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However, low luminescence efficiency and short emission wavelength limit their development. This work designs three luminogens with CL properties (CLgens) by introducing <jats:italic>n<\/jats:italic>\u2010electron\u2010involved through\u2010space conjugation (TSC) into diarylmethane. Apart from single\u2010photon excited long\u2010wavelength (686\u2005nm) and high\u2010efficiency (29\u2009%) CL, two\u2010photon clusteroluminescence (TPCL) is successfully achieved in such small luminogens with only two isolated heteroatomic units. TSC stabilized in the aggregate state has been proven to realize efficient spatial electron delocalization similar to conventionally conjugated compounds. Encouraged by the excellent TPCL properties, two\u2010photon imaging of blood vessels in vivo and biocompatibility verification utilizing CLgens are also achieved. This work illustrates the essential role of TSC in promoting nonlinear optical properties of CLgens and may facilitate further design and development of the next generation of bioprobes with excellent biocompatibility.<\/jats:p>","DOI":"10.1002\/anie.202413751","type":"journal-article","created":{"date-parts":[[2024,8,28]],"date-time":"2024-08-28T02:05:11Z","timestamp":1724810711000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Two\u2010Photon Clusteroluminescence Enabled by Through\u2010Space Conjugation for In Vivo Bioimaging"],"prefix":"10.1002","volume":"64","author":[{"given":"Jianyu","family":"Zhang","sequence":"first","affiliation":[{"name":"MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou 3100587 China"},{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology Clear Water Bay  Kowloon Hong Kong 999077 China"},{"name":"Present address: Stratingh Institute for Chemistry University of Groningen  Groningen 9747 AG, The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hanchen","family":"Shen","sequence":"additional","affiliation":[{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology Clear Water Bay  Kowloon Hong Kong 999077 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zuping","family":"Xiong","sequence":"additional","affiliation":[{"name":"MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou 3100587 China"},{"name":"Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University  Hangzhou 311215 China"},{"name":"Centre of Healthcare Materials Shaoxing Institute Zhejiang University  Shaoxing 312000 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lidong","family":"Du","sequence":"additional","affiliation":[{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology Clear Water Bay  Kowloon Hong Kong 999077 China"},{"name":"MOE Frontiers Science Center for Precision Oncology Faculty of Health Sciences University of Macau  Macao 999078 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Moxin","family":"Li","sequence":"additional","affiliation":[{"name":"MOE Frontiers Science Center for Precision Oncology Faculty of Health Sciences University of Macau  Macao 999078 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinwen","family":"Ou","sequence":"additional","affiliation":[{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology Clear Water Bay  Kowloon Hong Kong 999077 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyan","family":"Zhu","sequence":"additional","affiliation":[{"name":"Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology Clear Water Bay  Kowloon Hong Kong 999077 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jacky W. 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