Bridge-Mediated Charge Separation in Isomeric N-Annulated Perylene Diimide Dimers

doi:10.1021/jacs.9b05723

CORC > 化学研究所 > 中国科学院化学研究所

	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
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2019-08-14
卷号	141 期号:32 页码:12789-12796
ISSN号	0002-7863
DOI	10.1021/jacs.9b05723
英文摘要	The 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.
语种	英语
WOS记录号	WOS:000481563500046
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/82664]
专题	中国科学院化学研究所
作者单位	Chinese Acad Sci, Inst Chem, Beijing 100190, Peoples R China
推荐引用方式 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.