Through diverse examples we have shown that controlling ϕ M rather than E DF T f makes the CIP-DFT approach widely applicable to computational studies of electrochemical systems under constant electrode potential conditions; this is true even in situations where the constant E DF T f method is not able to mimic the applied electrode potential. The broad applicability of CIP-DFT originates from the rigorous definition of (single) electrode potentials given in Eq. ( ). CIP-DFT directly fixes the experimentally relevant electron bath electrochemical potential (μ bath e