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At ultrahigh pressure (>110 GPa), H 2 S is converted into a metallic phase that becomes superconducting with a record T c  of approximately 200 K. It has been proposed that the superconducting phase is body‐centered cubic H 3 S (Im   3  ‾   m, a=3.089 Å) resulting from the decomposition reaction 3 H 2 S→2 H 3 S+S. The analogy between H 2 S and H 2 O led us to a very different conclusion. The well‐known dissociation of water into H 3 O +  and OH −  increases by orders of magnitude under pressure. H 2 S is anticipated to behave similarly under pressure, with the dissociation process 2 H 2 S→H 3 S + +SH −  leading to the perovskite structure (SH − )(H 3 S + ). This phase consists of corner‐sharing SH 6  octahedra with SH −  ions at each A site (the centers of the S 8  cubes). DFT calculations show that the perovskite (SH − )(H 3 S + ) is thermodynamically more stable than the Im   3  ‾   m structure of H 3 S, and suggest that the A site hydrogen atoms are most likely fluxional even at T c  .

Structure and Composition of the 200 K‐Superconducting Phase of H 2 S at Ultrahigh Pressure: The Perovskite (SH − )(H 3 S + )