Optical control of excited states of alpha-perylene crystal was realized by a femtosecond optimized pulse shaping method using Genetic Algorithm (GA). We succeeded in controlling the emission spectral feature of an a-perylene crystal; the intensity of E-emission was increased by a factor of 1.4 without the change of Y-emission intensity. Furthermore, we found a near-infrared pulse shape whose multi-photon excitation efficiency is larger than that of a single femtosecond pulse by a factor of two. On the auto-correlation traces of these shaped pulses, the several satellite peaks appeared beside the main peak. The origin and mechanism of the attained change were discussed. (C) 2003 Elsevier B.V. All rights reserved.