A combined experimental and theoretical study of the photo-physical, laser properties and  molecular structures of three relatively recent Pyrromethene (PM) class dyes, PM597, PM580 and PM567, have been carried out. Laser characteristics of these three PM dyes were compared with three other widely used Rhodamine (RH) class dyes, RH6G, RHB and KRS, using a  arrow-band dye laser setup, transversely pumped by the second harmonic (532 nm) of a Q-switched Nd-YAG laser. In addition to generating comparative data of these dyes for optimal use in dye lasers, we observed that unlike the RH dyes, the PM dyes show high efficiencies and wide tunability, despite the low fluorescence yield and high rate of non-radiative decay. Particularly, PM597 dye, in spite of a very low quantum yield of fluorescence (f = 0.42), high non-radiative decay rate, and a large distortion from planarity in its excited state, when used in a laser cavity it exhibited similar laser efficiency and a beneficially wider tuning curve in comparison to other two PM dyes. Theoretical studies were carried out applying density functional theory and time-dependent density functional theory (DFT/TDDFT) to obtain new information on ground and the first excited state geometrical parameters of the PM dyes. Good correlation between calculated molecular properties and experimental results was observed for the evolution of the longest wavelength absorption maximum.