Band alignment study at the SrTaO2N / H2O interface varying lattice constants and surface termination from first-principles calculations

BASTIDAS BRICEÑO, R.C.; FERNANDEZ, V.I.; ALONSO, R.E.

Computational Condensed Matter

Elsevier B.V.

Año: 2023 vol. 34

In the search for new renewable energy to replace fossil fuels, Hydrogen is one of the most promising candidates for clean energy production. But cheap Hydrogen separation and storage is still a big challenge. Photoelectrochemical devices look promising for the decomposition of the water molecule into 2H2 + O2. Every day new materials and combinations are discovered or invented to improve the efficiency of the complex total process. A necessary condition for the photoelectrochemical process to work without a bias voltage is that the minimum of the semiconductor conduction band must be more positive than the reduction potential H+ to H2, whereas the maximum of the semiconductor valence band must be more negative than the oxidation potential of H2O to O2. Thus, band alignment studies in interfaces of semiconductors with water become of vital importance. In this work, first-principles calculations based on density–functional theory (DFT) in the all-electron and the pseudo-potential approaches have been performed for the analysis of the band alignment in SrTaO2N/H2O interfaces. Different surface orientations were analyzed, together with the dependence of the gap and band alignment with lattice constants for systems grown on mismatched substrates. Water structures were built from classical molecular dynamics and its electronic structure calculated using DFT. The calculations show that the SrTaO2N (001) is suitable for photoelectrochemical applications on a wide range of lattice constant a, except for a compression/elongation of −2%, −1% and 3%, while SrTaO2N (110) results suitable for photoelectrochemical devices over a wider range of lattice constants from −1% to 3%.