Zhou Fangfang 
Published: October 2021

AbstractIn the tumor microenvironment, T cells, B cells, and many other cells play important and distinct roles in anti‐tumor immunotherapy. Although the immune checkpoint blockade and adoptive cell transfer can elicit durable clinical responses, only a few patients benefit from these therapies. Increased understanding of tumor‐infiltrating immune cells can provide novel therapies and drugs that induce a highly specific anti‐tumor immune response to certain groups of patients. Herein, the recent research progress on tumor‐infiltrating B cells and T cells, including CD8+ T cells, CD4+ T cells, and exhausted T cells and their role in anti‐tumor immunity, is summarized. Moreover, several anti‐tumor therapy approaches are discussed based on different immune cells and their prospects for future applications in cancer treatment.
Accelerated Electron Transfer in Nanostructured Electrodes Improves the Sensitivity of Electrochemical Biosensors
Authors: Fu Kaiyu , Seo Ji‐Won , Kesler Vladimir , Maganzini Nicolo , Wilson Brandon D. , Eisenstein Michael , Murmann Boris , Soh H. Tom 
Published: October 2021

AbstractElectrochemical biosensors hold the exciting potential to integrate molecular detection with signal processing and wireless communication in a miniaturized, low‐cost system. However, as electrochemical biosensors are miniaturized to the micrometer scale, their signal‐to‐noise ratio degrades and reduces their utility for molecular diagnostics. Studies have reported that nanostructured electrodes can improve electrochemical biosensor signals, but since the underlying mechanism remains poorly understood, it remains difficult to fully exploit this phenomenon to improve biosensor performance. In this work, electrochemical aptamer biosensors on nanoporous electrode are optimized to achieve improved sensitivity by tuning pore size, probe density, and electrochemical measurement parameters. Further, a novel mechanism in which electron transfer is physically accelerated within nanostructured electrodes due to reduced charge screening, resulting in enhanced sensitivity is proposed and experimentally validated. In concert with the increased surface areas achieved with this platform, this newly identified effect can yield an up to 24‐fold increase in signal level and nearly fourfold lower limit of detection relative to planar electrodes with the same footprint. Importantly, this strategy can be generalized to virtually any electrochemical aptamer sensor, enabling sensitive detection in applications where miniaturization is a necessity, and should likewise prove broadly applicable for improving electrochemical biosensor performance in general.
Trojan Horse‐Like Nano‐AIE Aggregates Based on Homologous Targeting Strategy and Their Photodynamic Therapy in Anticancer Application
Authors: Li Yin , Zhang Rongyuan , Wan Qing , Hu Rong , Ma Yao , Wang Zhiming , Hou Jianquan , Zhang Weijie , Tang Ben Zhong 
Published: October 2021

AbstractPhotodynamic therapy (PDT) has become a promising candidate for cancer theranostics; however, traditional photosensitizers (PSs) usually exhibit weak fluorescence and poor reactive oxygen species (ROS) generation efficiency when aggregated. Recently, aggregation‐induced emission (AIE) luminogens have shown great potential in the development of novel PSs owing to their excellent aggregation‐induced ROS generation (AIG‐ROS) activity. However, there are still concerns that must be addressed. In this study, two near‐infrared (NIR) emitters (PI and PTI) are synthesized with AIG‐ROS characteristic. PTI exhibit a valuable redder emission with more effective intersystem crossing (ISC) process than PI. The two AIE‐active PSs show excellent lipid droplet (LD)‐specific targeting ability. The detailed therapeutic mechanism of PDT in LDs specificity is also investigated. The mechanism of oxidation of polyunsaturated fatty acids (PUFAs) in LDs to form toxic lipid peroxides (LPOs) and thereby causing cellular ferroptosis is confirmed first. Homologous targeting is also used to achieve tumor targeting via coating PSs with active cancer cell membranes. Biomimetic aggregates exhibit good targeting ability, and an improved PDT antitumor effect via AIG‐ROS activity. These findings offer a clear route to develop advanced PSs with good targeting specificity. A template has also been provided for studying the therapeutic mechanism of AIE‐active PSs.
Universal‐Descriptors‐Guided Design of Single Atom Catalysts toward Oxidation of Li2S in Lithium–Sulfur Batteries
Authors: Zeng Zhihao , Nong Wei , Li Yan , Wang Chengxin 
Published: October 2021

AbstractThe sulfur redox kinetics critically matters to superior lithium–sulfur (Li–S) batteries, for which single atom catalysts (SACs) take effect on promoting Li2S redox process and mitigating the shuttle behavior of lithium polysulfide (LiPs). However, conventional trial‐and‐error strategy significantly slows down the development of SACs in Li–S batteries. Here, the Li2S oxidation processes over MN4@G catalysts are fully explored and energy barrier of Li2S decomposition (Eb) is identified to correlate strongly with three parameters of energy difference between initial and final states of Li2S decomposition, reaction energy of Li2S oxidation and LiS bond strength. These three parameters can serve as efficient descriptors by which two excellent SACs of MoN4@G and WN4@G are screened which give rise to Eb values of 0.58 and 0.55 eV, respectively, outperforming other analogues in adsorbing LiPs and accelerating the redox kinetics of Li2S. This method can be extended to a wider range of SACs by coupling MN4 moiety with heterostructures and heteroatoms beyond N where WN4@G/TiS2 heterointerface is predicted to exhibit enhanced catalytic performance for Li2S decomposition with Eb of 0.40 eV. This work will help accelerate the process of designing a wider range of efficient catalysts in Li–S batteries and even beyond, e.g. alkali‐ion‐Chalcogen batteries.
Orders of Recombination in Complete Perovskite Solar Cells – Linking Time‐Resolved and Steady‐State Measurements
Authors: Wolff Christian M. , Bourelle Sean A. , Phuong Le Quang , Kurpiers Jona , Feldmann Sascha , Caprioglio Pietro , Marquez Jose Antonio , Wolansky Jakob , Unold Thomas , Stolterfoht Martin , Shoaee Safa , Deschler Felix , Neher Dieter 
Published: October 2021

AbstractIdeally, the charge carrier lifetime in a solar cell is limited by the radiative free carrier recombination in the absorber which is a second‐order process. Yet, real‐life cells suffer from severe nonradiative recombination in the bulk of the absorber, at interfaces, or within other functional layers. Here, the dynamics of photogenerated charge carriers are probed directly in pin‐type mixed halide perovskite solar cells with an efficiency >20%, using time‐resolved optical absorption spectroscopy and optoelectronic techniques. The charge carrier dynamics in complete devices is fully consistent with a superposition of first‐, second‐, and third‐order recombination processes, with no admixture of recombination pathways with non‐integer order. Under solar illumination, recombination in the studied solar cells proceeds predominantly through nonradiative first‐order recombination with a lifetime of 250 ns, which competes with second‐order free charge recombination which is mostly if not entirely radiative. Results from the transient experiments are further employed to successfully explain the steady‐state solar cell properties over a wide range of illumination intensities. It is concluded that improving carrier lifetimes to >3 µs will take perovskite devices into the radiative regime, where their performance will benefit from photon‐recycling.
In Situ Infrared Micro and Nanospectroscopy for Discharge Chemical Composition Investigation of Non‐Aqueous Lithium–Air Cells
Authors: Nepel Thayane C. M. , Anchieta Chayene G. , Cremasco Leticia F. , Sousa Bianca P. , Miranda André N. , Oliveira Lorrane C. C. B. , Francisco Bruno A. B. , Júlio Julia P. de O. , Maia Francisco C. B. , Freitas Raul O. , Rodella Cristiane B. , Filho Rubens M. , Doubek Gustavo 
Published: October 2021

AbstractMetal–air batteries, such as Li–air, may be the key for large‐scale energy storage as they have the highest energy density among all electrochemical devices. However, these devices suffer from irreversible side reactions leading to battery failure, especially when ambient air is used as the O2 source, so a deep understanding over the surface chemistry evolution is imperative for building better devices. Herein, a multi‐scale (nano‐micro) FTIR analysis is made over the electrode surface during cell discharge employing synchrotron infrared nanospectroscopy (SINS) for the first time, to track the chemical composition changes at the nanoscale which are successfully correlated with in operando micro‐FTIR characterization. The in situ results reveal homogeneous product distribution from the nano to the micro scale, and that the discharge rate does not interfere in chemical composition. In operando micro‐FTIR shows the atmosphere dependency over Li products formation; the presence of HCOO– species occurring due to CO2 electroreduction in water, LiOH and Li2CO3, are also detected and even the lowest concentration of CO2 and H2O affects the O2 reactions. Finally, evidence of the Li2O2 reaction with DMSO forming DMSO2 after just 140 s of cell discharge shows this new technique's relevance in aiding the search for stable electrolytes.
International Retrospective Cohort Study of Conversion Therapy for Stage IV Gastric Cancer 1 (CONVO‐GC‐1)
Authors: Yoshida Kazuhiro , Yasufuku Itaru , Terashima Masanori , Young Rha Sun , Moon Bae Jae , Li Guoxin , Katai Hitoshi , Watanabe Masahiko , Seto Yasuyuki , Hoon Noh Sung , Kwang Yang Han‐ , Ji Jiafu , Baba Hideo , Kitagawa Yuko , Morita Satoshi , Nishiyama Masahiko , Kodera Yasuhiro ,   CONVO‐GC‐1 Study Group, Federation of Asian Clinical Oncology (FACO)
Published: October 2021

AbstractAimMuch attention has been paid to conversion therapy for stage IV gastric cancer, however, its operative comorbidities and survival benefit have not yet been clarified. CONVO‐GC‐1, an international retrospective cohort study, was designed to investigate the role of conversion surgery in Japan, Korea, and China.MethodsThe rate of operative complications was the primary endpoint and the overall survival (OS), according to the four‐category criteria previously published (Gastric Cancer:19; 2016), was analyzed as the secondary endpoint.ResultsA total of 1206 patients underwent surgery after chemotherapy with curative intent. Operative complications were observed in 290 (24.0%) patients in all grades, including pancreatic fistula and surgical site infection. The median survival time (MST) of all resected patients was 36.7 mo (M) and those of R0, R1, and R2 resection were 56.6 M, 25.8 M, and 21.7 M, respectively. Moreover, the MST of R0 patients were 47.8 M, 116.7 M, 44.8 M in categories 1, 2, and 3, respectively, and not reached in category 4. Interestingly, the MST of P1 patients was as favorable as that of P0CY1 patients if R0 resection was achieved. The MST of patients with liver metastasis was also favorable regardless of the number of lesions, and the MST of patients with para‐aortic lymph node (LN) No 16a1/b2 metastasis was not inferior to that of patients with para‐aortic LN No 16a2/b1 metastasis.ConclusionConversion therapy for stage IV gastric cancer is safe and could be a new therapeutic strategy to improve the survival of patients, especially those with R0 resection.
Incongruent phylogenies and their implications for the study of diversification, taxonomy, and genome size evolution of Rhododendron
Authors: Khan Gulzar , Nolzen Jennifer , Schepker Hartwig , Albach Dirk C. 
Published: October 2021

AbstractPremiseClassification of taxa depends on the quality of inferred phylogenies. Rhododendron, a highly species‐rich genus (>1156 species) of woody plants, has a highly debated infrageneric classification, due to its huge diversity, homoplasy in key characters, and incongruence among data sets. We provide a broad coverage of representative species to resolve Rhododendron infrageneric phylogeny and highlight the areas of incongruence. We further investigate the effect of polyploidy and genome size evolution on diversification of Rhododendron.MethodsWe generated two plastid and two nuclear loci for 260 Rhododendron species. We analyzed the loci separately as well as concatenated, utilizing both likelihood and Bayesian methods. We tested incongruence both among the data sets and with previous studies. We estimated genome sizes for 125 species through flow cytometry.ResultsOur results suggest stronger support for larger subgenera; however, the smaller subgenera pose several problems; for example, R. tomentosum (former genus Ledum) occupies incongruent positions based on different DNA regions. The main shift to higher diversification in the genus occurs in the Himalayan/Southeast Asian clade of R. subg. Hymenanthes. We found that polyploidy occurs in almost all subgenera but most frequently within R. subg. Rhododendron sections Rhododendron and Schistanthe.ConclusionsWe endorse the recognition of five major clades at the subgeneric level, but a number of species cannot be confidently assigned to these clades due to incongruency. With regard to genome size evolution, results support previous reports that genome sizes of tropical plants are lower than those of colder and temperate regions and that genome downsizing promotes diversification.
Phylogenomics and continental biogeographic disjunctions: insight from the Australian starflowers (Calytrix)
Authors: Nge Francis J. , Biffin Ed , Waycott Michelle , Thiele Kevin R. 
Published: October 2021

AbstractPremiseContinental‐scale disjunctions and associated drivers are core research interests in biogeographic studies. Here, we selected a species‐rich Australian plant genus (Calytrix; Myrtaceae) as a case study to investigate these patterns. Species of this endemic Australian starflower genus have a disjunct distribution across the mesic fringes of the continent and are largely absent from the arid center.MethodsWe used high‐throughput sequencing to generate unprecedented resolution and near complete species‐level nuclear and plastid phylogenies for Calytrix. BioGeoBEARS and biogeographic stochastic mapping were used to infer ancestral areas, the relative contributions of vicariance and dispersal events, and directionality of dispersal.ResultsPresent‐day disjunctions in Calytrix are explained by a combination of scenarios: (1) retreat of multiple lineages from the continental center to the more mesic fringes as Australia became progressively more arid, with subsequent extinction in the center as well as (2) origination of ancestral lineages in southwestern Australia (SWA) for species‐rich clades. The SWA biodiversity hotspot is a major diversification center and the most common source area of dispersals, with multiple lineages originating in SWA and subsequently spreading to the adjacent arid Eremaean region.ConclusionsOur results suggest that major extinction, as a result of cooling and drying of the Australian continent in the Eocene–Miocene, shaped the present‐day biogeography of Calytrix. We hypothesize that this peripheral vicariance pattern, which is similar to the African Rand flora, may explain the disjunctions of many other Australian plant groups. Further studies with densely sampled phylogenies are required to test this hypothesis.
Work‐relatedness of lateral epicondylitis: Systematic review including meta‐analysis and GRADE work‐relatedness of lateral epicondylitis
Authors: Bretschneider S. Fransje , Los Felicia S. , Eygendaal Denise , Kuijer P. Paul F. M. , van der Molen Henk F. 
Published: October 2021

AbstractBackgroundLateral epicondylitis (LE) is a highly prevalent musculoskeletal disorder in workers, often associated with physically demanding work. Knowledge of work‐relatedness of LE is crucial to develop appropriate preventive measures. This study investigates the prospective association between work‐related physical risk factors and LE.MethodsA systematic literature review was conducted in MedLine using PubMed from January 1, 2010 until February 16, 2021. Published reports were included if: (1) LE was clinically assessed, (2) exposure to work‐related physical risk factors was assessed, and (3) associations between LE and work‐related physical risk factors were reported in prospective studies. Quality of evidence was assessed using the Grading of Recommendations, Assessment, Development and Evaluation.ResultsIn total, 318 workers with LE from a population of 5036 workers in five studies were included. Meta‐analyses revealed high‐quality evidence for associations between LE and a Strain Index (SI) score >5.1 (odds ratio [OR]: 1.75, 95% confidence interval (CI): 1.11–2.78) and moderate‐quality evidence for forearm rotation >4 h/day or forearm rotation ≥45° for ≥45% time (OR: 1.85, 95% CI: 1.10–3.10). Gripping, flexion and extension of the wrist, and repetitive movements showed no significant associations with LE.ConclusionHigh‐quality evidence was found indicating that a higher SI increased the risk of LE. Moderate‐quality evidence was found for an association between forearm rotation and LE. No associations were found between other physical risk factors and LE. Primary preventive interventions should focus on a reduction of the SI and of high forearm rotation in work.