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Coupling molecular rigidity and flexibility on fused backbones for NIR-II photothermal conversion
Authors:Yonglin He  Hailiang Liao  Shanzhi Lyu  Xiao-Qi Xu  Zhengke Li  Iain McCulloch  Wan Yue  Yapei Wang
Affiliation:Department of Chemistry, Renmin University of China, Beijing 100872 China.; State Key Laboratory of Optoelectronic Materials and Technologies, Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, Guangzhou Key Laboratory of Flexible Electronic Materials and Wearable Devices, School of Materials Science and Engineering, Sun Yat-Sen University, Guangzhou 510275 China.; Department of Chemistry, University of Oxford, 12 Mansfield Road, Oxford OX1 3TA UK
Abstract:Great attention is being increasingly paid to photothermal conversion in the near-infrared (NIR)-II window (1000–1350 nm), where deeper tissue penetration is favored. To date, only a limited number of organic photothermal polymers and relevant theory have been exploited to direct the molecular design of polymers with highly efficient photothermal conversion, specifically in the NIR-II window. This work proposes a fused backbone structure locked via an intramolecular hydrogen bonding interaction and double bond, which favors molecular planarity and rigidity in the ground state and molecular flexibility in the excited state. Following this proposal, a particular class of NIR-II photothermal polymers are prepared. Their remarkable photothermal conversion efficiency is in good agreement with our strategy of coupling polymeric rigidity and flexibility, which accounts for the improved light absorption on going from the ground state to the excited state and nonradiative emission on going from the excited state to the ground state. It is envisioned that such a concept of coupling polymeric rigidity and flexibility will offer great inspiration for developing NIR-II photothermal polymers with the use of other chromophores.

Low bandgap and large deformation generally conflict each other. This work couples molecular rigidity and flexibility by intramolecular hydrogen bonds and double bonds to achieve NIR-II light absorption and reinforced internal conversion at the same time.
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