中文摘要：

采用含时密度泛函理论与响应函数理论相结合的方法,研究了两种实验室新合成的水溶性双光子荧光次氯酸根（ClO-）探针分子HCH和HCM的单光子吸收、双光子吸收和荧光发射性质。计算结果表明,HCH和HCM分子与ClO-反应后,生成物的光吸收和光发射性质均发生明显变化,相应的吸收和发射峰位都发生了明显蓝移,荧光强度展现出明显的增强。另外,两探针分子都具有较大的双光子吸收截面,且与ClO-反应后,生成物的双光子吸收截面值显著增加,因此两分子均可作为性能优良的双光子荧光探针分子。此外,通过分析HCH和HCM分子与ClO-反应前后的Mulliken电荷布居情况,从理论上证实了该系列荧光探针分子的识别机理是C=N异构化。

英文摘要：

The one- and two-photon absorption and emission properties of the two newly synthesized watersoluble two-photon fluorescent probes （HCH and HCM） for the detection of CIO were investigated using time- dependent density functional theory in combination with response theory. Dramatic changes in the photophysical properties of the molecules following reaction with CIO- were predicted. The photoabsorption and photoemission peaks for both compounds were clearly blue shifted, while the emission intensities were enhanced. Both probes were also found to have large two-photon cross sections. Importantly, in the presence of CIO- the two-photon cross section of the molecules increased significantly, which indicated that both HCH and HCM should be good two-photon fluorescent probes for sensing CIO-. The responsive mechanism of the probes was explored by analyzing the molecular Mulliken charge population, which was attributed to C=N isomedzation.