Electrochemical stability and light-harvesting ability of silicon photoelectrodes in aqueous environments
arXiv:1808.00392 · doi:10.1063/1.5093810
Abstract
We consider the factors that affect the photoactivity of silicon electrodes for the water-splitting reaction using a self-consistent continuum solvation (SCCS) model of the solid-liquid interface. This model allows us to calculate the charge-voltage response, Schottky barriers, and surface stability of different terminations while accounting for the interactions between the charge-pinning centers at the surface and the depletion region of the semiconductor. We predict that the most stable oxidized surface does not have a favorable Schottky barrier, which further explains the low solar-to-hydrogen performance of passivated silicon electrodes.
20 pages, 5 figures, plus supporting information
References in corpus (11)
- Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
- Hubbard parameters from density-functional perturbation theory
- Controlling the Schottky barrier at MoS2|metal contacts by inserting a BN monolayer
- Schottky barrier formation and band bending revealed by first principles calculations
- Quantum-continuum simulation of underpotential deposition at electrified metal-solution interfaces
- Continuum models of the electrochemical diffuse layer in electronic-structure calculations
- First-Principles Approach for Energy Level Alignment at Aqueous Semiconductor Interfaces
- Koopmans-compliant spectral functionals for extended systems
- Quantum-continuum simulation of the electrochemical response of pseudocapacitor electrodes from realistic conditions
- Quantum-continuum calculation of the surface states and electrical response of silicon in solution
- Voltage effects on the stability of Pd ensembles in Pd-Au/Au(111) surface alloys