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Deciphering Oxygen-Independent Augmented Photodynamic Oncotherapy by Facilitating the Separation of Electron-Hole Pairs |
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| Authors: | Dr. Xiaoming Hu Dr. Zhuting Fang Fengwei Sun Caijun Zhu Mingxuan Jia Dr. Xiaofei Miao Dr. Lingting Huang Prof. Wenbo Hu Prof. Quli Fan Prof. Zhen Yang Prof. Wei Huang |
| Affiliation: | 1. Strait Institute of Flexible Electronics (SIFE, Future Technologies), Fujian Key Laboratory of Flexible Electronics, Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE), Fuzhou, 350117 China Jiangxi Key Laboratory of Nanobiomaterials, School of Materials Science and Engineering, East China Jiaotong University, Nanchang, 330013 China State Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM), Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China These authors contributed equally to this work.;2. Department of Interventional Radiology, Fujian Provincial Hospital, Shengli Clinical Medical College of Fujian Medical University, No. 134, Dongjie Road, Fuzhou, 350001 China These authors contributed equally to this work.;3. Strait Institute of Flexible Electronics (SIFE, Future Technologies), Fujian Key Laboratory of Flexible Electronics, Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE), Fuzhou, 350117 China;4. Jiangxi Key Laboratory of Nanobiomaterials, School of Materials Science and Engineering, East China Jiaotong University, Nanchang, 330013 China;5. Frontiers Science Center for Flexible Electronics, Xi'an Institute of Flexible Electronics (IFE), Northwestern Polytechnical University, Xi'an, 710072 China;6. State Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM), Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China |
| Abstract: | Developing Type-I photosensitizers provides an attractive approach to solve the dilemma of inadequate efficacy of photodynamic therapy (PDT) caused by the inherent oxygen consumption of traditional Type-II PDT and anoxic tumor microenvironment. The challenge for the exploration of Type-I PSs is to facilitate the electron transfer ability of photosensitization molecules for transforming oxygen or H2O to reactive oxygen species (ROS). Herein, we propose an electronic acceptor-triggered photoinduced electron transfer (a-PET) strategy promoting the separation of electron-hole pairs by marriage of two organic semiconducting molecules of a non-fullerene scaffold-based photosensitizer and a perylene diimide that significantly boost the Type-I PDT pathway to produce plentiful ROS, especially, inducing 3.5-fold and 2.5-fold amplification of hydroxyl (OH⋅) and superoxide (O2−⋅) generation. Systematic mechanism exploration reveals that intermolecular electron transfer and intramolecular charge separation after photoirradiation generate a competent production of radical ion pairs that promote the Type-I PDT process by theoretical calculation and ultrafast femtosecond transient absorption (fs-TA) spectroscopy. By complementary tumor diagnosis with photoacoustic imaging and second near-infrared fluorescence imaging, this as-prepared nanoplatform exhibits fabulous photocytotoxicity in harsh hypoxic conditions and terrific cancer revoked abilities in living mice. We envision that this work will broaden the insight into high-efficiency Type-I PDT for cancer phototheranostics. |
| Keywords: | organic semiconducting phototheranostics photodynamic therapy Type-I photosensitizer intermolecular electron transfer NIR-II fluorophores |