Exploring the polarization degrees of freedom in collinear two-dimensional infrared spectroscopy

We exploit the polarization degrees of freedom in order to optimize interferometer-based 2D-IR spectroscopy in the pump-probe geometry. Signals can be amplified, scattering background can be fully eliminated and intramolecular angles can be determined with improved accuracy. Simple manipulation of the polarization of all four fields gives direct access to individual tensor elements and dispersive signals.