New Line Narrowing Effects in the Infrared Collision-Induced Spectra of Molecular Hydrogens in Liquid Neon

Abstract
The first spectroscopic observation of the relative (solute-solute) diffusion in a fluid environment is reported. New, unusually sharp Q1q(J) lines developing against the diffuse background in the collision-induced fundamental IR bands of hydrogen isotopomers (H2, D2, and HD) dissolved in liquid Ne (T25K) are studied as functions of the solute concentration x. In all cases, the Q1q intensity parabolically scales with x, accompanied by a striking narrowing of the line shapes. The narrowing, as revealed by the pH2 solution studies, is due to a faster growth with x of the sharper solute-solute induced component of the single Q1q(0) line. The latter as well as other observed solute-solute lines are strongly narrowed by fast velocity decorrelations and are signatures of microscopic-scale diffusion. Also, a first observation of the solute-solvent induced JJ+4 transitions is reported.