bluuebunny/crossref_metadata_2025 huggingface dataset:
Giant Hall Switching by Surface‐State‐Mediated Spin‐Orbit Torque in a Hard Ferromagnetic Topological Insulator
Authors: Tai Lixuan , He Haoran , Chong Su Kong , Zhang Huairuo , Huang Hanshen , Qiu Gang , Ren Yuxing , Li Yaochen , Yang Hung‐Yu , Yang Ting‐Hsun , Dong Xiang , Dai Bingqian , Qu Tao , Shu Qingyuan , Pan Quanjun , Zhang Peng , Xue Fei , Li Jie , Davydov Albert V. , Wang Kang L.
Published: September 2024

Topological insulators (TI) and magnetic topological insulators (MTI) can apply highly efficient spin‐orbit torque (SOT) and manipulate the magnetization with their unique topological surface states (TSS) with ultrahigh efficiency. Here, efficient SOT switching of a hard MTI, V‐doped (Bi,Sb)2Te3 (VBST), with a large coercive field that can prevent the influence of an external magnetic field, is demonstrated. A giant switched anomalous Hall resistance of 9.2 kΩ is realized, among the largest of all SOT systems, which makes the Hall channel a good readout and eliminates the need to fabricate complicated magnetic tunnel junction (MTJ) structures. The SOT switching current density can be reduced to 2.8 × 105 A cm−2, indicating its high efficiency. Moreover, as the Fermi level is moved away from the Dirac point by both gate and composition tuning, VBST exhibits a transition from edge‐state‐mediated to surface‐state‐mediated transport, thus enhancing the SOT effective field to (1.56 ± 0.12) × 10−6 T A−1 cm2 and the interfacial charge‐to‐spin conversion efficiency to 3.9 ± 0.3 nm−1. The findings establish VBST as an extraordinary candidate for energy‐efficient magnetic memory devices.
High‐Efficiency, Prevascularization‐Free Macroencapsulation System for Subcutaneous Transplantation of Pancreatic Islets for Enhanced Diabetes Treatment
Authors: Jeon Seunggyu , Heo Jun‐Ho , Myung Noehyun , Shin Ji Yeong , Kim Min Kyeong , Kang Hyun‐Wook
Published: September 2024

Pancreatic islet macroencapsulation systems for subcutaneous transplantation have garnered significant attention as a therapy for Type I diabetes due to their minimal invasiveness and low complication rates. However, the low vascular density of subcutaneous tissue threatens the long‐term survival of islets. To address this issue, prevascularized systems are introduced but various challenges remain, including system complexity and vascular‐cell immunogenicity. Here, a novel prevasculature‐free macroencapsulation system designed as a multilayer sheet, which ensures sufficient mass transport even in regions with sparse vasculature, is presented. Islets are localized in top/bottom micro‐shell layers (≈300 µm thick) to maximize proximity to the surrounding host vasculature. These sheets, fabricated via bioprinting using rat islets and alginate‐based bio‐ink, double islet viability and optimize islet density, improving insulin secretion function by 240%. The subcutaneous transplantation of small islet masses (≈250 islet equivalent) into diabetic nude mice enable rapid (<1 day) recovery of blood glucose, which remain stable for >120 days. Additionally, antifibrotic drug‐loaded multilayer sheets facilitate blood glucose regulation by rat islets at the subcutaneous sites of diabetic immunocompetent mice for >35 days. Thus, this macroencapsulation system can advance the treatment of Type I diabetes and is also effective for islet xenotransplantation in subcutaneous tissue.
Untethered & Stiffness‐Tunable Ferromagnetic Liquid Robots for Cleaning Thrombus in Complex Blood Vessels
Authors: Li Zhuofan , Zhang Shanfei , Wang Qi , Xu Yizhuo , Li Yike , Chen Xiaojun , Chen Peng , Chen Dezhi , Shi Yunsong , Su Bin
Published: September 2024

Thrombosis is a significant threat to human health. However, the existing clinical treatment methods have limitations. Magnetic soft matter is used in the biomedical field for years, and ferromagnetic liquids exhibit tunable stiffness and on‐demand movement advantages under magnetic fields. In this study, a ferromagnetic liquid robot (FMLR) is developed and applied it to thrombus removal in complex blood vessels. The FMLR consisted of Fe3O4 magnetic nanoparticles and dimethyl silicone oil. The FMLR can pass through a narrow complex maze through shape deformation by tailoring the intensity and direction of the external magnetic field. Finite element simulation analysis is used to validate the mechanism of controllable FMLR movements. Importantly, the storage modulus of FMLR can be tuned from 0.1 to 2018 Pa by varying the external magnetic intensity, ensuring its effectiveness in removing rigid and stubborn thrombi present on the vascular walls. Toward medical robotic applications, FMLR can be used in telerobotic neurointerventional. Experiments demonstrating the capability of FMLR to remove thrombi in the ear veins of rabbits are conducted. This study introduces an efficient approach for thrombus elimination, broadening the utilization of FMLRs within the realm of clinical medicine.
Constructing Organic Phosphorescent Scintillators with Enhanced Triplet Exciton Utilization Through Multi‐Mode Radioluminescence for Efficient X‐Ray Imaging
Authors: Li Huanhuan , Liu Yitong , Zhao Wei , Cao Hengyu , Yan Xin , Zhang Shuman , Yan Xi , Li Hui , Tao Ye , Xie Gaozhan , Li Wei , Chen Runfeng , Huang Wei
Published: September 2024

The development of organic phosphorescent scintillators with high exciton utilization efficiency has attracted significant attention but remains a difficult challenge because of the inherent spin‐forbidden feature of X‐ray‐induced triplet excitons. Herein, a design strategy is proposed to develop organic phosphorescent scintillators through thermally activated exciton release to convert stabilized spin‐forbidden triplet excitons to spin‐allowed singlet excitons, which enables singlet exciton‐dominated multi‐mode emission simultaneously from the lowest singlet, triplet, and stabilized triplet states. The resultant scintillators demonstrate a maximum photoluminescence efficiency of 65.8% and a minimum X‐ray radiation detection limit of 110 nGy s−1; this allows efficient radiography imaging with a spatial resolution of ≈10.0 lp mm−1. This study advances the fundamental understanding of exciton dynamics under X‐ray excitation, significantly broadening the practical use of phosphorescent materials for safety‐critical industries and medical diagnostics.
Confined Flash Printing and Synthesis of Stable Perovskite Nanofilms under Ambient Conditions
Authors: Liu Yuxin , Knaus Tanja , Wei Zheng , Zhang Junfang , Damian Matteo , Ronneberger Sebastian , Zhu Xingjun , Seeberger Peter H. , Zhang Hong , Mutti Francesco G. , Loeffler Felix F.
Published: September 2024

The fabrication of stable perovskite nanofilm patterns is important for the development of functional optical devices. However, current production approaches are limited by the requirement for strict inert gas protection and long processing times. Here, a confined flash printing synthesis method is presented to generate perovskite nanofilms under ambient conditions, combining precursor transfer, perovskite synthesis, crystallization, and polymer protection in a single step within milliseconds. A laser simultaneously prints and induces the flash synthesis, confined in a polymer nanofilm, under normal ambient conditions. Due to its simplicity and flexibility, the method enables the combination and screening of many different perovskite precursor materials on various substrates. Besides for the development of novel perovskite materials and devices, the nanofilms can be applied for biodetection. The unique H2O2‐responsive property of the ultrathin perovskite quantum dot film is applied for biomolecule detection based on oxidase‐catalyzed enzymatic reactions.
Nanosonosensitizer Optimization for Enhanced Sonodynamic Disease Treatment
Authors: Zhang Min , Sun Dandan , Huang Hui , Yang Dayan , Song Xinran , Feng Wei , Jing Xiangxiang , Chen Yu
Published: September 2024

Low‐intensity ultrasound‐mediated sonodynamic therapy (SDT), which, by design, integrates sonosensitizers and molecular oxygen to generate therapeutic substances (e.g., toxic hydroxyl radicals, superoxide anions, or singlet oxygen) at disease sites, has shown enormous potential for the effective treatment of a variety of diseases. Nanoscale sonosensitizers play a crucial role in the SDT process because their structural, compositional, physicochemical, and biological characteristics are key determinants of therapeutic efficacy. In particular, advances in materials science and nanotechnology have invigorated a series of optimization strategies for augmenting the therapeutic efficacy of nanosonosensitizers. This comprehensive review systematically summarizes, discusses, and highlights state‐of‐the‐art studies on the current achievements of nanosonosensitizer optimization in enhanced sonodynamic disease treatment, with an emphasis on the general design principles of nanosonosensitizers and their optimization strategies, mainly including organic and inorganic nanosonosensitizers. Additionally, recent advancements in optimized nanosonosensitizers for therapeutic applications aimed at treating various diseases, such as cancer, bacterial infections, atherosclerosis, and autoimmune diseases, are clarified in detail. Furthermore, the biological effects of the improved nanosonosensitizers for versatile SDT applications are thoroughly discussed. The review concludes by highlighting the current challenges and future opportunities in this rapidly evolving research field to expedite its practical clinical translation and application.
Broadband Spin and Orbital Momentum Modulator Using Self‐Assembled Nanostructures
Authors: Liu Yuanfeng , Zhou Le , Guo Mengfan , Xu Zongqi , Ma Jing , Wen Yongzheng , Litchinitser Natalia M. , Shen Yang , Sun Jingbo , Zhou Ji
Published: September 2024

The structural symmetry of solids plays an important role in defining their linear and nonlinear optical properties. The quest for versatile, cost‐effective, large‐scale, and defect‐free approaches and materials platforms for tailoring structural and optical properties on demand is underway since decades. A self‐assembled spherulite material comprised of synthesized molecules with large dipole moments aligned azimuthally, forming a vortex polarity with spontaneously broken symmetry, is experimentally demonstrated. This unique self‐assembled structure enables new linear and nonlinear light–matter interactions, including generating optical vortex beams with complex spin states and on‐demand topological charges at the fundamental, doubled, and tripled frequencies. This work will likely enable numerous applications in areas such as high‐dimensional quantum information processing with large capacity and high security, spatiotemporal optical vortices, and a novel optical manipulation and trapping platform.
Reversing Immune Checkpoint Inhibitor–Associated Cardiotoxicity via Bioorthogonal Metabolic Engineering–Driven Extracellular Vesicle Redirecting
Authors: Fan Miao , Zhang Xing , Liu Huifang , Li Lanya , Wang Fei , Luo Li , Zhou Xiaohan , Liang Xing‐Jie , Zhang Jinchao , Li Zhenhua
Published: September 2024

The cardiotoxicity induced by immune checkpoint inhibitors (ICIs) is associated with high mortality rates. T cells play an important role in ICI‐induced cardiac injury. The inhibition of local T‐cell activity is considered an effective strategy for alleviating ICI‐related cardiotoxicity. Tumor‐derived extracellular vesicles (EVs) contribute to immunosuppression via PD‐L1 overexpression. In this study, a bioorthogonal metabolic engineering–driven EV redirecting (Biomeder) strategy for in situ engineered EVs with myocardial‐targeting peptides is developed. Accumulated tumor‐derived EV (TuEVs) reverses the immune environment in the heart by increasing PD‐L1 levels in cardiomyocytes and/or by directly inhibiting T‐cell activity. More importantly, it is found that the redirection of TuEVs further disrupts immunosuppression in tumors, which facilitates anti‐tumor activity. Thus, redirecting TuEVs to the heart simultaneously enhances the antitumor efficacy and safety of ICI‐based therapy. Furthermore, the Biomeder strategy is successfully expanded to prevent ICI‐induced type 1 diabetes. This Biomeder technique is a universal method for the treatment of various ICI‐related adverse events.
Design Metrics for Highly Reflective Fibrous Insulation
Authors: Koutsakis Georgios , Deliwala Nikhil , Clarke David R.
Published: September 2024

The high melting temperatures, large optical bandgaps, and large refractive indices of oxides favor their use as fibrous insulation at extreme temperatures where radiative heat transfer is significant. In this work, the reflectance of mats of fibers is modeled with the Monte Carlo (MC) method using the fiber optical properties (such as the scattering efficiency and scattering coefficient), the fiber radius, refractive index, volume fraction (fv), as well as the thickness of insulation (L). Two key metrics are identified for the design of highly reflective insulation. One is a novel metric, the Kuhn scattering length, which is based on an analogy between the anisotropic random walks in MC radiative transfer and polymer physics. It is used to determine approximate the effective thickness of insulation (fvL). The second is a size metric, which indicates that fiber mats are most reflective when the fiber radius is . The model is validated on experimental measurements of commercially available insulation consisting of fibers with 3–5 µm radius.
Apple Tree Root‐Derived Biochar/Iron Oxide Triphasic Nanocomposite for Wastewater Treatment and Microwave Absorption
Authors: Mahmoodi Mahsa , Aslibeiki Bagher , Ghosh Sagnik , Hasani Leila , Slimani Sawssen , Vattuone Luca , Peddis Davide , Sarkar Tapati
Published: September 2024

In this work, two major sources of pollution: (1) Water pollution due to heavy metals, and (2) Electromagnetic wave (EMW) pollution, often regarded as the fourth category of pollution (after air, water, and soil pollution) are addressed. A unique bio‐based triphasic nanocomposite (Fe3O4/α‐Fe2O3/carbon) is synthesized and its superior properties are demonstrated to address both types of environmental pollution. The nanocomposite, derived from lightweight apple tree roots, is used for Pb (II) ion removal from aqueous solutions via adsorption and magnetic separation. The biomass‐derived highly porous biochar decorated with iron‐oxide showed adsorption efficiency of nearly 100% and corresponding capacity of 149 mg.g−1 under optimal conditions for initial Pb (II) concentration of 50 mg.L−1. Furthermore, a remarkable adsorption capacity of 731 mg.g−1 is achieved using lower amount of the adsorbent for a slightly lower efficiency (97%). In addition, the mesoporous composite showed excellent EMW absorption efficiency with effective absorption bandwidth of 7.8 GHz and reflection loss of −61.7 dB, arising from very good impedance matching, and high dielectric and magnetic losses. This work establishes the multifunctional properties of the synthesized composite, and addresses the UN Sustainable Development Goal (SDG) 6 (Clean water and sanitation) and SDG 13 (Climate action, including pollution management).
Design of Carboxylic Acid‐Functionalized Poly(Butylene Adipate‐co‐Terephthalate) for Recyclable and Biodegradable Zero‐Waste Paper Packaging
Authors: Elkholy Hazem M. , Hamdani Syeda Shamila , Alghaysh Manal O. , Wyman Ian , Duncan Emily , Wang Yun , Li Kecheng , Rabnawaz Muhammad
Published: September 2024

Demand for water‐ and oil‐repellent‐coated paper as an alternative to plastics is growing, but the challenge is that coated paper lacks concurrent recyclability and biodegradability. Reported herein is a novel carboxylic acid‐functionalized poly(butylene adipate‐co‐terephthalate) (CPBAT) copolymer investigated for recyclable and repulpable water‐borne paper coatings. The CPBAT synthesized here is characterized by spectroscopic methods. Paper coated with waterborne CPBAT exhibited excellent water, oil, moisture, and gas barrier properties suitable for packaging applications. The recyclability and repulpability of the CPBAT‐coated paper are successfully validated via certified TAPPI methods. This work demonstrates the first successful preparation of coated paper that is per‐ and polyfluoroalkyl substances (PFAS)‐free, recyclable, and biodegradable, with significant benefits for the environment and human health.
3D‐Printed Breast Prosthesis that Smartly Senses and Targets Breast Cancer Relapse
Authors: Wang Lu , Ye Chenyang , Xue Xiangjie , Xie Mingjun , Zhi Yicheng , Feng Xiao , Zhao Pengcheng , Zhou Jichun , Mi Mi , Li Jinrui , Gu Qinhao , Zhao Ye , Chen Jiaxin , Zhou Yi , Xue Yanan , Fu Zexin , Zhou Liuyi , Chen Lulu , Pan Lei , Sun Yi , Wang Linbo , Wu Sufan , He Yong , Wang Ji
Published: September 2024

Breast reconstruction is essential for improving the appearance of patients after cancer surgery. Traditional breast prostheses are not appropriate for those undergoing partial resections and cannot detect and treat locoregional recurrence. Personalized shape prostheses that can smartly sense tumor relapse and deliver therapeutics are needed. A 3D‐printed prosthesis that contains a therapeutic hydrogel is developed. The hydrogel, which is fabricated by crosslinking the polyvinyl alcohol with N1‐(4‐boronobenzyl)‐N3‐(4‐boronophenyl)‐N1, N1, N3, N3‐tetramethylpropane‐1,3‐diaminium, is responsive to reactive oxygen species (ROS) in the tumor microenvironment. Specifically, RSL3, a ferroptosis inducer that is loaded in hydrogels, can trigger tumor ferroptosis. Intriguingly, RSL3 encapsulated in the ROS‐responsive hydrogel exerts antitumor effects by increasing the numbers of tumor‐infiltrated CD4+ T cells, CD8+ T cells, and M1 macrophages while reducing the number of M2 macrophages. Therefore, this new prosthesis not only allows personalized shape reconstruction, but also detects and inhibits tumor recurrence. This combination of aesthetic appearance and therapeutic function can be very beneficial for breast cancer patients undergoing surgery.
Novel Insights into Enzymatic Thermostability: The “Short Board” Theory and Zero‐Shot Hamiltonian Model
Authors: Liao Min , Feng Shihao , Liu Xiaoqing , Xu Guoshun , Li Sicong , Bai Yingguo , Luo Huiying , Yao Bin , Wang Haobo , Tu Tao
Published: September 2024

Understanding the mechanism underlying thermostabilization in naturally stable enzymes and enhancing the thermostability of unstable enzymes are crucial aspects in enzyme engineering. Despite the development of various engineering methods, there remains substantial scope for improvement. In this study, a novel concept termed as the “short board” theory is proposed, which conceptualizes proteins as barrels with each component representing a jagged board. Notably, optimizing modifications to the shortest board yields optimal enhancements in terms of thermostability performance. To validate this theory, α‐amylase, an industrial bulk enzyme with multiple domains, is employed as a model enzyme. The existence of “short boards” and their impact on thermostability modification are demonstrated at the domain, residue, and atomic levels through experimental confirmation using domain substitution. Furthermore, a novel thermostable design and prediction model called Zero‐Shot Hamiltonian (ZSH) is established and evaluated on α‐amylase. This coevolutionary approach based on thermostability and deep learning exhibits remarkable success exclusively when applied to enzymes with fixed short boards. The integration of the “short board” theory with the ZSH model presents an innovative tool for enhancing enzymatic thermostability.
Anomalous Polarons in Two‐Dimensional Organometallic Perovskite Ferroelectric
Authors: Yu Junhong , Han Yadong , Yang Yunfan , Zhang Hang , Liu Yi , Xu Jinlong , Sun Zhihua , Hu Jianbo
Published: September 2024

The concept of ferroelectric polarons is proposed to partially explain the exceptional optoelectronic properties observed in lead halide perovskites (LHPs). It is intriguing but unclear how this proposal, which involves local or transient polarizations, applies in general to 2D LHPs with long‐range ferroelectricity. Here, this work presents a pioneering time‐domain experimental investigation of polarons in ferroelectric (IA)2(MA)2Pb3Br10 (IMPB; IA is isoamylammonium and MA is methylammonium) using transient absorption spectroscopy. Compared to non‐ferroelectric LHPs, IMPB exhibits several distinct polaronic properties closely associated with macroscopic polarizations of ferroelectricity, including a prolonged polaron formation time (≈1.1 ps), a Stark splitting of the bleaching (≈63 meV), and a giant polaron Mott density (≈7.6 × 1018 cm−3). These findings broaden the realm of 2D polaron systems and reveal the decisive role of static/unidirectional polarizations on polaron physics in 2D LHPs.
Bifidobacterium pseudolongum‐Derived Bile Acid from Dietary Carvacrol and Thymol Supplementation Attenuates Colitis via cGMP‐PKG‐mTORC1 Pathway
Authors: Zhang Ke , Xu Yangbin , Zheng Yining , Zhang Ting , Wu Yujiang , Yan Yiting , Lei Yu , Cao Xi , Wang Xiaolong , Yan Frances , Lei Zhaomin , Brugger Daniel , Chen Yulin , Deng Lu , Yang Yuxin
Published: September 2024

Carvacrol and thymol (CAT) have been widely recognized for their antimicrobial and anti‐inflammatory properties, yet their specific effects on colitis and the mechanisms involved remain insufficiently understood. This study establishes a causative link between CAT administration and colitis mitigation, primarily through the enhancement of Bifidobacterium pseudolongum abundance in the colon. This increase promotes the production of secondary bile acids, particularly hyodeoxycholic acid (HDCA) and 12‐ketodeoxycholic acid (12‐KCAC), which exert anti‐inflammatory effects. Notably, CAT does not alleviate colitis symptoms in germ‐free mice, indicating the necessity of gut microbiota. This research uncovers a novel regulatory mechanism where HDCA and 12‐KCAC inhibit colonic inflammation by reducing the expression of transmembrane guanylate cyclase 1A in the colonic epithelium. This downregulation elevates intracellular Ca2+ and cGMP levels, activating protein kinase G (PKG). Activated PKG subsequently suppresses the mTOR signaling pathway, thereby ameliorating dextran sulfate sodium (DSS)‐induced colonic damage. These findings highlight potential metabolites and therapeutic targets for preventing and treating colitis. Bifidobacterium pseudolongum, HDCA, and 12‐KCAC emerge as promising candidates for therapeutic interventions in colitis and related disorders characterized by impaired tight junction function.
Operando Decoding Ion‐Conductive Switch in Stimuli‐Responsive Hydrogel by Nanodiamond‐Based Quantum Sensing
Authors: Dou Ruqiang , Li Zan , Zhu Guoli , Lin Chao , Liu Frank X. , Wang Biao
Published: September 2024

Thermal‐responsive hydrogels are developed as ion‐conductive switchs for energy storage devices, however, the molecule mechanism of switch on/off remains unclear. Here, poly(N‐isopropylacrylamide‐co‐acrylamide) hydrogel is synthesized as a model material and nanodiamond (ND) based quantum sensing for phase change study is developed. First, micro‐scale phase separation with cross‐linked mesh structure after sol‐gel transition is visualized in situ and water molecules are trapped by polymer chains and on a chemically “frozen” state. Then, the nano‐scale inhomogeneous distributions of viscosity, thermal conductivity and ionic mobility in hydrogel at high temperature are observed by measuring the rotation, translation and zero‐field splitting of NDs. Besides, the ionic mobility of hydrogel is found to be dependent not only on temperature but also on polymer concentration. These observations suggested that the physical “wall” induced by inhomogeneous phase separation at microscopic scale blocked the ion conduction pathways, providing a potential intrinsic explanation for ion migration shut‐down of ionic hydrogels at high temperature.
Advances and Applications of Oxidized van der Waals Transition Metal Dichalcogenides
Authors: Kim Brian S. Y. , Ngo Tien Dat , Hassan Yasir , Chae Sang Hoon , Yoon Soon‐Gil , Choi Min Sup
Published: September 2024

The surface oxidation of 2D transition metal dichalcogenides (TMDs) has recently gained tremendous technological and fundamental interest owing to the multi‐functional properties that the surface oxidized layer opens up. In particular, when integrated into other 2D materials in the form of van der Waals heterostructures, oxidized TMDs enable designer properties, including novel electronic states, engineered light‐matter interactions, and exceptional‐point singularities, among many others. Here, the evolving landscapes of the state‐of‐the‐art surface engineering technologies that enable controlled oxidation of TMDs down to the monolayer‐by‐monolayer limit are reviewed. Next, the use of oxidized TMDs in van der Waals heterostructures for different electronic and photonic device platforms, materials growth processes, engineering concepts, and synthesizing new condensed matter phenomena is discussed. Finally, challenges and outlook for future impact of oxidized TMDs in driving rapid advancements across various application fronts is discussed.
Thermosensitive Hydrogel with Programmable, Self‐Regulated HIF‐1α Stabilizer Release for Myocardial Infarction Treatment
Authors: Deng Kaicheng , Hua Yuyan , Gao Ying , Zheng Houwei , Jiang Yangzi , Wang Yaping , Gao Changyou , Ren Tanchen , Zhu Yang
Published: September 2024

HIF‐1α (hypoxia induced factor‐1α), a vital protective signal against hypoxia, has a short lifetime after myocardial infarction (MI). Increasing HIF‐1α stability by inhibiting its hydroxylation with prolyl hydroxylases inhibitors such as DPCA (1,4‐dihydrophenonthrolin‐4‐one‐3‐carboxylic acid) presents positive results. However, the optimal inhibitor administration profile for MI treatment is still unexplored. Here, injectable, thermosensitive hydrogels with programmable DPCA release are designed and synthesized. Hydrogel degradation and slow DPCA release are coupled to form a feedback loop by attaching pendant DPCA to polymer backbone, which serve as additional crosslinking points through π–π and hydrophobic interactions. Pendant carboxyl groups are added to the copolymer to accelerate DPCA release. Burst release in the acute phase for myocardial protection and extended near zero‐order release across the inflammatory and fibrotic phases with different rates are achieved. All DPCA‐releasing hydrogels upregulate HIF‐1α, decrease apoptosis, promote angiogenesis, and stimulate cardiomyocyte proliferation, leading to preserved cardiac function and ventricular geometry. Faster hydrogel degradation induced by faster DPCA release results in a HIF‐1α expression eight times of healthy control and better therapeutic effect in MI treatment. This research demonstrates the value of precise regulation of HIF‐1α expression in treating MI and other relevant diseases and provides an implantable device‐based modulation strategy.
Scaling Behavior in the Spectral and Power Density Dependent Photovoltaic Response of Hot Polaronic Heterojunctions
Authors: Kressdorf Birte , Hoffmann Jörg , Dehning Annika , Blöchl Peter E. , Seibt Michael , Jooss Christian
Published: September 2024

Strongly correlated manganites can be considered as model systems for the study of photovoltaic harvesting of hot polarons that can be excited from the electronically ordered ground state. In order to gain basic understanding of hot polaron harvesting, the deviations of the photovoltaic response of a heterojunction with polaronic absorber from a conventional semiconductor are analyzed. Specifically, the spectral and photon power density dependence of the open circuit voltage Uoc and the short circuit current density Jsc in heterojunctions consisting of orbital ordered Pr1‐xCaxMnO3 (x = 0.1, PCMO) thin films epitaxially grown on single crystalline (100) SrTiO3 (STO) and Nb‐doped (100) SrTiO3 (STNO) substrates are investigated. The observed behavior is fundamentally different from conventional solar cells, in which Uoc is limited by fast carrier relaxation to the band edges. Whereas the spectral and photon power dependence of Uoc of conventional semiconductor junctions is well described by the Shockley‐Queisser (SQ) theory, the hot polaron junctions surprisingly show a scaling law behavior of Uoc. Such scaling laws otherwise apply to equilibrium order parameters in second‐order phase transitions. It is concluded that its physical origin is the unique dependence of the quasi‐Fermi level splitting on temperature, photon energy, and power density in a hot polaron system.
Intensity‐Modulated Photocurrent and Photovoltage Spectroscopy for Characterizing Charge Dynamics in Solar Cells
Authors: Wang Yanlong , Zheng Haofeng , Xiao Jin , Liu Yanan , Liu Qi , Ma Xuyu , Hu Jing , Zou Dechun , Hou Shaocong
Published: September 2024

Intensity‐modulated photocurrent and photovoltage spectroscopy (IMPS/IMVS) are powerful tools in optoelectronics such as photoelectrochemistry and photovoltaics, as they demonstrate distinct charge dynamic processes at different frequencies. Unlike the material characterization techniques, IMPS/IMVS offer an approach for investigating the dynamic behavior of charge carriers and ions from the device perspective. This review examines IMPS/IMVS from both theories and experiments to understand the intricate charge dynamics in solar cells with various materials and structures. To accommodate different types of cells, four primary theoretical models including the rate constant model, drift‐diffusion model, equivalent circuit model, and distribution of relaxation times, are evaluated in detail. In the future, the incorporation of IMPS/IMVS with other time‐domain and frequency‐domain methods, along with imaging techniques, can significantly facilitate the characterization of charge dynamics with enhanced convenience, spatial dimensions, and accuracy.
Anti‐Swelling Supramolecule‐Crosslinked Hydrogel Interphase for Stable Zn Metal Anodes
Authors: Luo Xuan , Nian Qingshun , Dong Qi , Ruan Digen , Cui Zhuangzhuang , Wang Zihong , Xiong Bing‐Qing , Ren Xiaodi
Published: September 2024

Aqueous Zn metal batteries show promise for large‐scale energy storage but face challenges including dendrite formation, volume changes, and side reactions. This study introduces a novel anti‐swelling supramolecule‐crosslinked hydrogel (SCH) interphase to stabilize Zn metal anodes. The SCH, composed of cyclodextrin molecules crosslinked with polyvinyl alcohol, offers a multifaceted approach to enhance anode stability. It homogenizes ion flux and suppresses Zn dendrite growth by creating well‐defined pathways for Zn2+ movement. The supramolecular structure selectively traps SO42− ions, effectively desolvating Zn2+ and enabling fast ion transportation. Additionally, by disrupting water cluster hydrogen bonds, SCH reduces free water activity, mitigating corrosion at the Zn surface. Electrochemical tests demonstrate the excellent performance of SCH‐Zn, with symmetric cells achieve lifespans of 1800 h at 4 mA cm−2/2 mAh cm−2 and 1100 h at 10 mA cm−2/5 mAh cm−2. Zn||Cu half‐cells maintain 99.7% Coulombic efficiency over 500 cycles, while full cells with polyaniline cathodes exhibit stable cycling for 1500 cycles at 5 A g−1 with no apparent capacity decay. These results highlight the effectiveness of the SCH in stabilizing Zn anodes. This study provides a new interfacial engineering strategy for high‐performance aqueous Zn batteries, potentially accelerating their practical implementation in large‐scale energy storage.
Room‐Temperature Single‐Molecule Infrared Imaging and Spectroscopy through Bond‐Selective Fluorescence
Authors: Wang Haomin , Kocheril Philip A. , Yang Ziguang , Lee Dongkwan , Naji Noor , Du Jiajun , Lin Li‐En , Wei Lu
Published: September 2024

Infrared (IR) spectroscopy stands as a workhorse for exploring bond vibrations, offering a wealth of chemical insights across diverse frontiers. With increasing focus on the regime of single molecules, obtaining IR‐sensitive information from individual molecules at room temperature would provide essential information about unknown molecular properties. Here, we leverage bond‐selective fluorescence microscopy, facilitated by narrowband picosecond mid‐IR and near‐IR double‐resonance excitation, for high‐throughput mid‐IR structural probing of single molecules. We robustly capture single‐molecule images and analyze the combined polarization dependence, vibrational peaks, linewidths, and lifetimes of probe molecules with representative scaffolds. From bulk to single molecules, we find that vibrational lifetimes remain consistent, while linewidths are narrowed by approximately twofold and anisotropy becomes more pronounced. Additionally, unexpected peak shifts from single molecules were observed, attributed to the generation of new modes due to previously unexplored dimerization, supported by quantum chemistry calculations. These findings underscore the importance of infrared analysis on individual single molecules in ambient environments, offering molecular information crucial for functional imaging and the investigation of the fundamental properties and utilities of luminescent molecules.
Small‐Molecule Mixed Ionic‐Electronic Conductors for Efficient N‐Type Electrochemical Transistors: Structure‐Function Correlations
Authors: Cho Yongjoon , Gao Lin , Yao Yao , Kim Jaehyun , Zhang Dayong , Forti Giacomo , Duplessis Isaiah , Wang Yuyang , Pankow Robert M. , Ji Xudong , Rivnay Jonathan , Marks Tobin J. , Facchetti Antonio
Published: September 2024

The fundamental challenge in electron‐transporting organic mixed ionic‐electronic conductors (OMIECs) is simultaneous optimization of electron and ion transport. Beginning from Y6‐type/U‐shaped non‐fullerene solar cell acceptors, we systematically synthesize and characterize molecular structures that address the aforementioned challenge, progressively introducing increasing numbers of oligoethyleneglycol (OEG; g) sidechains from 1 g to 3 g, affording OMIECs 1gY, 2gY, and 3gY, respectively. The crystal structure of 1gY preserves key structural features of the Yn series: a U‐shaped/planar core, close π–π molecular stacking, and interlocked acceptor groups. Versus inactive Y6 and Y11, all of the new glycolated compounds exhibit mixed ion‐electron transport in both conventional organic electrochemical transistor (cOECT) and vertical OECT (vOECT) architectures. Notably, 3gY with the highest OEG density achieves a high transconductance of 16.5 mS, an on/off current ratio of ~106, and a turn‐on/off response time of 94.7/5.7 ms in vOECTs. Systematic optoelectronic, electrochemical, architectural, and crystallographic analysis explains the superior 3gY‐based OECT performance in terms of denser ngY OEG content, increased crystallite dimensions with decreased long‐range crystalline order, and enhanced film hydrophilicity which facilitates ion transport and efficient redox processes. Finally, we demonstrate an efficient small‐molecule‐based complementary inverter using 3gY vOECTs, showcasing the bioelectronic applicability of these new small‐molecule OMIECs.
Tailoring the Properties of Chemically Recyclable Polyethylene‐Like Multiblock Polymers by Modulating the Branch Structure
Authors: Zhao Yucheng , Rettner Emma M. , Battson Megan E. , Hu Zhitao , Miscall Joel , Rorrer Nicholas A. , Miyake Garret M.
Published: September 2024

Developing plastics that fill the need of polyolefins yet are more easily recyclable is a critical need to address the plastic waste crisis. However, most efforts in this vein have focused on high‐density polyethylene (PE), while many different types of PE exist. To create broadly sustainable PE with modular properties, we present the synthesis, characterization, and demonstration of materials applications for chemically recyclable PE‐like multiblock polymers prepared from distinct hard and soft blocks using ruthenium‐catalyzed dehydrogenative polymerization. By altering the branching pattern within the soft blocks, a series of PE‐like multiblock polymers were synthesized with tunable glass transition temperatures (Tg) while maintaining consistent high melting temperatures (Tm). A clear U‐shape trend between Tg and mechanical properties was found, showcasing their potential as sustainable materials with tailored properties spanning commercial linear low‐density polyethylene (LLDPE) and low‐density polyethylene (LDPE). These materials offer adjustable adhesive strength to metal and demonstrate chemical recyclability and selective depolymerization in mixed plastic streams, promoting circularity and separation.
Constructing Unsaturated Ru Atom Arrays Confined in Mn Oxides to Boost Neutral Water Reduction
Authors: Hu Qi , Cao Jianyong , Qi Shuai , Meng Na , Zhao Jingwen , Huang Tianchi , You Jiao , Liang Taiyu , Shang Chunyan , Yu Jiaying , Yang Hengpan , He Chuanxin
Published: September 2024

Recently, Ru single atoms supported on carbon nanomaterials have demonstrated ultrahigh activity for acid hydrogen evolution reaction (HER), however their neutral HER activity remains low due to the sluggish kinetics for both the water dissociation step to generate H* intermediates and subsequent H* recombination in neutral electrolytes. Here, we synthesize ordered low‐coordinated Ru atom arrays confined in Mn oxides (i.e., Li4Mn5O12) for concurrently boosting the water dissociation and H* recombination, thus achieving a 6‐fold HER activity enhancement than commercial Pt/C in neutral media. Control experiments indicate that low‐coordinated Ru atoms with strong affinity to oxygen atoms of water molecules facilitate the water dissociation to rapidly generate H*. More importantly, both electrochemical and theoretic results uncover that the array‐like structure allows the activation of two water molecules on two adjacent Ru atoms for enabling direct H*−H* recombination via the Tafel step, while isolated Ru atoms can only activate water one by one for recombining H* via the sluggish Heyrovsky step. Clearly, this work paves new avenues to boosting the electrocatalytic activity by constructing ordered metal atoms assembles with controllable coordination environments.
Controlling the Redox Chemistry of Cobalt Radiopharmaceuticals
Authors: Lin Wilson , Śmiłowicz Dariusz , Joaqui‐Joaqui M. Andrey , Bera Abhijit , Zhong Zhuoran , Aluicio‐Sarduy Eduardo , Mixdorf Jason C. , Barnhart Todd E. , Engle Jonathan W. , Boros Eszter
Published: September 2024

The elementally matched 55Co2+/3+ (t1/2=17.53 h, Iβ+=77 %)/58mCo2+/3+ (t1/2=9.10 h, internal conversion=100 %) radioisotope pair is of interest for development of paired diagnostic/therapeutic radiopharmaceuticals. Due to the accessibility of the nat/55Co2+/3+ redox couple, the redox state can be readily modulated. Here, we show that macroscopic and radiochemical redox reactions can be closely monitored and controlled using spectroscopic and radiochemical methods. We employ model systems to inform how to selectively synthesize thermodynamically favored oxidation state coordination complexes. In addition to exogenous oxidants, our data indicates that 55Co‐induced radiolysis of water efficiently and directly drives selective oxidation to the 55Co3+ species under no‐carrier added (n.c.a.) conditions. Our synthetic strategies subsequently stabilize the respective 55Co2+ or 55Co3+ species for targeted positron emission tomography imaging in a mouse tumor model.
Intermolecular 1,2‐Aminoboration of Alkynes and the Critical Role of Electron‐Rich Alkynes
Authors: Dotzauer Simon , Jayaraman Arumugam , Reinhart David , Braunschweig Holger
Published: September 2024

The intramolecular 1,2‐aminoboration of alkynes by aminoboranes is rare and invariably requires a catalyst to proceed, while the intermolecular aminoboration of alkynes is yet entirely unknown. Through an exploration of the significance of electronics in alkynes for activating the B−N σ‐bond of aminoboranes, we demonstrate in this work the first intermolecular 1,2‐aminoboration of alkynes. These reactions employ a series of (amino)dihaloboranes and aminoboronic esters, mild reaction conditions, and no catalysts, yielding syn‐addition alkene products with the incorporation of two crucial functionalities: amino and boryl. While highly electron‐rich examples can afford the aminoborated products (Z)‐2‐borylethenamines, other alkynes, including unactivated and less electron‐rich examples, do not lead to the corresponding aminoborated products due to the fundamental impediment that the reactions are significantly endergonic.
Pairing Oxygen Reduction and Water Oxidation for Dual‐Pathway H2O2 Production
Authors: Sun Xin , Yang Jindi , Zeng Xiangkang , Guo Lijun , Bie Chuanbiao , Wang Zhuyuan , Sun Kaige , Sahu Aloka Kumar , Tebyetekerwa Mike , Rufford Thomas E. , Zhang Xiwang
Published: September 2024

Hydrogen peroxide (H2O2) is a crucial chemical applied in various industry sectors. However, the current industrial anthraquinone process for H2O2 synthesis is carbon‐intensive. With sunlight and renewable electricity as energy inputs, photocatalysis and electrocatalysis have great potential for green H2O2 production from oxygen (O2) and water (H2O). Herein, we review the advances in pairing two‐electron O2 reduction and two‐electron H2O oxidation reactions for dual‐pathway H2O2 synthesis. The basic principles, paired redox reactions, and catalytic device configurations are introduced initially. Aligning with the energy input, the latest photocatalysts, electrocatalysts, and photo‐electrocatalysts for dual‐pathway H2O2 production are discussed afterward. Finally, we outlook the research opportunities in the future. This minireview aims to provide insights and guidelines for the broad community who are interested in catalyst design and innovative technology for on‐site H2O2 synthesis.
Enhanced chitosan and carboxymethylcellulose scaffolds with natural fiber reinforcement for hernia repair meshes
Authors: Rodríguez Guadalupe de Jesús , Patiño‐Herrera Rosalba , Zavala‐Alonso Verónica , Armendáriz‐Alonso Edgar F. , Cruz‐Guerrero Rosario , Pérez Elias
Published: September 2024

Chitosan (Chi) and carboxymethylcellulose (CMC) scaffolds, with and without reinforcement by Luffa cylindrica (Lc) or Asclepias curassavica (Ac), were synthesized to evaluate their potential application as hernia repair meshes. These meshes are crucial as they provide structural support to weakened tissues, reducing the risk of hernia recurrence and promoting faster recovery. They improve patient outcomes by enhancing the durability and effectiveness of hernia repairs. Chi scaffolds exhibited lower porosity compared to CMC scaffolds, with fiber inclusion enhancing porosity. The CMC4‐Ac scaffold demonstrated the highest porosity at 67.2%, which is crucial for supporting cell growth and tissue regeneration. All scaffolds exhibited exceptional hydration levels, which is vital for cell growth. Scanning electron microscope (SEM) images revealed open pores in the CMC4 scaffolds, which enhances tissue formation. Tensile strength tests indicated that all scaffolds surpassed the minimum requirements, with CMC4‐Ac standing out for its exceptional properties. CMC scaffolds showed greater degradation, which was mitigated by fiber reinforcement. Chi scaffolds absorbed more Croton draco extract (Cdext) but exhibited lower release rates compared to CMC scaffolds. No hemolytic and non‐cytotoxicity effects were observed. CMC4‐Ac emerged as the most promising scaffold due to its superior properties, making it suitable for hernia repair meshes.
Syntheses of Novel Spirobenzazepinoindole Derivatives via Lewis‐Acid Catalyzed Pictet‐Spengler Cyclization
Authors: Bansal Diksha , Nataraj Gokulprasanth , Sivaganesan Pooja , Das Mrinal Kanti , Chaudhuri Saikat
Published: September 2024

The syntheses of novel spirobenzazepinoindole derivatives has been achieved through a highly efficient and synthetic route. The approach involves a two‐step reaction, utilizing indole derivatives, 2‐amino benzyl alcohol, and ninhydrin as key starting materials under mild reaction conditions. The reaction proceeds via a sequential cascade process involving cyclization, condensation and spiro‐annulation, leading to the formation of the spirobenzazepinoindole core structure in good to excellent yields. The method offers broad substrate scope, high atom economy, and operational simplicity. The synthesized spirobenzazepinoindoles were fully characterized by spectroscopic techniques, including NMR (1H & 13C), IR and mass spectrometry. The methodology provides a valuable tool for the rapid generation of structurally complex spirobenzazepinoindoles, which could serve as scaffolds for the development of new therapeutic agents.
Geometric stabilization of discrete‐time systems via dissipativity approach and output feedback control
Authors: Wen Xinyuan , Yang Fan , Ren Yuanhong , Bai Xuejie
Published: September 2024

Geometric stabilizability is studied for nonlinear discrete‐time systems (DTS) utilizing linear static output feedback (SOF). Initially, a linear SOF controller is designed such that nonlinear DTS achieve geometric stabilizability. Utilizing the concept of geometric QSR‐dissipativity (GQSR‐D), a condition both sufficient and necessary is proffered to guarantee geometric stabilizability for nonlinear DTS. Subsequently, the necessary conditions of linear matrix inequality (LMI) are delineated to ascertain the stability of a system employing linear SOF. A new sufficient and necessary condition is provided aiming to stabilize the linear time‐invariant (LTI) DTS based on GQSR‐D. Lastly, examples are furnished to elucidate the efficacy of the results, thereby reinforcing their practical applicability.
Pricing Cyber Insurance: A Geospatial Statistical Approach
Authors: Ballestra L. V. , D'Amato V. , Fersini P. , Forte S. , Greco F.
Published: September 2024

Cyberspace is a dynamic ecosystem consisting of interconnected data, devices, and individuals, with multiple network layers comprising identifiable nodes. Location‐based information can significantly improve cyber resilience decision‐making and facilitate the development of innovative cyber risk pricing tools. This article is based on a methodology that uses company geospatial data to accurately estimate the number of expected losses arising from cyberattacks. Our approach aims to build and compare statistical spatial models that allow pricing cyber policies more effectively than traditional non‐spatial methods by incorporating all available data. By accounting for spatial dependence, we can assess the risk of data breaches and contribute to the design of more efficient cyber risk policies for the insurance market.
Interfacial challenges and recent advances of solid‐state lithium metal batteries
Authors: Jeong Wooyoung , Yun Jonghyeok , Lee Jong‐Won
Published: September 2024

Growing market demands on portable electronics, electric vehicles, and energy storage system calls for the development of high‐energy density lithium (Li) batteries. Li metal is considered as a promising anode material owing to their high capacity and low electrochemical potential. However, high reactivity of Li metal with conventional flammable liquid electrolytes easily forms Li dendrites, which may cause short‐circuit and even catching fire, obstructing the wide application of Li metal batteries. Although non−/less‐flammable solid electrolytes have replaced the conventional liquid electrolytes, solid‐state Li metal batteries (SSLMBs) suffer from lower Li+ conductivities, chemical/electrochemical incompatibilities toward Li metal, and inhomogeneous Li+ flux at the interfaces. Therefore, many researchers have devoted themselves to solve these problems. For a better understanding on the current issues and recent advances, this article provides (1) a review on various solid electrolytes with high Li+ conductivity and their interfacial issues in SSLMBs, and (2) recent progress in stabilization of the interface between the Li node and solid electrolytes, including an electrolyte modification (e.g., composition, additives) and introduction of an interlayer.