Physical Review Letters 107 255503 (2011)
Hydrogen sulfide (H2S) and hydrogen (H2) crystallize into a ‘guest-host’ structure at 3.5 GPa and, at the initial formation pressure, the rotationally disordered component molecules exhibit weak van der Waals-type interactions. With increasing pressure, hydrogen bonding develops and strengthens between neighboring H2S molecules, reflected in a pronounced drop in S-H vibrational stretching frequency and also observed in first-principles calculations. At 17 GPa, an ordering process occurs where H2S molecules orient themselves to maximize hydrogen bonding and H2 molecules simultaneously occupy a chemically distinct lattice site. Intermolecular forces in the H2S+H2 system may be tuned with pressure from the weak hydrogen-bonding limit to the ordered hydrogen-bonding regime, resulting in a novel clathrate structure stabilized by cooperative interactions.
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