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Against expectations, robust switchable ferroelectricity has been recentlyobserved in ultrathin (1 nm) ferroelectric films exposed to air [V. Garcia $et$$al.$, Nature {\bf 460}, 81 (2009)]. Based on first-principles calculations, weshow that the system does not polarize unless charged defects or adsorbatesform at the surface. We propose electrochemical processes as the most likelyorigin of this charge. The ferroelectric polarization of the film adapts to thebound charge generated on its surface by redox processes when poling the film.This, in turn, alters the band alignment at the bottom electrode interface,explaining the observed tunneling electroresistance. Our conclusions aresupported by energetics calculated for varied electrochemical scenarios.

Electrochemical ferroelectric switching: The origin of polarization reversal in ultrathin films