Spectral and phase shaping of femtosecond laser pulses is used to selectively excite vibrational wave packets on the ground (S-0) and excited (S-1) electronic states in the laser dye LD690. The transient absorption signals observed following excitation near the peak of the ground-state absorption spectrum are characterized by a dominant 586 cm(-1) vibrational mode. This vibration is assigned to a wave packet on the S-0 potential energy surface. When the excitation pulse is tuned to the blue wing of the absorption spectrum, a lower frequency 568 cm(-1) vibration dominates the response. This lower frequency mode is assigned to a vibrational wave packet on the S-1 electronic state. The spectrum and phase of the excitation pulse also influence both the dephasing of the vibrational wave packet and the amplitude profiles of the oscillations as a function of probe wavelength. Excitation by blue-tuned, positively chirped pulses slows the apparent dephasing of the vibrational coherences compared with a transform-limited pulse having the same spectrum. Blue-tuned negatively chirped excitation pulses suppress the observation of coherent oscillations in the ground state.