The theoretical principles of the method of polarized laser probing of an aspherical atmospheric aerosol, oriented in space, are considered. An approach to estimating the effectness of methods of spectroscopic diagnostics of organic molecules, based on the study of photophysical processes occurring in them, is described. The possibilities of optical diagnostics of gaseous and aerosol media by short and ultrashort pulses on the basis of nonsteady and nonlinear effects are demonstrated.