We report on the vibrational population relaxation dynamics of three tetracene vibrational modes (1462, 1383, and 1293 cm(-1)) in eight n-alkane solvents. The 1462 and 1383 cm(-1) resonances in tetracene are Raman-active fundamental vibrational modes, and the 1293 cm(-1) mode is a Raman-active combination mode (307 + 986 cm(-1)). The vibrational population relaxation times (T-1) for these modes range from <10 to similar to 40 ps, depending on the identity of the solvent and the vibrational mode. These data are indicative of local solvent organization around the tetracene molecule. Comparison of these data to those we reported previously for perylene in the same solvents indicates that n-alkane solvent-solute coupling is more efficient for tetracene, in general, than for perylene. We interpret the comparatively efficient relaxation of tetracene in terms of short-range molecular alignment.