Persistent radical cations can be generated in V ∝ PMO, a periodic mesoporous organosilica incorporating a viologen in its silicate framework. Photoexcitation of V ∝ PMO forms a geminate viologen-halide ion pair that can undergo rapid charge recombination or electron hopping to form the nongeminate ion pair, which persists for minutes (see picture). In contrast, viologen-halide CT complexes in solution undergo complete charge recombination on the sub-nanosecond timescale.