Results of an experimental study on the unusual "inverse" charge state (H+Na-) in salts where the H+ ion is sequestered, combined with our earlier theoretical calculations on an unsequestered model compound (Me3N-H+...Na-), prompted us to further investigate such systems. In particular, we examined Et3N-H+...K- because considerations of the proton affinity of the amine and of the metal-hydride bond strength suggested that this ion-pair complex might be more stable to proton abstraction than was Me3N-H+...Na-. In the present work, the ground-state potential energy surface of the Et3N-H+...K- ion pair was examined using second-order Moller-Plesset perturbation theory and 6-311++G** basis sets. We found Et3N-H+...K- to be metastable to dissociation with a barrier of 8 kcal mol(-1) (computed at the CCSD(T) level of theory). This barrier indeed is substantially larger than that found earlier for (Me3N-H+...Na-) and suggests that unsequestered inverse-charged H+M- ion-pair salts may offer a reasonable route to creating high-energy materials if a means for synthesizing them in the laboratory can be designed.