Electronically Resonant Coherent Multidimensional Vibrational Spectroscopy John C. Wright, Department of Chemistry, University of Wisconsin- Madison Coherent Multidimensional FWM Spectroscopy is performed by tuning three excitation frequencies to molecular transitions that excite transitions from the ground state, g, to either state a or s. The excitations create the coherences indicated by the two letters. Dotted arrows indicate coherence transfer transitions where the thermal bath causes an entanglement of two states to evolve to a different entanglement. The coherences indicated by boxes emit light. The black box arises from purely radiative excitations while the red boxes arise from coherence transfer. The 2a, s coherence emission is forbidden so the coherence transfer emission can dominate. A monochromator can discriminate against the different output frequencies and isolate the a particular set of coherence transfer pathways. Since there are multiple pathways to a given output coherence, the pathways interfere and create modulations when the time delays between the three pulses are changed. The figure to the left shows such modulations. Coherence transfer provides a new way to perform multidimensional spectroscopy and identify coupling between different quantum states. -J. Phys. Chem. 111, 1163 (2007)