Evolution from a molecular Rydberg gas to an ultracold plasma in a seeded supersonic expansion of NO

We report the spontaneous formation of a plasma from a gas of cold Rydberg molecules. Double-resonant laser excitation promotes nitric oxide, cooled to 1 K in a seeded supersonic molecular beam, to single Rydberg states extending as deep as 80 cm${}^{-1}$ below the lowest ionization threshold. The density of excited molecules in the illuminated volume is as high as 1 x 10${}^{13}$ cm${}^{-3}$. This population evolves to produce prompt free electrons and a durable cold plasma of electrons and intact NO${}^{+}$ ions.