A detailed theoretical study on the excited-state hydrogen-bonding dynamics and the proton transfer mechanism for a novel white-light fluorophore

doi:10.1002/jccs.201800045

	A detailed theoretical study on the excited-state hydrogen-bonding dynamics and the proton transfer mechanism for a novel white-light fluorophore
	Yang, Dapeng 1,3; Gao, Haiyan 1; Yang, Guang 2; Jia, Min 1; Song, Xiaoyan 1; Zhang, Qiaoli 1
刊名	JOURNAL OF THE CHINESE CHEMICAL SOCIETY
	2019
卷号	66 期号:1 页码:56-61
关键词	frontier molecular orbital infrared spectra intramolecular hydrogen bond potential energy curves proton transfer
ISSN号	0009-4536
DOI	10.1002/jccs.201800045
通讯作者	Gao, Haiyan(hygao0371@163.com)
英文摘要	In this work, density functional theory (DFT) and time-dependent DFT (TDDFT) methods were used to investigate the excited-state dynamics of the excited-state hydrogen-bonding variations and proton transfer mechanism for a novel white-light fluorophore 2-(4-[dimethylamino]phenyl)-7-hyroxy-6-(3-phenylpropanoyl)-4H-chromen-4-one (1). The methods we adopted could successfully reproduce the experimental electronic spectra, which shows the appropriateness of the theoretical level in this work. Using molecular electrostatic potential (MEP) as well as the reduced density gradient (RDG) versus the product of the sign of the second largest eigenvalue of the electron density Hessian matrix and electron density (sign[(2)]), we demonstrate that an intramolecular hydrogen bond O1-H2O3 should be formed spontaneously in the S-0 state. By analyzing the chemical structures, infrared vibrational spectra, and hydrogen-bonding energies, we confirm that O1-H2O3 should be strengthened in the S-1 state, which reveals the possibility of an excited-state intramolecular proton transfer (ESIPT) process. On investigating the excitation process, we find the S-0 S-1 transition corresponding to the charge transfer, which provides the driving force for ESIPT. By constructing the potential energy curves, we show that the ESIPT reaction results in a dynamic equilibrium in the S-1 state between the forward and backward processes, which facilitates the emission of white light.
资助项目	Key Scientific Research Project of Colleges and Universities of Henan Province of China[16B140002] ; Key Scientific Research Project of Colleges and Universities of Henan Province of China[18A140023] ; Science and Technology Research Project of Henan Province[172102210391] ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China[2014GGJS-283]
WOS关键词	INTRAMOLECULAR CHARGE-TRANSFER ; FLUORESCENCE ; SOLVENT ; SINGLE ; GENERATION ; SOLVATION ; TDDFT
WOS研究方向	Chemistry
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000459598500007
资助机构	Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Science and Technology Research Project of Henan Province ; Science and Technology Research Project of Henan Province ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Science and Technology Research Project of Henan Province ; Science and Technology Research Project of Henan Province ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Science and Technology Research Project of Henan Province ; Science and Technology Research Project of Henan Province ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Key Scientific Research Project of Colleges and Universities of Henan Province of China ; Science and Technology Research Project of Henan Province ; Science and Technology Research Project of Henan Province ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China ; Aid Project for the Mainstay Young Teachers in Henan Provincial Institutions of Higher Education of China
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/166024]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Gao, Haiyan
作者单位	1.North China Univ Water Resources & Elect Power, Sch Math & Stat, Zhengzhou 450046, Henan, Peoples R China 2.Jiaozuo Univ, Basic Teaching Dept, Jiaozuo, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam Theoret & Computat, Dalian, Peoples R China
推荐引用方式 GB/T 7714	Yang, Dapeng,Gao, Haiyan,Yang, Guang,et al. A detailed theoretical study on the excited-state hydrogen-bonding dynamics and the proton transfer mechanism for a novel white-light fluorophore[J]. JOURNAL OF THE CHINESE CHEMICAL SOCIETY,2019,66(1):56-61.
APA	Yang, Dapeng,Gao, Haiyan,Yang, Guang,Jia, Min,Song, Xiaoyan,&Zhang, Qiaoli.(2019).A detailed theoretical study on the excited-state hydrogen-bonding dynamics and the proton transfer mechanism for a novel white-light fluorophore.JOURNAL OF THE CHINESE CHEMICAL SOCIETY,66(1),56-61.
MLA	Yang, Dapeng,et al."A detailed theoretical study on the excited-state hydrogen-bonding dynamics and the proton transfer mechanism for a novel white-light fluorophore".JOURNAL OF THE CHINESE CHEMICAL SOCIETY 66.1(2019):56-61.