Design strategies for pulse sequences in multidimensional optical spectroscopies

A unified description of resonant multiple-pulse experiments in coupled spin-1/2 systems in NMR spectroscopy and two-level systems in optical spectroscopy is presented. The connection between the NMR product operator formalism and the Liouville space pathways in optical spectroscopy is established. We show how the information obtained in various strong field two and three pulse NMR experiments can be extracted by combining heterodyne detected phase-controlled weak field signals generated at different directions. These results allow the design of sequences of weak optical pulses that accomplish the same goals as strong field multidimensional NMR spectroscopy. (C) 2001 American Institute of Physics.