Publication Details (including relevant citation information):
Garrett-Roe, S. and Hamm, P. J. Chem. Phys. 130, 164510 (2009).
We demonstrate a method to collect purely absorptive three-dimensional fifth-order vibrational spectra (3D-IR) on the model system CO2 in H2O. The 6 beam interferometer is described, as well as a method to experimentally determine the phase of the 3D spectrum. The measured spectra agree very well with simulations of the data based on the cumulant expansion. There are five peaks corresponding to different paths up and down the vibrational ladder; their positions, signs, and amplitudes agree with theoretical predictions. Based on the agreement between the simulations and measurements, we conclude that cascaded lower order signals contribute negligibly to the observed signal.
Address (URL): http://dx.doi.org/10.1063/1.3122982