Vibrational frequencies and stark tuning rate with continuum electro-chemical models and grand canonical density functional theory

This archive provides the AiiDA workflows, metadata, and computational datasets associated with the study of vibrational frequencies and Stark tuning rates at electrochemical interfaces within the framework of grand-canonical density functional theory (GC-DFT) combined with continuum electrochemical models.

In this work, the electrochemical potential is treated as a degree of freedom by adjusting the number of electrons in the Kohn-Sham equations, enabling simulations at fixed potential. Based on the relationship between free energy and grand potential, physical properties such as atomic forces, vibrational frequencies, and Stark tuning rates are consistently evaluated. While atomic forces are found to be equivalent to Hellmann-Feynman forces in the canonical ensemble, vibrational frequencies and Stark tuning rates exhibit distinct behavior under grand-canonical conditions.

The archive contains input parameters, workflows, and computed results obtained using finite-displacement methods for the evaluation of vibrational properties and Stark tuning rates. These data enable the reproduction of the results reported in the associated publication and provide a reference for future studies of electrochemical interfaces under constant potential conditions.