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Notes: The cosmic ray simulator consists of a 50 l cylindrical stainless steel chamber. A rotable cold finger milled of a silver (111) monocrystal optimizes heat conductivity and is connected to a programmable, closed cycle helium refrigerator allowing temperature control of an attached silver wafer between 10 and 340 K (±0.5 K). Oil-free ultrahigh vacuum (UHV) conditions of ≈10−10 mbar are provided by a membrane, drag, and cryopump, hence guaranteeing a vacuum system free of any contamination. Ice layers of defined crystal structures and reproducible thickness of (5±1) μm are achieved by depositing gases, e.g., CH4, CD4, CD4/O2, and CH4/O2, with a computer-assisted thermovalve on the cooled wafer. These frosts are irradiated at 10 and 50 K with 7.3 MeV protons and 9 MeV α particles of the compact cyclotron CV28 in Forschungszentrum Jülich up to doses of 150 eV per molecule, i.e., simulating the distribution maximum of galactic cosmic ray particles interacting with primordial matter in space during 0.7×109 yr. During the experiments, gas phase and solid state are monitored for the first time quantitatively on line and in situ by a quadrupole mass spectrometer (QMS) via matrix interval arithmetic and a Fourier transform infrared spectrometer (FTIR) in an absorption-reflection mode at 62.5°.For the first time, a cosmic ray simulator allows detailed and reproducible mechanistic studies on the interaction of cosmic ray particles with frozen gases in space based on pressure conditions (hydrocarbon free UHV conditions, the limitation of condensations of residual gases during an experiment to less than one monolayer), temperature regime (the use of silver monocrystals, FTIR in reflection, optimized ion currents, and target thicknesses 〈5 μm restrict temperature increasing to 14 K), and defined target systems. In combination with two on line and in situ analyses techniques, i.e., FTIR and QMS, the machine yields unprecedented options such as computing the heating of the ice surfaces directly exposed to the ion beam by a calibrated QMS and a complete quantification of product distribution. Preliminary results indicate a strong temperature-dependent component of the reaction mechanisms in the frosts: surface layers are heated by impinging ions to (14±1) K and yield (70%–100%) of higher molecular weight species, such as C11D24, whereas 10 K regions produce majority of simpler hydrocarbons, e.g., C3D8. Second, O2 contaminations influence the experiments dramatically by trapping of diffusive H atoms as O2H and, thus, yield oxygen-containing yellow to brown residues after heating to 293 K. Irradiation of pure methane targets, however, produce no residues. But an increasing concentration of H atoms exceeding (6%±3%) leads to ejection of up to 90% of the frosts into vacuum. © 1995 American Institute of Physics.