Multidimensional femtosecond correlation spectroscopies of electronic and vibrational excitations.

摘要: Femtosecond visible and infrared analogues of multiple-pulse nuclear magnetic resonance techniques provide novel snapshot probes into the structure electronic vibrational dynamics complex molecular assemblies such as photosynthetic antennae, proteins, hydrogen-bonded liquids. A classical-oscillator description these spectroscopies in terms interacting quasiparticles (rather than transitions among global eigenstates) is developed sets stage for designing new pulse sequences inverting multidimensional signals to yield structures. Considerable computational advantages a clear physical insight origin response relevant coherence sizes are provided by real-space analysis underlying coherence-transfer pathways Liouville space.