Anion-order driven polar interfaces at LaTiO$_2$N surfaces

Abstract: Perovskite oxynitrides have recently attracted attention for their ability to photocatalytically split water. Compared to oxides the arrangement of anions in the material represents a further structural degree of freedom. The bulk oxynitride LaTiO$_2$N prefers a bonding-dominated \textit{cis} nitrogen arrangement, while we have previously shown that the (001) surface prefers a non-polar \textit{trans} order to compensate polarity. Here we consider, using density functional theory calculations, the polar/non-polar interface that would necessarily be present between the two anion orders. We show that the Ti-terminated surface will adopt up to two \textit{trans} ordered surface layers, which has a beneficial effect on the oxygen evolution efficiency. We then consider the hypothetical case of a polar \textit{cis} ordered surface layer atop a non-polar \textit{trans} bulk and show that similar electronic reconstructions as in the LaAlO$_3$/SrTiO$_3$ interface can be expected when interfaces between different anion orders are engineered in one and the same oxynitride material.