In an earlier paper (Cohen and Coulson(3), referred to hereafter as I), it was shown that satisfactory energy eigenvalues and eigenfunctions for various even σ-states of may be obtained using a single-centre expansion, provided that the radial functions are properly determined. In particular, the ground-state energy at the equilibrium internuclear separation of 2 a.u. was found to be within 0·25% of the exact value (Bates, Ledsham and Stewart (2)), and the eigenfunction reproduced all the characteristics of the exact wave-function. The method has now been extended to the odd σ-states, as well as to the two lowest π-states (2pπu, 3dπg), and the results are in good agreement with the calculations of Bates et al.