Modulation of electron carrier density at the n-type LaAlO3/SrTiO3 interface by water adsorption

TL;DR

This study uses first-principles calculations to show how water adsorption and dissociation at the LaAlO3 surface can modulate the electronic properties and carrier density of the LaAlO3/SrTiO3 interface, enabling control over its conductivity.

Contribution

It reveals the effects of water molecule dissociation on the electronic structure and carrier density at the LAO/STO interface, proposing methods to control interface conductivity through water adsorption.

Findings

Water dissociation shifts the valence band maximum, reducing the band gap.

At 1/2 ML dissociated water coverage, the interface becomes metallic.

Carrier density increases with more dissociated water molecules.

Abstract

We investigate energetic stability and dissociation dynamics of water adsorption at the LaAlO3 surface of the n-type LaAlO3/SrTiO3 (LAO/STO) interface and its effect on electronic properties of the interface by carrying out first-principles electronic structure calculations. In an ambient atmosphere at room temperature the configuration of 1 monolayer (ML) of water molecules including 3/4 ML of dissociated water molecules adsorbed at the surface is found to be most stable, the configuration of 1 ML of dissociated water molecules is metastable. Water molecule dissociation induces a shift-up of the valence band maximum (VBM) of the LAO surface, reducing the gap between the VBM of the LAO surface and the conduction band minimum of the STO. For the LAO/STO interface with three LAO unit-cell layers, once the coverage of dissociated water molecules reaches 1/2 ML the gap is closed, the interface becomes metallic and the carrier density at the LAO/STO interface increases with increasing the coverage of dissociated water molecules. Our findings suggest two ways to control the conductivity at the LAO/STO interface: (I) insulator-metal transition by adsorbing a mount of water at the bare surface; (II) carrier density change by the transition between the most stable and the metastable adsorption configurations for 1 ML coverage in an ambient atmosphere at room temperature.