At temperatures between 100 and 110 K, exposing the (100) face of NaCl to unsaturated SO2 gas yields a stable adlayer. infrared spectra of adsorbed SO2 contain complex resonances near the origins of the molecular symmetric and asymmetric stretching vibrations. On photometric grounds the absolute coverage of the surface is found to be one molecule per exposed Na+Cl- ion pair. The spectra of this monolayer consist of several sharp lines overlapping one broad feature for each molecular mode. By comparison to vibrational excitons in simpler systems, the coexistence of crystalline and amorphous adlayer structures is strongly indicated. This partial ordering is pressure dependent, and develops spontaneously on a time scale of minutes. The disordered component, in contrast, is never in equilibrium with the gas phase. Computational simulations have detailed the microscopic basis of this behavior, Accurate ab initio models of the SO2 molecule and NaCl(100) surface were used in a Monte Carlo simulation of the experimental conditions. At both half and full coverage, an amorphous two-dimensional condensate developed. This is minimally consistent with the polarized infrared photometry. Seemingly equilibrated Monte Carlo runs retained some memory of the initial molecular configuration, again consistent with hysteresis observed in the spectroscopic experiments. No structural order developed in the simulations, but the energetic state of affairs was clarified : the potential driving adsorption and condensation is deep in comparison to available thermal energy, but relatively insensitive to molecular orientation.