Conformational Folding Activates Photoinduced Electron Transfer  

作　　者：Shiqing Huang Syed Ali Abbas Abedi Zhifeng Li Rongrong Huang Xiaoyu Yan Mohammad Izadyar Qinglong Qiao Yu Fang Zhaochao Xu Xiaogang Liu 

机构地区：[1]Fluorescence Research Group,Singapore University of Technology and Design,Singapore 487372 [2]School of Chemistry and Life Resources,Renmin University of China,Beijing 100872 [3]CAS Key Laboratory of Separation Science for Analytical Chemistry,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023 [4]Research Center for Modeling and Computational Sciences,Faculty of Science,Ferdowsi University of Mashhad,Mashhad 9177948974 [5]Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),School of Chemistry and Chemical Engineering,Shaanxi Normal University,Xi’an,Shaanxi 710119

出　　处：《CCS Chemistry》2024年第11期2804-2813,共10页中国化学会会刊（英文）

基　　金：supported by the Ministry of Education,Singapore(MOE-T2EP10222-0001);the Singapore University of Technology and Design(SUTD)Kickstarter Initiative(No.SKI 2021_04_09);the National Natural Science Foundation of China(22225806,22078314,22278394,and 22378385);the Dalian Institute of Chemical Physics(DICPI202142 and DICPI202436).

摘　　要：Photoinduced electron transfer(PET)is a critical process in many functional materials,underpinning various technological applications(i.e.,fluorescent probes and photocatalysts).Despite its signifi-cance,the detailed structural dynamics of PET,particularly during the excited state,remain poorly understood.This study investigates the mechanisms of conformational folding and their implications for activating PET in molecular systems characterized by a fluorophore-spacer-receptor configuration.We demonstrate that traditional computational models,primarily based on frontier molecular orbitals,often fall short in capturing these conformational dynamics,leading to inadequate explanations of PET phenomena.With the incorporation of conformational folding,our computational model has achieved excellent agreement with experimental data,thereby resolving several long-standing debates on PET mechanisms.This mechanistic advancement not only deepens our understanding of PET but also opens new avenues for designing advanced functional materials.We have thus successfully demonstrated the imaging of lysosomes in live cells using a PET probe.

关 键 词：Photoinduced electron transfer conformational folding BIOIMAGING excited-state dynamics advanced materials 

分 类 号：O64[理学—物理化学]