The intensity and polarization of the twilight-sky background were measured during the epoch of “purple lights” after the Raikoke volcanic eruption in the summer of 2019. The increase in brightness paired with the decrease in polarization was registered, and the changes were especially noticeable in the dusk segment. The altitude distribution of aerosol particles and their mean size were found with previously developed techniques. The median radius of the lognormal distribution (0.11 μm) is typical of the background conditions or weak eruptions; however, the aerosols were mostly concentrated in the upper troposphere and near the tropopause rather than in the stratosphere. From comparison with satellite data obtained almost a decade ago after similar eruptions (like those of the Kasatochi volcano and others), it has been shown that the properties of their aerosols are similar, which confirms that the purple light phenomenon observed in 2019 was of volcanic origin.