bluuebunny/crossref_metadata_2025_split huggingface dataset:
Crown Ether‐Functionalized Complex Emulsions as an Artificial Adaptive Material Platform
Authors: Djalali Saveh , Simón Marqués Pablo , Frank Bradley D. , Zeininger Lukas 
Published: October 2021

AbstractResponsive materials capable of autonomously regulating and adapting to molecular recognition‐induced chemical events hold great promise in the design of artificial chemo‐intelligent life‐like soft material platforms. In this context, the design of a synthetically minimal artificial emulsion platform that, regulated by interfacial supramolecular recognition events, is capable to autonomously and reversibly adapt to its chemical environment is reported. The systems exhibit programmed up‐ and down‐regulating capabilities that are realized via selective assembly of synthesized crown ether surfactants onto one hemisphere of anisotropic biphasic emulsion droplets. Dynamic and reversible interfacial host–guest complexation of, for example, metal and ammonium ions or amino acids transduce into interface‐triggered morphological reconfigurations of the complex emulsion droplets, which mediate their ability to selectively present, hide, or expand liquid–liquid interfaces. The separate responsive modalities are then used to showcase the utility of such adaptive soft material platforms for a self‐regulated uptake and release of metal ions or phase‐transfer catalysts, a biomimetic recognition of biomolecules including amino acids, carbohydrates, and antibodies, and for triggered surface‐encoded payload release applications.
Organophosphorus Hybrid Solid Electrolyte Interphase Layer Based on LixPO4 Enables Uniform Lithium Deposition for High‐Performance Lithium Metal Batteries
Authors: Wang Qian , Wan Jing , Cao Xin , Wen Rui , Guo YuGuo , Liu Wen , Zhou Henghui 
Published: October 2021

AbstractLithium metal is a promising anode candidate for the next‐generation rechargeable battery system because of its highest specific capacity and lowest potential. However, low Coulombic efficiency (CE) and the formation of Li dendrites during the cycling process seriously hinder its practical application. Here, an organophosphorus hybrid flexible solid electrolyte interphase (SEI) layer is proposed based on a surface chelation strategy using phytic acid (PA) as Li metal surface treatment chemicals. Different from the traditional SEI layer, the polynuclear complex between PA and Li+ serves as a “connecter” in this SEI layer, which not only ensures its mechanical flexibility but also improves its lithiophilic property and ionic conductivity. With these advantages, the Li || Cu cells exhibit a high CE of 99.0% over 500 cycles at a current density of 0.5 mA cm−2. Li || Li symmetrical cells can also maintain a stable Li plating/stripping process over 2500 h at a high current density of 10.0 mA cm−2. Besides, all Li metal batteries (Li || S, Li || NCM, Li || LFP et al.) based on this strategy exhibit long cycling life and high capacity retention. This surface chelation strategy is believed to offer a new avenue to fabricate a stable and efficient SEI layer for practical application of Li metal batteries.
β‐Phase‐Rich Laser‐Induced Hierarchically Interactive MXene Reinforced Carbon Nanofibers for Multifunctional Breathable Bioelectronics
Authors: Sharifuzzaman Md , Zahed Md Abu , Sharma Sudeep , Rana S M Sohel , Chhetry Ashok , Shin Young Do , Asaduzzaman Md , Zhang Shipeng , Yoon Sanghyuk , Hui Xue , Yoon Hyosang , Park Jae Y. 
Published: October 2021

AbstractHierarchically interactive 3D‐porous soft carbon nanofibers (CNFs) have great potential for wearable bioelectronic interfaces, yet 90% of CNFs are derived from expensive polyacrylonitrile associated with complex production methods. Here, another cost‐effective fluoropolymer, poly(1,1‐difluoroethylene) (PDFE), is introduced to investigate its transition chemistry and structural evolution over laser‐induced carbonization (LIC). The impregnation of Ti3C2Tx‐MXene followed by dehydrofluorination is believed to be crucial to enhance the β‐phase and reinforce PDFE‐based nanofibers. It is explored that the β‐phase of the dehydrofluorinated MXene‐PDFE nanofibers is converted into an sp2‐hybridized hexagonal graphitic structure by cyclization/cross‐linking decomposition during LIC. Remarkably, this approach generates laser‐induced hierarchical CNFs (LIHCNFs) with a high carbon yield (54.77%), conductivity (sheet resistance = 4 Ω sq−1), and stability over 500 bending/releasing cycles (at 10% bending range). Using LIHCNFs, a skin‐compatible breathable and reusable electronic‐tattoo is engineered for monitoring long‐term biopotentials and human–machine interfaces for operating home electronics. The LIHCNFs‐tattoo with high breathability (≈14 mg cm−2 h−1) forms compliant contact with human skin, resulting in low electrode‐skin impedance (23.59 kΩ cm2) and low‐noise biopotential signals (signal‐to‐noise ratio, SNR = 41 dB). This finding offers a complementary polymer precursor and carbonization method to produce CNFs with proper structural features and designs for multifunctional biointerfaces.
Optimized Charge Transport in Molecular Semiconductors by Control of Fluid Dynamics and Crystallization in Meniscus‐Guided Coating
Authors: Yildiz Okan , Wang Zuyuan , Borkowski Michal , Fytas George , Blom Paul W. M. , Michels Jasper J. , Pisula Wojciech , Marszalek Tomasz 
Published: October 2021

AbstractThe effects of the casting speed and solute concentration on the crystallization of 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) during meniscus‐guided coating (MGC) are investigated, and three morphological subregimes with increasing casting speed are identified: I) an isotropic domain‐like structure; II) unidirectionally aligned crystalline bands; and III) a corrugated dendritic morphology. Interestingly, increasing the solute concentration does not affect these morphologies but merely the associated transition velocities. Numerical simulation of both the fluid dynamics in the coating bead and the crystallization itself not only explains these morphological trends but also the decrease in the width of the crystalline bands of morphology II with the casting speed. They demonstrate that the latter provides an optimal processing window for organic field‐effect transistors, with minimized charge trapping, maximized on/off ratio, and reliability factor.
The Evolution of Photoluminescence Properties of PEA2SnI4 Upon Oxygen Exposure: Insight into Concentration Effects
Authors: Ju Yangyang , Wu Xian‐gang , Huang Sheng , Dai Guang , Song Tinglu , Zhong Haizheng 
Published: October 2021

AbstractThe time evolution of the photoluminescence properties in phenylethylammonium tin halide perovskite (PEA2SnI4) film as a function of oxygen concentration is reported. Photo‐brightening and reversible photoluminescence quenching are observed in PEA2SnI4 film at ultralow oxygen concentration (< 1.5 vol%). In the case of 1.5 vol% < [O2] < 21 vol%, the photoluminescence emission of PEA2SnI4 film can be partially recovered after resetting the samples to nitrogen box. As the oxygen concentration further increases with the range of 21 to 95 vol%, the photoluminescence emission of PEA2SnI4 film is significantly quenched and can only be slightly recovered after removing it to the nitrogen box. By correlating the material characterizations and theoretical analysis, the interactions between PEA2SnI4 and oxygen contain physisorption and chemical reactions are illustrated. Depending on the oxygen concentration, the chemical reactions between PEA2SnI4 and oxygen can be reversible and/or irreversible. The insights into oxygen concentration effects provide a guideline to optimize the stability of PEA2SnI4 for achieving high‐performance optoelectronic devices.
A Biofilm Microenvironment‐Activated Single‐Atom Iron Nanozyme with NIR‐Controllable Nanocatalytic Activities for Synergetic Bacteria‐Infected Wound Therapy
Authors: Xu Qiqi , Hua Yusheng , Zhang Yuetong , Lv Mingzhu , Wang Huan , Pi Yang , Xie Jiani , Wang Chengyan , Yong Yuan 
Published: October 2021

AbstractBiofilm microenvironment (BME)‐activated antimicrobial agents display great potential for improved biofilm‐related infection therapy because of their superior specificities and sensitivities, effective eliminations, and minimal side effects. Herein, BME‐activated Fe‐doped polydiaminopyridine nanofusiform‐mediated single‐atom nanozyme (FePN SAzyme) is presented for photothermal/chemodynamic synergetic bacteria‐infected wound therapy. The photothermal therapy (PTT) function of SAzyme can be specifically initiated by the high level of H2O2 and further accelerated through mild acid within the inflammatory environment through “two‐step rocket launching‐like” process. Additionally, the enhanced chemodynamic therapy (CDT) for the FePN SAzyme can also be endowed by producing hydroxyl radicals through reacting with H2O2 and consuming glutathione (GSH) of the BME, thereby contributing to more efficient synergistic therapeutic effect. Meanwhile, FePN SAzyme could catalyze biofilm‐overexpressed H2O2 decomposing into O2 and overcome the hypoxia of biofilm, which significantly enhances the susceptibility of biofilm and increases the synergistic efficacy. Most importantly, the synergistic therapy of bacterial‐induced infection diseases can be switched on by the internal and external stimuli simultaneously, resulting in minimal nonspecific damage to healthy tissue. These remarkable characteristics of FePN SAzyme not only develop an innovative strategy for the BME‐activated combination therapy but also open a new avenue to explore other nanozyme‐involved nanoplatforms for bacterial biofilm infections.
Interactions of Metal Nanoclusters with Light: Fundamentals and Applications
Authors: Chen Tiankai , Lin Hongbin , Cao Yitao , Yao Qiaofeng , Xie Jianping 
Published: October 2021

AbstractThe interactions of materials with light determine their applications in various fields. In the past decade, ultrasmall metal nanoclusters (NCs) have emerged as a promising class of optical materials due to their unique molecular‐like properties. Herein, the basic principles of optical absorption and photoluminescence of metal NCs, their interactions with polarized light, and light‐induced chemical reactions, are discussed, highlighting the roles of the core and protecting ligands/motifs of metal NCs in their interactions with light. The metal core and protecting ligands/motifs determine the electronic structures of metal NCs, which are closely related to their optical properties. In addition, the protecting ligands/motifs of metal NCs contribute to their photoluminescence and chiral origin, further promoting the interactions of metal NCs with light through various pathways. The fundamentals of light–NC interactions provide guidance for the design of metal NCs in optical applications, which are discussed in the second part. In the last section, some strategies are proposed to further understand light–NC interactions, highlighting the challenges and opportunities. It is hoped that this work will stimulate more research on the optical properties of metal NCs and their applications in various fields.
ZnS@BSA Nanoclusters Potentiate Efficacy of Cancer Immunotherapy
Authors: Cen Dong , Ge Qiwei , Xie Congkun , Zheng Qiang , Guo Jiansheng , Zhang Yuqi , Wang Yifan , Li Xiang , Gu Zhen , Cai Xiujun 
Published: October 2021

AbstractAlthough immunotherapy such as immune checkpoint inhibitors has shown promising efficacy in cancer treatment, the responsiveness among patients is relatively limited. Activation of the cyclic guanosine monophosphate‐adenosine monophosphate synthase/interferon gene stimulator (cGAS/STING) signaling pathway to upregulate innate immunity has become an emerging strategy for enhancing tumor immunotherapy. Herein, ZnS@BSA (bovine serum albumin) nanoclusters synthesized via a self‐assembly approach are reported, where the released zinc ions under acidic tumor microenvironment significantly enhance cGAS/STING signals. Meanwhile, intracellular zinc ions can produce reactive oxygen species, which is further facilitated by the generated H2S gas from ZnS@BSA via specifically inhibiting catalase in hepatocellular carcinoma cells. It is found that the nanoclusters activate the cGAS/STING signals in mice, which promotes the infiltration of CD8+ T cells at the tumor site and cross‐presentation of dendritic cells, leading to an improved immunotherapy efficacy against hepatocellular carcinoma.
Self‐Assembled Carbon Superstructures Achieving Ultra‐Stable and Fast Proton‐Coupled Charge Storage Kinetics
Authors: Song Ziyang , Miao Ling , Ruhlmann Laurent , Lv Yaokang , Zhu Dazhang , Li Liangchun , Gan Lihua , Liu Mingxian 
Published: October 2021

AbstractDesigning ingenious and stable carbon nanostructures is critical but still challenging for use in energy storage devices with superior electrochemistry kinetics, durable capacitive activity, and high rate survivability. To pursue the objective, a simple self‐assembly strategy is developed to access carbon superstructures built of nanoparticle embedded plates. The carbon precursors, 2,4,6‐trichloro‐1,3,5‐triazine and 2,6‐diaminoanthraquinone can form porous organic polymer with “protic salt”‐type rigid skeleton linked by −NH2+Cl−− “rivets”, which provides the cornerstone for hydrogen‐bonding‐guided self‐assembly of the organic backbone to superstructures by π−π plane stacking. The ameliorative charge density distribution and decreased adsorption energy in as‐fabricated carbon superstructures allow the high accessibility of the build‐in protophilic sites and efficient ion diffusion with a low energy barrier. Such superstructures thus deliver ultra‐stable charge storage and fast proton‐coupled kinetics at the structural−chemical defects, contributing to unprecedented lifespan (1 000 000 cycles), high‐rate capability (100 A g−1) for carbon‐based supercapacitors, and an ultrahigh energy density (128 Wh kg−1) for Zn‐ion hybrid supercapacitors. The self‐assembled carbon superstructures significantly improve the all‐round electrochemical performances, and hold great promise for efficient energy storage.
Towards High Performance Li–S Batteries via Sulfonate‐Rich COF‐Modified Separator
Authors: Xu Jie , An Shuhao , Song Xianyu , Cao Yongjie , Wang Nan , Qiu Xuan , Zhang Yu , Chen Jiawei , Duan Xianli , Huang Jianhang , Li Wei , Wang Yonggang 
Published: October 2021

AbstractLithium–sulfur (Li–S) batteries are held great promise for next‐generation high‐energy‐density devices; however, polysulfide shuttle and Li‐dendrite growth severely hinders their commercial production. Herein, a sulfonate‐rich COF (SCOF‐2) is designed, synthesized, and used to modify the separator of Li–S batteries, providing a solution for the above challenges. It is found that the SCOF‐2 features stronger electronegativity and larger interlayer spacing than that of none/monosulfonate COFs, which can facilitate the Li+ migration and alleviate the formation of Li‐dendrites. Density functional theory (DFT) calculations and in situ Raman analysis demonstrate that the SCOF‐2 possesses a narrow bandgap and strong interaction on sulfur species, thereby suppressing self‐discharge behavior. As a result, the modified batteries deliver an ultralow attenuation rate of 0.047% per cycle over 800 cycles at 1 C, and excellent anti‐self‐discharge performance by a low‐capacity attenuation of 6.0% over one week. Additionally, even with the high‐sulfur‐loading cathode (3.2–8.2 mgs cm‐2) and lean electrolyte (5 µL mgs‐1), the batteries still exhibit ≈80% capacity retention over 100 cycles, showing great potential for practical application.
Ultrafast Thermal Imprinting of Plasmonic Hotspots
Authors: Askes Sven H. C. , Garnett Erik C. 
Published: October 2021

AbstractPlasmonic photochemistry is driven by a rich collection of near‐field, hot charge carrier, energy transfer, and thermal effects, most often accomplished by continuous wave illumination. Heat generation is usually considered undesirable, because noble metal nanoparticles heat up isotropically, losing the extreme energy confinement of the optical resonance. Here it is demonstrated through optical and heat‐transfer modelling that the judicious choice of nanoreactor geometry and material enables the direct thermal imprint of plasmonic optical absorption hotspots onto the lattice with high fidelity. Transition metal nitrides (TMNs, e.g., TiN/HfN) embody the ideal material requirements, where ultrafast electron–phonon coupling prevents fast electronic heat dissipation and low thermal conductivity prolongs the heat confinement. The extreme energy confinement leads to unprecedented peak temperatures and internal heat gradients (>10 K nm−1) that cannot be achieved using noble metals or any current heating method. TMN nanoreactors consequently yield up to ten thousand times more product in pulsed photothermal chemical conversion compared with noble metals (Ag, Au, Cu). These findings open up a completely unexplored realm of nano‐photochemistry, where adjacent reaction centers experience substantially different temperatures for hundreds of picoseconds, long enough for bond breaking to occur.
Organic Single Crystals with High Photoluminescence Quantum Yields Close to 100% and High Mobility for Optoelectronic Devices
Authors: Tao Jingwei , Liu Dan , Jing Jiangbo , Dong Huanli , Liu Leijing , Xu Bin , Tian Wenjing 
Published: October 2021

AbstractOrganic single crystals with excellent optical and electrical properties are critical for the development of organic optoelectronics. Herein, two compounds 9,10‐bis([N,N‐diphenyl]‐4′‐phenylethynyl)anthracene (TPA‐An) and 9,10‐bis([1′,3′‐diphenyl]‐5′‐phenylethynyl)anthracene (TBA‐An) are synthesized by introducing two different luminescent groups, triphenylamine and 1,3‐diphenylbenzene, at the 9,10 positions of anthracene via triple bond connection. Single crystals based on TPA‐An and TBA‐An with a ribbon morphology obtained through the slow solvent‐evaporation method exhibit high photoluminescence quantum yields (PLQYs) of 98% and 99% at room temperature, and remarkable hole mobilities of 0.45 and 0.15 cm2 V−1 s−1 in single‐crystal organic field‐effect transistors (SC‐OFETs). Furthermore, UV phototransistors based on the two single crystals obtain photosensitivities of 1.03 × 103 and 3.45 × 104, ultrahigh photoresponsivities of 7.19 × 105 and 1.50 × 105 A W−1, and the detectivities exceeding 1.40 × 1016 and 1.60 × 1017 Jones.
Self‐Powered InP Nanowire Photodetector for Single‐Photon Level Detection at Room Temperature
Authors: Zhu Yi , Raj Vidur , Li Ziyuan , Tan Hark Hoe , Jagadish Chennupati , Fu Lan 
Published: October 2021

AbstractHighly sensitive photodetectors with single‐photon level detection are one of the key components to a range of emerging technologies, in particular the ever‐growing field of optical communication, remote sensing, and quantum computing. Currently, most of the single‐photon detection technologies require external biasing at high voltages and/or cooling to low temperatures, posing great limitations for wider applications. Here, InP nanowire array photodetectors that can achieve single‐photon level light detection at room temperature without an external bias are demonstrated. Top‐down etched, heavily doped p‐type InP nanowires and n‐type aluminium‐doped zinc oxide (AZO)/zinc oxide (ZnO) carrier‐selective contact are used to form a radial p–n junction with a built‐in electric field exceeding 3 × 105 V cm−1 at 0 V. The device exhibits broadband light sensitivity and can distinguish a single photon per pulse from the dark noise at 0 V, enabled by its design to realize near‐ideal broadband absorption, extremely low dark current, and highly efficient charge carrier separation. Meanwhile, the bandwidth of the device reaches above 600 MHz with a timing jitter of 538 ps. The proposed device design provides a new pathway toward low‐cost, high‐sensitivity, self‐powered photodetectors for numerous future applications.
Tin Halide Perovskites: From Fundamental Properties to Solar Cells
Authors: Pitaro Matteo , Tekelenburg Eelco Kinsa , Shao Shuyan , Loi Maria Antonietta 
Published: October 2021

AbstractMetal halide perovskites have unique optical and electrical properties, which make them an excellent class of materials for a broad spectrum of optoelectronic applications. However, it is with photovoltaic devices that this class of materials has reached the apotheosis of popularity. High power conversion efficiencies are achieved with lead‐based compounds, which are toxic to the environment. Tin‐based perovskites are the most promising alternative because of their bandgap close to the optimal value for photovoltaic applications, the strong optical absorption, and good charge carrier mobilities. Nevertheless, the low defect tolerance, the fast crystallization, and the oxidative instability of tin halide perovskites currently limit their efficiency. The aim of this review is to give a detailed overview of the crystallographic, photophysical, and optoelectronic properties of tin‐based perovskite compounds in their multiple forms from 3D to low‐dimensional structures. At the end, recent progress in tin‐based perovskite solar cells are reviewed, mainly focusing on the detail of the strategies adopted to improve the device performances. For each subtopic, the current challenges and the outlook are discussed, with the aim to stimulate the community to address the most important issues in a concerted manner.
High‐Performance Harsh‐Environment‐Resistant GaOX Solar‐Blind Photodetectors via Defect and Doping Engineering
Authors: Hou Xiaohu , Zhao Xiaolong , Zhang Ying , Zhang Zhongfang , Liu Yan , Qin Yuan , Tan Pengju , Chen Chen , Yu Shunjie , Ding Mengfan , Xu Guangwei , Hu Qin , Long Shibing 
Published: October 2021

AbstractGallium oxide (Ga2O3), with an ultrawide bandgap, is currently regarded as one of the most promising materials for solar‐blind photodetectors (SBPDs), which are greatly demanded in harsh environment, such as space exploration and flame prewarning. However, realization of high‐performance SBPDs with high tolerance toward harsh environments based on low‐cost Ga2O3 material faces great challenges. Here, defect and doping (DD) engineering towards amorphous GaOX (a‐GaOX) has been proposed to obtain ultrasensitive SBPDs for harsh condition application. Serious oxygen deficiency and doping compensation of the engineered a‐GaOX film ensure the high response currents and low dark currents, respectively. Annealing item in nitrogen of DD engineering also incurs the recrystallization of material, formation of nanopores by oxygen escape, and suppression of sub‐bandgap defect states. As a result, the tailored GaOX SBPD based on DD engineering not only harvests a record‐high responsivity rejection ratio (R254 nm/R365 nm) of 1.8 × 107, 102 times higher detectivity, and 2 × 102 times faster decay speed than the control device, but also keeps a high responsivity, high photo‐to‐dark current ratio, and sharp imaging capability even at high temperature (280 °C) or high bias (100 V). The proposed DD engineering provides an effective strategy towards highly harsh‐environment‐resistant GaOX SBPDs.