Constructive techniques for controlling a coupled, heteronuclear spin system, via bounded amplitude sinusoidal pulses are presented. The technique prepares exactly any desired unitary generator in a rotating frame, through constant controls. Passage to the original coordinates provides a procedure to prepare arbitrary unitary generators, via bounded amplitude piecewise sinusoidal pulses whose frequency is one of the two Larmor frequencies and whose phase takes one of two values. The techniques are based on a certain Cartan decomposition of SU (4) available in the literature. A method for determining the parameters entering this Cartan decomposition, in terms of the entries of the target unitary generator, is also provided.