Scuola Normale Superiore di Pisa, Piazza dei Cavalieri 7, 56100 Pisa, Italy.
Phys Chem Chem Phys. 2010 Jul 28;12(28):8016-23. doi: 10.1039/b927489h. Epub 2010 Jun 3.
Using a time-dependent density functional theory approach and taking into account bulk solvent effects, we investigate the absorption and fluorescence spectra of Nile Red. In particular, we have assessed both the planar and twisted intramolecular charge transfer mechanism by using a panel of exchange correlation functionals including both global and range-separated hybrids, refined solvent models and the simulation of vibronic couplings. It turned out that the appropriate choice of the functional is of prime importance to obtain, not only quantitatively accurate values, but also qualitatively correct evolution of the spectral features with respect to the dihedral angles of the amino group. At the light of this study, the interpretation of the experimental data is critically re-examined and compared to typical dual-fluorescent molecules.
我们采用含时密度泛函理论方法并考虑体相溶剂效应，研究了尼罗红的吸收和荧光光谱。特别地，我们通过使用一系列交换相关泛函（包括全局和范围分离混合泛函、改进的溶剂模型和振子耦合的模拟）评估了平面和扭曲的分子内电荷转移机制。结果表明，选择合适的泛函对于获得不仅定量准确而且在氨基二面角方面定性正确的光谱特征演化是至关重要的。基于这项研究，我们对实验数据的解释进行了批判性的重新检查，并与典型的双荧光分子进行了比较。
