The greater part of the experimental research, described in this thesis, has been devoted to an investigation, by direct electrical methods, of the formation of ionised molecules in mercury vapour and helium. […] This thesis is divided into four parts. The first contains a brief outline of the quantum theory of the atom and the molecule, a summary of our present knowledge of the interchange of energy in various collision processes, and a discussion of the theory of the thermionic emission from a heated filament and its applications. Particular reference for the development of the experimental research described in Parts 2, 3 and 4.