Interaction-induced dipole moment of the Ar–H2 dimer: Dependence on the H2 bond length

Abstract

We present ab initio calculations of the interaction-induced dipole moment of the Ar-H2 van der Waals dimer. The primary focus of our calculations is on the H2 bond length dependence of the dipole moment, which determines the intensities of both the collision-induced H2 upsilon = 1 <-- 0 fundamental band in gaseous Ar-H2 mixtures and the dopant-induced H2 upsilon = 1 <-- 0 absorption feature in Ar-doped solid H2 matrices. Our calculations employ large atom-centered basis sets, diffuse bond functions positioned between the two monomers, and a coupled cluster treatment of valence electron correlation; core-valence correlation effects appear to make negligible contributions to the interaction-induced dipole moment for the Ar-H2 configurations considered here.