Zhang Yujin, Hu Wei
School of Science, Qilu University of Technology, Jinan 250353, China.
Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China.
Materials (Basel). 2017 Jan 25;10(2):108. doi: 10.3390/ma10020108.
Nonlinear optical properties of a series of newly-synthesized molecular fluorescent probes for Hg containing the same acceptor (rhodamine group) are analyzed by using time-dependent density functional theory in combination with analytical response theory. Special emphasis is placed on evolution of the probes' optical properties in the absence and presence of Hg. These compounds show drastic changes in their photoabsorption and photoemission properties when they react with Hg, indicating that they are excellent candidates for ratiometric and colorimetric fluorescent chemosensors. Most importantly, the energy donor moiety is found to play a dominant role in sensing performance of these probes. Two-photon absorption cross sections of the compounds are increased with the presence of Hg, which theoretically suggests the possibility of the probes to be two-photon fluorescent Hg sensors. Moreover, analysis of molecular orbitals is presented to explore responsive mechanism of the probes, where the fluorescence resonant energy transfer process is theoretically demonstrated. Our results elucidate the available experimental measurements. This work provides guidance for designing efficient two-photon fluorescent probes that are geared towards biological and chemical applications.
采用含时密度泛函理论结合解析响应理论，分析了一系列新合成的含相同受体（罗丹明基团）的汞分子荧光探针的非线性光学性质。特别强调了在有无汞存在的情况下探针光学性质的演变。这些化合物与汞反应时，其光吸收和光发射性质发生了剧烈变化，表明它们是比率型和比色型荧光化学传感器的极佳候选物。最重要的是，发现能量供体部分在这些探针的传感性能中起主导作用。化合物的双光子吸收截面随着汞的存在而增加，这在理论上表明了这些探针成为双光子荧光汞传感器的可能性。此外，还对分子轨道进行了分析，以探索探针的响应机制，从理论上证明了荧光共振能量转移过程。我们的结果阐明了可用的实验测量方法。这项工作为设计面向生物和化学应用的高效双光子荧光探针提供了指导。
