Through a series of Raman spectroscopy studies, we investigate the behaviour of hydrogen-helium and hydrogen-nitrogen mixtures at high pressure across wide ranging concentrations. We find that there is no evidence of chemical association, miscibility, nor any demixing of hydrogen and helium in the solid state up to pressures of 250 GPa at 300 K. In contrast, we observe the formation of concentration-dependent N 2 -H 2 van der Waals solids, which react to form N-H bonded compounds above 50 GPa. Through this combined study, we can demonstrate that the recently claimed chemical association of H 2 -He can be attributed to significant N 2 contamination and subsequent formation of N 2 -H 2 compounds.Understanding the behaviour of molecular mixtures under pressure is of a great importance to many scientific fields varying from chemistry to the studies of internal structures of astronomical bodies [1, 3]. A wide range of phenomena have been observed in high-pressure molecular-mixtures such as phase separation, co-crystallisation, host-guest structures and chemical reaction [4][5][6][7]. Since the discovery of solid van der Waals compounds in the highpressure helium-nitrogen system [8], binary mixtures of elemental gasses have attracted much attention. Subsequently, each binary mixture of the four lightest elemental gasses: H 2 , He, N 2 and O 2 have been studied at high pressure [9][10][11][12][13][14][15]. Recently, there has been renewed interest in studies of both the hydrogen-helium and hydrogen-nitrogen systems at high pressure investigating the synthesis of compounds through the reaction of the constituent molecules [1-3, 18, 19].H 2 and helium are predicted to be chemically inert with one another, across a wide P-T and concentration regime [21][22][23][24][25][26]. Theoretical simulations motivated by potential miscibility within the Jovian planets, find evidence that even at these extreme conditions, hydrogen and helium are still phase separated. Due to the theoretical predictions of no chemical reactivity between hydrogen and helium, there have been few experimental studies on mixtures. Early studies exploring the eutectic phase diagram of hydrogen-helium mixtures found that in the two-fluid state the hydrogen intramolecular vibrational mode is markedly redshifted in Herich concentrations, and was explained semiquantitatively by a helium compressional effect.[10] However in the solid state, the two species were shown to be completely immiscible up to 15 GPa. This observation of immiscibility was utilized to grow single crystals of H 2 , and measure the equation of state up to 100 GPa without an observable reaction between the two. [13] A recent high pressure study exploring H 2 -He interactions as a function of mixture concentration, claimed the unprecedented appearance of hydrogen-helium solids at pressures below 75 GPa [1]. Through the appearance of a vibrational Raman band at an approximate frequency to that calculated for the H-He stretch in a linear H-He-F molecule, the authors claim the formation of H-He b...