Electronic Couplings for Singlet Oxygen Photosensitization and Its Molecular Orbital Overlap Description  

光敏化反应生成单线态氧的电子耦合计算及共分子轨道重叠描述

作　　者：Jiaying Chen Tongmei Ma Shuming Bai Qiang Shi 陈嘉颖;马彤梅;白书明;史强(华南理工大学化学与化工学院,广州510641;中国科学院化学研究所分子动态与稳态结构国家重点实验室,北京分子科学国家研究中心,北京100190;中国科学院大学,北京100049;怀柔综合性国家科学中心物质科学实验室,北京101407)

机构地区：[1]School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510641,China [2]Beijing National Laboratory for Molecular Sciences,State Key Laboratory for Structural Chemistry of Unstable and Stable Species,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China [3]University of Chinese Academy of Sciences,Beijing 100049,China [4]Physical Science Laboratory,Huairou National Comprehensive Science Center,Beijing 101407,China

出　　处：《Chinese Journal of Chemical Physics》2022年第1期219-226,I0058-I0061,I0065,共13页化学物理学报（英文）

基　　金：the supports from the Chinese Academy of Sciences(CAS);Institute of Chemistry,CAS;the supports from the National Natural Science Foundation of China(No.21933011);the Beijing Municipal Science&Technology Commission(No.Z191100007219009);the K.C.Wong Education Foundation;the support from the National Natural Science Foundation of China(No.21773073)。

摘　　要：The reaction of triplet fusion,also named triplet-triplet annihilation,has attracted a lot of research interests because of its wide applications in photocatalytic,solar cells,and bioimaging.As for the singlet oxygen photosensitization,the reactive singlet oxygen species are generated through the energy transfers from photosensitizer(PS)to ground triplet oxygen molecule.In this work,we computed the electronic coupling for singlet oxygen photosensitization using the nonadiabatic coupling from the quantum chemical calculation.Then we utilized the molecular orbital(MO)overlaps to approximate it,where the MOs were computed from isolated single molecules.As demonstrated with quantitative results,this approach well describes the distribution of the coupling strength as the function of the intermolecular distance between the sensitizer and O_(2),providing us a simple but effective way to predict the coupling of triplet fusion reactions.

关 键 词：Triplet fusion Singlet oxygen PHOTOSENSITIZATION Electronic coupling Molecular orbital overlap 

分 类 号：O641.122[理学—物理化学]