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We report conclusive evidence of an efficient cooling mechanism via the electronic radiative transitions of hot small molecular anions isolated in vacuum. We stored C6(-) and C6H(-) in an ion storage ring and observed laser-induced electron detachment with delays up to several milliseconds. The terminal hydrogen atom caused a drastic change in the decay profiles. The decay of photoexcited C6H(-) is slow and nonexponential, which can be explained by depletion cooling, whereas that for C6(-) occurs extremely fast, on a time scale below 0.1 ms and can only be explained by electronic radiative cooling via low-lying electronic excited states.

We have detected visible photons emitted from the thermally populated electronic excited state, namely recurrent fluorescence (RF), of C_{6}^{-} stored in an electrostatic ion storage ring. Clear evidence is provided to distinguish RF from normal fluorescence, based on the temporal profile of detected photons synchronized with the revolution of C_{6}^{-} in the ring, for which the time scale is far longer than the lifetime of the intact photoexcited state. The relaxation (cooling) process via RF is likely to be commonplace for isolated molecular systems and crucial to the stabilization of molecules in interstellar environments.