bluuebunny/crossref_metadata_2025_split huggingface dataset:
In Situ Reconstruction Post‐Treatment for Efficient Carbon‐Based Hole‐Conductor‐Free Printable Mesoscopic Perovskite Solar Cells
Authors: Han Chuanzhou , Du Jiankang , Liu Zhiyang , Gao Qiaojiao , Chen Xiayan , Xiang Junwei , Xiao Xufeng , Cheng Yanjie , Chen Kai , Xia Minghao , Liu Jiale , Yang Li‐Ming , Zhou Yang , Mei Anyi , Han Hongwei 
Published: August 2024

AbstractPerovskite solar cells are regarded as the most promising and disruptive photovoltaic of the new generation. Carbon‐based hole‐conductor‐free printable mesoscopic perovskite solar cells (p‐MPSCs) with three mesoscopic layers have garnered considerable interest owing to their simple manufacturing process and cost‐effective raw materials, signaling the potential for commercialization. However, the energy level mismatch between the perovskite and the carbon electrode as well as defects at perovskite grain boundaries inevitably lead to additional non‐radiative carrier recombination and large voltage loss. In this study, a facile in situ reconstruction post‐treatment approach is employed to integrate lead sulfide (PbS) and the two‐dimensional (2D) perovskite K2PbI4 into the mesoporous scaffolds of p‐MPSCs. In this way, grain boundary defects are effectively passivated and the ion migration is suppressed by introducing 2D perovskite K2PbI4 at grain boundaries. Besides, the incorporation of PbS leads to the downward shift of the Fermi level for perovskite, which enhances hole collection within the device by optimizing band alignment at the perovskite/carbon interface. Consequently, an improved efficiency exceeding 20% is achieved for p‐MPSCs with no significant performance degradation observed over a storage period of 235 days. This strategy provides a facile and novel approach toward fabricating highly efficient and stable p‐MPSCs.
Artificial Spider Silk Materials: From Molecular Design, Mesoscopic Assembly, to Macroscopic Performances
Authors: Shi Yu‐Xiao , Zhu Ya‐Jiao , Qian Zhi‐Gang , Xia Xiao‐Xia 
Published: August 2024

AbstractSpider silk is one of the strongest and toughest fibrous materials available in nature. Its superior properties make it a good candidate for applications in various fields ranging from protective body armor to scaffolds for medical implants. However, harvesting a substantial amount of natural spider silk remains challenging because spiders cannot be easily bred. With the development of synthetic biology and its integration with materials science, considerable research has been directed toward engineering and production of synthetic spider silk materials. Here the study overviews general strategies on molecular design, mesoscopic assembly, and macroscopic regulation of artificial spider silk materials. The insights into the correlation between silk protein sequences, mesoscopic assemblies, and macroscopic material properties are provided for guiding de novo design and engineering of next‐generation spider silk materials. This review also emphasizes the challenges and future perspectives for advancing the translational research on these designer functional materials for diverse applications.
Shifting d‐band Center: An Overlooked Factor in Broadening Electromagnetic Wave Absorption Bandwidth
Authors: Yao Kai , Pan Fei , Liang Hongsheng , Zhang Xiang , Li Lixin , Song Lixin , Yang Yang , Yuan Bin , Lu Wei 
Published: August 2024

AbstractAbsorption bandwidth is one of the key performance metrics for electromagnetic wave (EMW) absorbers. Traditional oxide absorbers, despite their merits such as abundance, long‐term stability, and low cost, have long been plagued by their inferior absorption bandwidth (typically less than 4 GHz). Herein, a novel concept is proposed: the introduction of cation vacancies and heterostructures into oxides can remarkably broaden their absorption bandwidth. A broadening value of 7.75 GHz is observed through this route, surpassing the broadening achieved by other existing engineering methods, by ≈100%. Crucially, this study discovers that a negative shift in the d‐band center, a previously overlooked factor, is responsible for this broadening phenomenon. By inducing cation vacancies and heterostructures, a negative shift in the d‐band center gives rise to an increase in carrier concentration and promotion of charge separation, resulting in higher conductive and polarization losses, ultimately leading to a broader absorption bandwidth. The applicability of this concept is validated in another distinctly different system, where the absorption bandwidth also experiences a remarkable increase (from 0 to 6.86 GHz). This study offers significant implications for designing wide bandwidth EMW absorbers and expands their applications in various scenarios such as wearable electronics and artificial intelligent devices.
Doubling Power Conversion Efficiency of Si Solar Cells
Authors: Li Zhigang , Chen Yingda , Guo Renqing , Wang Shuang , Wang Weike , Wang Tianle , Zhao Shuaitao , Li Jiteng , Wu Jianbo , Jin Zhongwen , Wang Sihan , Wei Bingqing 
Published: August 2024

AbstractImproving solar cells' power conversion efficiency (PCE) is crucial to further the deployment of renewable electricity. In addition, solar cells cannot function at exceedingly low temperatures owing to the carrier freeze‐out phenomenon. This report demonstrates that through temperature regulation, the PCE of monocrystalline single‐junction silicon solar cells can be doubled to 50–60% under monochromatic lasers and the full spectrum of AM 1.5 light at low temperatures of 30–50 K by inhibiting the lattice atoms' thermal oscillations for suppressing thermal loss, an inherent feature of monocrystalline Si cells. Moreover, the light penetration, determined by its wavelength, plays a critical role in alleviating the carrier freeze‐out effect and broadening the operational temperature range of silicon cells to temperatures as low as 10 K. Understanding these new observations opens tremendous opportunities for designing solar cells with even higher PCE to provide efficient and powerful energy sources for cryogenic devices and outer and deep space explorations.
Tailoring Polaron Dimensions in Lead‐Tin Hybrid Perovskites
Authors: Gao Lei , Zhang Heng , Zhang Yong , Fu Shuai , Geuchies Jaco J. , Valli Donato , Saha Rafikul Ali , Pradhan Bapi , Roeffaers Maarten , Debroye Elke , Hofkens Johan , Lu Junpeng , Ni Zhenhua , Wang Hai I. , Bonn Mischa 
Published: August 2024

AbstractCharge carriers in the soft and polar perovskite lattice form so‐called polaron quasiparticles, charge carriers dressed with a lattice deformation. The spatial extent of a polaron is governed by the material's electron‐phonon interaction strength, which determines charge carrier effective mass, mobility, and the so‐called Mott polaron density, that is, the maximum stable density of charge carriers that a perovskite can support. Despite its significance, controlling polaron dimensions has been challenging. Here, experimental substantial tuning of polaron dimensions is reported by lattice engineering, through Pb/Sn substitution in CH3NH3SnxPb1−xI3. The polaron dimension is deduced from the Mott polaron density, which can be composition‐tuned over an order of magnitude, while charge carrier mobility occurs through band transport, and remains substantial across all compositions, ranging from 10 s to 100 s cm2 V s−1 at room temperature. The effective modulation of polaron size can be understood by considering the bond asymmetry after carrier injection as well as the random spatial distribution of Pb/Sn ions. This study underscores the potential for tailoring polaron dimensions, which is crucial for optimizing applications prioritizing either high charge carrier density or high mobility.
Water‐Templated Growth of Interfacial Superglue Polymers for Tunable Thin Films and In Situ Fluid Encapsulation
Authors: Jampani Venkata S. R. , Škarabot Miha , Mur Urban , Baigl Damien , Jonas Ulrich , Lagerwall Jan P. F. , Ravnik Miha , Anyfantakis Manos 
Published: August 2024

AbstractThin polymer films (TPFs) are indispensable elements in numerous technologies ranging from liquid encapsulation to biotechnology to electronics. However, their production typically relies on wet chemistry involving organic solvents or chemical vapor deposition, necessitating elaborate equipment and often harsh conditions. Here, an eco‐friendly, fast, and facile synthesis of water‐templated interfacial polymers based on cyanoacrylates (superglues, CAs) that yield thin films with tailored properties is demonstrated. Specifically, by exposing a cationic surfactant‐laden water surface to cyanoacrylate vapors, surfactant‐modulated anionic polymerization produces a manipulable thin polymer film with a thickness growth rate of 8 nm min−1. Furthermore, the shape and color of the film are precisely controlled by the polymerization kinetics, wetting conditions, and/or exposure to patterned light. Using various interfaces as templates for film growth, including the free surface of drops and soap bubbles, the developed method advantageously enables in situ packaging of chemical and biological cargos in liquid phase as well as the encapsulation of gases within solidified bubbles. Simple, versatile, and biocompatible, this technology constitutes a potent platform for programmable coating and soft/smart encapsulation of fluids.
Plasmonic Resonance Shifts in Gold Nanoparticles‐Thermochromic VO2 Thin Film Hybrid Platforms: A Joint Experimental and Numerical Study
Authors: Savorianakis Grégory , Rousseau Cédric , Sergievskaya Anastasiya , Rosolen Gilles , Voué Michel , Maes Bjorn , Konstantinidis S. 
Published: August 2024

AbstractThe combination of the phase transition in thermochromic vanadium dioxide (VO2) with plasmonic nanoparticles paves the way for applications in various fields, including optical sensing, advanced coatings, and dynamic optical devices. This study presents a simple fabrication method to control both the size and surface coverage of NPs combined with VO2. First, a thermochromic VO2 coating with a phase transition at 68 °C is synthesized using reactive magnetron sputtering. Then, monodisperse 30 nm diameter gold NPs are bonded to the VO2 surface using (3‐aminopropyl)trimethoxysilane (APTMS) linkers, examining the effect of immersion duration on surface coverage. Two platforms are developed: a VO2 thin film with a monolayer of NPs and a configuration with NPs between two VO2 films. The temperature‐dependent plasmonic response of these platforms is measured by extinction spectroscopy, showing a significant wavelength resonance shift of approximately 10 nm for the first platform and 20 nm for the second. Optical simulations analyze this shift over various geometries, from isolated NPs to fully covered NPs, achieving a 60 nm shift for NPs embedded in a thin VO2 film. This study demonstrates an effective approach to synthesizing thermochromic VO2 coatings with gold NPs, offering insights into the plasmonic properties of hybrid platforms.
Ultra‐Thin Metal Oxide Superstructure of Pd(001) as Passivation Interlayer at Organic/Metal Interface
Authors: Majumdar Isheta , Goto Francesco , Calloni Alberto , Duò Lamberto , Ciccacci Franco , Bussetti Gianlorenzo 
Published: August 2024

AbstractAt organic molecule/metal interfaces for electronic applications, it is required of the metal surface to be passivated in view of preserving the molecular properties of the ordered organic layer. This can be achieved by screening the metal with a single atomic layer of O, namely, ultra‐thin metal oxide (UTMO) layers. Cobalt tetraphenylporphyrins (CoTPP) on oxygen passivated Fe(001), with 1 ML O coverage, have revealed a molecule/substrate decoupling effect due to the formation of an ultra‐thin Fe oxide layer at the interface. However, the threshold concentration of surface O required to observe the decoupling effect has not been assessed yet. In this work, the possibility of stabilizing different ultra‐thin Pd oxide superstructures, characterized by a different number of O atoms per unit cell, is exploited to investigate the O decoupling effect on CoTPP films. Two Pd oxide superstructures are considered: Pd(001)‐p(2 × 2)O and Pd(001)‐p(√5 × √5)R27°O, with 0.25 and 0.80 ML O coverages, respectively, which are characterized by low‐energy electron diffraction (LEED), X‐ray and ultra‐violet photoelectron spectroscopies (XPS/UPS) and inverse photoemission spectroscopy (IPES). The results suggest a lower limit of 0.80 ML O coverage as a passivation interlayer to obtain an ordered and decoupled CoTPP monolayer on Pd(001).
Silica‐Rich Sol‐Gel Ink for Two‐Photon Direct Laser Writing of Microscale Structures and Optical Elements
Authors: Bin Nun Moran , Gvishi Raz , Dana Yoav , Garcia Yehudit , Marom Dan M. , Atar Nurit , Porat Omer , Bar Galit 
Published: August 2024

AbstractInnovative materials enable two‐photon polymerization for precise additive fabrication of intricate optical components. Existing polymeric inks suffer from poor optical performance due to their high organic content. Silica‐rich sol‐gel ink (75 wt%, under ambient conditions) is presented for high‐precision three‐dimensional (3D) printing of microscale structures and optical devices. A photoinitiator with high‐efficiency nonlinear absorption is introduced to initiate two‐photon polymerization. Utilizing a commercial direct laser writing system, 3D‐printing is demonstrated including the optimization of printing parameters and ink characterization. The optical performance of the printed microscale elements using the new sol‐gel ink surpasses commercially available polymeric inks on key metrics: Printed elements exhibit extremely low surface roughness, 3nm; visible and near‐IR light transmission is greater than 90%; Printed elements present enhanced mechanical and chemical resistance to common organic solvents; Structures exhibit low isotropic shrinkage, <10%; Elements withstand continuous‐wave laser intensities exceeding 7 × 105 W cm−2. Direct writing onto an optical fiber tip with no need for surface functionalization is presented, with the demonstration of a tall waveguide taper (≈1:5 aspect ratio) with low losses and modal crosstalk, and a freestanding photonic lantern mode multiplexer. The new ink can be utilized in a variety of applications and across many materials, requiring compact, durable, and complex optical elements.
Photocatalyst‐Free Wavelength‐Dependant Sequential Ring Transformations of Pyrazolo[1,2‐a]pyrazolones
Authors: Kulašić Ines , Petek Nejc , Brodnik Helena , Grošelj Uroš , Svete Jurij , Štefane Bogdan 
Published: August 2024

AbstractWe report sequential wavelength‐selective photochemical transformations of 1‐alkenylpyrazolo[1,2‐a]pyrazolones to pyrazolo[1,2‐a][1,2]diazepines or cyclobuta[c]pyrazolo[1,2‐a]pyrazolones. Irradiation of 1‐alkenylpyrazolo[1,2‐a]pyrazolones with visible‐light (blue LED, 457 nm) induced selective ‘ring switching’ transformation into pyrazolo[1,2‐a][1,2]diazepines, which underwent electrocyclisation yielding cyclobuta[c]pyrazolo[1,2‐a]pyrazolones upon irradiation with UV−A light (black LED, 365 nm). Due to the very narrow irradiation wavelength now available from OLED sources, the selective formation of either 5,7‐bicyclic or 5,5,4‐tricyclic ring systems from the 5,5‐bicyclic starting material is possible by changing the wavelength of the irradiation source. The transformations took place under mild conditions in the absence of additives or photocatalysts. Mechanistic studies indicate that these transformations proceed through the formation of an excited triplet state of the substrate, followed by selective homolytic C(1)−N(8) bond cleavage, intersystem crossing, and cyclization of the zwitterionic intermediate on the ground potential energy surface. The subsequent photoinduced disrotatory stereospecific 4π‐electrocyclization of the 5,7‐bicyclic systems leads to 3D‐rich 5,5,4‐tricyclic products.
Visible‐Light‐Initiated Uranyl‐Catalyzed Hydrosilylation and Hydrosulfonylation of Alkenes and Alkynes
Authors: Gong Xingxing , Zhao Qianyi , Zhu Congqing 
Published: August 2024

AbstractThis study investigates the visible‐light‐initiated uranyl(VI)‐catalyzed activation of Si−H bonds through direct hydrogen atom transfer, which facilitates the formation of silyl radicals from silanes. The silyl radical can abstract a chlorine atom from the sulfonyl chloride, leading to the generation of sulfonyl radicals. These silyl radicals and sulfonyl radicals could react with alkenes and alkynes, achieving the first example of uranyl‐catalyzed hydrosilylation and hydrosulfonylation of unsaturated C−C bonds. This method features mild reaction conditions and a broad substrate scope, and exhibits exceptional functional‐group tolerance. Consequently, it is suitable for the late‐stage functionalization of drug derivatives.
Visible Light‐Induced Cyanomethyl Radical Triggered Cascade Cyclization of Phenyl‐Linked 1,6‐Enynes with a‐Halogenated Acetonitriles
Authors: Hu Xiao , Chen Bo‐Xin , Bo Xiang‐Lin , Zhang Qing‐Fang , Hu Lin‐Ping , Teng Ming‐Yu , Huang Guo‐Li , Liu Bo 
Published: August 2024

AbstractPhoto‐promoted cyanomethyl radical procedures for the preparation of 2,3‐dihydro‐1H‐indenes and 2,8‐dihydrocyclopenta[a]indenes from phenyl‐linked 1,6‐enynes with α‐halogenated acetonitriles are reported. The iodocyanomethylation/cyclization is performed via an atom‐transfer radical addition (ATRA) strategy under photocatalyst‐ and oxidant‐free conditions. In particular, the photoinduced cyanomethylative cascade bicyclization is carried out under the fac‐Ir(ppy)3/Na2CO3 catalystic symtem and visible light irradiation. These methods offer a one‐step and atom‐economical access to diverse cyano‐group containing five‐membered rings with broad substrate scope and high selectivity. A plausible reaction mechanism is also proposed.
History Matching Reservoir Models With Many Objective Bayesian Optimization
Authors: Samoil Steven , Fare Clyde , Jordan Kirk E. , Chen Zhangxin 
Published: August 2024

ABSTRACTReservoir models for predicting subsurface fluid and rock behaviors can now include upwards of billions (and potentially trillions) of grid cells and are pushing the limits of computational resources. History matching, where models are updated to match existing historical data more closely, is conducted to reduce the number of simulation runs and is one of the primary time‐consuming tasks. As models get larger the number of parameters to match increases, and the number of objective functions increases, and traditional methods start to reach their limitations. To solve this, we propose the use of Bayesian optimization (BO) in a hybrid cloud framework. BO iteratively searches for an optimal solution in the simulations campaign through the refinement of a set of priors initialized with a set of simulation results. The current simulation platform implements grid management and a suite of linear solvers to perform the simulation on large scale distributed‐memory systems. Our early results using the hybrid cloud implementation shown here are encouraging on tasks requiring over 100 objective functions, and we propose integrating BO as a built‐in module to efficiently iterate to find an optimal history match of production data in a single package platform. This paper reports on the development of the hybrid cloud BO based history matching framework and the initial results of the application to reservoir history matching.
The role of hyperbranched polyesters in acrylamide‐based polymers as thickening agents in aqueous solutions
Authors: Meleán Brito Ramses S. , Padró Juan M. , Pinzón Barrantes John J. , Villa‐Pérez Cristian , Strumia Miriam C. , Milanesio Juan M. , Mattea Facundo 
Published: August 2024

AbstractAcrylamide polymers are typically used in industrial and healthcare sectors as thickening agents; however, their thickening capabilities rely mainly in their molecular mass. A versatile and simple strategy to improve their performance is the copolymerization with specific monomers or their chemical modification with structures like dendritic or hyperbranched molecules. This study introduces a novel acrylamide‐acrylic acid polymer grafted with minor proportions (≤4.0 wt%) of Boltorn H30, a hyperbranched polyester monomer. The incorporation of Boltorn H30 aims to exploit the hyperbranched architecture's impact on the viscosity and rheological behavior of polymer solutions. Polymers with 0.4 and 4.0 polyester wt% characterized by several analytical techniques displayed improved viscosity in aqueous solution compared against the parent poly(acrylamide‐co‐acrylic acid). Results revealed that while the molecular mass distribution changed between 20% and 94%, the thickening capabilities significantly improved with increments of 2.7 and 3.8 times compared to that of the original polymers. These findings demonstrate that even with a minimal incorporation of hyperbranched polyesters, the abundance of hydroxyl groups fosters extensive hydrogen bonding, resulting in enhanced viscosity properties of the polymer.
Mutual Amplification of GLI2/Hedgehog and Transcription Factor JUN/AP‐1 Signaling in Fibroblasts in Systemic Sclerosis: Potential Implications for Combined Therapies
Authors: Bergmann Christina , Chenguiti Fakhouri Sara , Trinh‐Minh Thuong , Filla Tim , Rius Rigau Aleix , Ekici Arif B. , Merlevede Benita , Hallenberger Ludwig , Zhu Honglin , Dees Clara , Matei Alexandru‐Emil , Auth Janina , Györfi Andrea‐Hermina , Zhou Xiang , Rauber Simon , Bozec Aline , Dickel Nicholas , Liang Chunguang , Kunz Meik , Schett Georg , Distler Jörg H.W. 
Published: August 2024

ObjectiveDeregulation of the cJUN/AP‐1 and hedgehog/GLI2 signaling pathways has been implicated in fibroblast activation in systemic sclerosis (SSc). However, the consequences of their concomitant up‐regulation are unknown. Here, we tested the hypothesis that mutual amplification of both pathways might drive persistent fibroblast activation.MethodsCultured fibroblasts and skin sections of patients with diffuse SSc and healthy volunteers were analyzed. cJUN/AP‐1 signaling and hedgehog/GLI2 signaling were inhibited using knockdown and pharmacologic approaches. Hedgehog signaling was activated in mice by fibroblast‐specific overexpression of constitutively active Smoothened.ResultscJUN and GLI2 are concomitantly up‐regulated and colocalize in fibroblasts of patients with SSc compared to healthy controls. Activation of hedgehog/GLI2 signaling induces the expression of cJUN in vitro and in vivo, whereas inactivation of GLI2 inhibits cJUN expression. Likewise, inactivation of cJUN impairs the expression of GLI2. This mutual regulation occurs at the level of transcription with binding of cJUN and GLI2 to specific binding motifs. Interference with this mutual amplification of cJUN signaling and GLI2 signaling inhibits fibroblast activation and collagen release: Inhibition of cJUN/AP‐1 signaling ameliorates hedgehog‐induced fibroblast activation and skin fibrosis in SmoACT mice with a reduction of skin thickness of 103% (P = 0.0043) in the treatment group compared to the fibrotic control group. Moreover, combined pharmacologic inhibition of cJUN/AP‐1 and hedgehog/GLI2 exerts additive antifibrotic effects in a model of TGFβ‐driven experimental fibrosis (TBRACT mice).ConclusionThe transcription factors cJUN and GLI2 reinforce each other's activity to promote fibroblast activation in SSc. Interruption of this crosstalk by combined inhibition of both pathways exerts additive antifibrotic effects at well‐tolerated doses.