Interfaces between water and semiconductors from first principles

We describe the characterization of pristine and electrified aqueous interfaces with semiconductors and insulators using first principles simulations and discuss how to integrate computational and experimental data to obtain molecular-level models for the prediction of multiple properties. We discuss interfacial vibrational [1] and the electronic properties [2], with focus on disordered carbon electrodes [3] and oxide photoelectrodes [2,4,5], and electrochemical properties. Finally, we present recent predictions on how to probe aqueous interfaces with quantum sensors [6].

 

[1] Raman Spectra of Electrified Si-Water Interfaces: First Principles Simulations, Zifan Ye et al.  J. Phys. Chem. Lett. 15, 51-68 (2024).

[2] e.g. p-Type BiVO4 for Solar O2 Reduction to H2O2, Daye Seo*, Vrindaa Somjit* et al. J. Am. Chem. Soc. 147, 3261–3273 (2025)

[3] Unlocking Mesoscopic Disorder in Graphitic Carbon with Spectroelectrochemistry, Ry Papadopoulos*, Benjamin Masters*, Arpan Kundu* et al. Angew. Chem. Int. Ed. e202420680 (2025).

[4] Effects of solvation and temperature on the energetics of BiVO4 surfaces with varying composition for solar water splitting, Giacomo Melani et al. ACS Energy Lett. 9, 5166-5171 (2024).

[5] Impact of the Atomic Structure at the BiVO4/TiO2 Interface on the Electronic Properties and Performance of BiVO4/TiO2 Photoanodes, Dae Han Wi*, Kana Ishisone*, et al. J. Am. Chem. Soc. 147, 34, 30851–30862 (2025).

[6] Probing aqueous interfaces with spin defects, Alfonso Castillo, Gustavo R. Perez-Lemus, Mykyta Onizhuk, and Giulia Galli Submitted, JCP 2025 (accepted).