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一种新型天然产物槲皮素的激发态分子内质子转移过程的理论研究

Theoretical Study of the ESIPT Process for a New Natural Product Quercetin.

作者信息

Yang Yunfan, Zhao Jinfeng, Li Yongqing

机构信息

Department of Physics, Liaoning University, Shenyang 110036, P. R. China.

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, P. R. China.

出版信息

Sci Rep. 2016 Aug 30;6:32152. doi: 10.1038/srep32152.

Abstract

The investigation of excited-state intramolecular proton transfer (ESIPT) has been carried out via the density functional theory (DFT) and the time-dependent density functional theory (TDDFT) method for natural product quercetin in dichloromethane (DCM) solvent. For distinguishing different types of intramolecular interaction, the reduced density gradient (RDG) function also has been used. In this study, we have clearly clarified the viewpoint that two kinds of tautomeric forms (K1, K2)originated from ESIPT processconsist inthe first electronic excited state (S1). The phenomenon of hydrogen bonding interaction strengtheninghas been proved by comparing the changes of infrared (IR) vibrational spectra and bond parameters of the hydrogen bonding groups in the ground state with that in the first excited state. The frontier molecular orbitals (MOs)provided visual electron density redistribution have further verified the hydrogen bond strengthening mechanism. It should be noted that the ESIPT process of the K2 form is easier to occur than that of the K1 form via observing the potential energy profiles. Furthermore, the RDG isosurfaces has indicated that hydrogen bonding interaction of the K2 form is stronger than that of the K1 formin the S1 state, which is also the reason why the ESIPT process of the K2 form is easier to occur.

摘要

通过密度泛函理论(DFT)和含时密度泛函理论(TDDFT)方法,对天然产物槲皮素在二氯甲烷(DCM)溶剂中的激发态分子内质子转移(ESIPT)进行了研究。为了区分不同类型的分子内相互作用,还使用了约化密度梯度(RDG)函数。在本研究中,我们明确阐明了这样一种观点,即由ESIPT过程产生的两种互变异构形式(K1、K2)存在于第一电子激发态(S1)中。通过比较基态和第一激发态中氢键基团的红外(IR)振动光谱和键参数的变化,证明了氢键相互作用增强的现象。前沿分子轨道(MOs)提供的可视化电子密度重新分布进一步验证了氢键增强机制。需要注意的是,通过观察势能曲线,K2形式的ESIPT过程比K1形式更容易发生。此外,RDG等值面表明,在S1态下,K2形式的氢键相互作用比K1形式更强,这也是K2形式的ESIPT过程更容易发生的原因。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25fd/5004185/6012ae3fc27b/srep32152-f1.jpg

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