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As highly reactive intermediates, radicals are responsible for a vast array of fundamental gas and condensed phase processes ranging from atmospheric chemistry1 to combustion2, 3 to molecular biology. 4 However, since concentrations under steady-state conditions can be vanishingly small, this enhanced reactivity also makes radical species experimentally challenging to study in detail. Consequently, there have been long standing efforts towards the development of increasingly sensitive methods for probing radicals under controlled laboratory conditions. 5–11 Although there has been a wealth of information obtained via the study of such radicals trapped in cryogenic matrices, 12, 13 of special fundamental interest are methods that produce high densities of radicals under isolated, gas-phase conditions, where interactions with the condensed phase environment can be neglected. Of particular relevance to this …