Non-linear density dependence of rotational line-broadening of HCl in dense argon

The rotational far-infrared spectra of HCl in argon at densities between 100 and 480 amagat and T = 162.5 K are presented. The observed density dependence of the width of the different rotational lines is non-linear and differs for high- and low-frequency lines. An Enskog correction to the collision frequency in the dense gas fails to account for the density dependence of the high rotational lines. It is argued that the many-body character of the relaxation mechanism should be taken into account. Comparison with the results of MD calculations on argon indicates that such an approach may explain the observed density dependence.