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The superconductivity of hydrides under high pressure has attracted a great deal of attention since the recent observation of the superconducting transition at 203 K in strongly compressed H 2 S. It has been realized that the stoichiometry of hydrides might change under high pressure, which is crucial in understanding the superconducting mechanism. In this study, PH 3 was studied to understand its superconducting transition and stoichiometry under high pressure using Raman, IR and X-ray diffraction measurements, as well as theoretical calculations. PH 3 is stable below 11.7 GPa and then it starts to dehydrogenate through two dimerization processes at room temperature and pressures up to 25 GPa. Two resulting phosphorus hydrides, P 2 H 4 and P 4 H 6 , were verified experimentally and can be recovered to ambient pressure. Under further compression above 35 GPa, the P 4 H 6 directly decomposed into elemental phosphorus. Low temperature can greatly hinder polymerization/decomposition under high pressure and retains P 4 H 6 up to at least 205 GPa. The superconductivity transition temperature of P 4 H 6 is predicted to be 67 K at 200 GPa, which agrees with the reported result, suggesting that it might be responsible for superconductivity at higher pressures. Our results clearly show that P 2 H 4 and P 4 H 6 are the only stable P-H compounds between PH 3 and elemental phosphorus, which is helpful for shedding light on the superconducting mechanism.

Stoichiometric evolutions of PH3 under high pressure: implication for high-Tc superconducting hydrides