Reply to: “Comment on ‘Stratospheric Aerosol Composition Observed by the Atmospheric Chemistry Experiment Following the 2019 Raikoke Eruption’ by Boone et al.” by Ansmann et al.

Abstract

AbstractThe question of stratospheric aerosol type following the Raikoke eruption is revisited. Raman lidar measurements suggest the aerosols are predominately smoke, while Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE‐FTS) results indicate the aerosols are predominately sulfate aerosols. The suggested mechanism of smoke particles self‐lofting into the stratosphere is inconsistent with observations in 2020, when more severe Siberian fires failed to invoke a response even vaguely similar to 2019. A side‐by side comparison of the Sarychev and Raikoke eruptions invalidates model calculations that suggest sulfate aerosols should be at levels too low to explain the observed aerosol loading. Structure in infrared absorption spectra provides conclusive evidence of composition, a unique fingerprint for identifying aerosol type. Such information cannot be misinterpreted so long as there is sufficient resolution and spectral coverage. ACE‐FTS infrared aerosol spectra often have an order of magnitude stronger absorption than that of background sulfate aerosols. These spectra can be accurately reproduced by laboratory measured sulfate aerosol spectroscopic information, providing unambiguous identification of the aerosols as sulfate. Visual inspection of thousands of infrared aerosol spectra from the period following the Raikoke eruption indicates the aerosols in the lower stratosphere are predominately sulfate, with no indication of smoke. The lidar study's identification of the aerosols as smoke was based primarily on observed lidar ratios that were more consistent with a material that absorbed significantly at the lidar wavelengths, inconsistent with expectations for sulfate aerosols. However, this could indicate the presence of a substance dissolved in the sulfate aerosols absorbing at those wavelengths rather than smoke particles.