We report on Auger stimulated ion desorption via Coulomb explosion from surface self-assembled alkylthiol and fluorocarbon molecular layers, triggered by K-capture decay of an imbedded radioactive 55Fe atom. The charge state of the ejecta is determined by charge exchange in binary atomic collisions in bulk and electron tunneling outside the solid, as well as by fragmentation of electronically excited molecules or molecular fragments. We describe the first nonbeam experiments documenting positive and abundant negative ion desorption due solely to core electron excitation after radioactive decay.