bluuebunny/crossref_metadata_2025_split huggingface dataset:
Liquid‐Metal‐Based Nanophotonic Structures for High‐Performance SEIRA Sensing
Authors: Miao Xianglong , Luk Ting Shan , Liu Peter Q. 
Published: January 2022

AbstractSurface‐enhanced infrared absorption (SEIRA) spectroscopy can provide label‐free, nondestructive detection and identification of analytes with high sensitivity and specificity, and therefore has been widely used for various sensing applications. SEIRA sensors usually employ resonant nanophotonic structures, which can substantially enhance the electric field and hence light–matter interactions by orders of magnitude in certain nanoscale hot spots of the devices. However, as ever, smaller hot spots are employed to further enhance the field, the delivery of analytes into such hot spots becomes increasingly challenging. Here, high‐performance nanophotonic SEIRA sensors based on nanopatch antennas with a liquid gallium ground plane are demonstrated, which not only lead to ultrahigh field confinement and enhancement, but also allow for convenient and efficient delivery of analytes into nanometric hot spots by employing a simple procedure suitable for point‐of‐care applications. The sensors exhibit superior sensitivity in the midinfrared spectral region. Around 10% molecular vibrational signals (i.e., the modulation of a sensor's reflection spectrum owing to the molecular vibrational modes of the analytes) near 2900 cm−1 are achieved from sensing monolayer 1‐octadecanethiol. This cost‐effective and reliable method for realizing liquid‐metal‐based nanophotonic structures provides a new strategy for developing high‐performance sensors and other photonics applications in the infrared region.
Synthetic Matrix Scaffolds Engineer the In Vivo Tumor Immune Microenvironment for Immunotherapy Screening
Authors: O'Melia Meghan J. , Mulero‐Russe Adriana , Kim Jihoon , Pybus Alyssa , DeRyckere Deborah , Wood Levi , Graham Douglas K. , Botchwey Edward , García Andrés J. , Thomas Susan N. 
Published: January 2022

AbstractImmunotherapy has emerged as one of the most powerful anti‐cancer therapies but is stymied by the limits of existing preclinical models with respect to disease latency and reproducibility. Additionally, the influence of differing immune microenvironments within tumors observed clinically and associated with immunotherapeutic resistance cannot be tuned to facilitate drug testing workflows without changing model system or laborious genetic approaches. To address this testing platform gap in the immune oncology drug development pipeline, the authors deploy engineered biomaterials as scaffolds to increase tumor formation rate, decrease disease latency, and diminish variability of immune infiltrates into tumors formed from murine mammary carcinoma cell lines implanted into syngeneic mice. By altering synthetic gel formulations that reshape infiltrating immune cells within the tumor, responsiveness of the same tumor model to varying classes of cancer immunotherapies, including in situ vaccination with a molecular adjuvant and immune checkpoint blockade, diverge. These results demonstrate the significant role the local immune microenvironment plays in immunotherapeutic response. These engineered tumor immune microenvironments therefore improve upon the limitations of current breast tumor models used for immune oncology drug screening to enable immunotherapeutic testing relevant to the variability in tumor immune microenvironments underlying immunotherapeutic resistance seen in human patients.
High‐Performance Memristors Based on Ultrathin 2D Copper Chalcogenides
Authors: Yin Lei , Cheng Ruiqing , Wen Yao , Zhai Baoxing , Jiang Jian , Wang Hao , Liu Chuansheng , He Jun 
Published: January 2022

AbstractCopper chalcogenides represent a class of materials with unique crystal structures, high electrical conductivity, and earth abundance, and are recognized as promising candidates for next‐generation green electronics. However, their 2D structures and the corresponding electronic properties have rarely been touched. Herein, a series of ultrathin copper chalcogenide nanosheets with thicknesses down to two unit cells are successfully synthesized, including layered Cu2Te, as well as nonlayered CuSe and Cu9S5, via van der Waals epitaxy, and their nonvolatile memristive behavior is investigated for the first time. Benefiting from the highly active Cu ions with low migration barriers, the memristors based on ultrathin 2D copper chalcogenide crystals exhibit relatively small switching voltage (≈0.4 V), fast switching speed, high switching uniformity, and wide operating temperature range (from 80 to 420 K), as well as stable retention and good cyclic endurance. These results demonstrate their tangible applications in future low‐power, cryogenic, and high temperature harsh electronics.
Synergistic Disruption of Metabolic Homeostasis through Hyperbranched Poly(ethylene glycol) Conjugates as Nanotherapeutics to Constrain Cancer Growth
Authors: Pan Dayi , Zheng Xiuli , Zhang Lu , Li Xin , Zhu Guonian , Gong Meng , Kopytynski Michal , Zhou Luonan , Yi Yong , Zhu Hongyan , Tian Xiaohe , Chen Rongjun , Zhang Hu , Gu Zhongwei , Gong Qiyong , Luo Kui 
Published: January 2022

AbstractCombination therapy is a promising approach for effective treatment of tumors through synergistically regulating pathways. However, the synergistic effect is limited, likely by uncontrolled co‐delivery of different therapeutic payloads in a single nanoparticle. Herein, a combination nanotherapeutic is developed by using two amphiphilic conjugates, hyperbranched poly(ethylene glycol)–pyropheophorbide‐a (Ppa) (HP‐P) and hyperbranched poly(ethylene glycol)–doxorubicin (DOX) (HP‐D) to construct co‐assembly nanoparticles (HP‐PD NPs) for controllably co‐loading and co‐delivering Ppa and DOX. In vitro and in vivo antitumor studies confirm the synergistic effect of photodynamic therapy and chemotherapy from HP‐PD NPs. Metabolic variations reveal that tumor suppression is associated with disruption of metabolic homeostasis, leading to reduced protein translation. This study uncovers the manipulation of metabolic changes in tumor cells through disruption of cellular homeostasis using HP‐PD NPs and provides a new insight into the rational design of synergistic nanotherapeutics for combination therapy.
A New Strategy for Microbial Taxonomic Identification through Micro‐Biosynthetic Gold Nanoparticles and Machine Learning
Authors: Yu Ting , Su Shixuan , Hu Jing , Zhang Jun , Xianyu Yunlei 
Published: January 2022

AbstractMicroorganisms can serve as biological factories for the synthesis of inorganic nanomaterials that can become useful as nanocatalysts, energy‐harvesting–storage components, antibacterial agents, and biomedical materials. Herein, the development of biosynthesis of inorganic nanomaterials into a simple, stable, and accurate strategy for distinguishing microorganisms from multiple classification levels (i.e., kingdom, order, genus, and species) without gene amplification, biochemical testing, or target recognition is reported. Gold nanoparticles (AuNPs) biosynthesized by different microorganisms differ in color of the solution, and their features can be characterized, including the particle size, the surface plasmon resonance (SPR) spectrum, and the surface potential. The inter‐relation between the features of micro‐biosynthetic AuNPs and the classification of microorganisms are exploited at different levels through machine learning to establish a taxonomic model. This model agrees well with traditional classification methods that offers a new strategy for microbial taxonomic identification. The underlying mechanism of this strategy is related to the biomolecules produced by different microorganisms including glucose, glutathione, and nicotinamide adenine dinucleotide phosphate‐dependent reductase that regulate the features of micro‐biosynthetic AuNPs. This work broadens the application of biosynthesis of inorganic materials through micro‐biosynthetic AuNPs and machine learning, which holds great promise as a tool for biomedical research.
Efficient and Ultraviolet‐Durable Nonfullerene Organic Solar Cells: From Interfacial Passivation and Microstructural Modification Perspectives
Authors: Lan Weixia , Gu Jialu , Gao Xiaohui , Gong Chunliu , Liu Yuanyuan , Zhang Weidong , Sun Yi , Yue Tao , Wei Bin , Zhu Furong 
Published: January 2022

AbstractUltraviolet (UV)‐durable organic solar cells (OSCs) are realized by incorporating a CdSe@ZnS quantum dots (QDs)‐modified PEDOT:PSS hole extraction layer (HEL). The use of the CdSe@ZnS QDs‐modified PEDOT:PSS HEL has an obvious improvement in UV‐durability of OSCs. A more than 50% reduction in the power conversion efficiency (PCE) is observed for a (PM6:Y6)‐based control OSC with a PEDOT:PSS HEL, under the 1000 min accelerated UV (365 nm, 16 W) aging test. Whereas a much reduced reduction of 35% in PCE is observed for the OSCs with a CdSe@ZnS QDs‐modified PEDOT:PSS HEL, under the same accelerated UV aging test condition. Results reveal that the Coulombic attraction between the PEDOT units and PSS chains in the PEDOT:PSS layer is disturbed due to the interaction between hydroxyl ligands of the CdSe@ZnS QDs and PSS through hydrogen bond, leading to an increase in the electric conductivity in PEDOT:PSS layer through transforming PEDOT quinoid structure to expanded‐coil structure. The use of the CdSe@ZnS QDs‐modified PEDOT:PSS HEL also favors the efficient operation of the nonfullerene acceptor (NFA)‐based OSCs through maintaining a high built‐in potential across the bulk heterojunction. The results demonstrate the importance of the interface engineering to alleviate UV light‐induced degradation processes of NFA‐based OSCs.
Highly Performed Fiber‐Based Supercapacitor in a Conjugation of Mesoporous MXene
Authors: Guo Zijiao , Lu Zan , Li Yue , Liu Wei 
Published: January 2022

AbstractWith the continuous demands for wearable electronics, the embeddable power sources have drawn attention to develop advanced electrode materials and feasible manufacture procedures. Fiber‐based flexible energy storage devices have the potential to be practically integrated by utilizing the high‐performance materials with precisely constructed structures. Herein, a novel approach is presented to achieve an outstanding fiber‐based supercapacitor by simultaneous wet‐spinning of mesoporous MXene (Ti3C2Tx) nanoflakes. The volumetric capacitance of the porous fiber is enhanced up to ≈145% when the content of mesoporous MXene reaches 15 wt%. The symmetric all‐solid‐state fiber supercapacitor shows an extraordinary capability of 821.5 F cm–3 at a current density of 0.5 A cm–3, which reflects an enormous improvement to that of a nonporous MXene fiber‐based supercapacitor. The measured energy density is 8.9 mWh cm–3 at a power density of 401 mW cm–3, which also indicates the effective synergy of the constructed pathways for ions and electrons. This work demonstrates the feasibility of scalable production of fiber‐based electrode materials with porous MXene for powering wearable applications.
Enabling Modular Autonomous Feedback‐Loops in Materials Science through Hierarchical Experimental Laboratory Automation and Orchestration
Authors: Rahmanian Fuzhan , Flowers Jackson , Guevarra Dan , Richter Matthias , Fichtner Maximilian , Donnely Phillip , Gregoire John M. , Stein Helge S. 
Published: January 2022

AbstractMaterials acceleration platforms (MAPs) operate on the paradigm of integrating combinatorial synthesis, high‐throughput characterization, automatic analysis, and machine learning. Within a MAP, one or multiple autonomous feedback loops may aim to optimize materials for certain functional properties or to generate new insights. The scope of a given experiment campaign is defined by the range of experiment and analysis actions that are integrated into the experiment framework. Herein, the authors present a method for integrating many actions within a hierarchical experimental laboratory automation and orchestration (HELAO) framework. They demonstrate the capability of orchestrating distributed research instruments that can incorporate data from experiments, simulations, and databases. HELAO interfaces laboratory hardware and software distributed across several computers and operating systems for executing experiments, data analysis, provenance tracking, and autonomous planning. Parallelization is an effective approach for accelerating knowledge generation provided that multiple instruments can be effectively coordinated, which the authors demonstrate with parallel electrochemistry experiments orchestrated by HELAO. Efficient implementation of autonomous research strategies requires device sharing, asynchronous multithreading, and full integration of data management in experimental orchestration, which to the best of the authors’ knowledge, is demonstrated for the first time herein.
Enhancing Penetration Ability of Semiconducting Polymer Nanoparticles for Sonodynamic Therapy of Large Solid Tumor
Authors: Wang Xin , Wu Min , Li Haoze , Jiang Jianli , Zhou Sensen , Chen Weizhi , Xie Chen , Zhen Xu , Jiang Xiqun 
Published: January 2022

AbstractSonodynamic therapy (SDT) holds growing promise in deep‐seated or large solid tumor treatment owing to its high tissue penetration depth ability; however, its therapeutic efficacy is often compromised due to the hypopermeable and hypoxic characteristics in the tumor milieu. Herein, a semiconducting polymer nanoparticle (SPNC) that synergistically enhances tumor penetration and alleviates tumor hypoxia is reported for sonodynamic therapy of large solid tumors. SPNC comprises a semiconducting polymer nanoparticle core as a sonodynamic converter coated with a poly (ethylene glycol) corona. An oxygen‐modulating enzyme, catalase, is efficiently conjugated to the surface of nanoparticles via the coupling reaction. Superior to its counterpart SPNCs (SPNC2 (84 nm) and SPNC3 (134 nm)), SPNC with the smallest size (SPNC1 (35 nm)) can efficiently penetrate throughout the tumor interstitium to alleviate whole tumor hypoxia in a large solid tumor model. Upon ultrasound (US) irradiation, SPNC1 can remotely generate sufficient singlet oxygen to eradicate tumor cells at a deep‐tissue depth. Such a single treatment of SPNC1‐medicated sonodynamic therapy effectively inhibits tumor growth in a large solid tumor mouse model. Therefore, this study provides a generalized strategy to synergistically overcome both poor penetration and hypoxia of large tumors for enhanced cancer treatment.
High‐Efficiency Non‐Fullerene Acceptors Developed by Machine Learning and Quantum Chemistry
Authors: Zhang Qi , Zheng Yu Jie , Sun Wenbo , Ou Zeping , Odunmbaku Omololu , Li Meng , Chen Shanshan , Zhou Yongli , Li Jing , Qin Bo , Sun Kuan 
Published: January 2022

AbstractY6 and its derivatives have greatly improved the power conversion efficiency (PCE) of organic photovoltaics (OPVs). Further developing high‐performance Y6 derivative acceptor materials through the relationship between the chemical structures and properties of these materials will help accelerate the development of OPV. Here, machine learning and quantum chemistry are used to understand the structure–property relationships and develop new OPV acceptor materials. By encoding the molecules with an improved one‐hot code, the trained machine learning model shows good predictive performance, and 22 new acceptors with predicted PCE values greater than 17% within the virtual chemical space are screened out. Trends associated with the discovered high‐performing molecules suggest that Y6 derivatives with medium‐length side chains have higher performance. Further quantum chemistry calculations reveal that the end acceptor units mainly affect the frontier molecular orbital energy levels and the electrostatic potential on molecular surface, which in turn influence the performance of OPV devices. A series of promising Y6 derivative candidates is screened out and a rational design guide for developing high‐performance OPV acceptors is provided. The approach in this work can be extended to other material systems for rapid materials discovery and can provide a framework for designing novel and promising OPV materials.
Toward Hydrogen‐Free and Dendrite‐Free Aqueous Zinc Batteries: Formation of Zincophilic Protective Layer on Zn Anodes
Authors: Hong Lin , Wang Liang‐Yu , Wang Yuling , Wu Xiuming , Huang Wei , Zhou Yongfeng , Wang Kai‐Xue , Chen Jie‐Sheng 
Published: January 2022

AbstractRechargeable aqueous Zn‐ion batteries (ZIBs) are regarded as one of the most promising devices for the next‐generation energy storage system. However, the uncontrolled dendrite growth on Zn metal anodes and the side hydrogen evolution reaction, which has not yet been well considered, hinder the practical application of these batteries. Herein, a uniform and robust metallic Sb protective layer is designed based on the theoretic calculation and decorated on Zn plate via in situ replacement reaction. Compared with the bare Zn plate, the as‐prepared Zn@Sb electrode provides abundant zincophilic sites for Zn nucleation, and homogenizes the electric field around the Zn anode surface, both of which promote the uniform Zn deposition to achieve a dendrite‐free morphology. Moreover, the Gibbs free energy (∆GH) calculation and in situ characterization demonstrate that hydrogen evolution reaction can be effectively suppressed by the Sb layer. Consequently, Sb‐modified Zn anodes exhibit an ultralow voltage hysteresis of 34 mV and achieve excellent cycling stability over 1000 h with hydrogen‐ and dendrite‐free behaviors. This work provides a facile and effective strategy to suppress both hydrogen evolution reaction and dendrite growth.
Development and Prospects of Halide Perovskite Single Crystal Films
Authors: Gao Wenxiu , Zhang Zhuolei , Xu Rukai , Chan Emory M. , Yuan Guoliang , Liu Jun‐Ming 
Published: January 2022

AbstractHalide perovskite single crystal (HPSC) films have demonstrated extraordinary performance in solar cells, photodetectors, and lighting applications, owing to the high carrier mobility, long carrier diffusion length, tunable bandgap, and large light absorption coefficients of these materials. Here, the recent development of the major HPSC thin films is reviewed systematically, including MAPbI3, α‐FAPbI3, MAPbBr3, CsPbBr3, with special emphasis on different classes of fabrication methods and thin‐film characteristics. Finally, the conclusion and prospects in this field are discussed in detail. It is anticipated that the HPSC thin films will lead to a compelling future for the rising electronic applications.
ULTRARAM: A Low‐Energy, High‐Endurance, Compound‐Semiconductor Memory on Silicon
Authors: Hodgson Peter D. , Lane Dominic , Carrington Peter J. , Delli Evangelia , Beanland Richard , Hayne Manus 
Published: January 2022

AbstractULTRARAM is a nonvolatile memory with the potential to achieve fast, ultralow‐energy electron storage in a floating gate accessed through a triple‐barrier resonant tunneling heterostructure. Here its implementation is reported on a Si substrate; a vital step toward cost‐effective mass production. Sample growth using molecular beam epitaxy commences with deposition of an AlSb nucleation layer to seed the growth of a GaSb buffer layer, followed by the III–V memory epilayers. Fabricated single‐cell memories show clear 0/1 logic‐state contrast after ≤10 ms duration program/erase pulses of ≈2.5 V, a remarkably fast switching speed for 10 and 20 µm devices. Furthermore, the combination of low voltage and small device capacitance per unit area results in a switching energy that is orders of magnitude lower than dynamic random access memory and flash, for a given cell size. Extended testing of devices reveals retention in excess of 1000 years and degradation‐free endurance of over 107 program/erase cycles, surpassing very recent results for similar devices on GaAs substrates.
Fast Charging Limits of Ideally Stable Metal Anodes in Liquid Electrolytes
Authors: Ma Bingyuan , Bai Peng 
Published: January 2022

AbstractNext‐generation high‐energy‐density batteries require ideally stable metal anodes, for which smooth metal deposits during battery recharging are considered a sign of interfacial stability that can ensure high efficiency and long cycle life. With the recent successes, whether the absolute morphological stability guarantees absolute electrochemical stability and safety has emerged as a critical question to be investigated in systematic experiments under practical conditions. Here, the ideally stable ingot‐type sodium metal anode is used as a model system to identify the fast‐charging limits, that is, highest safe current density, of metal anodes. The results show that metal penetration can still occur at relatively low current densities, but the overpotentials at the penetration depend on the pore sizes of the separators and surprisingly follow a simple mathematical model developed as the Young–Laplace overpotential. This study suggests that the success of stable metal batteries with even the ideally smooth metal anode requires the holistic design of the electrolyte, separator, and metal anodes to ensure penetration‐free operation.
Boosting the Thermoelectric Performance of PbSe from the Band Convergence Driven By Spin‐Orbit Coupling
Authors: Cai Jianfeng , Yang Junxuan , Liu Guoqiang , Xu Liang , Wang Xuemei , Hu Haoyang , Tan Xiaojian , Jiang Jun 
Published: January 2022

AbstractPbSe has been expected to be a competitor of the excellent thermoelectric material PbTe, whereas its performance has proved to be limited by its intrinsic electronic structure. In this work, the improved thermoelectric performance of PbSe originating in the novel spin‐orbit coupling effect is reported. By alloying with NaSbSe2, valence band convergence and bandgap enlargement are achieved in PbSe, resulting in a significantly enlarged Seebeck coefficient. Theoretical calculations indicate that a modified electronic structure by spin‐orbit coupling would lead to exotic thermoelectric properties and that it prefers a lower carrier concentration than the known optimal value for PbSe. When Cd‐doping is introduced to decrease the carrier concentration, a high peak ZT of 1.6 at 850 K and a remarkable average ZT of 0.95 are obtained in Pb0.8Na0.1Sb0.08Cd0.02Se. Among the reported high ZT PbSe‐based compounds, the sample exhibits the highest Seebeck coefficient and lowest thermal conductivity. This study provides an insight into band structure tuning of Lead chalcogenides and promotes a new strategy for the optimization of thermoelectric performance.
Progress and Perspectives of Organosulfur for Lithium–Sulfur Batteries
Authors: Pan Zhiyong , Brett Dan J. L. , He Guanjie , Parkin Ivan P. 
Published: January 2022

AbstractLithium–sulfur batteries (LSBs) with high theoretical capacity are regarded as the most promising candidates for next‐generation energy storage systems. However, the low conductivity, high volume change, and shuttle effect need to be addressed before the commercialization of LSBs. Organosulfur with covalent CS bonds can solve these problems when applied as different components of LSBs. Recent advances of application of organosulfur as cathodes, electrolytes, interlayers, and binders in LSBs are reviewed. Finally, the prospects for organosulfur are proposed from both the perspectives of mechanism understanding and practical applications.