Comparisons between measured and calculated aerosol scattering, backscattering, and absorption coefficients were made based on in situ, ground-based measurements during the Melpitz INTensive (MINT) and Lindenberg Aerosol Characterization Experiment 1998 (LACE 98) field studies. Furthermore, airborne measurements made with the same type of instruments are reviewed and compared with the ground-based measurements. Agreement between measured and calculated values is on the order of ¿20% for scattering and backscattering coefficients. A sensitivity analysis showed a large influence on the calculated particle scattering and backscattering coefficients resulting from sizing uncertainties in the measured number size distributions. Measured absorption coefficients were significantly smaller than the corresponding calculated values. The largest uncertainty for the calculated absorption coefficients resulted from the size-dependent fraction of elemental carbon (EC) of the aerosol. A correction for the measured fractions of EC could significantly improve the agreement between measured and calculated absorption coefficients. The overall uncertainty of the calculated values was investigated with a Monte Carlo method by simultaneously and randomly varying the input parameters of the calculations, where the variation of each parameter was bounded by its uncertainty. The measurements were mostly found to be within the range of uncertainties of the calculations, with uncertainties for the calculated scattering and backscattering coefficients of about ¿20% and for the absorption coefficients of about ¿30%. Thus, to increase the accuracy of calculated scattering, backscattering, and absorption coefficients, it is crucial to further reduce the error in particle number size distribution measurement techniques. In addition, further improvement of the techniques for measuring absorption coefficients and further investigation of the measurement of the fraction of EC of the aerosol is necessary.