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Although perovskite oxides hold promise in applications ranging from solidoxide fuel cells to catalysts, their surface chemistry is poorly understood atthe molecular level. Here we follow the formation of the first monolayer ofwater at the (001) surfaces of Sr$_{n+1}$Ru$_n$O$_{3n+1}$ ($n$ = 1, 2) usinglow-temperature scanning tunnelling microscopy, X-ray photoelectronspectroscopy, and density functional theory. These layered perovskites cleavebetween neighbouring SrO planes, yielding almost ideal, rocksalt-like surfaces.An adsorbed monomer dissociates and forms a pair of hydroxide ions. The OHstemming from the original molecule stays trapped at Sr-Sr bridge positions,circling the surface OH with a measured activation energy of 187 $\pm$ 10 meV.At higher coverage, dimers of dissociated water assemble into one-dimensionalchains and form a percolating network where water adsorbs molecularly in thegaps. Our work shows the limitations of applying surface chemistry conceptsderived for binary rocksalt oxides to perovskites.

Adsorption of water at the SrO surface of ruthenates