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Bridge-Mediated Charge Separation in Isomeric N-Annulated Perylene Diimide Dimers
Guo, Yuanyuan; Ma, Zetong; Niu, Xinmiao; Zhang, Wei; Tao, Min; Guo, Qianjin; Wang, Zhaohui; Xia, Andong
2019-08-14
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume141Issue:32Pages:12789-12796
AbstractThe possibility and rate of charge separation (CS) in donor-bridge-acceptor molecules mainly depend on two factors: electronic coupling and solvent effects. The question of how CS occurred in two identical chromophores is fundamental, as it is particularly interesting for potential molecular electronics applications and the photosynthetic reaction centers (RCs). Conjugated bridge definitely plays a crucial role in electronic coupling. To determine the bridge-mediated charge separation dynamics between the two identical chromophores, the isomeric N-annulated perylene diimide dimers (para-BDNP and meta-BDNP) with different conjugated bridge structures have been comparatively investigated in different solvents using femtosecond transient absorption spectra (fs-TA). It is found that the charge separation is disfavored in weak polar solvent, whereas direct spectroscopic signatures of radicals are observed in polar solvents, and the rate of charge separation increases as the solvent polarity increasing. To our surprise, the rate of charge separation in m-BDNP is more than an order of magnitude slower than that in p-BDNP, although there is a larger negative Delta G(CS) in m-BDNP. The slow CS rate that occurred in m-BDNP mainly results from the intrinsic destructive interference of the wave function through the meta-substituted bridge. The roles of solvent effects in free energy and electronic coupling for charge separation are further identified with quantum calculations.
DOI10.1021/jacs.9b05723
Indexed BySCI
Language英语
WOS IDWOS:000481563500046
EI Accession Number1520-5126
Citation statistics
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/82664
Collection中国科学院化学研究所
AffiliationChinese Acad Sci, Inst Chem, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
Guo, Yuanyuan,Ma, Zetong,Niu, Xinmiao,et al. Bridge-Mediated Charge Separation in Isomeric N-Annulated Perylene Diimide Dimers[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(32):12789-12796.
APA Guo, Yuanyuan.,Ma, Zetong.,Niu, Xinmiao.,Zhang, Wei.,Tao, Min.,...&Xia, Andong.(2019).Bridge-Mediated Charge Separation in Isomeric N-Annulated Perylene Diimide Dimers.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(32),12789-12796.
MLA Guo, Yuanyuan,et al."Bridge-Mediated Charge Separation in Isomeric N-Annulated Perylene Diimide Dimers".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.32(2019):12789-12796.
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