The third-order Raman spectrum of argon pairs

Abstract

The third-order susceptibility of binary complexes of argon atoms, and hence the associated Raman spectra of bound pairs Ar₂ (‘van der Waals molecule’), and of free pairs Ar-Ar in collisional interaction (‘collision-induced Raman spectra’), which are inseparable in an actual measurement, are computed. The computations show that optical heterodyne Raman induced Kerr effect spectroscopy OHD-RIKES) offers sufficient sensitivity to obtain well-resolved rotational dimer spectra even at temperatures as high as 300 K.