Competing electronic states emerging on polar surfaces.

Reticcioli, Michele; Wang, Zhichang; Schmid, Michael; Wrana, Dominik; Boatner, Lynn A; Diebold, Ulrike; Setvin, Martin; Franchini, Cesare · Nat Commun · 2022

basic_science · Level V

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Abstract

Excess charge on polar surfaces of ionic compounds is commonly described by the two-dimensional electron gas (2DEG) model, a homogeneous distribution of charge, spatially-confined in a few atomic layers. Here, by combining scanning probe microscopy with density functional theory calculations, we show that excess charge on the polar TaO<sub>2</sub> termination of KTaO<sub>3</sub>(001) forms more complex electronic states with different degrees of spatial and electronic localization: charge density waves (CDW) coexist with strongly-localized electron polarons and bipolarons. These surface electronic reconstructions, originating from the combined action of electron-lattice interaction and electronic correlation, are energetically more favorable than the 2DEG solution. They exhibit distinct spectroscopy signals and impact on the surface properties, as manifested by a local suppression of ferroelectric distortions.