This dataset contains comprehensive measurements of aerosol microphysical, chemical, and optical properties derived for both dry and ambient conditions from in situ measurements made during the four ATom campaigns. The dataset includes composition-resolved size distributions the integrated mass of sulfate, organics, nitrate, sea salt, dust, black carbon, and other compounds in coarse and fine fractions; extinction and absorption coefficients from each species at both dry and ambient conditions; asymmetry parameters; Angstrom exponents; and fitted lognormal functions to describe the size distribution. Optical parameters are calculated for 10 wavelengths from the near UV to the near IR, and size distributions range from 3 nm to 50 um in diameter. One file contains these data at 1-minute time intervals. Another file contains a subset of these data averaged into 1-km vertical bins for each vertical profile the aircraft made, as well as composition-resolved integrated aerosol optical depth derived from each profile. The concentration of cloud condensation nuclei is calculated for 5 supersaturations.