Coherent Multi-Dimensional Spectroscopy: Experimental Considerations, Direct Comparisons and New Capabilities


Optical Coherent Multidimensional Spectroscopy (CMDS) has been developed to probe the electronic states of a diverse range of complex systems. The great advantage of CMDS over linear spectroscopy is the ability to separate and quantify different types of interactions. To do this, multiple carefully controlled femtosecond laser pulses drive a non-linear response in the sample. A specific component of this non-linear response is selected and its amplitude and phase measured. There are several challenges for the experimental realization of optical CMDS, yet there have been several different approaches developed, each with their own advantages and limitations. Identifying the best approach then becomes dependent on the sample and the information being sought. Here we review the various experimental considerati