Abstract A second-derivative smoothing technique, commonly used in inversion work, is applied to the problem of inferring total columnar ozone amounts and aerosol optical depths. The application is unique in that the unknowns (i.e., total columnar ozone and aerosol optical depth) may be solved for directly without employing standard inversion methods. It is shown, however, that by employing inversion constraints, better solutions are normally obtained. The current method requires radiometric measurements of total optical depth through the Chappuis ozone band. It assumes no a priori shape for the aerosol optical depth versus wavelength profile and makes no assumptions about the ozone amount. Thus, the method is quite versatile and able to deal with varying total ozone and various aerosol size distributions. The technique is applied first in simulation, then to 119 days of measurements taken in Tucson, Arizona, that are compared to TOMS values for the same dates. The technique is also applied to two measure...