Two-dimensional IR-spectroscopy: polarization anisotropy effects Original Research Article

The anisotropic properties of the three-pulse heterodyned echo are developed with particular application to the infrared echo spectroscopy of dipeptides. Rotational relaxation processes are considered in the spherical rotor approximation. It is shown that the various Feynman paths involved in reaching the two-dimensional Bohr frequencies can be distinguished by polarization measurements involving the four fields involved in the heterodyned-stimulated echo.