The Multiresonant Family of Coherent Multidimensional Laser Spectroscopy- Examples in Vibrational Spectroscopy and Quantum Confined Nanostructures

John C. Wright

Department of Chemistry, University of Wisconsin, Madison, WI 53706

The discovery of optical analogues of multidimensional NMR that use phase matching and phase cycling has opened the new field of coherent multidimensional spectroscopy (CMDS). In analogy to NMR, the full power of this field rests on the ability to create and manipulate multiple quantum coherences (MQCs) between a wide variety of electronic and vibrational states. MQCs are formed by exciting multiple quantum states quickly enough to insure that the quantum mechanical phase oscillations of each state are maintained and reemit beams of light at all of the frequency differences between the states composing the MQCs. MQCs are only formed between states that are coupled so excitation of one affects all of the others. Multiresonant CMDS is a particularly interesting approach because it is a frequency domain method that only requires phase coherence between the excitation beams during the creation of the MQCs. That freedom allows the use of different excitation frequencies to create MQCs containing any mixture of electronic and vibrational states. This approach provides enhanced multidimensional resolution, line narrowing, isolation of coupled states, elimination of background, and coherent and incoherent dynamics. This talk will show examples of how the different multiresonant methods are used to resolve individual vibrational and electronic quantum states and their dynamics in molecular spectroscopy and nanostructure applications.