Abstract
A theory is presented to describe the effect of angle- and position-dependent intermolecular forces on the rotation-vibration correlation in infrared and anisotropic Raman spectra of diluted van der Waals solutions. The correlation functions are presented in the form of a series. Its leading term is the simple product of rotational and vibrational correlation functions, whereas its higher-order terms give successive corrections to this simple approximation. The corresponding spectral densities are discussed. The coupling effects predicted by the theory are different in infrared and in anisotropic Raman.