ABSTRACT Semi-empirical Quantum-Chemical calculations of the photophysical molecular properties of cyanoanthracene and surrounding argon cell under different thermodynamical conditions were performed using the MD DL_POLY code. Photophysical scheme of the lowest energy levels and transition probabilities was plotted for the individual molecule. Vibrational profiles of the long-wave absorption electronic band and the first excited Frank-Condon singlet state with fluorescent live-times of the oscillating molecule were obtained. Based on the theoretical results, experimental spectroscopic data have been interpreted.