bluuebunny/crossref_metadata_2025_split huggingface dataset:
“Red Carbon”: A Rediscovered Covalent Crystalline Semiconductor
Authors: Odziomek Mateusz , Giusto Paolo , Kossmann Janina , Tarakina Nadezda V. , Heske Julian , Rivadeneira Salvador M. , Keil Waldemar , Schmidt Claudia , Mazzanti Stefano , Savateev Oleksandr , Perdigón‐Toro Lorena , Neher Dieter , Kühne Thomas D. , Antonietti Markus , López‐Salas Nieves 
Published: August 2022

AbstractCarbon suboxide (C3O2) is a unique molecule able to polymerize spontaneously into highly conjugated light‐absorbing structures at temperatures as low as 0 °C. Despite obvious advantages, little is known about the nature and the functional properties of this carbonaceous material. In this work, the aim is to bring “red carbon,” a forgotten polymeric semiconductor, back to the community's attention. A solution polymerization process is adapted to simplify the synthesis and control the structure. This allows one to obtain this crystalline covalent material at low temperatures. Both spectroscopic and elemental analyses support the chemical structure represented as conjugated ladder polypyrone ribbons. Density functional theory calculations suggest a crystalline structure of AB stacks of polypyrone ribbons and identify the material as a direct bandgap semiconductor with a medium bandgap that is further confirmed by optical analysis. The material shows promising photocatalytic performance using blue light. Moreover, the simple condensation–aromatization route described here allows the straightforward fabrication of conjugated ladder polymers and can be inspiring for the synthesis of carbonaceous materials at low temperatures in general.
Monolithic Integration of Perovskite Photoabsorbers with IGZO Thin‐Film Transistor Backplane for Phototransistor‐Based Image Sensor
Authors: Chen Tong , Wang Chunyun , Yang Guoshen , Lou Qiang , Lin Qingping , Zhang Shengdong , Zhou Hang 
Published: August 2022

AbstractMonolithic integration of perovskite materials and their optoelectronic devices with well‐developed thin‐film transistor (TFT) backplane is leading to new applications in displays and image sensors. Herein, a scalable polyimide assisted patterning approach for monolithic integration of perovskite based high‐sensitive phototransistor array on indium gallium zinc oxide (IGZO) active matrix backplane is introduced. Polyimide vias are first formed by conventional photolithography process, through which uniform perovskite films of arbitrary patterns with feature size less than 20 µm are fabricated by spin‐on‐patterning method. Using this technique, patterns of quasi 2D perovskite photoabsorbing layer are precisely deposited onto the channel area of the photosensing IGZO TFT, forming high‐performance phototransistors with responsivity and detectivity reaching 835.7 A W−1 and 5.4 × 1012 Jones, respectively. An image sensor with 8 × 8 pixels array containing both photosensing perovskite/IGZO transistors and switching IGZO transistors is demonstrated, in which the switching IGZO transistor elements on the backplane are protected by the non‐patterned region of the polyimide encapsulation layer. This whole fabrication process is compatible with TFT manufacturing process and will significantly reduce the cost needed for constructing next generation high‐resolution image sensors.
Highly Durable Compact Sleeve Triboelectric–Electromagnetic Hybrid Nanogenerator for Broadband Triggered Energy Harvesting and Active Wind Speed Sensing
Authors: Rui Pinshu , Li Dongpeng , Zi Zhenfa , Zhao Yan 
Published: August 2022

AbstractTriboelectric nanogenerator (TENG) has great potential in harvesting low‐frequency environmental mechanical energy, but the unavoidable friction between tribo‐layers limits the frequency range and efficiency of energy harvesting. Herein, a lower friction and high‐performance triboelectric–electromagnetic hybrid nanogenerator (TE‐HNG) is proposed to harvest broadband rotation energy. The compact sleeve multi‐unit TENG and electromagnetic generator are integrated to achieve respective complementary in electrical output and energy harvesting frequencies. The charge‐supplement type TENG with a single arched fluorinated ethylene propylene film design can not only supplement the charge dissipation of the Nylon surface in time but also ensure the stable output of TENG. The influences of the rotation speed on the electrical output and optimal load of TENG are systematically studied. As a self‐powered active wind speed sensor, the TE‐HNG device can detect the wind speed as low as 1 m s−1, which indicates that the TE‐HNG can harvest broadband wind energy (≈1 m s−1). Triggered by the wind, the TE‐HNG device can not only power the temperature/humidity sensor to work steadily and continuously but also realize the full‐automatic and self‐powered operation of the environmental meteorological monitoring system by combining the energy management and wireless transmission module.
Hierarchical Graphene‐Dye Bilayers for Multimodal Optoelectronic Sensing and Decoupling of Complex Stimuli
Authors: Khatib Muhammad , Rapoport Shelley , Zohar Orr , Mansour Elias , Zheng Youbin , Tang Ning , Saliba Walaa , Mulytin Yana , Huynh Tan‐Phat , Haick Hossam 
Published: August 2022

AbstractSignals obtained by chemical or calorimetric sensors are highly coupled and complex, making it very challenging to precisely detect and discriminate between simultaneous stimuli. The development of sensors that provide multiple sensory outputs is a good way to tackle such a long‐lasting challenge. Herein, a new design of multimodal sensors capable of generating both colorimetric and electrical sensory outputs is introduced. This is achieved by coupling two functional nanolayers, graphene (electrically active) and dyes (colorimetric) in which each layer can work either autonomously or in conjugation with the other sensing layer. It is shown that the interfacial interaction of graphene with the wide variety of dyes creates unique interfacial sensing sites for the detection of chemicals. This endows each sensor or sensor array, in the format of (opto)electronic nose, with a “fingerprint” of varying bonding possibilities, enlarging the spectrum of gas–sensor interactions. Furthermore, it is shown that the hierarchical nanobilayer structure allows the separation and discrimination of volatile organic compounds (VOCs) based on their diffusion kinetics. Taken together, the bilayer design qualifies as a superior sensor compared to unimodal devices by offering improved detection limits, wider dynamic ranges, and higher sensitivity and selectivity in the binary discrimination of a wide range of stimuli (temperature, relative humidity, and VOCs).
Constructing Soft Perovskite–Substrate Interfaces for Dynamic Modulation of Perovskite Film in Inverted Solar Cells with Over 6200 Hours Photostability
Authors: Lv Wenxuan , Hu Zhaoying , Qiu Wei , Yan Dongdong , Li Meicheng , Mei Anyi , Xu Ligang , Chen Runfeng 
Published: August 2022

AbstractHigh‐performance perovskite solar cells (PSCs) depend heavily on the quality of perovskite films, which is closely related to the lattice distortion, perovskite crystallization, and interfacial defects when being spin‐coated and annealed on the substrate surface. Here, a dynamic strategy to modulate the perovskite film formation by using a soft perovskite–substrate interface constructed by employing amphiphilic soft molecules (ASMs) with long alkyl chains and Lewis base groups is proposed. The hydrophobic alkyl chains of ASMs interacted with poly(triarylamine) (PTAA) greatly improve the wettability of PTAA to facilitate the nucleation and growth of perovskite crystals, while the Lewis base groups bound to perovskite lattices significantly passivate the defects in situ. More importantly, this soft perovskite–substrate interface with ASMs between PTAA and perovskite film can dynamically match the lattice distortion with reduced interfacial residual strain upon perovskite crystallization and thermal annealing owing to the soft self‐adaptive long‐chains, leading to high‐quality perovskite films. Thus, the inverted PSCs show a power conversion efficiency approaching 20% with good reproducibility and negligible hysteresis. More impressively, the unencapsulated device exhibits state‐of‐the‐art photostability, retaining 84% of its initial efficiency under continuous simulated 1‐sun illumination for more than 6200 h at elevated temperature (≈65 °C).
Advances of Various Heterogeneous Structure Types in Molecular Junction Systems and Their Charge Transport Properties
Authors: Shin Jaeho , Eo Jung Sun , Jeon Takgyeong , Lee Takhee , Wang Gunuk 
Published: August 2022

AbstractMolecular electronics that can produce functional electronic circuits using a single molecule or molecular ensemble remains an attractive research field because it not only represents an essential step toward realizing ultimate electronic device scaling but may also expand our understanding of the intrinsic quantum transports at the molecular level. Recently, in order to overcome the difficulties inherent in the conventional approach to studying molecular electronics and developing functional device applications, this field has attempted to diversify the electrical characteristics and device architectures using various types of heterogeneous structures in molecular junctions. This review summarizes recent efforts devoted to functional devices with molecular heterostructures. Diverse molecules and materials can be combined and incorporated in such two‐ and three‐terminal heterojunction structures, to achieve desirable electronic functionalities. The heterojunction structures, charge transport mechanisms, and possible strategies for implementing electronic functions using various hetero unit materials are presented sequentially. In addition, the applicability and merits of molecular heterojunction structures, as well as the anticipated challenges associated with their implementation in device applications are discussed and summarized. This review will contribute to a deeper understanding of charge transport through molecular heterojunction, and it may pave the way toward desirable electronic functionalities in molecular electronics applications.
Long‐Duration and Non‐Invasive Photoacoustic Imaging of Multiple Anatomical Structures in a Live Mouse Using a Single Contrast Agent
Authors: Khadria Anjul , Paavola Chad D. , Zhang Yang , Davis Samuel P. X. , Grealish Patrick F. , Maslov Konstantin , Shi Junhui , Beals John M. , Oladipupo Sunday S. , Wang Lihong V. 
Published: August 2022

AbstractLong‐duration in vivo simultaneous imaging of multiple anatomical structures is useful for understanding physiological aspects of diseases, informative for molecular optimization in preclinical models, and has potential applications in surgical settings to improve clinical outcomes. Previous studies involving simultaneous imaging of multiple anatomical structures, for example, blood and lymphatic vessels as well as peripheral nerves and sebaceous glands, have used genetically engineered mice, which require expensive and time‐consuming methods. Here, an IgG4 isotype control antibody is labeled with a near‐infrared dye and injected into a mouse ear to enable simultaneous visualization of blood and lymphatic vessels, peripheral nerves, and sebaceous glands for up to 3 h using photoacoustic microscopy. For multiple anatomical structure imaging, peripheral nerves and sebaceous glands are imaged inside the injected dye‐labeled antibody mass while the lymphatic vessels are visualized outside the mass. The efficacy of the contrast agent to label and localize deep medial lymphatic vessels and lymph nodes using photoacoustic computed tomography is demonstrated. The capability of a single injectable contrast agent to image multiple structures for several hours will potentially improve preclinical therapeutic optimization, shorten discovery timelines, and enable clinical treatments.
Chemical Strain Engineering of MAPbI3 Perovskite Films
Authors: Yalcinkaya Yenal , Hermes Ilka M. , Seewald Tobias , Amann‐Winkel Katrin , Veith Lothar , Schmidt‐Mende Lukas , Weber Stefan A.L. 
Published: August 2022

AbstractThis study introduces a new chemical method for controlling the strain in methylammonium lead iodide (MAPbI3) perovskite crystals by varying the ratio of Pb(Ac)2 and PbCl2 in the precursor solution. To observe the effect on crystal strain, a combination of piezoresponse force microscopy (PFM) and X‐ray diffraction (XRD) is used. The PFM images show an increase in the average size of ferroelastic twin domains upon increasing the PbCl2 content, indicating an increase in crystal strain. The XRD spectra support this observation with strong crystal twinning features that appear in the spectra. This behavior is caused by a strain gradient during the crystallization due to different evaporation rates of methylammonium acetate and methylammonium chloride as revealed by time‐of‐flight secondary ion mass spectroscopy and grazing incidince X‐ray diffraction measurements. Additional time‐resolved photoluminescence shows an increased carrier lifetime in the MAPbI3 films prepared with higher PbCl2 content, suggesting a decreased trap density in films with larger twin domain structures. The results demonstrate the potential of chemical strain engineering as a simple method for controlling strain‐related effects in lead halide perovskites.
Kinetically guided high‐yield and rapid production of ε‐caprolactone in a microreactor system
Authors: Yang Yue , Du Wei , Qian Gang , Duan Xuezhi , Gu Xiongyi , Zhou Xinggui , Yang Zhirong , Zhang Jing 
Published: August 2022

AbstractIndustrial production of ε‐caprolactone, the monomer of biodegradable polycaprolactone, consists of acetic acid peroxidation and the Baeyer–Villiger oxidation of cyclohexanone in semi‐batch reactors. The strong exothermic feature of the latter and ease of ε‐caprolactone hydrolysis significantly affects the production efficiency. Here, collective effects of kinetic studies and density functional theory (DFT) calculations reveal activation energy of the Baeyer–Villiger oxidation is higher than that of ε‐caprolactone hydrolysis and the hydrolysis barrier is controlled by hydrogen bond energy of the reaction medium. Then, we developed a microreactor system to intensify heat transfer thereby allowing safe and efficient production of ε‐caprolactone. A yield of 99.6% was achieved within minutes via consecutive two‐step reactions of peroxidation and the Baeyer–Villiger oxidation, as compared with state‐of‐the‐art yield of 96% in hours of industrial operation. The high selectivity is attributed to high reaction temperature allowed by the microreactor and DFT‐guided choice of solvent to mitigate the hydrolysis.
Topology, Oxidation States, and Charge Transport in Ionic Conductors
Authors: Pegolo Paolo , Baroni Stefano , Grasselli Federico 
Published: August 2022

AbstractRecent theoretical advances, based on a combination of concepts from Thouless' topological theory of adiabatic charge transport and a newly introduced gauge‐invariance principle for transport coefficients, have permitted to connect (and reconcile) Faraday's picture of ionic transport—whereby each atom carries a well‐defined integer charge—with a rigorous quantum description of the electronic charge‐density distribution, which hardly suggests its partition into well defined atomic contributions. In this paper, these progresses are reviewed; in particular, it is shown how, by relaxing some general topological conditions, charge may be transported in ionic conductors without any net ionic displacements. After reporting numerical experiments which corroborate these findings, a new connection between the topological picture and the well‐known Marcus–Hush theory of electron transfer is introduced in terms of the topology of adiabatic paths drawn by atomic trajectories. As a significant byproduct, the results reviewed here permit to classify different regimes of ionic transport according to the topological properties of the electronic structure of the conducting material. Finally, a few recent applications to energy materials and planetary sciences are reported.
Order‐dependent and delay‐dependent conditions for stability and stabilization of fractional‐order time‐varying delay systems using small gain theorem
Authors: Jin Xiao‐Chuang , Lu Jun‐Guo 
Published: August 2022

AbstractIn this paper, the stability and stabilization problems for fractional‐order time‐varying delay systems are investigated. Firstly, by casting the stability problem as one of robust stability analysis problems and utilizing the small gain theorem, an order‐dependent and delay‐dependent stability condition for fractional‐order time‐varying delay systems is developed. Taking advantage of the information of order and delay, the stability condition is less conservative than the existing results. Then, state feedback controllers that stabilize fractional‐order time‐varying delay systems are developed. To tackle the computational difficulty of the controller design method, a local optimization algorithm is proposed. Finally, numerical examples are provided to illustrate that the proposed criteria are valid and less conservative than the existing ones.
Microglia activation in the mPFC mediates anxiety‐like behaviors caused by Staphylococcus aureus strain USA300
Authors: Zou Jiao , Shang Weilong , Yang Ling , Liu Tianyao , Wang Lian , Li Xin , Zhao Jinghui , Rao Xiancai , Gao Junwei , Fan Xiaotang 
Published: August 2022

AbstractIntroduction: Staphylococcus aureus (S. aureus) is considered as one of the major causative agents of serious hospital‐ and community‐acquired infections. Recent studies have reported that S. aureus infection induced neuroinflammation and was linked with some mental disorders. To evaluate the effects of S. aureus infection on abnormal behaviors, we conducted the present study.Methods: A S. aureus USA300‐infected mouse model was established using bacterial suspension injection into tail vein. A series of behavioral tests were performed after USA300 infection. The expression of cytokines was detected in serum and mPFC. The number and some morphological parameters of microglia were also evaluated by immunofluorescence staining.Results: Anxiety‐like behaviors, instead of locomotor activity impairment or depression‐like behaviors, were observed in mice infected with S. aureus USA300 compared with control. S. aureus USA300 infection caused overexpression of IL‐6, TNF‐α, and IL‐1β in serum, resulted in microglial over‐activation and excessive release of proinflammatory cytokines in the mPFC. In addition, overexpression of TLR2 accompanied by increased GLS1 and p‐STAT3 was observed in the mPFC of mice infected with S. aureus USA300.Conclusion: This study provides evidence that S. aureus USA300 infection can lead to neuroinflammation in the mPFC of mice, which may contribute to the development of anxiety.
The association between body mass index and efficacy of pembrolizumab as second‐line therapy in patients with recurrent/metastatic head and neck squamous cell carcinoma
Authors: Zhang Xinyi , Rui Mengyu , Lin Chao , Li Zhi , Wei Dongliang , Han Ruxue , Ju Houyu , Ren Guoxin 
Published: August 2022

AbstractBackgroundRecent evidence suggested a potential correlation between BMI and the efficacy of immune checkpoint inhibitors in cancer patients. This study aimed to evaluate the prognostic value of the body mass index (BMI) in recurrent/metastatic head and neck squamous cell carcinoma (R/M HNSCC) patients treat with pembrolizumab.MethodsThe current retrospective cohort study enrolled 49 R/M HNSCC patients underwent at least one cycle of pembrolizumab as second‐line treatment from June 2018 to October 2020. Survival analysis of immunotherapy prognosis and risk factor analysis of age, gender, BMI, ECOG‐PS, CPS, rT‐stage, tumor site, and tube feeding.ResultsAmong the 49 patients, the BMI at the time of immunotherapy ranged from 14.5 to 32.0 kg/m2. The Kaplan–Meier analysis showed that the BMI was significantly correlated with overall survival time (OS, p = 0.0007) and progression‐free survival time (PFS, p = 0.0012). BMI, gender, prior treatment, serum albumin level, ECOG‐PS, CPS and rT‐stage were analyzed in multivariate Cox regression model analysis after adjusted for potential confounding clinical variables. Patients with underweight (OS:HR = 6.862, 95% CI:1.566–30.064, p = 0.011; PFS:HR = 5.672, 95% CI:1.364–23.586, p = 0.017);ECOG≥2 (OS:HR = 0.250, 95% CI:0.086–0.731, p = 0.011;PFS:HR = 0.284, 95% CI:0.101–0.805, p = 0.018); CPS <1(OS: HR = 4.34, 95% CI:1.271–15.464, p = 0.019; PFS:HR = 3.859, 95% CI:1.180–12.618, p = 0.025) and rT4‐stage(OS:HR = 4.380, 95% CI:1.452–13.209, p = 0.009;PFS: HR = 3.799, 95% CI:1.240–11.638, p = 0.019) suffered higher risk of mortality.ConclusionsThe BMI at the time of clinical diagnosis was showed to be an independent predictive factor for R/M HNSCC patients receiving pembrolizumab. Compared with normal weight patients, underweight patients have worse clinical prognosis.
The Unprecedented [S4N2O10]2−Anion in the Molecular Gold Complexes [Au2Br2(S4N2O10)2] and [Au2Cl2(S4N2O10)2](S2O5Cl2)
Authors: Rennebaum Tobias , van Gerven David , Wickleder Mathias S. 
Published: August 2022

AbstractThe reaction of hexachlorophosphazene, P3N3Cl6, with SO3and the gold halides AuCl3and AuBr3, respectively, leads to the new cyclic anionic tetramer, [S4N2O10]2−, which is coordinated to Au3+in the dimeric complexes [Au2X2(S4N2O10)2] (X=Cl, Br). The [S4N2O10]2−anion can be seen as the condensation product of two sulfate anions, [SO4]2−,and two amidosulfate anions, [NH2SO3]−.
Use of O3 and O3/H2O2 for degradation of organic matter from Bayer liquor towards new resource management: Kinetic and mechanism
Authors: Pastor Miguel Antonio Soplin , Botelho Junior Amilton Barbosa , Tenório Jorge Alberto Soares , Espinosa Denise Crocce Romano , Baltazar Marcela dos Passos Galluzzi 
Published: August 2022

AbstractSince the quality of bauxite resources has decreased and the organic carbon content has increased, different approaches are explored to remove the organic matter in alumina production. Advanced oxidative processes (AOPs) represent a possibility since they are widely used as an alternative for treating wastewaters to degrade organic pollutant molecules and in hydrometallurgy processes. For this reason, the goal of the project was the ozonation of Bayer liquor for organic matter removal. The ozone concentration was evaluated over time, as well as the H2O2 concentration and temperature. Results showed that the total organic carbon (TOC) removal achieved 19% in the most optimized condition with a kinetic rate of 0.0157 h−1 –21.9 mg/L O3, 0.05 mol/L H2O2 at 80°C. The colour of the liquor changed from dark brown to white‐yellow, indicating that the size of the organic compounds had decreased. Also, 95.4% of degraded TOC formed CO2, and almost 50% of the organic matter was oxalate compounds. The energy required for ozone production versus removed organic matter demonstrated that the technique proposed might be technically and economically feasible to be applied in the Bayer process. The study demonstrates the application of AOP in an extremely alkaline condition.