We present new results on the quantum control of systems with infinitely large Hilbert spaces. A control-theoretic analysis of the control of trapped-ion quantum states via optical pulses is performed. We demonstrate how resonant bichromatic fields can be applied in two contrasting ways--one that makes the system completely uncontrollable and the other that makes the system controllable. In some interesting cases, the Hilbert space of the qubit-harmonic oscillator can be made finite, and the Schrödinger equation controllable via bichromatic resonant pulses. Extending this analysis to the quantum states of two ions, a new scheme for producing entangled qubits is discovered.