Rotational and vibrational pattern interpretation for high-resolution coherent 3D spectroscopy.

High-resolution coherent multidimensional spectroscopy provides an alternative to conventional methods for generating rotationally resolved electronic spectra of gas phase molecules. In addition to revealing information such as the relationships among peaks, it can provide clearly recognizable patterns for spectra that otherwise appear patternless due to rotational congestion. Despite this improvement, high-resolution coherent 2D spectroscopy can still exhibit congestion problems; expansion to the second dimension is often not sufficient to prevent overlapping of peaks from different patterns.

High-resolution coherent three-dimensional spectroscopy of Br2.

In the past, high-resolution spectroscopy has been limited to small, simple molecules that yield relatively uncongested spectra. Larger and more complex molecules have a higher density of peaks and are susceptible to complications (e.g.