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Controllable Secondary through-space interaction and Clusteroluminescence

CCS Chemistry 2023年第12期5卷 2832-2844页

作者： Zuping Xiong Jianyu Zhang Lei Wang Yuan Xie Yipu Wang Zujin Zhao Haoke Zhang Jing Zhi Sun Feihe Huang Ben Zhong Tang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027 Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation CenterZhejiang UniversityHangzhou 311215 Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and ReconstructionThe Hong Kong University of Science and TechnologyHong Kong Center for AIE Research College of Materials Science and EngineeringShenzhen UniversityShenzhen 518061 State Key Laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSouth China University of TechnologyGuangzhou 51064 Centre of Healthcare Materials Shaoxing InstituteZhejiang UniversityShaoxing 312000 Stoddart Institute of Molecular Science Department of ChemistryZhejiang UniversityHangzhou 310058 School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen 518172

Nonconjugated clusteroluminogens(CLgens),such as proteins and polystyrene,have become increasingly important in *** show many advantages over traditional conjugated dyes with fused aromatic rings in biological ***,CLgens have historically been unheeded because of their weak visible emissions in the aggregate state,namely clusteroluminescence(CL).Changing the electronic structures of CLgens by precisely regulating the intramolecular throughspace interaction(TSI)to improve their photophysical properties remains an enormous ***,we propose a general strategy to construct a higher-level intramolecular TSI,namely secondary TSI constructed by the primary TSI and a TSI linker,in multi-aryl-substituted alkanes(MAAs).By introducing methyl and phenyl into 1,1,3,3-tetraphenylpropane,the modified MAAs show efficient CL with high luminescence quantum yield(-40%)and long emission wavelength(-530 nm).Then,comprehensive experiments and theoretical studies demonstrate that molecular rigidity and overlap of subunits play pivotal roles in improving these hierarchical *** work not only provides a feasible strategy to achieve controllable manipulation of hierarchical TSIs and CL but also establishes comprehensive TSI-based aggregate photophysics.

关键词： through-space interaction clusteroluminescence aggregation-induced emission alkanes electronic structures aggregate photophysics

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Clusteroluminescence:A gauge of molecular interaction

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Chinese Chemical Letters 2023年第5期34卷 165-173页

作者： Bin Liu Bo Chu Lixun Zhu Haoke Zhang Wang-Zhang Yuan Zheng Zhao Wen-Ming Wan Xing-Hong Zhang School of Energy and Power Engineering North University of ChinaTaiyuan 030051China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesShanghai Key Lab of Electrical Insulation and Thermal AgingShanghai Electrochemical Energy Devices Research CenterShanghai Jiao Tong UniversityShanghai 200240China School of Science and Engineering The Chinese University of Hong KongShenzhen 518172China State Key Laboratory of Structural Chemistry Key Laboratory of Coal to Ethylene Glycol and Its Related TechnologyCenter for Excellence in Molecular SynthesisFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Clusteroluminescence(CL)materials,as an emerging class of luminescent materials with unique photophysical properties,have received increasing attention owing to their great theoretical significance and potential for biological *** much progress has been made in the design,synthesis and application of CL materials,there is still a big challenge in the emission *** far,throughspace interaction has been proposed as the preliminary mechanism of the corresponding clusterizationtriggered emission(CTE)effect,but a systematic theory is still *** review summarizes the current mechanistic understanding of CL materials including organic/inorganic small molecules,and polymers with/without isolated aromatic *** addition,some strategies to achieve high quantum yield,adjustable emission color,and persistent room temperature phosphorescence in CL materials are also *** last,a perspective of the mechanism and application of CL materials are demonstrated,which inspire the researchers working on the development of new kinds of functional materials.

关键词： Clusteroluminescence Clusterization-triggered emission through-space interaction Non-conjugated structure

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STUDY ON THE through-space AND through-BOND interactionS IN TRICYCLO 4,2,2,2 DODECADIENE-1.5

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Journal of Wuhan University of Technology(Materials Science) 1995年第3期10卷 6-13页

作者：刘韩星 WUHAN UNIV TECHNOL RES INST ADV MATWUHAN 430070PEOPLES R CHINA

through-space interactions of pi orbiatl and sigma orbital in molecule tricycle 4,2,2,2,dodecadiene -1.5 were studied by means of DV-X alpha SVF method using a model molecule that consists of two ethylenes with interdeck distance D. The results show the through-space interactions of the title molecule decrease with the increasing of D,the through-space interactions of pi orbital are larger than that of sigma orbital. Furthermore, through-bond interactions of the pi orbtial and sigma orbital were analyzed basing on the calculations of the electronic structure of the title molecule. Both through-space and through-bond interactions are Large and,the net interactions are small. The calculated ionization potential energies of the title molecule which were obtained by transition-state procedure are in good agreement with the PE spectroscopy.

关键词： through-space interaction through-bond interaction tricyclo 4,2,2,2 dodecadinene-1.5

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Synthesis and Properties of a through-space Interacting Diradicaloid

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Precision Chemistry 2023年第3期1卷 183-191页

作者： Takuya Kodama Yasukazu Hirao Takashi Kubo Department of Chemistry Graduate School of ScienceOsaka UniversityToyonakaOsaka 560-0043Japan Innovative Catalysis Science Division Institute for Open and Transdisciplinary Research Initiatives(ICSOTRI)Osaka UniversitySuitaOsaka 565-0871Japan

Knowledge about electronic structures is important to gain an understanding of the unique functional properties of *** this study,we synthesized and characterized a diradicaloid in which two phenalenyl radical sites are coupled antiferromagnetically via a through-space *** results of quantum chemical,physicochemical(^(1)H NMR,electronic absorption,cyclic voltammetry,SQUID,ESR),and chemical reactivity studies show that this diradicaloid has singlet diradical *** assessment of the nature of the bonding interaction between two radical sites in this species using DFT calculations demonstrates that a small spatial overlap between the two SOMOs in this diradicaloid provides an efficient electron exchange path for the singlet state to be substantially lower in energy than the triplet state.

关键词： through-space interaction phenalenyl radical singlet diradical diradicaloid antiferromagnetic interaction

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