From Ultrafast Structure Determination to Steering Reactions: Mixed IR/Non-IR Multidimensional Vibrational Spectroscopies.

摘要: Ultrafast multidimensional infrared spectroscopy is a powerful method for resolving features of molecular structure and dynamics that are difficult or impossible to address with linear spectroscopy. Augmenting the IR pulse sequences by resonant nonresonant UV, Vis, NIR pulses considerably extends range application creates techniques possibilities far beyond pure experiment. These include surface-specific 2D-IR sub-monolayer sensitivity, ultrafast determination in non-equilibrium systems, triggered exchange correlate reactant product bands, exploring interplay electronic nuclear degrees freedom, investigation interactions between Raman- IR-active modes, imaging chemical contrast, sub-ensemble-selective photochemistry, even steering reaction selective excitation. We give an overview useful mixed IR/non-IR sequences, discuss their differences, illustrate potential.