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Induced Absolute Configuration of Achiral Tetradentate Ligands in Metal–Organic Frameworks for Circularly Polarized luminescence

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Chinese Journal of Chemistry 2024年第11期42卷 1260-1266页

作者： Hong-Ru Fu Dan-Dan Ren Kun Zhang Hong Chen Xiaoyan lu Qing-Rong Ding lu-fang ma College of Chemistry and Chemical Engineering Luoyang Normal UniversityLuoyangHenan471934 China College of materials&Chemical Engineering China Three Gorges UniversityYichangHubei443002 China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian350002 China

The crystallization of chiral molecules is of great significance to understand the origin and evolution of hierarchical chirality and reveal the relationships between structural chirality and circularly polarized luminescence(CPL)***,we report two pairs of chiral metal–organic frameworks(MOFs)(DCF-17/LCF-17,DCF-18/LCF-18)by utilizing tetradentate ligands tetra(3-imidazoylphenyl)ethylene(TIPE)and 4,4'-[4',5'-bis[4-(4-pyridinyl)phenyl][1,1':2',1”-terphenyl]-4,4”-diyl]bis[pyridine](TPPP)as *** can be observed that the spontaneous resolution of the achiral ligands is converted into the induced resolution,and the ligands form the absolute configuration by using enantiopure camphoric acid(cam)as chiral induced reagent(CIR).As a result,the racemate MOFs can be driven to generate absolute homochiral *** two achiral MOFs[Cd(D-cam)(TPPP)_(0.5)](AF-1,AF=achiral framework)and[Cd(L-cam)(TPPP)_(0.5)](AF-2)were *** position disorder of D/L-cam skeleton causes the generation of nonchiralization,further leading to disappearance of symmetry breaking of *** the perspective of structure,this is the first report which reveals the chiral transfer and nonchiralization between chiral induced agents and tetradentate ***,DCF-17 and LCF-17 show CPL with luminescence dissymmetry factor(glum)of–1.0×10^(-2)and+9.2×10^(–3),*** work provides the useful evidences to reveal the induced chiral crystallization and the construction of CPL-active crystalline materials.

关键词： Metal-organic frameworks Circularly polarized luminescence Chirality induction Spontaneous resolution Chirality transfer

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Size-controlled synthesis and near-infrared photothermal response of Cp^(*)Rh-based metalla[2]catenanes and rectangular metallamacrocycles

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Chinese Chemical Letters 2024年第6期35卷 337-343页

作者： Ying Zhao Yin-Hang Chai Tian Chen Jie Zheng Ting-Ting Li Francisco Aznarez Li-Long Dang lu-fang ma College of Chemistry and Chemical Engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang 471934China College of Chemistry Zhengzhou UniversityZhengzhou 450001China Shanghai Key Laboratory of Molecular Catalysis and Innovative materials State Key Laboratory of Molecular Engineering of PolymersDepartment of ChemistryFudan UniversityShanghai 200438China

A variety of research reports on novel supramolecular topologies have been published over the last ***,it is still a great challenge to tap into the inner functional properties of these ***,two tetranuclear metallamacrocycles 1 and 2 and four octonuclear[2]catenanes 3-6 were constructed successfully via a coordination-driven self-assembly strategy,by conscious design and use of the tetramethyl bidentate pyridine ligand L1,and the appropriate selection of six binuclear half-sandwich rhodium building units with different longitudinal *** complexes have been fully characterized by single crystal X-ray diffraction analysis and NMR ***,near-infrared photothermal studies of the obtained[2]catenanes reveal different photothermal response in solid and solution states,which may be attributed to a strong fluorescence quenching effect of the half-sandwich organometallic fragment and different conjugated effect of Cp^(*)Rh based building blocks in the interlocking *** photothermal conversion efficiencies of[2]catenanes 4-6 fall in the range 30.5%-16.5% *** contribution aims to play a key role in the experimental development of Cp^(*)-based photothermal materials.

关键词： Catenanes Photothermal materials Supramolecular topologies Half-sandwich fragment 3,3'-N-donor analogues

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Two comparable Ba-MOFs with similar linkers for enhanced CO_(2)capture and separation by introducing N-rich groups

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Rare Metals 2021年第2期40卷 499-504页

作者： Ying Zhao Jiao Liu Min-Le Han Guo-Ping Yang lu-fang ma Yao-Yu Wang College of Chemistry and Chemical Engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang471934China Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education Shaanxi Key Laboratory of Physico-Inorganic ChemistryCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an710127China

Two new different metal-organic frameworks(MOFs)[Ba(L1)(H_(2)O)_(2)]_(n)·nH_(2)O(MOF 1)and[Ba(L2)(-n2 O)_(2)]_(n)·0.5 nDMF·0.5 nH_(2)O(MOF 2)were yielded by the assembly of oxygen-friendly Ba(Ⅱ)ions and two similar linkers,namely 2-(imidazol-1-yl)terephthalic acid(H_(2)L1)and 2-(1 H-1,2,4-triazol-1-yl)terephthalic acid(H_(2)L2).Single-crystal X-ray diffractions(XRD)indicate that MOF1 is a new three-dimensional(3 D)stacking dense network formed by the one-dimensional(1 D)rod-shaped chains and L1 linkers,whereas MOF 2 presents a 3 D nanotube porous framework with cylindrical tunnels based on the 1 D loop chains as the secondary building units(SBUs)by replacing the imidazole group in H_(2)L1 with the triazole group in H_(2)*** a result,MOF 2 has a higher density of active sites and Lewis acid sites in the porous surface of nanotube than MOF ***,the CO_(2)capture and separation capacity of MOF 2 is great higher than that of CH_(4)at298 K.

关键词： MOFs Similar linkers Secondary building units(SBUs) CO_(2)capture Isosteric heat

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Low-thermal-budget synthesis of monolayer MoS2

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Science China materials 2024年第1期67卷 372-374页

作者： Zongmeng Yang Shibo fang Jing lu State Key Laboratory for Mesoscopic Physics and School of Physics Peking University Collaborative Innovation Center of Quantum matter Beijing Key Laboratory for magnetoelectric materials and Devices (BKL-MEMD) Peking University Peking University Yangtze Delta Institute of Optoelectronics Key Laboratory for the Physics and Chemistry of Nanodevices Peking University Beijing Key Laboratory of Quantum Devices Peking University

Two-dimensional (2D) materials, such as MoS2, have been considered as a competitive coordinate for future electronics due to their excellent electrostatics and high mobility [1–3]. Moreover, the potential integration of 2D materials with silicon circuits can present increased density and multifunction in future heterogeneously integrated circuits [4,5]. However, the high thermal-budget during Mo S2 synthesis exceeds the temperature requirement of direct integration with Si in the back-end-of-line (BEOL) fabrication process [6–8].

关键词： FILMS

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A rigorous real-time acoustic positioning method for ocean bottom seismic exploration

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Satellite Navigation 2024年第1期5卷 168-190页

作者： Jinye ma Shouchuan fang Jianhu Zhao School of Geodesy and Geomatics Wuhan University129 Luoyu RoadWuhan430079China Institute of marine Science and Technology Wuhan UniversityWuhan430079China Surveying Service Center BGP Inc.CNPCZhuozhou072751HebeiChina

The conventional technique for positioning seafloor geophones in ocean bottom seismic exploration encounters several challenges,including the significant impact of outliers on positioning results,underutilization of high-precision observations,and low efficiency in real-time data *** issues inevitably affect the quality of seismic exploration *** address these challenges and enhance the accuracy of geophone positioning,this paper proposes a rigorous real-time acoustic positioning method for geophones based on sequential adjustment and Baarda's outlier detection *** proposed method comprises three key steps:grouping the original acoustic observations,constructing the intra-group acoustic positioning model,and synthesizing the positioning results across the different *** validity and practicality of this approach are confirmed through a simulation experiment as well as the field experiment conducted in the Bohai Sea,*** results demonstrate that the proposed method effectively eliminates outliers in the original observations and maximizes the utilization of high-quality *** to traditional acoustic positioning methods,it significantly reduces positioning errors from meters to decimeters,and in some cases can achieve centimeter-level *** the sound velocity profile in the operating sea area is measured,the method can attain the posterior standard deviation at the millimeter level and positioning errors within 10 *** the sound velocity profile is unknown,the method can achieve the posterior standard deviation at centimeter-level and positioning errors of approximately 20 cm.

关键词： Ocean bottom seismic exploration Geophone positioning Acoustic positioning method Sequential adjustment Outlier detection

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Self-assembled all-oxides three-phase vertically aligned nanocomposite thin film with multifunctionality

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Nano Research 2024年第9期17卷 8226-8232页

作者： Jijie Huang Yuan fang Ping lu Juanjuan lu Haiyan Wang School of materials Shenzhen Campus of Sun Yat-sen UniversityShenzhen 518107China School of materials Engineering Purdue UniversityWest LafayetteIN 47907USA Sandia National Laboratories AlbuquerqueNew Mexico 87185USA School of Electrical and Computer Engineering Purdue UniversityWest LafayetteIN 47907USA

Multi-phase vertically aligned nanocomposite(MP-VAN)thin films represent a promising avenue for achieving complex multifunctionality,exploring novel interfacial phenomena,and enabling complex metamaterial designs and *** this study,a novel self-assembled all-oxides three-phase VAN system was conceptualized and fabricated utilizing pulsed laser deposition(PLD)with a single composite *** microstructural analysis reveals the presence of three distinct phases:LiNbO_(3),CeO_(2-x),and LiNbCe_(1-x)O_(y)within the MP-VAN ***,ferroelectric,dielectric,optical anisotropy,and magnetic properties were systematically investigated to showcase the multifunctionality inherent in these *** work presents a pioneering approach to designing and realizing MP-VAN systems,and opens up opportunities for tailoring the complex three-dimensional(3D)physical properties and property coupling of VAN films towards diverse device applications.

关键词： thin film three-phase vertically aligned nanocomposite multifunctionality ferroelectricity optical anisotropy

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Experimental distillation of tripartite quantum steering with an optimal local filtering operation

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Photonics Research 2024年第3期12卷 552-562页

作者： QIAN-XI ZHANG XIAO-XU fang HE lu School of Physics State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China Shenzhen Research Institute of Shandong University Shenzhen 518057China

Multipartite Einstein-Podolsky-Rosen(EPR)steering admits multipartite entanglement in the presence of uncharacterized verifiers,enabling practical applications in semi-device-independent *** applications generally require stronger steerability,while the unavoidable noise weakens steerability and consequently degrades the performance of quantum information ***,we propose the local filtering operation that can maximally distill genuine tripartite EPR steering from N copies of three-qubit generalized Greenberger-Horne-Zeilinger states,in the context of two semi-device-independent *** optimal filtering operation is determined by the maximization of assemblage *** and numerical results indicate the advantage of the proposed filtering operation when N is finite and the steerability of initial assemblages is ***,a proof-of-principle demonstration of two-copy distillation is realized with the optical *** advantage of the optimal local filtering operation is confirmed by the distilled assemblage in terms of higher assemblage fidelity with perfectly genuine tripartite steerable assemblages,as well as the greater violation of the inequality to witness genuine tripartite steerable *** results benefit the distillation of multipartite EPR steering in practice,where the number of copies of initial assemblages is generally finite.

关键词： filtering distillation optimal

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Efficient photocatalytic biomass-alcohol conversion with simultaneous hydrogen evolution over ultrathin 2D NiS/Ni-CdS photocatalyst

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Chinese Chemical Letters 2024年第7期35卷 422-427页

作者： Zongyi Huang Cheng Guo Quanxing Zheng Hongliang lu Pengfei ma Zhengzhong fang Pengfei Sun Xiaodong Yi Zhou Chen State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of materials Key Laboratory of High Performance Ceramic Fibers(Xiamen University)Ministry of EducationXiamen UniversityXiamen 361005China Technology Center China Tobacco Fujian Industrial Co.Ltd.Xiamen 361021 China

The photocatalytic conversion of biomass into high-value chemicals,coupled with simultaneous hydrogen(H_(2))evolution,leveraging the electrons and holes generated by solar energy,holds great promise for addressing energy *** this study,we constructed a dual functional photocatalytic system formed by NiS loaded on Ni doped two-dimensional(2D)CdS nanosheet(NiS/Ni-CdSNS)heterostructure for visible-light-driven H_(2)evolution and ethanol oxidation to ***,the 2D NiS/NiCdSNS exhibited significant activity and selectivity in both photocatalytic H_(2)evolution and ethanol oxidation,achieving yields of 7.98 mmol g^(-1)h^(-1)for H_(2)and 7.33 mmol g^(-1)h^(-1)for *** heterogeneous interface of the composite facilitated efficient charge separation,while NiS provided abundant sites for proton reduction,thereby promoting the overall dual-functional photocatalytic *** functional theory calculations further reveal that both Ni doping and NiS loading can reduce the reaction energy barrier of ethanol oxidation of free radicals,and NiS/Ni-CdSNS composite materials exhibit stronger ethanol C-H activation ability to generate key intermediate·CH(OH)CH_(3)on the *** work serves as a valuable guide for the rational design of efficient dual functional photocatalytic systems that combine H_(2)evolution with the selective conversion of organic compounds into high-value chemicals.

关键词： Photocatalysis Biomass-alcohol oxidation H_(2)evolution Dual-functional catalysis

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CToMP: a cycle-task-oriented memory protection scheme for unmanned systems

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Science China(Information Sciences) 2024年第6期67卷 399-417页

作者： Chengyan ma Ning XI Di lu Yebo FENG Jianfeng ma School of Cyber Engineering Xidian University School of Computer Science and Technology Xidian University Department of Computer and Information Science University of Oregon

Memory corruption attacks(MCAs) refer to malicious behaviors of system intruders that modify the contents of a memory location to disrupt the normal operation of computing systems, causing leakage of sensitive data or perturbations to ongoing processes. Unlike general-purpose systems, unmanned systems cannot deploy complete security protection schemes, due to their limitations in size, cost and *** in unmanned systems are particularly difficult to defend against. Furthermore, MCAs have diverse and unpredictable attack interfaces in unmanned systems, severely impacting digital and physical sectors. In this paper, we first generalize, model and taxonomize MCAs found in unmanned systems currently, laying the foundation for designing a portable and general defense approach. According to different attack mechanisms,we found that MCAs are mainly categorized into two types — return2libc and return2shellcode. To tackle return2libc attacks, we model the erratic operation of unmanned systems with cycles and then propose a cycle-task-oriented memory protection(CToMP) approach to protect control flows from tampering. To defend against return2shellcode attacks, we introduce a secure process stack with a randomized memory address by leveraging the memory pool to prevent Shellcode from being executed. Moreover, we discuss the mechanism by which CTo MP resists the return-oriented programming(ROP) attack, a novel variant of return2libc attacks. Finally, we implement CTo MP on CUAV V5+ with Ardupilot and Crazyflie. The evaluation and security analysis results demonstrate that the proposed approach CTo MP is resilient to various MCAs in unmanned systems with low footprints and system overhead.

关键词： unmanned system memory corruption attack memory protection system security randomized memory address

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Local field potentials,spiking activity,and receptive fields in human visual cortex

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Science China(Life Sciences) 2024年第3期67卷 543-554页

作者： lu luo Xiongfei Wang Junshi lu Guanpeng Chen Guoming luan Wu Li Qian Wang fang fang School of Psychological and Cognitive Sciences and Beijing Key Laboratory of Behavior and Mental Health Peking UniversityBeijing 100871China School of Psychology Beijing Sport UniversityBeijing 100084China Department of Neurosurgery Sanbo Brain HospitalCapital Medical UniversityBeijing 100093China Beijing Key Laboratory of Epilepsy Epilepsy CenterSanbo Brain HospitalCapital Medical UniversityBeijing 100093China IDG/McGovern Institute for Brain Research Peking UniversityBeijing 100871China Peking-Tsinghua Center for Life Sciences Peking UniversityBeijing 100871China Beijing Institute for Brain Disorders Beijing 100069China State Key Laboratory of Cognitive Neuroscience and Learning and IDG/McGovern Institute for Brain Research Beijing Normal UniversityBeijing 100875China

The concept of receptive field(RF) is central to sensory neuroscience. Neuronal RF properties have been substantially studied in animals,while those in humans remain nearly unexplored. Here, we measured neuronal RFs with intracranial local field potentials(LFPs) and spiking activity in human visual cortex(V1/V2/V3). We recorded LFPs via macro-contacts and discovered that RF sizes estimated from lowfrequency activity(LFA, 0.5–30 Hz) were larger than those estimated from low-gamma activity(LGA, 30–60 Hz) and high-gamma activity(HGA, 60–150 Hz). We then took a rare opportunity to record LFPs and spiking activity via microwires in V1 simultaneously. We found that RF sizes and temporal profiles measured from LGA and HGA closely matched those from spiking activity. In sum, this study reveals that spiking activity of neurons in human visual cortex could be well approximated by LGA and HGA in RF estimation and temporal profile measurement, implying the pivotal functions of LGA and HGA in early visual information processing.

关键词： human visual cortex receptive field intracranial EEG local field potential spiking activity

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