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Photophysical Property of Photoactive Molecules with Multibranched Push-Pull Structures
Ying-ying Wang,Xiao-nan Ma,Silvije Vdovi?,Lin-yin Yan,Xue-fei Wang,Qian-jin Guo,An-dong Xia*
Author NameAffiliationE-mail
Ying-ying Wang The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China  
Xiao-nan Ma The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China  
Silvije Vdovi? The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China  
Lin-yin Yan The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China  
Xue-fei Wang The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China  
Qian-jin Guo The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China  
An-dong Xia* The State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China andong@iccas.ac.cn 
Abstract:
The structure-property characteristics of a series of newly synthesized intramolecular charge-transfer (ICT) compounds, single-branch monomer with triphenylmethane as electron donor and 2,1,3-benzothiadiazole as acceptor, the corresponding two-branch dimer and three-branch trimer, have been investigated by means of steady-state and femtosecond time-resolved stimulated emission fluorescence depletion (FS TR-SEP FD) techniques in different polar solvents. The TD-DFT calculations are further performed to explain the observed ICT properties. The interpretation of the experimental results is based on the comparative stud-ies of the series of compounds which have increased amount of identical branch moiety. The similarity of the absorption and fluorescence spectra as well as strong solvent-dependence of the spectral properties for the three compounds reveal that the excited state of the dimer and trimer are nearly the same with that of the monomer, which may localize on one branch. It is found that polar excited state emerged through multidimensional intramolecular charge transfer from the donating moiety to the acceptor upon excitation, and quickly relaxed to one branch before emission. Even so, the red-shift in the absorption and emission spectra and decreased fluorescence radiative lifetime with respect to their monomer counterpart still suggest some extent delocalization of excited state in the dimer and trimer upon excitation. The similar behavior of their excited ICT state is demonstrated by FS TR-SEP FD mea-surements, and shows that the trimer has the largest charge-separate extent in all studied three samples. Finally, steady-state excitation anisotropy measurements has further been carried out to estimate the nature of the optical excitation and the mechanism of energy redistribution among the branches, where no plateau through the ICT band suggests the intramolecular excitation transfer process between the branches in dimer and trimer.
Key words:  Branched intramolecular charge transfer molecule, Fluorescence decay, Fem-tosecond time-resolved stimulated emission fluorescence depletion, Steady-state excitation anisotropy
FundProject:
具有电子推拉结构的多支化分子的光物理特性的研究
王营营,马骁楠,Silvije Vdovi?,阎林胤,王雪飞,郭前进,夏安东*
摘要:
利用稳态光谱和飞秒时间分辨荧光亏蚀的技术,研究了不同溶剂中一系列有分子内电荷转移特性的分子的结构与光物理性质的关系,研究体系为三苯胺作为电子给体,2,1,3-苯并噻二唑作为受体的单支分子及其对应的两支和三支分子. 并结合TD-DFT计算进一步解释了实验中所观察到的现象. 三个分子相似的吸收和荧光光谱以及强的溶剂依赖光谱特性表明两支与三支分子激发态与单支分子相似,表明激发态都定域在其中一支上. 激发时多支分子内发生多维电荷转移,然后快速地定域到某一支上发射. 另一方面多支分子相对于单支分子吸收和发射光谱的红
关键词:  多支化分子内电荷转移,荧光衰减,飞秒时间分辨荧光亏蚀,稳态激发各向异性
DOI:10.1088/1674-0068/24/05/563-571
分类号: