Departamento de Química Física, Sección de Químicas, Facultad del Medio Ambiente and INAMOL, Universidad de Castilla-La Mancha, Carlos III S/N 45071 Toledo, Spain.
J Am Chem Soc. 2010 Apr 21;132(15):5507-14. doi: 10.1021/ja100771j.
Exploring the interactions of molecules with silica-based mesoporous and nanoparticle materials at the atomic level and understanding of the forces that govern such H-bonds and electrostatic interactions are of fundamental importance to nanocatalysis, nanomedicine, and nanophotonics. In our approach, we studied in single-molecule time and spectral domains a proton-transfer chromophore complexed (by diffusion) and covalently bonded to MCM-41 mesoporous nanomaterial and silica particles. The results reveal strong dependence of the distribution and behavior of the interacting single molecule with the nanopores on the mode of sample preparation and nature of the involved interaction. The change at the single molecule level results in an up to 126 nm (approximately 4650 cm(-1)) spectral shift (from 462 to 588 nm) and almost two times longer lifetime. Furthermore, a change in the electronic charges of the mesoporous framework results in significant narrowing in the emission band of the guest. The results are explained in terms of electronic nanoconfinement but at a single-molecular level.
探索分子与基于二氧化硅的介孔和纳米颗粒材料在原子水平上的相互作用，了解控制氢键和静电相互作用的力，对于纳米催化、纳米医学和纳米光子学至关重要。在我们的方法中，我们在单分子时间和光谱域中研究了通过扩散配位并通过共价键合到 MCM-41 介孔纳米材料和二氧化硅颗粒上的质子转移发色团复合物。结果表明，与纳米孔相互作用的单个分子的分布和行为强烈依赖于样品制备方式和涉及的相互作用的性质。单分子水平的变化导致光谱位移高达 126nm（约 4650cm-1）（从 462nm 到 588nm），寿命延长近两倍。此外，介孔骨架的电子电荷的变化导致客体的发射带显著变窄。结果根据电子纳米限制来解释，但在单分子水平上。
