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However, so far, surprisingly few cases of non\u2010fluorescent MPM probes have been\u00a0reported, and their imaging performances are relatively limited. Herein, this study introduces a highly efficient third harmonic generation (THG) probe based on semiconducting oligomer derivatives (BTICs), which exhibit strong THG responses under NIR\u2010IIb (1700\u00a0nm) excitation. Leveraging halogen chemistry, semiconducting oligomers with varying halogen substitutions and nanoparticles (NPs)\u00a0exhibit unexpectedly high THG performance across different aggregation states upon NIR\u2010IIb excitation. The BTICs NPs exhibit a large THG conversion efficiency (1215\u00a0\u00d7\u00a010\n                    <jats:sup>\u221284<\/jats:sup>\n                    cm\n                    <jats:sup>6<\/jats:sup>\n                    s\n                    <jats:sup>2<\/jats:sup>\n                    photon\n                    <jats:sup>\u22122<\/jats:sup>\n                    ) and exceptional resistance to photobleaching. Furthermore, the biocompatibility and in vivo THG angiography capabilities of BTICs NPs are validated, achieving the visualisation of deep\u2010brain vasculature with unprecedented spatial resolution at a record\u2010high imaging depth of 1745\u00a0\u00b5m. The pioneering exploitation of semiconducting oligomer\u2010based THG probes establishes a new class of high\u2010performance materials, enabling ultra\u2010deep THG imaging of the\u00a0brain and advancing the design of next\u2010generation THG imaging platforms.\n                  <\/jats:p>","DOI":"10.1002\/adma.202417085","type":"journal-article","created":{"date-parts":[[2025,5,27]],"date-time":"2025-05-27T03:41:43Z","timestamp":1748317303000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Rational Design of Semiconducting Oligomer for Third Harmonic Generation Bioimaging of Ultradeep Brain Imaging with NIR\u2010IIb Excitation"],"prefix":"10.1002","volume":"37","author":[{"given":"Qi","family":"Zhao","sequence":"first","affiliation":[{"name":"College of Pharmaceutical Sciences Soochow University  Suzhou 215123 P. R. 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