High Resolution Coherent 2D Spectroscopy

The purpose of this article is to describe recent progress on the use of coherent two-dimensional spectroscopy for investigating the electronic spectroscopy of gas phase molecules. Unlike conventional high resolution spectra where peaks are distributed along a single axis, high resolution coherent 2D spectra reveal informative patterns along two orthogonal frequency domains. The technique can successfully produce these patterns in situations where one-dimensional spectra appear patternless due to complexity and congestion. Molecular spectra that are difficult to analyze because of strongly perturbing effects (e.g., conical intersections) may be studied using this new technique. Several innovations, such as the ability to graphically separate rotational and vibrational information by clustering peaks and the ability to use multiple clusters to overcome spectral congestion help provide high resolution coherent 2D spectroscopy with the ability to analyze spectra that have previously resisted analysis.