Vibrational eigenvalues with estimated errors <5x10(-2) cm(-1) and their corresponding cm eigenfunctions for J=0 5D (planar) acetylene modeled by the Halonen-Child-Carter potential-energy surface are obtained using an energy-shifted, imaginary-time Lanczos propagation of symmetry-adapted wave packets. A lower resolution (similar to 4 cm(-1)) vibrational eigenspectrum of the system is also calculated by the Fourier transform of the autocorrelation of an appropriate wave packet. The eigenvalues from both approaches are in excellent agreement. The wave function of the molecule is represented in a direct-product discrete variable representation (DVR) with nearly 300 000 grid points. Our results are compared with the previously reported theoretical and experimental values. We use our 69 computed eigenstates as a basis to perform an optimal control simulation of selective two-photon excitation of the symmetric CH-stretch made with an infrared, linearly polarized, transform-limited, and subpicosecond-picosecond laser guise. The resulting optimal laser pulses, which are then tested on the full DVR grid, fall within the capabilities of current powerful, subpicosecond, and tunable light sources. (C) 1997 American Institute of Physics.