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Liquid water can support positive and negative hydrated charge defects, creating a chemical regime in which selective stoichiometric removal or generation of one dissolved charge may produce a counterion-deficient aqueous phase. A chemistry-first theoretical framework is developed for such states using liquid water as the anchor system. The central claim is chemical rather than electrostatic: the dissolved phase may lack conventional ionic counterions even though global charge conservation remains exact. The physical analysis is introduced only to explain that chemical claim, to show why the bulk liquid remains approximately electroneutral on the Maxwell timescale, why any finite net charge is localized at the phase boundary, and why charge above the Rayleigh limit leaks or discharges to the surroundings until the interface returns below the capillary stability threshold. The positive and negative aqueous branches are written explicitly through He2+ +H2O(l) −−−→ He(g) +2H+(aq) + 1/2O2(g) and 2e– + 2H2O(l) −−−→ 2OH– (aq) + H2(g). The oxygen lone-pair regions are identified as the highest localized occupied electron density in water and therefore as the most natural local electronic site for low-energy helium-ion electron scavenging. A conservative entry-energy criterion is imposed such that the incoming-particle kinetic energy remains at most one-tenth of the energy required to cleave the weakest bond in the solvent. For water, taking the O–H bond energy as approximately 5.15 eV, this gives Eentry ≤ 0.515 eV. A thermodynamic bookkeeping section makes explicit that conversion of one mole of He2+ to neutral helium corresponds to an internal energy release of approximately 7623 kJmol−1, so any practical implementation of the positive branch would require active cooling and heat removal. The resulting framework yields explicit equations for stoichiometric current scaling, transport, interfacial charge localization, Rayleigh-limited discharge, thermodynamic cycling, and scale-general operation from laboratory volumes to ton-scale reactors, provided the same admissibility inequalities remain satisfied.