School of Biological Engineering, Dalian Polytechnic University, Dalian 116034, P. R. China.
Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Qingdao 266237, P. R. China.
J Phys Chem A. 2021 Apr 15;125(14):2866-2875. doi: 10.1021/acs.jpca.1c00108. Epub 2021 Apr 6.
This study investigates the fluorescence quenching mechanism of formaldehyde detection probe Naph1 and its contrast probe Naph3 in water samples and discussed the effect of the electron-donating group and electron-withdrawing group on fluorescence characteristics based on density functional theory (DFT) and time-dependent density functional theory (TD-DFT). We optimized the structures of the four probes Naph1, Naph1-S, Naph3, and Naph3-S (Scheme 1) and calculated the absorption and emission spectra, which were in good agreement with the experiment. Frontier molecular orbitals (FMOs) were used to analyze the charge arrangement in the excited state. To investigate the intramolecular proton transfer (ESIPT) phenomenon, a potential energy curve was constructed. The amount of fragment charge transfer was analyzed by the IFCT method, and then it was determined whether there was an intramolecular charge transfer (ICT) process. It was found that there was an ICT process in Naph3. The electronic effect of the functional groups did not determine the ICT characteristics and the fluorescence characteristics of the substance. Furthermore, the spin-orbit coupling (SOC) constant based on the intersystem crossing (ISC) was supplemented, which showed that the fluorescence quenching of Naph1 and Naph3 was caused by the ISC and the corresponding quenching of Naph3-S was caused by charge transfer (CT) in the excited state.
本研究通过密度泛函理论(DFT)和含时密度泛函理论(TD-DFT),探讨了在水溶液中甲醛检测探针 Naph1 及其对比探针 Naph3 的荧光猝灭机制,并基于此讨论了供电子基团和吸电子基团对荧光特性的影响。我们优化了四种探针 Naph1、Naph1-S、Naph3 和 Naph3-S(方案 1)的结构,并计算了吸收和发射光谱,其与实验结果吻合良好。运用前线分子轨道(FMO)分析了激发态下的电荷排布。为研究分子内质子转移(ESIPT)现象,构建了势能曲线。通过内坐标虚频(IFCT)方法分析了片段电荷转移的数量,进而确定是否存在分子内电荷转移(ICT)过程。结果表明,Naph3 中存在 ICT 过程。官能团的电子效应并不能决定物质的 ICT 特征和荧光特性。此外,补充了基于系间窜越(ISC)的自旋轨道耦合常数(SOC),结果表明,Naph1 和 Naph3 的荧光猝灭是由 ISC 引起的,而相应的 Naph3-S 的猝灭是由激发态下的电荷转移(CT)引起的。